Jing-Juan Xu

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Name: 徐静娟
Organization: Nanjing University , China
Department: School of Chemistry and Chemical Engineering
Title: NULL(PhD)

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Co-reporter:Hui Zhang;Hong-Yuan Chen
The Journal of Physical Chemistry C September 11, 2008 Volume 112(Issue 36) pp:13886-13892
Publication Date(Web):Publication Date (Web): August 19, 2008
DOI:10.1021/jp802012h
A simple one-step electrodeposition method was used to fabricate various gold nanostructures on glassy carbon electrodes in a low concentration of HAuCl4 solution (5 mM). The morphologies of final gold nanostructures can be easily controlled by varying the pH of the precursors or the deposition temperature. X-ray powder diffraction, scanning electronic microscopy, transmission electron microscopy, contact angle measurements, and electrochemical methods were used to characterize them. Hierarchical waxberry-like gold nanostructures with high active surface areas were obtained in pH 4 bath, and they had a higher catalytic performance for the reduction of oxygen than the other nanogold. These gold structures also displayed an extraordinary superhydrophobicity and the contact angle increased with the increase of deposition temperature and time. Their electrocatalytic response to the oxidation of glucose was also investigated. A sensitive enzyme-free sensor can be easily developed for the detection of glucose in pH 7.4 phosphate buffer solution.
Co-reporter:Fan Yang, Ting-Ting Zhang, Shan-Shan Li, Pei Song, Kai Zhang, Qi-Yuan Guan, Bin Kang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry October 3, 2017 Volume 89(Issue 19) pp:10239-10239
Publication Date(Web):September 8, 2017
DOI:10.1021/acs.analchem.7b01582
It is a great challenge to design a drug delivery system with a controlled manner, especially one triggered by an exclusive endogenous disease marker and with an easily tracked release process. Herein, we developed a drug delivery platform of carbon dots which were connected to a stem-loop molecular beacon loaded with doxorubicin and polyethylene glycol modified folic acid. Such a platform enables one to release drugs on demand under the stimuli of endogenous microRNA-21, and turn on the fluorescence of carbon dots and doxorubicin, which allows one to monitor the drug release process. The intracellular experiment indicated that folic acid could mediate endocytosis of the nanocarrier, and the overexpressed endogenous microRNA-21 served as a unique key to unlock the drug nanocarrier by competitive hybridization with the molecular beacon, which finally resulted in fluorescence recovery and realized a chemotherapeutic effect within human breast cancer cells. The nanocarrier may have potential application in personalized treatment of different cancer subtypes in which the corresponding miRNAs are overexpressed.
Co-reporter:Qiu-Mei Feng, Yue-Hua Guo, Jing-Juan Xu, and Hong-Yuan Chen
ACS Applied Materials & Interfaces May 24, 2017 Volume 9(Issue 20) pp:17637-17637
Publication Date(Web):May 4, 2017
DOI:10.1021/acsami.7b04553
A novel DNA tetrahedron-structured electrochemiluminescence (ECL) platform for bioanalysis with programmable DNA cyclic amplification was developed. In this work, glucose oxidase (GOD) was labeled to a DNA sequence (S) as functional conjugation (GOD-S), which could hybridize with other DNA sequences (L and P) to form GOD-S:L:P probe. In the presence of target DNA and a help DNA (A), the programmable DNA cyclic amplification was activated and released GOD-S via toehold-mediated strand displacement. Then, the obtained GOD-S was further immobilized on the DNA tetrahedral scaffolds with a pendant capture DNA and Ru(bpy)32+-conjugated silica nanoparticles (RuSi NPs) decorated on the electrode surface. Thus, the amount of GOD-S assembled on the electrode surface depended on the concentration of target DNA and GOD could catalyze glucose to generate H2O2 in situ. The ECL signal of Ru(bpy)32+-TPrA system was quenched by the presence of H2O2. By integrating the programmable DNA cyclic amplification and in situ generating H2O2 as Ru(bpy)32+ ECL quencher, a sensitive DNA tetrahedron-structured ECL sensing platform was proposed for DNA detection. Under optimized conditions, this biosensor showed a wide linear range from 100 aM to 10 pM with a detection limit of 40 aM, indicating a promising application in DNA analysis. Furthermore, by labeling GOD to different recognition elements, the proposed strategy could be used for the detection of various targets. Thus, this programmable cascade amplification strategy not only retains the high selectivity and good capturing efficiency of tetrahedral-decorated electrode surface but also provides potential applications in the construction of ECL biosensor.Keywords: biosensors; DNA tetrahedron; electrochemiluminescence (ECL); multilayers; programmable DNA cyclic amplification;
Co-reporter:Jun Hu, Qi-Yuan Guan, Jiang Wang, Xiao-Xiao Jiang, Zeng-Qiang Wu, Xing-Hua Xia, Jing-Juan XuHong-Yuan Chen
Analytical Chemistry February 7, 2017 Volume 89(Issue 3) pp:
Publication Date(Web):January 17, 2017
DOI:10.1021/acs.analchem.6b04218
In the work, we showed that the use of nanoemitters (tip dimension <1 μm, typically ∼100 nm) could dramatically reduce the nonspecific metal adduction to peptide or protein ions as well as improve the matrix tolerance of electrospray ionization mass spectrometry (ESI-MS). The proton-enriched smaller initial droplets are supposed to have played a significant role in suppressing the formation of metal adduct ions in nanoemitters. The proton-enrichment effect in the nanoemitters is related to both the exclusion-enrichment effect (EEE) and the ion concentration polarization effect (ICP effect), which permit the molecular ions to be regulated to protonated ones. Smaller initial charged droplets generated from nanoemitters need less fission steps to release the gas-phase ions; thus, the enrichment effect of salt was not as significant as that of microemitters (tip dimension >1 μm), resulting in the disappearing of salt cluster peaks in high mass-to-charge (m/z) region. The use of nanoemitters demonstrates a novel method for tuning the distribution of the metal-adducted ions to be in a controlled manner. This method is also characterized by ease of use and high efficiency in eliminating the formation of adduct ions, and no pretreatment such as desalting is needed even in the presence of salt at millimole concentration.
Co-reporter:Yin-Zhu Wang, Cong-Hui Xu, Wei Zhao, Qi-Yuan Guan, Hong-Yuan Chen, and Jing-Juan Xu
Analytical Chemistry August 1, 2017 Volume 89(Issue 15) pp:8050-8050
Publication Date(Web):June 29, 2017
DOI:10.1021/acs.analchem.7b01494
We report a multicolor ECL device based on closed bipolar electrode (BPE) for the visualized sensing of prostate-specific antigen (PSA) in human blood serum. As the emission color of concomitant electrochemiluminophores is potential resolved, similar to a three-electrode system, selective excitation of ECL could be achieved by tuning the interfacial potential at the poles of BPE. Via modulating the resistance of BPE, multicolor ECL emission of [Ru(bpy)3]2+ and [Ir(ppy)3] mixture using tripropylamine (TPrA) as the co-reactant was observed at the anode and the principle was elaborated. The concept was utilized to the quantification of clinical biomarkers with the color variation. A PSA concentration dependent silver bridge was constructed in the gap of the BPEs as an electric conductivity modulator. On the basis of a multicolor BPE-ECL device, the cutoff values (4.0 and 10.0 ng/mL) of human PSA could be recognized with naked eyes by the green–yellow–red ECL emission changing. As the first multicolor ECL device in biological analysis, BPE may raise the application of potential-resolved ECL to a new level.
Co-reporter:Yi-Fan Ruan, Nan Zhang, Yuan-Cheng Zhu, Wei-Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry August 1, 2017 Volume 89(Issue 15) pp:7869-7869
Publication Date(Web):June 26, 2017
DOI:10.1021/acs.analchem.6b05153
We have developed sensitive photoelectrochemical (PEC) detection of cysteine using the gold nanoparticles (Au NPs) equipped perovskite Bi4NbO8Cl heterostructure. The Bi4NbO8Cl was prepared by a solid-state reaction, and the Au NPs/Bi4NbO8Cl electrode was made through the electrostatic layer-by-layer self-assembly technique. The Au NPs/Bi4NbO8Cl electrode provided much enhanced photocurrent with a great increase compared to the bare Bi4NbO8Cl electrode and allowed for the plasmon-enhanced PEC detection of cysteine with good performance. It demonstrated rapid response, high stability, wide linear detection range and certain selectivity, implying its great promise in its application. Therefore, the Au NPs/Bi4NbO8Cl heterostructure has provided a promising platform for the development of PEC bioanalysis. More generally, these findings offered an insight into the exploitation of perovskite materials for PEC bioanalytical purposes.
Co-reporter:Xue-Jiao Yang, Kai Zhang, Ting-Ting Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry April 4, 2017 Volume 89(Issue 7) pp:4216-4216
Publication Date(Web):March 16, 2017
DOI:10.1021/acs.analchem.7b00267
In situ detection and monitoring of telomerase is of great importance as it is a relatively specific cancer target. However, the complexity of the biological system makes it difficult for the nanoprobe to keep absolutely stable and have a low background in living cells. This study designs a probe termed Förster resonance energy transfer (FRET) nanoflare to achieve ratiometric fluorescent detection of intracellular telomerase with higher specificity, which can effectively resist the disturbance from DNase I and GSH, etc. The probe is composed of a gold nanoparticle (AuNP) which is functioned with telomerase primer sequences (TS) and flares fluorescently labeled donors and acceptors at two terminals. In the presence of telomerase, flares are displaced from the primer sequences and form hairpin structures, so that the donors and acceptors are brought into close proximity, resulting in high FRET efficiency. The probe exhibits good performance for efficiently distinguishing tumor cells from normal cells and monitoring the change of intracellular telomerase activity during treatment with telomerase-related drugs, showing great potential for cancer diagnosis and estimating therapeutic effect.
Co-reporter:Jiang Wang, Xiao-Xiao Jiang, Wei Zhao, Jun Hu, Qi-Yuan Guan, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2017 Volume 171(Volume 171) pp:
Publication Date(Web):15 August 2017
DOI:10.1016/j.talanta.2017.04.071
•A simple membrane extraction device was made and coupled to ESI-MS.•On-line MS analysis of complex matrices without sample pretreatment was achieved based on the homemade device.•The detection procedures including extraction, mixing and ionization could be finished in 10 s.•Chiral ofloxacin in milk was quantitatively analyzed using the proposed method.The direct separation and analysis of chiral drugs in the complex matrix systems are meaningful and challenging. As the most common broad-spectrum antibiotic, levofloxacin has a strong antibacterial ability, but its enantiomer, dextrofloxacin can cause serious harm to human health. In this work, we reported a rapid on-line extraction/ionization device coupled with Electrospray Mass Spectrometry (ESI-MS) for chiral analysis of ofloxacin enantiomers in complex matrix of milk. Since ofloxacin is difficult to dissolve in water and most organic solvents, the procedure of separating ofloxacin in complex system is often complicated. Using the homemade apparatus, the sample pretreatment process was greatly simplified. Milk sample was directly injected and chiral ofloxacin in the sample was extracted at PTFE membrane for further ionization. It took less than 10 s to finish all the procedures including sampling, extraction, reagents mixing, ionization and mass analysis. Utilizing reaction thermodynamics method, trimeric cluster ion [NiΙΙ(ref)2Ofloxacin-H]+ was formed and collisionally dissociated to get chiral resolution of levofloxacin and dextrofloxacin due to the different relative stabilities of the two diastereomeric clusters produced through the dissociation of NiΙΙ bound trimeric clusters. With the proposed method, qualitative and quantitative chiral analysis of ofloxacin in milk was successfully achieved in a simple and fast way.We built a simple and universal sample extraction/ionization device for on-line analysis of chiral ofloxacin in milk via Electrospray Mass Spectrometry (ESI-MS). Using electrospray ionization MS2 with kinetic method, quick qualification and quantification of ofloxacin enantiomers was realized by adding central metal ions and reference ligands in the extraction solution to form mass-selected trimetric cluster ions by electrospray ionization. This strategy greatly simplified the detection procedures of extraction, reaction agent mixing and ionization with total detection time less than 10 sDownload high-res image (137KB)Download full-size image
Co-reporter:Yizhong Shen, Yidan Sun, Runqi Yan, Erquan Chen, Huan Wang, Deju Ye, Jing-Juan Xu, Hong-Yuan Chen
Biomaterials 2017 Volume 148(Volume 148) pp:
Publication Date(Web):1 December 2017
DOI:10.1016/j.biomaterials.2017.09.026
Semiconductor quantum dots (QDs) have served as superior optically active nanomaterials for molecular imaging and photodynamic therapy (PDT), but the low singlet oxygen (1O2) quantum yield and lack of tumor selectivity have limited their applications for tumor PDT in vivo. Here, we report the rational engineering of QDs into tumor-targeting hybrid nanoparticles through micelle-encapsulating a pre-assembled unique QD-Zn-porphyrin complex, a highly fluorescent organic photosensitizer rhodamine 6G (R6G), and a near-infrared fluorophore NIR775 with folic acid labeled phospholipid polymers. These nanoparticles have large porphyrin payloads and strong light absorption capability, thus contributing to an extremely high 1O2 quantum yield (∼0.91) via an efficient dual energy transfer process. In vivo studies show that they can preferably accumulate in tumors through folate receptor-mediated active delivery, permitting non-invasive fluorescence imaging and effective PDT of tumors in living mice. This study highlights the utility of hybrid semiconductor QDs for both tumor imaging and PDT in vivo.Rational engineering of semiconductor QDs into tumor targeting hybrid nanoparticles through micelle-encapsulating pre-assembled unique TMPyP-Zn-QD complexes, R6G and NIR775 with phospholipid polymers was demonstrated, enabling a dual energy transfer process to trigger remarkable 1O2 quantum yield (∼0.91) and a preferential accumulation in tumors for effective tumor PDT in living mice.Download high-res image (298KB)Download full-size image
Co-reporter:Jin-Wen Shangguan;Yu Liu;Jian-Bin Pan;Bi-Yi Xu;Hong-Yuan Chen
Lab on a Chip (2001-Present) 2017 vol. 17(Issue 1) pp:120-127
Publication Date(Web):2016/12/20
DOI:10.1039/C6LC01250G
In this paper, we propose a generalized concept of microfluidic polydimethylsiloxane (PDMS) on paper (POP) devices, which combines well the merits of paper chips and PDMS chips. First, we optimized the conditions for accurate PDMS spatial patterning on paper, based on screen printing and a high temperature enabled superfast curing technique, which enables PDMS patterning to an accuracy of tens of microns in less than ten seconds. This, in turn, makes it available for seamless, reversible and reliable integration of the resulting paper layer with other PDMS channel structures. The integrated POP devices allow for both porous paper and smooth channels to be spatially defined on the devices, greatly extending the flexibility for designers to be able to construct powerful functional structures. To demonstrate the versatility of this design, a prototype POP device for the colorimetric analysis of liver function markers, serum protein, alkaline phosphatase (ALP) and aspartate aminotransferase (AST), was constructed. On this POP device, quantitative sample loading, mixing and multiplex analysis have all been realized.
Co-reporter:Jin-Wen Shangguan;Yu Liu;Jian-Bin Pan;Bi-Yi Xu;Hong-Yuan Chen
Lab on a Chip (2001-Present) 2017 vol. 17(Issue 1) pp:120-127
Publication Date(Web):2016/12/20
DOI:10.1039/C6LC01250G
In this paper, we propose a generalized concept of microfluidic polydimethylsiloxane (PDMS) on paper (POP) devices, which combines well the merits of paper chips and PDMS chips. First, we optimized the conditions for accurate PDMS spatial patterning on paper, based on screen printing and a high temperature enabled superfast curing technique, which enables PDMS patterning to an accuracy of tens of microns in less than ten seconds. This, in turn, makes it available for seamless, reversible and reliable integration of the resulting paper layer with other PDMS channel structures. The integrated POP devices allow for both porous paper and smooth channels to be spatially defined on the devices, greatly extending the flexibility for designers to be able to construct powerful functional structures. To demonstrate the versatility of this design, a prototype POP device for the colorimetric analysis of liver function markers, serum protein, alkaline phosphatase (ALP) and aspartate aminotransferase (AST), was constructed. On this POP device, quantitative sample loading, mixing and multiplex analysis have all been realized.
Co-reporter:Kai Zhang;Xue-Jiao Yang;Wei Zhao;Ming-Chen Xu;Hong-Yuan Chen
Chemical Science (2010-Present) 2017 vol. 8(Issue 7) pp:4973-4977
Publication Date(Web):2017/06/26
DOI:10.1039/C7SC00909G
Regulation of gene expression is highly important in the area of cell biology. In this work a novel convenient and versatile strategy is reported which permits both gene regulation and imaging in living cells. An oligonucleotide-based biomimetic probe was designed to target an RNA-induced silencing complex (RISC) and served as an agent for the modulation of c-Myc protein expression in living cells through regulating the RNA interference (RNAi) pathway. In this probe, a DNA strand (Strand1) serving as the frame was immobilized on a AuNP with a thiol group at the 5′ end. Strand2, designed to recognize the target RISC with an RNA fragment, was hybridized with the complementary sequence of Strand1. In the original state, the fluorescence of the Cy3 modifier at the 5′ end of Strand2 was quenched by both the AuNP and BHQ2, which labelled the 3′ end of Strand1. In the presence of RISC, Strand2 was cleaved, resulting in a shorter oligo part with a corresponding lower melting temperature than that of the original full-length Strand2. The shorter oligonucleotide strand containing the Cy3 fluorophore was released, accompanied by a recovered fluorescence signal. Through evaluating the fluorescence intensity, the competition for RISC was dynamically monitored in single cells. Furthermore, capturing RISC by this probe resulted not only in restored fluorescence intensity but also increased c-Myc oncogene expression. Hence, gene expression could be selectively and precisely regulated and imaged via the RISC targeting probe. The synthetic method for the biomimetic probe is universally applicable, and facilitates the fundamental study of RNAi pathways, or development of a gene regulation strategy without cytokine activation. The gene regulation and imaging strategy will accelerate the unveiling of the basic role of the RISC cleavage interaction, the mystery of RNA-silencing and therapeutic monitoring of cancer.
Co-reporter:Shan-Wen Hu, Shu Qiao, Bi-Yi Xu, Xiang Peng, Jing-Juan XuHong-Yuan Chen
Analytical Chemistry 2017 Volume 89(Issue 3) pp:
Publication Date(Web):December 27, 2016
DOI:10.1021/acs.analchem.6b04891
Though microfluidic paper analytical devices (μPADs) have attracted paramounting attentions in recent years as promising devices for low cost point-of-care tests, their real applications for blood analysis are still challenged by integrating sample preparation with different detection modes on a same μPAD. Herein, we developed a novel μPAD, which well coupled automatic serum extraction with reliable dual mode iron health tests: fluorescent analysis for Fe3+ and colorimetric ELISA for ferritin. All these functions are made available by in situ carbon dots (CDs) and AuNPs sequential patterning techniques. For CDs immobilization, hydrothermal reaction was taken on paper, to which a patterned through-hole polydimethylsiloxane (PDMS) mask was applied. None fluorescence CDs (nF-CDs) were generated on exposed regions, while the fluorescent CDs (F-CDs) were generated simultaneously on covered regions. Sensitive serum iron quantification was realized on the F-CDs modified regions, where Fe3+ ion can selectively quench the fluorescence of F-CDs. For AuNPs immobilization, electroless plating was taken on nF-CDs modified regions. The resulting AuNPs on nF-CDs layer on one hand triggered the coagulation of blood cells and thus led to the longest ever wicking distance for serum separation, on the other hand facilitated colorimetric enzyme linked immunosorbent assay (ELISA) for detection of serum ferritin. Combining the two readings, the μPAD can provide reliable measurement for serum iron and serum ferritin in whole blood. Furthermore, as CDs and AuNPs modified μPAD has the features of easy handling, low-cost, lightweight, and disposability, it is accounting for a promising prototype for whole blood point-of-care analysis.
Co-reporter:Tao Yu, Ting-Ting Zhang, Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2017 Volume 165() pp:570-576
Publication Date(Web):1 April 2017
DOI:10.1016/j.talanta.2017.01.026
•A novel colorimetric/fluorescent dual-mode sensor is presented for the detection of Hg2+.•Hybridization chain reaction (HCR) combining multifunctional Au NPs is employed for the signal amplification.•Hg2+ down to 1.0 nM could be identified by naked eyes.•The fluorescence can be performed at a broader range of salt concentration.A highly sensitive colorimetric/fluorescent dual-mode sensor based on hybridization chain reaction (HCR) combining multifunctional Au NPs is presented for the detection of Hg2+ in aqueous solution. In Hg2+ absent solution, the surface of Au NPs was covered by hairpin auxiliary DNAs and a single strand DNA (ssDNA), which prevented Au NPs from salt-induced aggregation. At the same time, the fluorescence intensity of the dye-labeled hairpin probes was significantly quenched by Au NPs. In the presence of Hg2+, T-Hg2+-T coordination chemistry between helper DNA and the hairpin probes was induced which triggered the formation of extended double-stranded DNA (dsDNA) polymers via HCR. The formed dsDNA polymers were stiffer which couldn’t attach to Au NPs, resulting in a red-to-blue color change along with salt-induced aggregation of Au NPs for colorimetric sensing. Meanwhile, the fluorescence of dye-labeled DNA turns on. Due to the HCR amplification effect, a highly sensitive detection of Hg2+ was achieved with detection limit of 0.1 nM. Colorimetry is suitable for the analysis in salt solution with concentration lower than 100 mM. It serves as an intuitive method that Hg2+ down to 1.0 nM could be identified by naked eyes. For high-concentration salt solutions such as industrial effluent, fluorescent sensing acts as a better choice. Both the color and fluorescence changes of the proposed sensor exhibited high selectivity against other metal ions. Lake water was collected and analyzed using the dual-mode sensor, the results confirmed the practicability of the proposed approach.A novel colorimetric/fluorescent dual-mode sensor is presented for the detection of Hg2+. The proposed strategy showed good selectivity to Hg2+ and the simultaneously colorimetric/fluorescent detection platform hold advantages of both easy observation and high sensitivity in salt solution with a broad range of concentration, which had good potential for environmental analysis.
Co-reporter:Guang-Sheng Qian;Ting-Ting Zhang;Wei Zhao;Hong-Yuan Chen
Chemical Communications 2017 vol. 53(Issue 34) pp:4710-4713
Publication Date(Web):2017/04/25
DOI:10.1039/C7CC00626H
Plasmon rulers (PRs) exploit the potential of plasmon coupling between individual pairs of noble metal nanoparticles in biological processes, especially single-molecule detection. Herein, for the first time, we report a strategy based on Ag PRs for in situ monitoring of the extension process of telomerase primer (TSP) activated by a single telomerase.
Co-reporter:Ting-Ting Zhang;Fan Yang;Xiang-ling Li;Wei Zhao;Hong-Yuan Chen
Chemical Communications 2017 vol. 53(Issue 41) pp:5614-5617
Publication Date(Web):2017/05/18
DOI:10.1039/C7CC02834B
A multifunctional Ag NP based nanocomposite was fabricated which realized accurate targeting of specific cancer cells and completely initiative therapy without any photoexcitation.
Co-reporter:Shan-Shan Li;Qi-Yuan Guan;Mengmeng Zheng;Yu-Qi Wang;Deju Ye;Bin Kang;Hong-Yuan Chen
Chemical Science (2010-Present) 2017 vol. 8(Issue 11) pp:7582-7587
Publication Date(Web):2017/10/23
DOI:10.1039/C7SC03218H
Intracellular biothiols mediate many important physiological and pathological processes. Due to their low content and competing thiol-reactivity, it is still an unmet challenge to quantify them within a complicated intracellular environment. Herein, we demonstrated a strategy to discriminate three biothiols, i.e. cysteine (Cys), homo-cysteine (Hcy) and glutathione (GSH), and quantify their concentrations within single living cells, using one platform of Raman probe. By monitoring the reaction kinetics of biothiols with Raman probes and discriminating their products with a quantitative principal component analysis (qPCA) method, these three biothiols could be simultaneously quantified in both cell lysis and single living cells. The concentrations of Cys, Hcy and GSH in single Hela cells were 158 ± 19 μM, 546 ± 67 μM and 5.07 ± 0.62 mM, respectively, which gives the precise concentrations of these three biothiols at a single cell level for the first time. This method provides a general strategy for discriminating each component from a mixed system and has potential for quantifying any biomolecules within an in vitro or in vivo biological environment.
Co-reporter:Bin Kang;Shan-Shan Li;Qi-Yuan Guan;Ai-Ping Chen;Pan-Ke Zhang;Li-Bin Zhang;Ji-Wu Wei;Hong-Yuan Chen
Chemical Science (2010-Present) 2017 vol. 8(Issue 2) pp:1243-1250
Publication Date(Web):2017/01/30
DOI:10.1039/C6SC02486F
Apoptosis and necrosis are distinct cell death processes related to many cellular pathways. In situ, quantitatively and dynamically monitoring such processes may provide vitally important information for cell studies. However, such a method still remains elusive, even though current immunochemical methodologies have developed extremely valuable tools. Herein, we demonstrate Raman spectroscopic metrics for validating and quantifying apoptotic and necrotic cells based on their distinct molecular vibrational fingerprints. It not only allows us to quantify apoptotic and necrotic cell populations in situ in adherent cell samples, but also to be capable of continuously monitoring the dynamical processes of apoptosis and necrosis at the same time in one sample. This method provides comparable results with the “gold standard” of flow cytometry, moreover, with several incomparable advantages. Our work offers a powerful new tool for cell apoptosis and necrosis assays and is expected to become a benchmark technology in biological and medical studies.
Co-reporter:Linfeng Sheng;Lesi Cai;Jie Liu;Sichun Zhang;Xinrong Zhang;Hong-Yuan Chen
Chemical Science (2010-Present) 2017 vol. 8(Issue 1) pp:748-754
Publication Date(Web):2016/12/19
DOI:10.1039/C6SC02610A
Metabolic azide amino acid labelling followed by the use of bioorthogonal chemistry is an efficient technique for imaging newly synthesized proteins. Recently, AHA-labelling together with the proximity-ligation assay was used to identify newly synthesized proteins of interest (POI) (Tom Dieck et al., Nat. Meth. 2015, 12, 411). Here we build on this study replacing the proximity-ligation assay with FRET to improve the spatial resolution. Herein, we develop a FRET-based strategy for imaging the newly synthesized endogenous POI within cells: a FRET acceptor is installed onto the newly synthesized proteins via click chemistry, and a FRET donor onto the POI via immunocytochemistry. We found that a photobleaching based FRET efficiency imaging mode and a fluorescence lifetime imaging mode showed the distribution of newly synthesized proteins more accurately compared to the direct observation of FRET signals. We demonstrated the capability of this FRET-based imaging method by visualizing several newly synthesized proteins including TDP-43, tubulin and CaMKIIα in different cell lines. This novel analytical imaging method could be used to visualize other specific endogenous proteins of interest in situ.
Co-reporter:Qiu-Mei Feng, Zhen Zhou, Mei-Xing Li, Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2017 Volume 90(Volume 90) pp:
Publication Date(Web):15 April 2017
DOI:10.1016/j.bios.2016.11.060
•A DNA tetrahedral scaffold-based platform for the construction of ECL biosensor is designed.•DNA tetrahedron provides necessary space for TSP extending and subsequent assembly of luminol labelled Au NPs.•Telomerase from HeLa cells was sensitively detected by the ECL enhancement from both CdS QDs and luminol.•This work suggests that DNA tetrahedral scaffolds serve as an excellent choice for the construction of SPR-ECL system.Proximal metallic nanoparticles (NPs) could quench the electrochemiluminescence (ECL) emission of semiconductor quantum dots (QDs) due to Förster energy transfer (FRET), but at a certain distance, the coupling of light-emission with surface plasmon resonance (SPR) result in enhanced ECL. Thus, the modification strategies and distances control between QDs and metallic NPs are critical for the ECL intensity of QDs. In this strategy, a SPR enhanced ECL sensor based on DNA tetrahedral scaffolds modified platform was reported for the detection of telomerase activity. Due to the rigid three-dimensional structure, DNA tetrahedral scaffolds grafting on the electrode surface could accurately modulate the distance between CdS QDs and luminol labelled gold nanoparticles (L-Au NPs), meanwhile provide an enhanced spatial dimension and accessibility for the assembly of multiple L-Au NPs. The ECL intensities of both CdS QDs (−1.25 V vs. SCE) and luminol (+0.33 V vs. SCE) gradually increased along with the formation of multiple L-Au NPs at the vertex of DNA tetrahedral scaffolds induced by telomerase, bringing in a dual-potential ECL analysis. The proposed method showed high sensitivity for the identification of telomerase and was successfully applied for the differentiation of cancer cells from normal cells. This work suggests that DNA tetrahedral scaffolds could serve as an excellent choice for the construction of SPR-ECL system.
Co-reporter:Linfeng Sheng, Lesi Cai, Jia Wang, Zhanping Li, Yuxiang Mo, Sichun Zhang, Jing-Juan Xu, Xinrong Zhang, Hong-Yuan Chen
International Journal of Mass Spectrometry 2017 Volume 421(Volume 421) pp:
Publication Date(Web):1 October 2017
DOI:10.1016/j.ijms.2017.07.008
•A strategy for visualization of newly synthesized proteins and specific lipids simultaneously by TOF-SIMS was demonstrated.•The localization of newly synthesized proteins and specific lipids during cells division is different.•3-dimension images of newly synthesized proteins and specific lipids are obtained during cell division.Cell growth and division are important processes for life. To understand the distribution and behaviors of the key molecules that dominate the cell growth and division still remains a challenge. Herein, we propose a strategy for visualization of newly synthesized proteins by TOF-SIMS coupled with metabolic incorporation of 15N labelled amino acids during the cell growth. Moreover, we simultaneously image phosphatidylcholine and cholesterol during the cell division, since TOF-SIMS is especially suitable for this kind of molecules. With the proposed strategy, 2-dimension and 3-dimension images of proteins and lipids are obtained during cell division. We found that phosphatidylcholine was widely distributed in the cleavage furrow while the newly synthesized proteins exist few in this region. This technique will be a valuable tool to study the molecular behaviors and their spatial distribution in single cell.A strategy for visualization of newly synthesized proteins and specific lipids simultaneously in single cell by TOF-SIMS was demonstrated. By introducing 15N arginine and 15N lysine into the newly synthesized proteins, we applied TOF-SIMS to simultaneously detect the characteristic peaks of 15N labelled amino acids and specific fragmented molecular ions of lipids, enabling us to image newly synthesized proteins and specific lipids at submicrometer resolution. This technique will be a valuable tool to study the molecular behaviours and their spatial distribution in single cell. Bi3+ LMIG was used to scan over the cell to acquire image; Ar3500+ was used to sputter over the cell to obtain depth profiles.Download high-res image (82KB)Download full-size image
Co-reporter:Xiang-Ling Li, Zhuo-Lei Zhang, Wei Zhao, Xing-Hua Xia, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Science 2016 vol. 7(Issue 5) pp:3256-3263
Publication Date(Web):04 Feb 2016
DOI:10.1039/C5SC04369G
Due to the complexity of biological systems and the ultralow concentration of analytes, improving the signal-to-noise ratio and lowering the limit of detection to allow highly sensitive detection is key to biomolecule analysis, especially intracellular analysis. Here, we present a method for highly sensitive imaging of mRNA in living cells by using novel invisible oriented probes to construct a turn-on signal generation mechanism from zero background. Two DNA probes (S1 and S2) are asymmetrically modified on two small gold nanoparticles (AuNPs) with a diameter of 20 nm. The hybridization of the two DNA probes with a single target mRNA leads to the formation of an AuNP dimer which shows a prominent plasmonic coupling effect. It generates a strong scattering signal from zero-background under a dark-field spectral analysis system. The unique design of the oriented assembly dimer has the ability to easily discriminate the target signal from the inherent cellular background noise in intracellular detection, thus making this approach a valuable technique for imaging single survivin mRNA and monitoring the distribution of survivin mRNA in tumor cells.
Co-reporter:Peng Wu, Xiandeng Hou, Jing-Juan Xu and Hong-Yuan Chen  
Nanoscale 2016 vol. 8(Issue 16) pp:8427-8442
Publication Date(Web):23 Mar 2016
DOI:10.1039/C6NR01912A
Ratiometric fluorescent sensors, which can provide built-in self-calibration for correction of a variety of analyte-independent factors, have attracted particular attention for analytical sensing and optical imaging with the potential to provide a precise and quantitative analysis. A wide variety of ratiometric sensing probes using small fluorescent molecules have been developed. Compared with organic dyes, exploiting semiconductor quantum dots (QDs) in ratiometric fluorescence sensing is even more intriguing, owing to their unique optical and photophysical properties that offer significant advantages over organic dyes. In this review, the main photophysical mechanism for generating dual-emission from QDs for ratiometry is discussed and categorized in detail. Typically, dual-emission can be obtained either with energy transfer from QDs to dyes or with independent dual fluorophores of QDs and dye/QDs. The recent discovery of intrinsic dual-emission from Mn-doped QDs offers new opportunities for ratiometric sensing. Particularly, the signal transduction of QDs is not restricted to fluorescence, and electrochemiluminescence and photoelectrochemistry from QDs are also promising for sensing, which can be made ratiometric for correction of interferences typically encountered in electrochemistry. All these unique photophysical properties of QDs lead to a new avenue of ratiometry, and the recent progress in this area is addressed and summarized here. Several interesting applications of QD-based ratiometry are presented for the determination of metal ions, temperature, and biomolecules, with specific emphasis on the design principles and photophysical mechanisms of these probes.
Co-reporter:Fei Xu, Yuan-Cheng Zhu, Zheng-Yuan Ma, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2016 vol. 52(Issue 14) pp:3034-3037
Publication Date(Web):14 Jan 2016
DOI:10.1039/C5CC09963C
Using single stranded DNA (ssDNA) as a distance controller and Au nanoparticles (NPs) functionalized with ssDNA as novel energy-transfer nanoprobes, an ultrasensitive energy-transfer based photoelectrochemical protein biosensor was realized.
Co-reporter:Tao Yu, Pan-Pan Dai, Jing-Juan Xu, and Hong-Yuan Chen
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 7) pp:4434
Publication Date(Web):January 29, 2016
DOI:10.1021/acsami.5b12117
Facile and efficient detection of cancer cells at their preclinical stages is one of the central challenges in cancer diagnostics. A direct, rapid, highly sensitive and specific biosensor for detection of cancer biomarkers is desirable in early diagnosis and prognosis of cancer. In this work, we developed, for the first time, an easy and intuitive dispersion-dominated colorimetric strategy for cancer cell detection based on combining multi-DNA released from an aptamer scaffold with cyclic enzymatic amplification, which was triggered by aptamer DNA conformational switch and demonstrated by non-cross-linking gold nanoparticles (Au NPs) aggregation. First, five kinds of messenger DNAs (mDNAs) were aligned on the cancer cell aptamers modified on magnetic beads (MBs) to form mDNAs-Apt-MBs biocompatible nanosensors. In the presence of target cells, the aptamer would bind to the receptors on the cell membranes, and mDNAs would be released, resulting in the first amplification that one biological binding event would cause the release of multiple kinds of mDNAs simultaneously. After magnetic separation, the released mDNAs were introduced into the cyclic enzymatic amplification to cleave more single strand DNA (ssDNA) fragments. Instead of modification of Au NPs, these fragments and mDNAs could be adsorbed on the surface of Au NPs to prevent particle aggregation and ensure the stability and color of solution in high salt environments. The linear response for HL-60 cells in a concentration range from 10 to 104 cells was obtained with a detection limit of four cells in buffer solution. Moreover, the feasibility of the proposed strategy was demonstrated in a diluted serum sample. This dual signal amplification method can be extended to other types of cancer cells, which has potential application in point-of-care cancer diagnosis.Keywords: aptamer; cancer cells recognition; colorimetric detection; dual signal amplification; gold nanoparticles; magnetic nanoparticle
Co-reporter:Qiu-Mei Feng, Yi-Zhong Shen, Mei-Xing Li, Zhuo-Lei Zhang, Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2016 Volume 88(Issue 1) pp:937
Publication Date(Web):December 2, 2015
DOI:10.1021/acs.analchem.5b03670
Here, a dual-wavelength ratiometric electrochemiluminescence (ECL) approach is reported based on resonance energy transfer (RET) from graphite-like carbon nitride nanosheet (g-C3N4 NS) to Ru(bpy)32+ for sensitive detection of microRNA (miRNA). In this approach, Au nanoparticles (Au NPs) functionalized g-C3N4 NS nanohybrid (Au-g-C3N4 NH) coated on glassy carbon electrode (GCE) could exhibit strong and stable ECL emissions with emission peak centered at 460 nm. The ECL emission at such wavelength matched well with the absorption peak of Ru(bpy)32+ as well as impeccably stimulating the emission of Ru(bpy)32+ at the wavelength of 620 nm, producing ECL-RET with high efficiency. Thus, based on the ECL signals quenching at 460 nm and increasing at 620 nm, a dual-wavelength ratiometric ECL-RET system was achieved. This system was then utilized for determination of target miRNA. With the attachment of thiol-modified molecular beacon on Au-g-C3N4 NH, target miRNA hybridized with the molecular beacon to form a DNA-RNA duplex. The obtained DNA-RNA duplex could be cleaved by duplex-specific nuclease to release target miRNA which would take part in the next cycle for further hybridization. Finally, the introducing of Ru(bpy)32+ was through the probe DNA-Ru(bpy)32+ complementary with the rest single-strand DNA on electrode. By measuring the ratio of ECL460 nm/ECL620 nm, we could accurately quantify the concentration of miRNA-21 in a wide range from 1.0 fM to 1.0 nM. This work provides an important reference for the study of dual-wavelength ECL ratiometry and also exhibits potential capability in the detection of nucleic acids.
Co-reporter:Hai-Wei Shi, Wei Zhao, Zhen Liu, Xi-Cheng Liu, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2016 Volume 88(Issue 17) pp:8795
Publication Date(Web):August 10, 2016
DOI:10.1021/acs.analchem.6b02204
We report a bipolar electrode (BPE) sensing platform for the temporal detection of cancer cells. Combining the advantages of anodic dissolution and electrochemiluminescence (ECL), this strategy shows an ultralow detection limit down to 5 cells/cm2. At the anode working as the reporting pole, Au NPs were assembled through DNA double strand, which served as both catalyzer for the ECL reaction of luminol/H2O2 and seeds for the chemical reduction of Ag, the anodic dissolution probe. The duration of Ag layer dissolution was positively correlated with the amount of Ag but negatively related to the controlled potential and the conductivity of the circuit. Therefore, it was possible to amplify a slight conductivity change through tuning the other two factors. As the formation of Ag@Au completely quenched the ECL emission of luminol, the ECL emission recovery reflected the extent of anodic dissolution. Through monitoring the ECL recovery time before and after the incubation of cells on the cathode, a few number of cells could be quantified due to slight difference of the conductivity. This method shows several merits. First, the combination of anodic dissolution and ECL significantly increases the detection sensitivity of BPE device. In addition, this strategy broadens the application of BPE for the ultrasensitive monitoring of cancer cells, which was applied to investigate the capture efficiencies of antibodies and aptamers toward MCF-7 and A549.
Co-reporter:Jun Hu, Xiao-Xiao Jiang, Jiang Wang, Qi-Yuan Guan, Pan-Ke Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2016 Volume 88(Issue 14) pp:7245
Publication Date(Web):June 14, 2016
DOI:10.1021/acs.analchem.6b01490
In this work, a synchronized polarization induced electrospray ionization (SPI-ESI) method is developed and applied for the analysis of single-cell samples. In SPI-ESI, periodic alternating current square wave voltage (AC-SWV) is applied to induce the bipolar spray and both positive-ion and negative-ion mass spectra are obtained through one measurement by synchronizing the mode of mass analyzer with the bipolar spray process. Compared with conventional nanoelectrospray ionization (nESI, flow rate < 1000 nL/min), ultralow spray flow rate (pico-electrospray ionization, pESI, flow rate < 1000 pL/min) is achieved in SPI-ESI without loss of its sensitivity. The decrease of flow rate prolongs the MS signal duration from single-cell samples to acquire ms2 data for components determination. To our knowledge, this is the first time to successfully achieve comprehensive analysis of single-cell samples by combining both positive-ion and negative-ion mass spectra. Ultimately, 86 components are profiled from single Allium cepa cells and 94 components are profiled from single PC-12 cells.
Co-reporter:Yuan-Cheng Zhu, Nan Zhang, Yi-Fan Ruan, Wei-Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2016 Volume 88(Issue 11) pp:5626
Publication Date(Web):May 6, 2016
DOI:10.1021/acs.analchem.6b01261
This work reports a plasmonic strategy capable of label-free yet amplified photoelectrochemical (PEC) immunoassay for the sensitive and specific detection of model protein p53, an important transcription factor that regulates the cell cycle and functions as a tumor suppressor. Specifically, on the basis of Au nanoparticles (NPs) deposited on hierarchically ordered TiO2 nanotubes (NTs), a protein G molecular membrane was used for immobilization of alkaline phosphatase (ALP) conjugated anti-p53 (ALP-a-p53). Due to the immunological recognition between the receptor and target, the plasmonic charge separation from Au NPs to the conduction band of TiO2 NTs could be influenced greatly that originated from multiple factors. The degree of signal suppression is directly associated with the target concentration, so by monitoring the changes of the plasmonic photocurrent responding after the specific binding, a new plasmonic PEC immunoassay could be tailored for label-free and amplified detection. The operating principle of this study could be extended as a general protocol for numerous other targets of interest.
Co-reporter:Huai-Rong Zhang, Yin-Zhu Wang, Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2016 Volume 88(Issue 5) pp:2884
Publication Date(Web):February 2, 2016
DOI:10.1021/acs.analchem.5b04716
In this work, we developed a visual electrochemiluminescence (ECL) sensing platform based on a dual-bipolar electrode (D-BPE) array chip. The chip was composed of two arrays of BPEs and three separated arrays of reservoirs filled with buffer, Ru(bpy)32+-TPrA and luminol solutions, respectively. Both BPEs served as ECL reporting platforms. By applying 6.0 V voltage, an array of orange electrochemiluminescence (ECL) signals belonging to Ru(bpy)32+ turned on. After adding DNAzyme and H2O2 in Ru(bpy)32+ and luminol reservoirs, the orange Ru(bpy)32+ signals decreased until vanished due to the quenching effect; meanwhile, a new array of blue ECL signals turned on because of the luminol-H2O2 ECL reaction. The designed D-BPE owns superior properties compared with the three-electrode system benefiting from the quantitative relation of bipolar systems, which greatly enhanced the ECL detection sensitivity. Meanwhile, the visual color-switch ECL and the ratiometric detecting principle made the results easier to evaluate and more accurate. Quantitative detection of HL-60 cancer cells from 320 cells/mL to 2.5 × 105 cells/mL with two linear ranges was achieved. The detection limit was down to 80 cells/mL. Finally, this D-BPE chip could distinguish the tumor cells from normal cells and provide a prospect for cancer diagnosis in a high-throughput, visual way.
Co-reporter:Qiu-Mei Feng, Meng-Jiao Zhu, Ting-Ting Zhang, Jing-Juan Xu and Hong-Yuan Chen  
Analyst 2016 vol. 141(Issue 8) pp:2474-2480
Publication Date(Web):08 Mar 2016
DOI:10.1039/C6AN00241B
A novel three-dimensionally structured DNA probe is reported to realize in situ “off–on” imaging of intracellular telomerase activity. The probe consists of a DNA tetrahedron and a hairpin DNA on one of the vertices of the DNA tetrahedron. It is composed of four modified DNA segments: S1–Au nanoparticle (NP) inserting a telomerase strand primer (TSP) and S2–S4, three Cy5 dye modified DNA segments. Fluorescence of Cy5 at three vertices of the DNA tetrahedron is quenched by the Au NP at the other vertex due to the effective fluorescence resonance energy transfer (FRET) (“off” state). When the probe meets telomerase, the hairpin structure changes to rod-like through complementary hybridization with the telomerase-triggered stem elongation product, resulting in a large distance between the Au NP and Cy5 and the recovery of Cy5 fluorescence (“on” state). The molar ratio of 3:1 between the reporter (Cy5) and the target related TSP makes the probe show high sensitivity and recovery efficiency of Cy5 in the presence of telomerase extracted from HeLa cells. Given the functional and compact nanostructure, the mechanically stable and noncytotoxic nature of the DNA tetrahedron, this FRET-based probe provides more opportunities for biosensing, molecular imaging and drug delivery.
Co-reporter:Jia-Dong Zhang, Wei-Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Journal of Electroanalytical Chemistry 2016 Volume 781() pp:56-61
Publication Date(Web):15 November 2016
DOI:10.1016/j.jelechem.2016.10.017
•A closed bipolar cell driven by three-electrode system for the studies of the electrochemical behavior is constructed.•The impacts of the reagents' concentration, electrode size and material on its electrochemical behaviors have been studied.•The experimental and the theoretical results agree with each other very well.•This research could deepen our understanding of bipolar chemistry and be useful for the future c-BPE-based applications.Here we report the studies on the electrochemical behaviors at a closed bipolar cell which is composed of two separated reaction cells containing a closed bipolar electrode (c-BPE) and its driving electrodes. The influence factors such as the concentration of the reagents, the size and material of the electrodes are studied experimentally and theoretically. And the experimental results fit with the theoretic calculation very well. Significantly, unlike the previous studies focusing on the coupling of the two c-BPE poles, this work also considers the effect of the reaction on the driving electrode on the electrochemical behavior. We believe that this research could deepen our understanding of bipolar chemistry and be useful for the future c-BPE-based applications.
Co-reporter:Yin-Zhu Wang, Wei Zhao, Pan-Pan Dai, Hai-Jie Lu, Jing-Juan Xu, Jing Pan, Hong-Yuan Chen
Biosensors and Bioelectronics 2016 Volume 86() pp:683-689
Publication Date(Web):15 December 2016
DOI:10.1016/j.bios.2016.07.067
•A spatial-resolved ECL ratiometry based on a closed biopolar electrode was designed.•Two ECL emitter/co-reactant systems were separated in space to limit mutual interference.•Neither optical filter nor spectrometer was required in this system which enhanced the sensitivity to a great extent.•Pt-PAMAM-DNAzyme was synthesized and served as quencher of ECL at the cathode but promoter of ECL at the anode.•Highly sensitive ratiometric detection of PSA was achieved with a linear range from 0.10 to 200 ng/mL.Herein, a spatial-resolved electrochemiluminescene (ECL) ratiometry based on a closed biopolar electrode (BPE) is reported for the highly sensitive detection of prostate specific antigen (PSA). Au@g-C3N4 NCs as one ECL emitter were firstly coated on the cathode of BPE, while the anode of the BPE served for calibration via another ECL substance, Ru(bpy)32+. The electroneutrality across the BPE makes the reactions on each pole of BPE electrically coupled. Thus one electrochemical sensing reaction at one pole of BPE could be quantified at both ends. A composite, Pt-PAMAM-DNAzyme was assembled on the surface of cathode via DNA hybridization between probe DNA and PSA aptamer. It acted as an ECL quencher of g-C3N4 via resonance energy transfer (RET) and catalyzing the reduction of O2, the co-reactant of g-C3N4. Meanwhile, it could promote the ECL of Ru(bpy)32+ at anode, since the catalytic reduction of O2 at the cathode increased the faradiac current flowing through the BPE. Based on this signal composite, an ECL “off-on” phenomenon was observed at the cathode, after Pt-PAMAM-DNAzyme was “peeled off” by PSA. Conversely, at the anode, an “on-off” ECL changing was obtained. Therefore, a sensitive ratiometry for PSA detection was achieved with a linear range from 0.10 to 200 ng/mL. Since the two ECL emitters were physically separated, the ratiometric system was relatively simple and neither optical filters nor spectrometer were required. The strategy combining the ECL ratiometry and BPE broadens the applications of BPE-ECL and shows good perspective in clinical application.
Co-reporter:Dr. Mei-Sheng Wu;Zhen Liu;Dr. Jing-Juan Xu; Hong-Yuan Chen
ChemElectroChem 2016 Volume 3( Issue 3) pp:429-435
Publication Date(Web):
DOI:10.1002/celc.201500361

