Co-reporter:Shuai Chen, Yue Quan, Yong-Liang Yu, and Jian-Hua Wang
ACS Biomaterials Science & Engineering March 13, 2017 Volume 3(Issue 3) pp:313-313
Publication Date(Web):January 24, 2017
DOI:10.1021/acsbiomaterials.6b00644
We report the first attempt of using graphene quantum dot–Ag nanoparticles (GQD/AgNP hybrids) as oxidase mimics and antibacterial agents. Unlike previous silver- and graphene-based materials, the GQD/AgNP hybrids exhibit a high oxidase-like catalytic activity and possess favorable stability in neutral medium within the range from room temperature to 60 °C. In accordance with their prominent enzyme activities, the GQD/AgNP hybrids show excellent antibacterial properties against Gram-negative and Gram-positive bacteria as well as drug resistant bacteria, with an ultralow minimal inhibitory concentration (2–4 μg/mL) against 1 × 107 to 1 × 108 μg/mL Escherichia coli and Staphylococcus aureus. In the presence of the GQD/AgNP hybrids, the fluorescence behavior after the introduction of 2′, 7′-dichlorofluorescin diacetate demonstrated a possible role of reactive oxidative species in the GQD/AgNP hybrid-mediated antibacterial therapeutic effect. Furthermore, TEM and SEM imaging identified concomitant disruption of the bacterial cell membrane and loss of barrier function during the sterilization process. Therefore, the GQD/AgNP hybrids exhibit vast potentials for serving as highly effective, broad-spectrum antibacterial agent for sterilization use without the need of additional stimulation by laser irradiation (photosensitization) or the provision of H2O2, facilitating their relative ease of use and cost-effectiveness.Keywords: Ag nanoparticle; antibacterial effect; graphene quantum dot; oxidase mimic; reactive oxidative species;
Co-reporter:Wanjun Zhang, Tong Liu, Hangyan Dong, Haihong Bai, Fang Tian, Zhaomei Shi, Mingli Chen, Jianhua Wang, Weijie Qin, and Xiaohong Qian
Analytical Chemistry June 6, 2017 Volume 89(Issue 11) pp:5810-5810
Publication Date(Web):May 16, 2017
DOI:10.1021/acs.analchem.6b04960
O-linked β-N-acetylglucosamine (O-GlcNAc) is a ubiquitous post-translational modification of proteins in eukaryotic cells. Despite their low abundance, O-GlcNAc-modified proteins play many important roles in regulating gene expression, signal transduction, and cell cycle. Aberrant O-GlcNAc proteins are correlated with many major human diseases, such as Alzheimer’s disease, diabetes, and cancer. Because of the extremely low stoichiometry of O-GlcNAc proteins, enrichment is required before mass spectrometry analysis for large-scale identification and in-depth understanding of their cellular function. In this work, we designed and synthesized a novel thermosensitive immobilized triarylphosphine reagent as a convenient tool for efficient enrichment of azide-labeled O-GlcNAc proteins from complex biological samples. Immobilization of triarylphosphine on highly water-soluble thermosensitive polymer largely increases its solubility and reactivity in aqueous solution. As a result, facilitated coupling is achieved between triarylphosphine and azide-labeled O-GlcNAc proteins via Staudinger ligation, due to the increased triarylphosphine concentration, reduced interfacial mass transfer resistance, and steric hindrance in homogeneous reaction. Furthermore, solubility of the polymer from complete dissolution to full precipitation can be easily controlled by simply adjusting the environmental temperature. Therefore, facile sample recovery can be achieved by increasing the temperature to precipitate the polymer-O-GlcNAc protein conjugates from solution. This novel immobilized triarylphosphine reagent enables efficient enrichment and sensitive detection of more than 1700 potential O-GlcNAc proteins from HeLa cell using mass spectrometry, demonstrating its potential as a general strategy for low-abundance target enrichment.
