Co-reporter:Ling-Xia Zuo, Wen-Jing Wang, Rong-Bin Song, Jing-Jing Lv, Li-Ping Jiang, and Jun-Jie Zhu
ACS Sustainable Chemistry & Engineering November 6, 2017 Volume 5(Issue 11) pp:10275-10275
Publication Date(Web):September 27, 2017
DOI:10.1021/acssuschemeng.7b02291
The demand on the highly efficient and low-cost cathodic electrocatalysts for commercialization of fuel cells is rapidly increasing. One smart route for obtaining these ideal electrocatalysts is extracting active carbon materials from natural and cheap biomass waste. Here, we prepared a novel nitrogen self-doped porous graphitic carbon nanosheets (NPGCNs-NaCl) derived from a nitrogen-rich pruning of Lycium barbarum L. using NaCl crystal as intercalation agent. The as-obtained NPGCNs-NaCl possessed porous structure, large surface area, increased content of nitrogen and high graphitic carbon, and thus making it with high electrocatalytic activity for oxygen reduction reaction (ORR). Most importantly, significantly enhanced stability and tolerance against methanol were observed compared with commercial Pt/C catalyst in alkaline solution. This work is believed to open a new avenue for manufacturing advanced and low-cost ORR electrocatalysts in fuel cells from biomass waste.Keywords: NaCl crystal intercalation; Nitrogen self-doped porous graphitic carbon nanosheets; Oxygen reduction reaction; Pruning of Lycium barbarum L.;
Co-reporter:Xiao-Mei Shi, Gao-Chao FanQingming Shen, Jun-Jie Zhu
ACS Applied Materials & Interfaces December 28, 2016 Volume 8(Issue 51) pp:
Publication Date(Web):December 8, 2016
DOI:10.1021/acsami.6b14466
Sensitive and accurate analysis of DNA is crucial to better understanding of DNA functions and early diagnosis of fatal disease. Herein, an enhanced photoelectrochemical (PEC) DNA biosensor was proposed based on dual-signal amplification via coupling inorganic–organic nanocomposites sensitization with λ-exonuclease (λ-Exo)-assisted target recycling. The short DNA sequence about chronic myelogenous leukemia (CML, type b3a2) was selected as target DNA (tDNA). ZnO nanoplates were deposited with CdS nanocrystals to form ZnO/CdS hetero-nanostructure, and it was used as PEC substrate for immobilizing hairpin DNA (hDNA). CdTe quantum dots (QDs) covalently linked with meso-tetra(4-carboxyphenyl)porphine (TCPP) to form CdTe/TCPP inorganic–organic nanocomposites, which were utilized as sensitization agents labeling at the terminal of probe DNA (pDNA). When the hDNA-modified sensing electrode was incubated with tDNA and λ-Exo, hDNA hybridized with tDNA, and meanwhile it could be recognized and cleaved by λ-Exo, resulting in the release of tDNA. The rest of nonhybridized hDNA would continuously hybridize with the released tDNA, cleave by λ-Exo, and set free the tDNA again. After λ-Exo-assisted tDNA recycling, more amounts of short DNA (sDNA) fragments coming from digestion of hDNA produced on the electrode and hybridized with CdTe/TCPP-labeled pDNA (pDNA-CdTe/TCPP conjugates). In this case, the sensitization of CdTe/TCPP inorganic–organic nanocomposites occurred, which evidently extend the absorption range and strengthened the absorption intensity of light energy, and accordingly the photocurrent signal significantly promoted. Through introducing the dual-signal amplification tactics, the developed PEC assay allowed a low calculated detection limit of 25.6 aM with a wide detection scope from 0.1 fM to 5 pM for sensitive and selective determination of tDNA.Keywords: DNA assay; photoelectrochemistry; sensitization; target recycling; λ-exonuclease;
Co-reporter:Jingjing Xue, Ziyi Zhang, Fenfen Zheng, Qin Xu, Jinchun Xu, Guizheng Zou, Lingling Li, and Jun-Jie Zhu
Analytical Chemistry August 15, 2017 Volume 89(Issue 16) pp:8212-8212
Publication Date(Web):July 21, 2017
DOI:10.1021/acs.analchem.7b02291
Halide perovskite materials have emerged as a new class of revolutionary photovoltaic and optoelectronic nanomaterials. However, the study on electrochemiluminescence (ECL) from halide perovskite nanomaterials is still in its infancy due to their instability, sensitivity, and difficulties in purification and film formation. Here, we propose a scraping coating method for the fabrication of high-quality halide perovskite quantum dot (QD) film on electrode, which shows dense and uniform packing with minimum grain size. When CsPbBr3 QDs are taken as model materials, highly efficient ECL can be obtained from such perovskite QD film with anhydrous ethyl acetate as both electrolyte and coreactant. The CsPbBr3 QD film displays intense and stable ECL with ultranarrow emission spectrum bandwidth (24 nm). The CsPbBr3 QD film shows an extremely high ECL efficiency which is up to 5 times relative to the standard Ru(bpy)32+/tri-n-propylamine system. This approach is universal and also applies to hybrid organic–inorganic halide perovskite QDs. This work not only extends the properties and applications of halide perovskite materials but also provides a new method for the in-depth study on the structure and properties of these kinds of materials.
Co-reporter:Ling-Xia Zuo, Li-Ping Jiang, E.S. Abdel-Halim, Jun-Jie Zhu
Ultrasonics Sonochemistry 2017 Volume 35(Part A) pp:219-225
Publication Date(Web):March 2017
DOI:10.1016/j.ultsonch.2016.09.021
Porous MnO2 as a non-noble metal oxygen reduction reaction (ORR) electrocatalyst was prepared by a simple sonochemical route. The as-prepared porous MnO2 exhibited higher electrocatalytic activity, superior stability and better methanol tolerance than commercial Pt/C catalyst in alkaline media. Furthermore, the ORR proceeded via a nearly four-electron pathway. Cyclic voltammetry (CV) and rotating-disk electrode (RDE) measurements verified that the ORR enhancement was attributed to the porous structure and good dispersity, which facilitated sufficient transport of ions, electrons, O2 and other reactants in the process of ORR. The results indicated that a facile and feasible sonochemical route could be used to prepare highly active porous MnO2 electrocatalyst for ORR, which might be promising for direct methanol fuel cells.
Co-reporter:Ling-Xia Zuo, Li-Ping Jiang, Jun-Jie Zhu
Ultrasonics Sonochemistry 2017 Volume 35(Part B) pp:681-688
Publication Date(Web):March 2017
DOI:10.1016/j.ultsonch.2016.02.006
For the alkaline fuel cell cathode reaction, it is very essential to develop novel catalysts with superior catalytic properties. Here, we report the synthesis of highly active and stable MoS2/Pd composites for the oxygen reduction reaction (ORR), via a simple, eco-friendly sonochemical method. The bulk MoS2 was first transformed into single and few layers MoS2 nanosheets through ultrasonic exfoliation. Then the exfoliated MoS2 nanosheets served as supporting materials for the nucleation and further in-situ growth of Pd nanoparticles to form MoS2/Pd composites via ultrasonic irradiation. Cyclic voltammetry and rotating disk voltammetry measurements demonstrate that as-prepared MoS2/Pd composites which provides a direct four-electron pathway for the ORR, have better electrocatalytic activity, long-term operation stability than commercial Pt/C catalyst. We expect that the present work would provide a promising strategy for the development of efficient oxygen reduction electrocatalyst. In addition, this study can also be extended to the preparation of other hybrid with desirable morphologies and functions.
Co-reporter:Guoliang Liu, Jingjing Li, Da-Qian Feng, Jun-Jie ZhuWei Wang
Analytical Chemistry 2017 Volume 89(Issue 1) pp:
Publication Date(Web):December 8, 2016
DOI:10.1021/acs.analchem.6b04362
An activatable silver nanoclusters beacon (ASNCB) was synthesized through a facile one-pot approach and applied for multiplex DNAs, small molecule, and protein sensing. Multifunctional single-stranded DNA sequences are rationally designed and used for ASNCB in situ synthesis. Via target-responsive structure transformation of ASNCB, target recognition induced ASNCB conformational transition and lit up the fluorescent signal of silver nanoclusters. By further implementing two different color ASNCBs (520 and 600 nm), the parallel multiplexed analysis of two target genes (Influenza A virus genes H1N1 and H5N1) is achieved. Additionally, with the introduction of aptamer for the design of the molecular beacon, the detections of small molecule adenosine triphosphate (ATP) and biomacromolecule thrombin have also been realized. This is the first time that an activatable fluorescent silver nanoclusters (Ag NCs)-based probe and the target recognition have been integrated into a single process, which provides a versatile platform for different analytes in a facile way. The successful application of our proposed ASNCB in real sample analysis and ATP imaging in living cells further displayed its promising potential for fluorescence sensing.
Co-reporter:Lingling Li, Ying Chen, and Jun-Jie Zhu
Analytical Chemistry 2017 Volume 89(Issue 1) pp:
Publication Date(Web):November 30, 2016
DOI:10.1021/acs.analchem.6b04675
Co-reporter:Chen Cui, Ying Chen, Dechen JiangJun-Jie Zhu, Hong-Yuan Chen
Analytical Chemistry 2017 Volume 89(Issue 4) pp:
Publication Date(Web):February 1, 2017
DOI:10.1021/acs.analchem.6b04305
In this work, a self-electrochemiluminous graphene oxide-capped Au@L012 nanocomposite was prepared as the label at carcinoembryonic (CEA) antibody to detect attomole CEA antigen. To maximize the luminescence intensity, L012 molecules (luminol analogue) were linked with poly(diallyldimethylammonium chloride) (PDDA) to form positive charged PDDA&L012 pairs, which were modified on negative charged Au@nafion nanoparticles to construct a Au@nafion@PDDA&L012 (Au@L012) complex. Graphene oxide with carboxyl groups was capped at Au@L012 complex through electrostatic interaction to serve as an effective matrix for the covalent attachment of CEA antibody. As compared with the traditional used Au nanoparticles modified with luminol, ∼740-fold increase of self-luminescence was observed from this new complex so that CEA antigen as low as 0.5 amol at electrode surface was measurable in the absence of any coreactant. Moreover, the nanocomposite was attached with CEA antigen at MCF-7 cells allowing the detection of CEA antigen from 72 cells. The success in the detection of surface antigen at small population of cells suggested the self-electrochemiluminescence nanocomposite as the new and biosafe label for the ECL immunoassay, which might push the application of ECL for the cellular immunoanalysis.
Co-reporter:Wenjing Wang;Shan Huang;Jingjing Li;Kai Rui;Sai Bi;Jian-Rong Zhang
Chemical Science (2010-Present) 2017 vol. 8(Issue 1) pp:174-180
Publication Date(Web):2016/12/19
DOI:10.1039/C6SC01953F
Telomerase plays a vital role in cancer and aging, and telomerase activity detection has drawn great attention recently. However, a feasible in situ imaging system for intracellular telomerase is still a challenge. Here, we develop a novel approach to image intracellular telomerase activity using DNA-based computation. A cascade nucleic acid logic gate that responded to intracellular telomerase was constructed. A telomerase substrate (TS) probe, extended by intracellular telomerase, worked as an input to initiate computation cascades. In this way, intracellular telomerase could be clearly indicated by fluorophore labeled nucleic acids as the output. Through one-step incubation, evaluation of the intracellular telomerase activity for a HeLa cell line and the ability to differentiate cancer cells from normal cells could be realized. Furthermore, the response of intracellular telomerase activity to a telomerase-inhibiting model drug was observed using the proposed method. Thus, this intracellular telomerase computation device will allow improvements in studying the relationship between telomerase and cancer, and may help to develop telomerase inhibitors. This finding also expands the applications of DNA computational techniques in cells.
Co-reporter:Cui-e Zhao;Panpan Gai;Rongbin Song;Ying Chen;Jianrong Zhang
Chemical Society Reviews 2017 vol. 46(Issue 5) pp:1545-1564
Publication Date(Web):2017/03/06
DOI:10.1039/C6CS00044D
During the past decade, biofuel cells (BFCs) have emerged as an emerging technology on account of their ability to directly generate electricity from biologically renewable catalysts and fuels. Due to the boost in nanotechnology, significant advances have been accomplished in BFCs. Although it is still challenging to promote the performance of BFCs, adopting nanostructured materials for BFC construction has been extensively proposed as an effective and promising strategy to achieve high energy production. In this review, we presented the major novel nanostructured materials applied for BFCs and highlighted the breakthroughs in this field. Based on different natures of the bio-catalysts and electron transfer process at the bio-electrode surfaces, the fundamentals of BFC systems, including enzymatic biofuel cells (EBFCs) and microbial fuel cells (MFCs), have been elucidated. In particular, the principle of electrode materials design has been detailed in terms of enhancing electrical communications between biological catalysts and electrodes. Furthermore, we have provided the applications of BFCs and potential challenges of this technology.
Co-reporter:Gaoxing Su;Huaqiao Jiang;Hongyan Zhu;Jing-Jing Lv;Guohai Yang;Bing Yan
Nanoscale (2009-Present) 2017 vol. 9(Issue 34) pp:12494-12502
Publication Date(Web):2017/08/31
DOI:10.1039/C7NR04046F
Plasmonic Au–Pd nanostructures have drawn significant attention for use in heterogeneous catalysis. In this study, palladium nanodendrite-tipped gold nanorods (PdND-T-AuNRs) were subjected to a facile fabrication under mild reaction conditions. The palladium amounts on the two tips were tunable. In the preparation of PdND-T-AuNRs, dense capped AuNRs, a low reaction temperature, and suitable stabilizing agents were identified as critical reaction parameters for controlling palladium nanodendrites deposited on both ends of AuNRs. After overgrowth with palladium nanodendrites, the longitudinal surface plasmonic resonance peaks of PdND-T-AuNRs were red-shifted from 810 nm to 980 nm. The electrocatalytic activity of PdND-T-AuNRs for ethanol oxidation was examined, which was a bit weaker than that of cuboid core–shell Au–Pd nanodendrites; however, PdND-T-AuNRs were more stable in ethanol electrooxidation. Moreover, the photocatalytic activity of PdND-T-AuNRs for Suzuki cross-coupling reactions was investigated. At room temperature, nearly 100% yield was obtained under laser irradiation. The results can further enhance our capability of fine-tuning the optical, electronic, and catalytic properties of the bimetallic Au–Pd nanostructures.
Co-reporter:Shuwen Guo;Tingxizi Liang;Yongshang Song;Ming Cheng;Xiao-Yu Hu;Leyong Wang
Polymer Chemistry (2010-Present) 2017 vol. 8(Issue 37) pp:5718-5725
Publication Date(Web):2017/09/26
DOI:10.1039/C7PY01259D
The development of smart and targeted drug delivery systems has promising potential to revolutionize cancer chemotherapy. Herein, supramolecular polymersomes were constructed using biocompatible water-soluble pillar[5]arene (WP5) and cationic poly(glutamamide)s (polymer 1) with good biodegradability. Based on the host–guest complexation between WP5 and butyl-ammonium groups on polymer 1, stable supramolecular macromolecular amphiphiles were obtained, which could self-assemble into supramolecular polymersomes. Furthermore, the generated polymersomes were able to encapsulate the hydrophilic anticancer drug mitoxantrone (MTZ) to achieve MTZ-loaded polymersomes. Importantly, decorated with biotin ligands on the surface, these polymersomes exhibited good targeting ability to deliver MTZ specifically to biotin receptor-positive cancer cells. After internalization into cancer cells, the loaded MTZ was released efficiently triggered by the acidic environment-induced polymersome disassembly. Moreover, MTZ-loaded polymersomes with targeting ligands on their surface could not only enhance the anticancer efficiency of MTZ but also effectively reduce the undesirable side effects on normal cells. The present work provides a novel strategy for the construction of smart supramolecular polymersomes, which may hold potential biomedical applications in targeted drug delivery.
Co-reporter:Rongguang Shi, Lu Huang, Xiaoxue Duan, Guohao Sun, Gui Yin, Ruiyong Wang, Jun-jie Zhu
Analytica Chimica Acta 2017 Volume 988(Volume 988) pp:
Publication Date(Web):2 October 2017
DOI:10.1016/j.aca.2017.07.055
•The fluorescent probe NBOH showed superior performance for pH detection in a wide pH range with relatively long emission wavelength.•This probe exhibited strong anti-interference ability, photostability and remarkable reversibility.•Flow cytometry study was carried out showing quantitatively that fluorescence intensity of probe NBOH in cancer cells is nearly tenfold of it in normal cells.•Fluorescence imaging of nude mouse indicated the probe can distinguish tumor tissue out of normal tissue in vivo.•The probe exhibited potential application in cancer removal surgery.Fluorescence imaging with tumor-specific fluorescent probe has emerged as a tool to aid surgeons in the identification and removal of tumor tissue. We report here a new lysosome-targeting fluorescent probe (NBOH) with BODIPY fluorephore to distinguish tumor tissue out of normal tissue based on different pH environment. The probe exhibited remarkable pH-dependent fluorescence behavior in a wide pH range from 3.0 to 11.0, especially a sensitive pH-dependent fluorescence change at pH range between 3.5 and 5.5, corresponding well to the acidic microenvironment of tumor cells, in aqueous solution. The response time of NBOH was extremely short and the photostability was proved to be good. Toxicity test and fluorescence cell imaging together with a sub-cellular localization study were carried out revealing its low biotoxicity and good cell membrane permeability. And NBOH was successfully applied to the imaging of tumor tissue in tumor-bearing mice suggesting potential application to surgery as a tumor-specific probe.Download high-res image (209KB)Download full-size image
Co-reporter:Ying Chen, Shiwei Zhou, Lingling Li, Jun-jie Zhu
Nano Today 2017 Volume 12(Volume 12) pp:
Publication Date(Web):1 February 2017
DOI:10.1016/j.nantod.2016.12.013
•The great potential of multifunctional nanomaterials for ECL bioanalysis is presented.•Deep insights into nanomaterials-based ECL biosensing strategies are discussed.•Recent significant developments of nanomaterials-based ECL biosensors are reviewed.•Novel applications of ECL resonance energy transfer and ECL imaging are highlighted.•Future challenges and prospects of nanomaterials-based ECL bioanalysis are concluded.Nanomaterials with wonderful optical, electrical and chemical properties are widely studied in recent decades. In electrochemiluminescence (ECL) sensing area, nanomaterials have also gained crescent attention for their excellent performance based on different functions, such as innovative luminophores, molecule carriers, electrode modification materials and reaction catalysts. Deep insight into ECL biosensing strategies with multifunctional nanomaterials will benefit the design of advanced sensors. Based on this, nanomaterials-based ECL biosensors have shown more promising potentials than traditional ones in analytical applications. After a brief overview of basic ECL principles and sensing approaches, herein, a general description of nanomaterials-based ECL biosensing is presented, especially with emphasis on recently developed ECL resonance energy transfer (ECL-RET) strategy. Finally, future outlooks are considered in building sensitive ECL biosensors.Download high-res image (97KB)Download full-size image
Co-reporter:Yingying Wang;Lihui Hu;Lingling Li
Journal of Analysis and Testing 2017 Volume 1( Issue 2) pp:13
Publication Date(Web):13 June 2017
DOI:10.1007/s41664-017-0015-7
Fluorescent gold nanoclusters (AuNCs) have recently emerged as a novel kind of promising fluorescent probes for high-performance sensors and bioimaging because of their ultrasmall size (<3 nm), strong luminescence, good photostability, and excellent biocompatibility. Over the past decade, we have witnessed growing popularity of AuNCs in analytical applications and enormous efforts have been devoted to their development. In this review, we provide an update on recent advances in the development of AuNCs in terms of physicochemical properties, synthesis strategies, and bioapplications. The optical, electrochemical, catalytical, and solvatochromic properties of AuNCs are first summarized, which are followed by different ligands or template-assisted controllable synthetic methods. Afterwards functionalization of AuNCs is described in terms of ligand exchange, bioconjugation, and noncovalent interaction. We then focus on the applications of AuNCs as fluorescent probes for detection of metal ions, inorganic anions, small biomolecules, proteins, nucleic acids, drug molecules, pH, and temperature. We also summarize the usage of metal NCs in cellular and in vivo targeting and imaging. Finally, we conclude with a brief look at the future challenges and prospects of the development of AuNCs.
Co-reporter:Shan Huang, Wenjing Wang, Fangfang Cheng, Huiqin Yao, Jun-Jie Zhu
Sensors and Actuators B: Chemical 2017 Volume 242() pp:347-354
Publication Date(Web):April 2017
DOI:10.1016/j.snb.2016.10.123
•The proposed method could realize detection of Hg2+ at low femtomolar concentration.•In this method, mercury could triggering the T-rich DNA machine to produce a large amount of product DNA for signal amplification.•The output PGM signals which came from glucose is related with the amount of product DNA, indirectly quantifying the concentration of Hg2+.•The PGM is expected to have a wide application in routine detection the concentration of Hg2+ in environmental water and biologic samples in everyone’s home.Mercury ion (Hg2+) has threats to human health and the environment even at a low concentration, thus it is desirable to propose a sensitive and portable method to detect it. In this work, it could realize detection of Hg2+ at low femtomolar concentration. Thymine-thymine (T-T) mismatches oligodeoxyribonucleotides were employed as specific recognition elements for selectively capturing Hg2+ to form hairpin structure and triggering the T-rich DNA machine operation to produce a large amount of product DNA for signal amplification. Product DNA connected capture DNA (Capt-DNA) with DNA-invertase conjugation which catalyzed sucrose into glucose. Thus, the output portable glucose meter (PGM) signals which came from glucose is related with the amount of product DNA, indirectly quantifying the concentration of Hg2+. It is shown that the detection limit of this method is as low as 10−17 M and linear range is 10−6–10−17 M without any complicated instrument. What’s more, this novel method could be applied in highly sensitive and selective Hg2+ detection in fish samples. Therefore, owing to the simple operability and portable use of PGM, this method is expected to have a wide application in routine detection the concentration of Hg2+ in environmental water and biologic samples in everyone’s home.
Co-reporter:Dan Guo;Rong-Bin Song;Hao-Hua Shao;Jian-Rong Zhang
Chemical Communications 2017 vol. 53(Issue 72) pp:9967-9970
Publication Date(Web):2017/09/05
DOI:10.1039/C7CC04666A
A new visible-light-assisted microbial fuel cell composed of a three-dimensional nitrogen-doped graphene self-standing sponge anode and a photoresponsive cathode has been developed for achieving multiple energy conversion and a higher power output.
Co-reporter:Yusheng Ji;Panpan Gai;Jun Feng;Linlin Wang;Jianrong Zhang
Journal of Materials Chemistry A 2017 vol. 5(Issue 22) pp:11026-11031
Publication Date(Web):2017/06/06
DOI:10.1039/C7TA01931A
Enzymatic biofuel cells (EBFCs) are considered as a promising approach to meet the requirements of power sources. Electrode materials, which are significant factors to affect the power output of EBFCs, have aroused great interest. Herein, we developed an EBFC using a Fe3O4–carbon nanofiber/gold nanoparticle hybrid as the substrate electrode for improving the performance of the power output. The open-circuit voltage (Eocv) of the designed EBFC reached 0.68 ± 0.03 V, and the maximum power density (Pmax) reached 126 ± 4.5 μW cm−2. The as-prepared EBFC showed 3 times higher Pmax compared to the EBFC based on the carbon nanofiber/gold nanoparticle hybrid, which was ascribed to the good electrocatalytic activity of Fe3O4 NP loaded carbon nanofibers (CNFs), the 3D porous structure of CNFs as well as the uniform distribution of Au NPs. The Fe3O4–CNF/gold nanoparticle hybrid is considered as a promising candidate for constructing electrochemical biosensors and biofuel cells.
Co-reporter:Yong-Ping Dong, Jiao Wang, Ying Peng, Jun-Jie Zhu
Biosensors and Bioelectronics 2017 Volume 94(Volume 94) pp:
Publication Date(Web):15 August 2017
DOI:10.1016/j.bios.2017.03.044
•Luminol ECL can be greatly enhanced by SiQDs in neutral condition.•ECL resonance energy transfer occurred between SiQDs and luminol.•An ECL aptasensor was fabricated to sensitively detect lysozyme.In the present work, electrogenerated chemiluminescence (ECL) of luminol was investigated in neutral condition at a gold electrode in the presence of silicon quantum dots (SiQDs). The results revealed that SiQDs can not only greatly enhance luminol ECL, but also act as energy acceptor to construct a novel ECL resonance energy transfer (ECL-RET) system with luminol. As a result, strong anodic ECL signal was obtained in neutral condition at the bare gold electrode, which is suitable for biosensing application. Lysozyme exhibited apparent inhibiting effect on the ECL-RET system, based on which an ECL aptasensor was fabricated for the sensitive detection of lysozyme. The proposed method showed high sensitivity, good selectivity, and wide linearity for the detection of lysozyme in the range of 5.0×10–14−5.0×10−9 g mL−1 with a detection limit of 5.8×10–15 g mL−1 (3σ). The results suggested that as-proposed luminol/SiQDs ECL biosensor will be promising in the detection enzyme.
Co-reporter:Wenjing Wang;Nitya Sai Reddy Satyavolu;Zhenkun Wu; Dr. Jian-Rong Zhang; Dr. Jun-Jie Zhu; Dr. Yi Lu
Angewandte Chemie 2017 Volume 129(Issue 24) pp:6902-6906
Publication Date(Web):2017/06/06
DOI:10.1002/ange.201701325
AbstractDNAzymes have enjoyed success as metal ion sensors outside cells. Their susceptibility to metal-dependent cleavage during delivery into cells has limited their intracellular applications. To overcome this limitation, a near-infrared (NIR) photothermal activation method is presented for controlling DNAzyme activity in living cells. The system consists of a three-stranded DNAzyme precursor (TSDP), the hybridization of which prevents the DNAzyme from being active. After conjugating the TSDP onto gold nanoshells and upon NIR illumination, the increased temperature dehybridizes the TSDP to release the active DNAzyme, which then carries out metal-ion-dependent cleavage, resulting in releasing the cleaved product containing a fluorophore. Using this construct, detecting Zn2+ in living HeLa cells is demonstrated. This method has expanded the DNAzyme versatility for detecting metal ions in biological systems under NIR light that exhibits lower phototoxicity and higher tissue penetration ability.
Co-reporter:Lingxia Zuo;Liping Jiang
Chinese Journal of Chemistry 2017 Volume 35(Issue 6) pp:969-976
Publication Date(Web):2017/06/01
DOI:10.1002/cjoc.201600829
The preparation of highly active electrocatalysts with good durability and low cost for fuel cells is highly desirable but still remains a significant challenge. Here we synthesized two dimensional (2D) C3N4 nanosheets supported palladium composites (C3N4/Pd) via a simple and convenient sonochemical approach. We have systematically studied the electrocatalytic performance of as-prepared catalysts. We found that the prepared C3N4/Pd composites possessed excellent catalytic activity and stability for oxygen reduction reaction (ORR) in alkaline media. Encouragingly, the C3N4/Pd catalysts exhibit the excellent electrocatalytic activity for methanol oxidation reaction (MOR) in alkaline media, even better than that of the commercial Pt/C catalyst. The excellent electrocatalytic performance of the 2D C3N4 nanosheets supported palladium composites catalysts results from their synergy effect between the ultrathin substrate material with large surface area and excellent dispersion of palladium nanoparticles. This study demonstrates that sonochemical method opens up a new avenue for the preparation of electrocatalysts for fuel cells. We expect these materials are likely to find uses in a broad range of applications, for example, fuel cells, solar cells, batteries and other electrochemical analysis.
Co-reporter:Penghui Zhang;Yan Wang;Jing Lian;Qi Shen;Chen Wang;Bohan Ma;Yuchao Zhang;Tingting Xu;Jianxin Li;Yongping Shao;Feng Xu
Advanced Materials 2017 Volume 29(Issue 36) pp:
Publication Date(Web):2017/09/01
DOI:10.1002/adma.201702311
Nanocarrier surface chemistry plays a vital role in mediating cell internalization and enhancing delivery efficiency during in vivo chemotherapy. Inspired by the ability of proteins to alter their conformation to mediate functions, a pH-/thermal-/glutathione-responsive polymer zipper consisting of cell-penetrating poly(disulfide)s and thermosensitive polymers bearing guanidinium/phosphate (Gu+/pY−) motifs to spatiotemporally tune the surface composition of nanocarriers for precise tumor targeting and efficient drug delivery is developed. Surface engineering allows the nanocarriers to remain undetected during blood circulation and favors passive accumulation at tumor sites, where the acidic microenvironment and photothermal heating break the pY−/Gu+ binding and rupture the zipper, thereby exposing the penetrating shell and causing enhanced cellular uptake via counterion-/thiol-/receptor-mediated endocytosis. The in vivo study demonstrates that by manipulating the surface states on command, the nanocarriers show longer blood circulation time, minimized uptake and drug leakage in normal organs, and enhanced accumulation and efficient drug release at tumor sites, greatly inhibiting tumor growth with only slight damage to normal tissues. If integrated with a photothermal dye approved by the U.S. Food and Drug Administration (FDA), polymer zipper would provide a versatile protocol for engineering nanomedicines with high selectivity and efficiency for clinical cancer treatment.
Co-reporter:Rong-Bin Song;YiChao Wu;Dr. Zong-Qiong Lin;Jian Xie;Chuan Hao Tan; Joachim Say Chye Loo; Bin Cao; Jian-Rong Zhang; Jun-Jie Zhu; Qichun Zhang
Angewandte Chemie 2017 Volume 129(Issue 35) pp:10744-10744
Publication Date(Web):2017/08/21
DOI:10.1002/ange.201706568
Die Beschichtung einzelner Bakterienzellen …… mit in situ gebildetem Polypyrrol wird von J. S. C. Loo, B. Cao, J. R. Zhang, J. J. Zhu et al. in ihrer Zuschrift auf S. 10652 beschrieben. Das Polypyrrol kann als leitfähiges Medium sowie als Schutzschicht fungieren. Ein erhöhter direkter kontaktbasierter extrazellulärer Elektronentransfer und eine bessere Lebensfähigkeit der Bakterienzellen werden beobachtet, wenn mit Polypyrrol beschichtete exoelektrogene Bakterien als Anode in mikrobiellen Brennstoffzellen eingesetzt werden.
Co-reporter:Rong-Bin Song;YiChao Wu;Dr. Zong-Qiong Lin;Jian Xie;Chuan Hao Tan; Joachim Say Chye Loo; Bin Cao; Jian-Rong Zhang; Jun-Jie Zhu; Qichun Zhang
Angewandte Chemie 2017 Volume 129(Issue 35) pp:10652-10656
Publication Date(Web):2017/08/21
DOI:10.1002/ange.201704729
AbstractCoating individual bacterial cells with conjugated polymers to endow them with more functionalities is highly desirable. Here, we developed an in situ polymerization method to coat polypyrrole on the surface of individual Shewanella oneidensis MR-1, Escherichia coli, Ochrobacterium anthropic or Streptococcus thermophilus. All of these as-coated cells from different bacterial species displayed enhanced conductivities without affecting viability, suggesting the generality of our coating method. Because of their excellent conductivity, we employed polypyrrole-coated Shewanella oneidensis MR-1 as an anode in microbial fuel cells (MFCs) and found that not only direct contact-based extracellular electron transfer is dramatically enhanced, but also the viability of bacterial cells in MFCs is improved. Our results indicate that coating individual bacteria with conjugated polymers could be a promising strategy to enhance their performance or enrich them with more functionalities.
Co-reporter:Rong-Bin Song;YiChao Wu;Dr. Zong-Qiong Lin;Jian Xie;Chuan Hao Tan; Joachim Say Chye Loo; Bin Cao; Jian-Rong Zhang; Jun-Jie Zhu; Qichun Zhang
Angewandte Chemie International Edition 2017 Volume 56(Issue 35) pp:10608-10608
Publication Date(Web):2017/08/21
DOI:10.1002/anie.201706568
Coating individual bacterial cells with in situ formed polypyrrole is described by J. S. C. Loo, B. Cao, J. R. Zhang, J.-J. Zhu et al. in their Communication on page 10516 ff. The coated polypyrrole can serve as a conductive medium as well as a protecting layer. Enhanced direct contact-based extracellular electron transfer and improved viability of bacterial cells are observed when polypyrrole-coated exoelectrogenic bacteria are employed as an anode in microbial fuel cells.
Co-reporter:Rong-Bin Song;YiChao Wu;Dr. Zong-Qiong Lin;Jian Xie;Chuan Hao Tan; Joachim Say Chye Loo; Bin Cao; Jian-Rong Zhang; Jun-Jie Zhu; Qichun Zhang
Angewandte Chemie International Edition 2017 Volume 56(Issue 35) pp:10516-10520
Publication Date(Web):2017/08/21
DOI:10.1002/anie.201704729
AbstractCoating individual bacterial cells with conjugated polymers to endow them with more functionalities is highly desirable. Here, we developed an in situ polymerization method to coat polypyrrole on the surface of individual Shewanella oneidensis MR-1, Escherichia coli, Ochrobacterium anthropic or Streptococcus thermophilus. All of these as-coated cells from different bacterial species displayed enhanced conductivities without affecting viability, suggesting the generality of our coating method. Because of their excellent conductivity, we employed polypyrrole-coated Shewanella oneidensis MR-1 as an anode in microbial fuel cells (MFCs) and found that not only direct contact-based extracellular electron transfer is dramatically enhanced, but also the viability of bacterial cells in MFCs is improved. Our results indicate that coating individual bacteria with conjugated polymers could be a promising strategy to enhance their performance or enrich them with more functionalities.
Co-reporter:Wenjing Wang;Nitya Sai Reddy Satyavolu;Zhenkun Wu; Dr. Jian-Rong Zhang; Dr. Jun-Jie Zhu; Dr. Yi Lu
Angewandte Chemie International Edition 2017 Volume 56(Issue 24) pp:6798-6802
Publication Date(Web):2017/06/06
DOI:10.1002/anie.201701325
AbstractDNAzymes have enjoyed success as metal ion sensors outside cells. Their susceptibility to metal-dependent cleavage during delivery into cells has limited their intracellular applications. To overcome this limitation, a near-infrared (NIR) photothermal activation method is presented for controlling DNAzyme activity in living cells. The system consists of a three-stranded DNAzyme precursor (TSDP), the hybridization of which prevents the DNAzyme from being active. After conjugating the TSDP onto gold nanoshells and upon NIR illumination, the increased temperature dehybridizes the TSDP to release the active DNAzyme, which then carries out metal-ion-dependent cleavage, resulting in releasing the cleaved product containing a fluorophore. Using this construct, detecting Zn2+ in living HeLa cells is demonstrated. This method has expanded the DNAzyme versatility for detecting metal ions in biological systems under NIR light that exhibits lower phototoxicity and higher tissue penetration ability.
Co-reporter:Feng Lu;Lin Yang;Yujie Ding
Advanced Functional Materials 2016 Volume 26( Issue 26) pp:4778-4785
Publication Date(Web):
DOI:10.1002/adfm.201600464
Photodynamic therapy (PDT) is a noninvasive and site-specific therapeutic technique for the clinical treatment of various of superficial diseases. In order to tuning the operation wavelength and improve the tissue penetration of PDT, rare-earth doped upconversion nanoparticles (UCNPs) with strong anti-stokes emission are introduced in PDT recently. However, the conventional Yb3+-sensitized UCNPs are excited at 980 nm which is overlapped with the absorption of water, thus resulting in strong overheating effect. Herein, a convenient but effective design to obtain highly emissive 795 nm excited Nd3+-sensitized UCNPs (NaYF4:Yb,Er@NaYF4:Yb0.1Nd0.4@NaYF4) is reported, which provides about six times enhanced upconversion luminescence, comparing with traditional UCNPs (NaYF4:Yb,Er@NaYF4). A colloidal stable and non-leaking PDT nanoplatform is fabricated later through a highly PEGylated mesoporous silica layer with covalently linked photosensitizer (Rose Bengal derivative). With as-prepared Nd3+-sensitized UCNPs, the nanoplatform can produce singlet oxygen more effective than traditional UCNPs. Significant higher penetration depth and lower overheating are demonstrated as well. All these features make as-prepared nanocomposites excellent platform for PDT treatment. In addition, the nanoplatform with uniform size, high surface area, and excellent colloidal stability can be extended for other biomedical applications, such as imaging probes, biosensors, and drug delivery vehicles.
Co-reporter:Fei Zhou, Tingting Zheng, E. S. Abdel-Halim, Liping Jiang and Jun-Jie Zhu
Journal of Materials Chemistry A 2016 vol. 4(Issue 17) pp:2887-2894
Publication Date(Web):29 Mar 2016
DOI:10.1039/C6TB00438E
A novel multifunctional nanoplatform was designed based on the combination of silver nanoparticles (AgNPs) with nucleolin-targeted and doxorubicin (Dox)-loaded manganese dioxide (MnO2) nanosheets to induce enhanced cancer cell apoptosis. MnO2 nanosheets fabricated on the surface of AgNPs served as efficient fluorescence quenchers of Dox. After being internalized into cancer cells, the fluorescence of Dox could be turned on gradually by intracellular glutathione (GSH) which reduces MnO2 into Mn2+ to release Dox. The synergetic effects of AgNP-induced apoptosis and subsequent Dox delivery resulted in enhanced cancer cell apoptosis. Annexin V-FITC/PI double staining, mitochondrial membrane potential (MMP) detection and reactive oxygen species (ROS) detection demonstrated the specific enhanced apoptosis of cancer cells. In this way, the novel nanoprobes can be used as promising theranostic agents for specific cancer therapy.
Co-reporter:Jingjing Zhao, Penghui Zhang, Zhimei He, Qian-Hao Min, E. S. Abdel-Halim and Jun-Jie Zhu
Chemical Communications 2016 vol. 52(Issue 33) pp:5722-5725
Publication Date(Web):18 Mar 2016
DOI:10.1039/C6CC01162D
Smart nanocarriers with switchable surfaces consisting of thermo-sensitive polymers and aptamers have been developed, through which the cellular uptake and photothermal therapy in five different cells could be spatial-temporally controlled on command, which is beneficial in maximizing therapy efficacy and minimizing side effects.
Co-reporter:Rong-Bin Song, Cui-E Zhao, Li-Ping Jiang, Essam Sayed Abdel-Halim, Jian-Rong Zhang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 25) pp:16170-16177
Publication Date(Web):June 7, 2016
DOI:10.1021/acsami.6b03425
Promoting the performance of microbial fuel cells (MFCs) relies heavily on the structure design and composition tailoring of electrode materials. In this work, three-dimensional (3D) macroporous graphene foams incorporated with intercalated spacer of multiwalled carbon nanotubes (MWCNTs) and bacterial anchor of Fe3O4 nanospheres (named as G/MWCNTs/Fe3O4 foams) were first synthesized and used as anodes for Shewanella-inoculated microbial fuel cells (MFCs). Thanks to the macroporous structure of 3D graphene foams, the expanded electrode surface by MWCNTs spacing, as well as the high affinity of Fe3O4 nanospheres toward Shewanella oneidensis MR-1, the anode exhibited high bacterial loading capability. In addition to spacing graphene nanosheets for accommodating bacterial cells, MWCNTs paved a smoother way for electron transport in the electrode substrate of MFCs. Meanwhile, the embedded bioaffinity Fe3O4 nanospheres capable of preserving the bacterial metabolic activity provided guarantee for the long-term durability of the MFCs. With these merits, the constructed MFC possessed significantly higher power output and stronger stability than that with conventional graphite rod anode.
Co-reporter:Ying Zhou, Jie Ding, Tingxizi Liang, E. S. Abdel-Halim, Liping Jiang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 10) pp:6423
Publication Date(Web):February 24, 2016
DOI:10.1021/acsami.6b01031
Fluorescent nanosensors have been widely applied in recognition and imaging of bioactive small molecules; however, the complicated surface modification process and background interference limit their applications in practical biological samples. Here, a simple, universal method was developed for ratiometric fluorescent determination of general small molecules. Taking superoxide anion (O2•–) as an example, the designed sensor was composed of three main moieties: probe carrier, rattle-type silica colloidal particles (mSiO2@hmSiO2 NPs); reference fluorophore doped into the core of NPs, fluorescein isothiocyanate (FITC); fluorescent probe for superoxide anion, hydroethidine (HE). In the absence of O2•–, the sensor just emitted green fluorescence of FITC at 518 nm. When released HE was oxidized by O2•–, the oxidation product exhibited red fluorescence at 570 nm and the intensity was linearly associated with the concentration of O2•–, while that of reference element remained constant. Accordingly, ratiometric determination of O2•– was sensitively and selectively achieved with a linear range of 0.2–20 μM, and the detection limit was calculated as low as 80 nM. Besides, the technique was also successfully applied for dual-emission imaging of O2•– in live cells and realized visual recognition with obvious fluorescence color change in normal conditions or under oxidative stress. As long as appropriate reference dyes and sensing probes are selected, ratiometric biosensing and imaging of bioactive small molecules would be achieved. Therefore, the design could provide a simple, accurate, universal platform for biological applications.Keywords: bioactive small molecules; FITC@mSiO2@hmSiO2; hydroethidine; ratiometric fluorescent sensor; superoxide anion
Co-reporter:Yingying Wang, Li-Ping Jiang, Shiwei Zhou, Sai Bi, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 40) pp:26532
Publication Date(Web):September 30, 2016
DOI:10.1021/acsami.6b08597
Due to the predictable conformation and programmable Watson–Crick base-pairing interactions, DNA has proven to be an attractive material to construct various nanostructures. Herein, we demonstrate a simple model of DNA polymerase-directed hairpin assembly (PDHA) to construct DNA nanoassemblies for versatile applications in biomedicine and biosensing. The system consists of only two hairpins, an initiator and a DNA polymerase. Upon addition of aptamer-linked initiator, the inert stems of the two hairpins are activated alternately under the direction of DNA polymerase, which thus grows into aptamer-tethered DNA nanoassemblies (AptNAs). Moreover, through incorporating fluorophores and drug-loading sites into the AptNAs, we have constructed multifunctional DNA nanoassemblies for targeted cancer therapy with high drug payloads and good biocompatibility. Interestingly, using the as-prepared AptNAs as building blocks, DNA nanohydrogels are self-assembled after centrifugation driven by liquid crystallization and dense packaging of DNA duplexes. Taking advantage of easy preparation and high loading capacity, the PDHAs are readily extended to the fabrication of a label-free biosensing platform, achieving amplified electrochemical detection of microRNA-21 (miR-21) with a detection limit as low as 0.75 fM and a dynamic range of 8 orders of magnitude. This biosensor also demonstrates excellent specificity to discriminate the target miR-21 from the control microRNAs and even the one-base mismatched one and further performs well in analyzing miR-21 in MCF-7 tumor cells.Keywords: cancer cell; DNA nanoassembly; drug delivery; microRNA; signal amplification
Co-reporter:Shiwei Zhou, Yingying Wang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 12) pp:7674
Publication Date(Web):March 6, 2016
DOI:10.1021/acsami.6b01010
B-cell lymphoma 2 (Bcl-2) and Bcl-2-associated X protein (Bax) are often used to monitor the apoptosis of tumor cells and evaluate cancer drug effect. In this work, a novel sandwich-type dual-signal-marked electrochemical biosensor was fabricated for simultaneous detection of Bcl-2 and Bax proteins. Reduced graphene oxide (RGO) layers were used as substrate to immobilize Bcl-2 and Bax antibodies for further capturing target antigens. CdSeTe@CdS quantum dots (QDs) and Ag nanoclusters (NCs) with antibody modification and mesoporous silica amplification were used as signal probes, which were proportional to the amount of Bcl-2 and Bax antigens. Mesoporous SiO2 can provide a larger surface area, more effectively charged by ethylene imine polymer or poly(diallyldimethylammonium chloride) to adsorb more probes. The Bcl-2 and Bax proteins were determined indirectly by the detection of oxidation peak currents of Cd and Ag using anodic stripping voltammetry, showing a good linear relationship in the protein concentration range from 1 ng/mL to 250 ng/mL. The detection limit of trace protein level was ∼0.5 fmol. The biosensor was further introduced to investigate Bcl-2 and Bax expressions from nilotinib-treated chronic myeloid leukemia K562 cells. With the increase of drug dosage and incubation time, the up-regulation for Bax and down-regulation for Bcl-2 were observed, which indicated that the apoptosis level of K562 cells could be regulated by Bcl-2 family. The ratio of Bax/Bcl-2 was further calculated for evaluation of its drug effect and apoptosis level. The limited cell amount for detection reached less than 1 × 103 cells, much lower than traditional methods. Furthermore, completely independent detection step and stable acid solutions containing Ag+ and Cd2+ for long-time storage contribute to reducing the error from the sample differences and avoiding the potential errors from the photodegradation of fluorescent probes, enzymolysis of DNA, or inactivation of enzyme during an excess experimental period.Keywords: apoptosis; Bax; Bcl-2; CML; electrochemical immunosensor
Co-reporter:Yong-Ping Dong, Ying Zhou, Jiao Wang, and Jun-Jie Zhu
Analytical Chemistry 2016 Volume 88(Issue 10) pp:5469
Publication Date(Web):April 21, 2016
DOI:10.1021/acs.analchem.6b00921
In the present work, strong anodic electrogenerated chemiluminescence (ECL) of Ru(bpy)32+ was observed at a graphene oxide modified glassy carbon electrode (GO/GCE) in the absence of coreactants. The electrocatalytical effect of GO on the oxidation of Ru(bpy)32+ suggested that GO itself can act as the coreactant of Ru(bpy)32+ ECL, which can be used to fabricate the ECL biosensor. Thiol group terminated adenosine triphosphate (ATP) aptamer was immobilized on the GO film via DNA hybridization. When gold nanoparticles/graphene oxide (AuNPs/GO) nanocomposites were modified on the aptamer through the S–Au bond to form a sandwich-like structure, the ECL resonance energy transfer (ECL-RET) could occur between Ru(bpy)32+ and AuNPs/GO nanocomposites, resulting in an apparent decrease of ECL signal. After the ECL sensor was incubated in ATP solution, the AuNPs/GO nanocomposites were released from the electrode due to the specific interaction between aptamer and ATP, leading to the increased ECL signal. On the basis of these results, an ECL aptasensor was fabricated and could be used in the sensitive and selective detection of ATP in the range of 0.02–200 pM with a detection limit of 6.7 fM (S/N = 3). The proposed ECL aptasensor can be applied in the detection of ATP in real samples with satisfactory results.