Abstract

An advanced biosensor based on a closed bipolar electrode (BPE)–electrochemiluminescence (ECL) strategy is proposed for cancer cell adhesion, specific recognition, and detection with dual biomarkers. The system consists of a two-channel polydimethylsiloxane (PDMS) chip (sensing channel and reporting channel) connected through a U-shaped indium tin oxide BPE at a glass surface. A sandwich-type cancer cell detection model is developed at the cathode of the BPE with two recognition molecules, folic acid (FA) and an aptamer. On the basis of the high affinity between FA and the folate receptor that is overexpressed at a cancer cell membrane as well as the excellent conductivity of graphene–Au conjugates, this strategy could achieve the sensitive detection of HL-60 cells, with a limit as low as 18 cells in 30 μL of cell suspension. Control experiments confirm that the sandwich assay specifically captures cancer cells and recognizes target cells.

Co-reporter:Yin-Zhu Wang, Nan Hao, Qiu-Mei Feng, Hai-Wei Shi, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2016 Volume 77() pp:76-82
Publication Date(Web):15 March 2016
DOI:10.1016/j.bios.2015.08.057
•A novel ratiometric ECL biosensor for cancer cells detection was designed.•g-C3N4 nanosheets immobilized on ITO electrode acted as reductive–oxidative ECL emitter.•Luminol in Ag–PAMAM–luminol biocomposite acted as oxidative–reductive ECL emitter.•Ag–PAMAM composite not only as the ECL quencher of g-C3N4, but also as the carrier for lots of luminol.•The ECL ratio between both emitters could be controlled by DNA hybridization.In this work, a dual-signaling electrochemiluminescence (ECL) ratiometric sensing approach for the detection of HL-60 cancer cells was reported for the first time. G-C3N4 nanosheets and Ag–PAMAM–luminol nanocomposits (Ag–PAMAM–luminol NCs) were prepared and served as reductive–oxidative and oxidative–reductive ECL emitters respectively. DNA probe functionalized Ag–PAMAM–luminol NCs would hybridize with aptamers modified onto magnetic beads. In the presence of HL-60 cells, the aptamer would conjugate with the target cell and release Ag–PAMAM–luminol NCs. After magnetic separation, released Ag–PAMAM–luminol NCs would hybridize with capture DNA on g-C3N4 nanosheets. ECL from g-C3N4 nanosheets coated on ITO electrode at −1.25 V (vs SCE) could be quenched by Ag–PAMAM–luminol NCs due to the resonance energy transfer (RET) from g-C3N4 nanosheets to Ag NPs. Meanwhile, Ag–PAMAM–luminol brought the ECL signal of luminol at +0.45 V (vs SCE). Thus, the concentration of HL-60 cancer cells could be quantified by both the quenching of ECL from g-C3N4 nanosheets and the enhancement of ECL from luminol. By measuring the ratio of ECL intensities at two excitation potentials, this approach could achieve sensitive and reliable detection for cancer cells in a wide range from 200 cells/mL to 9000 cells/mL with the detection limit of 150 cells (S/N=3).
Co-reporter:Hai-Wei Shi, Wei Zhao, Zhen Liu, Xi-Cheng Liu, Mei-Sheng Wu, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2016 Volume 154() pp:169-174
Publication Date(Web):1 July 2016
DOI:10.1016/j.talanta.2016.03.059
•A sensitive ECL approach based on a closed ITO bipolar electrode for PSA detection in human serum was provided.•A dual-amplification strategy on both poles of closed bipolar electrodes was proposed.•Th@SiO2 NPs were introduced as both recognition probes for PSA and signal amplification indicators.•The approach could detect PSA in a wide range from 0.1 pg/mL to 0.1 μg/mL.A highly sensitive electrogenerated chemiluminescence (ECL) biosensor was developed on the basis of a closed bipolar electrode (BPE) apparatus for the analysis of prostate specific antigen (PSA). Bipolar modifications bring up two different stages of enhancement on the same electrode. Anodic enhancement was conducted by modifying gold nanoparticles (Au NPs) to catalyze the anodic ECL reaction between luminol and hydrogen peroxide. Cathodic introduction of thionine tagged PSA antibody led to a further pertinently enhancement synchronized with the PSA amount variation, because the existence of thionine greatly increased the rate of electron gains on cathode, leading to the corresponding acceleration of anodic ECL reaction. The more thionine modified target molecules were introduced, the faster luminol was oxidized, the higher faraday current approached, and sensitive quantification was realized in correlation with the responsive ECL intensity differences. The quantification resulted in a good determination range between 0.1 pg/mL and 0.1 µg/mL. This strategy mainly took advantage of the special structure of closed BPE to realize a simultaneous amplification on both ends of BPE. Moreover, the platform had a potential of providing a multi-functional strategy for the realization of other bio-detections by simply substituting the PSA sandwich structure with other bio-structures.A joint enhancement of closed bipolar electrode (BPE) ECL biosensor for PSA detection has been fabricated by introducing Au NPs on anode to catalyze anodic luminol-H2O2 reaction and modifying silica beads wrapped thionine (Th@SiO2 NPs) on the cathode to increase systematic electron transfer which could further enhance the ECL intensity. This sensor combines sensitivity, wide detection as well as range practicability.
Co-reporter:Shan-Wen Hu, Bi-Yi Xu, Shu Qiao, Ge Zhao, Jing-Juan Xu, Hong-Yuan Chen, Fu-Wei Xie
Talanta 2016 Volume 150() pp:455-462
Publication Date(Web):1 April 2016
DOI:10.1016/j.talanta.2015.12.052
•.A novel gas collecting platform was fabricated for simultaneous sample extraction.•Nicotine accumulation is determined in a simulated respiration process.•Relationships between times, distances away from smokers and nicotine are clarified.In this work, we report a novel microfluidic gas collecting platform aiming at simultaneous sample extraction and multiplex mass spectrometry (MS) analysis. An alveolar-mimicking elastic polydimethylsiloxane (PDMS) structures was designed to move dynamically driven by external pressure. The movement was well tuned both by its amplitude and rhythm following the natural process of human respiration. By integrating the alveolar units into arrays and assembling them to gas channels, a cyclic contraction/expansion system for gas inhale and exhale was successfully constructed. Upon equipping this system with a droplet array on the alveolar array surface, we were able to get information of inhaled smoke in a new strategy. Here, with cigarette smoke as an example, analysis of accumulation for target molecules during passive smoking is taken. Relationships between the breathing times, distances away from smokers and inhaled content of nicotine are clarified. Further, by applying different types of extraction solvent droplets on different locations of the droplet array, simultaneous extraction of nicotine, formaldehyde and caproic acid in sidestream smoke (SS) are realized. Since the extract droplets are spatially separated, they can be directly analyzed by MS which is fast and can rid us of all complex sample separation and purification steps. Combining all these merits, this small, cheap and portable platform might find wide application in inhaled air pollutant analysis both in and outdoors.A novel microfluidic gas collecting platform aiming at simultaneous sample extraction and multiplex mass spectrometry analysis has been developed. This small, cheap and portable platform might find wide application in inhaled air pollutant analysis both in and outdoors.
Co-reporter:Peng Wu, Chaoying Xu, Xiandeng Hou, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Science 2015 vol. 6(Issue 8) pp:4445-4450
Publication Date(Web):21 May 2015
DOI:10.1039/C5SC01497B
Fingerprints are a unique characteristic of an individual. Recently, it has been realized that fingerprints carry more information about individuals than just their identity, for example, they may identify potential addicts and terrorists carrying explosives. Therefore, the development of imaging moieties capable of both fingerprint staining and drug/explosive visualization is of significant importance for forensic chemistry. Here we developed a nanohybrid comprising green- and red-emitting QDs for simultaneous fingerprint imaging and TNT visualization in fingerprints. The red-emitting Cu-doped ZnCdS (Cu–ZnCdS) QDs were embedded into silica nanoparticles and the green-emitting ZnCdS QDs were anchored onto the surface of the silica nanoparticles and further functionalized with polyallylamine (PAA). Both components of the nanohybrid, i.e., the PAA-functionalized green QDs and red QD-doped silica nanoparticles, could be explored for fingerprint imaging. Due to the formation of a Meisenheimer complex between TNT and PAA, the green-emitting QDs could be quenched by TNT, meanwhile the red-emitting QDs were inert. Therefore, the nanohybrid exhibited a traffic light-type fluorescence color change (green-yellow-red) to TNT concentration in the range of 40–400 μM. This method is promising for potential applications in security-screening needs in public areas such as airports and train stations.
Co-reporter:Xiao-Rong Li, Ming-Chen Xu, Hong-Yuan Chen and Jing-Juan Xu  
Journal of Materials Chemistry A 2015 vol. 3(Issue 21) pp:4355-4362
Publication Date(Web):21 Apr 2015
DOI:10.1039/C5TB00312A
Bimetallic Au@Pt@Au triple-layered core–shell nanoparticles consisting of a Au core, Pt inner shell, and an outer shell composed of Au protuberances on graphene oxide (GO) nanosheets were successfully prepared by a galvanic replacement and reagent reduction reaction. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and cyclic voltammetry (CV) were employed to characterize the GO-supported Au@Pt@Au (GO/Au@Pt@Au) nanocomposites. The as-prepared catalyst has peroxidase-like activity, allowing it to express high electrocatalytic ability in hydrogen peroxide (H2O2) oxidation and reduction, thus leading to a highly sensitive H2O2 bi-directional amperometric sensing. The bi-directional sensor showed a linear range from 0.05 μM to 17.5 mM with a detection limit of 0.02 μM (S/N = 3) at an applied potential of +0.5 V and a linear range from 0.5 μM to 110 mM with a detection limit of 0.25 μM (S/N = 3) at an applied potential of −0.3 V. The proposed sensor was tested to determine H2O2 released from living cells and shows good application potential in biological electrochemistry.
Co-reporter:Yingshu Guo, Jia liu, Guangxu Yang, Xiaofeng Sun, Hong-Yuan Chen and Jing-Juan Xu  
Chemical Communications 2015 vol. 51(Issue 5) pp:862-865
Publication Date(Web):20 Nov 2014
DOI:10.1039/C4CC08428D
A conveniently amplified DNAzyme-based fluorescence strategy was designed for highly sensitive detection of ATP or reduced thiol based on the introduction of an ATP aptamer or a disulfide bond in the bioconjugates of magnetic nanoparticles (MNP) and polystyrene microsphere–DNAzyme complexes (PSM–DNAzyme).
Co-reporter:Yan-Yan Zhang, Qiu-Mei Feng, Jing-Juan Xu, and Hong-Yuan Chen
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 47) pp:26307
Publication Date(Web):November 11, 2015
DOI:10.1021/acsami.5b09129
In this work, oligonucleotide-encapusulated silver nanoclusters were applied in the electrochemiluminescence (ECL) system of CdS nanocrystals (NCs)/ K2S2O8 based on dual ECL quenching effects. We found that the ECL emission of CdS NCs matched well with the absorption band of oligonucleotide encapsulated Ag nanoclusters, which could act as the energy acceptor of CdS NCs ECL so as to lead to an effective ECL resonance energy transfer (RET). On the other hand, the Ag nanoclusters could also catalyze electrochemical reduction of K2S2O8, resulting in increased consumption of ECL coreactant near the working electrode and decreased ECL intensity from CdS NCs. On the basis of the dual ECL quenching effects, a sensitive ECL biosensor for detection of microRNA was successfully achieved with a wide linear range from 10 fM to 100 pM.Keywords: electrochemiluminescence; microRNA detection; resonance energy transfer; silver nanoclusters; synergistic quenching effect
Co-reporter:Shan-Wen Hu, Bi-Yi Xu, Wei-ke Ye, Xing-Hua Xia, Hong-Yuan Chen, and Jing-Juan Xu
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 1) pp:935
Publication Date(Web):December 19, 2014
DOI:10.1021/am5075216
We propose a novel method to obtain versatile droplets arrays on a regional hydrophilic chip that is fabricated by PDMS soft lithography and regional plasma treatment. It enables rapid liquid dispensation and droplets array formation just making the chip surface in contact with solution. By combining this chip with a special Christmas Tree structure, the droplets array with concentrations in gradient is generated. It possesses the greatly improved performance of convenience and versatility in bioscreening and biosensing. For example, high throughput condition screening of toxic tests of CdSe quantum dots on HL-60 cells are conducted and cell death rates are successfully counted quickly and efficiently. Furthermore, a rapid biosensing approach for cancer biomarkers carcinoma embryonic antigen (CEA) is developed via magnetic beads (MBs)-based sandwich immunoassay methods.Keywords: droplets array; liquid dispensation; rapid analysis; surface wettability
Co-reporter:Mei-Sheng Wu, Xiao-Tao Sun, Meng-Jiao Zhu, Hong-Yuan Chen and Jing-Juan Xu  
Chemical Communications 2015 vol. 51(Issue 74) pp:14072-14075
Publication Date(Web):29 Jul 2015
DOI:10.1039/C5CC06229B
A mesoporous silica film-assisted amplification method is reported for the first time for the sensitive electrochemiluminescence detection of cancer cells.
Co-reporter:Nan Hao, Pan-Pan Dai, Tao Yu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2015 vol. 51(Issue 70) pp:13504-13507
Publication Date(Web):13 Jul 2015
DOI:10.1039/C5CC05350A
A dual target-recycling amplification strategy for sensitive detection of microRNAs based on duplex-specific nuclease and catalytic hairpin assembly was reported for the first time.
Co-reporter:Jing Wang, Xiang-Ling Li, Jia-Dong Zhang, Nan Hao, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2015 vol. 51(Issue 58) pp:11673-11676
Publication Date(Web):09 Jun 2015
DOI:10.1039/C5CC03693C
Using the DNA bio-gate and duplex-specific nuclease assisted target recycling, a facile electrochemiluminescence assay was developed for the sensitive detection of survivin mRNA.
Co-reporter:Zheng-Yuan Ma, Yi-Fan Ruan, Nan Zhang, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2015 vol. 51(Issue 39) pp:8381-8384
Publication Date(Web):31 Mar 2015
DOI:10.1039/C5CC01832C
Based on the assay of DNA binding proteins upon visible light irradiation, a photoelectrochemical sensor was constructed for successfully probing a DNA–protein interaction for the first time.
Co-reporter:Wei-Wei Zhao, Ying-Mei Han, Yuan-Cheng Zhu, Nan Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2015 Volume 87(Issue 11) pp:5496
Publication Date(Web):May 18, 2015
DOI:10.1021/acs.analchem.5b01360
Photoelectrochemical (PEC) immunoassay is an attractive methodology as it allows for an elegant and sensitive protein assay. However, advanced PEC immunoassay remains challenging and the established amplifications rely almost exclusively on the labeling of various enzymes, which usually suffer the inferior stabilities. Here we report the development and validation of the DNA labeling that leads to a unique amplification probe for the sensitive PEC immunoassay of HIV-1 capsid protein, p24 antigen, an important biomarker of human immune deficiency virus (HIV). Following the sandwich immunobinding, the DNA tags could be released and the subsequent dipurinization of the oligonucleotide strands enables the easy oxidation of free nucleobases at a CdTe quantum dots (QDs) modified ITO transducer. Such DNA tags induced PEC amplification and readout permits the exquisite assay of HIV-1 p24 antigen with high sensitivity. As compared to the existing method of enzymatic labeling, the easy preparation and stability of these labels make them very suitable for PEC amplification. Another merit of this method is that it separates the immunobinding from the PEC transducer, which eliminates the commonly existing affection during the biorecognition processes. This work paves a new route for the PEC immunoassay of HIV-1 p24 antigen and provides a general format for the PEC biomolecular detection by means of the DNA labeling.
Co-reporter:Pan-Pan Dai, Tao Yu, Hai-Wei Shi, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2015 Volume 87(Issue 24) pp:12372
Publication Date(Web):November 13, 2015
DOI:10.1021/acs.analchem.5b03890
Semiconductor nanocrystals usually suffer from weak electrogenerated chemiluminescence (ECL) emissions compared with conventional organic emitters. In this work, we propose, for the first time, a very convenient but effective way to greatly enhance ECL emission of semiconductor TiO2 nanotubes (NTs) by H2O2 and K2S2O8 as dual coreactants, generating ECL emission ca. 6.3 and 107 times stronger than that of K2S2O8 or H2O2 as an individual coreactant, respectively. Scanning electron microscopy, X-ray diffraction, and electron paramagnetic resonance spectral studies were carried out to investigate the ECL enhancement mechanism. The ECL enhancement of TiO2 NTs by the K2S2O8–H2O2 system was supposed to originate from the coordination of H2O2 to the TiO2 surface and the synergy effect between H2O2 and K2S2O8 in the ECL process. The coordination of H2O2 to the surface of TiO2 could stabilize the electrogenerated coreactant-related radical OH• (hydroxyl radical), which could obviously promote the amount of sulfate radical anion (SO4•—) near the electrode surface by inducing decomposition of K2S2O8 into SO4•— or inhibiting the consumption of SO4•— by its reaction with H2O. The holes (h+) released from SO4•— were injected into the valence band of TiO2, resulting in more TiO2+, which combined with the electrons coming from the conduction band with an enhanced light emission. Moreover, this enhancement effect was also applicable to ECL of a CdS nanocrystal film on a glass carbon electrode, with ca. 2.74- and 148.3-fold enhanced ECL intensity correspondingly, indicating wide applications in the development of semiconductor nanocrystal-based ECL biosensors.
Co-reporter:Wei-Wei Zhao, Jing Wang, Yuan-Cheng Zhu, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2015 Volume 87(Issue 19) pp:9520
Publication Date(Web):May 29, 2015
DOI:10.1021/acs.analchem.5b00497
Co-reporter:Mei-Sheng Wu, Zhen Liu, Hai-Wei Shi, Hong-Yuan Chen, and Jing-Juan Xu
Analytical Chemistry 2015 Volume 87(Issue 1) pp:530
Publication Date(Web):December 2, 2014
DOI:10.1021/ac502989f
This paper describes a novel electrochemiluminescence (ECL) imaging platform for simultaneous detection of cancer biomarkers based on a closed bipolar electrode (BPE) array. It consists of two separated channel arrays: detection channel array and sensing channel array, which are connected by a group of parallel ITO BPEs on a glass substrate. Besides, two parallel ITO strips are fabricated at the two sides of BPE array and employed as driving electrodes. After Au films are electrochemically deposited on the cathodes of the BPE array, nanobioprobes including biorecognition elements (aptamer or antibody) and a novel electrochemical tag, which is synthesized by doping thionine in silica nanoparticles (Th@SiO2 NPs), are introduced into the cathodes by immunoreaction or DNA hybridization. The Th@SiO2 coupled nanobioprobes as both recognition probes and signal amplification indicators could mediate the ECL signals of Ru(bpy)32+/tripropylamine (TPA) on the anodes of BPE array through faradaic reaction due to the charge neutrality of BPE. Thus, multiplex detection of cancer biomarkers (adenosine triphosphate (ATP), prostate-specific antigen (PSA), α-fetoprotein (AFP) and thrombin) is realized by forming specific sensing interfaces onto the cathodic poles of BPEs in different sensing channels and reported by the ECL images of the Ru(bpy)32+/TPA system on the anodic poles of BPEs in detection channels. The results demonstrate that this visual ECL platform enables sensitive detection with excellent reproducibility, which may open a new door toward the development of simple, sensitive, cost-effective, and high throughput detection methods on biochips.
Co-reporter:Cai-Yu Lu, Jing-Juan Xu, Zong-Hua Wang, Hong-Yuan Chen
Electrochemistry Communications 2015 Volume 52() pp:49-52
Publication Date(Web):March 2015
DOI:10.1016/j.elecom.2015.01.015
•A novel electrochemical biosensor for cancer cell detection was developed.•The aptamer–cancer cell interaction was transduced into DNA-based assay.•The sensitivity can be dramatically enhanced by supersandwich G-quadruplex DNAzyme.A novel electrochemical biosensor for cancer cell detection was developed based on aptamer-based competition and supersandwich G-quadruplex DNAzyme amplification strategy. Due to the stronger affinity between the aptamer and cancer cells than that with its complementary oligonucleotide, the complementary oligonucleotide will be facilely replaced. As a consequence, we can detect cancer cells indirectly by detecting the releasing DNA which is proportional to the concentration of K562 cells. Through the supersandwich G-quadruplex DNAzyme amplification strategy, the sensitivity can be dramatically enhanced with detection limit down to 14 cells.
Co-reporter:De-Man Han, Lu-Yi Jiang, Wen-Yuan Tang, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2015 Volume 51() pp:72-75
Publication Date(Web):February 2015
DOI:10.1016/j.elecom.2014.12.002
•Photoelectrochemical sensor for Hg2 + was firstly fabricated by energy transfer.•Photocurrent was decreased by energy transfer between CdS QDs and Au NPs.•Interference can be neglected for the specific interaction of T–Hg2 +–T.•A simple and general protocol for PEC detection of metal ions was opened.A novel photoelectrochemical (PEC) sensor for mercury ions (Hg2 +) was fabricated based on the energy transfer (ET) between CdS quantum dots (QDs) and Au nanoparticles (NPs) with the formation of T–Hg2 +–T pairs. In the presence of Hg2 + ions, a T-rich single-strand (ss) DNA labeled with Au NPs could hybridize with another T-rich ssDNA anchored on the CdS QDs modified electrode, through T–Hg2 +–T interactions, rendering the Au NPs in close proximity with the CdS QDs and hence the photocurrent decrease due to the ET between the CdS QDs and the Au NPs. Under the optimal condition, the photocurrent decrease was proportional to the Hg2 + concentration, ranging from 3.0 × 10− 9 to 1.0 × 10− 7 M, with the detection limit of 6.0 × 10− 10 M.
Co-reporter:Jing-Juan Xu
Science Bulletin 2015 Volume 60( Issue 23) pp:2067-2068
Publication Date(Web):2015 December
DOI:10.1007/s11434-015-0943-4
Co-reporter:Pan-Pan Dai, Jin-Yi Li, Tao Yu, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2015 Volume 141() pp:97-102
Publication Date(Web):15 August 2015
DOI:10.1016/j.talanta.2015.03.021
•Double signal amplification with Au NPs and isothermal circular reaction is used.•Magnetic beads and aptamers are employed to capture and separate HL-60 cells.•Aptamer–target binding event is transformed into physically detectable signal.•The detection limit of this method could be equivalent down to 10 cells.Here we have developed a sensitive cancer cell amplified detection method which combined Au NPs enhanced electrochemiluminescence (ECL) of CdS nanocrystals (NCs) film, with isothermal circular amplification reaction of polymerase. In DNA circular amplification detection system, hairpin DNA beacon/Au NPs composite modified CdS NCs film was used as an ECL emitter. Messenger DNA is hybridized with the aptamer modified on magnetic beads (MBs) to form MB–Au bioconjugates. In the presence of HL-60 cell, the aptamer would conjugate with the glycoprotein at cell surface and messenger DNA sequence would be released. The released messenger DNA sequence was then introduced into the cycle amplification system to trigger circular polymerizations. This assay allows us to determine the released messenger DNA equivalent to 10 cells and exhibits a significant specificity for HL-60 cells.An ultrasensitive ECL cell sensor has been developed by combining Au NPs enhanced electrochemiluminescence (ECL) of CdS nanocrystals (NCs) film, with isothermal circular amplification reaction of polymerase. This sensor has the excellent selectivity, dramatic enhancement of ECL and lower detection limit for cancer cells detection.
Co-reporter:Dr. Peng Wu;Dr. Jian-Bing Pan;Xiang-Ling Li; Xieng Hou; Jing-Juan Xu; Hong-Yuan Chen
Chemistry - A European Journal 2015 Volume 21( Issue 13) pp:5129-5135
Publication Date(Web):
DOI:10.1002/chem.201405798

Abstract

Photoelectrochemical (PEC) biosensing with semiconductor quantum dots (QDs) has received great attention because it integrates the advantages of both photo-excitation and electrochemical detection. During the photon-to-electricity conversion in PEC processes, electron–hole (charge) separation competes with electron–hole recombination, and the net effect essentially determines the performance of PEC biosensors. Herein, we propose a new approach for slowing down electron–hole recombination to increase charge separation efficiency for PEC biosensor development. Through doping with Mn2+, a pair of d bands (4T1 and 6A1) is inserted between the conduction and valence bands of CdS QDs, which alters the electron–hole separation and recombination dynamics, allowing the generation of long-lived charge carriers with ms-scale lifetime that decay about 104–105-fold more slowly than in the case of undoped QDs. Photocurrent tests indicated that Mn2+ doping resulted in an approximately 80 % increase in photocurrent generation compared with undoped CdS QDs. For application, the Mn-doped CdS QDs were coated on the surface of a glassy carbon electrode and functionalized with a cell surface carbohydrate-specific ligand (3-aminophenylboronic acid). In this way, a sensitive cytosensor for K562 leukemia cells was constructed. Moreover, the sugar-specific binding property of 3-aminophenylboronic acid allowed the electrode to serve as a switch for the capture and release of cells. This has been further explored with a view to developing a reusable PEC cytosensing platform.