Co-reporter:Liming Shen, Meiling Chen, Linlin Hu, Xuwei Chen, and Jianhua Wang
Langmuir December 31, 2013 Volume 29(Issue 52) pp:16135-16140
Publication Date(Web):December 31, 2013
DOI:10.1021/la404270w
Carbon dots (C-dots) have been proven to show the capability for direct reduction of Ag+ to elemental silver (Ag0) without additional reducing agent or external photoirradiation by incubating Ag+ with C-dots for 5 min in a water bath at 50 °C. Silver nanoparticles (Ag-NPs) are simultaneously formed with an average size of 3.1 ± 1.5 nm and grew on carbon dots. This process involves the oxidation of amine or phenol hydroxyl groups on the aromatic ring of C-dots. Meanwhile C-dots protect and stabilize the Ag-NPs from aggregation in aqueous medium; that is, the Ag-NPs are stable at least for 45 days in aqueous medium. The formed Ag-NPs cause significant resonance light scattering (RLS), which correlates closely with the concentration of silver cation, and this facilitates quantitative detection of silver in aqueous medium.
Co-reporter:Qing Chen, Xue Hu, Dan-Dan Zhang, Xu-Wei Chen, and Jian-Hua Wang
Bioconjugate Chemistry December 20, 2017 Volume 28(Issue 12) pp:2976-2976
Publication Date(Web):November 21, 2017
DOI:10.1021/acs.bioconjchem.7b00597
The bioconjugation of a polyoxometalate (POMs), i.e., dodecavanadate (V12O32), to DNA strands produces a functional labeled DNA primer, V12O32-DNA. The grafting of DNA primer onto streptavidin-coated magnetic nanoparticles (SVM) produces a novel composite, V12O32-DNA@SVM. The high binding-affinity of V12O32 with the ATP binding site in myosin subfragment-1 (S1) facilitates favorable adsorption of myosin, with an efficiency of 99.4% when processing 0.1 mL myosin solution (100 μg mL–1) using 0.1 mg composite. Myosin adsorption fits the Langmuir model, corresponding to a theoretical adsorption capacity of 613.5 mg g–1. The retained myosin is readily recovered by 1% SDS (m/m), giving rise to a recovery of 58.7%. No conformational change is observed for myosin after eliminating SDS by ultrafiltration. For practical use, high-purity myosin S1 is obtained by separation of myosin from the rough protein extract from porcine left ventricle, followed by digestion with α-chymotryptic and further isolation of S1 subfragment. The purified myosin S1 is identified with matrix-assisted laser desorption/ionization time-of-flight/mass spectrometry, giving rise to a sequence coverage of 38%.
Co-reporter:Lu Han, Ya-Nan Hao, Xing Wei, Xu-Wei Chen, Yang Shu, and Jian-Hua Wang
ACS Biomaterials Science & Engineering December 11, 2017 Volume 3(Issue 12) pp:3230-3230
Publication Date(Web):October 30, 2017
DOI:10.1021/acsbiomaterials.7b00643
A novel core–shell nanostructure, hollow copper sulfide nanosphere–doxorubicin (DOX)/graphene oxide (GO) (CuS–DOX/GO), is constructed for the purpose of controlled drug delivery and improved photothermo-chemotherapeutic effect. The CuS–DOX/GO nanocomposite is configured by employing dual photothermal agents, where the core, hollow CuS nanoparticle, acts as delivery-carrier for doxorubicin, and the shell, PEGylated GO nanosheet, prohibits leakage of the drug. DOX can be efficiently loaded onto the hollow CuS nanoparticles, and its subsequent release from CuS–DOX/GO nanocomposite is triggered in a pH- and near-infrared light-dependent manner. Moreover, integration of the two photothermal agents significantly improves the photothermal performance of this system. Ultimately, the combination of phototherapy and chemotherapy based on this system results in a much higher HeLa cell killing efficacy with respect to that for a single chemotherapy mode, as demonstrated by in vitro cytotoxicity tests.Keywords: cancer therapy; controlled drug delivery; copper sulfide; graphene oxide; photothermal therapy;