Co-reporter:Yong-Ping Dong, Gang Chen, Ying Zhou, and Jun-Jie Zhu
Analytical Chemistry 2016 Volume 88(Issue 3) pp:1922
Publication Date(Web):January 5, 2016
DOI:10.1021/acs.analchem.5b04379
Caspase-3 is one of the most frequently activated cysteine proteases during the apoptosis process and has been identified as a well-established cellular marker of apoptosis. In this study, a novel approach for the sensitive determination of caspase-3 activity was proposed using electrochemiluminescence (ECL) of Ru(bpy)32+-doped silica (Ru@SiO2) with tripropylamine (TPA) as coreactant. A nanocomposite containing gold nanoparticles (AuNPs), poly(dimethyldiallyl ammonium chloride) (PDDA), and multiwalled carbon nanotubes (CNTs) was fabricated as an ECL platform. The biotinylated DEVD-peptide (biotin-Gly-Asp-Gly-Asp-Glu-Val-Asp-Gly-Cys) was immobilized on the nanocomposite surface via the strong bonding interaction between AuNPs and the thiol group. Then the streptavidin-modified Ru(bpy)32+-doped silica (Ru@SiO2-SA) was immobilized on the ECL platform via the specific interaction between biotin and streptavidin to generate ECL signal. Caspase-3 can specifically recognize and cleave the N-terminus of DEVD, leading to the loss of the biotin label and the decrease of ECL intensity to determine the activity of caspase-3. The results revealed a new ECL avenue for the sensitive and specific monitor of caspase-3, and the platform could be utilized to evaluate anticancer drugs.
Co-reporter:Gao-Chao Fan, Hua Zhu, Dan Du, Jian-Rong Zhang, Jun-Jie Zhu, and Yuehe Lin
Analytical Chemistry 2016 Volume 88(Issue 6) pp:3392
Publication Date(Web):February 24, 2016
DOI:10.1021/acs.analchem.6b00144
A new, ultrasensitive photoelectrochemical immunosensing platform was established on the basis of CdSeTe@CdS:Mn core–shell quantum dots-sensitized TiO2 coupled with signal amplification of CuS nanocrystals conjugated signal antibodies. In this proposal, carcinoembryonic antigen (CEA, Ag) was selected as an example of target analyte to show the analytical performances of the platform. Specifically, TiO2-modified electrode was first assembled with CdSeTe alloyed quantum dots (AQDs) via electrostatic adsorption assisted by oppositely charged polyelectrolyte, and then further deposited with CdS:Mn shells on the surface of CdSeTe AQDs via successive ionic layer adsorption and reaction strategy, forming TiO2/CdSeTe@CdS:Mn sensitization structure, which was used as photoelectrochemical matrix to immobilize capture CEA antibodies (Ab1); signal CEA antibodies (Ab2) were labeled with CuS nanocrystals (NCs) to form Ab2–CuS conjugates, which were employed as signal amplification elements when specific immunoreaction occurred. The ultrahigh sensitivity of this immunoassay resulted from the following two aspects. Before detection of target Ag, the TiO2/CdSeTe@CdS:Mn sensitization structure could adequately harvest the exciting light with different bands, evidently expedite the electron transfer, and effectively depress the charge recombination, resulting in noticeably increased photocurrent. When target Ag existed, the Ab2–CuS conjugates could dramatically decrease the photocurrent due to competitive absorption of exciting light and consumption of electron donor for CuS NCs coupled with steric hindrance of Ab2 molecules. The fabricated photoelectrochemical immunosensor showed a low limit of detection of 0.16 pg/mL and a wide linear range from 0.5 pg/mL to 100 ng/mL for CEA detection, and it also exhibited good specificity, reproducibility, and stability.
Co-reporter:Gao-Chao Fan, Xiao-Mei Shi, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2016 Volume 88(Issue 21) pp:10352
Publication Date(Web):October 17, 2016
DOI:10.1021/acs.analchem.6b03473
Generally, photoanode-based photoelectrochemical immunoassay possesses obvious photocurrent response and lower detection limit for ideal sample detection, but it has the inherent imperfection of poor anti-interference capability for real sample detection. Photocathode-based immunoassay can well avoid the intrinsic drawback of photoanode-based immunoassay, but it has low photocurrent response resulting in less good sensitivity. Herein, a promising new cathode photoelectrochemical immunosensing platform integrating photocathode with photoanode was reported for accurate and sensitive detection of biomarkers. In this proposal, prostate-specific antigen (PSA, Ag) was chosen as a model of target analyte to exhibit the analytical performances of this platform. TiO2/CdS:Mn hybrid structure modified indium–tin oxide (ITO) electrode served as photoanode, whereas CuInS2 microflowers modified ITO electrode was selected as photocathode. The transducer elements of PSA antibody (Ab) were modified on photocathode to fabricate a label-free cathode immunosensing electrode. The proposed immunosensing platform possesses two distinct advantages simultaneously. First, it has good anti-interference capability for the detection of real biological samples, since the biorecognition events occurred on photocathode. Second, the photoelectrochemical system owns evident photocurrent response and low detection limit for target Ag detection thanks to the introduction of the photoanode. Moreover, the proposed immunosensing platform also exhibits good specificity, reproducibility, and stability, and meanwhile it opens up a new horizon to construct other kinds of photoelectrochemical biosensors.
Co-reporter:Guohai Yang, Yazhou Zhou, Horng-Bin Pan, Chengzhou Zhu, Shaofang Fu, Chien M. Wai, Dan Du, Jun-Jie Zhu, Yuehe Lin
Ultrasonics Sonochemistry 2016 Volume 28() pp:192-198
Publication Date(Web):January 2016
DOI:10.1016/j.ultsonch.2015.07.021
•A facile ultrasonic-assisted method was developed for fabrication of Pd–Pt/CNTs.•Pd–Pt/CNTs exhibited high activities for electro-oxidation of ethanol and methanol.•The possible reason for the electrocatalytic activity of Pd–Pt/CNTs was proposed.Herein, a facile ultrasonic-assisted strategy was proposed to fabricate the Pd–Pt alloy/multi-walled carbon nanotubes (Pd–Pt/CNTs) nanocomposites. A good number of Pd–Pt alloy nanoparticles with an average of 3.4 ± 0.5 nm were supported on sidewalls of CNTs with uniform distribution. The composition of the Pd–Pt/CNTs nanocomposites could also be easily controlled, which provided a possible approach for the preparation of other architectures with anticipated properties. The Pd–Pt/CNTs nanocomposites were extensively studied by electron microscopy, induced coupled plasma atomic emission spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy, and applied for the ethanol and methanol electro-oxidation reaction in alkaline medium. The electrochemical results indicated that the nanocomposites had better electrocatalytic activities and stabilities, showing promising applications for fuel cells.
Co-reporter:Shanhu Liu, Ziyi Zhang, Shiwei Zhou, Li-Ping Jiang and Jun-Jie Zhu
Analyst 2016 vol. 141(Issue 2) pp:567-569
Publication Date(Web):19 Oct 2015
DOI:10.1039/C5AN01780G
An electrochemical-TUNEL method was developed for a cell sensor. A 3-D bio-interface based on CNT@PDA–FA was employed in the cytosensor, which significantly improved the cell capture. By coupling with a QD-based nanoprobe and electrochemical stripping analysis, the cytosensor exhibited attractive performance for detection of apoptotic cells.
Co-reporter:Yong-Ping Dong, Jiao Wang, Ying Peng, Jun-Jie Zhu
Journal of Electroanalytical Chemistry 2016 Volume 781() pp:109-113
Publication Date(Web):15 November 2016
DOI:10.1016/j.jelechem.2016.05.024
•CdS quantum dots/graphene (CdS/GR) nanocomposites were prepared.•Strong luminol ECL was obtained at the CdS/GR modified electrode.•ECL resonance energy transfer could occur between luminol and CdS/GR.•Cytochrome C could be sensitively detected using ECL method.Electrogenerated chemiluminescence (ECL) behaviors of luminol were comparatively studied at CdS quantum dos, graphene, and CdS/graphene (CdS/GR) nanocomposites modified gold electrodes in neutral condition. The most intense anodic ECL signal was obtained at the CdS/GR nanocomposites modified gold electrode (CdS/GR/GE). The anodic ECL of luminol (ECL-1) located at ~ 0.50 V (vs SCE) was increased nearly 50-times compared with the bare gold electrode. Besides, two stronger anodic ECL peaks (ECL-2 and ECL-3) were observed at 1.0 V and 1.4 V (vs SCE), respectively. The fluorescence and the UV–vis absorption spectra revealed that resonance energy transfer between luminol and CdS/GR nanocomposites was possible. The ECL spectra further demonstrated the occurrence of ECL resonance energy transfer (ECL-RET), which resulted in strong ECL-2 and ECL-3. Cytochrome C could significantly inhibit the intensities of the anodic ECL peaks, and could be sensitively detected.Electrogenerated chemiluminescence resonance energy transfer can occur between luminol and CdS/graphene nanocomposite. Strong anodic ECL peaks can be obtained in neutral condition. Cytochrome C can inhibit the anodic ECL signals and can be sensitively detected.
Co-reporter:Yong-Ping Dong, Ying Zhou, Jiao Wang, Jun-Jie Zhu
Sensors and Actuators B: Chemical 2016 Volume 226() pp:444-449
Publication Date(Web):April 2016
DOI:10.1016/j.snb.2015.09.020
•ECL resonance energy transfer can occur between lucigenin and CdSe QDs.•The strong anodic ECL can be obtained in the presence of bromide.•Cytochrome C can be sensitively detected.Electrogenerated chemiluminescence (ECL) of lucignein often suffered from weak signal at positive potential in neutral condition. In the present study, strong anodic ECL was obtained in neutral lucigenin solution at a CdSe quantum dots modified glassy carbon electrode. Electrochemical results suggested that CdSe quantum dots can catalyze the oxidation of lucigenin and bromide, which can generate the anodic ECL. The fluorescence and the ECL spectra revealed that ECL resonance energy transfer (ECL-RET) can occur between lucigenin and CdSe quantum dots. The oxidation product of bromide can promote ECL-RET and increase the anodic ECL signal significantly. The mechanisms of the anodic ECL based on the ECL-RET were proposed. Cytochrome C exhibited apparent inhibiting effect on the anodic ECL emission, based on which a sensitive ECL sensor for the detection of cytochrome C was established.
Co-reporter:Pan-Pan Gai, Yu-Sheng Ji, Wen-Jing Wang, Rong-Bin Song, Cheng Zhu, Yun Chen, Jian-Rong Zhang, Jun-Jie Zhu
Nano Energy 2016 Volume 19() pp:541-549
Publication Date(Web):January 2016
DOI:10.1016/j.nanoen.2015.03.035
•An ultrasensitive self-powered cytosensor based on biofuel cells was fabricated.•The captured cells could cause the decrease in power output of cytosensor.•The power output of the self-powered cytosensor could be restored.•The detection limit of the self-powered BFC cytosensor was 4 cells (S/N=3).We developed an ultrasensitive self-powered cytosensor based on biofuel cells (BFC) for the detection of acute leukemia CCRF-CEM cells. The core component of the BFC cytosensor was composed of an aptamer (Sgc8c)-functionalized cathode and a nitrogen-doped graphene/gold nanoparticles/glucose oxidase (NG/AuNPs/GOD) anode, which generated a maximum power output density (Pmax) of 115 μW cm−2. Once the negatively charged CCRF-CEM cells were captured by the cathode via aptamer recognition, their dramatic steric hindrance and electrostatic repulsion to the redox probe [Fe(CN)6]3− efficiently blocked the electron transfer between the probe and the cathode surface, and thereby caused a remarkable decrease in power output of the BFC, which could be used to sensitively detect the cells. Notably, the power output density of the BFC cytosensor could be restored when the captured CCRF-CEM cells were released from the aptamer-functionalized cathode by raising the temperature of the cathode to alter the specific conformation of the aptamer. Then the re-activated cathode could capture CCRF-CEM cells once again achieving the regeneration of the BFC cytosensor. This self-powered BFC cytosensor showed a linear relationship between the Pmax and the logarithm of the cell numbers over a range of 5–50,000 cells (r=0.9979) with a detection limit of 4 cells (S/N=3), which is expected to have potential application as a powerful point-of-care tool for the early detection of circulating tumor cells.We developed an ultrasensitive self-powered cytosensor based on biofuel cells for the detection of acute leukemia CCRF-CEM cells. By virtue of the high specific aptamer and sensitive power output signal, the detection limit of the BFC cytosensor was determined to be 4 cells.
Co-reporter:Gao-Chao Fan
The Journal of Physical Chemistry C 2016 Volume 120(Issue 29) pp:15657-15665
Publication Date(Web):October 15, 2015
DOI:10.1021/acs.jpcc.5b08131
A novel photoelectrochemical aptasensor for adenosine triphosphate (ATP) detection was developed by introducing inorganic–organic photoactive nanocomposites as sensitization agents to achieve significant signal amplification. Specifically, a TiO2/Au hybrid structure was first fabricated by decorating Au nanoparticles on the surface of TiO2 film, which then was used as the photoelectrochemical matrix for the immobilization of ATP aptamer probes; amino-functionalized CdS:Mn (CdS:Mn-NH2) nanocrystals covalently bound with Ru(bpy)2(dcbpy)2+ (bpy = 2,2′-bipyridine; dcbpy = 2,2′-bipyridine-4,4′-dicarboxylic acid) to form CdS:Mn@Ru(bpy)2(dcbpy) photoactive nanocomposites, which were employed as signal amplification element labeling on the terminal of ATP aptamer probes. The ATP detection was performed via the photocurrent variation produced by the conformation change of ATP aptamer probes after specifically binding with ATP molecules. Before incubation with ATP, the ATP aptamer probe hybridized with its partly complementary DNA to form a rodlike double helix, which made the labeled sensitization agents of CdS:Mn@Ru(bpy)2(dcbpy) far from the TiO2/Au electrode surface, resulting in depressed sensitization effect. In the presence of ATP, the ATP aptamer probe specifically bound with ATP molecule to form a G-quadruplex structure, which made the CdS:Mn@Ru(bpy)2(dcbpy) very close to the TiO2/Au electrode surface, resulting in noticeably enhanced photocurrent intensity due to full activation of the sensitization effect. Accordingly, a signal-on photoelectrochemical aptasensor was constructed. The designed aptasensor exhibited a wide linear range from 0.5 pM to 5 nM with a low detection limit of 0.18 pM for ATP detection.
Co-reporter:Penghui Zhang, Chen Wang, Jingjing Zhao, Anqi Xiao, Qi Shen, Linting Li, Jianxin Li, Junfeng Zhang, Qianhao Min, Jiangning Chen, Hong-Yuan Chen, and Jun-Jie Zhu
ACS Nano 2016 Volume 10(Issue 3) pp:3637
Publication Date(Web):February 23, 2016
DOI:10.1021/acsnano.5b08145
In chemotherapy, it is a great challenge to recruit endogenous stimuli instead of external intervention for targeted delivery and controlled release; microRNAs are the most promising candidates due to their vital role during tumorigenesis and significant expression difference. Herein, to amplify the low abundant microRNAs in live cells, we designed a stimuli-responsive DNA Y-motif for codelivery of siRNA and Dox, in which the cargo release was achieved via enzyme-free cascade amplification with endogenous microRNA as trigger and ATP (or H+) as fuel through toehold-mediated strand displacement. Furthermore, to realize controlled release in tumor cells, smart nanocarriers were constructed with stimuli-responsive Y-motifs, gold nanorods, and temperature-sensitive polymers, whose surfaces could be reversibly switched between PEG and RGD states via photothermal conversion. The PEG corona kept the nanocarriers stealth during blood circulation to protect the Y-motifs against nuclease digestion and enhance passive accumulation, whereas the exposed RGD shell under near-infrared (NIR) irradiation at tumor sites facilitated the specific receptor-mediated endocytosis by tumor cells. Through modulating NIR laser, microRNA, or ATP expressions, the therapy efficacies to five different cell lines were finely controlled, presenting NIR-guided accumulation, massive release, efficient gene silence, and severe apoptosis in HeLa cells; in vivo study showed that a low dosage of nanocarriers synergistically inhibited the tumor growth by silencing gene expression and inducing cell apoptosis under mild NIR irradiation, though they only brought minimum damage to normal organs. The combination of nanomaterials, polymers, and DNA nanomachines provided a promising tool for designing smart nanodevices for disease therapy.Keywords: aptamer; DNA nanomachine; drug delivery; microRNA; smart nanocarriers
Co-reporter:Yongbing Lou, Yixin Zhao and Jun-Jie Zhu
Nanoscale Horizons 2016 vol. 1(Issue 2) pp:125-134
Publication Date(Web):12 Oct 2015
DOI:10.1039/C5NH00039D
Quantum dots (QDs) have received great interest for diverse applications over the past few decades due to their unique photophysical properties like their tunable band gap, facile solution processability and versatile surface functionalization with different ligands. Quantum dot based optical analysis techniques with high sensitivity and selectivity have been developed to detect anions in aqueous solution for environmental monitoring, medicinal diagnostics, and the analysis of biological samples and industrial processes. Here we review the latest research progress of semiconductor QDs for sensing of anions in aqueous solution or in vivo, and discuss the photophysical mechanisms and outlook for the potential development in QD based optical sensing for anions.
Co-reporter:Hua Zhu, Gao-Chao Fan, E.S. Abdel-Halim, Jian-Rong Zhang, Jun-Jie Zhu
Biosensors and Bioelectronics 2016 Volume 77() pp:339-346
Publication Date(Web):15 March 2016
DOI:10.1016/j.bios.2015.09.051
•A novel, enhanced photoelectrochemical immunoassay was developed for CA19-9 detection.•TiO2NWs/Au/CdSe@ZnS sensitized structure could evidently promote photocurrent intensity.•Ab2@V2+ conjugates could significantly decrease the photocurrent detection signal.•The proposed photoelectrochemical protocol presented ultrahigh sensitivity.A novel, enhanced photoelectrochemical immunoassay was established for sensitive and specific detection of carbohydrate antigen 19-9 (CA19-9, Ag). In this protocol, TiO2 nanowires (TiO2NWs) were first decorated with Au nanoparticles to form TiO2NWs/Au hybrid structure, and then coated with CdSe@ZnS quantum dots (QDs) via the layer-by-layer method, producing TiO2NWs/Au/CdSe@ZnS sensitized structure, which was employed as the photoelectrochemical matrix to immobilize capture CA19-9 antibodies (Ab1); whereas, bipyridinium (V2+) molecules were labeled on signal CA19-9 antibodies (Ab2) to form Ab2@V2+ conjugates, which were used as signal amplification elements. The TiO2NWs/Au/CdSe@ZnS sensitized structure could adequately absorb light energy and dramatically depress electron–hole recombination, resulting in evidently enhanced photocurrent intensity of the immunosensing electrode. While target Ag were detected, the Ab2@V2+ conjugates could significantly decrease the photocurrent detection signal because of strong electron-withdrawing property of V2+ coupled with evident steric hindrance of Ab2. Thanks to synergy effect of TiO2NWs/Au/CdSe@ZnS sensitized structure and quenching effect of Ab2@V2+ conjugates, the well-established photoelectrochemical immunoassay exhibited a low detection limit of 0.0039 U/mL with a wide linear range from 0.01 U/mL to 200 U/mL for target Ag detection. This proposed photoelectrochemical protocol also showed good reproducibility, specificity and stability, and might be applied to detect other important biomarkers.
Co-reporter:Li He, Lingling Li, Wenjing Wang, E.S. Abdel-Halim, Jianrong Zhang, Jun-Jie Zhu
Talanta 2016 Volume 146() pp:209-215
Publication Date(Web):1 January 2016
DOI:10.1016/j.talanta.2015.08.053
•High performance NIR CdSeTe/CdS/C QDs were synthesized for the first time.•Core–shell CdSeTe/CdS/C QDs showed low cytotoxicity and good biocompatibility.•Labeled CdSeTe/CdS/C QDs could target cancer cell efficiency and specificity.In this study, double shelled NIR CdSeTe/CdS/C quantum dots (QDs) were synthesized by a liquid phase method. The as-prepared QDs showed low cytotoxicity and good biocompatibility due to the formation of carbon shell. The imaging of targeted Human cervical carcinoma cells (HeLa cells) indicates that the CdSeTe/CdS/C QDs have excellent optical properties and cell viability. These results clearly shows that the CdSeTe/CdS/C QDs can be a good candidate for bioapplications.For the sake of minimizing the breakdown of the QDs by oxidation and reducing cytotoxicity, we capped CdSeTe QDs with binary CdS and carbon shells. The double shelled QDs exhibited outstanding optical properties and good biocompatibility, showing potential in bioimaging.
Co-reporter:Jingjing Li, Fangfang Cheng, Haiping Huang, Lingling Li and Jun-Jie Zhu
Chemical Society Reviews 2015 vol. 44(Issue 21) pp:7855-7880
Publication Date(Web):27 Jul 2015
DOI:10.1039/C4CS00476K
Activatable imaging probes as alternatives to “always on” imaging probes have attracted more and more attention due to their improved sensitivity and specificity. They are commonly designed to amplify or boost imaging signals only in response to specific biomolecular recognition or interaction. Thus, the design strategies play a vital role in the fabrication of activatable imaging probes. In this review, we focus on the design mechanisms and biological applications of those nanomaterial-based activatable imaging probes reported in the past five years, benefitting greatly from the good development of nanotechnology. These probes not only include the most studied activatable fluorescence imaging probes, but also cover more activatable MR imaging probes based on nanoparticle contrast agents and activatable photoacoustic imaging probes, providing more bases for clinical translation.
Co-reporter:Zixuan Chen; Jingjing Li; Xueqin Chen; Juntao Cao; Jianrong Zhang; Qianhao Min
Journal of the American Chemical Society 2015 Volume 137(Issue 5) pp:1903-1908
Publication Date(Web):January 21, 2015
DOI:10.1021/ja5112628
This article describes a multimodified core–shell gold@silver nanoprobe for real-time monitoring the entire autophagy process at single-cell level. Autophagy is vital for understanding the mechanisms of human pathologies, developing novel drugs, and exploring approaches for autophagy controlling. A major challenge for autophagy study lies in real-time monitoring. One solution might come from real-time detection of in situ superoxide radicals (O2•–), because it is the main regulator of autophagy. In this work, our proposed nanoprobes were etched by O2•– and gave a notable wavelength change in the plasmon resonance scattering spectra. Both the experimental and simulated results suggested the wavelength change rate correlated well with O2•– level. This response enabled its application in real-time in situ quantification of O2•– during autophagy course. More importantly, with the introduction of “relay probe” operation, two types of O2•–-regulating autophagy processes were successfully traced from the beginning to the end, and the possible mechanism was also proposed.
Co-reporter:Hao Zhu, Yujie Ding, Anqi Wang, Xu Sun, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 vol. 3(Issue 3) pp:458-464
Publication Date(Web):15 Oct 2014
DOI:10.1039/C4TB01320D
A novel aptasensor was fabricated for the detection of lysozyme and DNA based on the fluorescence resonance energy transfer (FRET) technique between upconversion nanoparticles (UCNPs) and a dye labeled aptamer. UCNPs can act as excellent emitters due to their low autofluorescence and high penetration depth of biosamples. NaYF4:Yb, Er nanoparticles as UCNPs were synthesized and attached with a dye labeled aptamer through a cationic polymer as an electrostatic linker to quench the upconversion fluorescence intensity. The intensity can be restored after the addition of lysozyme or the complementary DNA (target DNA) because of their strong interaction with the aptamer. The sensor provided a linear concentration range from 30 to 210 nM for lysozyme and 40 to 200 nM for the target DNA, the limit of detection was 2.5 nM and 2.8 nM, respectively. The sensor was also used to monitor the lysozyme level in both human saliva and serum samples, and the results were consistent with the reported values. The method was simple and convenient without the extra procedure of bioconjugation, and could be put to use for the determination of various targets in the future.
Co-reporter:Wei-Wei Xiong, Jin-Qiang Chen, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 vol. 3(Issue 9) pp:1929-1934
Publication Date(Web):17 Dec 2014
DOI:10.1039/C4TC02492C
Zinc triselenide (ZrSe3) and hafnium triselenide (HfSe3) nanobelts were synthesized using a chemical vapor transport method. Photodetectors based on individual nanobelts of ZrSe3 and HfSe3 were fabricated on SiO2/Si substrates, respectively, and the optoelectronic properties of both were evaluated. The ZrSe3 nanobelt photodetector showed a good photoresponse to wavelengths ranging from 405 nm to 780 nm. Under illumination with 650 nm light, the ratio of photoswitch currents reached 1.97 with a light on/off period of 50 s at a bias voltage of 5 V. The HfSe3 nanobelt photodetector also showed good photoresponse to wavelengths ranging from 405 nm to 650 nm, and the ratio of photoswitch currents, under illumination with 532 nm light, reached 2.2 with a light on/off period of 50 s at a bias voltage of 5 V. The photoresponse time of both the photodetectors was less than 0.4 s. The results demonstrated that ZrSe3 and HfSe3 nanobelts possessed excellent photoconductivity, and suggested that these photodetectors would have potential applications under a range of visible light conditions.
Co-reporter:Yun Chen, Panpan Gai, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 vol. 3(Issue 21) pp:11511-11516
Publication Date(Web):20 Apr 2015
DOI:10.1039/C5TA01432H
Enzymatic biofuel cells (EBFCs) utilize redox enzymes as the catalysts to produce energy from green and renewable fuels, and are considered as promising, environmentally friendly power sources. However, EBFCs are limited by the relatively slow rate of electron transfer between enzymes and electrodes, which is a major barrier to improving EBFC power output. In this study, enzymes were bound to the hydrophilic, carboxyl group functionalized graphene–gold nanoparticle hybrid, and the hybrid as electrode material was able to increase the rate of electron transfer in the EBFC. The open-circuit voltage (Eocvcell) of this designed EBFC reached 1.16 ± 0.02 V, and the maximal power density (Pmax) was as high as 1.96 ± 0.13 mW cm−2. Two as-prepared EBFC units arranged in series were able to light up red and yellow light-emitting diodes (LEDs). Also, using these EBFCs, the Eocvcell and Pmax retained 80% and 66% of their optimal values over 70 days, respectively. This fabricated EBFC is expected to find applications in the bioenergy fields.
Co-reporter:Panpan Gai, Rongbin Song, Cheng Zhu, Yusheng Ji, Wengjing Wang, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 vol. 51(Issue 94) pp:16763-16766
Publication Date(Web):25 Sep 2015
DOI:10.1039/C5CC07520C
An exogenous redox-free, membrane-less enzyme biofuel cell-based ultrasensitive self-powered cytosensing platform was fabricated. With the ultrahigh sensitivity and the merits of not requiring external power sources or exogenous reagents, the device has great potential as a point-of-care tool for early diagnosis of cancer in vivo.
Co-reporter:Panpan Gai, Rongbin Song, Cheng Zhu, Yusheng Ji, Yun Chen, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 vol. 51(Issue 79) pp:14735-14738
Publication Date(Web):06 Aug 2015
DOI:10.1039/C5CC06062A
A novel ternary hybrid of carbon nanotubes/graphitic carbon nitride nanosheets/gold nanoparticles was prepared and used as robust substrate electrodes for fabricating membrane-less glucose/O2 enzyme biofuel cells (EBFCs), and a remarkably improved power output was observed for the prepared EBFC.
Co-reporter:Feng Lu, Jinfeng Wang, Lin Yang and Jun-Jie Zhu
Chemical Communications 2015 vol. 51(Issue 46) pp:9447-9450
Publication Date(Web):30 Apr 2015
DOI:10.1039/C5CC01725D
A facile one-pot approach was developed for the synthesis of colloidal stable, monodisperse, highly PEGylated mesoporous silica coated copper sulfide nanocomposites for the combination of photothermal therapy and chemotherapy. The proposed method can also be extended to the synthesis of other metal sulfide nanocomposites.
Co-reporter:Gao-Chao Fan, Hua Zhu, Qingming Shen, Li Han, Ming Zhao, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 vol. 51(Issue 32) pp:7023-7026
Publication Date(Web):16 Mar 2015
DOI:10.1039/C5CC01935D
High-efficient exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites was applied to develop an enhanced photoelectrochemical aptasensing platform with ultrahigh sensitivity, good selectivity, reproducibility and stability.
Co-reporter:Hui Xia, Lingling Li, Zhouyang Yin, Xiandeng Hou, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 1) pp:696
Publication Date(Web):December 5, 2014
DOI:10.1021/am506980d
A dual signal amplification strategy for electrochemiluminescence (ECL) aptasensor was designed based on biobar-coded gold nanoparticles (Au NPs) and DNAzyme. CdSeTe@ZnS quantum dots (QDs) were chosen as the ECL signal probes. To verify the proposed ultrasensitive ECL aptasensor for biomolecules, we detected thrombin (Tb) as a proof-of-principle analyte. The hairpin DNA designed for the recognition of protein consists of two parts: the sequences of catalytical 8–17 DNAzyme and thrombin aptamer. Only in the presence of thrombin could the hairpin DNA be opened, followed by a recycling cleavage of excess substrates by catalytic core of the DNAzyme to induce the first-step amplification. One part of the fragments was captured to open the capture DNA modified on the Au electrode, which further connected with the prepared biobar-coded Au NPs-CdSeTe@ZnS QDs to get the final dual-amplified ECL signal. The limit of detection for Tb was 0.28 fM with excellent selectivity, and this proposed method possessed good performance in real sample analysis. This design introduces the new concept of dual-signal amplification by a biobar-coded system and DNAzyme recycling into ECL determination, and it is promising to be extended to provide a highly sensitive platform for various target biomolecules.Keywords: 8−17 DNAzyme; biobar-coded Au NPs; CdSeTe@ZnS QDs; dual signal amplification; electrochemiluminescence; protein
Co-reporter:Jie Ding, Jing Yao, Jingjing Xue, Rong Li, Bo Bao, Liping Jiang, Jun-jie Zhu, and Zhiwei He
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 32) pp:18145
Publication Date(Web):July 30, 2015
DOI:10.1021/acsami.5b05618
Chemotherapy is the use of chemical drugs to prevent cancer cell proliferation, invasion, and metastasis, but a serious obstacle is that chemotherapeutics strikes not only on cancerous cells, but also on normal cells. Thus, anticancer drugs without side effects should be developed and extracted. (-)-Epigallocatechin-3-gallate (EGCG), a major ingredient of green tea, possesses excellent medicinal values, such as anticancer effects, DNA-protective effects, etc. However, EGCG will be mostly metabolized if it is directly orally ingested. Here, we report a drug delivery system (DDS) for loading EGCG to enhance its stability, promising target and anticancer effects in vitro and in vivo. The designed DDS is composed of three main moieties: anticancer drug, EGCG; drug vector, colloidal mesoporous silica (CMS); target ligand, breast tumor-homing cell-penetrating peptide (PEGA-pVEC peptide). Based on the results of CCK-8 assay, confocal imaging, cell cycle analysis, and Western blot, the anticancer effect of EGCG was increased by loading of EGCG into CMS and CMS@peptide. In vivo treatment displayed that CMS had a not obvious influence on breast tumor bearing mice, but CMS@peptide@EGCG showed the greatest tumor inhibition rate, with about 89.66%. H&E staining of organs showed no tissue injury in all experimental groups. All the above results prove that EGCG is an excellent anticancer drug without side effects and CMS@peptide could greatly promote the efficacy of EGCG on breast tumors by targeted accumulation and release, which provide much evidence for the CMS@peptide as a promising and targeting vector for DDS.Keywords: (-)-epigallocatechin-3-gallate; colloidal mesoporous silica; drug delivery system; PEGA-pVEC peptide; targeted therapy;
Co-reporter:Jingjing Xue, Xinyi Chen, Shanglin Liu, Fenfen Zheng, Li He, Lingling Li, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 34) pp:19126
Publication Date(Web):August 13, 2015
DOI:10.1021/acsami.5b04766
The polyaniline (PAN)-coated CdSeTe quantum dots (QDs) were prepared by in situ polymerization of aniline on the surface of CdSeTe QDs. The PAN-coated CdSeTe QDs has a tremendously enhanced fluorescence (∼40 times) and improved biocompatibility compared to the uncoated CdSeTe QDs. The fluorescence intensity of the PAN-coated CdSeTe QDs can be adjusted by controlling the construction parameters of the PAN shell. The kinetics of the in situ controllable polymerization process was studied by varying the temperature, and the apparent activation energy of polymerization was estimated. With the same method, a series of the PAN derivatives were also tested to coat the CdSeTe QDs in this study. All the QDs showed a significant enhancement of the fluorescence intensity and better biocompatibility. The significantly enhanced fluorescence can provide highly amplified signal for luminescence-based cell imaging.Keywords: cell imaging; enhanced fluorescence; in situ polymerization; polyanilines; quantum dots
Co-reporter:Fang-Fang Cheng, Ting-Ting He, Hai-Tiao Miao, Jian-Jun Shi, Li-Ping Jiang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 4) pp:2979
Publication Date(Web):January 14, 2015
DOI:10.1021/am508690x
MicroRNAs (miRNAs) have emerged as new candidates as diagnostic and prognostic biomarkers for the detection of a wide variety of cancers; thus, sensitive and selective detection of microRNAs is significant for early-phase cancer diagnosis and disease prevention. A novel and simple electrochemical miRNA biosensor was developed using Cd2+-modified titanium phosphate nanoparticles as signal unit, two DNA as capture probes, and Ru(NH3)63+ as electron transfer mediator. Large quantities of cadmium ions were mounted in titanium phosphate spheres to output the electrochemical signal. Because of the presence of Ru(NH3)63+ molecules that interacted with DNA base-pairs as electron wire, the electrochemical signal significantly increased more than 5 times. This approach achieved a wide dynamic linear range from 1.0 aM to 10.0 pM with an ultralow limit detection of 0.76 aM, exerting a substantial enhancement in sensitivity. Moreover, the proposed biosensor was sufficiently selective to discriminate the target miRNAs from homologous miRNAs and could be used for rapid and direct analysis of miRNAs in human serum. Therefore, this strategy provides a new and ultrasensitive platform for miRNA expression profiling in biomedical research and clinical diagnosis.Keywords: electrochemical biosensor; electron transfer; microRNAs; titanium phosphate
Co-reporter:Hongying Liu, Zhimei He, Li-Ping Jiang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 8) pp:4913
Publication Date(Web):February 11, 2015
DOI:10.1021/am508994w
A facile and rapid strategy was developed for the synthesis of ultrabright luminescent carbon nanodots (CDs) with tunable wavelength from 464 to 556 nm by introducing glutaraldehyde into the precursor solution under microwave irradiation. The fluorescence properties, including excitation and emission wavelength, quantum yield, and size of the CDs, were adjusted by changing the amount of glutaraldehyde and poly(ethylenimine). Several methods such as high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and dynamic light scattering, UV–vis, fluorescence, and Fourier transform infrared spectroscopy were employed to study the morphology and the properties of CDs. The luminescence mechanism was also discussed. In addition, confocal microscopy imaging revealed that the as-prepared CDs could be used as effective fluorescent probes in the cell imaging without obvious cytotoxicity. Moreover, a novel sensor for the detection of Co2+ was proposed on the basis of Co2+-induced fluorescence quenching. These superior properties demonstrated the potential application of the CDs in cellular imaging and ion sensing.Keywords: carbon nanodots; Co2+; imaging; microwave; wavelength-tunable
Co-reporter:Qianhao Min, Siyuan Li, Xueqin Chen, E. S. Abdel-Halim, Li-Ping Jiang, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 18) pp:9563
Publication Date(Web):March 25, 2015
DOI:10.1021/acsami.5b01006
Global characterization and in-depth understanding of phosphoproteome based on mass spectrometry (MS) desperately needs a highly efficient affinity probe during sample preparation. In this work, a ternary nanocomposite of magnetite/ceria-codecorated titanoniobate nanosheet (MC-TiNbNS) was synthesized by the electrostatic assembly of Fe3O4 nanospheres and in situ growth of CeO 2 nanoparticles on pre-exfoliated titanoniobate and eventually utilized as the probe and catalyst for the enrichment and dephosphorylation of phosphopeptides. The two-dimensional (2D) structured titanoniobate nanosheet not only promoted the efficacy of capturing phosphopeptides with enlarged surface area, but also functioned as a substrate for embracing the magnetic anchor Fe3O4 to enable magnetic separation and mimic phosphatase CeO2 to produce identifying signatures of phosphopeptides. Compared to single-component TiNbNS or CeO2 nanoparticles, the ternary nanocomposite provided direct evidence of the number of phosphorylation sites while maintaining the enrichment efficiency. Moreover, by altering the on-sheet CeO2 coverage, the dephosphorylation activity could be fine-tuned, generating continuously adjustable signal intensities of both phosphopeptides and their dephosphorylated tags. Exhaustive detection of both mono- and multiphosphorylated peptides with precise counting of their phosphorylation sites was achieved in the primary mass spectra in the cases of digests of standard phosphoprotein and skim milk, as well as a more complex biological sample, human serum. With the resulting highly informative mass spectra, this multifunctional probe can be used as a promising tool for the fast and comprehensive characterization of phosphopeptides in MS-based phosphoproteomics.Keywords: 2D nanosheet; dephosphorylation; enrichment; phosphopeptide; ternary nanocomposite;
Co-reporter:Jun-Tao Cao, Peng-Hui Zhang, Yan-Ming Liu, E. S. Abdel-Halim, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 27) pp:14878
Publication Date(Web):June 18, 2015
DOI:10.1021/acsami.5b03519
This work describes a versatile microfluidic platform for evaluation of cell-surface glycan expression at the single-cell level using quantum dots (QDs) tagged with phenylboronic acid. The platform was integrated with dual microwell arrays, allowing the introduction of cells in two states using the same cell culture chamber. The simultaneous analysis of cells in the same environment minimized errors resulting from different culture conditions. As proof-of-concept, the expressions of sialic acid (SA) groups on K562 cells, with or without 3′-azido-3′-deoxythymidine (AZT) treatment, were evaluated in the same chamber. 3-Aminophenylboronic acid functionalized CdSeTe@ZnS-SiO2 QDs (APBA-QDs) were prepared as probes to recognize SA groups on K562 cells with only one-step labeling. The results showed that the expression of SA moieties on K562 cells was increased by 18% and 31% after treatment with 20 and 40 μM AZT, respectively. Performing the drug treatment and control experiments simultaneously in the same chamber significantly improved the robustness and effectiveness of the assay. The strategy presented here provides an alternative tool for glycan analysis in a sensitive, high-throughput, and effective manner.Keywords: dual microwell array; K562 cells; microfluidic platform; QDs-APBA; sialic acid;
Co-reporter:Qingming Shen, Li Han, Gaochao Fan, Jian-Rong Zhang, Liping Jiang, and Jun-Jie Zhu
Analytical Chemistry 2015 Volume 87(Issue 9) pp:4949
Publication Date(Web):April 14, 2015
DOI:10.1021/acs.analchem.5b00679
A novel “signal-on” photoelectrochemical (PEC) biosensor for sensitive detection of human T-cell lymphotropic virus type II (HTLV-II) DNA was developed on the basis of enzymatic amplification coupled with terminal deoxynucleotidyl transferase (TdT)-mediated extension strategy. The intensity of the photocurrent signal was proportional to the concentration of the HTLV-II DNA-target DNA (tDNA) by dual signal amplification. In this protocol, GR-CdS:Mn/ZnS nanocomposites were used as photoelectric conversion material, while pDNA was used as the tDNA recognizing unit. Moreover, the TdT-mediated extension and the enzymatic signal amplification technique were used to enhance the sensitivity of detection. Using this novel dual signal amplification strategy, the prototype of PEC DNA sensor can detect as low as ∼0.033 fM of HTLV-II DNA with a linear range of 0.1–5000 fM, with excellent differentiation ability even for single-base mismatches. This PEC DNA assay opens a promising platform to detect various DNA targets at ultralow levels for early diagnoses of different diseases.
Co-reporter:Ming Zhao, Gao-Chao Fan, Jing-Jia Chen, Jian-Jun Shi, and Jun-Jie Zhu
Analytical Chemistry 2015 Volume 87(Issue 24) pp:12340
Publication Date(Web):November 24, 2015
DOI:10.1021/acs.analchem.5b03721
A highly sensitive and selective photoelectrochemical (PEC) biosensor for Hg2+ detection was developed on the basis of the synergistic effect of exciton energy transfer (EET) between CdS quantum dots (QDs) and Au nanoparticles (NPs) coupled with sensitization of rhodamine 123 (Rh123) for signal amplification. First, the TiO2/CdS hybrid structure obtained by depositing CdS QDs on TiO2 film was employed as a matrix for immobilizing probe DNA (pDNA). Next, Rh123 was introduced into the pDNA terminal, and then Au NP labeled target DNA (Au-tDNA) was hybridized with pDNA to form a rod-like double helix structure. The detection of Hg2+ was based on a conformational change of the pDNA after incubating with Hg2+. In the absence of Hg2+, Rh123 was located away from the electrode surface due to the DNA hybridization, leading to inhibition of the sensitization effect, and meanwhile, the occurrence of EET between CdS QDs and Au NPs resulted in a photocurrent decrease. However, after incubating with Hg2+, the rod-like double helix was disrupted, and the energy transfer was broken. In this case, the photocurrent recovered, and meanwhile, the folded pDNA made the labeled Rh123 move closer to the electrode surface, leading to the formation of the sensitization structure, which evidently increased the photocurrent intensity. The sensitivity of the biosensor for Hg2+ detection was greatly enhanced for the dual signal amplification strategy. The linear range was 10 fM to 200 nM, with a detection limit of 3.3 fM. This biosensor provides a promising new platform for detecting various heavy metal ions at ultralow levels.
Co-reporter:Jie Ding, Ying Zhou, Jingjing Li, Liping Jiang, Zhiwei He, and Jun-Jie Zhu
Analytical Chemistry 2015 Volume 87(Issue 24) pp:12290
Publication Date(Web):November 24, 2015
DOI:10.1021/acs.analchem.5b03580
The high-performance and noninvasive screening of heterogeneous tumor subtypes in vivo is particularly desirable for the diagnosis and symptomatic treatment of cancer. Therefore, we report a near-infrared (NIR) fluorescence tracer “smartly identified HER2” (SI-HER2) for rapid, accurate, and highly specific screening of HER2 overexpressed breast cancer. An antibody against HER2 protein receptor, EP1045Y, was conjugated with NIR emitting CdSeTe/CdS/ZnS QDs via polyhistidine-driven self-assembly approach. The further adsorption of black hole quencher 3 on antibody enabled a “turn on” fluorescence response of the fluorescence tracer to HER2 protein receptor. Aside from the capability of differentiating the HER2 overexpressed MCF-7 cells from its counterparts, the fluorescence tracer can also accurately and rapidly identify the HER2 overexpressed breast tumor subtype in two tumors-bearing mouse model, providing a platform for the investigation of advanced pathways to distinguish the different breast cancer subtypes.
Co-reporter:Fen-Fen Zheng, Peng-Hui Zhang, Yu Xi, Jing-Jia Chen, Ling-Ling Li, and Jun-Jie Zhu
Analytical Chemistry 2015 Volume 87(Issue 23) pp:11739
Publication Date(Web):November 2, 2015
DOI:10.1021/acs.analchem.5b03131
Great challenges in investigating the release of drug in complex cellular microenvironments necessitate the development of stimuli-responsive drug delivery systems with real-time monitoring capability. In this work, a smart drug nanocarrier based on fluorescence resonance energy transfer (FRET) is fabricated by capping graphene quantum dots (GQDs, the acceptor) onto fluorescent mesoporous silica nanoparticles (FMSNs, the donor) via ATP aptamer for real-time monitoring of ATP-triggered drug release. Under extracellular conditions, the fluorescence of FMSNs remains in the “off” state in the low ATP level which is unable to trigger the release of drug. Once specifically recognized and internalized into the target tumor cells by AS1411 aptamer, in the ATP-rich cytoplasm, the conformation switch of the ATP aptamer causes the shedding of the GQDs from the nanocarriers, leading to the release of the loaded drugs and consequently severe cytotoxicity. Simultaneously, the fluorescence of FMSNs turns “on” along with the dissociation of GQDs, which allows real-time monitoring of the release of drug from the pores. Such a drug delivery system features high specificity of dual-target recognition with AS1411 and ATP aptamer as well as high sensitivity of the FRET-based monitoring strategy. Thus, the proposed multifunctional ATP triggered FRET-nanocarriers will find potential applications for versatile drug-release monitoring, efficient drug transport, and targeted cancer therapeutics.