Co-reporter:Qiumei Feng;Hongyuan Chen;Jingjuan Xu
Science China Chemistry 2015 Volume 58( Issue 5) pp:810-818
Publication Date(Web):2015 May
DOI:10.1007/s11426-014-5295-4
A novel disposable paper-based bipolar electrode (BPE) array is fabricated for multiplexed electrochemiluminescence (ECL) detection of pathogenic DNAs. This proposed BPE array device consists of 15 units, each consisting of six sensing cells and two reporting cells patterned using hydrophobic wax. A hairpin structure DNA assembled on the cathodes of BPEs hybridizes with Pt nanoparticles (NPs) labeled probe DNA in the presence of complementary target DNA. The introduction of Pt NPs catalyzes the reduction of dissolved O2 at cathodes and induces an enhanced ECL signal from Ru(bpy)32+/tripropylamine (TPrA) at the anodes of BPEs. The dissolved O2 lost in reduction reaction could be promptly replenished due to the relatively large contact area of the paper-based cells with air, which ensures the stability of ECL signal. This obtained paper-based BPE array sensor showed excellent performances for the multiplexed analysis of the syphilis (Treponema pallidum) gene, the immunodeficiency virus gene (HIV) and hepatitis B virus gene (HBV).
Co-reporter:Wei-Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Chemical Reviews 2014 Volume 114(Issue 15) pp:7421
Publication Date(Web):June 16, 2014
DOI:10.1021/cr500100j
Co-reporter:Peng Wu, Xiandeng Hou, Jing-Juan Xu, and Hong-Yuan Chen
Chemical Reviews 2014 Volume 114(Issue 21) pp:11027
Publication Date(Web):October 9, 2014
DOI:10.1021/cr400710z
Co-reporter:Xiao-Rong Li, Xiang-Ling Li, Ming-Chen Xu, Jing-Juan Xu and Hong-Yuan Chen  
Journal of Materials Chemistry A 2014 vol. 2(Issue 6) pp:1697-1703
Publication Date(Web):31 Oct 2013
DOI:10.1039/C3TA14276K
Gold nanodendrites (AuNDs) monodispersed on graphene oxide (GO) nanosheets were successfully prepared using a clean synthesis method at room temperature and then applied for advanced oxygen reduction reaction (ORR). Herein, GO was used as the electron donors for reducing AuCl4− instead of any additional reductants and surfactants, leading to AuNDs with excellent monodispersity, uniformity and purity. The as-prepared AuNDs-loaded GO (AuNDs–GO) exhibit high electrocatalytic activity and a dominant four-electron pathway toward ORR. The AuNDs–GO also exhibit superior stability and methanol tolerance to a commercial Pt–C catalyst, making it a promising nanoelectrocatalyst in fuel cells and other electrochemical devices. This simple, straightforward, and general method is of significance for preparing high-performance metal nanocatalysts with a well-controlled morphology on appropriate supporting materials.
Co-reporter:Zong-Hua Wang, Cai-Yu Lu, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2014 vol. 50(Issue 10) pp:1178-1180
Publication Date(Web):26 Nov 2013
DOI:10.1039/C3CC48356H
A dual-functional electrochemical biosensor for adenosines and hydrogen peroxide from cancer cells was developed based on a traditional switchable electrochemical sensing format and ATP improved G-quadruplex DNAzyme as a biolabel.
Co-reporter:Meng Xiong, Nan Hao, Tao Yu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2014 vol. 50(Issue 71) pp:10303-10306
Publication Date(Web):14 Jul 2014
DOI:10.1039/C4CC04410J
An ideal nanoporous poly(N-isopropylacrylamide) membrane has been fabricated in glass microchannels by means of spatially controlled photopatterning technology for a high level of enrichment and cleanup of nucleic acids.
Co-reporter:Qiu-Mei Feng, Jian-Bin Pan, Huai-Rong Zhang, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2014 vol. 50(Issue 75) pp:10949-10951
Publication Date(Web):15 May 2014
DOI:10.1039/C4CC03102D
A disposable paper-based bipolar electrode (BPE) was reported for the first time for the sensitive electrochemiluminescence detection of a prostate specific antigen (PSA).
Co-reporter:Zheng-Yuan Ma, Jian-Bin Pan, Cai-Yu Lu, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2014 vol. 50(Issue 81) pp:12088-12090
Publication Date(Web):12 Aug 2014
DOI:10.1039/C4CC05373G
Using CdS QD-tagged mercury-specific oligonucleotides, a novel folding-based photoelectrochemical sensor has been successfully fabricated for reagentless and highly sensitive Hg2+ detection.
Co-reporter:Nan Hao, Jin-Yi Li, Meng Xiong, Xing-Hua Xia, Jing-Juan Xu, and Hong-Yuan Chen
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 15) pp:11869
Publication Date(Web):July 28, 2014
DOI:10.1021/am5039938
We present a facilely prepared graphene oxide (GO)/ poly(dimethylsiloxane) (PDMS) composite by dispersing nanosized GO in PDMS. On the basis of the combination of photothermal effects of GO and grafted thermoresponsive polymer, poly(N-isopropylacrylamide) (PNIPAAm), an optical-driving approach for remote control of localized wettability is realized. And this method has been successfully applied in the spatially controlled reversible protein adsorption in microfluidic devices.Keywords: protein adsorption, microfluidics, graphene, photothermal conversion; wettability
Co-reporter:Huai-Rong Zhang, Yin-Zhu Wang, Mei-Sheng Wu, Qiu-Mei Feng, Hai-Wei Shi, Hong-Yuan Chen and Jing-Juan Xu  
Chemical Communications 2014 vol. 50(Issue 83) pp:12575-12577
Publication Date(Web):29 Aug 2014
DOI:10.1039/C4CC06302C
A novel visual electrochemiluminescence (ECL) analysis strategy for detection of telomerase activity is reported on a microarray chip, with G-quadruplex deoxyribozyme (DNAzyme) and luminol modified Au nanoparticles (NPs) as double-catalytic amplification labels.
Co-reporter:Nan Hao, Xiang-Ling Li, Huai-Rong Zhang, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2014 vol. 50(Issue 94) pp:14828-14830
Publication Date(Web):08 Oct 2014
DOI:10.1039/C4CC06801G
A ratiometric electrochemiluminescent biosensor for the detection of microRNAs based on cyclic enzyme amplification and distance dependent resonance energy transfer was reported for the first time.
Co-reporter:Jing Liu, Cai-Yu Lu, Hong Zhou, Jing-Juan Xu, and Hong-Yuan Chen
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 22) pp:20137
Publication Date(Web):October 21, 2014
DOI:10.1021/am505726b
In this work, we report a simple and novel electrochemical multiplexed immunosensor on a flexible polydimethylsiloxane (PDMS) slice deposited with 8 × 8 nano-Au film electrodes for simultaneous detection of prostate specific antigen (PSA), prostate specific membrane antigen (PSMA), and interleukin-6 (IL-6). Primary antibodies linked with magnetic beads (Ab1-MBs) were modified on the nano-Au film electrodes via magnetic force. In the presence of corresponding antigen, horse radish peroxidase–secondary antibody-conjugated gold nanorods (HRP-Ab2-gold NRs) were brought into the surface of electrodes, generating obvious electrochemical signals of H2O2 reduction reactions. Based on this, the designed immunosensor provide good performance in sensitivity and specificity during the detection of above three biomarkers for prostate cancer. The electrochemical multiplexed immunosensor was verified for selective and accurate detection of complex samples in human serum. Data suggested that the reported multiplexed immunosensing strategy holds great promise for applications in clinical assay and diseases diagnosis.Keywords: electrochemical immunosensor; flexible electrode; microchip array; multiplexed measurement; prostate cancer
Co-reporter:Xiang-Ling Li, Nan Hao, Hong-Yuan Chen, and Jing-Juan Xu
Analytical Chemistry 2014 Volume 86(Issue 20) pp:10239
Publication Date(Web):September 17, 2014
DOI:10.1021/ac502553u
“On-demand” drug release can maximize therapeutic efficacy for specific states of malignancies and minimize drug toxicity to healthy cells. Meanwhile, there is lack of a real-time monitoring platform to accurately investigate the amount of anticancer drugs released, especially nonfluorescent ones. So it is significant to integrate both issues in one ideal drug delivery system. To achieve this, here we present a novel stimuli-responsive controlled drug delivery system toward the tumor marker survivin mRNA, using a real-time monitoring approach based on the fluorescence resonance energy transfer (FRET) strategy to quantify the process of drug release. First, 7-amino-4-methlcoumarin (AMCA) dye terminated short oligonucleotide (FlareA) will hybridize with fluorescein isothiocyanate (FITC) labeled long oligonucleotide (S1F), which contains a recognition element to a specific RNA transcript, to form a FRET pair capped on the pores of mesoporous silica nanoparticles (MSNs). Following a target-recognition reaction, the target with a longer strand displaces the FlareA strand to form a longer and more stable duplex with S1F, which leads to the removal of the capped oligonucleotide from the MSNs and triggers the release of the entrapped cargo while FRET between AMCA and FITC is broken. The relevant change in donor and acceptor fluorescence signal can be used to monitor the unlocking and release event in real-time. Further investigations have also demonstrated that this release system possesses the capacity of modulating the extent of drug release according to the cell states, giving the platform an equally broad spectrum of applications in anticancer therapy.
Co-reporter:Wei-Wei Zhao, Ru Chen, Pan-Pan Dai, Xiang-Ling Li, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2014 Volume 86(Issue 23) pp:11513
Publication Date(Web):November 18, 2014
DOI:10.1021/ac503969e
Photoelectrochemical (PEC) immunoassay has received increasing attention owing to its good analytical performance and attractive potential for future protein assay. This Letter represents a novel and general strategy for elegant PEC immunoassay of the important cardiac marker troponin T (cTnT) at neutral conditions. Specifically, we first developed an efficient CdS quantum dots (QDs)/TiO2 nanoparticles (NPs) photoelectrode, on the basis of which an exquisite β-galactosidase (β-Gal) catalytic system was integrated with sandwich immunobinding for probing cTnT. In pH 7.4, β-Gal could catalyze the conversion of p-aminophenyl galactopyranoside (PAPG) to p-aminophenol (PAP), which could be easily photo-oxidized to p-quinone imine (PQI). Because the resulting photocurrent was directly related with the target concentration, an innovative PEC immunoassay could be realized for cTnT detection. The neutral operating condition of this protocol would greatly contribute to its wide applicability for protein assay. This work provides the first PEC immunoassay toward cardiac marker and, more significantly, opens a different perspective for future PEC immunoassay development through a general sensing protocol.
Co-reporter:Yan-Yan Zhang, Hong Zhou, Peng Wu, Huai-Rong Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2014 Volume 86(Issue 17) pp:8657
Publication Date(Web):August 6, 2014
DOI:10.1021/ac501532y
Nanocrystals (NCs) usually suffer from weak electrogenerated chemiluminescence (ECL) emissions compared with conventional luminescent reagents like Ru(bpy)32+. In this work, we proposed a simple in situ activation approach by dipping CdS NCs film on glass carbon electrode (CdS NCs/GCE) in an activation solution containing H2O2 and citric acid, resulting in a ∼58-fold enhancement of ECL intensity in the presence of coreactant H2O2. During activation, CdS NCs were oxidized by H2O2 to smaller ones which resulted in more surface S vacancies; meanwhile, citric acid played an important role in stabilizing NCs. The ECL enhancing mechanism was investigated in detail, and the coordination of H2O2 to surface excess Cd2+ ions (S vacancies) on the CdS NCs surface formed in activation was the main factor which could stabilize the electrogenerated radicals, resulting in an enhanced ECL. ECL from the activated CdS NCs/GCE could be quenched in Na2S solution due to the bonding of S(II) to excess Cd2+ ions on the surface of CdS NCs. On the basis of this, we then used the activated CdS NCs/GCE as an ECL probe for the detection of Na2S which showed good performance including a wide linear range of 5 nM to 20 μM and good anti-interference ability. Moreover, this ECL probe was successfully applied for hydrogen sulfide (H2S) detection in a biological system.
Co-reporter:Mei-Sheng Wu, Li-Jing He, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2014 Volume 86(Issue 9) pp:4559
Publication Date(Web):April 7, 2014
DOI:10.1021/ac500591n
This work describes a new electrochemiluminescence resonance energy transfer (ECL-RET) system with graphene oxide(GO)–Au/RuSi@Ru(bpy)32+/chitosan (CS) composites as the ECL donor and Au@Ag2S nanoparticles (NPs) as ECL the acceptor for the first time. The ECL signal observed by the application of GO–Au/RuSi@Ru(bpy)32+/CS composites was enhanced for 5-fold compared to that of RuSi@Ru(bpy)32+/CS in the presence of coreactant tripropylamine (TPA) due to the increased surface area and improved electrical conductivity by using graphene oxide–gold nanoparticles (GO–Au) composite materials. In addition, we synthesized Au@Ag2S core–shell NPs, whose UV–vis absorption spectrum shows good spectral overlap with the ECL spectrum of GO–Au/RuSi@Ru(bpy)32+/CS composites by adjusting the amount of Na2S and AgNO3 in the process of synthesis. The distance between energy donor and acceptor was studied to get the highly effective ECL-RET. Then, this ECL-RET system was developed for sensitive and specific detection of target DNA, and the ECL quenching efficiency (ΔI/I0, ΔI = I0 – I) was found to be logarithmically related to the concentration of the target DNA in the range from 10 aM to 10 pM.
Co-reporter:Huai-Rong Zhang, Mei-Sheng Wu, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2014 Volume 86(Issue 8) pp:3834
Publication Date(Web):March 19, 2014
DOI:10.1021/ac403960g
Here, we report a novel type of signal-on dual-potential electrochemiluminescence (ECL) approach for telomerase detection based on bifunctionalized luminol–gold nanoparticles (L–Au NPs). In this approach, CdS nanocrystals (NCs) were first coated on glassy carbon electrode, and then thiol-modified telomerase primer was attached on CdS NCs via Cd–S bond. In the presence of telomerase and dNTPs, the primer could be extended. Telomerase primer would hybridize with its complementary DNA, and the extended part would hybridize with the capture DNA which was tagged with L–Au NPs. In the presence of coreactant H2O2, the L–Au NPs could not only enhance the ECL intensity of CdS NCs at −1.25 V (vs SCE) induced by the surface plasmon resonance (SPR) of Au NPs but also produce a new ECL signal at +0.45 V (vs SCE) that resulted from luminol in L–Au NPs. Both signals at two potentials increased with the increase of telomerase concentration. This method could be used to detect the telomerase from 100 to 9000 HL-60 cells and investigate the apoptosis of tumor cells. The ratio of the two signal increments (ΔECLLuminol/ΔECLCdS NCs), which showed a high consistency value for different numbers of cells, could be used to verify the reliability of tests. This dual-potential ECL strategy showed great promise in avoiding false positive or negative results in bioanalysis.
Co-reporter:Jia-Dong Zhang, Meng Xiong, Nan Hao, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2014 Volume 47() pp:54-57
Publication Date(Web):October 2014
DOI:10.1016/j.elecom.2014.06.014
•A microarray with 8 × 5 pairs of ITO and 8 Pt-Ag/AgCl coaxial electrodes was built.•Each cell with 2 ITO discs could be constructed by patterning PDMS upon ITO glass.•Pt-Ag/AgCl coaxial electrode with compact structure was removeable and durable.•Detecting units on the chip were mutually independent and owned well uniformity.•Two tumor markers were detected simultaneously with high-throughput manner.Here a novel electrochemical microarray platform towards high-throughput detection is presented. This microarray owns 8 × 5 well-organized oval cells and 8 × 5 pairs of ITO discs (two ITO discs for each pair in one cell). 8 mobile and aligned Pt–Ag/AgCl coaxial electrodes with compact configuration, where Pt column is used for counter electrode and Ag/AgCl for reference electrode, are inserted in 8 cells separately and made up 8 groups of three-electrode detection system together with 8 pairs of ITO discs. To demonstrate the applicability of such design, two kinds of bioconjugates, carboxyl graphene nanosheets–methylene blue (CGS–MB) and carboxyl graphene nanosheets–Prussian blue (CGS–PB) nanocomposites selected as model redox indicators and crosslinked with two kinds of antibodies were coated on the pair of ITO discs to realize a high-throughput detection of two tumor markers based on the increasing spatial blocking and impedance from the formed immunocomplex.
Co-reporter:Jia-Dong Zhang, Tao Yu, Jin-Yi Li, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2014 Volume 49() pp:75-78
Publication Date(Web):December 2014
DOI:10.1016/j.elecom.2014.08.013
•An ITO bipolar array was designed.•AgNP-rGO composites were simultaneously coated on all cathodes of a bipolar array by one-step electrodeposition.•AgNP-rGO composites exhibited notable electrocatalytic activity to H2O2.•This bipolar array realized high-throughput visual detection of H2O2 by ECL imaging.An ITO bipolar array for electrochemiluminescence (ECL) imaging of H2O2 was reported. Silver nanoparticle-reduced graphene oxide (AgNP-rGO) composites were simultaneously coated on the cathodes of a bipolar array via a one-step electrodeposition approach. Compared to naked ITO, the above composites exhibited notable electrocatalytic activity to H2O2. The concentration of H2O2 could be indicated by the ECL image of Ru(bpy)32 +/2-(dibutylamino) ethanol (DBAE) at anodes based on charge balance. This chip system, not only provides a fast manner to prepare nanocomposites on bipolar electrodes (BPEs), but also can realize high-throughput visual detection.
Co-reporter:Qiu-Mei Feng, Zhen Liu, Hong-Yuan Chen, Jing-Juan Xu
Electrochemistry Communications 2014 Volume 49() pp:88-92
Publication Date(Web):December 2014
DOI:10.1016/j.elecom.2014.10.015
•Paper-based electrochemiluminescence biosensor was designed for the detection of cancer cells.•The ECL intensity of RuSi@Ru(bpy)32 + NPs loaded on the aptamer directly reflects the amount of HL-60 cancer cells.•This assay offered great potential for simple, cost-effective, portable and sensitive analysis of cancer cells.Here a novel paper-based electrochemiluminescence (ECL) device was developed for the detection of HL-60 cancer cells. In this approach, porous filter paper as a thin-layer electrochemical cell connected to a sheet of ITO working electrode. Au nanoparticles (Au NPs) and graphene were coated on the surface of ITO to immobilize capture HS-DNA. Then, the aptamer of HL-60 cancer cells, which is labeled with Ru(bpy)32 +-conjugated silica nanoparticles (RuSi@Ru(bpy)32 +) is hybridized with the capture DNA to form bioconjugates. In the presence of HL-60 cells, the aptamer would conjugate with glycoprotein at cell surface and RuSi@Ru(bpy)32 + NP-aptamer would be released. After the dissociation of RuSi@Ru(bpy)32 + NP-aptamer from the surface of ITO, ECL signal would decline. This simple, portable and disposable testing platform could detect HL-60 cancer cells down to 56 cells/mL.
Co-reporter:Wei-Wei Zhao, Meng Xiong, Xiao-Rong Li, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2014 Volume 38() pp:40-43
Publication Date(Web):January 2014
DOI:10.1016/j.elecom.2013.10.035
•Photoelectrochemical (PEC) bioanalysis•Mini review•Introductory concepts and main principles are provided.•The basic signaling mechanisms are highlighted using recent illustrative examples.Photoelectrochemical (PEC) bioanalysis has attracted considerable research interest due to its desirable properties, and its rapid evolution has resulted in great progress in bioanalytical applications. This mini review aims to provide a snapshot of the introductory concepts and main principles of PEC bioanalysis, as well as the basic classification of the established signaling strategies with recent illustrative examples.
Co-reporter:Jin-Yi Li, Zeng-Qiang Wu, Jing-Juan Xu, Cheng-Yong Li, Hong-Yuan Chen and Xing-Hua Xia  
RSC Advances 2014 vol. 4(Issue 85) pp:45074-45081
Publication Date(Web):28 Aug 2014
DOI:10.1039/C4RA08834D
Porous anodic alumina (PAA) film is composed of highly ordered and controllable structures, and their extensive application requires the understanding of their growing mechanism. Herein, we present a localized oxidation model to unravel the phenomena of PAA growth, showing that random processes converge into an ordered formation due to the unique characteristics of ion transport confinement in alumina. The anodizing voltage shows a quadratic relationship with barrier layer depth. In addition, we predict the furcate conditions of PAA and the voltage threshold to produce a PAA by our model.
Co-reporter:Li Deng, Ying Du, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2014 59() pp: 58-63
Publication Date(Web):
DOI:10.1016/j.bios.2014.03.012
Co-reporter:Hai-Wei Shi, Mei-Sheng Wu, Ying Du, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2014 Volume 55() pp:459-463
Publication Date(Web):15 May 2014
DOI:10.1016/j.bios.2013.12.045
•An ECL approach on a wireless ITO bipolar electrode for adenosine detection in cancer cells was provided.•Ferrocene as DNA tag was introduced on cathodic pole to enhance the ECL of Ru(bpy)32+/TPA system on anodic pole•The ECL on the anodic pole could be decreased by the adenosine-induced removal of ferrocene-aptamer on the cathodic pole.•The approach could detect adenosine in a wide range from 1.0 fM to 0.10 μM.Here we report a novel approach for the detection of adenosine in cancer cells by electrochemiluminescence (ECL) on a wireless indium tin oxide bipolar electrode (BPE). In this approach, ferrocene (Fc) which is labeled on adenosine aptamer is enriched on one pole of the BPE by hybridization with its complementary DNA (ssDNA) and oxidized to Fc+ under an external voltage of 5.0 V at the two ends of BPE. Then, a reversed external voltage was added on the BPE, making Fc+ enriched pole as cathode. The presence of Fc+ promotes the oxidation reaction on the anodic pole of the BPE, resulting in a significant increase of ECL intensity using Ru(bpy)32+/tripropylamine (TPA) system as test solution. The presence of target adenosine was reflected by the ECL signal decrease on the anodic pole caused by the target-induced removal of ferrocene-aptamer on the cathodic pole. The decrease of ECL signal was logarithmically linear with the concentration of ATP in a wide range from 1.0 fM to 0.10 μM. This ECL biosensing system could accurately detect the level of adenosine released from cancer cells.
Co-reporter:Mei-Sheng Wu, Da-Jing Yuan, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Science 2013 vol. 4(Issue 3) pp:1182-1188
Publication Date(Web):21 Dec 2012
DOI:10.1039/C2SC22055E
Rapid and sensitive detection of tumor biomarkers plays a critical role in the early diagnosis of cancer and better understanding of disease progression. We report here a novel wireless electrochemiluminescence (ECL) strategy for visualizing prostate-specific antigen (PSA) on the basis of electrical switch control of ECL generation on bipolar electrodes (BPEs). The visual device comprises a two-channel microfluidic chip with two indium tin oxide (ITO) bands with a gap of 200 μm. The gap between the two ITO bands in one channel could be regarded as an electrical switch, the conductivity of which controls ECL generation on the ITO bands in the other channel, which are used as bipolar electrodes (BPEs). The electronic conductivity of the electrical switch could be tuned by PSA guided silver particles deposition via an immunosandwich assembly and a silver enhancement strategy. At the “on” state of the electrical switch, PSA induced deposition of silver particles forms an electronic circuit between the adjacent BPEs and makes them behave like a continuous H-shaped BPE, which results in only one ECL signal. Meanwhile, the external voltage for driving the oxidation reactions of Ru(bpy)32+ and TPA is significantly reduced compared with the “off” state. This important characterization of the electrical switch could eliminate the background signal and enable a sensitive measurement of PSA by observing the ECL lightspots on BPEs, providing a simple and sensitive visual means of detecting cancer biomarkers. Besides, this two-channel design avoids the chemical interference between sensing and reporting reactions. Combining the advantages of BPE and the high visual sensitivity of the electrical switch, it could be easily expected to achieve sensitive screening of other biomarkers.
Co-reporter:Hong Zhou, Yan-Yan Zhang, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2013 vol. 49(Issue 22) pp:2246-2248
Publication Date(Web):01 Feb 2013
DOI:10.1039/C3CC38990A
Based on the K-doped graphene–CdS:Eu NC composites and the nicking endonuclease (NEase) assisted strand-scission cycle, we have developed an ultrasensitive and selective electrochemiluminescence (ECL) DNA biosensor using the G-quadruplex–hemin-based DNAzyme which acts as an electrocatalyst for the reduction of H2O2, the coreactant of CdS:Eu NCs ECL.
Co-reporter:Fen-Ying Kong, Bi-Yi Xu, Ying Du, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2013 vol. 49(Issue 11) pp:1052-1054
Publication Date(Web):12 Nov 2012
DOI:10.1039/C2CC37675J
A branched electrode platform was proposed for label-free and reagentless simultaneous tumor markers detection based on different redox substrates.
Co-reporter:Li-Jing He, Mei-Sheng Wu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2013 vol. 49(Issue 15) pp:1539-1541
Publication Date(Web):04 Jan 2013
DOI:10.1039/C2CC38508B
A reusable potassium ion biosensor was reported for the first time based on the reversible DNA structural change and the interaction between surface plasmons of Au nanoparticles (NPs) and the ECL emission of CdS nanocrystals (NCs).
Co-reporter:Jing Liu, Cai-Yu Lu, Hong Zhou, Jing-Juan Xu, Zong-Hua Wang and Hong-Yuan Chen  
Chemical Communications 2013 vol. 49(Issue 59) pp:6602-6604
Publication Date(Web):03 Jun 2013
DOI:10.1039/C3CC43532F
A new dual-functional electrochemical biosensor for the detection of prostate specific antigen (PSA) and telomerase activity was successfully developed based on a sandwich immunobinding format and telomerization assisted hemin–G-quadruplex-based DNAzyme as a biolabel.
Co-reporter:Wei-Wei Zhao, Shu Shan, Zheng-Yuan Ma, Lin-Na Wan, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2013 Volume 85(Issue 24) pp:11686
Publication Date(Web):December 2, 2013
DOI:10.1021/ac403691a
To date, almost all the established photoelectrochemical (PEC) enzymatic biosensors require the surface-confinement procedure to immobilize enzyme as biorecogniton element for probing various analytes of interest. This Letter develops a novel example without such necessity. Specifically, we first prepared a BiOI nanoflakes (NFs)/TiO2 nanoparticles (NPs) p–n heterojunction as the photoelectrode, on the basis of which acetylcholine esterase (AChE) antibody was introduced via the bridging of protein A. In such a system, enzyme could keep its optimal state in the solution if in the absence of inhibitor; otherwise, the degree of enzyme inhibition would correlate closely with the concentration of inhibitor. After immunoreaction between AChE and its antibody, the inhibitor concentration could then be determined by the biocatalytic reaction-controlled PEC response. Integrated with other enzyme-based biosystems, this simple configuration could serve as a general method for assaying enzyme inhibition or activities.
Co-reporter:Mei-Sheng Wu, Da-Jing Yuan, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2013 Volume 85(Issue 24) pp:11960
Publication Date(Web):November 12, 2013
DOI:10.1021/ac402889z
Here we developed a novel hybrid bipolar electrode (BPE)–electrochemiluminescence (ECL) biosensor based on hybrid bipolar electrode (BPE) for the measurement of cancer cell surface protein using ferrocence (Fc) labeled aptamer as signal recognition and amplification probe. According to the electric neutrality of BPE, the cathode of U-shaped ITO BPE was electrochemically deposited by Au nanoparticles (NPs) to enhance its conductivity and surface area, decrease the overpotential of O2 reduction, which would correspondingly increase the oxidation current of Ru(bpy)32+/tripropylamine (TPA) on the anode of BPE and resulting a ∼4-fold enhancement of ECL intensity. Then a signal amplification strategy was designed by introducing Fc modified aptamer on the anode surface of BPE through hybridization for detecting the amount of mucin-1 on MCF-7 cells. The presence of Fc could not only inhibit the oxidation of Ru(bpy)32+ because of its lower oxidation potential, its oxidation product Fc+ could also quench the ECL of Ru(bpy)32+/TPA by efficient energy-transfer from the excited-state Ru(bpy)32+* to Fc+, making the ECL intensity greatly quenched. On the basis of the cathodic Au NPs induced ECL enhancing coupled with anodic Fc induced signal quenching amplification, the approach allowed detection of mucin-1 aptamer at a concentration down to 0.5 fM and was capable of detecting a minimum of 20 MCF-7 cells. Besides, the amount of mucin-1 on MCF-7 cells was calculated to be 9041 ± 388 molecules/cell. This approach therefore shows great promise in bioanalysis.
Co-reporter:Wei-Wei Zhao, Zheng-Yuan Ma, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2013 Volume 85(Issue 18) pp:8503
Publication Date(Web):August 29, 2013
DOI:10.1021/ac402523p
Usually, the photoelectrochemical (PEC) bioanalysis necessitates ready photoactive materials as signal sources to convert the specific biological events into electrical signals. Herein, the first PEC bioanalysis without the necessity of ready visible-light-active species was demonstrated. We use an enzyme catalytic process to couple with the unique surface chemistry of semiconductive nanocrystalline, whereby its electronic properties could be modified spontaneously during the enzymatic reaction. Specifically, the enzymatic hydrolysis of ascorbic acid 2-phosphate by alkaline phosphatase is allowed to interact on the TiO2 nanoparticles (NPs) matrix. PEC tests reveal that the self-coordination of the biocatalyzed enediol-ligands onto the undercoordinated surface defect sites would in situ form a ligand-to-metal charge transfer (CT) complex, endowing the inert semiconductor with strong absorption bands in the visible region, and hence underlying a novel and general PEC bioanalysis strategy.
Co-reporter:Huai-Rong Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2013 Volume 85(Issue 11) pp:5321
Publication Date(Web):May 22, 2013
DOI:10.1021/ac400992u
Inspired by dual-wavelength fluorescence ratiometric method which could reduce the influence from the environmental change, here, we present a novel dual-potential electrochemiluminescence (ECL) ratiometric sensing approach. CdS nanocrystal (NC) and luminol as two different ECL emitters are employed. ECL from CdS NCs coated on glassy carbon electrode at −1.25 V (vs SCE) could be quenched by closely contacted Pt nanoparticles (NPs) via a biological binding event, while ECL from luminol at +0.45 V (vs SCE) could be enhanced by the same Pt NPs, in the presence of their common coreactant of H2O2. Thus, the quenching of ECL from CdS NCs and the enhancement of ECL from luminol could indicate the same biological binding event. With the mp53 oncogene as a model DNA molecule, a molecular beacon (MB) containing a 20-base loop, which is complementary with the mp53 oncogene, is immobilized on CdS NCs/GCE first; Pt NPs are then captured on CdS NCs surface by DNA hybridization between the MB and mp53 oncogene labeled on Pt NPs. By measuring the ratio of ECL intensities at two excitation potentials, this approach could sensitively detect the concentration of target DNA in a wide range from 5.0 fM to 1.0 pM. The sensing scheme is general and can be utilized for many other biological binding events.
Co-reporter:Nan Hao, Meng Xiong, Jia-dong Zhang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2013 Volume 85(Issue 24) pp:11715
Publication Date(Web):November 12, 2013
DOI:10.1021/ac403215g
This paper describes a portable thermo-powered high-throughput visual electrochemiluminescence (ECL) sensor for the first time. This sensor is composed of a tiny power supply device based on thermal-electrical conversion and a facile prepared array electrode. The ECL detection could be conducted with thermo-power, which is easily accessible. For example, hot water, a bonfire, or a lighted candle enables the detection to be conducted. And the assay can be directly monitored by the naked eye semiquantitatively or smart phones quantitatively. Combined with transparent electrode and array microreactors, a portable high-throughput sensor was achieved. The portable device, avoiding the use of an electrochemical workstation to generate potential and a photomultiplier tube to receive the signal, is not only a valuable addition for traditional methods but also a suitable device for field operation or point-of-care testing.
Co-reporter:Xiang-Ling Li, Shu Shan, Meng Xiong, Xing-Hua Xia, Jing-juan Xu and Hong-Yuan Chen  
Lab on a Chip 2013 vol. 13(Issue 19) pp:3868-3875
Publication Date(Web):16 Jul 2013
DOI:10.1039/C3LC50587A
The rapid recognition of cancer cells and detection of tumor biomarker survivin mRNA plays a critical role in the early diagnosis of many cancers. Based on the integration of specific cancer cell capture and intracellular survivin mRNA detection, this work presents a novel and sensitive on-chip approach for the bioanalysis of survivin mRNA in a single living cell. The microchannel surface was firstly modified with a prostate stem cell antigen (PSCA) monoclonal antibody as the recognition element for prostate cancer cells (PC-3). As a result of the antigen-antibody specific affinity interactions, PC-3 cells could be selectively captured on the microchannel surface. After cell capture, nano-sized graphene oxide-poly(ethylene glycol) bis(amine) (NGO-PEG) was employed as a quencher and carrier of a signal tag, fluorescein isothiocyanate (FITC)-labeled antisense oligonucleotide (F-S1), which is complementary to part of survivin mRNA (target survivin mRNA), to transfect into the captured PC-3 cells. Upon the selective binding of S1 to intracellular survivin mRNA, F-S1 will be released from the NGO-PEG, inducing the fluorescence recovery of FITC. This antibody-based microfluidic device enables simple and inexpensive monitoring of the amount of survivin mRNA in single captured cell without the need for sample pretreatment. The survivin mRNA content in each PC-3 cell was estimated to be (4.8 ± 1.8) × 106 copies. This strategy opens a different perspective for ultrasensitive survivin mRNA detection, which may facilitate the early screening for malignancy.
Co-reporter:Bi-Yi Xu, Shan-Wen Hu, Guang-Sheng Qian, Jing-Juan Xu and Hong-Yuan Chen  
Lab on a Chip 2013 vol. 13(Issue 18) pp:3714-3720
Publication Date(Web):24 Jun 2013
DOI:10.1039/C3LC50676B
In this work a novel microfluidic platform for cell culture and assay is developed. On the chip a static cell culture region is coupled with dynamic fluidic nutrition supply structures. The cell culture unit has a sandwich structure with liquid channels on the top, the cell culture reservoir in the middle and gas channels on the bottom. Samples can be easily loaded into the reservoir and exchange constantly with the external liquid environment by diffusion. Since the flow direction is perpendicular to the liquid channel on the top of the reservoir, the cells in the reservoir are shielded from shear-force. By assembling the basic units into an array, a steady concentration gradient can be generated. Cell culture models both for continuous perfusion and one-off perfusion were established on the chip. Both adherent and suspended cells were successfully cultured on the chip in 2D and 3D culture modes. After culturing, the trapped cells were recovered for use in a later assay. As a competitive candidate for a standard cell culture and assay platform, this chip is also adaptable for cytotoxicity and cell growth assays.
Co-reporter:Jing Liu, Hong Zhou, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2013 Volume 32() pp:27-30
Publication Date(Web):July 2013
DOI:10.1016/j.elecom.2013.03.034
•Employing PSA and survivin mRNA as dual-biomarkers in prostate cancer detection.•Nano-structured gold electrode and direct electrochemical output.•Logic gate of “AND” mode greatly reduced the possibility of false-positive assay.As single biomarker often has inadequate predictive value in clinical examination, we designed a dual-biomarker “AND” logic device that defines the concentration of prostate-specific antigen (PSA) and survivin mRNA as inputs and the increase in faradaic current from intercalation agent Co(phen)33 + as output for prostate cancer (CaP) diagnosis on Au nano-film covered gold electrode surfaces. Primary capture antibody (Ab1) was first immobilized on AuNP electrode, then while both PSA and survivin mRNA exist, current of Co(phen)33 + observably increased due to the formation of dsDNA structure between survivin antisensoligonucleotide connected secondary detection antibody (Ab2) and survivin mRNA. And when one of the two biomarkers was absent, no obvious current increment was found. Thus the designed “AND” logic gate greatly reduced the possibility of false-positive assay from non-cancerous prostate diseases such as prostatic hyperplasia and prostatitis in diagnosis of CaPs.
Co-reporter:Fen-Ying Kong, Bi-Yi Xu, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2013 Volume 39(Issue 1) pp:177-182
Publication Date(Web):15 January 2013
DOI:10.1016/j.bios.2012.07.023
An electrochemical method for the simultaneous detection of two different tumor markers, carcinoembryonic antigen (CEA) and α-fetoprotein (AFP), in one-pot, using CdS/DNA and PbS/DNA nanochains as labels was developed. Herein, magnetic beads (MBs) as bimolecule immobilizing carriers, were used for co-immobilization of primary anti-CEA and anti-AFP antibodies. The distinguishable signal labels were synthesized by in situ growth of CdS and PbS nanoparticles on DNA chains, respectively, which were further employed to label the corresponding secondary antibodies. A sandwich-type immunoassay format was formed by the biorecognition of the antigens and corresponding antibodies. The assay was based on the peak currents of Cd2+ and Pb2+ dissolved from CdS and PbS nanoparticles by HNO3 using square wave stripping voltammetry. Experimental results show that the multiplexed electrochemical immunoassay has enabled the simultaneous monitoring of CEA and AFP in a single run with wide working ranges of 0.1– 100 ng mL−1 for CEA and 0.5–200 ng mL−1 for AFP. The detection limits reach to 3.3 pg mL−1 for CEA and 7.8 pg mL−1 for AFP.Highlight► CdS and PbS QDs/DNA nanochains were prepared by in situ growth method. ► QDs/DNA nanochains were used to label secondary CEA and AFP antibody to amplify the signal. ► The linear shape of DNA can help to reduce the steric hindrance compared to the sphere carriers. ► The protocol enabled the simultaneous monitoring of CEA and AFP in a single run. ► The approach showed wide working ranges and lower detection limits.
Co-reporter:Jing Wang, Wei-Wei Zhao, Hong Zhou, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2013 Volume 41() pp:615-620
Publication Date(Web):15 March 2013
DOI:10.1016/j.bios.2012.09.041
In this work, we firstly enunciated the presence of synergy effect between the electron and energy transfer in an electrochemiluminescence (ECL) system involving the CdS NCs and Au NPs, based on which an amplified ECL biosensor was constructed for sensitive detection of DNA–protein interactions. Specifically, Au NPs modified on electrode, following by assembled probe DNA. Then the modified GCE was hybridized with SiO2@CdS/DNA conjugates. With DNA duplex as a rigid spacer, Au NPs could not only accelerate the electron transfer but also produce the surface plasma resonance upon excited ECL of CdS NCs. However, the enhanced ECL could be greatly suppressed by the binding of target protein. The prepared biosensor possesses excellent analytical performance with the linear range of target protein from 0.015 to 150 nM.Highlights► The presence of both electron transfer and energy transfer between CdS NCs and Au NPs was firstly enunciated. ► SiO2@CdS nanocomposites were used as DNA tags for DNA-binding protein biosensing. ► Based on the synergy effect between electron and energy transfer, ECL signal from CdS NCs was amplified. ► The work exploited advanced ECL bioassay for DNA-binding protein.
Co-reporter:Xiao-Rong Li;Fen-Ying Kong;Jing Liu;Tong-Ming Liang;Hong-Yuan Chen
Advanced Functional Materials 2012 Volume 22( Issue 9) pp:1981-1988
Publication Date(Web):
DOI:10.1002/adfm.201103025

Abstract

Chemical modification with foreign atoms is a leading strategy to intrinsically modify the properties of host materials. Among them, potassium (K) modification plays a critical role in adjusting the electronic properties of carbon materials. Graphene, a true 2D carbon material, has shown fascinating applications in electrochemical sensing and biosensing. In this work, a facile and mild strategy to K-modifying in graphene at room-temperature is reported for the first time. X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), transmission electron microscopy (TEM), Raman spectra, and cyclic voltammetry are used to characterize this K-modified graphene. The K-modified graphene is capable of acting as an electron transfer medium and more efficiently promotes charge transfer than unmodified graphene. A highly sensitive and stable amperometric sensor based on its excellent electrocatalytic activity toward the oxidation of NO2 is proposed. The sensor shows a linear range from 0.5 μM to 7.8 mM with a detection limit of 0.2 μM at a signal-to-noise ratio of 3. The modified electrode has excellent analytical performance and can be successfully applied in the determination of NO2 released from liver cancer and leukemia cells and shows good application potential in biological systems.