Co-reporter:Wanying Zeng;Jianhua Wang;Xuwei Chen;Xu Yang
Langmuir August 4, 2015 Volume 31(Issue 30) pp:8379-8385
Publication Date(Web):2017-2-22
DOI:10.1021/acs.langmuir.5b02031
Protein transfer from aqueous medium into ionic liquid is an important approach for the isolation of proteins of interest from complex biological samples. We hereby report a solid-cladding/liquid-core/liquid-cladding sandwich optical waveguide system for the purpose of monitoring the dynamic mass-transfer behaviors of hemoglobin (Hb) at the aqueous/ionic liquid interface. The optical waveguide system is fabricated by using a hydrophobic IL (1,3-dibutylimidazolium hexafluorophosphate, BBimPF6) as the core, and protein solution as one of the cladding layer. UV–vis spectra are recorded with a CCD spectrophotometer via optical fibers. The recorded spectra suggest that the mass transfer of Hb molecules between the aqueous and ionic liquid media involve accumulation of Hb on the aqueous/IL interface followed by dynamic extraction/transfer of Hb into the ionic liquid phase. A part of Hb molecules remain at the interface even after the accomplishment of the extraction/transfer process. Further investigations indicate that the mass transfer of Hb from aqueous medium into the ionic liquid phase is mainly driven by the coordination interaction between heme group of Hb and the cationic moiety of ionic liquid, for example, imidazolium cation in this particular case. In addition, hydrophobic interactions also contribute to the transfer of Hb.
Co-reporter:Peng-Fei Guo, Dan-Dan Zhang, Zhi-Yong Guo, Ming-Li Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces August 30, 2017 Volume 9(Issue 34) pp:28273-28273
Publication Date(Web):August 8, 2017
DOI:10.1021/acsami.7b08942
Novel unilamellar and homogeneous titanate nanosheets were prepared by anchoring (3-aminopropyl)triethoxysilane (APTES) and chelating copper ions, also know by the short form Cu-APTES-TiNSs. The nanosheets were uniform two-dimensional lamellas/monolayers with a thickness of 1.9 nm, and they were further characterized by atomic force microscopy, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectra, X-ray diffraction, X-ray photoelectron spectroscopy, inductively coupled plasma mass spectrometry, and N2 adsorption–desorption. The copper-decorated titanate nanosheets possess a copper content of 4.28 ± 0.14% and exhibit a favorable selectivity to the adsorption of hemoglobin, with a considerable capacity of 5314.2 mg g–1. The adsorbed hemoglobin is easily collected with a recovery rate of 91.3% by using 0.5% w/v sodium dodecyl sulfate as an eluent. Circular dichroism spectra confirmed that virtually no conformational alteration is observed for hemoglobin. Cu-APTES-TiNSs are further applied for the selective adsorption of hemoglobin from the human whole blood.Keywords: copper-decorated nanosheets; hemoglobin; selective isolation; titanate nanosheets; unilamellar nanomaterials;
Co-reporter:Yu-Ting Zhuang, Wei Gao, Yong-Liang Yu, Jian-Hua Wang
Materials & Design 2017 Volume 130(Volume 130) pp:
Publication Date(Web):15 September 2017
DOI:10.1016/j.matdes.2017.05.081
•3D porous CuFe2O4 cages were fabricated using a facile gas-forming strategy.•The cage structure provided this catalyst a high surface area and porosity.•The catalyst exhibited excellent activity for reduction of nitroaromatics and dyes.