Co-reporter:Wen-Jing Wang, Jing-Jing Li, Kai Rui, Pan-Pan Gai, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2015 Volume 87(Issue 5) pp:3019
Publication Date(Web):February 11, 2015
DOI:10.1021/ac504652e
We report an electrochemical sensor for telomerase activity detection based on spherical nucleic acids gold nanoparticles (SNAs AuNPs) triggered mimic-hybridization chain reaction (mimic-HCR) enzyme-free dual signal amplification. In the detection strategy, SNAs AuNPs and two hairpin probes were employed. SNAs AuNPs as the primary amplification element, not only hybridized with the telomeric repeats on the electrode to amplify signal but also initiated the subsequent secondary amplification, mimic-hybridization chain reaction of two hairpin probes. If the cells’ extracts were positive for telomerase activity, SNAs AuNPs could be captured on the electrode. The carried initiators could trigger an alternative hybridization reaction of two hairpin probes that yielded nicked double helices. The signal was further amplified enzyme-free by numerous hexaammineruthenium(III) chloride ([Ru(NH3)6]3+, RuHex) inserting into double-helix DNA long chain by electrostatic interaction, each of which could generate an electrochemical signal at appropriate potential. With this method, a detection limit of down to 2 HeLa cells and a dynamic range of 10–10 000 cells were achieved. Telomerase activities of different cell lines were also successfully evaluated.
Co-reporter:Hao Zhu, Feng Lu, Xing-Cai Wu and Jun-Jie Zhu
Analyst 2015 vol. 140(Issue 22) pp:7622-7628
Publication Date(Web):21 Sep 2015
DOI:10.1039/C5AN01634G
A novel fluorescent resonant energy transfer (FRET) biosensor was fabricated for the detection of hepatitis B virus (HBV) DNA using poly(ethylenimine) (PEI) modified upconversion nanoparticles (NH2-UCNPs) as energy donor and gold nanoparticles (Au NPs) as acceptor. The PEI modified upconversion nanoparticles were prepared directly with a simple one-pot hydrothermal method, which provides high quality amino-group functionalized UCNPs with uniform morphology and strong upconversion luminescence. Two single-stranded DNA strands, which were partially complementary to each other, were then conjugated with NH2-UCNPs and Au NPs. When DNA conjugated NH2-UCNPs and Au NPs are mixed together, the hybridization between complementary DNA sequences on UCNPs and Au NPs will lead to the quenching of the upconversion luminescence due to the FRET process. Meanwhile, upon the addition of target DNA, Au NPs will leave the surface of the UCNPs and the upconversion luminescence can be restored because of the formation of the more stable double-stranded DNA on the UCNPs. The sensor we fabricated here for target DNA detection shows good sensitivity and high selectivity, which has the potential for clinical applications in the analysis of HBV and other DNA sequences.
Co-reporter:Panpan Gai, Yusheng Ji, Yun Chen, Cheng Zhu, Jianrong Zhang and Jun-Jie Zhu
Analyst 2015 vol. 140(Issue 6) pp:1822-1826
Publication Date(Web):02 Feb 2015
DOI:10.1039/C4AN02323D
A high power output, membrane-less formic acid/O2 enzymatic biofuel cell was fabricated, in which nitrogen-doped graphene was proven to be effective for recycling the NAD+/NADH cofactor at a nitrogen-doped graphene/gold nanoparticle/formate dehydrogenase bioanode in the catalytic oxidation of formic acid.
Co-reporter:Rui Ban, E. S. Abdel-Halim, Jianrong Zhang and Jun-Jie Zhu
Analyst 2015 vol. 140(Issue 4) pp:1046-1053
Publication Date(Web):18 Dec 2014
DOI:10.1039/C4AN02161D
A novel luminescence probe based on mono-6-amino-β-cyclodextrin (NH2-β-CD) functionalised gold nanoclusters (β-CD-AuNC) was designed for dopamine (DA) detection. The NH2-β-CD molecules were conjugated onto the surface of 11-mercaptoundecanoic acid capped AuNCs (11-MUA-AuNC) via a carbodiimide coupling reaction. The integrity of the β-CD cavities was preserved on the surface of AuNCs and they retained their capability for molecular DA host–guest recognition. DA could be captured by the β-CD cavities to form an inclusion complex in which the oxidised DA could quench the fluorescence of the β-CD-AuNC probe by electron transfer. The probe could be used to quantify DA in the range of 5–1000 nM with a detection limit of 2 nM. This sensitivity was 1–2 orders of magnitude higher than that in previously reported methods. Interference by both ascorbic acid (AA) and uric acid (UA) was not observed. Therefore, the β-CD-AuNC probe could be directly used to determine the DA content in biological samples without further separation. This strategy was successfully applied to a DA assay in spiked human serum samples and it exhibited remarkable accuracy, sensitivity and selectivity.
Co-reporter:Cui-e Zhao, Panpan Gai, Rongbin Song, Jianrong Zhang and Jun-Jie Zhu
Analytical Methods 2015 vol. 7(Issue 11) pp:4640-4644
Publication Date(Web):30 Apr 2015
DOI:10.1039/C5AY00976F
Electricity generation in microbial fuel cells (MFCs) greatly depends on anode materials, which directly affect bacterial attachment on the anode surface and extracellular electron transfer (ETT) between microorganisms and the electrode. Herein, graphene/Au (G/Au) composites were used as a novel anode material for Shewanella-inoculated MFCs. The current generation and power density of the MFCs with a G/Au modified carbon paper (CP/G/Au) anode were significantly improved compared with a conventional carbon paper (CP) anode. This could be attributed to its large surface area, excellent conductivity and good biocompatibility for enhanced bacterial loading on the anode surface and improved EET efficiency between the microbe and the electrode.
Co-reporter:Hongying Liu, Youbing Lou, Fei Zhou, Hao Zhu, E.S. Abdel-Halim, Jun-Jie Zhu
Biosensors and Bioelectronics 2015 Volume 71() pp:249-255
Publication Date(Web):15 September 2015
DOI:10.1016/j.bios.2015.04.048
•A triple-signal amplification strategy was proposed to assay the activity of TDG.•This assay is based on the DNA-QDs dendrimer-like superstructure probes.•This assay exhibited acceptable selectivity, reproducibility and stability.•The proposed biosensor was successfully applied to measuring TDG in HeLa cell.A triple-signal amplification strategy was proposed for highly sensitive and selective detection of thymine DNA glycosylase (TDG) by coupling a dendrimer-like DNA label with the electrochemical method and quantum dots (QDs) tagging. The DNA-QDs dendrimer-like superstructure was designed by DNA hybridization and covalent assembling. Benefiting from outstanding performance of the amplification strategy, this assay showed high sensitivity, extraordinary stability, and easy operation. The limit of detection could reach 0.00003 U µL−1 with a splendid specificity. The TDG content in different concentration of HeLa cell was also determined. This assay opens a new horizon for both qualitative and quantitative detection of TDG, holding great promise for potential application in cancer cell research and clinical diagnostics.
Co-reporter:Gaoxing Su, Chi Yang, and Jun-Jie Zhu
Langmuir 2015 Volume 31(Issue 2) pp:817-823
Publication Date(Web):December 18, 2014
DOI:10.1021/la504041f
Hydroxyphenol compounds are often used as reductants in controlling the growth of nanoparticles. Herein, dopamine was used as an effective reductant in seed-mediated synthesis of gold nanorods (GNRs). The as-prepared GNRs (83 × 16 nm) were monodisperse and had a high degree of purity. The conversion ratio from gold ions to GNRs was around 80%. In addition, dopamine worked as an additive. At a very low concentration of hexadecyltrimethylammonium bromide (CTAB; 0.025 M), thinner and shorter GNRs (60 × 9 nm) were successfully prepared. By regulating the concentration of silver ions, CTAB, seeds, and reductant, GNRs with longitudinal surface plasmon resonance (LSPR) peaks ranging from 680 to 1030 nm were synthesized. The growth process was tracked using UV–vis–NIR spectroscopy, and it was found that a slow growth rate was beneficial to the formation of GNRs.
Co-reporter:Penghui Zhang, Zhimei He, Chen Wang, Jiangning Chen, Jingjing Zhao, Xuena Zhu, Chen-Zhong Li, Qianhao Min, and Jun-Jie Zhu
ACS Nano 2015 Volume 9(Issue 1) pp:789
Publication Date(Web):December 19, 2014
DOI:10.1021/nn506309d
MicroRNAs (miRNAs), as key regulators in gene expression networks, have participated in many biological processes, including cancer initiation, progression, and metastasis, indicative of potential diagnostic biomarkers and therapeutic targets. To tackle the low abundance of miRNAs in a single cell, we have developed programmable nanodevices with MNAzymes to realize stringent recognition and in situ amplification of intracellular miRNAs for multiplexed detection and controlled drug release. As a proof of concept, miR-21 and miR-145, respectively up- and down-expressed in most tumor tissues, were selected as endogenous cancer indicators and therapy triggers to test the efficacy of the photothermal nanodevices. The sequence programmability and specificity of MNAzyme motifs enabled the fluorescent turn-on probes not only to sensitively profile the distributions of miR-21/miR-145 in cell lysates of HeLa, HL-60, and NIH 3T3 (9632/0, 14147/0, 2047/421 copies per cell, respectively) but also to visualize trace amounts of miRNAs in a single cell, allowing logic operation for graded cancer risk assessment and dynamic monitoring of therapy response by confocal microscopy and flow cytometry. Furthermore, through general molecular design, the MNAzyme motifs could serve as three-dimensional gatekeepers to lock the doxorubicin inside the nanocarriers. The drug nanocarriers were exclusively internalized into the target tumor cells via aptamer-guided recognition and reopened by the endogenous miRNAs, where the drug release rates could be spatial-temporally controlled by the modulation of miRNA expression. Integrated with miRNA profiling techniques, the designed nanodevices can provide general strategy for disease diagnosis, prognosis, and combination treatment with chemotherapy and gene therapy.Keywords: DNAzyme; drug delivery; intracellular imaging; logic operation; microRNAs;
Co-reporter:Tingting Zheng ; Qingfeng Zhang ; Sheng Feng ; Jun-Jie Zhu ; Qian Wang ;Hui Wang
Journal of the American Chemical Society 2014 Volume 136(Issue 6) pp:2288-2291
Publication Date(Web):January 27, 2014
DOI:10.1021/ja500169y
We have discovered that magnetic Fe3O4 nanoparticles exhibit an intrinsic catalytic activity toward the electrochemical reduction of small dye molecules. Metallic nanocages, which act as efficient signal amplifiers, can be attached to the surface of Fe3O4 beads to further enhance the catalytic electrochemical signals. The Fe3O4@nanocage core–satellite hybrid nanoparticles show significantly more robust electrocatalytic activities than the enzymatic peroxidase/H2O2 system. We have further demonstrated that these nonenzymatic nanoelectrocatalysts can be used as signal-amplifying nanoprobes for ultrasensitive electrochemical cytosensing.
Co-reporter:Yujie Ding, Hao Zhu, Xiaoxia Zhang, Jiangang Gao, E. S. Abdel-Halim, Liping Jiang and Jun-Jie Zhu
Nanoscale 2014 vol. 6(Issue 24) pp:14792-14798
Publication Date(Web):09 Oct 2014
DOI:10.1039/C4NR04380D
Upconversion nanophosphors (UCNPs) are extremely useful for analytical applications, since they display a high signal-to-noise ratio, and their photobleaching can be ignored. Herein, a novel upconversion nanocomposite composed of β-cyclodextrin (β-CD) derivative modified UCNPs and rhodamine B (RB) was prepared for the detection of cholesterol (Cho). The upconversion luminescence (UCL) emission can serve as a Cho-sensing signal by an effective fluorescence resonance energy transfer (FRET) process, using UCNPs as the donor and RB as the quencher. The sensor for Cho detection in human serum shows excellent sensitivity and selectivity, which has the potential for clinical applications in the analysis of other biological and environmental samples.
Co-reporter:Wei-Wei Xiong, Jin-Qiang Chen, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 vol. 2(Issue 35) pp:7392-7395
Publication Date(Web):11 Jul 2014
DOI:10.1039/C4TC01039F
HfS3 nanobelts were directly synthesized via a simple chemical vapor transport method. A field-effect transistor and photodetector was further fabricated based on an individual HfS3 nanobelt, and its electrical and optoelectronic properties were evaluated. The output characteristic curves of the FET revealed a typical p-type semiconducting behavior. The photodetector has an ultralow dark current (0.04 pA) and a large on/off ratio (337.5) illuminated by 405 nm light with 1.2 mW cm−2. It demonstrated excellent stability and sensitivity to 405 nm light. The results suggest that the HfS3 nanobelts are promising for application in nanoscale electronic and optoelectronic devices. The research will play a positive role in nanodevice research of one-dimensional transition-metal trichalcogenide nanostructure.
Co-reporter:Yongbing Lou, Yixin Zhao, Jinxi Chen and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 vol. 2(Issue 4) pp:595-613
Publication Date(Web):01 Nov 2013
DOI:10.1039/C3TC31937G
Colloidal semiconductor nanocrystals or quantum dots (QDs) have been facilitating the development of sensitive fluorescence sensors over the past decade, due to their unique photophysical properties, versatile surface chemistry and ligand binding ability, and the possibility of the encapsulation in different materials or attachment to different functional materials, while retaining their native luminescence property. The optical metal ion chemosensors with high sensitivity and selectivity have been developed due to the importance of the metal ions' fundamental roles, possessed in a wide range of biological processes and the aquatic environment. This review addresses the different sensing strategies with chemically modified QD hybrid structures for the sensing of metal ions in aqueous solution or an in vivo environment, and discusses the photophysical mechanisms in the different sensor systems while comparing their detecting/sensing selectivity. The perspectives for the future potential developments in QD based optical sensing for metal ions are discussed.
Co-reporter:Yujie Ding, Xiaoxia Zhang, Hao Zhu and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 vol. 2(Issue 5) pp:946-952
Publication Date(Web):31 Oct 2013
DOI:10.1039/C3TC31608D
A novel route was developed by doping rare-earth ions (RE3+) with large ionic radii (such as La3+, Ce3+, Sm3+, Eu3+, Tb3+, Dy3+, Yb3+ and Lu3+) for aspect ratio modification of KSc2F7 nanocrystals (NCs). The results revealed that the shape of the nanocrystals could be readily tuned from one-dimensional long nanorods to zero-dimensional ultrasmall nanospheres. The aspect ratio of the NCs could be adjusted over a broad range from 45 to 1 by changing the dopant or doping concentration. Interestingly it was found that doping of a lanthanide with a larger ionic radius was equivalent to increasing the amount of the dopant on the aspect ratio evolution. The NCs doped with different RE3+ also exhibited multifunctionality, including upconversion (UC) and downconversion (DC) emissions as well as paramagnetic properties.
Co-reporter:Lingling Li, Gehui Wu, Tao Hong, Zhouyang Yin, Dong Sun, E. S. Abdel-Halim, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 4) pp:2858
Publication Date(Web):January 24, 2014
DOI:10.1021/am405305r
A rapid and sensitive fluorescence sensing system for melamine based on charge transfer quenching of the fluorescence of graphene quantum dots (GQDs) in the presence of Hg2+ is proposed. The synthesized GQDs were strongly luminescent with predominantly aromatic sp2 domains. Melamine could coordinate with mercury through nitrogen atoms in both its amine and triazine groups and bring more Hg2+ to the surface of GQDs through π–π stacking, thus leading to quenching of the GQDs’ fluorescence. The quenching mechanism was investigated in detail and ascribed to charge transfer from the GQDs to Hg2+ with melamine acting as the linkage agent. The melamine demonstrated a linear range 0.15–20 μM and a detection limit of 0.12 μM, which was far below the regulatory level, suggesting the promising practical usage of this sensing system. This sensing system also possessed high selectivity for melamine in the presence of possible interferences. Finally, this novel sensor was successfully applied for melamine detection in raw milk and satisfactory recovery was achieved.Keywords: charge transfer; fluorescence quenching; graphene quantum dots; melamine; mercury ions; sensor;
Co-reporter:Feng Lu, Tennyson L. Doane, Jun-Jie Zhu and Clemens Burda
Chemical Communications 2014 vol. 50(Issue 6) pp:642-644
Publication Date(Web):28 Oct 2013
DOI:10.1039/C3CC47124A
After ligand exchange with PEG, Au NPs with differently mixed surface functionalities co-exist in the as-synthesized sample. It is found that the poorly grafted nanoparticles can be simply removed using a chromatographic method, and the well grafted nanoparticles can be eluted as a function of the core size.
Co-reporter:Shiwei Zhou, Yong Kong, Qingming Shen, Xiaolin Ren, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 23) pp:11680
Publication Date(Web):November 5, 2014
DOI:10.1021/ac502969x
Chronic myeloid leukemia (CML) is a malignant clone disease of hematopoietic stem cells. At present, the most effective therapy for CML is bone marrow transplantation, but this procedure is expensive, and it is often difficult to find appropriately matched bone marrow donors. As an alternative to marrow transplantation, a more effective anticancer drug should be developed to cure the disease; in addition, an effective system to evaluate the activity of the drug needs to be developed. Herein, we present a novel antileukemia drug evaluation method based on a multisignal amplified photoelectrochemical sensing platform that monitors the activity of caspase-3, a known marker of cell apoptosis. Manganese-doped CdS@ZnS core–shell nanoparticles (Mn:CdS@ZnS) were synthesized via a simple wet chemical method, which provided a stable photocurrent signal. A DEVD–biotin peptide and streptavidin-labeled alkaline phosphatise (SA-ALP) were immobilized successively at these nanoparticles through amide bonding and through specific interaction between biotin and streptavidin, respectively. The photocurrent of this sensing platform improved as the ALP hydrolyzed the substrate 2-phospho-l-ascorbic acid (AAP) to ascorbic acid (AA), a more efficient electron donor. The activity of caspase-3 was detected using this sensing platform, and thus, the efficacy of nilotinib for targeting K562 CML cells could be evaluated. The results indicate that nilotinib can effectively induce apoptosis of the K562 cells. This sensing platform exhibited sensitive, reproductive, and stable performance in studying the nilotinib-induced apoptosis of K562 CML cells, and the platform could be utilized to evaluate other anticancer drugs.
Co-reporter:Gao-Chao Fan, Li Han, Hua Zhu, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 24) pp:12398
Publication Date(Web):November 24, 2014
DOI:10.1021/ac504027d
An ultrasensitive photoelectrochemical sandwich immunoassay was developed to detect matrix metalloproteinase-2 (MMP-2, antigen, Ag) based on CdS:Mn/CdTe cosensitized TiO2 nanotubes (TiO2-NTs) and signal amplification of SiO2@Ab2 conjugates. Specifically, the TiO2-NTs electrode was first deposited with CdS:Mn by successive ionic layer adsorption and reaction technique and then further coated with CdTe quantum dots (QDs) via the layer-by-layer method, forming TiO2-NTs/CdS:Mn/CdTe cosensitized structure, which was employed as a matrix to immobilize capture MMP-2 antibodies (Ab1); whereas, SiO2 nanoparticles were coated with signal MMP-2 antibodies (Ab2) to form SiO2@Ab2 conjugates, which were used as signal amplification elements via the specific antibody–antigen immunoreaction between Ag and Ab2. The ultrahigh sensitivity of this immunoassay derived from the two major reasons as below. First, the TiO2-NTs/CdS:Mn/CdTe cosensitized structure could adequately absorb the light energy, dramatically promote electron transfer, and effectively inhibit the electron–hole recombination, resulting in significantly enhanced photocurrent intensity of the sensing electrode. However, in the presence of target Ag, the immobilized SiO2@Ab2 conjugates could evidently increase the steric hindrance of the sensing electrode and effectively depress the electron transfer, leading to obviously decreased photocurrent intensity. Accordingly, the well-designed photoelectrochemical immunoassay exhibited a low detection limit of 3.6 fg/mL and a wide linear range from 10 fg/mL to 500 pg/mL for target Ag detection. Meanwhile, it also presented good reproducibility, specificity, and stability and might open a new promising platform for the detection of other important biomarkers.
Co-reporter:Jing Ji, Li He, Yuanyuan Shen, Pingping Hu, Xinghua Li, Li-Ping Jiang, Jian-Rong Zhang, Lingling Li, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 7) pp:3284
Publication Date(Web):February 27, 2014
DOI:10.1021/ac500351d
A surprising electrochemiluminescence (ECL) enhancement effect in graded-gap CdSeTe@ZnS-SiO2 quantum dot (QD) bilayers was observed and used to create an ultrasensitive immunoassay. CdSeTe@ZnS-SiO2 QDs of two different sizes were used as a donor–acceptor pair, owing to their tunable energy and low biotoxicity. The graded-gap CdSeTe@ZnS-SiO2 QD bilayers were fabricated by layer-by-layer assembly of differently sized CdSeTe@ZnS-SiO2 QDs on a glutaraldehyde-activated electrode. Benefiting from a short interlayer distance and perfect spectral overlap in the graded-gap QD bilayers, highly efficient ECL resonance energy transfer (ECLRET)-based energy funneling was observed, wherein excitons from trapped states could be effectively recycled. Consequently, the observed ECL enhancement for the bilayers was more than four times greater than that observed for reference samples. The graded-gap QD bilayers were utilized in an ECL biosensor for the detection of carcinoembryonic antigen (CEA). The proposed method featured a detection limit of 0.4 pg mL–1 CEA with a linear calibration range from 1 pg mL–1 to 200 ng mL–1. This method represents a novel approach for versatile detection of biomolecules in research and clinical applications.
Co-reporter:Qianhao Min, Xiaoxia Zhang, Xueqin Chen, Siyuan Li, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 18) pp:9122
Publication Date(Web):August 19, 2014
DOI:10.1021/ac501943n
Gas-phase N-doped graphene (gNG) was synthesized by a modified thermal annealing method using gaseous melamine as nitrogen source and then for the first time applied as a matrix in negative ion matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) for small molecule analysis. Unlike the complicated adducts produced in positive ion mode, MS spectra obtained on gNG matrix in negative ion mode was only featured by deprotonated molecule ion peaks without matrix interference. By the gNG assisted desorption/ionization (D/I) process, some applications were carried out on a wide range of low-molecular weight (MW) analytes including amino acids, fatty acids, peptides, anabolic androgenic steroids as well as anticancer drugs, with an extraordinary laser desorption/ionization (LDI) efficiency over traditional α-cyano-4-hydroxycinnamic acid (CHCA) and other carbon-based materials in the negative ion detection mode. By comparison of a series of graphene-based matrixes, two main factors of matrix gNG were unveiled to play a decisive role in assisting negative ion D/I process: a well-ordered π-conjugated system for laser absorption and energy transfer; pyridinic-doped nitrogen species functioning as deprotonation sites for proton capture on negative ionization. The good salt tolerance and high sensitivity allowed further therapeutic monitoring of anticancer drug nilotinib in the spiked human serum, a real case of biology. Signal response was definitely obtained between 1 mM and 1 μM, meeting the demand of assessing drug level in the patient serum. This work creates a new application branch for nitrogen-doped graphene and provides an alternative solution for small molecule analysis.
Co-reporter:Gao-Chao Fan, Li Han, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 21) pp:10877
Publication Date(Web):October 8, 2014
DOI:10.1021/ac503043w
A TiO2/CdS:Mn hybrid structure cosensitized with two different sizes of CdTe quantum dots (QDs) was designed to develop a novel and ultrasensitive photoelectrochemical DNA assay. In this protocol, TiO2/CdS:Mn hybrid structure was prepared by successive adsorption and reaction of Cd2+/Mn2+ and S2– ions on the surface of TiO2 film and then was employed as matrix for immobilization of hairpin DNA probe, whereas large-sized CdTe–COOH QDs and small-sized CdTe–NH2 QDs as signal amplification elements were successively labeled on the terminal of hairpin DNA probe. The target DNA detection was based upon the photocurrent change originated from conformation change of the hairpin DNA probe after hybridization with target DNA. In the absence of target DNA, the immobilized DNA probe was in the hairpin form and the anchored different sizes of CdTe–COOH and CdTe–NH2 QDs were close to the TiO2/CdS:Mn electrode surface, which led to a very strong photocurrent intensity because of the formation of the cosensitized structure. However, in the presence of target DNA, the hairpin DNA probe hybridized with target DNA and changed into a more rigid, rodlike double helix, which forced the multianchored CdTe QDs away from the TiO2/CdS:Mn electrode surface, resulting in significantly decreased photocurrent intensity because of the vanished cosensitization effect. By using this cosensitization signal amplification strategy, the proposed DNA assay could offer an ultrasensitive and specific detection of DNA down to 27 aM, and it opened up a new promising platform to detect various DNA targets at ultralow levels for early diagnoses of different diseases.
Co-reporter:Yong-Ping Dong, Ting-Ting Gao, Ying Zhou, and Jun-Jie Zhu
Analytical Chemistry 2014 Volume 86(Issue 22) pp:11373
Publication Date(Web):October 31, 2014
DOI:10.1021/ac5033319
In this work, electrogenerated chemiluminescence resonance energy transfer (ECL-RET) between luminol as a donor and CdSe@ZnS quantum dots (QDs) as an acceptor was reported in neutral conditions. It was observed that a glassy carbon electrode modified with CdSe@ZnS quantum dots (CdSe@ZnS/GCE) can catalyze the luminol oxidation to promote the anodic luminol ECL without coreactants. The intensity of anodic luminol ECL (0.60 V) at the CdSe@ZnS/GCE was enhanced more than 1 order of magnitude compared with that at the bare GCE. Another stronger anodic ECL peak observed at more positive potential (1.10 V) could be assigned to the ECL-RET between the excited state of luminol and the QDs. A label-free ECL aptasensor for the detection of thrombin was fabricated based on the synergic effect of the electrocatalysis and the ECL-RET. The approach showed high sensitivity, good selectivity, and wide linearity for the detection of thrombin in the range of 10 fM–100 pM with a detection limit of 1.4 fM (S/N = 3). The results suggested that the as-proposed luminol–QDs ECL biosensor will be promising in the detection of protein.
Co-reporter:Guo-Hai Yang, Abulikemu Abulizi, Jun-Jie Zhu
Ultrasonics Sonochemistry 2014 Volume 21(Issue 6) pp:1958-1963
Publication Date(Web):November 2014
DOI:10.1016/j.ultsonch.2014.01.020
•The AuNPs/BNS nanocomposites have been synthesized by a sonochemical route.•The method needs no reducing or stabilizing agents.•The AuNPs/BNS nanocomposites exhibited good catalytic activity toward the reduction of H2O2.A simple sonochemical route was developed for the preparation of gold nanoparticles/boron nitride sheets (AuNPs/BNS) nanocomposites without using reducing or stabilizing agents. Transmission electron microscopy, scanning electron microscopy, X-ray diffraction, and UV–vis absorption spectra were used to characterize the structure and morphology of the nanocomposites. The experimental results showed that AuNPs with approximately 20 nm were uniformly attached onto the BNS surface. It was found that the AuNPs/BNS nanocomposites exhibited good catalytic activity for the reduction of H2O2. The modified electrochemical sensor showed a linear range from 0.04 to 50 mM with a detection limit of 8.3 μM at a signal-to-noise ratio of 3. The findings provide a low-cost approach to the production of stable aqueous dispersions of nanoparticles/BNS nanocomposites.
Co-reporter:Abulikemu Abulizi, Guo-Hai Yang, Jun-Jie Zhu
Ultrasonics Sonochemistry 2014 Volume 21(Issue 1) pp:129-135
Publication Date(Web):January 2014
DOI:10.1016/j.ultsonch.2013.07.013
•The Cu2O–rGO composites have been synthesised by a one-step sonochemical route.•The morphology and composition of Cu2O–rGO could be well controlled.•The Cu2O–rGO composites displayed superior photocatalytic activity.An easy, one-step synthesis of Cu2O–reduced graphene composites (Cu2O–rGO) was developed using a simple sonochemical route without any surfactants or templates. The morphology and structure of the Cu2O–rGO composites were characterised using techniques such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). The results indicated that the Cu2O sphere is approximately 200 nm in diameter and composed of small Cu2O particles approximately 20 nm in diameter. The morphology and composition of the Cu2O–rGO composites could be well controlled by simply changing the mole ratio of the reactants under ultrasonic irradiation. The Cu2O–rGO composites displayed better photocatalytic performance for the degradation of methyl orange (MO) than pure Cu2O spheres, which may have potential applications in water treatment, sensors, and energy storage.
Co-reporter:Abulikemu Abulizi, Kenji Okitsu, Jun-Jie Zhu
Ultrasonics Sonochemistry 2014 Volume 21(Issue 3) pp:1174-1181
Publication Date(Web):May 2014
DOI:10.1016/j.ultsonch.2013.10.019
•Reduction of GO to rGO was accelerated by 20 kHz ultrasound irradiation.•High power ultrasound and long pulse mode enhanced the rate of rGO formation.•High temperature, high pH and large amount of l-AA enhanced the rate of rGO formation.•Pseudo rate and activation energy of rGO formation were measured.•Physicochemical effects during acoustic cavitation enhanced the reduction of GO with l-AA.The reduction of graphene oxide (GO) to graphene (rGO) was achieved by using 20 kHz ultrasound in l-ascorbic acid (l-AA, reducing agent) aqueous solutions under various experimental conditions. The effects of ultrasound power, ultrasound pulse mode, reaction temperature, pH value and l-AA amount on the rates of rGO formation from GO reduction were investigated. The rates of rGO formation were found to be enhanced under the following conditions: high ultrasound power, long pulse mode, high temperature, high pH value and large amount of l-AA. It was also found that the rGO formation under ultrasound treatment was accelerated in comparison with a conventional mechanical mixing treatment. The pseudo rate and pseudo activation energy (Ea) of rGO formation were determined to discuss the reaction kinetics under both treatment. The Ea value of rGO formation under ultrasound treatment was clearly lower than that obtained under mechanical mixing treatment at the same condition. We proposed that physical effects such as shear forces, microjets and shock waves during acoustic cavitation enhanced the mass transfer and reaction of l-AA with GO to form rGO as well as the change in the surface morphology of GO. In addition, the rates of rGO formation were suggested to be affected by local high temperatures of cavitation bubbles.
Co-reporter:Jian-Jun Shi, Sheng Wang, Ting-Ting He, E.S. Abdel-Halim, Jun-Jie Zhu
Ultrasonics Sonochemistry 2014 Volume 21(Issue 2) pp:493-498
Publication Date(Web):March 2014
DOI:10.1016/j.ultsonch.2013.06.003
•Pulsed sonoelectrochemical technique was employed to synthesize water-soluble CdTe quantum dots.•Need no precursor preparation and N2 protection.•The size and luminescence of QDs can be easily adjusted for use as promising building blocks.A facile and fast one-pot method has been developed for the synthesis of CdTe quantum dots (QDs) in aqueous phase by a sonoelectrochemical route without the protection of N2. The morphology, structure and composition of the as-prepared products were investigated by high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and energy dispersive X-ray spectrometer (EDS). The influences of current intensity, current pulse width, and reaction temperature on the photoluminescence (PL) and quantum yield (QY) of the products were studied. The experimental results showed that the water-soluble CdTe QDs with high PL qualities can be conveniently synthesized without precursor preparation and N2 protection, and the PL emission wavelength and QY can be effectively controlled by adjusting some parameters. This method can be expected to prepare other QDs as promising building blocks in solar cell, photocatalysis and sensors.
Co-reporter:Abulikemu Abulizi, Guo Hai Yang, Kenji Okitsu, Jun-Jie Zhu
Ultrasonics Sonochemistry 2014 Volume 21(Issue 5) pp:1629-1634
Publication Date(Web):September 2014
DOI:10.1016/j.ultsonch.2014.03.030
•Reduction of MnO4− to MnO2 and MnO2 to Mn2+ could be precisely controlled by sonochemical reduction.•Solution pH affected the reduction of MnO4− and morphology of the formed MnO2.•Optimum irradiation time was important to synthesize δ-MnO2 particles with high yields.MnO2 was synthesized by sonochemical reduction of MnO4− in water under Ar atmosphere at 20 °C, where the effects of solution pH on the reduction of MnO4− were investigated. The obtained XRD results showed that poor crystallinity δ-MnO2 was formed at pH 2.2, 6.0 and 9.3. When solution pH was increased from 2.2 to 9.3, the morphologies of δ-MnO2 changed from aggregated sheet-like or needle-like structures to spherical nanoparticles and finally to cubic or polyhedron nanoparticles. After further irradiation, MnO2 was readily reduced to Mn2+. It was confirmed that H2O2 and H atoms formed in the sonolysis of water acted as reductants for both reduction for MnO4− to MnO2 and MnO2 to Mn2+. The optimum irradiation time for the effective synthesis of MnO2 was 13 min at pH 2.2, 9 min at pH 6.0, 8 min at pH 9.3, respectively.
Co-reporter:Fang-Fang Cheng, Jing-Jing Zhang, Ting-Ting He, Jian-Jun Shi, E. S. Abdel-Halim and Jun-Jie Zhu
Analyst 2014 vol. 139(Issue 16) pp:3860-3865
Publication Date(Web):22 May 2014
DOI:10.1039/C4AN00777H
The expression of microRNAs (miRNAs) is related to some cancer diseases. Recently, miRNAs have emerged as new candidate diagnostic and prognostic biomarkers for detecting a wide variety of cancers. Due to low levels, short sequences and high sequence homology among family members, the quantitative miRNA analysis is still a challenge. A novel electrochemical biosensor with triple signal amplification for the ultrasensitive detection of miRNA was developed based on phosphatase, redox-cycling amplification, a bimetallic Pd–Pt supported graphene functionalized screen-printed gold electrode, and two stem-loop structured DNAs as target capturers. The proposed biosensor is highly sensitive due to the enhanced electrochemical signal of Pd–Pt supported graphene and sufficiently selective to discriminate the target miRNA from homologous miRNAs in the presence of loop-stem structure probes with T4 DNA ligase. Therefore, this strategy provided a new and ultrasensitive platform for amplified detection and subsequent analysis of miRNA in biomedical research and clinical diagnosis.
Co-reporter:Jingjing Li, Jun-Jie Zhu, Kai Xu
TrAC Trends in Analytical Chemistry 2014 Volume 58() pp:90-98
Publication Date(Web):June 2014
DOI:10.1016/j.trac.2014.02.011
•Synthesis and bioconjugation of fluorescent metal nanoclusters (NCs) (Ag, Au, Cu, Pt).•Fluorescent metal NCs probe metal ions, small molecules, and nucleic acids.•We include use of fluorescent metal NCs for protein detection.•We review use of metal NCs in cellular and in-vivo targeting and imaging.•We envision the prospects for research on fluorescent metal NCs in the future.Fluorescent metal nanoclusters (NCs) are a class of emerging fluorescent materials. They have excellent photostability and biocompatibility with sub-nanometer size and are easy to synthesize. Taking advantage of these features, fluorescent metal NCs have been involved in exciting developments of analytical methods for fluorescent biosensing and bioimaging. In this review, we first summarize the approaches to synthesis and bioconjugation for fluorescent metal NCs (Ag, Au, Cu and Pt). We then highlight their applications as fluorescent probes for metal ions, small molecules, nucleic acids, and protein detection. We also summarize the use of metal NCs in cellular and in-vivo targeting and imaging. Finally, we envision the various prospects for research on fluorescent metal NCs in the future.
Co-reporter:Jian-Jun Shi, Ting-Ting He, Fang Jiang, E.S. Abdel-Halim, Jun-Jie Zhu
Biosensors and Bioelectronics 2014 Volume 55() pp:51-56
Publication Date(Web):15 May 2014
DOI:10.1016/j.bios.2013.11.056
•A multi-analyte electrochemical immunoassay is developed for ultrasensitive detecting IL-6 and MMP-9.•This method utilizes PS@PDA-metal nanocomposites based on GNR-modified heated screen-printed carbon electrode.•This sensor exhibits high sensitivity, convenient operability, stability and acceptable reproducibility.An ultrasensitive electrochemical immunoassay was developed for rapid detection of interleukin-6 (IL-6) and matrix metallopeptidase-9 (MMP-9); the method utilized PS@PDA-metal nanocomposites based on graphene nanoribbon (GNR)-modified heated screen-printed carbon electrode (HSPCE). Because of the good hydrophilicity and low toxicity, GNRs were used to immobilize antibodies (Ab) and amplify the electrochemical signal. PS@PDA-metal was used to label antibodies and generate a strong electrochemical signal in acetic buffer. A sandwich strategy was adopted to achieve simultaneous detection of MMP-9 and IL-6 based on HSPCE without cross-talk between adjacent electrodes in the range of 10−5 to 103 ng mL−1 with detection limits of 5 fg mL−1 and 0.1 pg mL−1 (S/N=3), respectively. The proposed method showed wide detection range, low detection limit, acceptable stability and good reproducibility. Satisfactory results were also obtained in the practical samples, thus showing this is a promising technique for simultaneous clinical detection of biocomponent proteins.
Co-reporter:Baodong Mao ; Chi-Hung Chuang ; Christopher McCleese ; Junjie Zhu ;Clemens Burda
The Journal of Physical Chemistry C 2014 Volume 118(Issue 25) pp:13883-13889
Publication Date(Web):June 2, 2014
DOI:10.1021/jp500872w
Near-infrared emitting AgInS2/ZnS nanocrystals were synthesized by carefully controlling the growth conditions in a Ag/In/Zn/S solution with less zinc relative to the other precursors. The role of having a smaller amount of zinc (8 atom %) was systematically investigated in an effort to understand the mechanism of the largely red-shifted emission. The AgInS2/ZnS nanocrystals can be transferred to aqueous solutions while retaining the emission intensity. The near-infrared emission and solubility in aqueous solutions make AgInS2/ZnS nanocrystals excellent candidates for bioimaging and photocatalytic applications.
Co-reporter:Yongbing Lou, Tingting He, Fang Jiang, Jian-Jun Shi, Jun-Jie Zhu
Talanta 2014 Volume 122() pp:135-139
Publication Date(Web):May 2014
DOI:10.1016/j.talanta.2014.01.016
•Immunosensor based on electrically heated carbon electrode (HCPE);•Combining the ERGO-AuPdNPs platform with AgNPs functionalized bionanolabel;•Sensitive and selective detection of IL-6 with a detection limit of 0.059 pg mL−1.A facile one-step electrochemical reduction method was developed to prepare electrochemically reduced graphene oxide (ERGO) and gold−palladium bimetallic nanoparticles (AuPdNPs) as the platform of immunosensor. A novel competitive electrochemical immunosensor was then proposed by combining the ERGO−AuPdNPs platform with silver nanoparticles (AgNPs) functionalized polystyrene bionanolabel for the sensitive detection of human interleukin-6 (IL-6). An electrically heated carbon electrode (HCPE) was introduced in the detection procedure of the immunosensor, and further improved the sensitivity. The immunosensor exhibited a wide linear response to IL-6 ranging from 0.1 to 100000 pg mL−1 with a detection limit of 0.059 pg mL−1. The proposed method showed good precision, broad linear range, acceptable stability and high reproducibility, and could be used for the detection of IL-6 in real samples, which possessed promising application in clinical research.Assembly procedure of IL-6−PS@PDA−AgNPs bionanolabel and schematic representation of the fabrication and measurement process of the competitive-type immunosensor.
Co-reporter:Jun-Tao Cao, Ying-Di Zhu, Rohit Kumar Rana, Jun-Jie Zhu
Biosensors and Bioelectronics 2014 Volume 51() pp:97-102
Publication Date(Web):15 January 2014
DOI:10.1016/j.bios.2013.07.025
•Microfluidic chip integrated with flexible electrochemical cytosensor was developed.•Electrochemical measurements and optical microscope observations was performed.•Label-free, on-site, and real-time monitoring of cell behavior.•Dynamic analysis of the proliferation and apoptosis of HeLa cells.•Exhibiting attractive performance in on-site monitoring of cell behavior.A novel microfluidic platform integrated with a flexible PDMS-based electrochemical cytosensor was developed for real-time monitoring of the proliferation and apoptosis of HeLa cells. The PDMS-gold film, which had a conductive smooth surface and was semi-transparent, facilitated electrochemical measurements and optical microscope observations. We observed distinct increases and decreases in peak current intensity, corresponding to cell proliferation in culture medium and apoptosis in the presence of an anticancer drug, respectively. This electrochemical analysis method permitted real-time, label-free monitoring of cell behavior, and the electrochemical results were confirmed with optical microscopy. The flexible microfluidic electrochemical platform presented here is suitable for on-site monitoring of cell behavior in microenvironments.
Co-reporter:Pan-Pan Gai, Cui-E Zhao, Ying Wang, E.S. Abdel-Halim, Jian-Rong Zhang, Jun-Jie Zhu
Biosensors and Bioelectronics 2014 Volume 62() pp:170-176
Publication Date(Web):15 December 2014
DOI:10.1016/j.bios.2014.06.043
•The nitrogen-doped graphene (NG) was found to have properties similar to NADH dehydrogenase.•An 800 mV decrease in the overpotential for NADH oxidation was observed.•NG modified electrodes showed excellent performance for the detection of NADH.•The fabricated formate biosensor exhibited remarkable performance for formate detection.•A biosensing platform was created for developing NAD+-dependent dehydrogenase biosensors.A novel electrochemical biosensing platform for nicotinamide adenine dinucleotide (NAD+)-dependent dehydrogenase catalysis was designed using the nitrogen-doped graphene (NG), which had properties similar to NADH dehydrogenase (CoI). NG mimicked flavin mononucleotide (FMN) in CoI and efficiently catalyzed NADH oxidation. NG also acted as an electron transport “bridge” from NADH to the electrode due to its excellent conductivity. In comparison with a bare gold electrode, an 800 mV decrease in the overpotential for NADH oxidation and CoI-like behavior were observed at NG-modified electrode, which is the largest decrease in overpotential for NADH oxidation reported to date. The catalytic rate constant (k) for the CoI-like behavior of NG was estimated to be 2.3×105 M−1 s−1, which is much higher than that of other previously reported FMN analogs. The Michaelis–Menten constant (Km) of NG was 26 μM, which is comparable to the Km of CoI (10 μM). Electrodes modified with NG and NG/gold nanoparticals/formate dehydrogenase (NG/AuNPs/FDH) showed excellent analytical performance for the detection of NADH and formate. This electrode fabrication strategy could be used to create a universal biosensing platform for developing NAD+-dependent dehydrogenase biosensors and biofuel cells.
Co-reporter:Penghui Zhang;Fangfang Cheng;Ri Zhou;Dr. Juntao Cao;Dr. Jingjing Li;Dr. Clemens Burda;Dr. Qianhao Min;Dr. Jun-Jie Zhu
Angewandte Chemie International Edition 2014 Volume 53( Issue 9) pp:2371-2375
Publication Date(Web):
DOI:10.1002/anie.201308920
Abstract
The design of an ideal drug delivery system with targeted recognition and zero premature release, especially controlled and specific release that is triggered by an exclusive endogenous stimulus, is a great challenge. A traceable and aptamer-targeted drug nanocarrier has now been developed; the nanocarrier was obtained by capping mesoporous silica-coated quantum dots with a programmable DNA hybrid, and the drug release was controlled by microRNA. Once the nanocarriers had been delivered into HeLa cells by aptamer-mediated recognition and endocytosis, the overexpressed endogenous miR-21 served as an exclusive key to unlock the nanocarriers by competitive hybridization with the DNA hybrid, which led to a sustained lethality of the HeLa cells. If microRNA that is exclusively expressed in specific pathological cell was screened, a combination of chemotherapy and gene therapy should pave the way for a targeted and personalized treatment of human diseases.