Co-reporter:Li Deng, Yun Shan, Jing-Juan Xu and Hong-Yuan Chen  
Nanoscale 2012 vol. 4(Issue 3) pp:831-836
Publication Date(Web):20 Dec 2011
DOI:10.1039/C1NR11470K
Eu3+ doped CdS nanocrystals (CdS:Eu NCs) were synthesized via a co-precipitation method. The doping of Eu3+ ions caused a 4-fold enhancement in electrochemiluminescence (ECL) intensity and more stable cathodic signals compared to pure CdS NCs. Such enhancement was mostly ascribed to doping-induced improvement in the stability of reduced NCs. A new emission peak around 620 nm was observed in ECL spectra of the doped NCs, which belongeded to the 5D0 → 7F2 transition of Eu3+ ions in CdS NCs. Correspondingly, a pair of oxidation and reduction peaks occurred at +1.01 V and +0.61 V because of the formation of Eu3+-surface states complex when the CdS:Eu NCs solution underwent cyclic voltammogram scanning. Benefiting from the strong ECL emission of the doped NCs and high affinity of the doped Eu3+ ions to oxygen, the CdS:Eu NCs film showed a great oxygen-sensitivity. The intense red luminescence of the characteristic transitions of Eu3+ in CdS:Eu NCs would also have enormous potential in bioanlytical systems.
Co-reporter:Wei-Wei Zhao, Chun-Yuan Tian, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 6) pp:895-897
Publication Date(Web):18 Nov 2011
DOI:10.1039/C1CC16775H
Visible light-activated localized surface plasmon resonance-based photoelectrochemical detection is reported for the first time.
Co-reporter:Bi-Yi Xu, Zhe-Qin Yang, Jing-Juan Xu, Xing-Hua Xia and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 95) pp:11635-11637
Publication Date(Web):13 Sep 2012
DOI:10.1039/C2CC35986C
Continuous CaCO3 hollow nanoparticle generation at room temperature with simultaneous molecule doping is realized on a liquid–gas dual phase microfluidic system.
Co-reporter:Wei-Wei Zhao, Long Zhang, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 76) pp:9456-9458
Publication Date(Web):11 Jul 2012
DOI:10.1039/C2CC34543A
A robust and specific photoelectrochemical approach for cell surface carbohydrates evaluation was achieved firstly based on carboxylic-group-containing free-base-porphyrin bridged 3-aminophenylboronic acid and a titania biosensing interface.
Co-reporter:Chun-Yuan Tian, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 66) pp:8234-8236
Publication Date(Web):27 Jun 2012
DOI:10.1039/C2CC34229D
The highly enhanced electrochemiluminescence from a nitrogen doped TiO2 nanotube array has been reported for the first time, and successfully applied to develop an ultrasensitive ECL aptasensor for the detection of adenosine in cancer cells.
Co-reporter:Jing Wang, Wei-Wei Zhao, Xiao-Rong Li, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 51) pp:6429-6431
Publication Date(Web):10 May 2012
DOI:10.1039/C2CC32767H
Based on the amplified signal from SiO2@CdS nanocomposites integrated with K-doped graphene, a new electrochemiluminescence biosensor was developed for the successful detection of transcription factor TATA-binding protein (TBP).
Co-reporter:Wei-Wei Zhao, Xiao-Ya Dong, Jing Wang, Fen-Ying Kong, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2012 vol. 48(Issue 43) pp:5253-5255
Publication Date(Web):23 Jan 2012
DOI:10.1039/C2CC17942C
A new photoelectrochemical immunoassay for prostate-specific antigen (PSA) was successfully developed with high sensitivity via immunogold labeling.
Co-reporter:Wei-Wei Zhao, Zheng-Yuan Ma, Pei-Pei Yu, Xiao-Ya Dong, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 2) pp:917
Publication Date(Web):December 12, 2011
DOI:10.1021/ac203184g
Herein we demonstrate the protocol of a biocatalytic precipitation (BCP)-based sandwich photoelectrochemical (PEC) horseradish peroxidase (HRP)-linked immunoassay on the basis of their synergy effect for the ultrasensitive detection of mouse IgG (antigen, Ag) as a model protein. The hybrid film consisting of oppositely charged polyelectrolytes and CdS quantum dots (QDs) is developed by the classic layer by layer (LbL) method and then employed as the photoactive antibody (Ab) immobilization matrix for the subsequent sandwich-type Ab-Ag affinity interactions. Improved sensitivity is achieved through using the bioconjugates of HRP-secondary antibodies (Ab2). In addition to the much enhanced steric hindrance compared with the original one, the presence of HRP would further stimulate the BCP onto the electrode surface for signal amplification, concomitant to a competitive nonproductive absorption that lowers the photocurrent intensity. As a result of the multisignal amplification in this HRP catalyzed BCP-based PEC immunoassay, it possesses excellent analytical performance. The antigen could be detected from 0.5 pg/mL to 5.0 ng/mL with a detection limit of 0.5 pg/mL.
Co-reporter:Zeng-Qiang Wu, Wen-Zhi Jia, Kang Wang, Jing-Juan Xu, Hong-Yuan Chen, and Xing-Hua Xia
Analytical Chemistry 2012 Volume 84(Issue 24) pp:10586
Publication Date(Web):November 26, 2012
DOI:10.1021/ac3030224
In biological metabolism, a given metabolic process usually occurs via a group of enzymes working together in sequential pathways. To explore the metabolism mechanism requires the understanding of the multienzyme coupled catalysis systems. In this paper, an approach has been proposed to study the kinetics of a two-enzyme coupled reaction using SECM combining numerical simulations. Acetylcholine esterase and choline oxidase are immobilized on cysteamine self-assembled monolayers on tip and substrate gold electrodes of SECM via electrostatic interactions, respectively. The reaction kinetics of this two-enzyme coupled system upon various separation distance precisely regulated by SECM are measured. An overall apparent Michaelis–Menten constant of this enzyme cascade is thus measured as 2.97 mM at an optimal tip–substrate gap distance of 18 μm. Then, a kinetic model of this enzyme cascade is established for evaluating the kinetic parameters of individual enzyme by using the finite element method. The simulated results demonstrate the choline oxidase catalytic reaction is the rate determining step of this enzyme cascade. The Michaelis–Menten constant of acetylcholine esterase is evaluated as 1.8 mM. This study offers a promising approach to exploring mechanism of other two-enzyme coupled reactions in biological system and would promote the development of biosensors and enzyme-based logic systems.
Co-reporter:Mei-Sheng Wu, Hai-Wei Shi, Li-Jing He, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 9) pp:4207
Publication Date(Web):April 10, 2012
DOI:10.1021/ac300551e
This paper describes a novel on-chip microarray platform based on an electrochemiluminescence resonance energy transfer (ECL-RET) strategy for rapid assay of cancer cell surface biomarkers. This platform consists of 64 antigen-decorated CdS nanorod spots with the diameter of 1.0 cm uniformly distributed on 16 indium tin oxide (ITO) strips, which is coated with a multichannel decorated polydimethylsiloxane (PDMS) slice to realize multiplexed determination of antigens. To shorten the immune reaction time in the microchannels and simplify the device, magnetic stirring and four-channel universal serial bus (USB) ports for plug-and-play were used. When Ru(bpy)32+ labeled antibodies were selectively captured by the corresponding antigens on the CdS nanorod spot array, ECL-RET from the CdS nanorod (donor) by cathodic emission in the presence of K2S2O8 to Ru(bpy)32+ (acceptor) occurred. With signal amplification of Ru(bpy)32+ and competitive immunoassay, carcinoembryonic antigen (CEA), α-fetoprotein (AFP), and prostate specific antigen (PSA) as models were detected on this microfluidic device via recording the increased ECL-RET signals on electrode surfaces. Furthermore, this multiplexed competitive immunoassay was successfully used for detecting cancer cell surface antigens via the specific antibody–cell interactions and cell counting via cell surface receptors and antigens on the CdS nanorod surface. This platform provides a rapid and simple but sensitive approach with microliter-level sample volume and holds great promise for multiplexed detection of antigens and antigen-specific cells.
Co-reporter:Xian-Bo Zhang, Zeng-Qiang Wu, Kang Wang, Jie Zhu, Jing-Juan Xu, Xing-Hua Xia, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 8) pp:3780
Publication Date(Web):March 20, 2012
DOI:10.1021/ac3003616
Continuous plasma separation will be greatly helpful for dynamic metabolite monitoring in kinetics research and drug development. In this work, we proposed a continuous on-chip plasma separation method based on the natural aggregating and sedimentation behavior of red blood cells at low shear rate. In this approach, a glass capillary was first used to realize quick and obvious delamination of blood cells from plasma. A novel “dual-elbow” connector was designed to change the direction of delamination. The blood was finally separated by laminar flow and bifurcation on the microchip. Results demonstrated that the present device can efficiently and stably separate plasma from blood in a continuous means, e.g., in a 4 h separation we did not observe clogging or a trend of clogging. In addition, the present approach can avoid the damage to cells which usually occurs in separation with high shear rate in a microchannel and possible contaminants to plasma. The proposed microchip device is robust, simple, and inexpensive for long time plasma separation with high plasma recovery and less sample consumption. The present work provides an effective tool for metabolite monitoring in pharmacokinetics research and drug development.
Co-reporter:Bi-Yi Xu, Shan-Wen Hu, Xiao-Na Yan, Xing-Hua Xia, Jing-Juan Xu and Hong-Yuan Chen  
Lab on a Chip 2012 vol. 12(Issue 7) pp:1281-1288
Publication Date(Web):15 Feb 2012
DOI:10.1039/C2LC20985C
In this study, steady liquid–gas phase separation is realized by applying a hydrophobic small microchannel array (SMA) to bridge two large microchannels, one for liquid phase and one for gas phase. In this structure, a capillary pressure difference between that in the SMA and the larger channel results in a steady liquid–gas interface. The generated liquid–gas interface allows for fast gas dissolving speed. By coupling the liquid–gas interface with a one directional fluidic field, a steady dissolved gas concentration gradient (DgCG) is generated. The DgCG distribution is easily designable for linear or exponential modes, providing improved flexibility for gas participated processes on chip. To demonstrate its applicability, a CO2 DgCG chip is fabricated and applied for screening CaCO3 crystal growth conditions in the DgCG chip. Crystals with transitional structures are successfully fabricated, which is consistent with the CO2 DgCG distribution.
Co-reporter:Bi-Yi Xu, Xiao-Na Yan, Jia-Dong Zhang, Jing-Juan Xu and Hong-Yuan Chen  
Lab on a Chip 2012 vol. 12(Issue 2) pp:381-386
Publication Date(Web):08 Nov 2011
DOI:10.1039/C1LC20741E
In this study, a simple and economical fabrication technique bridging micro- and nanostructures is proposed. Glass molds with micro-nanostructures are fabricated by glass microlithography. The microlithography provides flexibility for structure design, and the glass etching contributes to transform the micro glass ridge to the nanoscale. Glass ridge structures with triangular cross sections are generated by undercutting, which coupled the isotropic character of glass and the shield effect of the top Cr layer upon HF etching. Further etching induced the height of the glass ridges to shrink from micro- to nanometres due to the edge effects. At the late etching stage, the geometrical change of the glass greatly slows down, which gives better control over the size of the glass ridge. By glass structure mold-copy, well repeatable, mechanically stable and tunable polydimethylsiloxane (PDMS) channels and cones are fabricated. Scanning electron microscopy (SEM) and laser interferometry (LI) are carried out to characterize the micro-nanostructures. To demonstrate their workability, sample preconcentration to a single nanochannel level is carried out.
Co-reporter:Mei-Sheng Wu, Guang-sheng Qian, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 12) pp:5407
Publication Date(Web):May 21, 2012
DOI:10.1021/ac3009912
We report an ultrasensitive wireless electrochemiluminescence (ECL) protocol for the detection of a nucleic acid target in tumor cells on an indium tin oxide bipolar electrode (BPE) in a poly(dimethylsiloxane) microchannel. The approach is based on the modification of the anodic pole of the BPE with antisense DNA as the recognition element, Ru(bpy)32+-conjugated silica nanoparticles (RuSi@Ru(bpy)32+) as the signal amplification tag, and reporter DNA as a reference standard. It employs the hybridization-induced changes of RuSi@Ru(bpy)32+ ECL efficiency for the specific detection of reporter DNA released from tumor cells. Prior to ECL detection, tumor cells are transfected with CdSe@ZnS quantum dot (QD)–antisense DNA/reporter DNA conjugates. Upon the selective binding of antisense DNA probes to intracellular target mRNA, reporter DNA will be released from the QDs, which indicates the amount of the target mRNA. The proof of concept is demonstrated using a proto-oncogene c-Myc mRNA in MCF-7 cells (breast cancer cell line) as a model target. The wireless ECL biosensor exhibited excellent ECL signals which showed a good linear range over 2 × 10–16 to 1 × 10–11 M toward the reporter DNA detection and could accurately quantify c-Myc mRNA copy numbers in living cells. C-Myc mRNA in each MCF-7 cell and LO2 cell was estimated to be 2203 and 13 copies, respectively. This wireless ECL strategy provides great promise in a miniaturized device and may facilitate the achievement of point of care testing.
Co-reporter:Wei-Wei Zhao, Pei-Pei Yu, Yun Shan, Jing Wang, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 14) pp:5892
Publication Date(Web):June 22, 2012
DOI:10.1021/ac300127s
With DNA as a rigid spacer, Ag nanoparticles (NPs) were bridged to CdS quantum dots (QDs) for the stimulation of exciton-plasmon interactions (EPI) in a photoelectrochemical (PEC) system. Due to their natural absorption overlap, the exciton of the QDs and the plasmon of Ag NPs could be induced simultaneously. The EPI resonant nature enabled manipulating photoresponse of the QDs via tuning interparticle distances. Specifically, the photocurrent of the QDs could be greatly attenuated and even be completely damped by the generated EPI. The work opens a different horizon for EPI investigation through an engineered PEC nanosystem, and provides a viable mechanism for new DNA sensing protocol.
Co-reporter:Wei-Wei Zhao, Zheng-Yuan Ma, Dong-Yang Yan, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2012 Volume 84(Issue 24) pp:10518
Publication Date(Web):November 30, 2012
DOI:10.1021/ac3028799
In this work, a novel photoelectrochemical (PEC) immunoanalysis format was developed for sensitive and specific detection of prostate-specific antigen (PSA) based on an in situ electron donor producing approach. Thioglycolic acid-capped CdS quantum dots (QDs) equipped TiO2 nanotubes (NTs) were fabricated via a facile electrostatic adsorption method. The coupling of CdS QDs and TiO2 NTs results in an enhanced excitation and photo-to-electric conversion efficiency. Using alkaline phosphatase catalytic chemistry to in situ generate ascorbic acid for electron donating, an exquisite immunosandwich protocol was successfully constructed for the PSA assay due to the dependence of the photocurrent signal on the concentration of electron donor. This work opens a different perspective for transducer design in PEC detection and provides a general format for future development of PEC immunoanalysis.
Co-reporter:Fen-Ying Kong, Xiao-Rong Li, Wei-Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2012 Volume 14(Issue 1) pp:59-62
Publication Date(Web):January 2012
DOI:10.1016/j.elecom.2011.11.004
Herein, we demonstrated a facile strategy for preparing high-loading Au nanoparticles using thionine functionalized graphene oxide as the supporting material. Glassy carbon electrodes modified with the as-obtained nanocomposites showed remarkably electrocatalytic activity towards the oxidation of glucose, leading to an enzymeless glucose sensor with a wide linear range and a lower detection limit of 0.05 μmol/L.Highlights► Using thionine to functionalize graphene oxide. ► High-loading Au NPs are obtained. ► As-obtained nanocomposites can be used as electrocatalysts toward the oxidation of glucose. ► Determination of glucose appears to be simple yet sensitive.
Co-reporter:Huai-Rong Zhang, Xing-Hua Xia, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2012 Volume 25() pp:112-115
Publication Date(Web):November 2012
DOI:10.1016/j.elecom.2012.09.039
We report here a sensitive electrochemiluminescence (ECL) approach for detection of HL-60 cancer cells based on Au nanoparticles (NPs) enhanced ECL of CdS nanocrystal (NC) film supplemented by magnetic separation. In this approach, capture DNA-1 modified CdS NC film was used as ECL emitter. Capture DNA-2, which is labeled with Au NP, is hybridized with the aptamer modified on magnetic beads (MBs) to form MB-Au NP bioconjugates. In the presence of HL-60 cells, the aptamer would conjugate with the glycoprotein at cell surface and Au NPs labeled capture DNA-2 would be released. After magnetic separation, the released Au NPs labeled capture DNA-2 is hybridized with the capture DNA-1 to enhance the ECL signal of CdS NC film. This approach could sensitively detect HL-60 cells with a linear calibration range from 20 to 1.0 × 106 cells/mL.Highlights► Au NPs were used to enhance the ECL of CdS NC film through energy transfer. ► Aptamer tagged magnetic beads were used as capture and separation tools. ► A detection limit of 20 HL-60 cancer cells per milliliter could be achieved.
Co-reporter:Chun-Yuan Tian, Wei-Wei Zhao, Jing Wang, Jing-Juan Xu and Hong-Yuan Chen  
Analyst 2012 vol. 137(Issue 13) pp:3070-3075
Publication Date(Web):01 May 2012
DOI:10.1039/C2AN35493D
This work reports an ECL immunoassay method for ultrasensitive detection of prostate protein antigen (PSA), by remarkably efficient energy-transfer induced electrochemiluminescence (ECL) quenching from the CdS nanoparticles (NPs) sensitized TiO2 nanotube array (CdS–TiO2 NTs) to the activated CdTe NPs functionalized multi-wall carbon nanotubes (CdTe–MWNTs) composite. The coupling of TiO2 and CdS NPs results in a cathodic ECL intensity 14.7 times stronger than that of the pure TiO2 NTs electrode, which could be efficiently quenched by the CdTe–MWNTs. The enhanced mechanism of TiO2 NTs ECL by CdS NPs was studied in detail by cyclic voltammetry and ECL spectroscopy. The strong absorption of the CdTe–MWNTs in the wavelength range of 400–800 nm renders them highly efficient for ECL quenching labeled on anti-PSA antibody. Based on a sandwich structure, we developed an ECL immunoassay method for the sensitive and selective detection of PSA. The ECL intensity decrement was logarithmically related to the concentration of the PSA in the range of 1.0 fg mL−1 to 10 pg mL−1 with a detection limit of 1 fg mL−1. Human serum samples were then tested using the proposed immunoassay with excellent correlations, suggesting that the proposed immunoassay method is of great promise in clinical screening of cancer biomarkers.
Co-reporter:Jing Liu, Hong Zhou, Jing-Juan Xu and Hong-Yuan Chen  
Analyst 2012 vol. 137(Issue 17) pp:3940-3945
Publication Date(Web):10 May 2012
DOI:10.1039/C2AN35463B
Survivin is a new member of apoptosis inhibition protein in cells which can promote cell proliferation and inhibit apoptosis through karyokinesis. Survivin mRNA in cells has become an important biomarker for early and accurate cancer diagnostics. Here, a switchable electrochemical sensor for survivin mRNA in living cells has been designed, which is based on the changes of electron transfer efficiency between ferrocene at the end of DNA and the electrode surface after reaction with survivin mRNA. The method was then used to study populations of individual cells with different levels of mRNA. Based on the different current changes, it was possible to evaluate different cell populations and cell status on the basis of the amount of mRNA levels in cells. This strategy may provide a new direction in the fabrication of high-performance electrochemical biosensors for the detection of biomolecules in living cells.
Co-reporter:Jing Wang, Wei-Wei Zhao, Chun-Yuan Tian, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2012 89() pp: 422-426
Publication Date(Web):
DOI:10.1016/j.talanta.2011.12.055
Co-reporter:Hong Zhou, Yan-Yan Zhang, Jing Liu, Jing-Juan Xu, and Hong-Yuan Chen
The Journal of Physical Chemistry C 2012 Volume 116(Issue 33) pp:17773-17780
Publication Date(Web):July 26, 2012
DOI:10.1021/jp305076g
This work provides a novel electrochemiluminescence resonance energy transfer (ECL-RET) system using CdS:Eu nanoscrytals (NCs) as an ECL donor and Au nanorods (Au NRs) as an ECL acceptor. CdS:Eu NC, prepared by doping 1.5% Eu3+ ions into CdS NCs, exhibits strong and stable cathodic ECL emissions in the presence of coreactant S2O82– ions with two ECL spectral bands at 450–550 nm from the host CdS and at 600–700 nm due to the energy transfer from host CdS to Eu3+ ions. Au nanorods (Au NRs) have two absorption peaks that are easily tuned to match well with the ECL emission spectrum of the CdS:Eu NCs film by adjusting the aspect ratio of the nanorods to get a highly effective ECL-RET. Here, we studied the spectrum, distance and shape dependence of the efficiency of ECL-RET between the NCs' ECL and different Au nanoparticles (Au NPs) on the basis of the stem-loop structure DNA with a 6-base-pair (bp) stem and a 12, 30, or 45 nucleotide (nct) loop. At the optimized conditions, the system could be used to ultrasensitivly and specifically detect target DNA, providing significant potential application in clinical analysis.
Co-reporter:Xiao-Ya Dong, Xiao-Na Mi, Long Zhang, Tong-Ming Liang, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2012 Volume 38(Issue 1) pp:337-341
Publication Date(Web):October–December 2012
DOI:10.1016/j.bios.2012.06.015
A novel DNAzyme-functionalized Pt nanoparticles/carbon nanotubes (DNAzyme/Pt NPs/CNTs) bioconjugate was fabricated as trace tag for ultrasensitive sandwich DNA detection. The Pt NPs/CNTs were prepared via layer-by-layer (LBL) assembly of the Pt NPs and polyelectrolyte on the carboxylated CNTs, followed by the functionalization with the DNAzyme and reporter probe DNA through the platinum—sulfur bonding. The subsequent sandwich-type DNA specific reaction would confine numerous DNAzyme/Pt NPs/CNTs bioconjugate onto the gold electrode surface for amplifying the signal. In the presence of 3,3′,5,5′ tetramethylbenzidine (TMB) which could be oxidized by the DNAzyme, electrochemical signals could be generated by chronoamperometry via the interrogation of reduction electrochemical signal of oxidized TMB. The constructed DNA sensor exhibited a wide linear response to target DNA ranging from 1.0 fM to 10 pM with the detection limit down to 0.6 fM and exhibited excellent selectivity against even a single base mismatch. In addition, this novel DNA sensor showed fairly good reproducibility, stability, and reusability.Highlights► Pt NPs/CNTs nanocomposite was prepared via layer-by-layer assembly. ► DNAzyme-functionalized Pt NPs/CNTs bioconjugate was used as trace tag for DNA sensing. ► The DNAzyme would catalyze the oxidation of 3,3′,5,5′ tetramethylbenzidine (TMB) with H2O2. ► Electrochemical signal was generated via the interrogation of reduction current of oxidized TMB.
Co-reporter:Xiao-Rong Li, Jing Liu, Fen-Ying Kong, Xin-Chun Liu, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2012 20() pp: 109-112
Publication Date(Web):
DOI:10.1016/j.elecom.2012.04.014
Co-reporter:Ping Tong, Wei-Wei Zhao, Lan Zhang, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2012 Volume 33(Issue 1) pp:146-151
Publication Date(Web):15 March 2012
DOI:10.1016/j.bios.2011.12.042
On the basis of aptamer-based rolling circle amplification (RCA) and magnetic beads (MBs), a highly sensitive electrochemical method was developed for the determination of Ochratoxin A (OTA). Initially, an amino-modified capture DNA was immobilized onto MBs for the following hybridization with an OTA aptamer and a phosphate labeled padlock DNA. In the presence of OTA, the aptamer would dissociate from the bioconjugate, and the padlock DNA would subsequently hybridize with the capture DNA to form a circular template with the aid of the T4 ligase. Next, capture DNA would act as primer to initiate a linear RCA reaction and hence generate a long tandem repeated sequences by phi29 DNA polymerase and dNTPs. Then, two quantum dots (QDs) labeled DNA probes were tagged on the resulted RCA product to indicate the OTA recognition event by electrochemical readout. This strategy, based on the novel design of OTA-mediated DNA circularization, the combination of RCA and double signal probes introduction, could detect OTA down to the level of 0.2 pg mL−1 with a dynamic range spanning more than 4 orders of magnitude. The proposed approach is tested to determine OTA in red wines and shows good application potential in real samples.Highlights► We presented a double-probe signal enhancing strategy for Ochratoxin A detection. ► Rolling circle amplification was introduced in this system. ► The method exhibited a low detection limit of 0.2 pg mL−1. ► This method could be used to detect Ochratoxin A in wine.
Co-reporter:Xiao-Rong Li, Bo Wang, Jing-Juan Xu and Hong-Yuan Chen  
Nanoscale 2011 vol. 3(Issue 12) pp:5026-5033
Publication Date(Web):04 Nov 2011
DOI:10.1039/C1NR11025J
A newly developed electrochemical biosensor for the determination of superoxide anions (O2˙−) released from cancer cells using potassium-doped multi-walled carbon nanotubes (KMWNTs)–1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM]PF6) ionic liquid composite gels is demonstrated. The KMWNTs–[BMIM]PF6 can electrocatalyze oxygen reduction to generate a strong current signal in neutral solution. Compared with KMWNTs without [BMIM]PF6 or MWNTs–[BMIM]PF6 composites, the KMWNTs–[BMIM]PF6 can enhance the oxygen reduction peak current by 6.2-fold and 2.8-fold, which greatly increases the detection sensitivity of oxygen. Then, O2˙− biosensors are fabricated by mixing superoxide dismutase (SOD) in the KMWNTs–[BMIM]PF6 gels via monitoring oxygen produced by an enzymic reaction between SOD/O2˙− without the help of electron mediators. The resulting biosensors show a linear range from 0.04 to 38 μM with a high sensitivity of 98.2 μA mM−1, and a lower detection limit of 0.024 μM. The common interferents such as hydrogen peroxide (H2O2), ascorbic acid (AA), uric acid (UA), and metabolites of neurotransmitters, do not interfere with the detection of O2˙−. The proposed biosensor is tested to determine O2˙−in vitro and from liver cancer and leukemia cells and shows good application potential in biological electrochemistry.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen  
Nanoscale 2011 vol. 3(Issue 7) pp:2916-2923
Publication Date(Web):02 Jun 2011
DOI:10.1039/C1NR10175G
This work reports an aptasensor for ultrasensitive detection of thrombin based on remarkably efficient energy-transfer induced electrochemiluminescence (ECL) quenching from CdS:Mn nanocrystals (NCs) film to CdTe QDs-doped silica nanoparticles (CdTe/SiO2 NPs). CdTe/SiO2 NPs were synthesized via the Stöber method and showed black bodies' strong absorption in a wide spectral range without excitonic emission, which made them excellent ECL quenchers. Within the effective distance of energy scavenging, the ECL quenching efficiency was dependent on the number of CdTe QDs doped into the silica NPs. Using ca. 200 CdTe QDs doped silica NPs on average of 40 nm in diameter as ECL quenching labels, attomolar detection of thrombin was successfully realized. The protein detection involves a competition binding event, based on thrombin replacing CdTe/SiO2 NPs labeled probing DNA which is hybridized with capturing aptamer immobilized on a CdS:Mn NCs film modified glassy carbon electrode surface by specific aptamer-protein affinity interactions. It results in the displacement of ECL quenching labels from CdS:Mn NCs film and concomitant ECL signal recovery. Owing to the high-content CdTe QDs in silica NP, the increment of ECL intensity (ΔIECL) and the concentration of thrombin showed a double logarithmic linear correlation in the range of 5.0 aM∼5.0 fM with a detection limit of 1aM. And, the aptasensor hardly responded to antibody, bovine serum albumin (BSA), haemoglobin (Hb) and lysozyme, showing good detection selectivity for thrombin. This long-distance energy scavenging could have a promising application perspective in the detection of biological recognition events on a molecular level.
Co-reporter:Mei-Sheng Wu, Hai-Wei Shi, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2011 vol. 47(Issue 27) pp:7752-7754
Publication Date(Web):26 May 2011
DOI:10.1039/C1CC12219C
In this paper, an electrochemiluminescence resonance energy transfer (ECL-RET) system from CdS quantum dot to Ru(bpy)32+ was developed for the first time. By the signal amplification of Ru(bpy)32+ and the specific antibody–cell surface interactions, this ECL-RET system could sensitively respond down to 12.5 SMMC-7721 cells per mL.
Co-reporter:Wei-Wei Zhao, Jing Wang, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2011 vol. 47(Issue 39) pp:10990-10992
Publication Date(Web):12 Sep 2011
DOI:10.1039/C1CC13952E
This work is the first report on the energy transfer between CdS quantum dots and Au nanoparticles for photoelectrochemical biosensing applications.
Co-reporter:Hong Zhou, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2011 vol. 47(Issue 29) pp:8358-8360
Publication Date(Web):21 Jun 2011
DOI:10.1039/C1CC12413G
We report here an ultrasensitive DNA detection approach which combines Au NPs enhanced electrochemiluminescence (ECL) of the CdS nanocrystal (NC) film with isothermal circular amplification reaction of polymerase and nicking endonuclease (NEase). By the double-signal amplification, this approach could sensitively respond down to 5 aM DNA.
Co-reporter:Jing Liu, Hong Zhou, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2011 vol. 47(Issue 15) pp:4388-4390
Publication Date(Web):09 Mar 2011
DOI:10.1039/C1CC10430F
A novel switch-cytosensing strategy has been designed, which is based on the changes of electron transfer efficiency between ferrocene at the end of DNA and the electrode surface before and after cell transfection. This strategy provided a general and convenient method to fabricate efficient electrochemical cell sensors.
Co-reporter:Jing Wang, Yun Shan, Wei-Wei Zhao, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2011 Volume 83(Issue 11) pp:4004
Publication Date(Web):April 25, 2011
DOI:10.1021/ac200616g
Interactions between surface plasmons (SP) of metallic surfaces and photoluminescence (PL) of semiconductor nanocrystal (S-NC) surfaces have been extensively investigated, and SP-induced PL enhancement has been used as a sensitive analytical technique. However, this SP induced electrochemiluminescence (ECL) enhancement is rarely studied. In this work, we report greatly enhanced ECL of CdS thin films by gold nanoparticles (Au NPs) for ultrasensitive detection of thrombin. The system was composed of a CdS NC film on glassy carbon electrode (GCE) as ECL emitter attached an aptamer of thrombin. Then, ssDNA–AuNP conjugates hybridized with the aptamer to form a separation length of ca. 12 nm between CdS NCs and Au NPs. The system showed 5-fold enhancement of ECL intensity as compared to that without Au NPs, which might be attributed to the long-distance interaction between the S-NCs and SPR field of noble metal nanoparticles (MNPs).We also found that the enhanced ECL could be influenced by the involving factors such as the separation distance, spectral overlap, and magnetic field. Such enhancement in combination with smart recognition of aptamer and target protein allowed us to construct an ultrasensitive aptasensor for attomolar detection of thrombin. The presence of target protein was reflected by the ECL signal decrease caused by the target-induced removal of ssDNA–AuNP conjugates. The decrease of ECL signal was logarithmically linear with the concentration of thrombin in a wide range from 100 aM to 100 fM. The principle described in this work could be also applied to many other bioassays.
Co-reporter:Hong Zhou, Jing Liu, Jing-Juan Xu, and Hong-Yuan Chen
Analytical Chemistry 2011 Volume 83(Issue 21) pp:8320
Publication Date(Web):September 16, 2011
DOI:10.1021/ac2022629
We report here a new electrochemiluminescence (ECL) approach for detection of single nucleotide polymorphisms (SNPs) based on isothermal cycle-assisted triple-stem probe labeled with Au nanoparticles (NPs) and CdTe NPs. The system is composed of a CdS nanocrystals (NCs) film on glassy carbon electrode (GCE) as ECL emitter attached a double-stem DNA probe labeled with Au NPs. Then, the third stem labeled with CdTe NPs hybridizes with the double-stem DNA to form a triple-stem probe with the two labels near the CdS NCs film. A dual-quenched ECL of CdS NCs film is achieved due to energy transfer (ET) from CdS NCs to Au NPs and CdTe NPs, which makes the sensor exhibit relatively low background. Once the one base mutant DNA (mDNA) sequence as target of SNPs analysis displaces the third stem and hybridizes with the double-stem probe, forcing Au NPs away from the CdS NCs film, an ECL enhancement by the ECL-induced surface plasmon resonance of Au NPs is observed. Furthermore, after an isothermal cycle induced by primer, polymerase, and nicking endonuclease (NEase), a further enhancement of ECL is obtained. Taking advantages of the isothermal circular amplification system and the triple-stem probe architecture which enables turning its high selectivity toward specific target sequences, the reported biosensor shows excellent discrimination capabilities of SNPs with high selectivity and low detection limit (35 aM).
Co-reporter:Mei-Sheng Wu, Bi-Yi Xu, Hai-Wei Shi, Jing-Juan Xu and Hong-Yuan Chen  
Lab on a Chip 2011 vol. 11(Issue 16) pp:2720-2724
Publication Date(Web):06 Jul 2011
DOI:10.1039/C1LC20143C
In this paper we report a transparent bipolar electrode based microfluidic chip–electrochemiluminescence (ECL) system for sensitive detection of folate receptors (FR) on cell membranes. This integrated system consists of a poly(dimethylsiloxane) (PDMS) layer containing a microchannel and a glass bottom sheet with indium tin oxide (ITO) strips as bipolar detectors. The ITO strips are fabricated using a PDMS micromold with carbon ink as a protective layer in place of traditional photoresist. The configuration of the bipolar electrode has great influence on the ECL intensity of Ru(bpy)32+/tripropylamine(TPA) system. Further studies show that folic acid (FA) can strongly inhibit the ECL of the Ru(bpy)32+/TPA system. Based on specific recognition between FA and FR on cell membrane, this microfluidic chip–ECL system is successfully applied for detecting the level of FR on human cervical tumor (HL-60) cells and MEF cells. It is found that the ECL intensity increases with the number of HL-60 cells in the range of 21 to 3.28 × 104cells/mL. The average level of FR on HL-60 cells is calculated to be 8.05 ± 0.75 × 10−18 mol/cell. While for MEF cells, it shows a much slower ECL increment than HL-60 cells due to the much lower FR level on MEF cells (5.30 ± 0.61 × 10−19 mol/cell). Moreover, exocytosis of FA after FR mediated endocytosis was observed according to the change of the ECL signal with the incubation time of HL-60 cells in the FA- Ru(bpy)32+/TPA system.
Co-reporter:Fen-Ying Kong, Xu-Zhu, Mao-Tian Xu, Jing-Juan Xu, Hong-Yuan Chen
Electrochimica Acta 2011 Volume 56(Issue 25) pp:9386-9390
Publication Date(Web):30 October 2011
DOI:10.1016/j.electacta.2011.08.018
A new signal amplification strategy employing nanocomposites composed of gold nanoparticles (GNPs) with DNA and methylene blue (MB) as labels has been developed to construct a novel immunosensor for the highly sensitive bioanalysis of carcinoembryonic antigen (CEA). To fabricate the label, DNA was first linked to GNPs through the formation of an Au–S bond. Next, the resulting bioconjugates were sequentially bound with MB via the guanine (G) bases in DNA specifically and then with secondary CEA antibody (Ab2) via the crosslinking of glutaraldehyde (GA). The receptor–analyte complex is formed by the biorecognition of the as-obtained MB labeled Ab2 with the primary CEA antibody (Ab1) immobilized on the surface of a modified GNP/Chitosan (Chits) composite electrode. After the receptor–analyte complex has formed, square wave voltammetry (SWV) was employed to oxidize the labeled MB in order to detect the CEA. This immunosensor shows a linear response from 0.10 to 2.0 pg mL−1 CEA with an improved detection limit of 0.05 pg mL−1 as compared to the conventional immunoassay. In addition, this new protocol shows acceptable stability, reproducibility and good recovery (97.5–110.0%) for CEA in human serum with great potential for clinical applications.
Co-reporter:Wei-Wei Zhao, Pei-Pei Yu, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2011 Volume 13(Issue 5) pp:495-497
Publication Date(Web):May 2011
DOI:10.1016/j.elecom.2011.02.031
The coupling of biocatalytic precipitation (BCP) to photoelectrochemical (PEC) biosensing for the development of rapid PEC sensors with ultrahigh sensitivity and excellent anti-interference ability is successfully realized. Horseradish peroxidase (HRP) was immobilized on the matrix of TiO2/CdS and 4-chloro-1-naphthol (4-CN) was chosen for the BCP-amplified PEC detection of H2O2. The HRP accelerated oxidation of 4-CN by H2O2 would yield insoluble product on the photoelectrode surface, on the basis of which the photocurrent be influenced. The detection limit of 5.0 × 10−10 M (S/N = 3) for the determination of H2O2 was achieved.Research Highlights► Photoelectrochemical (PEC) biosensing as platform. ► Biocatalytic precipitation (BCP) is integrated. ► BCP-amplified ultrasensitive PEC biosensing is realized. ► Interference problem could be avoided.
Co-reporter:Xiao-Rong Li, Jing-Juan Xu, Hong-Yuan Chen
Electrochimica Acta 2011 Volume 56(Issue 25) pp:9378-9385
Publication Date(Web):30 October 2011
DOI:10.1016/j.electacta.2011.08.020
We demonstrate herein a newly developed serum total cholesterol biosensor by using the direct electron transfer of cholesterol oxidase (ChOx), which is based on the immobilization of cholesterol oxidase and cholesterol esterase (ChEt) on potassium-doped multi-walled carbon nanotubes (KMWNTs) modified electrodes. The KMWNTs accelerate the electron transfer from electrode surface to the immobilized ChOx, achieving the direct electrochemistry of ChOx and maintaining its bioactivity. As a new platform in cholesterol analysis, the resulting electrode (ChOx/KMWNTs/GCE) exhibits a sensitive response to free cholesterol, with a linear range of 0.050–16.0 μmol L−1 and a detection limit of 5.0 nmol L−1 (S/N = 3). Coimmobilization of ChEt and ChOx (ChEt/ChOx/KMWNTs/GCE) allows the determination of both free cholesterol and esterified cholesterol. The resulting biosensor shows the same linear range of 0.050–16.0 μmol L−1 for free cholesterol and cholesteryl oleate, with the detection limit of 10.0 and 12.0 nmol L−1 (S/N = 3), respectively. The concentrations of total (free and esterified) cholesterol in human serum samples, determined by using the techniques developed in the present study, are in good agreement with those determined by the well-established techniques using the spectrophotometry.
Co-reporter:Hong-Lei Gou, Xian-Bo Zhang, Ning Bao, Jing-Juan Xu, Xing-Hua Xia, Hong-Yuan Chen
Journal of Chromatography A 2011 Volume 1218(Issue 33) pp:5725-5729
Publication Date(Web):19 August 2011
DOI:10.1016/j.chroma.2011.06.102
As a label-free alternative of conventional flow cytometry, chip-based impedance measurement for single cell analysis has attracted increasing attentions in recent years. In this paper, we designed a T-shape microchannel and fabricated a pair of gold electrodes located horizontally on each side of the microchannel using a transfer printing method. Instant electric signals of flowing-through single cells were then detected by connecting the electrodes to a Keithley resistance and capacitance measurement system. Experimental results based on the simultaneous measurement of resistance and capacitance demonstrated that HL-60 and SMMC-7721 cells could be differentiated effectively. Moreover, SMMC-7721 cells at normal, apoptotic and necrotic status can also be discriminated in the flow. We discussed the possible mechanism for the discrimination of cell size and cell status by electrical analysis, and it is believed that the improvement of detection with our design results from more uniform distribution of the electric field. This microfluidic design may potentially become a promising approach for the label-free cell sorting and screening.
Co-reporter:Ping Tong, Lan Zhang, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2011 Volume 29(Issue 1) pp:97-101
Publication Date(Web):15 November 2011
DOI:10.1016/j.bios.2011.07.075
A new “signal-on” aptasensor for ultrasensitive detection of Ochratoxin A (OTA) in wheat starch was developed based on exonuclease-catalyzed target recycling. To construct the aptasensor, a ferrocene (Fc) labeled probe DNA (S1) was immobilized on a gold electrode (GE) via Au–S bonding for the following hybridization with the complementary OTA aptamer, with the labeled Fc on S1 far from the GE surface. In the presence of analyte OTA, the formation of aptamer-OTA complex would result in not only the dissociation of aptamer from the double-strand DNA but also the transformation of the probe DNA into a hairpin structure. Subsequently, the OTA could be liberated from the aptamer-OTA complex for analyte recycling due to the employment of exonuclease, which is a single-stranded DNA specific exonuclease to selectively digest the appointed DNA (aptamer). Owing to the labeled Fc in close proximity to the electrode surface caused by the formation of the hairpin DNA and to the analyte recycling, differential pulse voltammetry (DPV) signal could be produced with enhanced signal amplification. Based on this strategy, an ultrasensitive aptasensor for the detection of OTA could be exhibited with a wide linear range of 0.005–10.0 ng mL−1 with a low detection limit (LOD) of 1.0 pg mL−1 OTA (at 3σ). The fabricated biosensor was then applied for the measurement of OTA in real wheat starch sample and validated by ELISA method.
Co-reporter:Xiao-Ya Dong, Xiao-Na Mi, Bo Wang, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2011 Volume 84(Issue 2) pp:531-537
Publication Date(Web):15 April 2011
DOI:10.1016/j.talanta.2011.01.060
An electrochemical approach for the sensitive detection of sequence-specific DNA has been developed. Horseradish peroxidase (HRP) assembled on the Fe3O4 nanoparticles (NPs) were utilized as signal amplification sources. High-content HRP was adsorbed on the Fe3O4 NPs via layer-by-layer (LbL) technique to prepare HRP-functionalized Fe3O4 NPs. Signal probe and diluting probe were then immobilized on the HRP-functionalized Fe3O4 NPs through the bridge of Au NPs. Thereafter, the resulting DNA–Au–HRP–Fe3O4 (DAHF) bioconjugates were successfully anchored to the gold nanofilm (GNF) modified electrode surface for the construction of sandwich-type electrochemical DNA biosensor. The electrochemical behaviors of the prepared biosensor had been investigated by the cyclic voltammetry (CV), chronoamperometry (i–t), and electrochemical impedance spectroscopy (EIS). Under optimal conditions, the proposed strategy could detect the target DNA down to the level of 0.7 fmol with a dynamic range spanning 4 orders of magnitude and exhibited excellent discrimination to two-base mismatched DNA and non-complementary DNA sequences.
Co-reporter:Xiao-Ya Dong, Xiao-Na Mi, Wei-Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2011 Volume 26(Issue 8) pp:3654-3659
Publication Date(Web):15 April 2011
DOI:10.1016/j.bios.2011.02.023
A novel and simple method for preparing cadmium sulfide nanoparticles (CdS NPs) functionalized colloidal carbon particles (CPs) has been successfully developed by in situ growing abundant CdS NPs on the surfaces of monodisperse carbon particles (CdS/CPs). The obtained CdS/CPs conjugates as signal amplification labels were further used for the ultrasensitive determination of thrombin. The CdS/CPs conjugates were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and UV–visible absorption spectrum (UV). The protein electrical detection involves a dual binding event, based on thrombin linked to the CdS/CPs tags and glass surface by the specific aptamer–protein affinity interactions and a succedent electrochemical stripping transduction. Owing to the high-content CdS NPs on carbon particles, this assay allowed a desirable detection limit of 6.0 × 10−17 M, which was 1000 times lower than that of only using CdS NPs as labels in the control experiments. This protocol exhibited excellent selectivity against these common proteins such as bovine plasma albumin, lysozyme and hemoglobin. The signal amplification approach proposed here provides a facile, cost-effective method for the ultrasensitive determination of thrombin in the practical samples.
Co-reporter:Shao-Peng Chen, Xiao-Dong Yu, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2011 Volume 26(Issue 12) pp:4779-4784
Publication Date(Web):15 August 2011
DOI:10.1016/j.bios.2011.06.001
A novel microfluidic immunoassay system for specific detection of hemoglobin A1c (HbA1c) was developed based on a three-component shell/shell/core structured magnetic nanocomposite Au/chitosan/Fe3O4, which was synthesized with easy handling feature of Fe3O4 by magnet, high affinity for gold nanoparticles of chitosan and good immobilization ability for anti-human hemoglobin-A1c antibody (HbA1c mAb) of assembled colloidal gold nanoparticles. The resulting HbA1c mAb/Au/chitosan/Fe3O4 magnetic nanoparticles were then introduced into microfluidic devices coupled with a gold nanoband microelectrode as electrochemical detector. After that, three-step rapid immunoreactions were carried out in the sequence of HbA1c, anti-human hemoglobin antibodies (Hb mAb) and the secondary alkaline phosphatase (AP)-conjugated antibody within 20 min. The current response of 1-naphtol obtained from the reaction between the secondary AP-conjugated antibody and 1-naphthyl phosphate (1-NP) increased proportionally to the HbA1c concentration. Under optimized electrophoresis and detection conditions, HbA1c responded linearly in the concentration of 0.05–1.5 μg mL−1, with the detection limit of 0.025 μg mL−1. This system was successfully employed for detection of HbA1c in blood with good accuracy and renewable ability. The proposed method proved its potential use in clinical immunoassay of HbA1c.
Co-reporter:Fen-Ying Kong, Mao-Tian Xu, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2011 Volume 85(Issue 5) pp:2620-2625
Publication Date(Web):15 October 2011
DOI:10.1016/j.talanta.2011.08.028
In this paper, gold nanoparticle–thionine–reduced graphene oxide (GNP–THi–GR) nanocomposites were prepared to design a label-free immunosensor for the sensitive detection of carcinoembryonic antigen (CEA). The nanocomposites with good biocompatibility, excellent redox electrochemical activity and large surface area were coated onto the glassy carbon electrode (GCE) surface and then CEA antibody (anti-CEA) was immobilized on the electrode to construct the immunosensor. The morphologies and electrochemistry of the formed nanocomposites were investigated by using scanning electron microscopy (SEM), ultraviolet–visible (UV–vis) spectrometry, electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). CV and differential pulse voltammetry (DPV) studies demonstrated that the formation of antibody–antigen complexes decreased the peak current of THi in the GNP–THi–GR nanocomposites. The decreased currents were proportional to the CEA concentration in the range of 10–500 pg/mL with a detection limit of 4 pg/mL. The proposed method was simple, fast and inexpensive for the determination of CEA at very low levels.Highlights► Gold nanoparticles–thionine–reduced graphene oxide (GNP–THi–GR) nanocomposites synthesized using THi molecules as interlinkers. ► GR has unique electrical conductivity, enlarged active surface area. ► THi has excellent redox activity. ► GNPs has large specific surface area, excellent biocompatibility, extraordinarily catalytic activity, good conductivity. ► The nanocomposites combined with the advantages of the three species suitable for a label-free immunosensor.
Co-reporter:Xue Zhong;Hai-Jing Bai;Hong-Yuan Chen ;Yu-Hua Zhu
Advanced Functional Materials 2010 Volume 20( Issue 6) pp:992-999
Publication Date(Web):
DOI:10.1002/adfm.200901915