•The catalyst was magnetically recoverable and showed good activity over 16 cycles.The design and preparation of high-performance catalysts with high catalytic activity and excellent durability that are both environmentally benign and cost-effective remains a considerable challenge. Herein, a facile strategy is reported for the fabrication of three-dimensional porous CuFe2O4 cages, shortly as 3D CuFe2O4@C, by bubbling oxygen produced in situ through a CuFe2O4 suspension, followed by thermal treatment in nitrogen atmosphere. The 3D CuFe2O4@C structure increases the surface area of CuFe2O4 and provides a porous support structure. It is proposed to be a key in preventing the aggregation of CuFe2O4 during practical use. 3D CuFe2O4@C is shown to be a highly active catalyst, not only for the hydrogenation of p-nitrophenol, but also for the reduction of methylene blue in aqueous medium. 3D CuFe2O4@C exhibits remarkable catalytic activity towards p-nitrophenol reduction, with a catalytic rate constant of 2.167 min− 1 that is 5.35 times higher than that with pristine CuFe2O4 (0.405 min− 1). In addition, the 3D CuFe2O4@C catalyst has a high saturation magnetization of 51.9 emu g− 1, indicating that it can be easily recycled using a magnet. The 3D porous metal oxide nanostructure shows promising potentials as candidates for the remediation of contaminated aquatic environments and meets the demands for addressing future environmental issues.A facile strategy is reported for the fabrication of three-dimensional porous CuFe2O4 cages (3D CuFe2O4@C) for the catalytic reduction of p-nitrophenol and methylene blue in aqueous phase.Download high-res image (157KB)Download full-size image
Co-reporter:Lu Han, Yang Zhang, Yue Zhang, Yang Shu, Xu-Wei Chen, Jian-Hua Wang
Talanta 2017 Volume 171(Volume 171) pp:
Publication Date(Web):15 August 2017
DOI:10.1016/j.talanta.2017.04.056
•A polypyrrole/Fe3O4-core/gold nanoshell (MGNSHs) therapeutic nanoplatform is configured for imaging-guided cancer treatment.•MGNSHs nanocomposites act as excellent MR/CT imaging contrast agent and photothermal therapeutic agent.•MGNSHs nanoplatform is capable of serving as SERS active substrate for cancer cell detection.For the purpose of improving the diagnosis and enhancing the photothermal therapeutic effect for cancer under near-infrared (NIR) laser irradiation, a novel magnetic therapeutic platform containing dual photothermal agents, polypyrrole (PPy) and gold nanoshell, is constructed. The nanostructure is composed of a magnetic PPy/Fe3O4-core and a gold nanoshell, which is capable of enhancing the contrast for both magnetic resonance (MR) and X-ray computed tomography (CT) imaging. By attaching Raman probes onto the surface of gold shell, the nanocomposites exhibit the potential to serve as surface-enhanced Raman scattering (SERS) active substrates for optical modality identification of cancer cell. The capability of the therapeutic nanoplatform as photothermal agent is further demonstrated by effective ablation of cancer cells upon exposure to NIR laser at 808 nm, which is highly promising for multimodal imaging-guided cancer treatment.We herein report an electrochemical biosensor for highly sensitive and selective detection of ATP and adenosine deaminase activity using functionalized grapheme as efficient electrochemical label. The specific binding of ATP and its aptamer can link the split aptamer modified grapheme and magnetic beads together. After enzyme catalysis and magnetic separation, grapheme material anchored on surface would efficiently facilitate electron transfer acting as electrochemical label, thus produce amplified electrochemical signals. Our work would will shed lights on new diagnostic applications of graphene, such as the design of biodevices for detection of other biomolecules DNA, protein, even cancer cells.Download high-res image (216KB)Download full-size image
Co-reporter:Ya-Jie Zhang, Yi Cai, Yong-Liang Yu, Jian-Hua Wang
Analytica Chimica Acta 2017 Volume 976(Volume 976) pp:
Publication Date(Web):11 July 2017
DOI:10.1016/j.aca.2017.04.055