Co-reporter:Gao-Chao Fan, Xiao-Lin Ren, Cheng Zhu, Jian-Rong Zhang, Jun-Jie Zhu
Biosensors and Bioelectronics 2014 Volume 59() pp:45-53
Publication Date(Web):15 September 2014
DOI:10.1016/j.bios.2014.03.011
•TiO2/CdS/CdSe dual co-sensitized structure could significantly enhance the photocurrent intensity.•TiO2/CdS/CdSe dual co-sensitized structure was employed to develop a novel photoelectrochemical immunoassay.•Competitive immunosensor for highly sensitive detection of human interleukin-6 was fabricated.•The proposed co-sensitization strategy presented high sensitivity, reproducibility, specificity and stability.Dual co-sensitized structure of TiO2/CdS/CdSe was designed to develop a novel photoelectrochemical immunoassay for highly sensitive detection of human interleukin-6 (IL-6). To construct a sensing electrode, TiO2/CdS hybrid was prepared by successive adsorption and reaction of Cd2+ and S2− ions on the surface of TiO2 and then was employed as matrix for immobilization of anti-IL-6 antibody, whereas CdSe QDs linked to IL-6 were used for signal amplification via the specific antibody–antigen immunoreaction between anti-IL-6 and IL-6–CdSe bioconjugate. Greatly enhanced sensitivity for IL-6 detection was derived from the new co-sensitization signal amplification strategy. First, the TiO2/CdS/CdSe co-sensitized structure extended the absorption range to long wavelength of white light, which adequately utilized the light energy. Second, the TiO2/CdS/CdSe co-sensitized structure possessed stepwise band-edge levels favoring ultrafast transfer of photogenerated electrons and significantly prompted the photoelectrochemical performance. Besides, the introduction of CdSe effectively prevented the recombination of photogenerated electrons in the conduction band of CdS, further causing an enhanced photocurrent. Accordingly, upon the co-sensitization strategy, a novel immunoassay based on the competitive binding of anti-IL-6 antibody with IL-6 antigen and IL-6–CdSe bioconjugate was developed, and it exhibited a wide linear range from 1.0 pg/mL to 100 ng/mL with a low detection limit of 0.38 pg/mL for IL-6 detection. The proposed co-sensitization strategy presented high sensitivity, reproducibility, specificity and stability, and also opened up a new promising platform for detection of other biomarkers.
Co-reporter:Shiwei Zhou, Tingting Zheng, Yangfan Chen, Jingjing Zhang, Linting Li, Feng Lu, Jun-Jie Zhu
Biosensors and Bioelectronics 2014 Volume 61() pp:648-654
Publication Date(Web):15 November 2014
DOI:10.1016/j.bios.2014.05.064
•It is the first attempt to study the effect of combining TRAIL with dasatinib for the therapy of CML.•The TRAIL combined with dasatinib was proven to be a more effective potential antileukemic agent than either of them alone.•It is the first work to use enzymatic reaction for detection of caspase-3 activity, enhancing the specifity of the sensor.•The environmentally friendly electrochemical platform could be used for retest without strong acid or heavy metal ions.In recent decades, advanced therapies and novel scientific drug evaluation systems for chronic myeloid leukemia (CML) treatment are very urgent due to its increasing morbidity. The combination of dasatinib with tumor necrosis factor (TNF)-related apoptosis-inducing ligand (TRAIL) was supposed to be effective for leukemia therapy. Taking full advantage of novel nano-biotechnology, we have developed a robust electrochemical cytosensing approach to profile the therapeutic effects of dasatinib and TRAIL by probing the activity of caspase-3 from apoptotic CML cells. The sensor was on a base of a glassy carbon electrode (GCE) modified with nano-materials composed of Au nanoparticles (AuNPs), poly(dimethyl diallyl ammonium chloride) (PDDA), and carbon nanotubes (CNTs). Then the platform immobilized the biotinylated DEVD-peptide (biotin-Gly-Asp-Gly-Asp-Glu-Val-Asp-Gly-Cys) via the strong bonding between AuNPs and the thiol group (Au–S bond). In particular, the sensor was then constructed with the environmentally friendly alkaline phosphatase (ALP) via the specific interaction between the biotin and streptavidin, and could retest detection indirectly for caspase-3 sensing by detecting the differential pulse voltammetry (DPV) signal of enzymatic catalysis product, ascorbic acid (AA). The results indicated that either dasatinib or TRAIL could successfully induce the apoptosis of CML cells, while the combination of dasatinib and TRAIL resulted in an improved therapeutic effect, suggesting a novel optimized strategy for CML therapy. This novel electrochemical sensing strategy exhibits attractive advantages of environmental benignity, simple performance, high stability, and may be readily expanded to evaluate other cancer therapeutic effects.
Co-reporter:Cui-e Zhao;Wen-Jing Wang;Dong Sun;Dr. Xin Wang; Jian-Rong Zhang; Jun-Jie Zhu
Chemistry - A European Journal 2014 Volume 20( Issue 23) pp:7091-7097
Publication Date(Web):
DOI:10.1002/chem.201400272
Abstract
A new nanostructured graphene/TiO2 (G/TiO2) hybrid was synthesized by a facile microwave-assisted solvothermal process in which amorphous TiO2 was assembled on graphene in situ. The resulting G/TiO2 hybrids were characterized by XRD, SEM, TEM, Raman spectroscopy, and N2 adsorption/desorption analysis. The electrochemical properties of the hybrids as anode materials for Shewanella-inoculated microbial fuel cells (MFCs) were studied for the first time, and they proved to be effective in improving MFC performance. The significantly improved bacterial attachment and extracellular electron-transfer efficiency could be attributed to the high specific surface area, active groups, large pore volume, and excellent conductivity of the nanostructured G/TiO2 hybrid, and this suggests that it could be a promising candidate for high-performance MFCs.
Co-reporter:Jingjing Li, Wenjing Wang, Defang Sun, Jiangning Chen, Peng-Hui Zhang, Jian-Rong Zhang, Qianhao Min and Jun-Jie Zhu
Chemical Science 2013 vol. 4(Issue 9) pp:3514-3521
Publication Date(Web):19 Jun 2013
DOI:10.1039/C3SC51538A
The use of small interfering RNA (siRNA) to silence target genes involved in disease has generated much excitement in the scientific community. While promising, the clinical application of RNA interference (RNAi) is still challenging in achieving effective delivery and tracking of siRNA to target cells. A new multifunctional probe comprising a cell-specific internalization aptamer, fluorescent silver nanoclusters (Ag NCs), and therapeutic siRNA was developed in one system for the specific delivery of siRNA into a target cell and for simultaneous noninvasive imaging. Different from described nanocarrier-based delivery methods which have to suffer from complicated conjugation, Ag NCs could be synthesized directly from the aptamer chimera. Sgc8c aptamer-functionalized Ag NCs as a cell-type specific siRNA delivery and imaging probe complements recent advances in PSMA aptamer-based siRNA delivery and nanomaterial-based molecular imaging. Besides, siRNA in the Ag NCs–streptavidin–siRNA complex displayed outstanding stability in both binding buffer and cell culture medium. The fluorescent intensity of biotinylated aptamer-functionalized Ag NCs was enhanced in acidic environment and no observable quenching of fluorescence occurred even after incubation for 48 h, which could benefit their usage in the intracellular environment. The facile synthetic process, good biocompatibility, excellent stability and comparable gene silencing effect with commercial reagent make it more promising for in vivo applications.
Co-reporter:Sai Bi, Bin Ji, Zhipeng Zhang and Jun-Jie Zhu
Chemical Science 2013 vol. 4(Issue 4) pp:1858-1863
Publication Date(Web):06 Feb 2013
DOI:10.1039/C3SC00043E
Supramolecular structures composed of padlock probes and primers were used to perform rolling circle amplification (RCA) which was achieved by metal ion (Hg2+ or Ag+) induced DNA ligase activity. In the presence of Hg2+ (or Ag+), the specific and strong interaction between thymidine–thymidine and Hg2+ (or cytosine–cytosine and Ag+) at the terminal of the padlock probe enabled the circularization of the padlock probe with primer in the aid of DNA ligase. An RCA process was then accomplished by DNA polymerase/dNTPs. The RCA product containing multiple tandem repeats could hybridize with a large number of molecular beacons (reporter), resulting in an enhanced fluorescence signal. This proposed single-input YES gate enabled the sensitive and selective detection of Hg2+ (or Ag+). Additionally, based on the principle of DNA hybridization and displacement, a NOT logic gate was constructed by designing a double-stranded fluorescence probe as reporter. Significantly, this assay was further applied to the construction of a complete set of two-input molecular-scale logic gates and three advanced logic devices.
Co-reporter:Cuie Zhao, Panpan Gai, Changhong Liu, Xin Wang, Hao Xu, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 vol. 1(Issue 40) pp:12587-12594
Publication Date(Web):14 Aug 2013
DOI:10.1039/C3TA12947K
Microbial fuel cells (MFCs) show promise as a technology for electricity generation from waste, and their performance critically depends on the electrode materials and their structures. Herein, a novel MFC anode was fabricated by electro-depositing polyaniline (PANI) networks onto graphene nanoribbons (GNRs)-coated carbon paper (CP/GNRs/PANI). This anode provides a large surface area for the attachment of bacterial cells and high conductivity to facilitate extracellular electron transfer (EET) from microbes to the electrode. Results showed that the anodic current density and power density of the CP/GNRs/PANI anode were much higher than those of each individual component as anode, indicating the synergistic effect between PANI and GNRs.
Co-reporter:Lingling Li, Gehui Wu, Guohai Yang, Juan Peng, Jianwei Zhao and Jun-Jie Zhu
Nanoscale 2013 vol. 5(Issue 10) pp:4015-4039
Publication Date(Web):10 Jan 2013
DOI:10.1039/C3NR33849E
To obtain graphene-based fluorescent materials, one of the effective approaches is to convert one-dimensional (1D) graphene to 0D graphene quantum dots (GQDs), yielding an emerging nanolight with extraordinary properties due to their remarkable quantum confinement and edge effects. In this review, the state-of-the-art knowledge of GQDs is presented. The synthetic methods were summarized, with emphasis on the top-down routes which possess the advantages of abundant raw materials, large scale production and simple operation. Optical properties of GQDs are also systematically discussed ranging from the mechanism, the influencing factors to the optical tunability. The current applications are also reviewed, followed by an outlook on their future and potential development, involving the effective synthetic methods, systematic photoluminescent mechanism, bandgap engineering, in addition to the potential applications in bioimaging, sensors, etc.
Co-reporter:Guohai Yang, Yongjie Li, Rohit Kumar Rana and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 vol. 1(Issue 5) pp:1754-1762
Publication Date(Web):28 Nov 2012
DOI:10.1039/C2TA00776B
A facile in situ assembly strategy was developed for the fabrication of Pt–Au alloy nanoparticles (NPs) on nitrogen-doped graphene (N–G) sheets, and the as-fabricated Pt–Au/N–G nanocomposites were suitable for electrochemical applications. As characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction analysis and inductively coupled plasma-atomic emission spectroscopy techniques, Pt–Au alloy NPs with an average size of 4–5 nm were uniformly distributed on the N–G surface through intrinsic covalent bonds. The Pt–Au/N–G nanocomposites exhibited excellent electrocatalytic activity and stability towards the methanol oxidation reaction with the highest capability observed for a Pt/Au atomic ratio of 3/1. The unique electrochemical features are distinctive from those of N-free nanocomposites and commercially available Pt/C catalysts, indicative of the alloying effect of Pt–Au and their synergistic interaction with the N–G sheet, which may open up new possibilities for the preparation of N–G-based nanocomposites for other intensive applications as well.
Co-reporter:Fang-Fang Cheng, Wei Chen, Li-Hui Hu, Gang Chen, Hai-Tao Miao, Chenzhong Li and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 vol. 1(Issue 38) pp:4956-4962
Publication Date(Web):22 Jul 2013
DOI:10.1039/C3TB20656D
Graphene/Au composites with a high positive charge, which is advantageous for the binding and condensation of negatively charged siRNA, are synthesized via an in situ reduction method, using PEI as a reductant and protective reagent. Owing to the sufficient amounts of amino groups, PEI-grafted graphene/Au composites can be further modified with methoxyl-PEG to acquire low cytotoxicity, novel blood compatibility, and optimal dispersibility in physiological environments. The obtained PEGylated PEI-grafted graphene/Au composites (PPGA) allow efficient loading of siRNA, forming PPGA/siRNA complexes to transport into HL-60 cells and downregulated anti-apoptosis Bcl-2 protein, indicating PPGA is a suitable platform for gene delivery. Moreover, PPGA display an enhanced photothermal response with respect to PPG under NIR laser irradiation, suggesting that PPGA can be used as an efficient photothermal agent.
Co-reporter:Wei-Wei Xiong, Guo-Hai Yang, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 vol. 1(Issue 33) pp:4160-4165
Publication Date(Web):24 Jun 2013
DOI:10.1039/C3TB20638F
Low-toxicity, highly luminescent, and water-soluble AgInS2/ZnS nanocrystals (NCs) have been synthesized via a microwave-assisted approach. The structure and optical features of the AgInS2/ZnS NCs were characterized by X-ray diffraction, high resolution transmission electron microscopy, Fourier transform infrared spectroscopy, ultraviolet visible absorption spectroscopy and photoluminescence (PL) spectroscopy. The as-synthesized AgInS2/ZnS NCs exhibited high PL quantum yields (40%) and long PL lifetimes (424.5 ns). Furthermore, the dynamic changes of the intracellular copper(II) levels in HeLa cells were monitored using the AgInS2/ZnS NCs as fluorescent probes. The results showed that the AgInS2/ZnS NCs as promising fluorescent probes can be used in the detection of intracellular copper ions in living cells.
Co-reporter:Yun Chen, Panpan Gai, Li Jin, Dong Zhu, Danbi Tian, E. S. Abdel-Halim, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 vol. 1(Issue 28) pp:3451-3457
Publication Date(Web):28 May 2013
DOI:10.1039/C3TB20513D
Poly(3,4-ethylenedioxythiophene) (PEDOT) nanowhiskers were fabricated in a [bmim][BF4] ionic liquid. The minimal size of the nanowhiskers is only 0.2 nm, and the size matches the thickness of a PEDOT single-molecular chain. They were successfully used as the electron transfer channels between the active center of hemoglobin (Hb) and an underlying electrode. The direct electron transfer process between Hb and the underlying electrode was realized without any electron mediator. Compared to that of a gold nanoparticle (AuNP)–Hb composite electrode, the catalytic current of a PEDOT nanowhiskers–AuNPs–Hb composite electrode for detecting H2O2 is increased 7 fold. A novel model of a H2O2 biosensor based on the PEDOT nanowhiskers–AuNPs–Hb composites was fabricated. The detection limit was estimated to be 0.6 μM at a signal/noise (S/N) ratio of 3, and the linear range of H2O2 concentration was from 1 μM to 1100 μM. Three constructed models of the biosensors showed a good stability, and all of them retained nearly 90% of their initial signals for 1 mM H2O2 when they were stored at 4 °C after 60 days. H2O2 concentration in contact lens nursing liquid was measured by the biosensor, and the results were in good agreement with the values provided by the supplier. It is shown that the PEDOT nanowhiskers can provide a new opportunity for the design of sensitive biosensors with long-term stability.
Co-reporter:Feng Lu, Adriana Popa, Shiwei Zhou, Jun-Jie Zhu and Anna Cristina S. Samia
Chemical Communications 2013 vol. 49(Issue 97) pp:11436-11438
Publication Date(Web):30 Oct 2013
DOI:10.1039/C3CC46658B
Magnetic field-responsive iron oxide-loaded hollow mesoporous silica nanocapsules that exhibit high drug loading capacity were synthesized using polymer nanospheres as sacrificial templates. Due to their magnetic field induced heating and remotely triggered drug release capabilities, these hybrid nanomaterials provide an excellent platform for the combination of hyperthermia and chemotherapy.
Co-reporter:Guo-Hai Yang, Jian-Jun Shi, Sheng Wang, Wei-Wei Xiong, Li-Ping Jiang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2013 vol. 49(Issue 91) pp:10757-10759
Publication Date(Web):27 Sep 2013
DOI:10.1039/C3CC45759A
A multifunctional boron nitride–gold nanocluster composite was fabricated using poly-diallyldimethylammonium chloride as a stabilizer and a linker. The as-fabricated composite could be used as a fluorescent or an electrochemical label for immunosensing in the sensitive detection of interleukin-6.
Co-reporter:Tingting Zheng, Rui Zhang, Qingfeng Zhang, Tingting Tan, Kui Zhang, Jun-Jie Zhu and Hui Wang
Chemical Communications 2013 vol. 49(Issue 72) pp:7881-7883
Publication Date(Web):11 Jul 2013
DOI:10.1039/C3CC44623A
We have developed a robust enzymatic peptide cleavage-based assay for the ultrasensitive dual-channel detection of matrix metalloproteinase-2 (MMP-2) in human serum using gold-quantum dot (Au-QD) core–satellite nanoprobes.
Co-reporter:Yujie Ding, Hao Zhu, Xiaoxia Zhang, Jun-Jie Zhu and Clemens Burda
Chemical Communications 2013 vol. 49(Issue 71) pp:7797-7799
Publication Date(Web):02 Jul 2013
DOI:10.1039/C3CC43926G
A novel fluorescence resonance energy transfer (FRET)-based probe, γ-cyclodextrin modified oleic acid–NaYF4:Yb, Ho upconversion nanoparticles functionalized with a rhodamine B derivative (RBD), has been achieved for Fe3+-sensing in aqueous solution with high sensitivity and selectivity.
Co-reporter:Cuie Zhao, Ying Wang, Fengjian Shi, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2013 vol. 49(Issue 59) pp:6668-6670
Publication Date(Web):04 Jun 2013
DOI:10.1039/C3CC42068J
The positively-charged ionic liquid functionalized graphene nanosheets (IL-GNS) were used as an anode in microbial fuel cells (MFCs), and proved effective for the high biocurrent generation and power output.
Co-reporter:Sai Bi, Tingting Zhao, Baoyu Luo and Jun-Jie Zhu
Chemical Communications 2013 vol. 49(Issue 61) pp:6906-6908
Publication Date(Web):12 Jun 2013
DOI:10.1039/C3CC43353F
A novel hybridization chain reaction-based branched rolling circle amplification combining the fabrication of multi-HRP-capped MNPs is developed for chemiluminescence detection of DNA methyltransferase activities and inhibitors with high sensitivity in a well-controlled manner.
Co-reporter:Peng-Hui Zhang, Jun-Tao Cao, Qian-Hao Min, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 15) pp:7417
Publication Date(Web):July 3, 2013
DOI:10.1021/am401740a
In this paper, we have developed a core-triple-shell structured multi-functional nanoprobe Fe3O4/SiO2/CdSeTe@ZnS–SiO2/polydopamine with strong fluorescence and a fast magnetic response for specifically recognizing, fluorescently labeling, and magnetically sorting target tumor cells on a microfluidic chip. The outer polydopamine layer not only effectively alleviated the quenching effect of the interlayer quantum dots but also provided a convenient and versatile functional interface to readily conjugate with the recognizing model molecules of aptamer KH1C12 with amine, thiol, or carboxyl groups. Moreover, the polydopamine isolation and PEG decoration equipped the as-fabricated nanoprobes with little cytotoxicity and nonspecific affinity, leading to the effective and specific profiling of the protein epitopes expressed on the target tumor cells. Taking advantage of the magnetic property and specific recognition, the modified nanoprobe was utilized to label and isolate HL-60 cells from a homogeneous cell mixture of HL-60 and K562 cells on a microfluidic chip. Combining with the high throughput of the microfluidic chip, 1.0 × 104 HL-60 cells were readily separated from 2.0 × 104 cells in only 10 min with 98% separation efficiency, markedly improved in comparison with conventional strategies. This study presents an innovative strategy for developing highly integrated nanoprobes of strong fluorescence and magnetic controllability, opening up a promising probe-based avenue for biological imaging and separation.Keywords: cell imaging; cell sorting; magnetic−fluorescent nanoprobe; microfluidic chip; polydopamine;
Co-reporter:Wei-Wei Xiong, Guo-Hai Yang, Xing-Cai Wu, and Jun-Jie Zhu
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 16) pp:8210
Publication Date(Web):August 4, 2013
DOI:10.1021/am402328t
In this Article, we present a facile microwave-assisted synthesis route for the preparation of water-soluble and high-quality CuInS2/ZnS nanocrystals (NCs) with glutathione as the stabilizer. The as-prepared CuInS2/ZnS NCs exhibited small particle sizes (∼3.3 nm), long photoluminescence lifetimes, and color-tunable properties ranging from the visible to the near-infrared by varying the initial ratio of Cu/In in the precursors. The low-toxicity, highly luminescent and biocompatible CuInS2/ZnS NCs were applied to cell imaging, showing that they could be used as promising fluorescent probes. Furthermore, the CuInS2/ZnS NCs were used as the signal labels for a fluoroimmunoassay of the biomarker IL-6, showing their great potential for use as reliable point-of-care diagnostics for biomarkers of cancer and other diseases.Keywords: color tunable; CuInS2/ZnS nanocrystals; fluoroimmunoassay; human interleukin-6; microwave assisted;
Co-reporter:Hongying Liu, Shouming Xu, Zhimei He, Anping Deng, and Jun-Jie Zhu
Analytical Chemistry 2013 Volume 85(Issue 6) pp:3385
Publication Date(Web):February 18, 2013
DOI:10.1021/ac303789x
In this work, a signal amplification supersandwich strategy was developed for highly selective and sensitive detection of cancer cells using aptamer-DNA concatamer-quantum dots (QDs) probes. First of all, electrode materials denoted as MWCNTs@PDA@AuNPs were fabricated by multiwall carbon nanotubes (MWCNTs), gold nanoparticles (AuNPs), and polydopamine (PDA) using a layer-by-layer technique. Then, the prepared bases as matrices were applied to bind concanavalin A (Con A), resulting in high stability, bioactivity, and capability for cell capture. Meanwhile, aptamer-DNA concatamer-QDs were designed via DNA hybridization followed by covalent assembling, which incorporated the specific recognition of the aptamer with the signal amplification of the DNA concatamer and QDs. With aptamer-DNA concatamer-QDs as recognizing probes, the model cancer cells (CCRF-CEM cells) were detected using a MWCNTs@PDA@AuNPs modified electrode with trapped Con A by means of fluorescence and electrochemical methods. The proposed supersandwich cytosensor showed high sensitivity with the detection limit of 50 cells mL–1. More importantly, it could distinguish cancer cells from normal cells, which indicated the promising applications of our method in clinical diagnosis and treatment of cancers.
Co-reporter:Tingting Zheng, Jia-Ju Fu, Lihui Hu, Fan Qiu, Minjin Hu, Jun-Jie Zhu, Zi-Chun Hua, and Hui Wang
Analytical Chemistry 2013 Volume 85(Issue 11) pp:5609
Publication Date(Web):April 26, 2013
DOI:10.1021/ac400994p
The variable susceptibility to the tumor necrosis factor-related apoptosis-inducing ligand (TRAIL) treatment observed in various types of leukemia cells is related to the difference in the expression levels of death receptors, DR4 and DR5, on the cell surfaces. Quantifying the DR4/DR5 expression status on leukemia cell surfaces is of vital importance to the development of diagnostic tools to guide death receptor-based leukemia treatment. Taking the full advantages of novel nanobiotechnology, we have developed a robust electrochemical cytosensing approach toward ultrasensitive detection of leukemia cells with detection limit as low as ∼40 cells and quantitative evaluation of DR4/DR5 expression on leukemia cell surfaces. The optimization of electron transfer and cell capture processes at specifically tailored nanobiointerfaces and the incorporation of multiple functions into rationally designed nanoprobes provide unique opportunities of integrating high specificity and signal amplification on one electrochemical cytosensor. The high sensitivity and selectivity of this electrochemical cytosensing approach also allows us to evaluate the dynamic alteration of DR4/DR5 expression on the surfaces of living cells in response to drug treatments. Using the TRAIL-resistant HL-60 cells and TRAIL-sensitive Jurkat cells as model cells, we have further verified that the TRAIL susceptibility of various types of leukemia cells is directly correlated to the surface expression levels of DR4/DR5. This versatile electrochemical cytosensing platform is believed to be of great clinical value for the early diagnosis of human leukemia and the evaluation of therapeutic effects on leukemia patients after radiation therapy or drug treatment.
Co-reporter:Guohai Yang, Lingling Li, Rohit Kumar Rana, Jun-Jie Zhu
Carbon 2013 Volume 61() pp:357-366
Publication Date(Web):September 2013
DOI:10.1016/j.carbon.2013.05.016
A new electrochemical immunosensor was developed for ultrasensitive detection of matrix metalloproteinase-2 (MMP-2), which is one of the key biomarkers in blood. In our approach, an effective assembly of well-defined gold nanoparticles on nitrogen-doped graphene sheets was demonstrated. The composite facilitated robust immobilization of antibodies, promoted electron transfer and exhibited excellent electrochemical activity, which are suitable for biosensing. The design of the immunosensor also involved a polydopamine functionalized graphene oxide hybrid conjugated to horseradish peroxidase-secondary antibodies by covalent bonds as a multi-labeled and biocompatible probe to increase the electrochemical response. This novel signal amplification strategy with a sandwich-type immunoreaction significantly enhanced the sensitivity of detection of biomarkers. The proposed immunosensor displayed excellent analytical performance in the detection of MMP-2 ranging from 0.0005 to 50 ng mL−1, with a detection limit of 0.11 pg mL−1. Furthermore, it not only exhibited good stability with adequate reproducibility and accuracy, but also demonstrated efficiency in the detection of MMP-2 in real samples.
Co-reporter:Guohai Yang, Juntao Cao, Lingling Li, Rohit Kumar Rana, Jun-Jie Zhu
Carbon 2013 Volume 51() pp:124-133
Publication Date(Web):January 2013
DOI:10.1016/j.carbon.2012.08.020
Here we demonstrate the fabrication of an effective cytosensor using carboxymethyl chitosan-functionalized graphene (CMC-G) prepared through chemical reduction of graphene oxide. The CMC-G hybrid was further characterized with UV–vis spectroscopy, Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, transmission electron microscopy and atomic force microscopy. Layer-by-layer assembly of CMC-G with polyethyleneimine and folic acid enabled the fabrication of a label-free electrochemical impedance spectroscopy cytosensor with high stability and biocompatibility. The proposed cytosensor exhibited good electrochemical behavior and cell-capture ability for HL-60 cells, and showed a wide linear range and low detection limit for quantification.
Co-reporter:Qianhao Min, Xueqin Chen, Xiaoxia Zhang and Jun-Jie Zhu
Lab on a Chip 2013 vol. 13(Issue 19) pp:3853-3861
Publication Date(Web):03 Jul 2013
DOI:10.1039/C3LC50548K
Herein we present a gravity-driven microdevice furnished with tunable TiO2 nanotube arrays (TNAs) inside as the separation medium for consecutive on-chip enrichment and isotope labeling of serum phosphopeptides. The 3D tubular architectures of TNAs dramatically enhanced the affinity towards phosphate-containing molecules and also provided a spacious microenvironment for isotope dimethyl labeling reactions. To maximize the efficiency and capacity of the phosphopeptide enrichment, nanoscale tailoring and microscale fabrication were employed for adjusting the TNAs’ pore sizes and the channel patterns. The S-shaped microdevice equipped with interior TNAs anodized at 25 V was utilised for consecutive serum processing, and further differential expression analysis of endogenous phosphopeptides between ovarian cancer patients and healthy women. The phosphorylated fibrinogen peptide A (FPA, AD[pS]GEGDFLAEGGGVR) was found to be down-regulated by about 4 times while its isoform (D[pS]GEGDFLAEGGGV) was 2.4-fold up-regulated in the patient specimens. In principle, this nanostructure-embedded model introduced tailor-made bioseparation materials into the microdevice, undoubtedly facilitating the workflow of sample pretreatment and thus assisting the analysis of disease-associated biomolecules in biomedical research.
Co-reporter:Zheng-Zhi Yin, Yongjie Li, Li-Ping Jiang, Rohit Kumar Rana, Jun-Jie Zhu
Analytica Chimica Acta 2013 Volume 781() pp:48-53
Publication Date(Web):5 June 2013
DOI:10.1016/j.aca.2013.04.011
•Haemin-modified iron(II, III) oxide (Fe3O4) nanoparticles were rapidly synthesised.•Magnetic Fe3O4/haemin show electrocatalytic activity towards trichloroacetic acid.•The response of sensor was studied via electrically heated electrodes.Haemin-functionalised magnetic iron(II, III) oxide (Fe3O4) nanoparticles (Fe3O4/haemin) were synthesised by changing the acidity of a solution of the two compounds. The nanoparticles were characterised by transmission electron microscopy, UV–vis absorption spectroscopy, X-ray diffraction, Fourier transform infrared spectroscopy, measurement of magnetisation, and electrochemical techniques. The properties of both haemin and Fe3O4 were retained. Thus, Fe3O4/haemin nanoparticles exhibited pronounced electrocatalytic activity towards trichloroacetic acid (TCA) like haemin itself. Interestingly, electrocatalytic activity towards TCA was affected by detection temperature, which was controlled via electrically heated carbon paste electrodes. The maximal catalytic current was 5.8 times higher at 60 °C than at room temperature (25 °C). This proposed electrochemical sensor for TCA possessed a linear detection range of 5–80 μM and a detection limit of 0.3 μM at 60 °C.
Co-reporter:Danchen Wang, Lihui Hu, Huiming Zhou, E.S. Abdel-Halim, Jun-Jie Zhu
Electrochemistry Communications 2013 Volume 33() pp:80-83
Publication Date(Web):August 2013
DOI:10.1016/j.elecom.2013.04.030
•An ultrasensitive electrochemical method is proposed for detection of microRNA-16.•Molecular beacon structure is designed to initiate RCA for the high selectivity.•To achieve signal amplification, RCA and quantum dots tagging are utilized.MicroRNA-16 (miR-16) frequently deleted or downregulated in patients with B cell chronic lymphocytic leukemia and thus can be used as promising biomarkers in B-CLL diagnosis and prognosis. Herein, an ultrasensitive miR-16 detection was carried out by combining rolling circle amplification (RCA), quantum dots tagging and anodic stripping voltammetric detection (ASV). The method could specifically quantify miR-16 over a 6-decade dynamic range and reach an ultra-low detection limit of 0.32 aM.
Co-reporter:Lihui Hu, Tingting Tan, Gang Chen, Kui Zhang, Jun-Jie Zhu
Electrochemistry Communications 2013 Volume 35() pp:104-107
Publication Date(Web):October 2013
DOI:10.1016/j.elecom.2013.08.004
•Polymerase-based target recycling amplification was used for fusion gene detection.•Cascade hybridization is utilized for further signal amplification.•Ultrasensitive biosensor was developed by using anodic stripping voltammetry.A specially tailored electrochemical biosensor for ultrasensitive detection of BCR/ABL fusion gene was developed with high selectivity, acceptable rapidity and excellent extensibility. Taking advantage of circular strand replacement polymerization, cascade hybridization reaction as well as quantum dot based signal amplification, the proposed biosensor showed high sensitivity with the detection limit down to 2 fM. This strategy offers a great promise to early diagnosis and prognosis of chronic myeloid leukemia.
Co-reporter:Fang-Fang Cheng, Guo-Xi Liang, Yuan-Yuan Shen, Rohit Kumar Rana and Jun-Jie Zhu
Analyst 2013 vol. 138(Issue 2) pp:666-670
Publication Date(Web):12 Nov 2012
DOI:10.1039/C2AN36434D
Hsp70 proteins are implicated in resistance to chemotherapy in cancers, the detection of which is important for cancer treatment and prognosis. In this work, we report the study on the detection of specific intracellular target protein in fixed cells using GlcNAc-conjugated CdSeTe QDs. The QDs were coupled with Con A via a carbodiimide reaction and then were further assembled with GlcNAc by lectin–carbohydrate interaction between Con A and GlcNAc. The obtained QDs-Con A-GlcNAc conjugates have an emission wavelength at 650 nm that is close to the near-infrared (NIR) regions and a specific recognition for Hsp70. These results show that the QDs-Con A-GlcNAc probe can be a promising tool for direct localization of the Hsp70 protein.
Co-reporter:Haiping Huang and Jun-Jie Zhu
Analyst 2013 vol. 138(Issue 20) pp:5855-5865
Publication Date(Web):08 Jul 2013
DOI:10.1039/C3AN01034A
As newly developed inorganic materials, semiconductor nanocrystals (NCs), or quantum dots (QDs), have received considerable attention because of their unique nano-related properties including high quantum yield, simultaneous excitation with multiple fluorescence colors, and electrochemical properties. This review presents a general description of the electrochemical properties of QDs with their electrochemical applications including indirect and direct effects. The fields of inorganic substance analysis, organic analysis, immunoanalysis, DNA analysis and aptamer analysis are discussed in detail.
Co-reporter:Kui Zhang, Tingting Tan, Jia-Ju Fu, Tingting Zheng and Jun-Jie Zhu
Analyst 2013 vol. 138(Issue 21) pp:6323-6330
Publication Date(Web):05 Aug 2013
DOI:10.1039/C3AN01255G
A robust, nanobiotechnology-based electrochemical cytosensing platform for the detection of acute leukemia cells was developed with high sensitivity, selectivity, acceptable rapidity and excellent extensibility. It utilized the competitive binding of cell-specific aptamers to acute leukemia cells and subsequent voltammetric quantification of the metal signature. Greatly enhanced sensitivity was achieved with dual signal amplification by using Fe3O4 magnetic nanoparticles (MNPs) as carriers to load a large amount of gold nanoparticles (AuNPs) and AuNP-catalyzed silver deposition. The proposed competitive cytosensor showed high sensitivity with a detection limit down to 10 cells. This simple and low-cost electrochemical cytosensing approach offers great promise to extend its application to early detection of human leukemia and possibly to other cancer cells.
Co-reporter:Jingjing Li and Jun-Jie Zhu
Analyst 2013 vol. 138(Issue 9) pp:2506-2515
Publication Date(Web):13 Feb 2013
DOI:10.1039/C3AN36705C
Quantum dots (QDs) have been facilitating the development of sensitive fluorescence biosensors over the past two decades due to their high quantum yield, narrow and tunable emission spectrum and good photostability. The new emerging QDs with improved biocompatibility further promote their biological applications. In this review, we first briefly introduce the prevalently used QDs and their preparation and bioconjugation approaches. Then we summarize QDs-based fluorescent biosensing for proteins and nucleic acids, and QDs-based applications in cellular and in vivo targeting and imaging. Last but not the least, we envision the potential QDs-based applications in future perspectives.
Co-reporter:Fang Jiang, Jing-Jing Zhang, Jian-Rong Zhang and Jun-Jie Zhu
Analyst 2013 vol. 138(Issue 7) pp:1962-1965
Publication Date(Web):08 Feb 2013
DOI:10.1039/C3AN00006K
A dual signal amplification strategy was designed for electrochemical detection of matrix metalloproteinase-9 with the integration of electrically heated carbon electrode technique and quantum dots labels.
Co-reporter:Feng Lu, Shiwei Zhou, Jun-Jie Zhu
International Journal of Hydrogen Energy 2013 Volume 38(Issue 29) pp:13055-13061
Publication Date(Web):30 September 2013
DOI:10.1016/j.ijhydene.2013.03.081
•Rapid photochemical synthesis of highly fluorescent Ag nanoclusters.•Large scale synthesis by using sunlight.•Enhanced fluorescent intensity with ionic liquid.•AgNCs is a promising photo-sensitizer in solar cell and water splitting devices.Fluorescent silver nanoclusters with a size of about 2 nm were synthesized within 90 s by irradiating a mixture of silver precursor and polymethacrylic acid sodium salt solution under Xe lamp. The proposed method was well optimized by a systematical investigation of experimental parameters, such as irradiation time, initial concentration, pH of the solution. The obtained nanoclusters were well dispersed in water and exhibited bright emission upon visible light excitation. This approach can be further extended to use solar light for the large scale synthesis. Strikingly, the emission intensity of as-prepared silver nanoclusters could be enhanced up to ∼60% by the addition of 1-(2′-hydroxylethyl)-3-methylimidazolium tetrafluoroborate ([HOEtMIm][BF4]) ionic liquid. Meanwhile, these nanoclusters, in between molecules and normal nanoparticles, intensely absorb light around 510 nm covering the most intense part of solar light, should be a promising visible light sensitizer in solar cell and water splitting applications.
Co-reporter:Rui Ban, Jingjing Li, Juntao Cao, Penghui Zhang, Jianrong Zhang and Jun-jie Zhu
Analytical Methods 2013 vol. 5(Issue 21) pp:5929-5937
Publication Date(Web):21 Aug 2013
DOI:10.1039/C3AY41189C
High-quality glutathione (GSH) capped ZnS:Mn/ZnS core/shell doped quantum dots (d-dots) with pure dopant emission band and excellent stability have been synthesized directly in aqueous media. The influences of experimental variables on the luminescent properties of the ZnS:Mn/ZnS nanocrystals have been investigated. The quantum yield of the dopant Mn photoluminescence in the as-prepared ZnS:Mn/ZnS core/shell d-dots can be up to 27.4%. The value is the highest reported to date for ZnS:Mn d-dots via the direct aqueous synthetic method. Their optical features and structure have been characterized by UV-Visible spectroscopy, photoluminescence (PL) spectroscopy, transmission electron microscopy (TEM) and X-ray diffraction (XRD) in detail. Additionally, the stability study against UV irradiation indicated that the obtained d-dots possess excellent photostability. Furthermore, the MTT assay demonstrated that the ZnS:Mn QDs do not exhibit any cytotoxicity toward HeLa cells up to a concentration of 600 μg mL−1. Using the Con A-mannose recognition system as a model, Con A functionalized ZnS:Mn/ZnS nanocrystals were prepared and successfully used for targeted mannosyl groups expression on the HeLa cells surface. Our investigation clearly shows that the GSH capped ZnS:Mn QDs are promising candidates as biological fluorescent labels.
Co-reporter:Dong Zhu, Wei Li, Hong-Mei Wen, Jian-Rong Zhang and Jun-Jie Zhu
Analytical Methods 2013 vol. 5(Issue 17) pp:4321-4324
Publication Date(Web):02 Jul 2013
DOI:10.1039/C3AY40907D
The improvement of analytical accuracy and S/N (signal to noise ratio) based on conventional homogeneous fluorometry was always limited because of high background noise from complicated sample ingredients, buffer solution and lysates. Herein, a self-assembled Mn-doped ZnSe quantum dot–methyl viologen nanohybrid as an OFF–ON fluorescent probe is presented for the time-resolved fluorescence detection of tiopronin, showing high S/N and selectivity with a low detection limit of 0.1 μmol L−1 and a linear response ranging from 4 to 160 μM. We anticipate that this probe will have promising applications for sensitive biosensing and drug analysis.
Co-reporter:Hong-Ying LIU, Jun-Jie ZHU
Chinese Journal of Analytical Chemistry 2013 Volume 41(Issue 5) pp:658-663
Publication Date(Web):May 2013
DOI:10.1016/S1872-2040(13)60646-5
Co-reporter:Yong Kong, Juan Li, Shun Wu, Wen Cheng, Rohit Kumar Rana, Jun-Jie Zhu
Sensors and Actuators B: Chemical 2013 Volume 183() pp:187-193
Publication Date(Web):5 July 2013
DOI:10.1016/j.snb.2013.03.139
The detection of human enterovirus 71 (EV 71), an important etiological agent of foot, hand and mouth disease, by a hybrid voltammetric immunosensor was proposed in this paper for the first time. Poly(o-phenylenediamine) (PoPD) film was formed on a glassy carbon electrode (GCE) by utilizing electropolymerization, which yielded an interface with amino groups for the subsequent assembly of gold nanoparticles (AuNPs). The electrochemical characteristics of the immunosensor were investigated by cyclic voltammetry (CV). The parameters influencing the performance of the resulting immunosensor were studied in detail. The current response of the proposed immunosensor decreased linearly in the EV 71 concentration range from 0.1 to 80 ng mL−1 with a detection limit of 0.04 ng mL−1 (signal-to-noise ratio of 3). Due to its simple preparation, good reproducibility and long-time stability, the proposed voltammetric immunosensor will be promising in the point-of-care diagnostics application of clinical screening of multiple diseases.
Co-reporter:Dong Sun;Li Jin;Yun Chen; Jian-Rong Zhang; Jun-Jie Zhu
ChemPlusChem 2013 Volume 78( Issue 3) pp:227-234
Publication Date(Web):
DOI:10.1002/cplu.201200206
Abstract
A graphene/poly(3,4-ethylenedioxythiophene) (G/PEDOT) hybrid was prepared by the in situ polymerization of 3,4-ethylenedioxythiophene using the precursor of graphene, graphene oxide, as an oxidant under microwave heating. The G/PEDOT hybrid was characterized by ultraviolet–visible absorption spectroscopy, Fourier transform infrared spectroscopy, atomic force microscopy, X-ray photoelectron spectroscopy, field-emission scanning electron microscopy, energy-dispersive X-ray spectroscopy, and electrochemical impedance spectroscopy. The electrochemical properties of G/PEDOT hybrid electrodes were investigated by cyclic voltammetry and galvanostatic charge–discharge measurements. The G/PEDOT hybrid as a supercapacitor electrode material afforded high specific capacitance and good cycling stability (93 % retention after 10 000 cycles at a high current density of 5 A g−1) during the charge–discharge process. A maximum specific capacitance as high as 270 F g−1 at a current density of 1 A g−1 was achieved in 1 M H2SO4 electrolyte solution. In addition, the energy density of the G/PEDOT hybrid reached 34 W h kg−1 at a power density of 25 kW kg−1.
Co-reporter:Ying Wang;Cui-e Zhao;Dong Sun; Jian-Rong Zhang; Jun-Jie Zhu
ChemPlusChem 2013 Volume 78( Issue 8) pp:823-829
Publication Date(Web):
DOI:10.1002/cplu.201300102
Abstract
A microbial fuel cell (MFC) is an innovative power-output device, which utilizes microorganisms to metabolize fuel and transfers electrons to the electrode surface. In this study, we decorated the surface of graphene (G) with a conducting polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), through galvanostatic electropolymerization to fabricate a G/PEDOT hybrid anode for an Escherichia coli MFC. Cyclic voltammetry and electrochemical impedance spectroscopy analyses illustrated that the G/PEDOT hybrid anode possesses a larger active surface area and lower charge-transfer resistance than three other kinds of anodes, namely, carbon paper (CP), graphene-modified carbon paper (CP/G), and PEDOT-modified carbon paper (CP/PEDOT). Scanning electron microscopy was used to investigate the bacteria growth on the four anodes. A compact biofilm was formed on the hybrid anode owing to the electrostatic interaction between the negatively charged bacteria and positively charged PEDOT backbone. The constant-load (1 KΩ) discharge curves of MFCs with CP, CP/G, CP/PEDOT, and G/PEDOT anodes revealed that the G/PEDOT electrode had good stability and high voltage output. The G/PEDOT anode generated a maximum power density of 873 mW m−2, which is about 15 times higher than that of CP (55 mW m−2) in an H-shaped dual-chamber MFC. All the experimental results suggest that the performance of the G/PEDOT hybrid anode is superior to the CP, CP/G, or CP/PEDOT anode.
Co-reporter:Dr. Yong-Jie Li;Meng-Jie Ma;Dr. Gui Yin;Dr. Yong Kong; Jun-Jie Zhu
Chemistry - A European Journal 2013 Volume 19( Issue 14) pp:4496-4505
Publication Date(Web):
DOI:10.1002/chem.201203521
Abstract
A novel strategy is developed for the fabrication of graphene–CdS (G–CdS) nanocomposites by in situ growth of CdS nanoparticles onto simultaneously reduced graphite oxide, which is noncovalently functionalized by sodium 1-pyrene sulfonate through strong π–π stacking interactions. Subsequently, cobalt 2,9,16,23-tetraaminophthalocyanine (CoTAPc) is self-assembled on the G–CdS nanocomposites through electrostatic interactions to produce phthalocyanine-sensitized G–CdS nanocomposites. The photoactive superstructure enhances the photocurrent generation capability, and presents an efficient photoelectrochemical immunosensing platform for the ultrasensitive detection of the prostate-specific antigen (PSA). The quantitative measurement of PSA is based on the decrease in the photocurrent intensity of the phthalocyanine-sensitized G–CdS nanocomposites, which results from an increase in the steric hindrance due to the formation of the immunocomplex. A linear relationship between the photocurrent decrease and the PSA concentration is obtained in the wide range from 1 pg mL−1 to 5 μg mL−1 with a detection limit of 0.63 pg mL−1. The proposed sensor shows high sensitivity, stability, reproducibility, and can become a promising platform for other biomolecular detection.
Co-reporter:Feng Lu;Shanhu Liu;Li-Ping Jiang
Journal of Nanoparticle Research 2013 Volume 15( Issue 1) pp:
Publication Date(Web):2013 January
DOI:10.1007/s11051-012-1401-8
CdSexTe1-x semiconductor alloy nanotubes (with an external diameter of 140 nm and an internal diameter of 100 nm) were successfully prepared based on the sacrificial template of Cd(OH)Cl nanorods, and were further in situ assembled with gold nanoparticles (AuNPs) via a sonochemical approach to form the CdSexTe1−x/Au nanotubes. The prepared CdSexTe1−x/Au nanotubes were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, energy-dispersive spectrometry, and X-ray photoelectron spectra. CdSexTe1−x/Au nanotubes could integrate the advantages of the electronic properties of CdSeTe and the biocompatible properties of AuNPs. A novel biosensor was fabricated after the immobilization of hemoglobin (Hb) on CdSexTe1−x/Au nanotubes. The immobilized Hb exhibited fast direct electron transfer and good electrocatalytic performance to H2O2.