Abstract

A newly developed electrochemical cell sensor for the determination of K562 leukemia cells using 3-aminophenylboronic acid (APBA)-functionalized multiwalled carbon nanotubes (MWCNTs) films is demonstrated. The films are generated by the covalent coupling between the NH2 groups in APBA and the COOH group in the acid-oxidized MWCNTs. As a result of the sugar-specific affinity interactions, the K562 leukemia cells are firmly bound to the APBA-functionalized MWCNTs film via boronic acid groups. Compared to electropolymerized APBA films, the presence of MWCNTs not only provides abundant boronic acid domains for cell capture, their high electrical conductivity also makes the film suitable for electrochemical sensing applications. The resulting modified electrodes are tested as cell detection sensors. This work presents a promising platform for effective cell capture and constructing reusable cytosensors.

Co-reporter:Guang-Li Wang, Jing-Juan Xu and Hong-Yuan Chen  
Nanoscale 2010 vol. 2(Issue 7) pp:1112-1114
Publication Date(Web):07 May 2010
DOI:10.1039/C0NR00084A
A highly sensitive and selective photoelectrochemical sensor for Cu2+ was developed based on the selective interaction between CdS quantum dots (QDs) immobilized on an indium tin oxide (ITO) electrode surface and Cu2+ in a triethanolamine (TEA) solution to form CuxS-doped CdS QDs, which disrupts the electron transfer from the conduction band of CdS to ITO and results in a decrease of photocurrent.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2010 vol. 46(Issue 23) pp:4187-4189
Publication Date(Web):11 May 2010
DOI:10.1039/C003124K
This work firstly reports an opto–magnetic interaction–induced enhancement of electrochemiluminescence (ECL) from CdS:Mn nanocrystals (NCs) film by superparamagnetic Fe3O4 nanoparticles and its application to sensitive immunosensing.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2010 vol. 46(Issue 28) pp:5079-5081
Publication Date(Web):17 Jun 2010
DOI:10.1039/C0CC00837K
Efficient electrochemiluminescence (ECL) quenching was achieved by functionalized CdTe quantum dots (QDs) through ECL energy scavenging, based on which ultrasensitive antigen detection could be realized.
Co-reporter:Bi-Yi Xu, Jing-Juan Xu, Xing-Hua Xia and Hong-Yuan Chen  
Lab on a Chip 2010 vol. 10(Issue 21) pp:2894-2901
Publication Date(Web):04 Oct 2010
DOI:10.1039/C005245K
This paper reports a new fabrication method of lithography-free nanochannel array. It is based on the cracking process on the surface of a polystyrene (PS) Petri-dish, one type of thermoplastic that is composed of uni-axial macromolecular chains. Under proper conditions, parallel nanochannels with equal interspaces are obtained. Control over the channel depth from 20 nm to 200 nm is achieved, with the channel length reaching tens of millimetres. The PDMS replication based on PS nanochannel array has been successfully carried out. In combination with the microstructure, both an ion enrichment device and a current rectification device are fabricated, and their quantified characters manifested the applicability of the channel array structure in nanofluidics.
Co-reporter:Shou-Nian Ding, Jing-Juan Xu, Dan Shan, Bu-Hong Gao, Hai-Xin Yang, Yue-Ming Sun, Serge Cosnier
Electrochemistry Communications 2010 Volume 12(Issue 5) pp:713-716
Publication Date(Web):May 2010
DOI:10.1016/j.elecom.2010.03.015
The enhanced visible absorbance related to electrochromic response (ECR) of CdS nanocrystals (NCs) thin film in aqueous solution was firstly investigated to elucidate the detailed electrochemiluminescence (ECL) mechanism of semiconductor NCs/H2O2 system. The recovery efficiency of ECR was found as the key factor to affect the intensity of ECL. This preliminary study between ECR and ECL of semiconductor NCs in aqueous solution can provide the profound guidance to fabricate enhanced “signal-off” kind ECL sensors to widen its application in analytical field.
Co-reporter:Shao-Peng Chen, Jian Wu, Xiao-Dong Yu, Jing-Juan Xu, Hong-Yuan Chen
Analytica Chimica Acta 2010 Volume 665(Issue 2) pp:152-159
Publication Date(Web):30 April 2010
DOI:10.1016/j.aca.2010.03.043
We proposed herein a novel approach for fabricating nanoband microelectrodes for electrochemical detection on an electrophoresis microchip. The metal films were first obtained via region-selective electroless deposition of gold or copper films on PDMS substrates by selective region plasma oxidation through shadow masking. Both metal films show uniform surfaces with the thickness at the level of 100 nm. By casting another PDMS layer on the metal films, the cross section of the sandwich structures can be used as nanoband microelectrodes, which can be renewed just by cutting. These nanoband microelectrodes are successfully used as electrochemical detectors in microchip electrophoresis for the detection of amino acids, proteins and neurotransmitter molecules. Moreover, integrating an Au-Cu double-metal detector with a double-channel electrophoresis system, we can easily distinguish electroactive amino acids from that of non-electroactive amino acids.
Co-reporter:Jiu-Ju Feng, Ai-Jun Wang, Jing Fan, Jing-Juan Xu, Hong-Yuan Chen
Analytica Chimica Acta 2010 Volume 658(Issue 1) pp:75-80
Publication Date(Web):18 January 2010
DOI:10.1016/j.aca.2009.10.052
A novel covalent strategy was developed to modify the poly(dimethylsiloxane) (PDMS) surface. Briefly, dextran was selectively oxidized to aldehyde groups with sodium periodate and subsequently grafted onto amine-functionalized PDMS surface via Schiff base reaction. As expected, the coated PDMS surface efficiently prevented the biomolecules from adsorption. Electro-osmotic flow (EOF) was successfully suppressed compared with that on the native PDMS microchip. Moreover, the stability of EOF was greatly enhanced and the hydrophilicity of PDMS surface was also improved. To apply thus-coated microchip, the separation of peptides, protein and neurotransmitters was investigated in detail. For comparison, these analytes were also measured on the native PDMS microchips. The results demonstrated that these analytes were efficiently separated and detected on the coated PDMS microchips. Furthermore, the relative standard deviations of their migration times for run-to-run, day-to-day, and chip-to-chip reproducibilities were in the range of 0.6–2.7%. In addition, the coated PDMS microchips showed good stability within 1 month.
Co-reporter:Yu-Hui Bai, Jin-Yi Li, Jing-Juan Xu and Hong-Yuan Chen  
Analyst 2010 vol. 135(Issue 7) pp:1672-1679
Publication Date(Web):24 May 2010
DOI:10.1039/B923847F
A novel method is described for the highly effective amplifying electrochemical response of DNA based on oligonucleotides functionalized with Au/Fe3O4 nanocomposites by the aid of silver (Ag) enhancement. Via electrostatic layer-by-layer (LBL) assembly, the prepared Fe3O4 nanoparticles form nano-clusters coated with a bilayer composed of polystyrene sulfonate sodium salt (PSS) and poly(diallyldimethylammonium chloride) (PDDA), which are in favor of adsorbing lots of gold nanoparticles (AuNPs) on the surface. The application of magnetic Fe3O4 made the procedures much more simple, convenient and feasible. The resulting composites were then used as labels via the Au–S bond for the DNA hybridization, followed by catalytic deposition of silver on the gold tags. Such an assay is then combined with a sensitive anodic stripping voltammetry (ASV) measurement of multiple silver nanoparticle tracers. A 27-mer sequence DNA target is detected at a glassy carbon (GC) electrode with a detection limit down to ca. 100 aM, which is 800 times lower than that obtained using gold nanoparticles only as labels in the control experiments. This Fe3O4/PSS/PDDA/Au composite offers a great promising future for the ultrasensitive detection of other biorecognition events.
Co-reporter:Shao-Peng Chen, Xiao-Dong Yu, Jing-Juan Xu and Hong-Yuan Chen  
Analyst 2010 vol. 135(Issue 11) pp:2979-2986
Publication Date(Web):28 Sep 2010
DOI:10.1039/C0AN00231C
In this paper an enzyme-carrier-based microfluidic chip coupled with a gold nanoband microelectrode as electrochemical detector for Triglyceride (TG) determination was developed by co-immobilized lipase, Glycerokinase (GK) and glycerol-3-phosphate oxidase (GPOx) on chitosan/Fe3O4 composite nanoparticles with a shell-core structure, which combined the advantageous features of microfluidic chips technology with magnetic beads. This procedure enabled the easy renewal of the microchip enzyme carrier after each determination in a highly reproducible manner. Several operational parameters such as working potential, buffer pH, adenosine triphosphate concentrations (ATP, mM), separation voltage and temperature were evaluated and optimized. The performance of enzyme-carrier-based microfluidic chip for TG determination was modulated by changing the length of enzyme carrier from 1.0 to 3.0 cm, and the linear ranges were changed from 0–4.0 mM to 0–10.0 mM with the detection limits from 15 μM to 6.0 μM. The enzyme carrier remained its 70% activity after 40 days storage. This system was successfully employed for on-line detection of TG in serums. The experimental results demonstrated that this enzyme carrier using magnetic beads based microfluidic chip provided a relatively simple, sensitive, miniature, and replaceable means for the accurate determination of TG in serum.
Co-reporter:Zheng Qian, Hai-Jing Bai, Guang-Li Wang, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2010 Volume 25(Issue 9) pp:2045-2050
Publication Date(Web):15 May 2010
DOI:10.1016/j.bios.2010.01.036
We demonstrated herein a newly developed photoelectrochemical cell-sensor for the determination of SMMC-7721 human hepatoma carcinoma cells (SMMC-7721 cells) by using a photosensitive CdS-polyamidoamine (G4) nano-composite film (CdS-PAMAM). The film was generated by electrodeposition method. The presence of PAMAM in the film eliminated the surface defects of CdS nanoparticles and therefore resulted in a greatly enhanced photocurrent and a reduced dark current. In the presence of the electron donor ascorbic acid (AA), the photoexcitation of this modified electrode potentiostated at 0 V versus Ag/AgCl led to an anodic photocurrent. As a result of the covalent coupling reactions, a layer of concanavalin A (ConA) was firmly bound to the functionalized CdS-PAMAM film via glutaraldehyde bridges. The resulting modified electrodes were tested as sensors for SMMC-7721 cell capture and detection via affinity interactions between ConA and mannosyl groups on cell surface. The cell concentration was measured from 5.0 × 103 to 1.0 × 107 cells mL−1 through the decrease in photocurrent intensity resulting from its specific binding onto the photosensitive film, the detection limit being 5.0 × 103 cells mL−1.
Co-reporter:Jian Wu, Hai-Jing Bai, Xian-Bo Zhang, Jing-Juan Xu and Hong-Yuan Chen
Langmuir 2010 Volume 26(Issue 2) pp:1191-1198
Publication Date(Web):September 1, 2009
DOI:10.1021/la902332q
We report an approach for fabricating a tunable wettability surface by electroless gold plating on poly(dimethylsiloxane) (PDMS). A two-layer structured gold film with a tight layer and a loose layer can be obtained on the surface of a PDMS chip when the PDMS chip is immersed in a gold plating solution at 30 °C for 4 h. Its wettability can be rapidly switched between superhydrophilicity and superhydrophobicity by plasma and heat treatments without any self-assembled monolayer, and the superhydrophobicity can be even changed from the gecko-foot-hair-like character to the lotus-leaf-like character. Benefiting from the various wettabilities of the prepared gold/PDMS composites, protein patterning is successfully achieved on a patterned superhydrophobic/superhydrophilic gold/PDMS composite; a superhydrophobic needle for transferring supersmall water droplets (1 μL) to a superhydrophobic surface is successfully fabricated.
Co-reporter:Xue Zhong ; Guang-Sheng Qian ; Jing-Juan Xu ;Hong-Yuan Chen
The Journal of Physical Chemistry C 2010 Volume 114(Issue 45) pp:19503-19508
Publication Date(Web):October 27, 2010
DOI:10.1021/jp106383p
In this paper, an interface constructed with fibronectin (Fn) functionalized multiple-walled carbon nanotubes (MWNTs) was prepared which can efficiently capture cells. The acid-treated MWNTs were covalently coupled with Fn in the presence of a coupling agent, thus realizing the efficient immobilization of Fn, and it was proven by infrared spectroscopy. Due to the specific binding of integrin receptor on cells and the arginine-glycine-aspartic acid amino acids (RGD) peptide contained in Fn, this interface not only has a property for capturing SMMC 7721 cells, but also efficiently retains viability of immobilized cells. The presence of MWNTs not only increases the surface area of the electrode but also promotes the electrochemical behavior of SMMC 7721 cells. In addition, we applied homemade heated glassy carbon electrodes to cell detection, which were indirectly heated by direct current. Profiting from the heat convection generated by the joule heat from direct current, the sensitivity of the detection of cell concentration was clearly meliorated. The biosensor based on heated electrode modified with Fn-MWNTs, presents a promising platform for sensitive cell detection.
Co-reporter:Xiao-Fei Wang;Yi Zhou;Hong-Yuan Chen
Advanced Functional Materials 2009 Volume 19( Issue 9) pp:1444-1450
Publication Date(Web):
DOI:10.1002/adfm.200801313