•A miniature DBD-OES detection approach is firstly integrated in a LOV platform.•It could readily achieve sample pretreatment, derivatization, nebulization and OES detection.•It provides a technique for the detection of cadmium at a sub μg L−1 level.•It is especially suitable for field analysis by virtue of small size.A miniature optical emission spectrometric (OES) system is developed by incorporating dielectric barrier discharge (DBD) microplasma as excitation source in a lab-on-valve (LOV) configuration for trace cadmium analysis. The entire system integrates bead injection (BI) sample pretreatment, post-column derivatization, in-situ nebulization and OES detection. Trace cadmium in sample solution is separated and preconcentrated by flowing through a 2-(5-Br-2-pyridylazo)-5-dethylaminophenol (5-Br-PADAP) loaded microcolumn in LOV, followed by elution with 20 μL of 0.1 M hydrochloric acid. The eluate after online derivatization with 5 μL of 0.2 M borate buffer solution containing 7.5% (v/v) ethanol is immediately transported into a pneumatic micronebulizer integrating DBD microplasma for cadmium excitation, and OES is recorded by using a charge coupled device (CCD) spectrometer. As a miniaturized analytical set-up, LOV provides an ideal sample-processing front-end with detection by DBD-OES, while introduction of DBD excitation source in LOV highly improves the analytical performances for trace metal species. With a sample volume of 1.0 mL, a detection limit of 0.06 μg L−1 and a linear range of 0.2–50 μg L−1 are achieved for cadmium, along with an enrichment factor of 38. The accuracy of the present system is confirmed by the determination of cadmium in certified reference materials, and further demonstrated by spiking recoveries of cadmium in real water samples.A miniature optical emission spectrometric (OES) system was developed by incorporating dielectric barrier discharge (DBD) microplasma as excitation source in a lab-on-valve (LOV) configuration for trace cadmium analysis.Download high-res image (173KB)Download full-size image
Co-reporter:Xiaoyan Wang;Ting Yang;Xiaoxiao Zhang;Mingli Chen;Jianhua Wang
Nanoscale (2009-Present) 2017 vol. 9(Issue 43) pp:16728-16734
Publication Date(Web):2017/11/09
DOI:10.1039/C7NR06292C
Mercury poses a serious threat to human health and the ecosystem. Its pollution is still prevalent in developing areas, which calls for the development of a simple on-site method for Hg2+ detection. Plasmonic nanosensors for mercury, especially those based on gold nanoparticles (AuNPs), have been increasingly developed due to the flourish of nanotechnology in the last decade. However, the limitation on either selectivity or stability hindered their practical applications. Herein, by taking advantage of the unique optical properties of AuNPs and the versatility of M13 phages, a novel Hg2+ sensing strategy is proposed. AuNPs grew in situ on the surface of Hg2+-binding M13 phages at room temperature and the resulting AuNP-phage networks were directly used for mercury sensing. Hg2+ was selectively captured by M13 phages indwelling in the networks and gathered around AuNPs, followed by the reduction into Hg(0) and deposition on the AuNP surfaces, wherein it resulted in a blue shift of the SPR band of AuNPs and an increase in the absorbance. An LOD of 8 × 10−8 mol L−1 was achieved based on the quantification of the absorption ratio of AuNPs at 525 and 650 nm. As the Hg2+ recognition was double guaranteed by the capture of Hg2+-binding phages as well as the unique affinity between mercury and gold, the sensing system showed a high selectivity and a superior interference tolerance capability, facilitating its practical applications in environmental water bodies without deterioration of the sensing performance.