Co-reporter:Juan Peng, Wei Gao, Bipin Kumar Gupta, Zheng Liu, Rebeca Romero-Aburto, Liehui Ge, Li Song, Lawrence B. Alemany, Xiaobo Zhan, Guanhui Gao, Sajna Antony Vithayathil, Benny Abraham Kaipparettu, Angel A. Marti, Takuya Hayashi, Jun-Jie Zhu, and Pulickel M. Ajayan
Nano Letters 2012 Volume 12(Issue 2) pp:844-849
Publication Date(Web):January 4, 2012
DOI:10.1021/nl2038979
Graphene quantum dots (GQDs), which are edge-bound nanometer-size graphene pieces, have fascinating optical and electronic properties. These have been synthesized either by nanolithography or from starting materials such as graphene oxide (GO) by the chemical breakdown of their extended planar structure, both of which are multistep tedious processes. Here, we report that during the acid treatment and chemical exfoliation of traditional pitch-based carbon fibers, that are both cheap and commercially available, the stacked graphitic submicrometer domains of the fibers are easily broken down, leading to the creation of GQDs with different size distribution in scalable amounts. The as-produced GQDs, in the size range of 1–4 nm, show two-dimensional morphology, most of which present zigzag edge structure, and are 1–3 atomic layers thick. The photoluminescence of the GQDs can be tailored through varying the size of the GQDs by changing process parameters. Due to the luminescence stability, nanosecond lifetime, biocompatibility, low toxicity, and high water solubility, these GQDs are demonstrated to be excellent probes for high contrast bioimaging and biosensing applications.
Co-reporter:Ling-Ling Li;Jing Ji;Rong Fei;Chong-Zhi Wang;Qian Lu;Jian-Rong Zhang;Li-Ping Jiang
Advanced Functional Materials 2012 Volume 22( Issue 14) pp:2971-2979
Publication Date(Web):
DOI:10.1002/adfm.201200166
Abstract
With the assistance of microwave irradiation, greenish-yellow luminescent graphene quantum dots (gGQDs) with a quantum yield (QY) up to 11.7% are successfully prepared via cleaving graphene oxide (GO) under acid conditions. The cleaving and reduction processes are accomplished simultaneously using microwave treatment without additional reducing agent. When the gGQDs are further reduced with NaBH4, bright blue luminescent graphene quantum dots (bGQDs) are obtained with a QY as high as 22.9%. Both GQDs show well-known excitation-dependent PL behavior, which could be ascribed to the transition from the lowest unoccupied molecular orbital (LUMO) to the highest occupied molecular orbital (HOMO) with a carbene-like triplet ground state. Electrochemiluminescence (ECL) is observed from the graphene quantum dots for the first time, suggesting promising applications in ECL biosensing and imaging. The ECL mechanism is investigated in detail. Furthermore, a novel sensor for Cd2+ is proposed based on Cd2+ induced ECL quenching with cysteine (Cys) as the masking agent.
Co-reporter:Yuanyuan Shen, Lingling Li, Qian Lu, Jing Ji, Rong Fei, Jianrong Zhang, E. S. Abdel-Halim and Jun-Jie Zhu
Chemical Communications 2012 vol. 48(Issue 16) pp:2222-2224
Publication Date(Web):03 Jan 2012
DOI:10.1039/C2CC16329B
Highly luminescent and low toxic glutathione-capped CdSeTe@ZnS–SiO2 quantum dots were successfully synthesized via a promising microwave strategy, and then applied in the detection of Cu2+.
Co-reporter:Jingjing Li, Xiaoqin Zhong, Fangfang Cheng, Jian-Rong Zhang, Li-Ping Jiang, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 9) pp:4140
Publication Date(Web):April 7, 2012
DOI:10.1021/ac3003402
As an emerging category of fluorescent metal nanoclusters, oligonucleotide-templated silver nanoclusters (Ag NCs) have attracted a lot of interest and have shown wide application in biorelated disciplines. However, the weak fluorescence emission and poor permeability to cell membranes tethered further intracellular applications of Ag NCs. AS1411 is an antiproliferative G-rich phosphodiester oligonucleotide and currently an anticancer agent under phase II clinical trials. Herein, we present a strategy to synthesize AS1411-functionalized Ag NCs with excellent fluorescence through a facile one-pot process. Confocal laser scanning microscopy and Z-axis scanning confirmed that the AS1411-functionalized Ag NCs could be internalized into MCF-7 human breast cancer cells and were able to specifically stain nuclei with red color. To our surprise, 3-[4,5-dimethylthiazol-z-yl]-2,5-diphenyltetrazolium bromide (MTT) assay demonstrated the Ag NCs were cytocompatible and showed better inhibition effects than pure AS1411 on MCF-7 human breast cancer cells. In addition, a universal design of the oligonucleotide scaffold for synthesis of Ag NCs was extended to other aptamers, such as Sgc8c and mucin 1 aptamer. Due to the facile synthesis procedure and capability of specific target recognition, this fluorescent platform will potentially broaden the applications of Ag NCs in biosensing and biological imaging.
Co-reporter:Jingjing Li, Xiaoqin Zhong, Hongquan Zhang, X. Chris Le, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 12) pp:5170
Publication Date(Web):May 15, 2012
DOI:10.1021/ac3006268
We present here a binding-induced fluorescence turn-on assay for protein detection. Key features of this assay include affinity binding-induced DNA hybridization and fluorescence enhancement of silver nanoclusters (Ag NCs) using guanine-rich DNA sequences. In an example of an assay for human α-thrombin, two aptamers (Apt15 and Apt29) were used and were modified by including additional sequence elements. A 12-nucleotide (nt) sequence was used to link the first aptamer with a nanocluster nucleation sequence at the 5′-end. The second aptamer was linked through a complementary sequence (12-nt) to a G-rich overhang at the 3′-end. Binding of the two aptamer probes to the target protein initiates hybridization between the complementary linker sequences attached to each aptamer and thereby bring the end of the G-rich overhang to close proximity to Ag NCs, resulting in a significant fluorescence enhancement. With this approach, a detection limit of 1 nM and a linear dynamic range of 5 nM–2 μM were achieved for human α-thrombin. This fluorescence assay is performed in a single tube, and it does not require washing or separation steps. The principle of the binding-induced DNA hybridization and fluorescence enhancement of Ag NCs can be extended to other homogeneous assay applications provided that two appropriate probes are available to bind with the same target molecule.
Co-reporter:Jun-Tao Cao, Xiao-Yao Hao, Ying-Di Zhu, Ken Sun, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 15) pp:6775
Publication Date(Web):July 16, 2012
DOI:10.1021/ac3013048
A microfluidic platform to evaluate the expression of multi-glycans on a cell surface was developed using electrochemical impedance spectroscopy (EIS) and optical microscope technique. In the microfluidic channel, four indium tin oxide (ITO) electrodes were modified with three lectins and one passivation agent, respectively, to selectively recognize the corresponding carbohydrate epitopes on the cell surface. The binding of the cells on the electrode array was monitored by the electrochemical impedance to evaluate the expression of cell surface glycans. The excellent optical transparency of ITO electrode permitted the microscopic observation of the cell binding simultaneously to substantiate the impedance measurement. Compared with the individual technology, the double-check mode increased the sensitivity and accuracy of the assay. The experimental results using these two techniques indicated that the cell binding ability decreased in the order WGA > Con A > PNA, which was consistent with the expression difference of carbohydrate epitopes on K562 cell surface. The proposed strategy was further used for facile evaluating the variations of glycan expression on living cells in response to drugs. The consumption of cell sample for each sensing interface in the whole experiments is merely 5 × 103 cells. This platform offers great promise for cancer-associated glycol-biomarkers screening and further helps cancer diagnosis and treatment.
Co-reporter:Li-Na Feng, Zhi-Ping Bian, Juan Peng, Fang Jiang, Guo-Hai Yang, Ying-Di Zhu, Di Yang, Li-Ping Jiang, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 18) pp:7810
Publication Date(Web):August 22, 2012
DOI:10.1021/ac301438v
A novel multianalyte electrochemical immunoassay was developed for ultrasensitive detection of human cardiopathy biomarkers cardiac troponin I (cTnI) and human heart-type fatty-acid-binding protein (FABP) using metal ion functionalized titanium phosphate nanospheres (TiP-metal ion) as labels. The metal ions could be detected directly through square wave voltammetry (SWV) without metal preconcentration, and the distinct voltammetric peaks had a close relationship with each sandwich-type immunoreaction. The position and size of the peaks reflected the identity and level of the corresponding antigen. The large amount of metal ions loading on the TiP nanospheres greatly amplified the detection signals, and the good biocompatibility of graphene nanoribbons (GONRs) retained good stability for the sandwich-type immunoassay. The proposed immunoassay exhibited high sensitivity and selectivity for the detection of cTnI and FABP. The linear relationships between electrochemical signals and the concentrations of cTnI and FABP were obtained in the range of 0.05 pg/mL–50 ng/mL and 0.05 pg/mL–50 ng/mL, respectively. The detection limits of cTnI and HIgG were 1 and 3 fg/mL (S/N = 3), respectively. Moreover, the immunoassay accurately detected the concentrations of cTnI and FABP in human serum samples, which were demonstrated to have excellent correlations with the standard enzyme linked immunosorbent assay (ELISA) method. The results suggested that the electrochemical immunoassay would be promising in the point-of-care diagnostics application of clinical screening of acute myocardial infarction (AMI) biomarkers.
Co-reporter:Jun-Tao Cao, Zi-Xuan Chen, Xiao-Yao Hao, Peng-Hui Zhang, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 22) pp:10097
Publication Date(Web):October 19, 2012
DOI:10.1021/ac302609y
Rich high-quality single-cell information from rare cell sample is very important for the quantitative systems biology description of cellular function. However, this type of data is often prohibited by the conventional analytical technology such as flow cytometry. In this paper, we described a microfluidic platform coupled with a quantum dots-based (QDs) immunofluorescence (IF) approach to measure the expression of glycans on the cell surface of single cells or cell population. Compared with conventional IF staining, the QDs-based IF probe exhibited higher brightness and stability against photobleaching. With the merits of the novel IF staining protocol and microfluidic platform, high-throughput IF staining was performed to measure the glycan expressions and the changes at single K562 cells after drug treatment. The protocol proposed here showed a high sensitivity on the glycan expression profile owing to the amplification of the signal in indirect IF staining. The size of cell sample was only 4 × 103 cells, which made the rare cell sample analysis accessible. This method may find widespread application for assessing cell-surface glycoprotein expression as well as analysis of the heterogeneity in cell populations in a high-throughput manner.
Co-reporter:Yong-Jie Li, Meng-Jie Ma, and Jun-Jie Zhu
Analytical Chemistry 2012 Volume 84(Issue 23) pp:10492
Publication Date(Web):November 9, 2012
DOI:10.1021/ac302853y
An ultrasensitive photoelectrochemical immunoassay of cancer biomarker α-fetoprotein (AFP) is proposed that uses titanium dioxide (TiO2) coupled with AFP–CdTe–GOx bioconjugate, which featured AFP antigen and glucose oxidase (GOx) labels linked to CdTe quantum dots (QDs) for signal amplification. The synthesized CdTe QDs yielded a homogeneous and narrow size distribution, which allowed the binding of AFP and GOx on CdTe QDs. Greatly enhanced sensitivity for AFP came from a dual signal amplification strategy. First, an effective matching of energy levels between the conduction bands of CdTe QDs and TiO2 allowed for fast electron injection from excited CdTe QDs to TiO2 upon irradiation, which reduced the recombination process of electron–hole pairs and prompted photoelectrochemical performance. Second, GOx enzyme could catalyze glucose to produce H2O2, which acted as a sacrificial electron donor to scavenge the photogenerated holes in the valence band of CdTe QDs, further causing an enhanced photocurrent. Thus, on the basis of the dual signal amplification strategy, the competitive immunosensor based on the specific binding of anti-AFP antibodies to AFP and AFP–CdTe–GOx bioconjugates was achieved. This proposed biosensor for AFP possessed largely increased linear detection range from 0.5 pg/mL to 10 μg/mL with a detection limit of 0.13 pg/mL. The proposed amplification strategy shows high sensitivity, stability, and reproducibility and can become a promising platform for other protein detection.
Co-reporter:Jian-Jun Shi, Yi-Jun Wang, Yue Ma, Qing-Ming Shen, Jun-Jie Zhu
Ultrasonics Sonochemistry 2012 Volume 19(Issue 5) pp:1039-1043
Publication Date(Web):September 2012
DOI:10.1016/j.ultsonch.2012.03.001
Bismuth-based nanostructures have attracted growing interest because of their promising thermoelectric properties and applications in optics and electronics. Pulsed sonoelectrochemical technique was selected to fabricate bismuth–antimony (BiSb) flake-like alloy in ethylene glycol aqueous solution. The formation mechanism for the BiSb alloy was discussed. Ultrasonic played an important role in regenerating electrode and promoting the formation of BiSb nanoflakes. Citrate and polyvinylpyrrolidone (PVP) were introduced as mixed controlling agents during the nucleation and growth process.Graphical abstract.Highlights► Pulsed sonoelectrochemical technique was used to synthesize and assemble BiSb alloy nanoflakes. ► PVP and citrate were employed as mixed controlling agents during the nucleation and growth process. ► Ultrasonic played an important role in regenerating electrode and promoting the formation of BiSb nanoflakes.
Co-reporter:Ting-Ting Zheng, Rui Zhang, Lanfang Zou and Jun-Jie Zhu
Analyst 2012 vol. 137(Issue 6) pp:1316-1318
Publication Date(Web):06 Dec 2011
DOI:10.1039/C2AN16023D
An electrochemical, label-free method was developed to detect folate receptor positive tumor cells by specific recognition of a polydopamine-coated carbon nanotubes–folate nanoprobe to cell-surface folate receptors. This strategy offers great promise to extend its application in studying the interaction of ligand and cell-surface receptor.
Co-reporter:Xiaomei Zhao, Shiwei Zhou, Qingming Shen, Li-Ping Jiang and Jun-Jie Zhu
Analyst 2012 vol. 137(Issue 16) pp:3697-3703
Publication Date(Web):13 Jun 2012
DOI:10.1039/C2AN35658A
A novel glutathione (GSH) photoelectrochemical biosensor was fabricated using the newly synthesized graphene–CdS (GR–CdS) nanocomposites. The GR–CdS nanocomposites were prepared by a fast, one-step, aqueous reaction. The as-prepared GR–CdS structure inherited the excellent electron transport of GR and facilitated the spatial separation of photo-generated charge carrier, therefore resulting in the enhanced photocurrent, and making it a promising candidate for developing photoelectrochemical biosensors. The proposed GSH sensor displays satisfactory analytical performance with an acceptable linear range from 0.01 to 1.5 mmol L−1 with a detection limit of 0.003 mmol L−1 at a signal-to-noise ratio of 3, and also shows an excellent specificity against anticancer drugs and can be successfully applied for GSH detection in real samples. The as-synthesized GR–CdS nanocomposites exhibited obviously enhanced photovoltaic properties, which could be extended to the detection of other enzymes and biomolecules, thus providing a promising platform for the development of photoelectrochemical biosensors.
Co-reporter:Feng Lu, Tennyson L. Doane, Jun-Jie Zhu, Clemens Burda
Inorganica Chimica Acta 2012 Volume 393() pp:142-153
Publication Date(Web):1 December 2012
DOI:10.1016/j.ica.2012.05.038
Gold nanoparticles (Au NPs) provide a unique platform for biomedical applications. Au NP-based sensors have been widely employed to detect many different chemicals and disease-related biomolecules. Recent research on drug delivery and therapy with Au NPs has also indicated attractive and promising prospects for future applications. In this invited review we will provide an overview of the use of Au NPs for diagnostic sensing and therapy applications.Graphical abstractThis review provides a historical overview of the development of gold nanoparticle synthesis and highlights the recent progress in using gold nanoparticles for the applications in diagnostic sensing and therapy.Highlights► Historical overview of the development of gold nanoparticle synthesis and applications in the field of biomedicine. ► Concise summary of work on gold nanoparticle sensors from the initial work to current state of the art. ► Concise summary of work using gold nanoparticles for drug delivery and therapeutic applications. ► Short overview of the authors’ work in these areas.
Co-reporter:Yajun Ji, Mingdao Zhang, Jiehu Cui, Keng-Chu Lin, Hegen Zheng, Jun-Jie Zhu, Anna Cristina S. Samia
Nano Energy 2012 Volume 1(Issue 6) pp:796-804
Publication Date(Web):November 2012
DOI:10.1016/j.nanoen.2012.08.006
Dye-sensitized solar cells (DSSCs) based on free-standing, double-walled TiO2 nanotubes with bamboo-like morphology have been prepared by a sequence of alternating voltage and two-step anodization treatments. The combination of double-walled and bamboo-like morphologies led to an increase in dye loading and an improvement in photoconversion performance. Subsequently, the fabricated dye-sensitized nanotubes used to prepare DSSCs that operate in a frontside illumination mode yielded a significantly high power conversion efficiency of 3.46%, which was approximately two times higher than DSSCs that were fabricated using traditional single-walled TiO2 nanotube arrays with smooth surfaces. In addition, DSSCs fabricated from nanotubes with higher bamboo ring densities exhibited better conversion efficiencies than those prepared from nanotubes with lower bamboo ring densities. The improved conversion efficiency can be attributed to increased dye loading in the combined double-walled and bamboo-like titania nanostructures.Graphical abstractDye-sensitized solar cells (DSSCs) based on free-standing, double-walled TiO2 nanotubes with bamboo-like morphology have been prepared and investigated. The fabricated DSSCs exhibited a significantly high power conversion efficiency of 3.46%, which was approximately two times higher than DSSCs that were fabricated using traditional single-walled TiO2 nanotube arrays with smooth surfaces.Highlights► Titania nanotubes with double-walled/bamboo structures were used in solar cells. ► Solar cells from double-walled/bamboo nanotubes show good conversion efficiencies. ► The improved conversion efficiency is due to an increase in nanotube-dye loading.
Co-reporter:Jian-Jun Shi, Wei Hu, Dan Zhao, Ting-Ting He, Jun-Jie Zhu
Sensors and Actuators B: Chemical 2012 173() pp: 239-243
Publication Date(Web):
DOI:10.1016/j.snb.2012.06.091
Co-reporter:Jun Geng ; Guang-Hui Song ; Xiang-Dong Jia ; Fang-Fang Cheng
The Journal of Physical Chemistry C 2012 Volume 116(Issue 7) pp:4517-4525
Publication Date(Web):January 23, 2012
DOI:10.1021/jp212092h
Hollow doughnut-like ZnO/Au nanocomposites have been synthesized through a fast one-step microwave-assisted hydrothermal route. The formation mechanism of the product is closely connected with the coordination and selective adsorption effect of trisodium citrate (TSC). Other different structures, such as ZnO nanorods/Au nanoparticles, ZnO nanodisks/Au nanoparticles, and ZnO nanospheres/Au nanoparticles have also been obtained in control experiments. The UV–vis and photoluminescence properties of the as-prepared hollow structures with different Au concentrations showed tunable UV and visible emission intensity. The hollow ZnO/Au nanocomposites are photostable with a strong resonance Raman signal. The colorimetric 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl tetrazolium bromide (MTT) assays showed that ZnO/Au nanomaterials have low biological cytotoxicity on human colon cancer cells (LOVO cells) at the concentration of 50 μg/mL. The as-prepared ZnO/Au nanocomposites with good biocompatibility may have potential applications in biomedicine and biosensors.
Co-reporter:Xiaomei Zhao;Shiwei Zhou;Dr. Li-Ping Jiang; Wenhua Hou;Dr. Qingming Shen; Jun-Jie Zhu
Chemistry - A European Journal 2012 Volume 18( Issue 16) pp:4974-4981
Publication Date(Web):
DOI:10.1002/chem.201102379
Abstract
Graphene–CdS (GR–CdS) nanocomposites were prepared in a one-step synthesis in aqueous solution. The synthetic approach was simple and fast, and it may be extended for the synthesis of other GR–metal-sulfide nanocomposites. The as-prepared GR–CdS nanocomposite films inherited the excellent electron-transport properties of GR. In addition, the heteronanostructure of the GR–CdS nanocomposites facilitated the spatial separation of the charge carriers, thus resulting in enhanced photocurrent intensity, which makes it a promising candidate for photoelectrochemical applications. This strategy was used for the fabrication of an advanced photoelectrochemical cytosensor, based on these GR–CdS nanocomposites, by using a layer-by-layer assembly process. This photoelectrochemical cytosensor showed a good photoelectronic effect and cell-capture ability, and had a wide linear range and low detection limit for Hela cells. The as-synthesized GR–CdS nanocomposites exhibited obviously enhanced photovoltaic properties, which could be an efficient platform for many other high-performance photovoltaic devices.
Co-reporter:Ling-Ling Li;Kun-Ping Liu;Guo-Hai Yang;Chun-Ming Wang;Jian-Rong Zhang
Advanced Functional Materials 2011 Volume 21( Issue 5) pp:869-878
Publication Date(Web):
DOI:10.1002/adfm.201001550
Abstract
A novel strategy is reported for the fabrication of poly(diallyldimethylammonium chloride) (PDDA)-protected graphene–CdSe (P-GR-CdSe) composites. An advanced electrogenerated chemiluminescence (ECL) immunosensor is proposed for the sensitive detection of human IgG (HIgG) by using the as-prepared P-GR-CdSe composites. The P-GR-CdSe composite film shows high ECL intensity, good electronic conductivity, fast response, and satisfactory stability, all of which holds great promise for the fabrication of ECL biosensors with improved sensitivity. After two successive steps of amplification via the conjugation of PDDA and gold nanoparticles (GNPs) in the film, high ECL intensity is observed. The ECL immunosensor has an extremely sensitive response to HIgG in a linear range of 0.02–2000 pg mL−1 with a detection limit of 0.005 pg mL−1. The proposed sensor exhibits high specificity, good reproducibility, and long-term stability, and may become a promising technique for protein detection.
Co-reporter:Kunping Liu, Jing-Jing Zhang, Fang-Fang Cheng, Ting-Ting Zheng, Chunming Wang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 vol. 21(Issue 32) pp:12034-12040
Publication Date(Web):05 Jul 2011
DOI:10.1039/C1JM10749F
A green and facile method for the preparation of gelatin functionalized graphene nanosheets (gelatin–GNS) was reported by using gelatin as a reducing reagent. Meanwhile, the gelatin also played an important role as a functionalized reagent to prevent the aggregation of the graphene nanosheets. The obtained biocompatible gelatin–GNS exhibited excellent stability in water and various physiological fluids including, cellular growth media as well as serum which were critical prerequisites for biomedicine application of graphene. Cellular toxicity test suggested that the gelatin–GNS was nontoxic for MCF-7 cells, even at a high concentration of 200 μg mL−1. Furthermore, the anticancer drug was loaded onto the gelatin–GNS at a high loading capacity via physisorption for cellular imaging and drug delivery. The doxorubicin/gelatin–GNS composite exhibited a high toxicity to kill MCF-7 cells and experienced a gelatin-mediated sustained release in vitro, which has the potential advantage of increasing the therapeutic efficacy. Therefore, the gelatin–GNS could be selected as an ideal drug carrier to be applied in biomedicine studies.
Co-reporter:Jian-Jun Shi, Guo-Hai Yang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 vol. 21(Issue 20) pp:7343-7349
Publication Date(Web):07 Apr 2011
DOI:10.1039/C1JM10333D
Sonoelectrochemical technique was successfully used to fabricate alloy–graphene nanocomposites. It not only provides a simple way to synthesize alloy nanoparticles, but also shows a general strategy for fabricating graphene-based nanostructures with anticipated properties. Pd was co-electrodeposited with Pt at different atomic ratios, and then was anchored with reduced graphene oxide (RGO) simultaneously in the presence of PDDA. The morphologies and structures of the as-prepared PDDA-RGO-PdPt nanocomposites were extensively investigated by transmission electron microscopy (TEM), scanning electron microscopy (SEM), and X-ray diffraction (XRD). The composition was evaluated by energy dispersive X-ray spectrometry (EDS) and inductively coupled plasma–atomic emission spectroscopy (ICP-AES). Raman spectra revealed the surface properties of graphene and its interaction with metallic nanoparticles. Cyclic voltammetric (CV) and chronoamperometric experiments further exhibited their catalytic activity and stability for the electro-oxidation of ethanol in alkaline media, which could be applied as promising electrocatalysts for direct alcohol fuel cells (DAFCs).
Co-reporter:Yun Chen, Yang Li, Dong Sun, Danbi Tian, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 vol. 21(Issue 21) pp:7604-7611
Publication Date(Web):08 Apr 2011
DOI:10.1039/C1JM10293A
The hydrophilic and carboxyl group functionalized graphene–gold nanoparticles (AuNPs) hybrid has been synthesized in situ. AuNPs can be scattered well on the graphene bilayer, and the loading amount of AuNPs can be controlled. Glucose oxidase (GOD) was successfully bound to the surface of the hybrid through a condensation reaction between terminal amino groups on the lysine residues of GOD and carboxyl groups on the AuNPs. The hybrid provided a suitable microenvironment for GOD to retain its biological activity. The direct and reversible electron transfer process between GOD and the hybrid electrode was realized without any supporting film or electron mediator. A novel model of the glucose biosensor based on the hybrid electrode was fabricated. Blood sugar concentrations measured in human serum samples by the glucose biosensor were in good agreement with the values provided by the Nanjing University hospital, and the average relative standard deviation was 3.2% for six successive measurements. Three constructed biosensors showed good stability, and all of them retained 80% of their initial signals after they were stored at 4 °C for four months. It is promising that the model of the glucose biosensor can be used as an effective candidate for the detection of blood sugar concentration in clinical diagnoses.
Co-reporter:Shanhu Liu, Feng Lu and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 9) pp:2661-2663
Publication Date(Web):12 Jan 2011
DOI:10.1039/C0CC04276E
Highly fluorescent Ag nanoclusters were prepared in aqueous solution via a rapid microwave-assisted green approach and used as a novel fluorescence probe for the determination of Cr3+ ions with high sensitivity and excellent selectivity.
Co-reporter:Yun Chen, Yuanyuan Shen, Dong Sun, Hongyi Zhang, Danbi Tian, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 42) pp:11733-11735
Publication Date(Web):26 Aug 2011
DOI:10.1039/C1CC13852A
A dispersible graphene/gold nanoclusters hybrid in aqueous solution was fabricated in situ based on the bilayer graphene template, and its electrogenerated chemiluminescence (ECL) behavior was studied.
Co-reporter:Qianhao Min, Xiaoxia Zhang, Hongyi Zhang, Fang Zhou and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 42) pp:11709-11711
Publication Date(Web):27 Sep 2011
DOI:10.1039/C1CC15151G
Fe3O4–graphene–TiO2 ternary composite networks were first synthesized, which exhibited high selectivity and capacity in the capture of phosphopeptides, due to the enhanced contact to phosphopeptides given by the graphene scaffold.
Co-reporter:Qianhao Min, Xiaoxia Zhang, Ren'an Wu, Hanfa Zou and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 38) pp:10725-10727
Publication Date(Web):24 Aug 2011
DOI:10.1039/C1CC13969J
Magnetic mesoporous silica with a magnetic cover and mesoporous core was synthesized, filled with trypsin and located in an S-shaped microfluidic reactor. High-molecular weight (MW) proteins were split to waste by fractionation, whilst low-MW proteins were retained on the chip to be digested.
Co-reporter:Jing-Jing Zhang, Yan Liu, Li-Hui Hu, Li-Ping Jiang and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 23) pp:6551-6553
Publication Date(Web):06 May 2011
DOI:10.1039/C1CC11565K
The proof-of-principle of the integration of electrically heated carbon paste electrode with immunoassay as a potential alternative for ultrasensitive detection of cytokines was demonstrated.
Co-reporter:Hongying Liu, Xiang Zhang, Ximei Wu, Liping Jiang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 14) pp:4237-4239
Publication Date(Web):25 Feb 2011
DOI:10.1039/C1CC00103E
Highly fluorescent and water-soluble gold nanoclusters (AuNCs) with near-infrared-emission and Au@AgNCs with yellow-emission were successfully prepared via a rapid sonochemical approach, and the as-prepared AuNCs could be applied in the determination of Cu2+ with a wider detection range and lower detection limit.
Co-reporter:Jing-Jing Zhang, Ting-Ting Zheng, Fang-Fang Cheng and Jun-Jie Zhu
Chemical Communications 2011 vol. 47(Issue 4) pp:1178-1180
Publication Date(Web):12 Nov 2010
DOI:10.1039/C0CC03494K
A novel electrochemical sensing platform for sensitive determination of caspase 3 activity and inhibition was developed by combining the site-specific recognition and cleavage of the DEVD-peptide with quantum dots as signal amplification.
Co-reporter:Jing-Jing Zhang, Ting-Ting Zheng, Fang-Fang Cheng, Jian-Rong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2011 Volume 83(Issue 20) pp:7902
Publication Date(Web):September 4, 2011
DOI:10.1021/ac201804b
The ability for early evaluation of therapeutic effects is a significant challenge in leukemia research. To address this challenge, we developed a novel electrochemical platform for ultrasensitive and selective detection of apoptotic cells in response to therapy. In order to construct the platform, a novel three-dimensional (3-D) architecture was initially fabricated after combining nitrogen-doped carbon nanotubes and gold nanoparticles via a layer-by-layer method. The formed architecture provided an effective matrix for annexin V with high stability and bioactivity to enhance sensitivity. On the basis of the specific recognition between annexin V and phosphatidylserine on the apoptotic cell membrane, the annexin V/3-D architecture interface showed a predominant capability for apoptotic cell capture. Moreover, a lectin-based nanoprobe was designed by noncovalent assembly of concanavalin A on CdTe quantum dots (QDs)-labeled silica nanospheres with poly(allylamine hydrochloride) as a linker. This nanoprobe incorporated both the specific carbohydrate recognition and the multilabeled QDs-based signal amplification. By coupling with the QDs-based nanoprobe and electrochemical stripping analysis, the proposed sandwich-type cytosensor showed an excellent analytical performance for the ultrasensitive detection of apoptotic cells (as low as 48 cells), revealing great potential toward the early evaluation of therapeutic effects.
Co-reporter:Dong Zhu, Yun Chen, Liping Jiang, Jun Geng, Jianrong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2011 Volume 83(Issue 23) pp:9076
Publication Date(Web):October 26, 2011
DOI:10.1021/ac202101u
Quantum dots (QDs) are generally used for the conventional fluorescence detection. However, it is difficult for the QDs to be applied in time-resolved fluorometry due to their short-lived emission. In this paper, high-quality Mn-doped ZnSe QDs with long-lived emission were prepared using a green and rapid microwave-assisted synthetic approach in aqueous solution. Fluorescence lifetime of the Mn-doped ZnSe QDs was extended as long as 400 μs, which was 10 000 times higher than that of conventional QDs such as CdS, CdSe, and CdTe. The QDs exhibited an excellent photostability over 35 h under continuous irradiation at 260 nm. Capped with mercaptopropionic acid (MPA), the Mn-doped ZnSe QDs were used for the time-resolved fluorescence detection of 5-fluorouracil (5-FU) with the detection limit of 128 nM. The relative standard deviation for seven independent measurements of 1.5 μM 5-FU was 3.8%, and the recovery ranged from 93% to 106%. The results revealed that the Mn-doped ZnSe QDs could be a good candidate as a luminescence probe for highly sensitive time-resolved fluorometry.
Co-reporter:Lingling Li, Hongying Liu, Yuanyuan Shen, Jianrong Zhang, and Jun-Jie Zhu
Analytical Chemistry 2011 Volume 83(Issue 3) pp:661
Publication Date(Web):January 12, 2011
DOI:10.1021/ac102623r
Electrogenerated chemiluminescence (ECL) emission was observed from the water-soluble, bovine serum albumin (BSA)-stabilized Au nanoclusters for the first time. The possible ECL mechanism was discussed according to the presented results and ascribed to the effective electron transfer from the conduction-band of excited indium tin oxide (ITO) to Au nanoclusters (NCs). A simple label-free method for the detection of dopamine has been developed based on the Au NCs ECL in aqueous media. The Au NCs could be an effective candidate for new types of ECL biosensors in the future due to their fascinating features, such as good water solubility, low toxicity, ease of labeling, and excellent stability.
Co-reporter:Jian-Jun Shi, Jun-Jie Zhu
Electrochimica Acta 2011 Volume 56(Issue 17) pp:6008-6013
Publication Date(Web):1 July 2011
DOI:10.1016/j.electacta.2011.04.099
A novel electrochemical sensor for chlorophenols was fabricated by using the Pd-graphene nanocomposite and ions liquid. The Pd-graphene nanocomposite was prepared via a sonoelectrochemical route, and the possible formation mechanism was proposed. Transmission electron microscopy, scanning electron microscopy, X-ray diffraction and Raman spectrum were used for the characterization of structure and morphology of the nanocomposite. The experimental results showed that Pd nanospheres comprised of small Pd nanoparticles were uniformly attached on graphene sheets. The electrocatalytic properties were investigated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV), which indicated that the Pd-graphene nanocomposite had high activity for chlorophenol oxidation. Herein, 2-chlorophenol was selected as the model molecules. The results showed that graphene played an important role in the fabrication of the chlorophenols sensor. The nanocomposite with large electrochemical active surface led to the excellent electrocatalytic activity, and ionic liquid further enhanced the catalytic activity of Pd-graphene for chlorophenols.Highlights► A novel nanocomposite with 3D Pd NPs on the graphene was fabricated via sonoelectrochemistry. ► The Pd-graphene nanocomposite had high electrocatalytic activity for chlorophenols oxidation. ► An electrochemical sensor for chlorophenols was constructed. ► Ionic liquid was chosen as linker to show an enhanced effect on the electrocatalysis.
Co-reporter:Rongjing Cui, Zhida Han, Jie Pan, E.S. Abdel-Halim, Jun-Jie Zhu
Electrochimica Acta 2011 Volume 58() pp:179-183
Publication Date(Web):30 December 2011
DOI:10.1016/j.electacta.2011.09.030
Poly(diallyldimethylammonium chloride) functionalized helical carbon nanotubes (PDDA-HCNTs) were successfully synthesized. The resulting PDDA-HCNTs composite has good conductivity, solubility and ferromagnetic property. The fabricated HCNTs could be conveniently separated and magnetically attached to the magnetic electrode owing to their excellent magnetic properties. An amperometric biosensor was firstly developed based on glucose oxidase (GOD) functionalized PDDA-HCNTs loaded on magnetic glass carbon electrode. The constructed biosensor exhibited excellent electrocatalytic activity and stability for the detection of glucose with a linear range from 5 to 85 μM and a low detection limit of 0.72 μM at 3σ. The present work offers a new avenue to broaden the applications of HCNTs in electrochemical biosensors.
Co-reporter:Qingming Shen, Qianhao Min, Jianjun Shi, Liping Jiang, Wenhua Hou, Jun-Jie Zhu
Ultrasonics Sonochemistry 2011 Volume 18(Issue 1) pp:231-237
Publication Date(Web):January 2011
DOI:10.1016/j.ultsonch.2010.05.011
In this paper, stabilizer-free gold nanoparticles (Au NPs) were synthesized by a facile pulse sonoelectrochemical method in the absence of stabilizer. The size and shape of the Au NPs can be controlled by adjusting current density, reaction time and the pH value of the precursor solution. The morphology and structure of the Au NPs were characterized by transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), UV–visable spectra (UV–vis), energy-dispersive X-ray (EDX) and X-ray diffraction (XRD). The pH value has a great effect on the size and dispersion of the obtained Au NPs. The Au NPs could further used as substrate for fabrication of HRP biosensor which exhibited excellent biocatalytical activity with high sensitivity and rapid response. This method provides a facile route for the synthesis of stabilizer-free Au NPs. Since the preparation process do not need the addition of any surfactants/capping agent, the resulting Au NPs are suitable for the applications in fields of biology and catalysis.
Co-reporter:Shanhu Liu, Feng Lu, Xiangdong Jia, Fangfang Cheng, Li-Ping Jiang and Jun-Jie Zhu
CrystEngComm 2011 vol. 13(Issue 7) pp:2425-2429
Publication Date(Web):01 Feb 2011
DOI:10.1039/C0CE00491J
A rapid microwave-assisted method was developed for the facile synthesis of a polyacid-conjugated Fe3O4 superparamagnetic hybrid. Field-emission scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, thermogravimetric and magnetic measurements, and a cytotoxicity assay were used to characterize the morphologies, structures, compositions and properties of the polyacid-conjugated Fe3O4 superparamagnetic hybrid. The hybrid is composed of superparamagnetic magnetite nanograins and presents a cluster-like structure; and its size range can be tuned from about 100 to 400 nm by varying the amount of FeCl3 in the system. The hybrid not only exhibits excellent magnetic properties, good biocompatibility, and high water-dispersibility, but also facilitates further coupling interaction with some guest molecules because of the abundant existence of uncoordinated carboxylate groups on its surface.
Co-reporter:Jun Geng, Xiang-Dong Jia and Jun-Jie Zhu
CrystEngComm 2011 vol. 13(Issue 1) pp:193-198
Publication Date(Web):27 Aug 2010
DOI:10.1039/C0CE00180E
The core/shell-type ZnO nanosphere/CdS nanorod and ZnO nanosphere/CdS nanoparticle composites have been selectively prepared through a simple ultrasound-assisted solution phase conversion process using monodispersed ZnO nanospheres as a starting reactant and in situ template. The formation mechanism of the products is closely connected with the sonochemical effect of ultrasonic irradiation. The photoluminescence and electrogenerated chemiluminescence properties of the as-prepared core/shell structures were investigated.
Co-reporter:Ke-Jing Huang, De-Jun Niu, Jun-Yong Sun, Jun-Jie Zhu
Journal of Electroanalytical Chemistry 2011 Volume 656(1–2) pp:72-77
Publication Date(Web):15 June 2011
DOI:10.1016/j.jelechem.2011.01.007
A sensitive label-free amperometric immunosensor was developed based on the amine-functionalized graphene (GR-NH2) and gold nanoparticles (AuNPs) composite modified carbon ionic liquid electrode (CILE). CILE was fabricated by using an ionic liquid of 1-octyl-3-methylimidazolium hexafluorophosphate as binder. The nanocomposite AuNPs/GR-NH2 had prominent biocompatibility, good electron transfer ability, large specific surface area, and primarily excellent adsorption. The negatively charged AuNPs could be adsorbed on the positively charged GR-NH2 modified CILE surface by electrostatic adsorption, and then to immobilize α-fetoprotein antibody (anti-AFP) for the assay of α-fetoprotein (AFP). The fabricated procedures and electrochemical behaviors of the immunosensor were characterized by electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The anti-AFP/AuNPs/GR-NH2 modified CILE was sensitive to AFP in linear relation between 1 and 250 ng mL−1 with the correlation coefficient of 0.995, and the detection limit (S/N = 3) was 0.1 ng mL−1 under the optimal conditions. In addition, the proposed immunosensor exhibited good sensitivity, selectivity, stability and long-term maintenance of bioactivity and it may be used to immobilize other biomoleculars to develop biosensor for the detection of other antigens or biocompounds.
Co-reporter:Qi-Xiu Gao, Xiao-Fang Wang, Xing-Cai Wu, You-Rong Tao, Jun-Jie Zhu
Microporous and Mesoporous Materials 2011 Volume 143(2–3) pp:333-340
Publication Date(Web):September 2011
DOI:10.1016/j.micromeso.2011.03.019
Mesoporous ZrO2 nanobelts (MZNs) have been prepared by a calcination route of ZrS3 nanobelts in air. The nanobelts prepared at 400–600 °C are the mixtures of tetragonal and monoclinic phases, and have well-distributed mesopores (pore diameter of about 3.4–3.6 nm). As the calcination temperature increased from 400 to 1200 °C, the structures changed from tetragonal to monoclinic phase, while the morphologies turned from regular nanobelts to bead-like nanowires, and the mesopores disappeared bit by bit. Fe-doped and Fe2O3-loaded MZNs have been prepared to compare the catalytic activities of Fe-doped, Fe2O3-loaded, and pure MZNs for methane combustion. The results showed that Fe2O3-loaded MZNs have rather high catalytic activity, suggesting its potential application in practice. Methane combustion data over the catalysts are well fitted by a first-order kinetic expression.Graphical abstractMesoporous ZrO2 nanobelts (MZNs) have been prepared by a calcination route of ZrS3 nanobelts in air. Fe-doped and Fe2O3-loaded MZNs have been prepared to compare the catalytic activities of Fe-doped, Fe2O3-loaded, and pure MZNs for methane combustion. The results showed that Fe2O3-loaded MZNs have rather high catalytic activity.Highlights► Novel method preparing mesoporous zirconia nanobelts (MZNs) was introduced. ► Fe-doped, Fe2O3-loaded, and pure MZNs were used as catalysts for methane combustion. ► Fe2O3-loaded MZNs showed enhancing catalytic activity. ► Kinetic data over the catalysts were well fitted by a first-order kinetic equation.
Co-reporter:Ying-Chun Gao, Kai Xi, Wei-Na Wang, Xu-Dong Jia and Jun-Jie Zhu
Analytical Methods 2011 vol. 3(Issue 10) pp:2387-2391
Publication Date(Web):15 Sep 2011
DOI:10.1039/C1AY05378G
Well-oriented 3D gold flower-like nanoparticles were successfully synthesized by a facile one-pot method, and the gold nanoflowers (AuNFs) were mixed with hemoglobin (Hb) to form a gold nanoflowers/hemoglobin composite. The composite was further combined with multiwalled carbon nanotubes on a glassy carbon electrode (GCE) to fabricate a novel biosensor. The sensor has high stability and bioactivity, and was studied by scanning electron microscopy (SEM) and cyclic voltammetry (CV). The hemoglobin/gold nanoflowers/multiwalled carbon nanotubes glassy carbon electrode (Hb/AuNFs/CNTs/GCE) either retained the Hb in similar native conformations or promoted direct electron transfer. Moreover, the sensor exhibited remarkable catalytic activity toward H2O2 and trichloroacetic acid (TCA). The linear relationship for the determination is in the range of 1.0–60 μM for H2O2 and 0.06–28 mM for TCA. The detection limits were 0.08 μM and 7.3 μM (S/N = 3), respectively.
Co-reporter:Hongying Liu, Guoxi Liang, E. S. Abdel-Halim and Jun-Jie Zhu
Analytical Methods 2011 vol. 3(Issue 8) pp:1797-1801
Publication Date(Web):06 Jul 2011
DOI:10.1039/C1AY05178D
A sensitive and selective quantum dots (QDs)-based fluorescence resonance energy transfer (FRET) biosensor was successfully fabricated for the detection of the cancer marker type IV collagenase. The cancer marker type IV collagenase could be determined by linking peptide between the donor-luminescent QDs and the acceptor-gold nanoparticles with small size (SAuNPs) based on FRET. Firstly, peptide terminated with cysteine could be bound to the surface of SAuNPs via the formation of Au–S bonds. Then QDs combined with the SAuNPs through the peptide. At this moment, the photoluminescence (PL) of the QDs was quenched. After type IV collagenase was added into the system, the SAuNPs could detach from QDs because the enzyme cleaves the peptide to lead to the disappearance of FRET, which allowed the fluorescence of the QDs to return. The enzymatic activity of type IV collagenase was related to the PL change of QDs-based FRET probes. The concentration of type IV collagenase was determined in the linear range of 0.05–10 μg mL−1 with a detection limit of 18 ng mL−1. This sensor opens a new route for monitoring the low activities of type IV collagenase in normal and cancerous cell cultures.
Co-reporter:Haiping Huang, Jingjing Li and Jun-Jie Zhu
Analytical Methods 2011 vol. 3(Issue 1) pp:33-42
Publication Date(Web):20 Dec 2010
DOI:10.1039/C0AY00608D
This review presents a general description of the electrochemiluminescence (ECL) related to quantum dots (QDs) and their analytical application. It briefly overviews the synthetic route of quantum dots. The basic mechanisms are given for QDs ECL behavior. Finally, new developments and improvements of its application in inorganic substance analysis, organics analysis, immunoassay and aptasensing assay are discussed.
Co-reporter:Hai-Ping HUANG, Jun-Jie ZHU
Chinese Journal of Analytical Chemistry 2011 Volume 39(Issue 7) pp:963-971
Publication Date(Web):July 2011
DOI:10.1016/S1872-2040(10)60450-1
Graphene is a single layer of carbon atoms in a closely packed honeycomb lattice. As a new class of two-dimensional nanomaterial, graphene has attracted considerable attention in terms of both the experimental and theoretical aspects in recent years. The unique nanostructure and its other properties endow graphene with potential applications such as capacitors, cell images, sensors, devices, drug delivery, and solar cells. This review presents a general description of preparation route for graphene and its composites in the last few years. The new developments and improvements in its electrochemical applications in inorganic analysis, organic analysis, immunoassay and other electrochemical fields are also discussed.
Co-reporter:Shanhu Liu;Feng Lu;Dr. Ruimin Xing ; Jun-Jie Zhu
Chemistry - A European Journal 2011 Volume 17( Issue 2) pp:620-625
Publication Date(Web):
DOI:10.1002/chem.201001789
Abstract
The catalytic activity of nanocrystal catalysts depends strongly on their structures. Herein, we report three distinct structures of Fe3O4 nanocrystals, cluster spheres, octahedra, and triangular plates, prepared by a similar hydrothermal procedure. Additionally, the three Fe3O4 nanostructures were used as peroxidase nanomimetics and the correlation between the catalytic activities and the structures was first explored by using 3,3′,5,5′-tetramethylbenzidine and H2O2 as peroxidase substrates. The results showed that the peroxidase-like activities of the Fe3O4 nanocrystals were structure dependent and followed the order cluster spheres>triangular plates>octahedra; this order was closely related to their preferential exposure of catalytically active iron atoms or crystal planes. Such investigation is of great significance for peroxidase nanomimetics with enhanced activity and utilization.