Abstract

This work describes for the first time signal-on electrochemiluminescence (ECL) enzyme biosensors based on cadmium sulfide nanocrystals (CdS NCs) formed in situ on the surface of multi-walled carbon nanotubes (MWCNTs). The MWCNT–CdS can react with H2O2 to generate strong and stable ECL emission in neutral solution. Compared with pure CdS NCs, the MWCNT–CdS can enhance the ECL intensity by 5.3-fold and move the onset ECL potential more positively for about 400 mV, which reduces H2O2 decomposition at the electrode surface and increases detection sensitivity of H2O2. Furthermore, the ECL intensity is less influenced by the presence of oxygen in solution. Benefiting from these properties, signal-on enzyme-based biosensors are fabricated by cross-linking choline oxidase and/or acetylcholine esterase with glutaraldehyde on MWCNT–CdS modified electrodes for detection of choline and acetylcholine. The resulting ECL biosensors show wide linear ranges from 1.7 to 332 µM and 3.3 to 216 µM with lower detection limit of 0.8 and 1.7 µM for choline and acetylcholine, respectively. The common interferents such as ascorbic acid and uric acid in electrochemical enzyme-based biosensors do not interfere with the ECL detection of choline and acetylcholine. Furthermore, both ECL biosensors possess satisfying reproducibility and acceptable stability.

Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen  
Chemical Communications 2009 (Issue 8) pp:905-907
Publication Date(Web):16 Jan 2009
DOI:10.1039/B821049G
The quenching of electrochemiluminescence (ECL) from a CdS:Mn nanocrystal film by proximal Au nanoparticles was observed as a result of Förster energy transfer, while an enhancement of ECL takes place after hybridization with target DNA due to the energy transfer of ECL excited surface plasmon resonances in AuNPs to the CdS:Mn NCs at large separation, based on which an ultrasensitive and specific DNA biosensor was constructed.
Co-reporter:Wei Zhao, Pei-Yu Ge, Jing-Juan Xu and Hong-Yuan Chen
Environmental Science & Technology 2009 Volume 43(Issue 17) pp:6724
Publication Date(Web):August 5, 2009
DOI:10.1021/es900841n
We report on a pair of highly sensitive amperometric biosensors for organophosphate pesticides (OPs) based on assembling acetylcholinesterase (AChE) on poly(dimethylsiloxane) (PDMS)−poly(diallydimethylammonium) (PDDA)/gold nanoparticles (AuNPs) composite film. Two AChE immobilization strategies are proposed based on the composite film with hydrophobic and hydrophilic surface tailored by oxygen plasma. The twin biosensors show interesting different electrochemical performances. The hydrophobic surface based PDMS-PDDA/AuNPs/choline oxidase (ChO)/AChE biosensor (biosensor-1) shows excellent stability and unique selectivity to hypertoxic organophosphate. At optimal conditions, this biosensor-1 could measure 5.0 × 10−10 g/L paraoxon and 1.0 × 10−9 g/L parathion. As for the hydrophilic surface based biosensor (biosensor-2), it shows no selectivity but can be commonly used for the detection of most OPs. Based on the structure of AChE, it is assumed that via the hydrophobic interaction between enzyme molecules and hydrophobic surface, the enzyme active sites surrounded by hydrophobic amino acids face toward the surface and get better protection from OPs. This assumption may explain the different performances of the twin biosensors and especially the unique selectivity of biosensor-1 to hypertoxic OPs. Real sample detection was performed and the omethoate residue on Cottomrose Hibiscus leaves was detected with biosensor-1.
Co-reporter:Ying Du, Jing-Juan Xu, Hong-Yuan Chen
Electrochemistry Communications 2009 Volume 11(Issue 8) pp:1717-1720
Publication Date(Web):August 2009
DOI:10.1016/j.elecom.2009.07.004
An ultrathin platinum film is fabricated on a nanoporous gold (NPG) scaffold through a catalytic chemical deposition method. The morphology and active surface area of the deposited Pt film, which will greatly influence the electro-catalytic properties of the catalyst, can be controlled by adjusting the deposition condition. Compared with bare NPG and high Pt loaded NPG, the performances of methanol electro-oxidation on the low-Pt-content bimetallic film are greatly improved, both in its catalytic current enhancement and signal stability. The best condition for methanol oxidation can be achieved when the area ratio of deposited Pt and uncovered Au was 3:1.
Co-reporter:Pei-Yu Ge, Ying Du, Jing-Juan Xu, Hong-Yuan Chen
Journal of Electroanalytical Chemistry 2009 Volume 633(Issue 1) pp:182-186
Publication Date(Web):1 August 2009
DOI:10.1016/j.jelechem.2009.05.010
Gold nanofilm, with a nanoporous morphology, was found to have the unique property to catalyze the oxidization of ascorbic acid (AA) and dopamine (DA), resulting in the improved electrochemical behavior of the two species and a negative shift of the oxidization potential of AA for about 300 mV. The catalytic oxidization of gold nanofilm to AA is mainly ascribed to its high surface energy, while the enhanced electron transfer ability of DA on the gold nanofilm is attributed to the strong interaction between DA and the electrode surface. Based on the peak separation of DA and AA, selective detection of DA was achieved on the gold nanofilm modified electrode. Differential pulse voltammetry (DPV) techniques and cyclic voltammetry (CV) were used to investigate the electrochemical behavior of AA and DA on the surface of the electrode. Afterwards, the obtained gold nanofilm was applied in selective detection of dopamine (DA) in the presence of ascorbic acid (AA) at near neutral pH by DPV in the optimized conditions. The linear range for DA was 1.5–27.5 μM. The electrode also shows good stability during detection.
Co-reporter:Guang-Li Wang, Pei-Pei Yu, Jing-Juan Xu and Hong-Yuan Chen
The Journal of Physical Chemistry C 2009 Volume 113(Issue 25) pp:11142-11148
Publication Date(Web):June 2, 2009
DOI:10.1021/jp902069s
We demonstrate herein a newly developed lable-free photoelectrochemical immunosensor using a CdS quantum dots (QDs) multilayer film coupled with a biospecific interaction. The CdS QDs multilayer film was prepared by layer-by-layer assembling positively charged poly(dimethyldiallylammonium chloride) (PDDA) and thioglycolic acid (TGA)-capped water-soluble CdS QDs with negative charges on the surface of an indium−tin oxide (ITO) electrode. Ascorbic acid (AA) was exploited as an efficient and nontoxic electron donor for scavenging photogenerated holes under mild solution medium. The photoexcitation of CdS QDs modified electrode potentiostated at 0 V (vs. Ag/AgCl) in the presence of 0.1 M AA led to a stable anodic photocurrent. To perform the immunoassay, goat antimouse IgG was conjugated onto CdS QDs modified electrode by using the classic EDC coupling reactions between COOH groups on the surfaces of the TGA capped CdS QDs and NH2 groups of the antibody. The concentrations of mouse IgG were measured through the decrease in photocurrent intensity resulting from the increase in steric hindrances due to the formation of the immunocomplex. The synthetic conditions (different Cd/S ratio and different pH) of CdS QDs and the number of PDDA/CdS bilayers could influence the photoelectrochemical properties of CdS QDs modified electrodes used for immunosensor construction. Under the optimal conditions, a linear relationship between photocurrent decrease and mouse IgG concentration was obtained in the range of 10 pg/mL to 100 ng/mL with a detection limit of 8.0 pg/mL. This strategy opens a new perspective for the application of QDs, which might be of great significance for QDs in photoelectrochemical bioanalysis in the future.
Co-reporter:Yu-Hui Bai, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2009 Volume 24(Issue 10) pp:2985-2990
Publication Date(Web):15 June 2009
DOI:10.1016/j.bios.2009.03.008
We report a simple approach for the selectively electrochemical sensing of cysteine (CySH) using β-MnO2 nanowires modified glassy carbon (GC) electrode via a direct and facile electrochemical co-deposition process with chitosan hydrogel. The electrode showed excellent electrocatalytic effect toward cysteine oxidation. A possible reaction mechanism related to the formation of surface complexes was proposed: the –SH group is the reacting group in the reaction between cysteine and MnO2, while the –NH2 group acts as an anchor to stabilize the surface complexes. The electrocatalytic behavior is further developed as a sensitive detection scheme for cysteine by amperometric measurement, which shows a large determination range of 0.5–630 μM and a low detection limit of 70 nM. Other nineteen amino acids in a 20-fold concentration do not interfere in the detection of cysteine. Furthermore, other biological species containing –SH group or SS bonds, such as glutathione, cystine, and bovine serum albumin (BSA), show no interferences because of steric hindrance and inactive SS bonds.
Co-reporter:Guang-Li Wang, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2009 Volume 24(Issue 8) pp:2494-2498
Publication Date(Web):15 April 2009
DOI:10.1016/j.bios.2008.12.031
Dopamine-coordinated photoactive TiO2 nanoporous films with a wide excitation range of light in the visible region (up to 580 nm) were prepared and used for sensitive detection of NADH. Colloidal TiO2 was firstly covered on an indium–tin oxide (ITO) electrode surface and sintered at 450 °C to form a nanoporous TiO2 film, then the electrode was dipped in a dopamine solution to form a dopamine–TiO2 charge transfer complex via coordinating dopamine with undercoordinated titanium atoms on the electrode surface. This charge transfer complex provided an anodic photocurrent under visible light and the photocurrent could be largely enhanced by NADH. The photocurrent enhancement might be due to the electron transfer between NADH and the holes localized on dopamine. A new photoelectrochemical methodology for sensitive detection of NADH at a relatively low potential was developed. The detection limit of NADH was 1.4 × 10−7 M, and the detection range could extend up to 1.2 × 10−4 M. The dopamine–TiO2 modified electrode exhibits its major advantages such as effective electronic transducer, fast response and easy fabrication for photoelectrochemical determination of NADH. This strategy largely reduces the destructive effect of UV light and the photogenerated holes of illuminated TiO2 to biomolecules and opens a new avenue for the applications of TiO2 in photoelectrochemical biosensing.
Co-reporter:Pei-Yu Ge, Wei Zhao, Ying Du, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics 2009 Volume 24(Issue 7) pp:2002-2007
Publication Date(Web):15 March 2009
DOI:10.1016/j.bios.2008.10.009
Based on the newly discovered artificial enzyme formed by mixing hemin with supramolecular hydrogels via the self-assembly of amphiphilic oligopeptides, we prepared a novel organic phase artificial enzyme electrode by coating the artificial enzyme on an electrode which was then covered with sodium alginate for protection. Scanning electron micrograph showed that the supramolecular hydrogel kept its nanofibers structure on the electrode surface. Hemin dispersed in the supermolecular hydrogel as monomer greatly promotes its direct electrochemistry behavior in organic solvents. At the same time, this electrode exhibited higher electrocatalytic ability to tert-butyl hydroperoxide (TBHP) than free hemin modified electrode (free hemin mainly present as dimer). As low as 27 μM TBHP could be detected with a linear range from 6.6 × 10−5 to 1.27 × 10−2 M via amperometric method. The biosensor can reach 95% of the steady-state current in about 10 ± 2 s. More importantly, it can be applied in both hydrophilic and hydrophobic solvents without adding extra buffer or mediators to them that cannot be received by most traditional organic phase enzyme electrodes. This unique property greatly promotes the development of the organic phase enzyme electrodes by facilitating the detection of different kinds of substrates of the hemin-based artificial enzyme soluble in hydrophilic and hydrophobic solvents. The artificial enzyme electrode was successfully used to determine organic peroxides in body lotion samples.
Co-reporter:Guang-Li Wang, Jing-Juan Xu, Hong-Yuan Chen, Shou-Zhong Fu
Biosensors and Bioelectronics 2009 Volume 25(Issue 4) pp:791-796
Publication Date(Web):15 December 2009
DOI:10.1016/j.bios.2009.08.027
A novel photoelectrochemical immunosensor based on TiO2/CdS hybrid modified electrode was developed. The TiO2/CdS hybrid modified electrode was obtained by alternately dipping the TiO2 modified indium–tin oxide (ITO) electrode into the [Cd(NH3)4]2+ and S2− solution repeatedly. Compared with the routine method using Cd2+ solution for CdS deposition, the as obtained TiO2/CdS electrode showed enhanced photocurrent intensity with fewer coating times. After the ITO/TiO2/CdS electrode was coated with chitosan (CS), α-fetoprotein (AFP) antibodies were covalently conjugated on the surface of the electrode. Thus, a label-free photoelectrochemical immunosensor for the detection of AFP was developed by monitoring the changes in the photocurrent signals of the electrode resulting from the immunoreaction. The immunosensor displayed a linear response to AFP in the ranges from 50 pg/mL to 50 ng/mL with a relatively low detection limit of 40 pg/ml. The photoelectrochemical results for the detection of AFP in five human sera showed acceptable accuracy. The method is simple, sensitive and specific. Moreover, the studied immunosensor possessed acceptable reproducibility and storage stability. The proposed methodology was potentially attractive for clinical immunoassay.
Co-reporter:Qing Zhang, Jing-Juan Xu, Yan Liu and Hong-Yuan Chen  
Lab on a Chip 2008 vol. 8(Issue 2) pp:352-357
Publication Date(Web):14 Nov 2007
DOI:10.1039/B716295M
We presented a simple approach for in-situ synthesis of poly(dimethylsiloxane) (PDMS)–gold nanoparticles composite film based on the special characteristics of PDMS itself. It is an environmentally safe synthesis method without the requirement of additional reducing/stabilizing agents. The region where the resulting gold nanoparticles distribute (in the matrix or on the surface of the polymer) and the size of the nanoparticles, as well as the colour of the free-standing films, can be simply controlled by adjusting the ratio of curing agent and the PDMS monomer. The chemical and optical properties of these composite films were studied. Using such a method, gold nanoparticle micropatterns on PDMS surfaces can be performed. And based on the gold nanoparticles micropattern, further modification with antibodies, antigens, enzymes and other biomolecules can be achieved. To verify this ability, an immobilized glucose oxidase (GOx) reactor in microchannels was built and its performance was studied. The experiments have shown that the resulting composite film may have a lot of potential merits in protein immobilization, immunoassays and other biochemical analysis on PDMS microchips.
Co-reporter:Wei Zhao, Si-Xin Sun, Jing-Juan Xu, Hong-Yuan Chen, Xiao-Jian Cao and Xiao-Hong Guan
Analytical Chemistry 2008 Volume 80(Issue 10) pp:3769
Publication Date(Web):March 26, 2008
DOI:10.1021/ac702395c
We report a simple electrochemical method for the identification of properties of peripheral nerve fibers, based on the detection of a neurotransmitter enzyme, acetylcholinesterase (AChE). A poly(diallydimethylammonium) (PDDA) adulterated poly(dimethylsiloxane) (PDMS) film is spin-coated on the surface of gold electrodes. Gold nanoparticles (AuNPs) are in situ synthesized on the polymer film, which act as “electron antennae” between the film and the electrode surface and also provide a biocompatible interface. This PDMS−PDDA/AuNPs film shows different adsorption sites to choline oxidase (ChO) and AChE; after incubation with ChO, the polymer−gold nanocomposite film also shows excellent adsorption ability to AChE. Moreover the adsorption sites of AChE would not be blocked by bovine serum albumin (BSA) which provides a good platform for the quantitative amperometric determination of AChE via the oxidation of the enzymatically generated H2O2 in the bienzyme system in the presence of acetylcholine. The detection limit is down to 1.0 unit/mL. The polymer−gold nanocomposite film shows excellent anti-interference ability to the coexistent electroactive substances such as ascorbic acid. Thus it was applied to determine AChE in peripheral nerve fibers homogenates and identify the motor and sensory fibers for the first time. Compared with histochemical staining methods, the electrochemical technique shows good accurate rate and faster response, which has good potential for a clinical application.
Co-reporter:Hui Zhang, Xue Zhong, Jing-Juan Xu and Hong-Yuan Chen
Langmuir 2008 Volume 24(Issue 23) pp:13748-13752
Publication Date(Web):November 7, 2008
DOI:10.1021/la8028935
Uniform Fe3O4 nanospheres with a diameter of 100 nm were rapidly prepared using a microwave solvothermal method. Then Fe3O4/polypyrrole (PPy) composite nanospheres with well-defined core/shell structures were obtained through chemical oxidative polymerization of pyrrole in the presence of Fe3O4; the average thickness of the coating shell was about 25 nm. Furthermore, by means of electrostatic interactions, plentiful gold nanoparticles with a diameter of 15 nm were assembled on the surface of Fe3O4/PPy to get Fe3O4/PPy/Au core/shell/shell structure. The morphology, structure, and composition of the products were characterized by transmission electronic microscopy (TEM), scanning electronic microscopy (SEM), X-ray powder diffraction (XRD), and Fourier transform infrared (FT-IR) spectroscopy. The resultant nanocomposites not only have the magnetism of Fe3O4 nanoparticles that make the nanocomposites easily controlled by an external magnetic field but also have the good conductivity and excellent electrochemical and catalytic properties of PPy and Au nanoparticles. Furthermore, the nanocomposites showed excellent electrocatalytic activities to biospecies such as ascorbic acid (AA).
Co-reporter:Xiao-Fei Wang, Jing-Juan Xu and Hong-Yuan Chen
The Journal of Physical Chemistry C 2008 Volume 112(Issue 45) pp:17581-17585
Publication Date(Web):2017-2-22
DOI:10.1021/jp807136s
ZnS nanocrystals are less toxic than cadmium chalcogenide materials, which might have more applications in biological detection. Yet more excitation energy during its electrochemiluminescence (ECL) process should be applied because of the wide energy gap (∼3.7 eV) of ZnS. Here, ECL of ZnS doped with Mn2+ nanocrystals (ZnS:Mn2+ NCs) modified on glassy carbon electrode was investigated in aqueous solution with the coreactant hydrogen peroxide (H2O2) for the first time. Besides the ECL process of pure ZnS NCs at a negative potential of more than −2.0 V vs SCE, a new ECL emission peak was observed at ca. −1.50 V vs SCE on the ZnS:Mn2+ NCs-modified glassy carbon electrode in pH 9.0 phosphate buffer solution. This new ECL emission was attributed to the excited state of Mn2+ lying in the Zn2+ sites. The concentration of Mn2+ doped in ZnS NCs played a key role in this new ECL process. Furthermore, this specific ECL emission was dependent on the concentration of H2O2. The largely decreased excitation energy of this new ECL emission would promote the application of doped ZnS NCs in the fields of biological and environmental analysis without the interference of hydrogen bubble in the ECL process.
Co-reporter:Yu-Hui Bai, Hui Zhang, Jing-Juan Xu and Hong-Yuan Chen
The Journal of Physical Chemistry C 2008 Volume 112(Issue 48) pp:18984-18990
Publication Date(Web):2017-2-22
DOI:10.1021/jp805497y
Manganese dioxides of different crystalline structures with different dimensionality (amorphous MnO2 nanoparticles, α-MnO2 nanoparticles, and β-MnO2 nanowires) were synthesized, characterized, and evaluated for their electrocatalytic activity to H2O2. Via a direct and facile electrochemical deposition method, MnO2 nanomaterials were codeposited onto glassy carbon (GC) electrodes with chitosan hydrogel. The catalytic oxidation current of amorphous MnO2 nanoparticles per unit mass to H2O2 is much larger than that of α-MnO2 nanoparticles and β-MnO2 nanowires; however, the catalytic oxidation current of amorphous MnO2 per unit surface area to H2O2 is the same as that of α-MnO2 nanoparticles and much less than that of one-dimensional β-MnO2 nanowires. The bicatalytic activity toward H2O2 of the electrodes modified with three different nanomaterials increases in the following order: amorphous MnO2 > α-MnO2 > β-MnO2. Further codeposition of chitosan hydrogel, choline oxidase (ChOx), and different MnO2 nanomaterials onto GC electrodes was applied to form choline biosensors. The biosensors modified with crystalline MnO2 respond to choline far more quickly than that modified with amorphous MnO2 in amperometric measurements. For the same concentration of choline, the response time is 8 s, 25 s, and 5 min for biosensors modified with β-MnO2, α-MnO2, and amorphous MnO2, respectively. The reasons for these phenomena were discussed in detail from the differences of the specific surface areas, the amounts of entrapped MnO2 on electrodes, crystalline structures, and dimensionality. The biosensors based on α-MnO2 nanoparticles and β-MnO2 nanowires were applied on amperometric detections of choline chloride with the linear ranges of 2.0 × 10−6−5.8 × 10−4 M and 1.0 × 10−6−7.9 × 10−4 M with the detection limits of 1.0 and 0.3 μM, respectively.
Co-reporter:Xin-Ai Li, Dong-Mei Zhou, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2008 Volume 75(Issue 1) pp:157-162
Publication Date(Web):15 March 2008
DOI:10.1016/j.talanta.2007.10.054
In this work, chloride, chlorate and perchlorate are fast separated on PDMS microchip and detected via in-channel indirect amperometric detection mode. With PDMS/PDMS microchip treated by oxygen plasma, anions chloride (Cl−), chlorate (ClO3−), and perchlorate (ClO4−) are separated within 35 s. Some parameters including buffer salt concentration, buffer pH, separation voltage and detection potential are investigated in detail. The separation conditions using 15 mM (pH 6.12) of 2-(N-morpholino)ethanesulfonic acid (MES) + l-histidine (l-His) as running buffer, −2000 V as separation voltage and 0.7 V as detection potential are optimized. Under this condition, the detection limits of Cl−, ClO3−, and ClO4− are 1.9, 3.6, and 2.8 μM, respectively.
Co-reporter:Xin-Ai Li, Dong-Mei Zhou, Jing-Juan Xu, Hong-Yuan Chen
Talanta 2007 Volume 71(Issue 3) pp:1130-1135
Publication Date(Web):28 February 2007
DOI:10.1016/j.talanta.2006.06.009
In-channel indirect amperometric detection mode for microchip capillary electrophoresis with positive separation electric field is successfully applied to some heavy metal ions. The influences of separation voltage, detection potential, the concentration and pH value of running buffer on the response of the detector have been investigated. An optimized condition of 1200 V separation voltage, −0.1 V detection potential, 20 mM (pH 4.46) running buffer of 2-(N-morpholino)ethanesulfonic acid (MES) + l-histidine (l-His) was selected. The results clearly showed that Pb2+, Cd2+, and Cu2+ were efficiently separated within 80 s in a 3.7 cm long native separation PDMS/PDMS channel and successfully detected at a single carbon fibre electrode. The theoretical plate numbers of Pb2+, Cd2+, and Cu2+ were 1.2 × 105, 2.5 × 105, and 1.9 × 105 m−1, respectively. The detection limits for Pb2+, Cd2+, and Cu2+ were 1.3, 3.3 and 7.4 μM (S/N = 3).
Co-reporter:Jing-Juan Xu, Wei Zhao, Xi-Liang Luo and Hong-Yuan Chen  
Chemical Communications 2005 (Issue 6) pp:792-794
Publication Date(Web):23 Dec 2004
DOI:10.1039/B416548A
A sensitive enzyme-based FET biosensor for lactate has been obtained by introducing MnO2 nanoparticles at the gate surface via a layer-by-layer assembling method.
Co-reporter:Yuan-Cheng Zhu, Fei Xu, Nan Zhang, Wei-Wei Zhao, Jing-Juan Xu, Hong-Yuan Chen
Biosensors and Bioelectronics (15 May 2017) Volume 91() pp:
Publication Date(Web):15 May 2017
DOI:10.1016/j.bios.2016.12.045
•Ag@Au asymmetric core–satellite nanoassembly was fabricated.•It was then applied for the novel energy-transfer-based PEC immunoassay.•The proposed format could serve as a general basis for PEC bioanalysis.This work reports the use of compositionally heterogeneous asymmetric Ag@Au core–satellite nanoassembly functionalized with DNA sequence as unique signaling nanoprobes for the realization of new energy-transfer-based photoelectrochemical (PEC) immunoassay of prostate- specific antigen (PSA). Specifically, the Ag@Au asymmetric core–satellite nanoassemblies (Ag@Au ACS) were fabricated on a two-dimensional glass substrate by a modified controlled assembly technique, and then functionalized with DNA sequences containing PSA aptamers as signaling nanoprobes. Then, the sandwich complexing between the PSA, its antibodies, and the signaling nanoprobes was performed on a CdS QDs modified indium tin oxide (ITO) electrode. The single stranded DNA can server as a facile mediator that place the Ag@Au ACS in proximity of CdS QDs, stimulating the interparticle exciton–plasmon interactions between Ag@Au ACS and CdS QDs and thus quenching the excitonic states in the latter. Since the damping effect is closely related to the target concentration, a novel energy-transfer-based PEC bioanalysis could be achieved for the sensitive and specific PSA assay. The developed biosensor displayed a linear range from 1.0×10−11 g mL−1 to 1.0×10−7 g mL−1 and the detection limit was experimentally found to be of 0.3×10–13 g mL−1. This strategy used the Ag@Au ACS-DNA signaling nanoprobes and overcame the deficiency of short operating distance of the energy transfer process for feasible PEC immunoassay. More significantly, it provided a way to couple the plasmonic properties of the Ag NPs and Au NPs in a single PEC bioanalytical system. We expected this work could inspire more interests and further investigations on the advanced engineering of the core–satellite or other judiciously designed nanostructures for new PEC bioanalytical uses with novel properties.
Co-reporter:Guang-Sheng Qian, Ting-Ting Zhang, Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2017 - vol. 53(Issue 34) pp:NaN4713-4713
Publication Date(Web):2017/03/31
DOI:10.1039/C7CC00626H
Plasmon rulers (PRs) exploit the potential of plasmon coupling between individual pairs of noble metal nanoparticles in biological processes, especially single-molecule detection. Herein, for the first time, we report a strategy based on Ag PRs for in situ monitoring of the extension process of telomerase primer (TSP) activated by a single telomerase.