Co-reporter:Yu-Ting Zhuang;Ting-Ting Zhu;Man Ruan;Yong-Liang Yu
Journal of Materials Chemistry A 2017 vol. 5(Issue 7) pp:3447-3455
Publication Date(Web):2017/02/14
DOI:10.1039/C6TA09774J
A facile and green approach for the preparation of a multifunctional ternary Fe2O3/graphitic-C3N4/graphene (FeCNG) nanocomposite with a porous structure is reported. This entails the growth of Prussian blue (PB) and adsorption of urea on graphene oxide (GO), followed by thermal pyrolysis of PB and urea leading to in situ formation of a porous N-doped graphene/iron oxide architecture. This strategy for the generation of FeCNG requires no structure-directing surfactants and gives rise to an N-doped composite capable of separation for recycling. The FeCNG architecture is capable of both rapid reduction of p-nitrophenol (4-NP) and efficient scavenging of Cr(VI) in aqueous media. The reduction of 4-NP to p-aminophenol by NaBH4 could be achieved within 3 min at 25 °C, using catalyst loadings as low as 1 mg. Cr(VI) adsorption was evaluated by Langmuir and pseudo-second-order models, offering a maximum equilibrium adsorption capacity of 149 mg g−1. In particular, Cr(VI) could be effectively adsorbed by the FeCNG nanocomposite and thereby reduced to less toxic Cr(III). By virtue of the enhanced catalytic performance and highly efficient adsorption of Cr(VI) across a wide pH range, the FeCNG nanocomposite possesses a broad application potential in energy and environmental sciences.
Co-reporter:Yang Zhang;Yan-Qin Chang;Lu Han;Yue Zhang;Ming-Li Chen;Yang Shu
Journal of Materials Chemistry B 2017 vol. 5(Issue 33) pp:6882-6889
Publication Date(Web):2017/08/23
DOI:10.1039/C7TB01528C
Mesoporous carbon nanomaterials have found applications in drug delivery and cancer therapy. However, it is still quite challenging to fabricate their multifunctional counterparts with high selectivity and efficiency for cancer theranostics. In this study, an alternative and multifunctional nanoplatform was developed, wherein mesoporous carbon nanoparticles (MCNs) were first encapsulated with a polyacrylic acid (PAA) shell, and after doxorubicin (DOX) loading, a polyethyleneimine (PEI) layer was coated to prevent the leakage of DOX. The MUC1 aptamer (Apt) was subsequently anchored onto the surface to provide the ability for specific recognition of cancer cells. This nanocarrier has been shortly termed as Apt@DP-DOX-MCN. The double polymer shells endowed the drug carrier platform with glutathione (GSH) and pH dual stimuli-responsive capability, and controllable release of the encapsulated drug molecule could be realized from the mesoporous and hollow structure, providing a 60% release of the loaded drug. Considering that most tumor sites exhibit more acidic environments or high redox potential, the pH- and GSH-sensitive release capability is particularly useful for controlled drug delivery in cancer therapy as it takes advantage of the inherent characteristics of tumor cells. The anchored MUC1 aptamer facilitates spatiotemporal therapy to improve selectivity towards the objective lesion site and decrease the off-target toxicity. Moreover, the targeted recognition and therapy of human lung adenocarcinoma cancer cells (A549) and breast cancer cells (MCF-7) was successfully achieved.
Co-reporter:Shuang Liu;Yi Cai;Yong-Liang Yu
Journal of Analytical Atomic Spectrometry 2017 vol. 32(Issue 9) pp:1739-1745
Publication Date(Web):2017/08/30
DOI:10.1039/C7JA00111H
An automated microelectrodialysis (μED)-liquid electrode discharge (LED)-optical emission spectrometric (OES) system was developed with the aim of potassium screening in serum, especially for a micro-sample volume. Potassium in serum was on-line extracted via a μED process and subsequently introduced into the LED microplasma to perform the optical emission detection at λem 766.5 nm. The optical emission intensity of potassium was measured using a charge-coupled device (CCD) spectrometer for quantitative analysis. A few important parameters governing the extraction of potassium by μED and its detection by LED-OES were investigated. The present system provides an excellent capability for eliminating matrix interference with a protein removal efficiency of >99%, by consuming a serum sample volume of 20 μL for each analysis. The entire analytical process, including sample introduction, pretreatment and detection, takes no more than 90 s. A detection limit of 0.6 mg L−1 was obtained along with a linear range of 2–70 mg L−1 and a RSD value of 4.8% at 5 mg L−1 potassium. The practical applicability of the μED-LED-OES system was demonstrated by the determination of potassium in serum certified reference materials and real human serum samples. The present system offers a potential strategy for screening the variation of the concentration of potassium in patients.