Co-reporter:Jingjing Li, Mi Xu, Haiping Huang, Jinjun Zhou, E.S. Abdel-Halimb, Jian-Rong Zhang, Jun-Jie Zhu
Talanta 2011 Volume 85(Issue 4) pp:2113-2120
Publication Date(Web):30 September 2011
DOI:10.1016/j.talanta.2011.07.055
A novel competitive electrochemical cytosensor was reported by using aptamer (Apt)-quantum dots (Qdots) conjugates as a platform for tumor cell recognition and detection. The complementary DNA (cDNA), aptamer and Qdots could be assembled to the gold electrode surface. When the target cells existed, they could compete with cDNA to bind with Apt-Qdots conjugates based on the specific recognition of aptamer to MUC1 protein overexpressed on the cell surface, which resulted in the denaturation of double-stranded DNA structure and the release of the Apt-Qdots conjugates from the electrode. Electrochemical stripping measurement was then employed to determine the Cd2+ concentration in Qdots left at the electrode. The peak current was inversely proportional to the logarithmic value of cell concentration ranging from 1.0 × 102 to 1.0 × 106 cells mL−1 with a detection limit of 100 cells mL−1. Meanwhile, the recognition of aptamer to the target cells could be clearly observed through the strong fluorescence from Qdots. This is an example of the combination of aptamer and nanoparticles for the application of cell analysis, which is essential to cancer diagnosis and therapy.
Co-reporter:Wei Wang, Wen-Ya Wu, Xiaoqin Zhong, Wei Wang, Qiang Miao, Jun-Jie Zhu
Biosensors and Bioelectronics 2011 Volume 26(Issue 7) pp:3110-3114
Publication Date(Web):15 March 2011
DOI:10.1016/j.bios.2010.10.034
A sensitive colorimetric detection for biomolecules based on aptamer was described. Poly(dimethylsiloxane) (PDMS)–gold nanoparticles (AuNPs) composite film was used as a platform for immobilizing anti-target aptamer. PDMS–AuNPs composite film only covered with aptamer showed high inhibiting ability towards silver reduction, after target molecules were conjugated on the modified surface, the catalytic efficiency of AuNPs for silver reduction was increased. In this system, the darkness density of silver enhancement was applied for target quantitative measurement. Lysozyme and adenosine 5′-triphosphate (ATP) were tested as the models, quantitative measurements with imaging software or semiquantitative measurements with naked eyes were carried out in the range of 1 × 10−2–1 μg/mL and 1 × 10−4–1 × 103 μg/mL, the volume of reagent using in each assay is 15 μL or less. We speculated that aptamer-target conjugates’ inhibition ability for AuNPs’ catalytic efficiency toward silver reduction might come from charge and spatial effects. This study can offer a completely novel and relatively general approach for colorimetrical aptamer sensors with good analytical properties and potential applications. The sensor could be coupled with digital transmission of images for remote monitoring system in diagnosis, food control, and environmental analysis.
Co-reporter:Zhengzhi Yin, Yan Liu, Li-Ping Jiang, Jun-Jie Zhu
Biosensors and Bioelectronics 2011 Volume 26(Issue 5) pp:1890-1894
Publication Date(Web):15 January 2011
DOI:10.1016/j.bios.2010.03.025
A novel immunosensor for sensitive detection of tumor necrosis factor α was reported. First of all, gold nanoparticles were uniformly assembled on the surface of poly (styrene-acrylic acid) nanospheres, which was used as the matrix to conjugate alkaline phosphatase (ALP). And then, the obtained composite was used as multi-enzyme functionalized label for immunoassay. Biocompatible polyaniline doped with poly (acrylic acid) was electro-polymerized at the glass carbon electrode to construct the matrix for the immobilization of antibody TNF-α. After the sandwich immunoreaction, the labeled ALP was used to hydrolyze α-naphthyl phosphate to produce the electroactive α-naphthol, which could be amperometrically detected. The results showed that the electrochemical signals were proportional to the logarithm of the antigen concentration in the range of 0.02–200.00 ng/mL with the detection limit of 0.01 ng/mL. The developed immunoassay showed high sensitivity, acceptable stability and reproducibility, which might have potentially broad applications in protein diagnostics and bioassay.
Co-reporter:Kunping Liu, Jing-Jing Zhang, Chunming Wang, Jun-Jie Zhu
Biosensors and Bioelectronics 2011 Volume 26(Issue 8) pp:3627-3632
Publication Date(Web):15 April 2011
DOI:10.1016/j.bios.2011.02.018
A sensitive electrochemical immunosensor with graphene-assisted signal amplification has been developed. In order to construct the base of the immunosensor, a novel hybrid architecture was initially fabricated by combining poly (diallyldimethylammonium chloride) functionalized graphene nanosheets (PDDA-G) and gold nanoparticles (AuNPs) via a simple sonication-induced assembly. The formed hybrid architecture provided an effective matrix for antibody immobilization with good stability and bioactivity. Subsequently, a smart, multilabel, and graphene-based nanoprobe that contains gold nanoparticles functionalized exfoliated graphene oxide and horseradish peroxidase-secondary antibodies was designed for constructing a novel sandwiched electrochemical immunosensor. Enhanced sensitivity was obtained by combining the advantages of high-binding capability and excellent electrical conductivity of hybrid architecture with the multilabel signal amplification. On the basis of the dual signal amplification strategy of graphene-based architecture and the multilabel, the immunosensor displayed excellent analytical performance for the detection of human IgG (HIgG) range from 0.1 to 200 ng/mL with a detection limit of 0.05 ng/mL at 3σ. Moreover, the proposed method showed good precision, acceptable stability and reproducibility, and could be used for the detection of HIgG in real samples. Therefore, the present strategy definitely paves a way for the wide application of graphene in clinical research.
Co-reporter:Qingming Shen ; Xiaomei Zhao ; Shiwei Zhou ; Wenhua Hou
The Journal of Physical Chemistry C 2011 Volume 115(Issue 36) pp:17958-17964
Publication Date(Web):August 3, 2011
DOI:10.1021/jp203868t
ZnO/CdS hierarchical nanospheres were prepared for photoelectrochemical selective sensing of Cu2+. Hierarchical ZnO nanospheres were first synthesized by the hydrolysis of zinc salt under ultrasound irradiation, and then CdS nanocrystals were selectively grown on the hierarchical ZnO nanospheres. The light scattering of ZnO nanospheres and the heterointerfaces between CdS and ZnO provided significant advantages for enhanced light absorption and charge separation, thus resulting in an improvement in the photocurrent intensity. A photoelectrochemical sensor was developed based on the interaction between Cu2+ and CdS. The results showed that this sensor has a good selectivity and high sensitivity for Cu2+ detection.
Co-reporter:Dr. Rongjing Cui;Dr. Zhida Han; Jun-Jie Zhu
Chemistry - A European Journal 2011 Volume 17( Issue 34) pp:9377-9384
Publication Date(Web):
DOI:10.1002/chem.201100478
Abstract
A combined hydrothermal/hydrogen reduction method has been developed for the mass production of helical carbon nanotubes (HCNTs) by the pyrolysis of acetylene at 475 °C in the presence of Fe3O4 nanoparticles. The synthesized HCNTs have been characterized by high-resolution transmission electron microscopy, scanning electron microscopy, X-ray diffraction analysis, vibrating sample magnetometry, and contact-angle measurements. The as-prepared helical-structured carbon nanotubes have a large specific surface area and high peroxidase-like activity. Catalysis was found to follow Michaelis–Menten kinetics and the HCNTs showed strong affinity for both H2O2 and 3,3′,5,5′,-tetramethylbenzidine (TMB). Based on the high activity, the HCNTs were firstly used to develop a biocatalyst and amperometric sensor. At pH 7.0, the constructed amperometric sensor showed a linear range for the detection of H2O2 from 0.5 to 115 μM with a correlation coefficient of 0.999 without the need for an electron-transfer mediator. Because of their low cost and high stability, these novel metallic HCNTs represent a promising candidate as mimetic enzymes and may find a wide range of new applications, such as in biocatalysis, immunoassay, and environmental monitoring.
Co-reporter:Juan Peng;Li-Na Feng; Kui Zhang;Jing-Jing Li;Dr. Li-Ping Jiang; Jun-Jie Zhu
Chemistry - A European Journal 2011 Volume 17( Issue 39) pp:10916-10923
Publication Date(Web):
DOI:10.1002/chem.201100899
Abstract
Multifunctional manganese carbonate microspheres with superparamagnetic and fluorescent properties were fabricated and used as biological labels. The Fe3O4@MnCO3 microspheres were synthesized by direct co-precipitation without any linker shell. The Fe3O4@MnCO3 microspheres have uniform size distribution and rough surface, which provides a promising template for the assembly of polyelectrolytes (PEs) and CdTe quantum dots (QDs). A luminescent CdTe shell was observed in Fe3O4@MnCO3@PE-CdTe spheres by confocal fluorescence imaging. With excellent solubility in water and rough surfaces, the multifunctional microsphere offers a friendly microenvironment for immobilization of α-fetoprotein (AFP) antibodies (Ab2) to fabricate Fe3O4@MnCO3@PE-CdTe-Ab2 architecture. By using the Fe3O4@MnCO3@PEs-CdTe-Ab2 bioconjugate as a label, a promising and versatile platform for fluorescence imaging and electrochemical immunosensing of cancer biomarker AFP was developed. The prepared electrochemical immunosensor shows high sensitivity and selectivity with a detection limit of 0.3 pg mL−1.
Co-reporter:Yuping Chen, Gang Yang, Zihui Zhang, Xiaoyan Yang, Wenhua Hou and Jun-Jie Zhu
Nanoscale 2010 vol. 2(Issue 10) pp:2131-2138
Publication Date(Web):08 Sep 2010
DOI:10.1039/C0NR00246A
Polyaniline-intercalated layered vanadium oxide nanocomposites were successfully synthesized by an one-pot hydrothermal method and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), Fourier transform infrared spectroscopy (FT-IR), and Raman spectroscopy. The effects of reaction conditions, such as pH value of the precursor solution, reaction temperature and time, and the amount of aniline on the structure and morphology of the obtained samples, were systematically investigated. Based on the experimental results, an in situ intercalation-polymerization-exfoliation mechanism was put forward for the formation of layered nanocomposites. The application of the resulting layered nanocomposite as the cathode material in lithium battery was tested and the results showed that the polyaniline-intercalated layered vanadium oxide nanocomposite prepared at 140 °C had a good cycling performance and might act as a promising cathode material for high-energy-density rechargeable lithium batteries.
Co-reporter:Dong Zhu, Xiaoxing Jiang, Cuie Zhao, Xiaolian Sun, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2010 vol. 46(Issue 29) pp:5226-5228
Publication Date(Web):23 Jun 2010
DOI:10.1039/C0CC00791A
A microwave-assisted synthetic procedure is presented for the preparation of low-toxic Mn:ZnSe/ZnS core/shell nanocrystals to label antibodies for selective detection of human immunoglobulin G (IgG) based on fluorescence resonance energy transfer (FRET) between the Mn:ZnSe/ZnS and Au nanoparticles (AuNPs).
Co-reporter:Guo-Xi Liang, Ling-Ling Li, Hong-Yin Liu, Jian-Rong Zhang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2010 vol. 46(Issue 17) pp:2974-2976
Publication Date(Web):05 Mar 2010
DOI:10.1039/C000564A
New water-soluble CdSeTe/ZnS core–shell quantum dots with excellent near-infrared emission were synthesized via an aqueous solution method; they showed strong electrogenerated chemiluminescence and favorable biocompatibility.
Co-reporter:Qianhao Min, Ren'an Wu, Liang Zhao, Hongqiang Qin, Mingliang Ye, Jun-Jie Zhu and Hanfa Zou
Chemical Communications 2010 vol. 46(Issue 33) pp:6144-6146
Publication Date(Web):27 Jul 2010
DOI:10.1039/C0CC00619J
In this study, the concept of size-selective proteolysis was first described by using the mesoporous silica-based trypsin nanoreactor. For analysis of a complex protein sample, low-MW proteins were preferentially digested for identification while high-MW proteins were excluded from digestion.
Co-reporter:Jing-Jing Zhang, Fang-Fang Cheng, Ting-Ting Zheng and Jun-Jie Zhu
Analytical Chemistry 2010 Volume 82(Issue 9) pp:3547
Publication Date(Web):April 6, 2010
DOI:10.1021/ac9026127
A new strategy for assessing cell surface carbohydrates and P-glycoprotein (P-gp) expression status and quantifying the cell numbers with an electrochemical immunoassay was designed. In order to construct the base of the cytosensor, a novel 3-D architecture was initially fabricated by combining nitrogen-doped carbon nanotubes, thionine, and gold nanoparticles via a simple layer-by-layer method. The formed architecture provided an effective matrix for concanavalin A (Con A) binding and made the immobilized Con A hold high stability and bioactivity. On the basis of the specific recognition of cell surface mannosyl groups to Con A, the Con A/3-D architecture interface showed a predominant capability for cell capture. With another coupled signal amplification based on a enzymatic catalytic reaction of HRP toward the oxidation of thionine by the H2O2, which was induced by two-step immunoreactions, the proposed cytosensor showed an excellent analytical performance for the detection of HeLa cells ranging from 8.0 × 102 to 2.0 × 107 cells mL−1 with a limit of detection of 500 cells mL−1. Moreover, with the use of preblocking procedures, the mannosyl groups and P-gp on single HeLa cell could be further detected to be (4 ± 2) × 1010 molecules of mannose moieties and 8.47 × 106 molecules of P-gp. This strategy offers great promise for sensitive detection of cancer cells and cell surface receptors and thus may help improve cancer diagnosis and treatment.
Co-reporter:Kunping Liu, Jingjing Zhang, Guohai Yang, Chunming Wang, Jun-Jie Zhu
Electrochemistry Communications 2010 Volume 12(Issue 3) pp:402-405
Publication Date(Web):March 2010
DOI:10.1016/j.elecom.2010.01.004
The functionalized graphene nanosheets (PDDA-G) with poly(diallyldimethylammonium chloride) (PDDA) were synthesized and used to combine with room temperature ionic liquid (RTIL). The resulting RTIL/PDDA-G composite displayed an enhanced capability for the immobilization of hemoglobin to realize its direct electrochemistry. Moreover, the RTIL/PDDA-G based biosensor exhibited excellent electrocatalytic activity for the detection of nitrate with a wide linear range from 0.2 to 32.6 μM and a low detection limit of 0.04 μM at 3σ. This work opens a new way to functionalized graphene nanosheets with good biocompatibility and solubility in biosensors.
Co-reporter:Wen-Ya Wu, Xiaoqin Zhong, Wei Wang, Qiang Miao, Jun-Jie Zhu
Electrochemistry Communications 2010 Volume 12(Issue 11) pp:1600-1604
Publication Date(Web):November 2010
DOI:10.1016/j.elecom.2010.09.005
In this article, we report a flexible poly(dimethylsiloxane) (PDMS)-based three-electrode sensor (FPT-Sensor). In PDMS basis, gold was chemically deposited as working and counter electrodes, and silver as the reference one, the device was flexible without inducing irreversible deformation or fatigue after electrochemical testing with forced deformations (the device was twisted, rolled, and stretched). This sensing system provides a route for producing in situ diagnosis sensing device which requires excellent flexibility to fit in various situations.
Co-reporter:Rongjing Cui, Jun-Jie Zhu
Electrochimica Acta 2010 Volume 55(Issue 27) pp:7814-7817
Publication Date(Web):30 November 2010
DOI:10.1016/j.electacta.2010.03.022
The gold nanoparticles/colloidal carbon sphere hybrid material was used for the immobilization of protein, and was developed in biosensing. The hybrid material was fabricated by the assembly of gold nanoparticles onto the surface of colloidal carbon spheres, which constructed a 3D antibody immobilization matrix on the glass carbon electrode and made the immobilized biomolecules hold high stability and bioactivity. After the sandwich-type immunoreaction, the formed HRP-labeled immunoconjugate showed good enzymatic activity for the oxidation of o-phenylenediamine by H2O2. The approach provided a linear response range between 5 and 250 ng/mL with a detection limit of 1.8 ng/mL. The immunosensor showed good precision, acceptable stability and reproducibility and could be used for the detection of human IgG in real samples, which provided a potential alternative tool for the detection of protein in clinical laboratory.
Co-reporter:Wei Wang, Wen-Ya Wu, Wei Wang, Jun-Jie Zhu
Journal of Chromatography A 2010 Volume 1217(Issue 24) pp:3896-3899
Publication Date(Web):11 June 2010
DOI:10.1016/j.chroma.2010.04.017
This paper described a convenient semiquantitative method for colorimetric detection of protein with self-calibration integrated on the test strip. Hydrophilic paper was employed as microfluidic device for running colorimetric assay, tree-shaped design was developed to ensure uniform microfluidic flow for multiple branches. The approach was validated with bovine serum albumin (BSA) colorimetric detection, and colorimetric results observed by naked eyes were consistent with that from apparatus. The device could be coupled with digital transmission of images for remote monitoring system for diagnosis, food control, and environmental analysis.
Co-reporter:Xiaojun Chen, Jinjun Zhou, Jie Xuan, Wei Yan, Li-Ping Jiang and Jun-Jie Zhu
Analyst 2010 vol. 135(Issue 10) pp:2629-2636
Publication Date(Web):06 Aug 2010
DOI:10.1039/C0AN00264J
A novel label-free highly sensitive electrochemical impedance spectroscopy (EIS) immunosensor was fabricated based on the highly ordered macroporous gold film (HOMGF) in the presence of room-temperature ionic liquid (IL) for the detection of human Apolipoprotein B-100 (ApoB-100). The antibody of ApoB-100 (Ab) was adsorbed directly onto the HOMGF electrode surface and maintained its bioactivity. After the residual active sites at the electrode were passivated by BSA, the mixture of BMIm+BF4− and silica sol was dropped onto the electrode to entrap the adsorbed Ab and BSA molecules firmly. The addition of IL could prevent the inactivation of Ab by releasing alcohol during the sol–gel process, and the conductivity of the IL-gel membrane was increased. Of particular interest is the fact that the fabricated immunosensor could be used at 60 °C. This could be attributed to the interconnected porosity of the IL-gel membrane, which can prevent Ab from unfolding and losing its bioactivities. The immunosensor also exhibited a highly sensitive response to ApoB-100 with the lowest concentration of 5 fg mL−1. The detection of ApoB-100 levels in five sera samples obtained from hospital showed acceptable accuracy with that using commercial immunonephelometry method.
Co-reporter:Yuping Chen, Chunliang Lu, Lin Xu, Ying Ma, Wenhua Hou and Jun-Jie Zhu
CrystEngComm 2010 vol. 12(Issue 11) pp:3740-3747
Publication Date(Web):12 Jul 2010
DOI:10.1039/C000744G
Single crystalline MoO3 nanobelts with width of 200–300 nm and the length up to several tens of micrometres were prepared by a facile hydrothermal method and characterized. Based on time- and temperature-dependent experiments, a solid–solution–solid transformation mechanism was proposed for the formation of crystalline MoO3 nanobelts. The as-prepared MoO3 nanobelts were used as a photocatalyst to degrade methylene blue (MB) under visible light irradiation and demonstrated a dramatic activity, indicating that the as-prepared MoO3 nanobelts were promising candidates for the photodegradation of organic dyes. A self-sensitization photocatalytic mechanism was suggested based on the experimental results.
Co-reporter:Haiping Huang, Jingjing Li, Yanglan Tan, Jinjun Zhou and Jun-Jie Zhu
Analyst 2010 vol. 135(Issue 7) pp:1773-1778
Publication Date(Web):17 May 2010
DOI:10.1039/C0AN00108B
Simple and convenient assays with quantum dots (QDs) as the labels for DNA detection are developed. The probe DNA modified with thiol was first immobilized on a pretreated Au electrode, and then the complementary DNA (cDNA) oligonucleotides were hybridized with the immobilized probes by immersing the probe-modified Au electrode into the cDNA oligonucleotide solution. Finally, the avidin-modified QDs were bound to the biosensor in the presence of biotin-modified cDNA. The fabrication process for the biosensor was monitored by electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). Different from the traditional sandwich-structure strategy, the QDs bind to the target DNA directly via the biotin–avidin-system. By observing the ECL signal and determination of the cadmium component in QDs, the DNA hybridization event was detected by ECL and square wave anodic stripping voltammetric technique (SWASV) respectively. For SWASV detection, the signal linearly increased with the increase of the logarithm of the cDNA concentration over the range of 50 nM ∼ 5 μM. The minimum detectable concentration is 50 pM. For ECL, it showed wider linearity range over 5 nM ∼ 5 μM and lower detectable concentration of 10 pM. This indicated that the ECL assay could be comparable to the conventional electrochemical assay. Furthermore, this biosensor possesses high selectivity over different sequences of target DNA oligonucleotides.
Co-reporter:Xuan Yang, Danchen Wang, Junjie Zhu, Claire Gu, Jin Z. Zhang
Chemical Physics Letters 2010 Volume 495(1–3) pp:109-112
Publication Date(Web):29 July 2010
DOI:10.1016/j.cplett.2010.06.065
Abstract
Surface enhanced Raman scattering (SERS) spectra of Rhodamine 6G adsorbed on silver nanoparticles have been measured using an optical fiber from 22 to 85 °C. The fiber carries both the laser excitation and SERS signal, providing a convenient scheme for in-situ SERS measurement at high-temperature microscale environments. It is found that although SERS intensity generally decreases with increasing temperature, the signal is still significant and stable at high-temperature up to 85 °C. More importantly, the SERS signal is reversible with respect to the temperature change. These results are important for high-temperature SERS applications in chemical and biological detection.
Co-reporter:Jinjun Zhou, Haiping Huang, Jie Xuan, Jianrong Zhang, Jun-Jie Zhu
Biosensors and Bioelectronics 2010 Volume 26(Issue 2) pp:834-840
Publication Date(Web):15 October 2010
DOI:10.1016/j.bios.2010.05.021
A sensitive electrochemical aptasensor was successfully fabricated for the detection of adenosine triphosphate (ATP) by combining three-dimensionally ordered macroporous (3DOM) gold film and quantum dots (QDs). The 3DOM gold film was electrochemically fabricated with an inverted opal template, making the active surface area of the electrode up to 9.52 times larger than that of a classical bare flat one. 5′-Thiolated ATP-binding aptamer (ABA) was first assembled onto the 3DOM gold film via sulfur–gold affinity. Then, 5′-biotinated complementary strand (BCS) was immobilized via hybridization reaction to form the DNA/DNA duplex. Since the tertiary structure of the aptamer was stabilized in the presence of target ATP, the duplex can be denatured to liberate BCS. The reaction was monitored by electrochemical stripping analysis of dissolved QDs which were bound to the residual BCS through biotin–streptavidin system. The decrease of peak current was proportional to the amount of ATP. The unique interconnected structure in 3DOM gold film along with the “built-in” preconcentration remarkably improved the sensitivity. ATP detection with high selectivity, wide linear dynamic range of 4 orders of magnitude and high sensitivity down to 0.01 nm were achieved. The results demonstrated that the novel strategy was feasible for sensitive ATP assay and provided a promising model for the detection of small molecules.
Co-reporter:Zhengzhi Yin, Rongjing Cui, Yan Liu, Liping Jiang, Jun-Jie Zhu
Biosensors and Bioelectronics 2010 Volume 25(Issue 6) pp:1319-1324
Publication Date(Web):15 February 2010
DOI:10.1016/j.bios.2009.10.021
A simple strategy for sensitive detection of human IgG using cadmium ions-functionalized polymer nanospheres as the label is presented. The polymer nanosphere consisted of hard poly-styrene core and biocompatible poly (acrylic acid) (PAA) shell. The carboxyl groups of hydrophilic shell were used to chelated with the cadmium ions, and then conjugate with antibody (Ab2) to fabricate metal ions marked bioconjugates as the label in immunoassay. For constructing the matrix of the immunosensor, the PAA-functionalized carbon nanotubes were used to modify disposable screen printed electrodes for the immobilization of antibody (Ab1). After sandwich immunoreaction, differential pulse voltammetry was used to oxidize the conjuncted cadmium for the detection of antigen. The obtained results provided a linear response range from 0.1 to 35.0 pg/mL human IgG with a lower detection limit of 0.06 pg/mL, which is prominently improved in comparison with conventional immunoassay. The usage of the chelation reaction offers a simple and convenient route for the preparation of metallo-immunoassay labels, and also avoids the complicated and time-consuming dissolving of metal component for ultrasensitive determination. This approach is expected to have wide applications in protein diagnostics and bioanalysis in the future.
Co-reporter:Xiaojun Chen, Kui Zhang, Jinjun Zhou, Jie Xuan, Wei Yan, Li-Ping Jiang, Jun-Jie Zhu
Biosensors and Bioelectronics 2010 Volume 25(Issue 5) pp:1130-1136
Publication Date(Web):15 January 2010
DOI:10.1016/j.bios.2009.09.038
A novel type of colloidal carbon sphere array (CSA) was developed for the fabrication of disposable electrochemical immunosensor. The CSA was successfully prepared on indium tin oxide (ITO) substrate in a simple manner and the scanning electron micrograph confirmed that a single-layered arrangement of the carbon spheres with its (1 1 1) plane paralleled the substrate's surface. The CSA modified electrode has a higher surface area and exhibits a more sensitive electrochemical response than a normal carbon-based electrode with the same geometric area. An Immunoglobin A (IgA) immunosensor was constructed by the covalent bonding of IgA antibody molecules with the CSA aided by large numbers of carboxyl groups on the surface of carbon spheres. The immunosensor exhibited a wide linear response to IgA ranging from 0.1 to 200 ng mL−1 by electrochemical impedance spectroscopy (EIS) technique. The detection of IgA levels in three sera obtained from hospital samples showed acceptable accuracy.
Co-reporter:Limin Liu, Bo Shen, Jianjun Shi, Fang Liu, Guo-Yuan Lu, Jun-Jie Zhu
Biosensors and Bioelectronics 2010 Volume 25(Issue 12) pp:2627-2632
Publication Date(Web):15 August 2010
DOI:10.1016/j.bios.2010.04.031
A novel mediator-free biosensor was constructed by the co-intercalation of negatively charged DNA and positively charged hemoglobin (Hb) in the interlayer galleries of layered α-zirconium phosphate (α-ZrP) with the delamination-assembly procedure at pH 5.5. X-ray diffraction and field-emission scanning electron microscopy results revealed the featured layered structure for the re-assembled DNA/Hb/α-ZrP composite. Infrared spectroscopy and circular dichroism results confirmed the coexistence of Hb and DNA in the composite and the considerably retained protein conformation of intercalated Hb. The direct electron transfer of Hb was facilitated by the co-intercalation of DNA and Hb. Because of the synergistic effect of α-ZrP host and co-intercalated DNA guest, the DNA/Hb/α-ZrP modified electrode exhibited good electrocatalytic response to H2O2 with higher sensitivity of 0.79 A M−1 cm−2 and lower detection of 4.28 × 10−7 M in the linear range of 7.28 × 10−7 to 9.71 × 10−5 M. Furthermore, the electrocatalytic activity of Hb in the DNA/Hb/α-ZrP composite retained at high temperature (85 °C) or in the presence of organic solvent (CH3CN), which could be the protection of α-ZrP nanosheets.
Co-reporter:Guo-Xi Liang, Hong-Ying Liu, Jian-Rong Zhang, Jun-Jie Zhu
Talanta 2010 Volume 80(Issue 5) pp:2172-2176
Publication Date(Web):15 March 2010
DOI:10.1016/j.talanta.2009.11.025
The near-infrared (NIR)-emitting CdSeTe alloyed quantum dots (AQdots) that capped with l-cysteine were applied for ultrasensitive Cu2+ sensing. The sensing approach was based on the fluorescence of the AQdots selectively quenched in the presence of Cu2+. Experimental results showed a low interference response towards other metal ions. The possible quenching mechanism was discussed on the basis of the binding between l-cysteine and the metal ions. In addition, biomolecules have low effect on the fluorescence due to the minimized interferences in NIR region. The response of the NIR optical sensor was linearly proportional to the concentration of Cu2+ ranging from 2 × 10−8 to 2 × 10−6 mol L−1. Furthermore, it has been successfully applied to the detection of Cu2+ in vegetable samples.
Co-reporter:Chang-Jie Mao, Jun Geng, Xing-Cai Wu and Jun-Jie Zhu
The Journal of Physical Chemistry C 2010 Volume 114(Issue 5) pp:1982-1988
Publication Date(Web):January 19, 2010
DOI:10.1021/jp907525p
Highly ordered SrMoO4 3D spherical superstructure assembled with nanosheets was synthesized via a facile and fast sonochemical route without any template. The products were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, and selected-area electron diffraction. The results showed that the as-synthesized self-assembled SrMoO4 spheres were composed of nanosheets with thickness of about 40−60 nm and width of 1 μm. The pH values and surfactants play an important role in the morphologies of the final sample. The possible mechanism for the formation of self-assembled SrMoO4 spherical superstructure is proposed. The luminescence properties of these SrMoO4 samples with different morphologies have also been investigated.
Co-reporter:Xianwen Kan, Qun Zhao, Dalin Shao, Zhirong Geng, Zhilin Wang and Jun-Jie Zhu
The Journal of Physical Chemistry B 2010 Volume 114(Issue 11) pp:3999-4004
Publication Date(Web):February 25, 2010
DOI:10.1021/jp910060c
A simple method for the preparation of core−shell micro/nanostructured magnetic molecularly imprinted polymers (MIPs) for protein recognition is described. Magnetic MIPs were synthesized by copolymering γ-aminopropyltrimethoxysilane and tetraethyl orthosilicate at the surface of Fe3O4 nanospheres, which were directly covalently bound with template molecule, bovine hemoglobin (BHb), through imine bond. Transmission electron microscopy and scanning electron microscopy images showed that the Fe3O4 nanospheres with diameter about 50−150 nm were coated with the MIPs layer with average thickness about 10 nm, which enabled the magnetic MIPs to have a sensitive and fast magnetic response. The proximity between the thickness of MIPs layer and the spatial size of BHb indicated that the imprinted sites almost situated at the surface of magnetic MIPs, leading a rapid adsorption saturation within 1 h. And the adsorption amounts of magnetic MIPs toward BHb were estimated to be 10.52 mg/g at pH 6.5, which was 4.6 times higher than that of magnetic nonmolecularly imprinted polymers. Meanwhile, the result of selective test showed that the magnetic MIPs had an excellent recognition capacity to BHb compared to the other nontemplate proteins. Except for the spatial size complementary between BHb and the binding sites in magnetic MIPs, the electrostatic interaction also was proven to be an important factor for recognizing the imprinting molecule.
Co-reporter:Wen-Ya Wu, Zhi-Ping Bian, Wei Wang, Wei Wang, Jun-Jie Zhu
Sensors and Actuators B: Chemical 2010 Volume 147(Issue 1) pp:298-303
Publication Date(Web):18 May 2010
DOI:10.1016/j.snb.2010.03.027
This paper described poly(dimethylsiloxane) (PDMS)-gold nanoparticles (AuNPs) composite film as basis with silver enhancement for colorimetric detection of cardiac troponin I (cTnI). Stable PDMS-AuNPs composite film was simply prepared with dropping HAuCl4 solution in PDMS microchip, gold nanoparticles were both used as nuclei for silver enhancement and as basis for adsorption of antibody, immunoassay was implemented after BSA blocking. Because of the inhibition ability difference for silver enhancement between BSA and antibody-antigen complex, darkness of silver deposition was relative to the amount of antigen. The proposed colorimetric method was applied for clinical sample cTnI detection, results were consistent with that from enzyme-linked immunosorbent assay (ELISA). The composite film could be coupled with digital transmission of images for remote monitoring system in diagnosis, food control, and environmental analysis.
Co-reporter:Xing-Hua Li;Lin Dai;Yan Liu;Xiao-Jun Chen;Wei Yan;Li-Ping Jiang
Advanced Functional Materials 2009 Volume 19( Issue 19) pp:3120-3128
Publication Date(Web):
DOI:10.1002/adfm.200901003
Abstract
A 3D ordered macroporous (3DOM) ionic-liquid-doped polyaniline (IL-PANI) inverse opaline film is fabricated with an electropolymerization method and gold nanoparticles (AuNPs) are assembled on the film by electrostatic adsorption, which offers a promising basis for biomolecular immobilization due to its satisfactory chemical stability, good electronic conductivity, and excellent biocompatibility. The AuNP/IL-PANI inverse opaline film could be used to fabricate an electrochemical impedance spectroscopy (EIS) immunosensor for the determination of Hepatitis B surface antigen (HBsAg). The concentration of HBsAg is measured using the EIS technique by monitoring the corresponding specific binding between HBsAg and HBsAb (surface antibody). The increased electron transfer resistance (Ret) values are proportional to the logarithmic value of the concentration of HBsAg. This novel immunoassay displays a linear response range between 0.032 pg mL−1 and 31.6 pg mL−1 with a detection limit of 0.001 pg mL−1. The detection of HBsAg levels in several sera showed satisfactory agreement with those using a commercial turbidimetric method.
Co-reporter:Xing-Hua Li;Lin Dai;Yan Liu;Xiao-Jun Chen;Wei Yan;Li-Ping Jiang
Advanced Functional Materials 2009 Volume 19( Issue 19) pp:
Publication Date(Web):
DOI:10.1002/adfm.200990089
Co-reporter:Liang Zhao, Peng Cheng, Jianxin Li, Yue Zhang, Miaomiao Gu, Jun Liu, Jianrong Zhang and Jun-Jie Zhu
Analytical Chemistry 2009 Volume 81(Issue 16) pp:7075
Publication Date(Web):July 27, 2009
DOI:10.1021/ac901121f
This technical note describes a facile technique to screen some anticancer drugs and evaluate their effects on nonadhesive leukemic cells in an easily fabricated microfluidic device by utilizing the Annexin V conjugated quantum dots as apoptosis detection probes. The cell immobilizing structures and gradient-generating channels were integrated within the device which was fabricated in one-single step. The nonadhesive leukemic HL-60 cells can be felicitously immobilized and cultured on the dam structures at a proper lateral pressure. We then delivered Annexin V functionalized quantum dots which can readily bind to the outer membrane of apoptotic cells and distinguish the apoptosis from unaffected cells with single cell level resolution. The diffusion time of quantum dots reduced to 5 min before imaging. The capabilities of evaluating drug effect on HL-60 cell line have been shown in both population way and individual cell level. The technique presented herein can bridge the gap between the quantum dots based in vitro cell imaging and the analysis of individual apoptotic cell in a microfluidic system, allows an easy operating protocol to screen some clinically available anticancer drugs.
Co-reporter:Haiping Huang, Guifen Jie, Rongjing Cui, Jun-Jie Zhu
Electrochemistry Communications 2009 Volume 11(Issue 4) pp:816-818
Publication Date(Web):April 2009
DOI:10.1016/j.elecom.2009.01.009
A novel quantum dots (QDs) ECL biosensor for the detection of lysozyme was developed. Lysozyme was first incubated with probes immobilized at Au electrode in order to form the aptamer-lysozyme bioaffinity complexes. And the free probes were hybridized with the 5′-biotin modified cDNA oligonucleotides to form double-stranded DNA (ds-DNA) oligonucleotides. Avidin-QDs were bound to these hybridized cDNA through the biotin-avidin-system. The ECL signal of the biosensor was responsive to the amount of QDs bonded to the cDNA oligonucleotides, which was indirectly inverse proportional to the combined target protein.
Co-reporter:Yuanyuan Wang, Xiaojun Chen, Jun-Jie Zhu
Electrochemistry Communications 2009 Volume 11(Issue 2) pp:323-326
Publication Date(Web):February 2009
DOI:10.1016/j.elecom.2008.11.056
The composite of C@SiO2 with gold nanoparticles (AuNPs–C@SiO2) was fabricated by layer-by-layer assembly technique and was used to fabricate a novel hydrogen peroxide (H2O2) biosensor. The composite was composed of a colloidal carbon sphere core with an average diameter of 200 nm and a porous silica shell with a uniform thickness of about 50 nm, and decorated with gold nanoparticles on the surface. The porous silica shell could promote the composite to show high bio-compatibility and chemical stability. The AuNPs–C@SiO2 composite combined with hemoglobin (Hb) was used to construct a novel biosensor for the determination of H2O2, displaying a wide linear range from 5.0 to 80 μM with a detection limit of 0.08 μM at 3σ. The Kmapp value for the biosensor was determined to be 71.49 μM.
Co-reporter:Guifen Jie, Lingling Li, Chao Chen, Jie Xuan, Jun-Jie Zhu
Biosensors and Bioelectronics 2009 Volume 24(Issue 11) pp:3352-3358
Publication Date(Web):15 July 2009
DOI:10.1016/j.bios.2009.04.039
Electrochemiluminescence (ECL) of CdSe quantum dots (QDs) was greatly enhanced by the combination of carbon nanotubes (CNTs) and poly (diallyldimethylammonium chloride) (PDDA) in the CdSe QDs film, and could successfully be used to develop a sensitive ECL immunosensor for the detection of human IgG (Ag). The novel CdSe QDs–CNTs composites exhibited high ECL intensity, good biocompatibility, and high stability, which held great promise for the fabrication of the ECL biosensors with improved sensitivity. After PDDA as a binding linker was conjugated to the CdSe QDs–CNTs composite film on the electrode, the ECL signal was significantly enhanced. Subsequently, gold nanoparticles (GNPs) assembled onto the CdSe QDs–CNTs/PDDA modified electrode could amplify the ECL signal once again. After antibody (Ab) was immobilized onto the electrode through GNPs, the ECL immunosensor was successfully fabricated. It is for the first time that the unique function of PDDA for enhancing QDs ECL was explored and used to develop an ECL biosensor. The principle of ECL detection for target Ag is based on the increment of steric hindrance after immunoreaction, which resulted in the decrease of ECL intensity. The Ag concentration was determined in the linear range of 0.002–500 ng L−1 with a detection limit of 0.6 pg mL−1. The sensor showed good fabrication and detection reproducibility, and the assay results were in acceptable agreement with the clinical sera tests, showing a promising clinical application. This work opened the new avenues for applying QDs ECL in highly sensitive bioassays.
Co-reporter:Haiping Huang, Jun-Jie Zhu
Biosensors and Bioelectronics 2009 Volume 25(Issue 4) pp:927-930
Publication Date(Web):15 December 2009
DOI:10.1016/j.bios.2009.08.008
A novel biosensor for the detection of thrombin was developed by using QDs electrochemiluminescence (ECL) technique. The thiol-terminated aptamer with 15 nucleotides (probe I) was first immobilized on Au electrode, and then thrombin was imported to form the aptamer–thrombin bioaffinity complexes. Another 5′-biotin modified aptamer (29 nucleotides, probe II) was next hybridized with the combined thrombin to form a sandwich type structure. Streptavidin modified QDs (avidin–QDs) were bound to probe II via the biotin–avidin-system. The QDs ECL signal was responsive to the amount of probe II, which was indirect proportional to the combined thrombin. The ECL intensity of the biosensor increased with the increase of thrombin concentration in the range of 0–20 μg mL−1. In addition, the biosensor exhibited the excellent selectivity responses and good stability toward the target analyte.
Co-reporter:Guo-Xi Liang, Hong-Cheng Pan, Ye Li, Li-Ping Jiang, Jian-Rong Zhang, Jun-Jie Zhu
Biosensors and Bioelectronics 2009 Volume 24(Issue 12) pp:3693-3697
Publication Date(Web):15 August 2009
DOI:10.1016/j.bios.2009.05.008
A novel sensing system based on the near infrared (NIR) fluorescence resonance energy transfer (FRET) between Mn:CdTe quantum dots (Qdots) and Au nanorods (AuNRs) was established for the detection of human IgG. The NIR-emitting Qdots linked with goat anti-human IgG (Mn:CdTe-Ab1) and AuNRs linked with rabbit anti-human IgG (AuNRs-Ab2) acted as fluorescence donors and acceptors, respectively. FRET occurred by human IgG with the specific antigen–antibody interaction. And human IgG was detected based on the modulation in FRET efficiency. The calibration graph was linear over the range of 0.05–2.5 μM of human IgG under optimal conditions. The proposed sensing system can decrease the interference of biomolecules in NIR region and increase FRET efficiency in optimizing the spectral overlap of AuNRs with Mn:CdTe Qdots. This method has great potential for multiplex assay with different donor–acceptor pairs.
Co-reporter:Shanhu Liu, Ruimin Xing, Feng Lu, Rohit Kumar Rana and Jun-Jie Zhu
The Journal of Physical Chemistry C 2009 Volume 113(Issue 50) pp:21042-21047
Publication Date(Web):November 19, 2009
DOI:10.1021/jp907296n
Monodispersed Fe3O4 nanospheres with hollow interior structures exhibiting high saturation magnetization of 83.0 emu g−1 were fabricated by a facile one-pot route. The fabrication process is very simple with only FeCl3·6H2O and anhydrous NaAc as the reactants in an ethylene glycol solution with no templates or surfactants involved. Field-emission scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and a superconducting quantum interference device magnetometer were used to characterize the morphologies, structures, and properties of the hollow magnetic nanospheres. A plausible mechanism based on oriented attachment and subsequent local Ostwald ripening is proposed. In addition, the experiments of the hollow nanospheres decorated with polyacrylic acids as drug carriers and Rhodamine 6G as a model drug, revealed pH- or salt-responsive release profiles, thus demonstrating the potential of these nanostructures in biomedical applications.
Co-reporter:Zhengzhi Yin, Jingjing Zhang, Li-Ping Jiang and Jun-Jie Zhu
The Journal of Physical Chemistry C 2009 Volume 113(Issue 36) pp:16104-16109
Publication Date(Web):August 12, 2009
DOI:10.1021/jp903589a
A poly(N-isopropylacrylamide) (PNIPAm) brush has been successfully fabricated on an indium tin oxide (ITO) film via a simple electrochemical route. The polymer thermoresponsive behavior was investigated with an electrically heated ITO electrode. This kind of electrode demonstrated a rapid response to heating up and down, and the results indicated that the polymer modified interface possessed a characteristic lower critical solution temperature (LCST) and showed ON/OFF switch behavior. Furthermore, the model protein of hemoglobin (Hb) was incorporated into the polymer by a thermal “breathing-in” process. The electrochemical experiments revealed that the film could provide a friendly microenvironment for Hb to promote direct electron transfer. A pair of well-defined redox peaks with a formal potential of −204 mV (verses saturated calomel electrode, SCE) was observed. The redox current of Hb gradually lowered when the prepared electrode was immersed into pH 7.0 PBS at 20 °C, indicating that incorporated Hb could be released from the PNIPAm film, which proved that the approach could provide a potential route in the design of responsive biocompatible surfaces.
Co-reporter:Qingming Shen, Qianhao Min, Jianjun Shi, Liping Jiang, Jian-Rong Zhang, Wenhua Hou and Jun-Jie Zhu
The Journal of Physical Chemistry C 2009 Volume 113(Issue 4) pp:1267-1273
Publication Date(Web):2017-2-22
DOI:10.1021/jp807881s
A simple sonoelectrochemical method was used to realize the morphology-controlled synthesis of palladium nanostructures at room temperature. The palladium spherical nanoparticles, multitwinned particles, and spherical spongelike particles (SSPs) were successfully prepared in the presence of different surfactants or polymers. It was found that the size and shape of the Pd nanostructures could be controlled by varying current density and pH value of the precursor solution. The Pd nanostructures were characterized by transmission electron microscopy, high-resolution transmission electron microscopy, field emission scanning electron microscopy, energy-dispersive X-ray, and X-ray diffraction. The possible formation mechanism was discussed. In addition, the electrocatalytic properties of the Pd nanostructures for direct alcohol oxidation in alkaline media were systematically investigated. The results showed that SSPs had a higher electrochemical active surface and result in more stable and better electrocatalytic properties than other Pd nanostructures for the ethanol electro-oxidation.
Co-reporter:Liang-Dong Feng, Miao-Miao Gu, Yan-Li Yang, Guo-Xi Liang, Jian-Rong Zhang and Jun-Jie Zhu
The Journal of Physical Chemistry C 2009 Volume 113(Issue 20) pp:8743-8749
Publication Date(Web):April 22, 2009
DOI:10.1021/jp900925p
A facile electrochemical approach was developed for the controllable synthesis of cerium hexacyanoferrate(II) (CeHCF(II)) flowerlike and fusiform Christmas-tree-like microparticles. The composition, morphology, and structure of the as-prepared CeHCF(II) products were characterized by the techniques such as powder X-ray diffraction (XRD), infrared spectroscopy (IR), thermogravimetry (TG), differential scanning calorimetry (DSC), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDS), and scanning electron microscopy (SEM). The formula of the prepared CeHCF(II) could be assigned to be KCe[Fe(CN)6]·4H2O. It was observed that the size and morphology of the CeHCF(II) microparticles were altered by electrodepositing potential and time, the molar ratio of Ce(NO3)3 and K3[Fe(CN)6], and the acidity of electrolyte. To the best of our knowledge, this morphologies of CeHCF(II) have not been reported before. The as-prepared CeHCF(II) microparticles showed good ultraviolet luminescent properties and high luminescent intensity.