Co-reporter:Ting-Ting Zhang, Fan Yang, Xiang-ling Li, Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2017 - vol. 53(Issue 41) pp:NaN5617-5617
Publication Date(Web):2017/05/02
DOI:10.1039/C7CC02834B
A multifunctional Ag NP based nanocomposite was fabricated which realized accurate targeting of specific cancer cells and completely initiative therapy without any photoexcitation.
Co-reporter:Bin Kang, Shan-Shan Li, Qi-Yuan Guan, Ai-Ping Chen, Pan-Ke Zhang, Li-Bin Zhang, Ji-Wu Wei, Jing-Juan Xu and Hong-Yuan Chen
Chemical Science (2010-Present) 2017 - vol. 8(Issue 2) pp:NaN1250-1250
Publication Date(Web):2016/10/03
DOI:10.1039/C6SC02486F
Apoptosis and necrosis are distinct cell death processes related to many cellular pathways. In situ, quantitatively and dynamically monitoring such processes may provide vitally important information for cell studies. However, such a method still remains elusive, even though current immunochemical methodologies have developed extremely valuable tools. Herein, we demonstrate Raman spectroscopic metrics for validating and quantifying apoptotic and necrotic cells based on their distinct molecular vibrational fingerprints. It not only allows us to quantify apoptotic and necrotic cell populations in situ in adherent cell samples, but also to be capable of continuously monitoring the dynamical processes of apoptosis and necrosis at the same time in one sample. This method provides comparable results with the “gold standard” of flow cytometry, moreover, with several incomparable advantages. Our work offers a powerful new tool for cell apoptosis and necrosis assays and is expected to become a benchmark technology in biological and medical studies.
Co-reporter:Zheng-Yuan Ma, Yi-Fan Ruan, Nan Zhang, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2015 - vol. 51(Issue 39) pp:NaN8384-8384
Publication Date(Web):2015/03/31
DOI:10.1039/C5CC01832C
Based on the assay of DNA binding proteins upon visible light irradiation, a photoelectrochemical sensor was constructed for successfully probing a DNA–protein interaction for the first time.
Co-reporter:Zong-Hua Wang, Cai-Yu Lu, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2014 - vol. 50(Issue 10) pp:NaN1180-1180
Publication Date(Web):2013/11/26
DOI:10.1039/C3CC48356H
A dual-functional electrochemical biosensor for adenosines and hydrogen peroxide from cancer cells was developed based on a traditional switchable electrochemical sensing format and ATP improved G-quadruplex DNAzyme as a biolabel.
Co-reporter:Fei Xu, Yuan-Cheng Zhu, Zheng-Yuan Ma, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2016 - vol. 52(Issue 14) pp:NaN3037-3037
Publication Date(Web):2016/01/14
DOI:10.1039/C5CC09963C
Using single stranded DNA (ssDNA) as a distance controller and Au nanoparticles (NPs) functionalized with ssDNA as novel energy-transfer nanoprobes, an ultrasensitive energy-transfer based photoelectrochemical protein biosensor was realized.
Co-reporter:Zheng-Yuan Ma, Jian-Bin Pan, Cai-Yu Lu, Wei-Wei Zhao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2014 - vol. 50(Issue 81) pp:NaN12090-12090
Publication Date(Web):2014/08/12
DOI:10.1039/C4CC05373G
Using CdS QD-tagged mercury-specific oligonucleotides, a novel folding-based photoelectrochemical sensor has been successfully fabricated for reagentless and highly sensitive Hg2+ detection.
Co-reporter:Yingshu Guo, Jia liu, Guangxu Yang, Xiaofeng Sun, Hong-Yuan Chen and Jing-Juan Xu
Chemical Communications 2015 - vol. 51(Issue 5) pp:NaN865-865
Publication Date(Web):2014/11/20
DOI:10.1039/C4CC08428D
A conveniently amplified DNAzyme-based fluorescence strategy was designed for highly sensitive detection of ATP or reduced thiol based on the introduction of an ATP aptamer or a disulfide bond in the bioconjugates of magnetic nanoparticles (MNP) and polystyrene microsphere–DNAzyme complexes (PSM–DNAzyme).
Co-reporter:Mei-Sheng Wu, Xiao-Tao Sun, Meng-Jiao Zhu, Hong-Yuan Chen and Jing-Juan Xu
Chemical Communications 2015 - vol. 51(Issue 74) pp:NaN14075-14075
Publication Date(Web):2015/07/29
DOI:10.1039/C5CC06229B
A mesoporous silica film-assisted amplification method is reported for the first time for the sensitive electrochemiluminescence detection of cancer cells.
Co-reporter:Nan Hao, Pan-Pan Dai, Tao Yu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2015 - vol. 51(Issue 70) pp:NaN13507-13507
Publication Date(Web):2015/07/13
DOI:10.1039/C5CC05350A
A dual target-recycling amplification strategy for sensitive detection of microRNAs based on duplex-specific nuclease and catalytic hairpin assembly was reported for the first time.
Co-reporter:Wei-Wei Zhao, Xiao-Ya Dong, Jing Wang, Fen-Ying Kong, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 43) pp:NaN5255-5255
Publication Date(Web):2012/01/23
DOI:10.1039/C2CC17942C
A new photoelectrochemical immunoassay for prostate-specific antigen (PSA) was successfully developed with high sensitivity via immunogold labeling.
Co-reporter:Meng Xiong, Nan Hao, Tao Yu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2014 - vol. 50(Issue 71) pp:NaN10306-10306
Publication Date(Web):2014/07/14
DOI:10.1039/C4CC04410J
An ideal nanoporous poly(N-isopropylacrylamide) membrane has been fabricated in glass microchannels by means of spatially controlled photopatterning technology for a high level of enrichment and cleanup of nucleic acids.
Co-reporter:Qiu-Mei Feng, Jian-Bin Pan, Huai-Rong Zhang, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2014 - vol. 50(Issue 75) pp:NaN10951-10951
Publication Date(Web):2014/05/15
DOI:10.1039/C4CC03102D
A disposable paper-based bipolar electrode (BPE) was reported for the first time for the sensitive electrochemiluminescence detection of a prostate specific antigen (PSA).
Co-reporter:Nan Hao, Xiang-Ling Li, Huai-Rong Zhang, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2014 - vol. 50(Issue 94) pp:NaN14830-14830
Publication Date(Web):2014/10/08
DOI:10.1039/C4CC06801G
A ratiometric electrochemiluminescent biosensor for the detection of microRNAs based on cyclic enzyme amplification and distance dependent resonance energy transfer was reported for the first time.
Co-reporter:Huai-Rong Zhang, Yin-Zhu Wang, Mei-Sheng Wu, Qiu-Mei Feng, Hai-Wei Shi, Hong-Yuan Chen and Jing-Juan Xu
Chemical Communications 2014 - vol. 50(Issue 83) pp:NaN12577-12577
Publication Date(Web):2014/08/29
DOI:10.1039/C4CC06302C
A novel visual electrochemiluminescence (ECL) analysis strategy for detection of telomerase activity is reported on a microarray chip, with G-quadruplex deoxyribozyme (DNAzyme) and luminol modified Au nanoparticles (NPs) as double-catalytic amplification labels.
Co-reporter:Fen-Ying Kong, Bi-Yi Xu, Ying Du, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2013 - vol. 49(Issue 11) pp:NaN1054-1054
Publication Date(Web):2012/11/12
DOI:10.1039/C2CC37675J
A branched electrode platform was proposed for label-free and reagentless simultaneous tumor markers detection based on different redox substrates.
Co-reporter:Li-Jing He, Mei-Sheng Wu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2013 - vol. 49(Issue 15) pp:NaN1541-1541
Publication Date(Web):2013/01/04
DOI:10.1039/C2CC38508B
A reusable potassium ion biosensor was reported for the first time based on the reversible DNA structural change and the interaction between surface plasmons of Au nanoparticles (NPs) and the ECL emission of CdS nanocrystals (NCs).
Co-reporter:Hong Zhou, Yan-Yan Zhang, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2013 - vol. 49(Issue 22) pp:NaN2248-2248
Publication Date(Web):2013/02/01
DOI:10.1039/C3CC38990A
Based on the K-doped graphene–CdS:Eu NC composites and the nicking endonuclease (NEase) assisted strand-scission cycle, we have developed an ultrasensitive and selective electrochemiluminescence (ECL) DNA biosensor using the G-quadruplex–hemin-based DNAzyme which acts as an electrocatalyst for the reduction of H2O2, the coreactant of CdS:Eu NCs ECL.
Co-reporter:Jing Liu, Cai-Yu Lu, Hong Zhou, Jing-Juan Xu, Zong-Hua Wang and Hong-Yuan Chen
Chemical Communications 2013 - vol. 49(Issue 59) pp:NaN6604-6604
Publication Date(Web):2013/06/03
DOI:10.1039/C3CC43532F
A new dual-functional electrochemical biosensor for the detection of prostate specific antigen (PSA) and telomerase activity was successfully developed based on a sandwich immunobinding format and telomerization assisted hemin–G-quadruplex-based DNAzyme as a biolabel.
Co-reporter:Mei-Sheng Wu, Hai-Wei Shi, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2011 - vol. 47(Issue 27) pp:NaN7754-7754
Publication Date(Web):2011/05/26
DOI:10.1039/C1CC12219C
In this paper, an electrochemiluminescence resonance energy transfer (ECL-RET) system from CdS quantum dot to Ru(bpy)32+ was developed for the first time. By the signal amplification of Ru(bpy)32+ and the specific antibody–cell surface interactions, this ECL-RET system could sensitively respond down to 12.5 SMMC-7721 cells per mL.
Co-reporter:Wei-Wei Zhao, Chun-Yuan Tian, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 6) pp:NaN897-897
Publication Date(Web):2011/11/18
DOI:10.1039/C1CC16775H
Visible light-activated localized surface plasmon resonance-based photoelectrochemical detection is reported for the first time.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2009(Issue 8) pp:NaN907-907
Publication Date(Web):2009/01/16
DOI:10.1039/B821049G
The quenching of electrochemiluminescence (ECL) from a CdS:Mn nanocrystal film by proximal Au nanoparticles was observed as a result of Förster energy transfer, while an enhancement of ECL takes place after hybridization with target DNA due to the energy transfer of ECL excited surface plasmon resonances in AuNPs to the CdS:Mn NCs at large separation, based on which an ultrasensitive and specific DNA biosensor was constructed.
Co-reporter:Jing Wang, Wei-Wei Zhao, Xiao-Rong Li, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 51) pp:NaN6431-6431
Publication Date(Web):2012/05/10
DOI:10.1039/C2CC32767H
Based on the amplified signal from SiO2@CdS nanocomposites integrated with K-doped graphene, a new electrochemiluminescence biosensor was developed for the successful detection of transcription factor TATA-binding protein (TBP).
Co-reporter:Chun-Yuan Tian, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 66) pp:NaN8236-8236
Publication Date(Web):2012/06/27
DOI:10.1039/C2CC34229D
The highly enhanced electrochemiluminescence from a nitrogen doped TiO2 nanotube array has been reported for the first time, and successfully applied to develop an ultrasensitive ECL aptasensor for the detection of adenosine in cancer cells.
Co-reporter:Wei-Wei Zhao, Long Zhang, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 76) pp:NaN9458-9458
Publication Date(Web):2012/07/11
DOI:10.1039/C2CC34543A
A robust and specific photoelectrochemical approach for cell surface carbohydrates evaluation was achieved firstly based on carboxylic-group-containing free-base-porphyrin bridged 3-aminophenylboronic acid and a titania biosensing interface.
Co-reporter:Bi-Yi Xu, Zhe-Qin Yang, Jing-Juan Xu, Xing-Hua Xia and Hong-Yuan Chen
Chemical Communications 2012 - vol. 48(Issue 95) pp:NaN11637-11637
Publication Date(Web):2012/09/13
DOI:10.1039/C2CC35986C
Continuous CaCO3 hollow nanoparticle generation at room temperature with simultaneous molecule doping is realized on a liquid–gas dual phase microfluidic system.
Co-reporter:Jing Liu, Hong Zhou, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2011 - vol. 47(Issue 15) pp:NaN4390-4390
Publication Date(Web):2011/03/09
DOI:10.1039/C1CC10430F
A novel switch-cytosensing strategy has been designed, which is based on the changes of electron transfer efficiency between ferrocene at the end of DNA and the electrode surface before and after cell transfection. This strategy provided a general and convenient method to fabricate efficient electrochemical cell sensors.
Co-reporter:Wei-Wei Zhao, Jing Wang, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2011 - vol. 47(Issue 39) pp:NaN10992-10992
Publication Date(Web):2011/09/12
DOI:10.1039/C1CC13952E
This work is the first report on the energy transfer between CdS quantum dots and Au nanoparticles for photoelectrochemical biosensing applications.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2010 - vol. 46(Issue 28) pp:NaN5081-5081
Publication Date(Web):2010/06/17
DOI:10.1039/C0CC00837K
Efficient electrochemiluminescence (ECL) quenching was achieved by functionalized CdTe quantum dots (QDs) through ECL energy scavenging, based on which ultrasensitive antigen detection could be realized.
Co-reporter:Yun Shan, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2010 - vol. 46(Issue 23) pp:NaN4189-4189
Publication Date(Web):2010/05/11
DOI:10.1039/C003124K
This work firstly reports an opto–magnetic interaction–induced enhancement of electrochemiluminescence (ECL) from CdS:Mn nanocrystals (NCs) film by superparamagnetic Fe3O4 nanoparticles and its application to sensitive immunosensing.
Co-reporter:Kai Zhang;Xue-Jiao Yang;Wei Zhao;Ming-Chen Xu;Hong-Yuan Chen
Chemical Science (2010-Present) 2017 - vol. 8(Issue 7) pp:
Publication Date(Web):2017/06/26
DOI:10.1039/C7SC00909G
Regulation of gene expression is highly important in the area of cell biology. In this work a novel convenient and versatile strategy is reported which permits both gene regulation and imaging in living cells. An oligonucleotide-based biomimetic probe was designed to target an RNA-induced silencing complex (RISC) and served as an agent for the modulation of c-Myc protein expression in living cells through regulating the RNA interference (RNAi) pathway. In this probe, a DNA strand (Strand1) serving as the frame was immobilized on a AuNP with a thiol group at the 5′ end. Strand2, designed to recognize the target RISC with an RNA fragment, was hybridized with the complementary sequence of Strand1. In the original state, the fluorescence of the Cy3 modifier at the 5′ end of Strand2 was quenched by both the AuNP and BHQ2, which labelled the 3′ end of Strand1. In the presence of RISC, Strand2 was cleaved, resulting in a shorter oligo part with a corresponding lower melting temperature than that of the original full-length Strand2. The shorter oligonucleotide strand containing the Cy3 fluorophore was released, accompanied by a recovered fluorescence signal. Through evaluating the fluorescence intensity, the competition for RISC was dynamically monitored in single cells. Furthermore, capturing RISC by this probe resulted not only in restored fluorescence intensity but also increased c-Myc oncogene expression. Hence, gene expression could be selectively and precisely regulated and imaged via the RISC targeting probe. The synthetic method for the biomimetic probe is universally applicable, and facilitates the fundamental study of RNAi pathways, or development of a gene regulation strategy without cytokine activation. The gene regulation and imaging strategy will accelerate the unveiling of the basic role of the RISC cleavage interaction, the mystery of RNA-silencing and therapeutic monitoring of cancer.
Co-reporter:Xiang-Ling Li, Zhuo-Lei Zhang, Wei Zhao, Xing-Hua Xia, Jing-Juan Xu and Hong-Yuan Chen
Chemical Science (2010-Present) 2016 - vol. 7(Issue 5) pp:NaN3263-3263
Publication Date(Web):2016/02/04
DOI:10.1039/C5SC04369G
Due to the complexity of biological systems and the ultralow concentration of analytes, improving the signal-to-noise ratio and lowering the limit of detection to allow highly sensitive detection is key to biomolecule analysis, especially intracellular analysis. Here, we present a method for highly sensitive imaging of mRNA in living cells by using novel invisible oriented probes to construct a turn-on signal generation mechanism from zero background. Two DNA probes (S1 and S2) are asymmetrically modified on two small gold nanoparticles (AuNPs) with a diameter of 20 nm. The hybridization of the two DNA probes with a single target mRNA leads to the formation of an AuNP dimer which shows a prominent plasmonic coupling effect. It generates a strong scattering signal from zero-background under a dark-field spectral analysis system. The unique design of the oriented assembly dimer has the ability to easily discriminate the target signal from the inherent cellular background noise in intracellular detection, thus making this approach a valuable technique for imaging single survivin mRNA and monitoring the distribution of survivin mRNA in tumor cells.
Co-reporter:Mei-Sheng Wu, Da-Jing Yuan, Jing-Juan Xu and Hong-Yuan Chen
Chemical Science (2010-Present) 2013 - vol. 4(Issue 3) pp:NaN1188-1188
Publication Date(Web):2012/12/21
DOI:10.1039/C2SC22055E
Rapid and sensitive detection of tumor biomarkers plays a critical role in the early diagnosis of cancer and better understanding of disease progression. We report here a novel wireless electrochemiluminescence (ECL) strategy for visualizing prostate-specific antigen (PSA) on the basis of electrical switch control of ECL generation on bipolar electrodes (BPEs). The visual device comprises a two-channel microfluidic chip with two indium tin oxide (ITO) bands with a gap of 200 μm. The gap between the two ITO bands in one channel could be regarded as an electrical switch, the conductivity of which controls ECL generation on the ITO bands in the other channel, which are used as bipolar electrodes (BPEs). The electronic conductivity of the electrical switch could be tuned by PSA guided silver particles deposition via an immunosandwich assembly and a silver enhancement strategy. At the “on” state of the electrical switch, PSA induced deposition of silver particles forms an electronic circuit between the adjacent BPEs and makes them behave like a continuous H-shaped BPE, which results in only one ECL signal. Meanwhile, the external voltage for driving the oxidation reactions of Ru(bpy)32+ and TPA is significantly reduced compared with the “off” state. This important characterization of the electrical switch could eliminate the background signal and enable a sensitive measurement of PSA by observing the ECL lightspots on BPEs, providing a simple and sensitive visual means of detecting cancer biomarkers. Besides, this two-channel design avoids the chemical interference between sensing and reporting reactions. Combining the advantages of BPE and the high visual sensitivity of the electrical switch, it could be easily expected to achieve sensitive screening of other biomarkers.
Co-reporter:Xiao-Rong Li, Ming-Chen Xu, Hong-Yuan Chen and Jing-Juan Xu
Journal of Materials Chemistry A 2015 - vol. 3(Issue 21) pp:NaN4362-4362
Publication Date(Web):2015/04/21
DOI:10.1039/C5TB00312A
Bimetallic Au@Pt@Au triple-layered core–shell nanoparticles consisting of a Au core, Pt inner shell, and an outer shell composed of Au protuberances on graphene oxide (GO) nanosheets were successfully prepared by a galvanic replacement and reagent reduction reaction. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and cyclic voltammetry (CV) were employed to characterize the GO-supported Au@Pt@Au (GO/Au@Pt@Au) nanocomposites. The as-prepared catalyst has peroxidase-like activity, allowing it to express high electrocatalytic ability in hydrogen peroxide (H2O2) oxidation and reduction, thus leading to a highly sensitive H2O2 bi-directional amperometric sensing. The bi-directional sensor showed a linear range from 0.05 μM to 17.5 mM with a detection limit of 0.02 μM (S/N = 3) at an applied potential of +0.5 V and a linear range from 0.5 μM to 110 mM with a detection limit of 0.25 μM (S/N = 3) at an applied potential of −0.3 V. The proposed sensor was tested to determine H2O2 released from living cells and shows good application potential in biological electrochemistry.
Co-reporter:Xiao-Rong Li, Xiang-Ling Li, Ming-Chen Xu, Jing-Juan Xu and Hong-Yuan Chen
Journal of Materials Chemistry A 2014 - vol. 2(Issue 6) pp:NaN1703-1703
Publication Date(Web):2013/10/31
DOI:10.1039/C3TA14276K
Gold nanodendrites (AuNDs) monodispersed on graphene oxide (GO) nanosheets were successfully prepared using a clean synthesis method at room temperature and then applied for advanced oxygen reduction reaction (ORR). Herein, GO was used as the electron donors for reducing AuCl4− instead of any additional reductants and surfactants, leading to AuNDs with excellent monodispersity, uniformity and purity. The as-prepared AuNDs-loaded GO (AuNDs–GO) exhibit high electrocatalytic activity and a dominant four-electron pathway toward ORR. The AuNDs–GO also exhibit superior stability and methanol tolerance to a commercial Pt–C catalyst, making it a promising nanoelectrocatalyst in fuel cells and other electrochemical devices. This simple, straightforward, and general method is of significance for preparing high-performance metal nanocatalysts with a well-controlled morphology on appropriate supporting materials.
Co-reporter:Peng Wu, Chaoying Xu, Xiandeng Hou, Jing-Juan Xu and Hong-Yuan Chen
Chemical Science (2010-Present) 2015 - vol. 6(Issue 8) pp:NaN4450-4450
Publication Date(Web):2015/05/21
DOI:10.1039/C5SC01497B
Fingerprints are a unique characteristic of an individual. Recently, it has been realized that fingerprints carry more information about individuals than just their identity, for example, they may identify potential addicts and terrorists carrying explosives. Therefore, the development of imaging moieties capable of both fingerprint staining and drug/explosive visualization is of significant importance for forensic chemistry. Here we developed a nanohybrid comprising green- and red-emitting QDs for simultaneous fingerprint imaging and TNT visualization in fingerprints. The red-emitting Cu-doped ZnCdS (Cu–ZnCdS) QDs were embedded into silica nanoparticles and the green-emitting ZnCdS QDs were anchored onto the surface of the silica nanoparticles and further functionalized with polyallylamine (PAA). Both components of the nanohybrid, i.e., the PAA-functionalized green QDs and red QD-doped silica nanoparticles, could be explored for fingerprint imaging. Due to the formation of a Meisenheimer complex between TNT and PAA, the green-emitting QDs could be quenched by TNT, meanwhile the red-emitting QDs were inert. Therefore, the nanohybrid exhibited a traffic light-type fluorescence color change (green-yellow-red) to TNT concentration in the range of 40–400 μM. This method is promising for potential applications in security-screening needs in public areas such as airports and train stations.
Co-reporter:Hong Zhou, Jing Liu, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2011 - vol. 47(Issue 29) pp:NaN8360-8360
Publication Date(Web):2011/06/21
DOI:10.1039/C1CC12413G
We report here an ultrasensitive DNA detection approach which combines Au NPs enhanced electrochemiluminescence (ECL) of the CdS nanocrystal (NC) film with isothermal circular amplification reaction of polymerase and nicking endonuclease (NEase). By the double-signal amplification, this approach could sensitively respond down to 5 aM DNA.
Co-reporter:Linfeng Sheng, Lesi Cai, Jie Liu, Sichun Zhang, Jing-Juan Xu, Xinrong Zhang and Hong-Yuan Chen
Chemical Science (2010-Present) 2017 - vol. 8(Issue 1) pp:NaN754-754
Publication Date(Web):2016/09/12
DOI:10.1039/C6SC02610A
Metabolic azide amino acid labelling followed by the use of bioorthogonal chemistry is an efficient technique for imaging newly synthesized proteins. Recently, AHA-labelling together with the proximity-ligation assay was used to identify newly synthesized proteins of interest (POI) (Tom Dieck et al., Nat. Meth. 2015, 12, 411). Here we build on this study replacing the proximity-ligation assay with FRET to improve the spatial resolution. Herein, we develop a FRET-based strategy for imaging the newly synthesized endogenous POI within cells: a FRET acceptor is installed onto the newly synthesized proteins via click chemistry, and a FRET donor onto the POI via immunocytochemistry. We found that a photobleaching based FRET efficiency imaging mode and a fluorescence lifetime imaging mode showed the distribution of newly synthesized proteins more accurately compared to the direct observation of FRET signals. We demonstrated the capability of this FRET-based imaging method by visualizing several newly synthesized proteins including TDP-43, tubulin and CaMKIIα in different cell lines. This novel analytical imaging method could be used to visualize other specific endogenous proteins of interest in situ.
Co-reporter:Jing Wang, Xiang-Ling Li, Jia-Dong Zhang, Nan Hao, Jing-Juan Xu and Hong-Yuan Chen
Chemical Communications 2015 - vol. 51(Issue 58) pp:NaN11676-11676
Publication Date(Web):2015/06/09
DOI:10.1039/C5CC03693C
Using the DNA bio-gate and duplex-specific nuclease assisted target recycling, a facile electrochemiluminescence assay was developed for the sensitive detection of survivin mRNA.
Immunoglobulin E
Benzonitrile,4-mercapto-
2,3,5,6-tetramethylbiphenyl-4,4'-diamine
6-Benzothiazolesulfonicacid, 2,2'-(1,2-hydrazinediylidene)bis[3-ethyl-2,3-dihydro-
Streptavidin
Thrombin
EC 1.1.3.4
2-(3,6-Diacetoxy-2,7-dichloro-9H-xanthen-9-yl)benzoic acid
Benzenesulfonic acid,4-[2-[4-(dimethylamino)phenyl]diazenyl]-