Co-reporter:Xiao Chen;Jing Jing Zhang;Jie Xuan;Jun Jie Zhu
Nano Research 2009 Volume 2( Issue 3) pp:210-219
Publication Date(Web):2009 March
DOI:10.1007/s12274-009-9019-6
A novel biosensor based on a myoglobin/gold nanoparticles/carbon spheres (Mb-AuNPs-CNs) 3-D architecture bioconjunction has been fabricated for the determination of hydrogen peroxide (H2O2). Cyclic voltammetry (CV), Fourier transform infrared (FT-IR) spectroscopy and scanning electron microscopy (SEM) were used to characterize the bioconjunction of the AuNPs-CNs with Mb. Experimental results demonstrate that the AuNPs-CNs hybrid material is more effective in facilitating electron transfer of the immobilized enzyme than CNs alone, which can be attributed to the unique nanostructure and larger surface area of the bioconjunction. The biosensor displayed good performance for the detection of H2O2 with a wide linear range from 0.28 μmol/L to 116.5 μmol/L and a detection limit of 0.12 μmol/L. The Michaelis-Menten constant KMapp value was estimated to be 0.3 mmol/L. The resulting biosensor exhibited fast amperometric response, and good stability, reproducibility, and selectivity to H2O2.
Co-reporter:Wei Wang;Wenya Wu;Fang Zhou;Jian-Rong Zhang;Qiang Miao
Chromatographia 2009 Volume 69( Issue 9-10) pp:897-901
Publication Date(Web):2009 May
DOI:10.1365/s10337-009-0996-0
Current-monitoring method is a widely used approach to measure electroosmotic flow (EOF) in microchip, but low and zero EOF is difficult to be measured. In this report, the mechanism of current-monitoring method was explained with Kohlraush regulation function principle, and an improved current-monitoring method was developed for low EOF measurement with tilting microchip. Fluid flow in the channel was accelerated with the help of hydrostatic pressure generated by tilting microchip, the time of dilute solution displacing the concentrated one in channel was shortened. EOF could be calculated according to the time difference between twice experiments under two different applied voltages by tilting microchip. Low even zero EOF could be measured by this improved current-monitoring method. Three modified microchips were characterized to verify the method. EOF in microchannels modified with poly(vinyl alcohol), bovine serum albumin and myoglobin were 0.27 ± 0.05, 0.16 ± 0.05 and −0.45 ± 0.04 × 10−4 cm2 V−1 s−1, respectively.
Co-reporter:JingJing Zhang;JunJie Zhu
Science China Chemistry 2009 Volume 52( Issue 6) pp:815-820
Publication Date(Web):2009 June
DOI:10.1007/s11426-009-0079-y
We report a novel bienzyme biosensor based on the assembly of the glucose oxidase (GOD) and horseradish peroxidase (HRP) onto the gold nanoparticles encapsulated mesoporous silica SBA-15 composite (AuNPs-SBA-15). Electrochemical behavior of the bienzyme bioconjugates biosensor is studied by cyclic voltammetry and electrochemical impedance spectroscopy. The results indicate that the presence of mesoporous AuNPs-SBA-15 greatly enhanced the protein loadings, accelerated interfacial electron transfer of HRP and the electroconducting surface, resulting in the realization of direct electrochemistry of HRP. Owing to the electrocatalytic effect of AuNPs-SBA-15 composite, the biosensor exhibits a sensitive response to H2O2 generated from enzymatic reactions. Thus the bienzyme biosensor could be used for the detection of glucose without the addition of any mediator. The detection limit of glucose was 0.5 μM with a linear range from 1 to 48 μM.
Co-reporter:XiaoJun Chen;Jie Xuan;LiPing Jiang;JunJie Zhu
Science China Chemistry 2009 Volume 52( Issue 11) pp:
Publication Date(Web):2009 November
DOI:10.1007/s11426-009-0249-y
A novel type of glucose sensor was fabricated based on a glucose oxidase (GOD)-N,N-dimethtylformamide (DMF)-[BMIm][BF4] composites modified three-dimensional ordered macroporous (3DOM) gold film electrode. The immobilized GOD exhibits a pair of well-defined reversible peaks in 50 mM pH 7.0 phosphate buffer solutions (PBS), which could be attributed to the redox of flavin adenine dinucleotide (FAD) in GOD. The research results show that ionic liquid ([BMIm][BF4]), DMF and 3DOM gold film are crucial for GOD to exhibit a pair of stable and reversible peaks. It is believed that the large active area of 3DOM gold film can increase the amount of immobilized GOD. Simultaneously, the application of IL enhances the stability of GOD and facilitates the electron transfer between GOD and the electrode. The synergetic effect of DMF can help the GOD to maintain its bioactivity better. GOD immobilized on the electrode exhibits the favorable electrocatalytic property to glucose, and the prepared sensor has a linear range from 10 to 125 nM with a detection limit of 3.3 nM at a signal-to-noise ratio of 3σ. The apparent Km (Michaelis- Menten constant) for the enzymatic reaction is 0.018 mM.
Co-reporter:Miaomiao Gu, Jingjing Zhang, Ye Li, Liping Jiang, Jun-Jie Zhu
Talanta 2009 Volume 80(Issue 1) pp:246-249
Publication Date(Web):15 November 2009
DOI:10.1016/j.talanta.2009.06.065
Gold nanoparticles (AuNPs) were assembled on the surface of polystyrene (PS) and polyaniline (PANI) core–shell nanocomposite (PS@PANI) for the immobilization of HL-60 leukemia cells to fabricate a cell electrochemical sensor. The immobilized cells exhibited irreversible voltammetric response and increased the electron transfer resistance with a good correlation to the logarithmic value of concentration ranging from 1.6 × 103 to 1.6 × 108 cells mL−1 with a limit of detection of 7.3 × 102 cells mL−1 at 10σ. This biosensor was simple, low cost and disposable, which implied that the PS@PANI/Au composites can regard as the potential applications for clinical applications.
Co-reporter:Rongjing Cui;Chang Liu;Jianming Shen;Di Gao;Hong-Yuan Chen
Advanced Functional Materials 2008 Volume 18( Issue 15) pp:2197-2204
Publication Date(Web):
DOI:10.1002/adfm.200701340
Abstract
A rapid microwave-hydrothermal method has been developed to prepare monodisperse colloidal carbon nanospheres from glucose solution, and gold nanoparticles (AuNPs) are successfully assembled on the surface of the colloidal carbon nanospheres by a self-assembly approach. The resulting AuNP/colloidal carbon nanosphere hybrid material (AuNP/C) has been characterized and is expected to offer a promising template for biomolecule immobilization and biosensor fabrication because of its satisfactory chemical stability and the good biocompatibility of AuNPs. Herein, as an example, it is demonstrated that the as-prepared AuNP/C hybrid material can be conjugated with horseradish peroxidase-labeled antibody (HRP-Ab2) to fabricate HRP-Ab2-AuNP/C bioconjugates, which can then be used as a label for the sensitive detection of protein. The amperometric immunosensor fabricated on a carbon nanotube-modified glass carbon electrode was very effective for antibody immobilization. The approach provided a linear response range between 0.01 and 250 ng mL−1 with a detection limit of 5.6 pg mL−1. The developed assay method was versatile, offered enhanced performances, and could be easily extended to other protein detection as well as DNA analysis.
Co-reporter:Wen-Yi Cai;Liang-Dong Feng;Shan-Hu Liu
Advanced Functional Materials 2008 Volume 18( Issue 20) pp:3127-3136
Publication Date(Web):
DOI:10.1002/adfm.200800531
Abstract
A Hemoglobin-CdTe-CaCO3@polyelectrolyte 3D architecture is synthesized by a stepwise layer-by-layer method and is further used to fabricate an electrochemistry biosensor. While the calcium carbonate (CaCO3) microsphere acts as an effective host for the loading of cadmium telluride (CdTe) quantum dots due to its channel-like structure, the polyelectrolyte layers further increase the loading amount and help in the formation of a thick and uniform quantum-dot “shell”, which not only improves the stability of the spheres in water, but also contributes to the fast and effective direct electron transfer between the protein redox center and the macroscopic electrode. The materials are characterized and compared, and the possible mechanism for the direct electrochemistry phenomenon is hypothesized. Our work not only provides a facile and effective route for the preparation of quantum-dot-loaded spheres, but also sets an example of how the structure of functional materials can be tuned and related to their applications. In addition, it is one of the few examples of using CaCO3 microspheres in quantum-dot loading and biosensing.
Co-reporter:Hongcheng Pan;Hongyu Lin;Qingming Shen
Advanced Functional Materials 2008 Volume 18( Issue 22) pp:3692-3698
Publication Date(Web):
DOI:10.1002/adfm.200800492
Abstract
Luminescent cadmium(II) (8-hydroxyquinoline) chloride (CdqCl) complex nanowires are synthesized via a sonochemical solution route. The results of X-ray photoelectron spectroscopy, energy dispersive X-ray analysis, infrared spectroscopy, elemental analysis (EA), and atomic absorption spectroscopy demonstrate that the chemical composition of the product is Cd(C9H6NO)Cl. Transmission electron microscopy and scanning electron microscopy images show that the CdqCl product is wire-like in structure, with a diameter of approximately 50 nm and an approximate length of 2–4 µm. The morphology and composition of the product can be transformed from Cdq2 micrometer-scaled flakes to CdqCl nanowires by increasing the ratio of CdCl2/q. A new fluorescent sensing strategy for detecting H2O2 and glucose is developed and is based on the combination of the luminescent nanowires and the biocatalytic growth of Au nanoparticles. The quenching effects of Au nanoparticles and on the fluorescence of CdqCl nanowires are investigated. The dominant factor for the fluorescence quenching of CdqCl nanowires is that the Stern–Volmer quenching constant of Au nanoparticles is larger than that of .
Co-reporter:Jian-Min Shen, Lin Xu, Yu-Ge Liu, Chun-Liang Lu, Wen-Hua Hou and Jun-Jie Zhu
Chemistry of Materials 2008 Volume 20(Issue 9) pp:3034
Publication Date(Web):April 10, 2008
DOI:10.1021/cm702966x
In this paper, bunches of amorphous carbon nanotubes (α-CNTs) have been successfully synthesized on a large scale from a solution-based reaction between ferrocene and carbon tetrachloride at 180 °C for 12 h. The α-CNT is 3−5 µm in length and ∼300/200 nm in diameter (outer/inner) and has a Brunauer–Emmett–Teller (BET) specific surface area of 431 m2 g−1 with a narrow pore distribution centered at 4.03 nm. The as-prepared α-CNTs showed a reversible capacity of ∼302 mA h g−1 and little hysteresis in the charge/discharge experiments of secondary lithium ion batteries, which suggested that the α-CNTs might become a new candidate as an electrode material in secondary lithium-ion batteries. Herein, a possible self-seeded surface-deposition growth mechanism of these α-CNTs has been proposed. This mechanism is of importance to understand the nucleation process in the solution phase and growth of other nanotubes through a similar seeded deposition process.
Co-reporter:Jian-Jun Miao, Gui-Fen Jie, Yu-Ping Chen, Lei Zhang, Li-Ping Jiang and Jun-Jie Zhu
Chemical Communications 2008 (Issue 32) pp:3762-3764
Publication Date(Web):13 Jun 2008
DOI:10.1039/B803645D
Novel chalcogenide lifebelts have been prepared by using a simple sacrificial template method, and their electrogenerated chemiluminescence properties were studied.
Co-reporter:Guifen Jie, Jingjing Zhang, Danchen Wang, Chao Cheng, Hong-Yuan Chen and Jun-Jie Zhu
Analytical Chemistry 2008 Volume 80(Issue 11) pp:4033
Publication Date(Web):April 25, 2008
DOI:10.1021/ac800052g
A novel strategy for the enhancement of electrochemiluminescence (ECL) was developed by combining CdSe nanocrystals (NCs), carbon nanotube−chitosan (CNT−CHIT), and 3-aminopropyl-triethoxysilane (APS). A label-free ECL immunosensor for the sensitive detection of human IgG (HIgG) was fabricated. The colloidal solution containing CdSe NCs/CNT−CHIT composite was first covered on the Au electrode surface to form a robust film, which showed high ECL intensity and good biocompatibility. After APS as a cross-linker was covalently conjugated to the CdSe NCs/CNT−CHIT film, the ECL intensity was greatly enhanced. And, an intensity about 20-fold higher than that of the CdSe NCs/CNT−CHIT film was observed. After antibody was bound to the functionalized film via glutaric dialdehyde (GLD), the modified electrode could be used as an ECL immunosensor for the detection of HIgG. The specific immunoreaction between HIgG and antibody resulted in the decrease in ECL intensity. The ECL intensity decreased linearly with HIgG concentration in the range of 0.02−200 ng mL−1, and the detection limit was 0.001 ng mL−1. The immunosensor has the advantages of high sensitivity, speed, specificity, and stability and could become a promising technique for protein detection.
Co-reporter:Fang Zhou, Wei Wang, Wen-Ya Wu, Jian-Rong Zhang, Jun-Jie Zhu
Journal of Chromatography A 2008 Volume 1194(Issue 2) pp:221-224
Publication Date(Web):20 June 2008
DOI:10.1016/j.chroma.2008.03.085
A novel method for low electroosmotic flow (EOF) rates measurement by tilting microchip which based upon the hydrostatic pressure conception and sampling zone method is described. Sampling zone could be detected in the tilting microchip but not in non-tilting one due to the hydrostatic pressure driven. The method is fulfilled to calculate low EOF rates by detecting the liquid flow velocity driven by hydrostatic pressure, and difference between the apparent mobility of the migrating analyte in two modes is caused by the effect of hydrostatic pressure. And then the EOF rates in unknown low EOF microchip can be calculated. Different microchannels modified with bovine serum albumin (BSA), myoglobin (MB) and polyvinyl alcohol (PVA) were used to verify the method, the EOF rate value was 1.73 ± 0.03, 1.21 ± 0.05, 0.34 ± 0.04 × 10−4 cm2 V−1 s−1, respectively. The results obtained by the proposed method were agreed well with conventional methods.
Co-reporter:Bo Zhou, Yong Ji, Yu-Fei Yang, Xing-Hua Li and Jun-Jie Zhu
Crystal Growth & Design 2008 Volume 8(Issue 12) pp:4394-4397
Publication Date(Web):November 12, 2008
DOI:10.1021/cg7011815
A simple and rapid microwave-assisted wet chemical route was developed for the preparation of Sb2Te3 hexagonal single-crystalline nanoplates with edge length of hundreds of nanometers. The products were characterized with X-ray powder diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), and selected area electron diffraction (SAED) techniques. The reaction mechanism was proposed and the effects of alkali, solvents, and stimulating factors such as ultrasonic wave and solvothermal process were studied. The effects of some additives were also discussed, and PVP (polyvinyl pyrrolidone) was found to be able to regularize and diminish the nanoplates.
Co-reporter:Dai Lin, Xu Jin-Zhong, Ding Tao, Zhu Jun-Jie, Wu Bin, Shen Chong-Yu, Jiang Yuan
Chinese Journal of Analytical Chemistry 2008 Volume 36(Issue 1) pp:87-90
Publication Date(Web):January 2008
DOI:10.1016/S1872-2040(08)60014-6
An analytical method was developed for the determination of tebufenozide and methoxyfenozide residues in vegetables. The procedure involves the extraction of tebufenozide and methoxyfenozide using alkali acetonitrile before solid-phase purification from the matrices. The tebufenozide and methoxyfenozide residues were subsequently determined by an electrospray mass spectrometer after separated by the reversed-HPLC. Mass Spectrum acquisition applied Selected Reaction Monitoring (SRM) to diagnostic transition reactions. The qualitative results were obtained based on the retention time, the precursor ion and two daughter ions, and the quantitative results were based on the intension of the characteristic m/z 297 ion and m/z 149 ion. The linear range was from 5.0–200 ng ml−1 and the correlation coefficients (r) were higher than 0.996. The average recovery ranges from 90% to 110% for tebufenozide and 70% to 80% for methoxyfenozide in the replicate sets of vegetable samples fortified with drug concentration of 4.0, 10.0 and 20 μg kg−1, and the relative standard deviations (RSD) were less than 8%. The detection limit and the quantification limit of the method were 1.0 and 4.0 μg kg−1, respectively. This method is quite suitable for determining the residues of tebufenozide and methoxyfenozide in vegetables.
Co-reporter:Hongcheng Pan, Rongjing Cui and Jun-Jie Zhu
The Journal of Physical Chemistry B 2008 Volume 112(Issue 51) pp:16895-16901
Publication Date(Web):December 4, 2008
DOI:10.1021/jp807251k
A near-infrared (NIR) fluorescence sensing strategy for glucose and xanthine has been developed based on the interaction between CdTe quantum dots (QDs) and biocatalytic generated Au nanoparticles. The fluorescence of CdTe QDs is modulated by changing concentration of AuCl4− and Au nanoparticles during the growth process of Au nanoparticles. Two cases were considered. In the first case, the glucose oxidase (GOx) catalyzes the oxidation of glucose to generate H2O2. Under the catalysis of Au nanoparticles seeds, the AuCl4− is reduced by the H2O2 to form the Au nanoparticles. In the second case, the xanthine oxidase acts as the reducing reagents to reduce AuCl4− forming Au nanoparticles. The interaction between CdTe quantum dots (QDs), AuCl4−, and Au nanoparticles resulted in the fluorescence changes of CdTe QDs, allowing the detection of glucose and xanthine. The effects of Au nanoparticles and AuCl4− on the fluorescence of CdTe QDs were discussed. A model was developed to explain the mechanism of the CdTe QDs fluorescence changes by biocatalytic growth of Au nanoparticles. The difference in the Stern−Volmer quenching constant between AuCl4− and Au nanoparticles is the dominant factor for the CdTe QDs fluorescence changes. The developed method provides low limits of detection, wide linear ranges, and detection wavelengths in the NIR region and can be easily extended to other substrate/oxidase systems.
Co-reporter:Qingming Shen, Liping Jiang, Hui Zhang, Qianhao Min, Wenhua Hou and Jun-Jie Zhu
The Journal of Physical Chemistry C 2008 Volume 112(Issue 42) pp:16385-16392
Publication Date(Web):2017-2-22
DOI:10.1021/jp8060043
A new and convenient sonoelectrochemical method was used to synthesize uniform three-dimensional (3D) dendritic Pt nanostructures (DPNs) at room temperature. The size and morphology of the final product could be controlled via simply adjusting the experiment parameters. The morphology and structure of the DPNs were characterized by transmission electron microscopy, high resolution transmission electron microscopy, field emission scanning electron microscopy, energy-dispersive X-ray, and X-ray diffraction. The formation process of the DPNs was carefully studied, and a spontaneous assembly mechanism was proposed based on the experimental results. Additionally, the electrocatalytic activity of the DPNs was evaluated using methanol and glucose as model molecules. The DPNs showed improved electrocatalytic activity toward methanol oxidation with respect to the monodisperse Pt nanoparticles; this improvement is due to the porosity structure and the greatly enhanced effective surface area. In addition, a sensitive enzyme-free biosensor can be easily developed for the detection of glucose in pH 7.4 phosphate buffer solution. The present method provides a new and simple strategy toward the fabrication of 3D DPNs with extensive applications.
Co-reporter:Yuge Liu, Xiaomiao Feng, Jianmin Shen, Jun-Jie Zhu and Wenhua Hou
The Journal of Physical Chemistry B 2008 Volume 112(Issue 30) pp:9237-9242
Publication Date(Web):July 4, 2008
DOI:10.1021/jp801938w
A novel nanocomposite with a core−shell structure containing polystyrene (PS), polyaniline (PANI), and Au nanoparticles (NPs) was synthesized. The nanocomposite was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). Cyclic voltammetric experiments indicated that the nanocomposite had excellent redox ability in a wide range of pH values. The existence of Au NPs resulted in a higher electrical conductivity of the nanocomposite. As a model, glucose oxidase (GOD) was entrapped onto the nanocomposite-modified glassy carbon electrode (GCE) and applied to construct a sensor. The immobilized GOD showed a pair of well-defined redox peaks and high catalytic activity for the oxidation of glucose.
Co-reporter:Liang-Dong Feng, Jian-Min Shen, Xing-Hua Li and Jun-Jie Zhu
The Journal of Physical Chemistry C 2008 Volume 112(Issue 20) pp:7617-7623
Publication Date(Web):April 24, 2008
DOI:10.1021/jp801129c
A facile electrochemical approach was developed for the controllable synthesis of bismuth hexacyanoferrate(II) (BiHCF(II)) nanoplates. The composition, morphology, and structure of the as-prepared BiHCF(II) nanoplates were characterized by the techniques such as infrared spectrum, thermogravimetry, inductively coupled plasma mass spectroscopy, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectrum, powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and selected area electron diffraction. The formula of the prepared BiHCF(II) nanoplates could be assigned to KBi[Fe(CN)6]·xH2O. It was observed that the nanoplates and their flowerlike aggregations could be obtained in the electrolytes containing different concentration of HNO3. The nanoplates were prepared at the potential for 0.2 V (versus SCE) and could be further grown to a good single-crystalline hexagonal microstructure at 0.6 V. To the best of our knowledge, the structures have not been reported before. The modified Au electrode by the BiHCF(II) nanoplates showed good electrochemical properties, especially with a stable anodic response over the pH range from 2.0 to 11.0. Also, the electrode possesses prominent electrocatalytic activity toward the reduction of hydrogen peroxide.
Co-reporter:Xianwen Kan, Qun Zhao, Zhong Zhang, Zhilin Wang, Jun-Jie Zhu
Talanta 2008 Volume 75(Issue 1) pp:22-26
Publication Date(Web):15 March 2008
DOI:10.1016/j.talanta.2007.08.038
A one-step precipitation polymerization synthesis was adopted for the preparation of molecularly imprinted polymers (MIPs) by using hydroquinone as a template molecule. The transmission electron microscopy (TEM) exhibited that the polymers were uniform spheres with the diameter of about 700 nm. The results of adsorption experiments showed that the microspherical imprinted polymers possessed fast adsorption dynamics. Compared to the structurally similar compounds, catechol and resorcinol, the MIPs exhibited a high recognizable capacity to hydroquinone. And the electrochemical sensor fabricated by modifying the prepared MIPs microsphere on the glassy carbon electrode surface was used to detect the hydroquinone concentration. The current response was proportional to the concentration of hydroquinone in the range of 2.0 × 10−6 to 1.0 × 10−4 mol/L with the detection limit of 1.0 × 10−6 mol/L.
Co-reporter:Bo Zhou, Bo Liu, Li-Ping Jiang, Jun-Jie Zhu
Ultrasonics Sonochemistry 2007 Volume 14(Issue 2) pp:229-234
Publication Date(Web):February 2007
DOI:10.1016/j.ultsonch.2006.04.001
Bi2Te3 hexagonal nanoflakes with controllable edge length ranging from ∼150 nm to as small as ∼10 nm were synthesized via an ultrasonic-assisted disproportionation route, using Te powder and Bi(NO3)3 · 5H2O as raw materials. The mechanochemical effects of the ultrasonic irradiation accelerated the reaction and were helpful to obtain relatively small and uniform nanocrystals. The products were characterized by X-ray powder diffraction, X-ray photoelectron spectra, transmission electron microscopy, and selected area electron diffraction techniques. Electrogenerated chemiluminescence of as-prepared Bi2Te3 was also reported for the first time.
Co-reporter:Qin Xu, Jun-Jie Zhu, Xiao-Ya Hu
Analytica Chimica Acta 2007 Volume 597(Issue 1) pp:151-156
Publication Date(Web):30 July 2007
DOI:10.1016/j.aca.2007.06.034
Co-reporter:Vijay Singh, T.K. Gundu Rao, Jun-Jie Zhu
Journal of Luminescence 2007 Volume 126(Issue 1) pp:1-6
Publication Date(Web):September 2007
DOI:10.1016/j.jlumin.2006.04.003
The present paper describes the synthesis of europium-doped calcium aluminate phosphor using the combustion method. An efficient blue emission phosphor can be prepared at reaction temperatures as low as 500 °C in a few minutes by this method. Characterization of the powder was done by X-ray diffraction, transmission electron microscopy, scanning electron microscope analysis and the optical properties were studied by photoluminescence spectra. Thermoluminescence (TL) studies also have been carried out on CaAl12O19:Eu2+ phosphor. The TL glow curve shows peaks at 174 and 240 °C. Defect centres formed in irradiated phosphor have been studied using the technique of electron spin resonance. Step annealing measurements indicate that one of the annealing stages of a defect centre appear to correlate with the release of carriers resulting in TL peak at 174 °C. The centre is characterized by an isotropic g-value of 2.0046 and is assigned to a F+ centre.
Co-reporter:Hongcheng Pan, Xiancong Tao, Changjie Mao, Jun-Jie Zhu, Fupei Liang
Talanta 2007 Volume 71(Issue 1) pp:276-281
Publication Date(Web):15 January 2007
DOI:10.1016/j.talanta.2006.03.057
A novel method was proposed to prepare a series of functionalized Ag2S nanoparticles capped with various aminopolycarboxylic acids. The as-prepared Ag2S nanoparticles were characterized by UV–vis, FTIR, resonance light scattering spectra (RLS) and transmission electron microscopy (TEM). Based on the RLS intensities enhanced by BSA-induced Ag2S nanoparticles aggregation, a sensitive RLS method for the detection BSA at nanogram levels was established. The detection limits for BSA are between 8.6 and 112.6 ng mL−1, depending on the different capping agents. The effects of various capping agents on the detection limits of BSA have been investigated. The detection limit is found to be dependent on the stability constant (log KMY) of the silver–aminopolycarboxyl complexes.
Co-reporter:Hui Yao, Nan Li, Jin-Zhong Xu, Jun-Jie Zhu
Talanta 2007 Volume 71(Issue 2) pp:550-554
Publication Date(Web):15 February 2007
DOI:10.1016/j.talanta.2006.04.025
Co-reporter:Bo Zhou, Jian-Rong Zhang, Liang Zhao, Jian-Min Zhu, Jun-Jie Zhu
Ultrasonics Sonochemistry 2006 Volume 13(Issue 4) pp:352-358
Publication Date(Web):May 2006
DOI:10.1016/j.ultsonch.2005.05.004
An ultrasonic-assisted solution-phase approach to tellurium bundles of nanowhiskers has been successfully established. It is a convenient and efficient process for the formation of Te nanowhiskers and their simultaneous assembly into tellurium bundles without using any templates. It was found that the transformation from Te powder to Te nanowhiskers involved the reversible disproportionation of tellurium. Sonication played a critical role for the formation of the Tellurium bundles of nanowhiskers. The bandgap of the Te nanowhiskers was calculated to be about 3.8 eV based on the UV–visible spectrum. The simplicity and rapidity of the procedure, and the newly discovered uniform morphology of the products made this synthesis promising and potential for related future applications.
Co-reporter:Gang Yang;Xiaomiao Feng;Wenhua Hou;Qin Xu
Macromolecular Rapid Communications 2006 Volume 27(Issue 1) pp:31-36
Publication Date(Web):19 DEC 2005
DOI:10.1002/marc.200500642
Summary: Polyaniline (PANI)/Au composite nanotubes and nanofibers are synthesized through a self-assembly process in the presence of camphorsulfonic acid and hydrochloric acid, as dopants, respectively. The PANI/Au composites are characterized by FT-IR, UV-vis, and thermogravimetric analysis to verify the incorporation of the Au nanoparticles and determine the Au content. Structural characterization is performed using SEM, TEM and X-ray diffraction. The presence of the Au nanoparticles results in an increased conductivity and improved crystallinity of the PANI. The self-assembly method employed here is a simple and inexpensive route to synthesize multifunctional nanotubes and nanofibers and could be extended to prepare other inorganic nanoparticle/PANI composites.
Co-reporter:Xiaomiao Feng;Yuge Liu;Gang Yang;Wenhua Hou
Journal of Applied Polymer Science 2006 Volume 101(Issue 3) pp:2088-2094
Publication Date(Web):24 MAY 2006
DOI:10.1002/app.23836
Polyaniline (PANI)/porous silica MCM-41 (MCM-41) composite was synthesized according to surface polymerization theory, and it was confirmed through comparing with PANI/solid silica (SiO2) by TGA and XPS techniques. The morphology and composition of the composite were also characterized by some techniques such as small-angle XRD, N2-adsorption isotherm, SEM, FTIR, and UV–vis. The thermal stability for the PANI/MCM-41 composite was enhanced when compared with that of pure PANI. With the increase in the concentration of HCl, the doping degree increased and UV-absorption peak at about 700 nm showed a red shift. The conductivity of the composite was enhanced by increasing the concentration of HCl. The results of FTIR showed that there was a strong interaction between PANI and MCM-41. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 2088–2094, 2006
Co-reporter:Vijay Singh, T.K. Gundu Rao, Jun-Jie Zhu
Journal of Solid State Chemistry 2006 Volume 179(Issue 8) pp:2589-2594
Publication Date(Web):August 2006
DOI:10.1016/j.jssc.2006.04.053
Preparation of Eu2+ ions activated strontium hexa-aluminate phosphor using the combustion method is described. An efficient phosphor can be prepared by this method at reaction temperatures as low as 500 °C in a few minutes. Powder X-ray diffraction (XRD), transmission electron microscopy, scanning electron microscope analysis were used to characterize the as prepared product and the optical properties were studied by photoluminescence (PL) spectra. Thermally stimulated luminescence studies also have been carried out on SrAl12O19:Eu2+ phosphor. The TSL glow curve is broad and indicates two dominant peaks at 206 and 345 °C. Defect centres formed in irradiated phosphor have been studied using the technique of electron spin resonance. One of the centres is characterized by an isotropic g-value of 2.0055 and is assigned to a F+ centre. The two annealing stages of F+ centre in the region 125–230 and 340–390 °C appear to correlate with the release of carriers resulting in TSL peaks at 206 and 345 °C, respectively.SEM image of SrAl12O19:Eu
Co-reporter:Bo Zhou, Yu Zhao, Lin Pu, Jun-Jie Zhu
Materials Chemistry and Physics 2006 Volume 96(2–3) pp:192-196
Publication Date(Web):10 April 2006
DOI:10.1016/j.matchemphys.2005.07.010
Nanocrystalline Bi2Te3 was synthesised via a microwave-assisted polyol method. Elemental Te and bismuth nitrate were used as Te and Bi source, respectively. The product was characterized by powder X-ray diffraction (XRD), selected area electron diffraction (SAED), X-ray photoelectron spectra (XPS) and transmission electron micrographs (TEM) measurements. The as-prepared Bi2Te3 was found to be the mixture of nanorods (20–50 nm in width and 200–400 nm in length) and hexagon nanoflakes (with edge length ranging from 90 to 150 nm). The possible mechanisms were also discussed.
Co-reporter:Vijay Singh, T.K. Gundu Rao, Jun-Jie Zhu, Manoj Tiwari
Materials Science and Engineering: B 2006 Volume 131(1–3) pp:195-199
Publication Date(Web):15 July 2006
DOI:10.1016/j.mseb.2006.04.015
Cerium dope CaS phosphor has been successfully prepared by solid state diffusion method. The phosphor is characterized by X-ray powder diffraction, transmission electron microscopy, selected area electron diffraction, thermogravimetric analysis and photoluminescence. Thermoluminescence and electron spin resonance studies also have been carried out on CaS:Ce phosphor. Irradiated CaS:Ce exhibits electron spin resonance (ESR) lines due to defect centres. The thermal annealing behaviour of one of the defect centres appears to correlate with the thermoluminescence (TL) peak at 135 °C. The centre is characterized by an isotropic g-value of 2.0036 and is assigned to a F+ centre.
Co-reporter:Ting Ren, Jin-Zhong Xu, Yi-Feng Tu, Shu Xu, Jun-Jie Zhu
Electrochemistry Communications 2005 Volume 7(Issue 1) pp:5-9
Publication Date(Web):January 2005
DOI:10.1016/j.elecom.2004.10.005
We report the first observation of electrogenerated chemiluminescence (ECL) from CdS spherical assemblies in both nonaqueous system and aqueous system. The CdS spherical assemblies consist of CdS nanocrystals about 5 nm in diameter. Four ECL peaks were found under cyclic voltammetric conditions. According to the annihilation mechanism and two-equivalent adsorbed surface state theory, the mechanism for ECL peaks was proposed. The morphology of the CdS spherical assemblies is proved to play an important role in maintaining the stability of partial electrogenerated species to generate the ECL light.
Co-reporter:Ming Yang, Jun-Jie Zhu, Jian-Jun Li
Materials Letters 2005 Volume 59(Issue 7) pp:842-845
Publication Date(Web):March 2005
DOI:10.1016/j.matlet.2004.10.063
Porous spheres of CuSCN nanoparticles with an average diameter of 0.4–0.6 μm have been prepared by a simple reaction between CuO suspension, NH2OH and KSCN in the presence of gelatin at 10 °C. Gelatin played a decisive role as an inhibitor of the direct attack of NH2OH, KSCN to CuO surfaces and coagulation of the growing CuSCN in producing porous spheres. The products were characterized by X-ray powder diffraction, transmission electron microscopy, and X-ray photoelectron spectra techniques.
Co-reporter:Yao Hui;Li Nan;Xu Jing-Zhong;Zhu Jun-Jie
Chinese Journal of Chemistry 2005 Volume 23(Issue 3) pp:
Publication Date(Web):4 APR 2005
DOI:10.1002/cjoc.200590275
A simple and promising glucose biosensor was constructed by successful entrapment of glucose oxidase (GOD) into chitosan matrix, which was cross-linked with glutaraldehyde (GA). This material provided good biocompatibility and the stabilizing microenvironment around the enzyme. The morphologies and properties of chitosan and chitosan/GOD were characterized by FTIR, UV-Vis and SEM techniques. This biosensor exhibited a fast amperometric response to glucose. The linear range for glucose determination was from 1×10−5 to 3.4×10−3 mol·L−1, with a detection limit of 5×10−6 mol·L−1 based on S/N=3. The biosensor could retaCin ca. 90% of its original activity after two weeks of storage under dry conditions at 4 °C.
Co-reporter:Bo Zhou, Jian-Min Hong, Jun-Jie Zhu
Materials Letters 2005 Volume 59(24–25) pp:3081-3084
Publication Date(Web):October 2005
DOI:10.1016/j.matlet.2005.05.026
Antimony dendrites have been successfully synthesized by a microwave-assisted method under ambient air from the solution containing antimony sodium tartrate. In the reaction, zinc powders were selected as a reductant for the fabrication. The as-prepared products were characterised by X-ray powder diffraction, transmission electron microscopy, and selected area electron diffraction. The dendrites were found to be composed of well-crystallized nanoflakes with size of 20–40 nm.
Co-reporter:Shu Xu, Wen-bo Zhao, Jian-Min Hong, Jun-Jie Zhu, Hong-Yuan Chen
Materials Letters 2005 Volume 59(2–3) pp:319-321
Publication Date(Web):February 2005
DOI:10.1016/j.matlet.2004.10.011
A photochemical reaction route was developed to synthesize bismuth selenide (Bi2Se3) nanoparticles and nanorods. In an aqueous solution, bismuth nitrate (Bi(NO3)3) reacted with sodium selenosufate in the presence of reducing agent and complexing agent, and the dispersed Bi2Se3 nanoparticles were obtained with the average size of 35 nm. The nanorods were prepared via an alumina template route in the same solution. We carried out experiments to study the formation mechanism in the morphology control of the products and found that series of factors played an effective role including the irradiation time, pH value, the reducing agents and the species of complexing agents. The products were characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM).
Co-reporter:Ming Yang, Jun-Jie Zhu
Materials Research Bulletin 2005 Volume 40(Issue 2) pp:265-270
Publication Date(Web):15 February 2005
DOI:10.1016/j.materresbull.2004.10.016
Nanoribbons and monodispersed nanocrystals of CuBr have been prepared by a simple reaction between CuO suspension, NH2OH·HCl and KBr in the presence of deionized gelatin at 10 °C. The products were characterized by X-ray powder diffraction, transmission electron microscopy and UV–vis absorption spectroscopy. The sizes of the monodispersed nanocrystals of CuBr were estimated by Debye-Scherrer formula according to XRD spectrum.
Co-reporter:Hui Wang, Jun-Jie Zhu
Ultrasonics Sonochemistry 2004 Volume 11(Issue 5) pp:293-300
Publication Date(Web):July 2004
DOI:10.1016/j.ultsonch.2003.06.002
A novel sonochemical method for the selective synthesis of α-HgS (cinnabar) and β-HgS (metacinnabar) nanoparticles in aqueous solutions is reported in this paper. α-HgS and β-HgS nanoparticles have been selectively prepared by choosing sodium thiosulfate and thiourea as the sulfur source respectively. To study the crystalline structure, size, morphology and composition of the products, characterization techniques including X-ray powder diffraction, transmission electron microscopy, selected area electron diffraction, X-ray photoelectron spectroscopy and energy-dispersive X-ray analysis are employed. The optical properties of the nanoparticles are investigated by UV–visible absorption spectroscopic measurements. The direct band gap of the as-prepared α-HgS nanoparticles with an average size of 12 nm is calculated to be 2.8 eV according to the absorption spectrum. In the case of the β-HgS nanoparticles with an average size of 13 nm, a broad absorption peak is observed in the UV–visible absorption spectrum, which can be ascribed to the special surface state of this sample. Probable mechanisms for the sonochemical formation of α-HgS and β-HgS nanoparticles in aqueous solutions are presented. The optimum pH value of the stock solutions and the effect of sonication time on the particle size are also investigated.
Co-reporter:Shu Xu;Hui Wang;Xin-Quan Xin;Hong-Yuan Chen
European Journal of Inorganic Chemistry 2004 Volume 2004(Issue 23) pp:
Publication Date(Web):7 OCT 2004
DOI:10.1002/ejic.200400242
An ultrasound-assisted in situ template approach has been developed for fabricating a series of nanoscale metal chalcogenides in the form of well-defined hollow spherical assemblies. These hollow spherical assemblies have well-controlled dimensions and are composed of uniform nanoparticles. Initially, metal hydroxide particles self-assemble into spherical templates generated in situ, and subsequent surface crystal growth leads to hollow spherical structures. Ultrasound irradiation plays a critical role both in the formation of the intermediate templates and in the crystal-growth process. This approach provides a convenient and efficient one-step pathway to the large-scale fabrication of hollow spherical nanostructures. It also represents a new demonstration of sonochemical effects on the formation and assembly of crystalline particles on the nanometer scale. (© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2004)
Co-reporter:Yu Zhao, Xue-Hong Liao, Jian-Min Hong, Jun-Jie Zhu
Materials Chemistry and Physics 2004 Volume 87(Issue 1) pp:149-153
Publication Date(Web):September 2004
DOI:10.1016/j.matchemphys.2004.05.026
Lead sulfide nanocrystals have been prepared by two novel routes in microwave heating and ultrasonic irradiation. In the experiments, lead acetate and thiourea are used as lead source and sulfur source, respectively. Different size and morphology of lead sulfide (PbS) nanocrystals can be obtained by using ethanol, distilled water, ethylene glycol and polyethylene glycol-200 as solvents. X-ray diffraction results show that the as-prepared PbS nanocrystals have a cubic structure. Probable mechanisms for the formation of PbS particles are also proposed.
Co-reporter:J.J. Zhu;S. Xu;H. Wang;J.M. Zhu;H.-Y. Chen
Advanced Materials 2003 Volume 15(Issue 2) pp:
Publication Date(Web):27 JAN 2003
DOI:10.1002/adma.200390033
Co-reporter:Ming Yang and Jun-Jie Zhu
Analyst 2003 vol. 128(Issue 2) pp:178-181
Publication Date(Web):20 Jan 2003
DOI:10.1039/B211373B
A new indirect voltammetric method for the determination of hydroxylamine is described. It is based on the reduction of an electroactive derivative of hydroxylamine on the surface of a magnetic electrode. The electroactive derivative produced by hydroxylamine reacted with magnetic polymer microspheres containing carbonyl groups on the surface. The experimental conditions are discussed. It was found that the peak potential (EP) of the derivative was −0.46 V (vs. Ag/AgCl) under optimum conditions. Hydroxylamine could be determined in the range of 5–2000 μg l−1 with the detection limit of 2 μg l−1 and relative standard deviation for the determination of 100 μg l−1 hydroxylamine was 2.35%. Satisfactory results were obtained for the determination of hydroxylamine in aqueous medium.
Co-reporter:Tao Ding, Jian-Rong Zhang, Su Long, Jun-Jie Zhu
Microelectronic Engineering 2003 Volume 66(1–4) pp:46-52
Publication Date(Web):April 2003
DOI:10.1016/S0167-9317(03)00023-6
A novel and quick method for the synthesis of PbS and HgS semiconductor nanoparticles using mercury acetate and lead acetate as source materials and sulfur powder employed as chalcogenide source by microwave heating in polyethylene glycol (PEG) solvent is presented in this paper. HgS and PbS nanoparticles were obtained with average sizes from 20 to 30 nm in PEG, which acts as both solvent and reducing agent. The products were characterized by powder X-ray analysis, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The probable mechanism was presented.
Co-reporter:Hui Wang, Jun-Jie Zhu, Jian-Min Zhu, Xue-Hong Liao, Shu Xu, Tao Ding and Hong-Yuan Chen
Physical Chemistry Chemical Physics 2002 vol. 4(Issue 15) pp:3794-3799
Publication Date(Web):19 Jun 2002
DOI:10.1039/B201394K
Nanocrystalline ceria (CeO2) particles have been successfully prepared via sonochemical and microwave assisted heating routes from aqueous solutions containing (NH4)2Ce(NO3)6, hexamethylenetetramine and poly (ethylene glycol)-19000 (PEG). The products were characterized by techniques such as powder X-ray diffraction, transmission electron microscopy, high-resolution transmission electron microscopy, selected area electron diffraction, Brunauer–Emmett–Teller nitrogen adsorption and UV–Visible absorption spectroscopy. Analysis of the results showed that the products had uniform shape, narrow size distribution and displayed conspicuous quantum size effects.
Co-reporter:Hui Wang, Shu Xu, Xiao-Ning Zhao, Jun-Jie Zhu, Xin-Quan Xin
Materials Science and Engineering: B 2002 Volume 96(Issue 1) pp:60-64
Publication Date(Web):1 October 2002
DOI:10.1016/S0921-5107(02)00337-9
A novel sonochemical method for preparation of mercury selenide has been developed based on the reaction of mercury acetate and sodium selenosulfate in an aqueous system at room temperature. Different complexing agents were used to control the particle size. X-ray powder diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) were used to determine the phase, purity, size and morphology of the products. The results showed that the HgSe nanoparticles with different sizes could be obtained in the presence of complexing agents.
Co-reporter:Jing-Jing Zhang, Fang-Fang Cheng, Ting-Ting Zheng, Jun-Jie Zhu
Biosensors and Bioelectronics (15 March 2017) Volume 89(Part 2) pp:937-945
Publication Date(Web):15 March 2017
DOI:10.1016/j.bios.2016.09.087
Co-reporter:Yong-Ping Dong, Jiao Wang, Ying Peng, Jun-Jie Zhu
Biosensors and Bioelectronics (15 March 2017) Volume 89(Part 2) pp:1053-1058
Publication Date(Web):15 March 2017
DOI:10.1016/j.bios.2016.10.011
Co-reporter:Qiao Liu, Cheng Ma, Xing-Pei Liu, Yu-Pin Wei, Chang-Jie Mao, Jun-Jie Zhu
Biosensors and Bioelectronics (15 June 2017) Volume 92() pp:
Publication Date(Web):15 June 2017
DOI:10.1016/j.bios.2017.02.027
•Uniform, water-soluble and nontoxic N-C QDs were firstly synthesized.•DNA functionalized N-C QDs as signal enhancers to construct an ultrasensitive ECL biosensor to detect miRNA-21.•Nicking enzymes (Nb.BbvCI) were utilized to trigger target cycling reaction to realize efficient signal amplification.An ultrasensitive electrochemiluminescence (ECL) biosensor for the detection of microRNA was developed based on nicking enzymes Nb.BbvCI mediated signal amplification (NESA). First, the hairpin probe1-N-CQDs with assistant probe and microRNA (miRNA) formed Y junction structure which was cleaved with the addition of nicking enzymes Nb.BbvCI to release miRNA and assistant probe. Subsequently, the released miRNA and assistant probe can initiate the next recycling process. The generation of numerous intermediate sequences nitrogen doped carbon quantum dots-DNA (N-CQDs-DNA) can further hybridize with hairpin probe2 immobilized on GO/Au composite modified electrode surface, the initial ECL intensity was enhanced. The ECL intensity would increase with increasing concentration of the target miRNA, and the sensitivity of biosensor would be promoted because of the efficient signal amplification of the target induced cycling reaction. The novel designed biosensor provided a highly sensitive and selective detection of miRNA-21 from 10 aM to104 fM with a relatively low detection limit of 10 aM. Thus, our strategy has a potential application in the clinical diagnosis.
Co-reporter:Jingjing Li, Jia You, Yinping Zhuang, Cuiping Han, Junfeng Hu, Aming Wang, Kai Xu and Jun-Jie Zhu
Chemical Communications 2014 - vol. 50(Issue 54) pp:NaN7110-7110
Publication Date(Web):2014/03/21
DOI:10.1039/C4CC00160E
We have designed a novel multifunctional DNA scaffold for the synthesis of fluorescent silver nanoclusters (Ag NCs) using a one-pot approach. The obtained DNA/Ag NCs presented a “light-up” and “spectrum-shift” response to target DNA in vitro and could further image the tumor-related mRNA in living cells.
Co-reporter:Gao-Chao Fan, Hua Zhu, Qingming Shen, Li Han, Ming Zhao, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 - vol. 51(Issue 32) pp:NaN7026-7026
Publication Date(Web):2015/03/16
DOI:10.1039/C5CC01935D
High-efficient exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites was applied to develop an enhanced photoelectrochemical aptasensing platform with ultrahigh sensitivity, good selectivity, reproducibility and stability.
Co-reporter:Feng Lu, Jinfeng Wang, Lin Yang and Jun-Jie Zhu
Chemical Communications 2015 - vol. 51(Issue 46) pp:NaN9450-9450
Publication Date(Web):2015/04/30
DOI:10.1039/C5CC01725D
A facile one-pot approach was developed for the synthesis of colloidal stable, monodisperse, highly PEGylated mesoporous silica coated copper sulfide nanocomposites for the combination of photothermal therapy and chemotherapy. The proposed method can also be extended to the synthesis of other metal sulfide nanocomposites.
Co-reporter:Panpan Gai, Rongbin Song, Cheng Zhu, Yusheng Ji, Yun Chen, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 - vol. 51(Issue 79) pp:NaN14738-14738
Publication Date(Web):2015/08/06
DOI:10.1039/C5CC06062A
A novel ternary hybrid of carbon nanotubes/graphitic carbon nitride nanosheets/gold nanoparticles was prepared and used as robust substrate electrodes for fabricating membrane-less glucose/O2 enzyme biofuel cells (EBFCs), and a remarkably improved power output was observed for the prepared EBFC.
Co-reporter:Panpan Gai, Rongbin Song, Cheng Zhu, Yusheng Ji, Wengjing Wang, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Communications 2015 - vol. 51(Issue 94) pp:NaN16766-16766
Publication Date(Web):2015/09/25
DOI:10.1039/C5CC07520C
An exogenous redox-free, membrane-less enzyme biofuel cell-based ultrasensitive self-powered cytosensing platform was fabricated. With the ultrahigh sensitivity and the merits of not requiring external power sources or exogenous reagents, the device has great potential as a point-of-care tool for early diagnosis of cancer in vivo.
Co-reporter:Shanhu Liu, Feng Lu and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 9) pp:NaN2663-2663
Publication Date(Web):2011/01/12
DOI:10.1039/C0CC04276E
Highly fluorescent Ag nanoclusters were prepared in aqueous solution via a rapid microwave-assisted green approach and used as a novel fluorescence probe for the determination of Cr3+ ions with high sensitivity and excellent selectivity.
Co-reporter:Sai Bi, Bin Ji, Zhipeng Zhang and Jun-Jie Zhu
Chemical Science (2010-Present) 2013 - vol. 4(Issue 4) pp:NaN1863-1863
Publication Date(Web):2013/02/06
DOI:10.1039/C3SC00043E
Supramolecular structures composed of padlock probes and primers were used to perform rolling circle amplification (RCA) which was achieved by metal ion (Hg2+ or Ag+) induced DNA ligase activity. In the presence of Hg2+ (or Ag+), the specific and strong interaction between thymidine–thymidine and Hg2+ (or cytosine–cytosine and Ag+) at the terminal of the padlock probe enabled the circularization of the padlock probe with primer in the aid of DNA ligase. An RCA process was then accomplished by DNA polymerase/dNTPs. The RCA product containing multiple tandem repeats could hybridize with a large number of molecular beacons (reporter), resulting in an enhanced fluorescence signal. This proposed single-input YES gate enabled the sensitive and selective detection of Hg2+ (or Ag+). Additionally, based on the principle of DNA hybridization and displacement, a NOT logic gate was constructed by designing a double-stranded fluorescence probe as reporter. Significantly, this assay was further applied to the construction of a complete set of two-input molecular-scale logic gates and three advanced logic devices.
Co-reporter:Feng Lu, Adriana Popa, Shiwei Zhou, Jun-Jie Zhu and Anna Cristina S. Samia
Chemical Communications 2013 - vol. 49(Issue 97) pp:NaN11438-11438
Publication Date(Web):2013/10/30
DOI:10.1039/C3CC46658B
Magnetic field-responsive iron oxide-loaded hollow mesoporous silica nanocapsules that exhibit high drug loading capacity were synthesized using polymer nanospheres as sacrificial templates. Due to their magnetic field induced heating and remotely triggered drug release capabilities, these hybrid nanomaterials provide an excellent platform for the combination of hyperthermia and chemotherapy.
Co-reporter:
Analytical Methods (2009-Present) 2013 - vol. 5(Issue 21) pp:
Publication Date(Web):
DOI:10.1039/C3AY41189C
High-quality glutathione (GSH) capped ZnS:Mn/ZnS core/shell doped quantum dots (d-dots) with pure dopant emission band and excellent stability have been synthesized directly in aqueous media. The influences of experimental variables on the luminescent properties of the ZnS:Mn/ZnS nanocrystals have been investigated. The quantum yield of the dopant Mn photoluminescence in the as-prepared ZnS:Mn/ZnS core/shell d-dots can be up to 27.4%. The value is the highest reported to date for ZnS:Mn d-dots via the direct aqueous synthetic method. Their optical features and structure have been characterized by UV-Visible spectroscopy, photoluminescence (PL) spectroscopy, transmission electron microscopy (TEM) and X-ray diffraction (XRD) in detail. Additionally, the stability study against UV irradiation indicated that the obtained d-dots possess excellent photostability. Furthermore, the MTT assay demonstrated that the ZnS:Mn QDs do not exhibit any cytotoxicity toward HeLa cells up to a concentration of 600 μg mL−1. Using the Con A-mannose recognition system as a model, Con A functionalized ZnS:Mn/ZnS nanocrystals were prepared and successfully used for targeted mannosyl groups expression on the HeLa cells surface. Our investigation clearly shows that the GSH capped ZnS:Mn QDs are promising candidates as biological fluorescent labels.
Co-reporter:Haiping Huang, Jingjing Li and Jun-Jie Zhu
Analytical Methods (2009-Present) 2011 - vol. 3(Issue 1) pp:NaN42-42
Publication Date(Web):2010/12/20
DOI:10.1039/C0AY00608D
This review presents a general description of the electrochemiluminescence (ECL) related to quantum dots (QDs) and their analytical application. It briefly overviews the synthetic route of quantum dots. The basic mechanisms are given for QDs ECL behavior. Finally, new developments and improvements of its application in inorganic substance analysis, organics analysis, immunoassay and aptasensing assay are discussed.
Co-reporter:Sai Bi, Tingting Zhao, Baoyu Luo and Jun-Jie Zhu
Chemical Communications 2013 - vol. 49(Issue 61) pp:NaN6908-6908
Publication Date(Web):2013/06/12
DOI:10.1039/C3CC43353F
A novel hybridization chain reaction-based branched rolling circle amplification combining the fabrication of multi-HRP-capped MNPs is developed for chemiluminescence detection of DNA methyltransferase activities and inhibitors with high sensitivity in a well-controlled manner.
Co-reporter:Yujie Ding, Hao Zhu, Xiaoxia Zhang, Jun-Jie Zhu and Clemens Burda
Chemical Communications 2013 - vol. 49(Issue 71) pp:NaN7799-7799
Publication Date(Web):2013/07/02
DOI:10.1039/C3CC43926G
A novel fluorescence resonance energy transfer (FRET)-based probe, γ-cyclodextrin modified oleic acid–NaYF4:Yb, Ho upconversion nanoparticles functionalized with a rhodamine B derivative (RBD), has been achieved for Fe3+-sensing in aqueous solution with high sensitivity and selectivity.
Co-reporter:Tingting Zheng, Rui Zhang, Qingfeng Zhang, Tingting Tan, Kui Zhang, Jun-Jie Zhu and Hui Wang
Chemical Communications 2013 - vol. 49(Issue 72) pp:NaN7883-7883
Publication Date(Web):2013/07/11
DOI:10.1039/C3CC44623A
We have developed a robust enzymatic peptide cleavage-based assay for the ultrasensitive dual-channel detection of matrix metalloproteinase-2 (MMP-2) in human serum using gold-quantum dot (Au-QD) core–satellite nanoprobes.
Co-reporter:Guo-Hai Yang, Jian-Jun Shi, Sheng Wang, Wei-Wei Xiong, Li-Ping Jiang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2013 - vol. 49(Issue 91) pp:NaN10759-10759
Publication Date(Web):2013/09/27
DOI:10.1039/C3CC45759A
A multifunctional boron nitride–gold nanocluster composite was fabricated using poly-diallyldimethylammonium chloride as a stabilizer and a linker. The as-fabricated composite could be used as a fluorescent or an electrochemical label for immunosensing in the sensitive detection of interleukin-6.
Co-reporter:Qianhao Min, Xiaoxia Zhang, Ren'an Wu, Hanfa Zou and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 38) pp:NaN10727-10727
Publication Date(Web):2011/08/24
DOI:10.1039/C1CC13969J
Magnetic mesoporous silica with a magnetic cover and mesoporous core was synthesized, filled with trypsin and located in an S-shaped microfluidic reactor. High-molecular weight (MW) proteins were split to waste by fractionation, whilst low-MW proteins were retained on the chip to be digested.
Co-reporter:Fei Zhou, Tingting Zheng, E. S. Abdel-Halim, Liping Jiang and Jun-Jie Zhu
Journal of Materials Chemistry A 2016 - vol. 4(Issue 17) pp:NaN2894-2894
Publication Date(Web):2016/03/29
DOI:10.1039/C6TB00438E
A novel multifunctional nanoplatform was designed based on the combination of silver nanoparticles (AgNPs) with nucleolin-targeted and doxorubicin (Dox)-loaded manganese dioxide (MnO2) nanosheets to induce enhanced cancer cell apoptosis. MnO2 nanosheets fabricated on the surface of AgNPs served as efficient fluorescence quenchers of Dox. After being internalized into cancer cells, the fluorescence of Dox could be turned on gradually by intracellular glutathione (GSH) which reduces MnO2 into Mn2+ to release Dox. The synergetic effects of AgNP-induced apoptosis and subsequent Dox delivery resulted in enhanced cancer cell apoptosis. Annexin V-FITC/PI double staining, mitochondrial membrane potential (MMP) detection and reactive oxygen species (ROS) detection demonstrated the specific enhanced apoptosis of cancer cells. In this way, the novel nanoprobes can be used as promising theranostic agents for specific cancer therapy.
Co-reporter:Yun Chen, Panpan Gai, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 - vol. 3(Issue 21) pp:NaN11516-11516
Publication Date(Web):2015/04/20
DOI:10.1039/C5TA01432H
Enzymatic biofuel cells (EBFCs) utilize redox enzymes as the catalysts to produce energy from green and renewable fuels, and are considered as promising, environmentally friendly power sources. However, EBFCs are limited by the relatively slow rate of electron transfer between enzymes and electrodes, which is a major barrier to improving EBFC power output. In this study, enzymes were bound to the hydrophilic, carboxyl group functionalized graphene–gold nanoparticle hybrid, and the hybrid as electrode material was able to increase the rate of electron transfer in the EBFC. The open-circuit voltage (Eocvcell) of this designed EBFC reached 1.16 ± 0.02 V, and the maximal power density (Pmax) was as high as 1.96 ± 0.13 mW cm−2. Two as-prepared EBFC units arranged in series were able to light up red and yellow light-emitting diodes (LEDs). Also, using these EBFCs, the Eocvcell and Pmax retained 80% and 66% of their optimal values over 70 days, respectively. This fabricated EBFC is expected to find applications in the bioenergy fields.
Co-reporter:Guohai Yang, Yongjie Li, Rohit Kumar Rana and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 - vol. 1(Issue 5) pp:NaN1762-1762
Publication Date(Web):2012/11/28
DOI:10.1039/C2TA00776B
A facile in situ assembly strategy was developed for the fabrication of Pt–Au alloy nanoparticles (NPs) on nitrogen-doped graphene (N–G) sheets, and the as-fabricated Pt–Au/N–G nanocomposites were suitable for electrochemical applications. As characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction analysis and inductively coupled plasma-atomic emission spectroscopy techniques, Pt–Au alloy NPs with an average size of 4–5 nm were uniformly distributed on the N–G surface through intrinsic covalent bonds. The Pt–Au/N–G nanocomposites exhibited excellent electrocatalytic activity and stability towards the methanol oxidation reaction with the highest capability observed for a Pt/Au atomic ratio of 3/1. The unique electrochemical features are distinctive from those of N-free nanocomposites and commercially available Pt/C catalysts, indicative of the alloying effect of Pt–Au and their synergistic interaction with the N–G sheet, which may open up new possibilities for the preparation of N–G-based nanocomposites for other intensive applications as well.
Co-reporter:Hao Zhu, Yujie Ding, Anqi Wang, Xu Sun, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 - vol. 3(Issue 3) pp:NaN464-464
Publication Date(Web):2014/10/15
DOI:10.1039/C4TB01320D
A novel aptasensor was fabricated for the detection of lysozyme and DNA based on the fluorescence resonance energy transfer (FRET) technique between upconversion nanoparticles (UCNPs) and a dye labeled aptamer. UCNPs can act as excellent emitters due to their low autofluorescence and high penetration depth of biosamples. NaYF4:Yb, Er nanoparticles as UCNPs were synthesized and attached with a dye labeled aptamer through a cationic polymer as an electrostatic linker to quench the upconversion fluorescence intensity. The intensity can be restored after the addition of lysozyme or the complementary DNA (target DNA) because of their strong interaction with the aptamer. The sensor provided a linear concentration range from 30 to 210 nM for lysozyme and 40 to 200 nM for the target DNA, the limit of detection was 2.5 nM and 2.8 nM, respectively. The sensor was also used to monitor the lysozyme level in both human saliva and serum samples, and the results were consistent with the reported values. The method was simple and convenient without the extra procedure of bioconjugation, and could be put to use for the determination of various targets in the future.
Co-reporter:Fang-Fang Cheng, Wei Chen, Li-Hui Hu, Gang Chen, Hai-Tao Miao, Chenzhong Li and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 - vol. 1(Issue 38) pp:NaN4962-4962
Publication Date(Web):2013/07/22
DOI:10.1039/C3TB20656D
Graphene/Au composites with a high positive charge, which is advantageous for the binding and condensation of negatively charged siRNA, are synthesized via an in situ reduction method, using PEI as a reductant and protective reagent. Owing to the sufficient amounts of amino groups, PEI-grafted graphene/Au composites can be further modified with methoxyl-PEG to acquire low cytotoxicity, novel blood compatibility, and optimal dispersibility in physiological environments. The obtained PEGylated PEI-grafted graphene/Au composites (PPGA) allow efficient loading of siRNA, forming PPGA/siRNA complexes to transport into HL-60 cells and downregulated anti-apoptosis Bcl-2 protein, indicating PPGA is a suitable platform for gene delivery. Moreover, PPGA display an enhanced photothermal response with respect to PPG under NIR laser irradiation, suggesting that PPGA can be used as an efficient photothermal agent.
Co-reporter:Wei-Wei Xiong, Jin-Qiang Chen, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2015 - vol. 3(Issue 9) pp:NaN1934-1934
Publication Date(Web):2014/12/17
DOI:10.1039/C4TC02492C
Zinc triselenide (ZrSe3) and hafnium triselenide (HfSe3) nanobelts were synthesized using a chemical vapor transport method. Photodetectors based on individual nanobelts of ZrSe3 and HfSe3 were fabricated on SiO2/Si substrates, respectively, and the optoelectronic properties of both were evaluated. The ZrSe3 nanobelt photodetector showed a good photoresponse to wavelengths ranging from 405 nm to 780 nm. Under illumination with 650 nm light, the ratio of photoswitch currents reached 1.97 with a light on/off period of 50 s at a bias voltage of 5 V. The HfSe3 nanobelt photodetector also showed good photoresponse to wavelengths ranging from 405 nm to 650 nm, and the ratio of photoswitch currents, under illumination with 532 nm light, reached 2.2 with a light on/off period of 50 s at a bias voltage of 5 V. The photoresponse time of both the photodetectors was less than 0.4 s. The results demonstrated that ZrSe3 and HfSe3 nanobelts possessed excellent photoconductivity, and suggested that these photodetectors would have potential applications under a range of visible light conditions.
Co-reporter:Yun Chen, Panpan Gai, Li Jin, Dong Zhu, Danbi Tian, E. S. Abdel-Halim, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 - vol. 1(Issue 28) pp:NaN3457-3457
Publication Date(Web):2013/05/28
DOI:10.1039/C3TB20513D
Poly(3,4-ethylenedioxythiophene) (PEDOT) nanowhiskers were fabricated in a [bmim][BF4] ionic liquid. The minimal size of the nanowhiskers is only 0.2 nm, and the size matches the thickness of a PEDOT single-molecular chain. They were successfully used as the electron transfer channels between the active center of hemoglobin (Hb) and an underlying electrode. The direct electron transfer process between Hb and the underlying electrode was realized without any electron mediator. Compared to that of a gold nanoparticle (AuNP)–Hb composite electrode, the catalytic current of a PEDOT nanowhiskers–AuNPs–Hb composite electrode for detecting H2O2 is increased 7 fold. A novel model of a H2O2 biosensor based on the PEDOT nanowhiskers–AuNPs–Hb composites was fabricated. The detection limit was estimated to be 0.6 μM at a signal/noise (S/N) ratio of 3, and the linear range of H2O2 concentration was from 1 μM to 1100 μM. Three constructed models of the biosensors showed a good stability, and all of them retained nearly 90% of their initial signals for 1 mM H2O2 when they were stored at 4 °C after 60 days. H2O2 concentration in contact lens nursing liquid was measured by the biosensor, and the results were in good agreement with the values provided by the supplier. It is shown that the PEDOT nanowhiskers can provide a new opportunity for the design of sensitive biosensors with long-term stability.
Co-reporter:Wei-Wei Xiong, Guo-Hai Yang, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 - vol. 1(Issue 33) pp:NaN4165-4165
Publication Date(Web):2013/06/24
DOI:10.1039/C3TB20638F
Low-toxicity, highly luminescent, and water-soluble AgInS2/ZnS nanocrystals (NCs) have been synthesized via a microwave-assisted approach. The structure and optical features of the AgInS2/ZnS NCs were characterized by X-ray diffraction, high resolution transmission electron microscopy, Fourier transform infrared spectroscopy, ultraviolet visible absorption spectroscopy and photoluminescence (PL) spectroscopy. The as-synthesized AgInS2/ZnS NCs exhibited high PL quantum yields (40%) and long PL lifetimes (424.5 ns). Furthermore, the dynamic changes of the intracellular copper(II) levels in HeLa cells were monitored using the AgInS2/ZnS NCs as fluorescent probes. The results showed that the AgInS2/ZnS NCs as promising fluorescent probes can be used in the detection of intracellular copper ions in living cells.
Co-reporter:Yongbing Lou, Yixin Zhao, Jinxi Chen and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 - vol. 2(Issue 4) pp:NaN613-613
Publication Date(Web):2013/11/01
DOI:10.1039/C3TC31937G
Colloidal semiconductor nanocrystals or quantum dots (QDs) have been facilitating the development of sensitive fluorescence sensors over the past decade, due to their unique photophysical properties, versatile surface chemistry and ligand binding ability, and the possibility of the encapsulation in different materials or attachment to different functional materials, while retaining their native luminescence property. The optical metal ion chemosensors with high sensitivity and selectivity have been developed due to the importance of the metal ions' fundamental roles, possessed in a wide range of biological processes and the aquatic environment. This review addresses the different sensing strategies with chemically modified QD hybrid structures for the sensing of metal ions in aqueous solution or an in vivo environment, and discusses the photophysical mechanisms in the different sensor systems while comparing their detecting/sensing selectivity. The perspectives for the future potential developments in QD based optical sensing for metal ions are discussed.
Co-reporter:Yujie Ding, Xiaoxia Zhang, Hao Zhu and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 - vol. 2(Issue 5) pp:NaN952-952
Publication Date(Web):2013/10/31
DOI:10.1039/C3TC31608D
A novel route was developed by doping rare-earth ions (RE3+) with large ionic radii (such as La3+, Ce3+, Sm3+, Eu3+, Tb3+, Dy3+, Yb3+ and Lu3+) for aspect ratio modification of KSc2F7 nanocrystals (NCs). The results revealed that the shape of the nanocrystals could be readily tuned from one-dimensional long nanorods to zero-dimensional ultrasmall nanospheres. The aspect ratio of the NCs could be adjusted over a broad range from 45 to 1 by changing the dopant or doping concentration. Interestingly it was found that doping of a lanthanide with a larger ionic radius was equivalent to increasing the amount of the dopant on the aspect ratio evolution. The NCs doped with different RE3+ also exhibited multifunctionality, including upconversion (UC) and downconversion (DC) emissions as well as paramagnetic properties.
Co-reporter:Wei-Wei Xiong, Jin-Qiang Chen, Xing-Cai Wu and Jun-Jie Zhu
Journal of Materials Chemistry A 2014 - vol. 2(Issue 35) pp:NaN7395-7395
Publication Date(Web):2014/07/11
DOI:10.1039/C4TC01039F
HfS3 nanobelts were directly synthesized via a simple chemical vapor transport method. A field-effect transistor and photodetector was further fabricated based on an individual HfS3 nanobelt, and its electrical and optoelectronic properties were evaluated. The output characteristic curves of the FET revealed a typical p-type semiconducting behavior. The photodetector has an ultralow dark current (0.04 pA) and a large on/off ratio (337.5) illuminated by 405 nm light with 1.2 mW cm−2. It demonstrated excellent stability and sensitivity to 405 nm light. The results suggest that the HfS3 nanobelts are promising for application in nanoscale electronic and optoelectronic devices. The research will play a positive role in nanodevice research of one-dimensional transition-metal trichalcogenide nanostructure.
Co-reporter:Jian-Jun Shi, Guo-Hai Yang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 - vol. 21(Issue 20) pp:NaN7349-7349
Publication Date(Web):2011/04/07
DOI:10.1039/C1JM10333D
Sonoelectrochemical technique was successfully used to fabricate alloy–graphene nanocomposites. It not only provides a simple way to synthesize alloy nanoparticles, but also shows a general strategy for fabricating graphene-based nanostructures with anticipated properties. Pd was co-electrodeposited with Pt at different atomic ratios, and then was anchored with reduced graphene oxide (RGO) simultaneously in the presence of PDDA. The morphologies and structures of the as-prepared PDDA-RGO-PdPt nanocomposites were extensively investigated by transmission electron microscopy (TEM), scanning electron microscopy (SEM), and X-ray diffraction (XRD). The composition was evaluated by energy dispersive X-ray spectrometry (EDS) and inductively coupled plasma–atomic emission spectroscopy (ICP-AES). Raman spectra revealed the surface properties of graphene and its interaction with metallic nanoparticles. Cyclic voltammetric (CV) and chronoamperometric experiments further exhibited their catalytic activity and stability for the electro-oxidation of ethanol in alkaline media, which could be applied as promising electrocatalysts for direct alcohol fuel cells (DAFCs).
Co-reporter:Yun Chen, Yang Li, Dong Sun, Danbi Tian, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 - vol. 21(Issue 21) pp:NaN7611-7611
Publication Date(Web):2011/04/08
DOI:10.1039/C1JM10293A
The hydrophilic and carboxyl group functionalized graphene–gold nanoparticles (AuNPs) hybrid has been synthesized in situ. AuNPs can be scattered well on the graphene bilayer, and the loading amount of AuNPs can be controlled. Glucose oxidase (GOD) was successfully bound to the surface of the hybrid through a condensation reaction between terminal amino groups on the lysine residues of GOD and carboxyl groups on the AuNPs. The hybrid provided a suitable microenvironment for GOD to retain its biological activity. The direct and reversible electron transfer process between GOD and the hybrid electrode was realized without any supporting film or electron mediator. A novel model of the glucose biosensor based on the hybrid electrode was fabricated. Blood sugar concentrations measured in human serum samples by the glucose biosensor were in good agreement with the values provided by the Nanjing University hospital, and the average relative standard deviation was 3.2% for six successive measurements. Three constructed biosensors showed good stability, and all of them retained 80% of their initial signals after they were stored at 4 °C for four months. It is promising that the model of the glucose biosensor can be used as an effective candidate for the detection of blood sugar concentration in clinical diagnoses.
Co-reporter:Kunping Liu, Jing-Jing Zhang, Fang-Fang Cheng, Ting-Ting Zheng, Chunming Wang and Jun-Jie Zhu
Journal of Materials Chemistry A 2011 - vol. 21(Issue 32) pp:NaN12040-12040
Publication Date(Web):2011/07/05
DOI:10.1039/C1JM10749F
A green and facile method for the preparation of gelatin functionalized graphene nanosheets (gelatin–GNS) was reported by using gelatin as a reducing reagent. Meanwhile, the gelatin also played an important role as a functionalized reagent to prevent the aggregation of the graphene nanosheets. The obtained biocompatible gelatin–GNS exhibited excellent stability in water and various physiological fluids including, cellular growth media as well as serum which were critical prerequisites for biomedicine application of graphene. Cellular toxicity test suggested that the gelatin–GNS was nontoxic for MCF-7 cells, even at a high concentration of 200 μg mL−1. Furthermore, the anticancer drug was loaded onto the gelatin–GNS at a high loading capacity via physisorption for cellular imaging and drug delivery. The doxorubicin/gelatin–GNS composite exhibited a high toxicity to kill MCF-7 cells and experienced a gelatin-mediated sustained release in vitro, which has the potential advantage of increasing the therapeutic efficacy. Therefore, the gelatin–GNS could be selected as an ideal drug carrier to be applied in biomedicine studies.
Co-reporter:Yusheng Ji, Panpan Gai, Jun Feng, Linlin Wang, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2017 - vol. 5(Issue 22) pp:NaN11031-11031
Publication Date(Web):2017/05/02
DOI:10.1039/C7TA01931A
Enzymatic biofuel cells (EBFCs) are considered as a promising approach to meet the requirements of power sources. Electrode materials, which are significant factors to affect the power output of EBFCs, have aroused great interest. Herein, we developed an EBFC using a Fe3O4–carbon nanofiber/gold nanoparticle hybrid as the substrate electrode for improving the performance of the power output. The open-circuit voltage (Eocv) of the designed EBFC reached 0.68 ± 0.03 V, and the maximum power density (Pmax) reached 126 ± 4.5 μW cm−2. The as-prepared EBFC showed 3 times higher Pmax compared to the EBFC based on the carbon nanofiber/gold nanoparticle hybrid, which was ascribed to the good electrocatalytic activity of Fe3O4 NP loaded carbon nanofibers (CNFs), the 3D porous structure of CNFs as well as the uniform distribution of Au NPs. The Fe3O4–CNF/gold nanoparticle hybrid is considered as a promising candidate for constructing electrochemical biosensors and biofuel cells.
Co-reporter:Xinxin Cong, Gao-Chao Fan, Xiaolei Wang, E. S. Abdel-Halim and Jun-Jie Zhu
Journal of Materials Chemistry A 2016 - vol. 4(Issue 36) pp:NaN6124-6124
Publication Date(Web):2016/08/08
DOI:10.1039/C6TB01807F
A novel, enhanced photoelectrochemical aptasensing platform was developed through integrating the sensitization effect of CdTe@CdS core–shell quantum dots (QDs) coupled with exonuclease-I (Exo-I) assisted target recycling for significant signal amplification. Carcinoembryonic antigen (CEA) was selected as the target analyte to exhibit the analytical performance of this platform. Specifically, nitrogen-doped mesoporous TiO2 (mTiO2:N) was firstly synthesized through an evaporation-induced self-assembly (EISA) method. Then, an mTiO2:N/Au hybrid structure was prepared through depositing Au nanoparticles on the surface of the mTiO2:N film and this acted as the photoelectrochemical matrix to immobilize the complementary DNA (cDNA) of the CEA aptamer probe (pDNA). CdTe@CdS core–shell QDs as sensitization agents were covalently bound at the front-end of pDNA. After pDNA was hybridized with cDNA, the labels of the CdTe@CdS core–shell QDs were very close to the mTiO2:N/Au electrode surface, resulting in an evidently enhanced photocurrent intensity due to the generation of the sensitization effect. When the aptasensor was incubated with CEA and Exo-I simultaneously, CdTe@CdS QD labeled pDNA (denoted QD–pDNA) became specifically bound with CEA and meanwhile was separated from the electrode surface, leading to an obviously weakened sensitization effect and a decreased photocurrent intensity. Moreover, as Exo-I could digest the single strand form of pDNA, the previously bound CEA was released and continuously interacted with the rest of the pDNA on the electrode surface, causing further decreased photocurrent intensity. The well-designed photoelectrochemical aptasensor exhibited a low detection limit of 0.12 pg mL−1 and a wide linear range from 0.5 pg mL−1 to 10 ng mL−1 for CEA detection, and it also showed good selectivity, reproducibility and stability. The proposed signal amplification strategy provides a promising universal photoelectrochemical platform for sensitively detecting various biomolecules at low levels.
Co-reporter:Wenjing Wang, Shan Huang, Jingjing Li, Kai Rui, Sai Bi, Jian-Rong Zhang and Jun-Jie Zhu
Chemical Science (2010-Present) 2017 - vol. 8(Issue 1) pp:NaN180-180
Publication Date(Web):2016/08/01
DOI:10.1039/C6SC01953F
Telomerase plays a vital role in cancer and aging, and telomerase activity detection has drawn great attention recently. However, a feasible in situ imaging system for intracellular telomerase is still a challenge. Here, we develop a novel approach to image intracellular telomerase activity using DNA-based computation. A cascade nucleic acid logic gate that responded to intracellular telomerase was constructed. A telomerase substrate (TS) probe, extended by intracellular telomerase, worked as an input to initiate computation cascades. In this way, intracellular telomerase could be clearly indicated by fluorophore labeled nucleic acids as the output. Through one-step incubation, evaluation of the intracellular telomerase activity for a HeLa cell line and the ability to differentiate cancer cells from normal cells could be realized. Furthermore, the response of intracellular telomerase activity to a telomerase-inhibiting model drug was observed using the proposed method. Thus, this intracellular telomerase computation device will allow improvements in studying the relationship between telomerase and cancer, and may help to develop telomerase inhibitors. This finding also expands the applications of DNA computational techniques in cells.
Co-reporter:Cui-e Zhao, Panpan Gai, Rongbin Song, Ying Chen, Jianrong Zhang and Jun-Jie Zhu
Chemical Society Reviews 2017 - vol. 46(Issue 5) pp:NaN1564-1564
Publication Date(Web):2017/02/17
DOI:10.1039/C6CS00044D
During the past decade, biofuel cells (BFCs) have emerged as an emerging technology on account of their ability to directly generate electricity from biologically renewable catalysts and fuels. Due to the boost in nanotechnology, significant advances have been accomplished in BFCs. Although it is still challenging to promote the performance of BFCs, adopting nanostructured materials for BFC construction has been extensively proposed as an effective and promising strategy to achieve high energy production. In this review, we presented the major novel nanostructured materials applied for BFCs and highlighted the breakthroughs in this field. Based on different natures of the bio-catalysts and electron transfer process at the bio-electrode surfaces, the fundamentals of BFC systems, including enzymatic biofuel cells (EBFCs) and microbial fuel cells (MFCs), have been elucidated. In particular, the principle of electrode materials design has been detailed in terms of enhancing electrical communications between biological catalysts and electrodes. Furthermore, we have provided the applications of BFCs and potential challenges of this technology.
Co-reporter:Ying-Chun Gao, Kai Xi, Wei-Na Wang, Xu-Dong Jia and Jun-Jie Zhu
Analytical Methods (2009-Present) 2011 - vol. 3(Issue 10) pp:NaN2391-2391
Publication Date(Web):2011/09/15
DOI:10.1039/C1AY05378G
Well-oriented 3D gold flower-like nanoparticles were successfully synthesized by a facile one-pot method, and the gold nanoflowers (AuNFs) were mixed with hemoglobin (Hb) to form a gold nanoflowers/hemoglobin composite. The composite was further combined with multiwalled carbon nanotubes on a glassy carbon electrode (GCE) to fabricate a novel biosensor. The sensor has high stability and bioactivity, and was studied by scanning electron microscopy (SEM) and cyclic voltammetry (CV). The hemoglobin/gold nanoflowers/multiwalled carbon nanotubes glassy carbon electrode (Hb/AuNFs/CNTs/GCE) either retained the Hb in similar native conformations or promoted direct electron transfer. Moreover, the sensor exhibited remarkable catalytic activity toward H2O2 and trichloroacetic acid (TCA). The linear relationship for the determination is in the range of 1.0–60 μM for H2O2 and 0.06–28 mM for TCA. The detection limits were 0.08 μM and 7.3 μM (S/N = 3), respectively.
Co-reporter:
Analytical Methods (2009-Present) 2013 - vol. 5(Issue 17) pp:
Publication Date(Web):
DOI:10.1039/C3AY40907D
The improvement of analytical accuracy and S/N (signal to noise ratio) based on conventional homogeneous fluorometry was always limited because of high background noise from complicated sample ingredients, buffer solution and lysates. Herein, a self-assembled Mn-doped ZnSe quantum dot–methyl viologen nanohybrid as an OFF–ON fluorescent probe is presented for the time-resolved fluorescence detection of tiopronin, showing high S/N and selectivity with a low detection limit of 0.1 μmol L−1 and a linear response ranging from 4 to 160 μM. We anticipate that this probe will have promising applications for sensitive biosensing and drug analysis.
Co-reporter:Hongying Liu, Guoxi Liang, E. S. Abdel-Halim and Jun-Jie Zhu
Analytical Methods (2009-Present) 2011 - vol. 3(Issue 8) pp:NaN1801-1801
Publication Date(Web):2011/07/06
DOI:10.1039/C1AY05178D
A sensitive and selective quantum dots (QDs)-based fluorescence resonance energy transfer (FRET) biosensor was successfully fabricated for the detection of the cancer marker type IV collagenase. The cancer marker type IV collagenase could be determined by linking peptide between the donor-luminescent QDs and the acceptor-gold nanoparticles with small size (SAuNPs) based on FRET. Firstly, peptide terminated with cysteine could be bound to the surface of SAuNPs via the formation of Au–S bonds. Then QDs combined with the SAuNPs through the peptide. At this moment, the photoluminescence (PL) of the QDs was quenched. After type IV collagenase was added into the system, the SAuNPs could detach from QDs because the enzyme cleaves the peptide to lead to the disappearance of FRET, which allowed the fluorescence of the QDs to return. The enzymatic activity of type IV collagenase was related to the PL change of QDs-based FRET probes. The concentration of type IV collagenase was determined in the linear range of 0.05–10 μg mL−1 with a detection limit of 18 ng mL−1. This sensor opens a new route for monitoring the low activities of type IV collagenase in normal and cancerous cell cultures.
Co-reporter:Jingjing Zhao, Penghui Zhang, Zhimei He, Qian-Hao Min, E. S. Abdel-Halim and Jun-Jie Zhu
Chemical Communications 2016 - vol. 52(Issue 33) pp:NaN5725-5725
Publication Date(Web):2016/03/18
DOI:10.1039/C6CC01162D
Smart nanocarriers with switchable surfaces consisting of thermo-sensitive polymers and aptamers have been developed, through which the cellular uptake and photothermal therapy in five different cells could be spatial-temporally controlled on command, which is beneficial in maximizing therapy efficacy and minimizing side effects.
Co-reporter:Feng Lu, Tennyson L. Doane, Jun-Jie Zhu and Clemens Burda
Chemical Communications 2014 - vol. 50(Issue 6) pp:NaN644-644
Publication Date(Web):2013/10/28
DOI:10.1039/C3CC47124A
After ligand exchange with PEG, Au NPs with differently mixed surface functionalities co-exist in the as-synthesized sample. It is found that the poorly grafted nanoparticles can be simply removed using a chromatographic method, and the well grafted nanoparticles can be eluted as a function of the core size.
Co-reporter:Cuie Zhao, Ying Wang, Fengjian Shi, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2013 - vol. 49(Issue 59) pp:NaN6670-6670
Publication Date(Web):2013/06/04
DOI:10.1039/C3CC42068J
The positively-charged ionic liquid functionalized graphene nanosheets (IL-GNS) were used as an anode in microbial fuel cells (MFCs), and proved effective for the high biocurrent generation and power output.
Co-reporter:Yuanyuan Shen, Lingling Li, Qian Lu, Jing Ji, Rong Fei, Jianrong Zhang, E. S. Abdel-Halim and Jun-Jie Zhu
Chemical Communications 2012 - vol. 48(Issue 16) pp:NaN2224-2224
Publication Date(Web):2012/01/03
DOI:10.1039/C2CC16329B
Highly luminescent and low toxic glutathione-capped CdSeTe@ZnS–SiO2 quantum dots were successfully synthesized via a promising microwave strategy, and then applied in the detection of Cu2+.
Co-reporter:Jing-Jing Zhang, Ting-Ting Zheng, Fang-Fang Cheng and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 4) pp:NaN1180-1180
Publication Date(Web):2010/11/12
DOI:10.1039/C0CC03494K
A novel electrochemical sensing platform for sensitive determination of caspase 3 activity and inhibition was developed by combining the site-specific recognition and cleavage of the DEVD-peptide with quantum dots as signal amplification.
Co-reporter:Hongying Liu, Xiang Zhang, Ximei Wu, Liping Jiang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 14) pp:NaN4239-4239
Publication Date(Web):2011/02/25
DOI:10.1039/C1CC00103E
Highly fluorescent and water-soluble gold nanoclusters (AuNCs) with near-infrared-emission and Au@AgNCs with yellow-emission were successfully prepared via a rapid sonochemical approach, and the as-prepared AuNCs could be applied in the determination of Cu2+ with a wider detection range and lower detection limit.
Co-reporter:Jing-Jing Zhang, Yan Liu, Li-Hui Hu, Li-Ping Jiang and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 23) pp:NaN6553-6553
Publication Date(Web):2011/05/06
DOI:10.1039/C1CC11565K
The proof-of-principle of the integration of electrically heated carbon paste electrode with immunoassay as a potential alternative for ultrasensitive detection of cytokines was demonstrated.
Co-reporter:Qianhao Min, Xiaoxia Zhang, Hongyi Zhang, Fang Zhou and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 42) pp:NaN11711-11711
Publication Date(Web):2011/09/27
DOI:10.1039/C1CC15151G
Fe3O4–graphene–TiO2 ternary composite networks were first synthesized, which exhibited high selectivity and capacity in the capture of phosphopeptides, due to the enhanced contact to phosphopeptides given by the graphene scaffold.
Co-reporter:Yun Chen, Yuanyuan Shen, Dong Sun, Hongyi Zhang, Danbi Tian, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2011 - vol. 47(Issue 42) pp:NaN11735-11735
Publication Date(Web):2011/08/26
DOI:10.1039/C1CC13852A
A dispersible graphene/gold nanoclusters hybrid in aqueous solution was fabricated in situ based on the bilayer graphene template, and its electrogenerated chemiluminescence (ECL) behavior was studied.
Co-reporter:Jian-Jun Miao, Gui-Fen Jie, Yu-Ping Chen, Lei Zhang, Li-Ping Jiang and Jun-Jie Zhu
Chemical Communications 2008(Issue 32) pp:NaN3764-3764
Publication Date(Web):2008/06/13
DOI:10.1039/B803645D
Novel chalcogenide lifebelts have been prepared by using a simple sacrificial template method, and their electrogenerated chemiluminescence properties were studied.
Co-reporter:Dong Zhu, Xiaoxing Jiang, Cuie Zhao, Xiaolian Sun, Jianrong Zhang and Jun-Jie Zhu
Chemical Communications 2010 - vol. 46(Issue 29) pp:NaN5228-5228
Publication Date(Web):2010/06/23
DOI:10.1039/C0CC00791A
A microwave-assisted synthetic procedure is presented for the preparation of low-toxic Mn:ZnSe/ZnS core/shell nanocrystals to label antibodies for selective detection of human immunoglobulin G (IgG) based on fluorescence resonance energy transfer (FRET) between the Mn:ZnSe/ZnS and Au nanoparticles (AuNPs).
Co-reporter:Guo-Xi Liang, Ling-Ling Li, Hong-Yin Liu, Jian-Rong Zhang, Clemens Burda and Jun-Jie Zhu
Chemical Communications 2010 - vol. 46(Issue 17) pp:NaN2976-2976
Publication Date(Web):2010/03/05
DOI:10.1039/C000564A
New water-soluble CdSeTe/ZnS core–shell quantum dots with excellent near-infrared emission were synthesized via an aqueous solution method; they showed strong electrogenerated chemiluminescence and favorable biocompatibility.
Co-reporter:Qianhao Min, Ren'an Wu, Liang Zhao, Hongqiang Qin, Mingliang Ye, Jun-Jie Zhu and Hanfa Zou
Chemical Communications 2010 - vol. 46(Issue 33) pp:NaN6146-6146
Publication Date(Web):2010/07/27
DOI:10.1039/C0CC00619J
In this study, the concept of size-selective proteolysis was first described by using the mesoporous silica-based trypsin nanoreactor. For analysis of a complex protein sample, low-MW proteins were preferentially digested for identification while high-MW proteins were excluded from digestion.
Co-reporter:Jingjing Li, Wenjing Wang, Defang Sun, Jiangning Chen, Peng-Hui Zhang, Jian-Rong Zhang, Qianhao Min and Jun-Jie Zhu
Chemical Science (2010-Present) 2013 - vol. 4(Issue 9) pp:NaN3521-3521
Publication Date(Web):2013/06/19
DOI:10.1039/C3SC51538A
The use of small interfering RNA (siRNA) to silence target genes involved in disease has generated much excitement in the scientific community. While promising, the clinical application of RNA interference (RNAi) is still challenging in achieving effective delivery and tracking of siRNA to target cells. A new multifunctional probe comprising a cell-specific internalization aptamer, fluorescent silver nanoclusters (Ag NCs), and therapeutic siRNA was developed in one system for the specific delivery of siRNA into a target cell and for simultaneous noninvasive imaging. Different from described nanocarrier-based delivery methods which have to suffer from complicated conjugation, Ag NCs could be synthesized directly from the aptamer chimera. Sgc8c aptamer-functionalized Ag NCs as a cell-type specific siRNA delivery and imaging probe complements recent advances in PSMA aptamer-based siRNA delivery and nanomaterial-based molecular imaging. Besides, siRNA in the Ag NCs–streptavidin–siRNA complex displayed outstanding stability in both binding buffer and cell culture medium. The fluorescent intensity of biotinylated aptamer-functionalized Ag NCs was enhanced in acidic environment and no observable quenching of fluorescence occurred even after incubation for 48 h, which could benefit their usage in the intracellular environment. The facile synthetic process, good biocompatibility, excellent stability and comparable gene silencing effect with commercial reagent make it more promising for in vivo applications.
Co-reporter:Jingjing Li, Fangfang Cheng, Haiping Huang, Lingling Li and Jun-Jie Zhu
Chemical Society Reviews 2015 - vol. 44(Issue 21) pp:NaN7880-7880
Publication Date(Web):2015/07/27
DOI:10.1039/C4CS00476K
Activatable imaging probes as alternatives to “always on” imaging probes have attracted more and more attention due to their improved sensitivity and specificity. They are commonly designed to amplify or boost imaging signals only in response to specific biomolecular recognition or interaction. Thus, the design strategies play a vital role in the fabrication of activatable imaging probes. In this review, we focus on the design mechanisms and biological applications of those nanomaterial-based activatable imaging probes reported in the past five years, benefitting greatly from the good development of nanotechnology. These probes not only include the most studied activatable fluorescence imaging probes, but also cover more activatable MR imaging probes based on nanoparticle contrast agents and activatable photoacoustic imaging probes, providing more bases for clinical translation.
Co-reporter:Cuie Zhao, Panpan Gai, Changhong Liu, Xin Wang, Hao Xu, Jianrong Zhang and Jun-Jie Zhu
Journal of Materials Chemistry A 2013 - vol. 1(Issue 40) pp:NaN12594-12594
Publication Date(Web):2013/08/14
DOI:10.1039/C3TA12947K
Microbial fuel cells (MFCs) show promise as a technology for electricity generation from waste, and their performance critically depends on the electrode materials and their structures. Herein, a novel MFC anode was fabricated by electro-depositing polyaniline (PANI) networks onto graphene nanoribbons (GNRs)-coated carbon paper (CP/GNRs/PANI). This anode provides a large surface area for the attachment of bacterial cells and high conductivity to facilitate extracellular electron transfer (EET) from microbes to the electrode. Results showed that the anodic current density and power density of the CP/GNRs/PANI anode were much higher than those of each individual component as anode, indicating the synergistic effect between PANI and GNRs.