Co-reporter:Lu Han, Jun-Mei Xia, Xin Hai, Yang Shu, Xu-Wei ChenJian-Hua Wang
ACS Applied Materials & Interfaces 2017 Volume 9(Issue 8) pp:
Publication Date(Web):February 8, 2017
DOI:10.1021/acsami.7b00246
A protein-stabilized multifunctional theranostic nanoplatform, gadolinium oxide-gold nanoclusters hybrid (Gd2O3–AuNCs), is constructed for multimodal imaging and drug delivery. The Gd2O3–AuNCs nanohybrid is developed by integrating Gd2O3 nanocrystals and gold nanoclusters into bovine serum albumin scaffold as a stabilizer. The nanohybrid exhibits favorable biocompatibility and is capable of enhancing the contrast in magnetic resonance and X-ray computed tomography imaging. Meanwhile, the integrated AuNCs component not only endows the nanohybrid to produce red fluorescence, but also sensitizes the generation of singlet oxygen (1O2) upon near-infrared laser stimulation at 808 nm. Bovine serum albumin surrounding the nanoparticles makes Gd2O3–AuNCs a brilliant carrier for the delivery of indocyanine green (ICG). ICG loading endows the Gd2O3–AuNCs–ICG nanocomposite with a near-infrared fluorescence imaging capability, and improves its photodynamic property and photothermal capability. Ultimately, further experiments have demonstrated that Gd2O3–AuNCs–ICG nanocomposite is a promising theranostic agent for image guided cancer therapy.Keywords: gadolinium oxide; gold nanocluster; magnetic resonance imaging; near-infrared fluorescence; photothermal/photodynamic therapy; X-ray computed tomography;
Co-reporter:Wen-Jing Wang;Jun-Mei Xia;Xin Hai;Ming-Li Chen
Environmental Science: Nano 2017 vol. 4(Issue 5) pp:1037-1044
Publication Date(Web):2017/05/18
DOI:10.1039/C7EN00027H
The nucleophilic substitution reaction between 4-chloro-7-nitro-2,1,3-benzoxadiazole (NBD-Cl) and –NH2 groups on amino-functionalized carbon dots (CDs) produces a novel carbon dot-based hybrid, CDs@NBD for short. In addition to the characteristic fluorescence emission of carbon dots at λex/λem = 360/443 nm, the CDs@NBD hybrid gives rise to new photoluminescence at λex/λem = 460/544 nm, which is significantly quenched by p-phenylenediamine (PPD) via static quenching. This provides a novel sensing approach for fluorometric detection of PPD with CDs@NBD as a probe. A linear calibration graph is obtained within two concentration ranges of 0.1–1.0 μmol L−1 and 1.0–10.0 μmol L−1, along with a detection limit of 56 nmol L−1 and a RSD of <3% (at 1.0 μmol L−1). The common coexisting species in environmental and biological sample matrices cause no obvious interferences on the detection of PPD. The colour change of the CDs@NBD hybrid solution with the variation in PPD concentration also facilitates visual detection of PPD, which further demonstrates promising applications in environmental and biological sample analysis.
Co-reporter:Dan-Dan Zhang;Peng-Fei Guo;Lin-Lin Hu;Xu-Wei Chen
Journal of Materials Chemistry B 2017 vol. 5(Issue 4) pp:750-756
Publication Date(Web):2017/01/25
DOI:10.1039/C6TB02733D
A novel polyoxometalate (POM)-based hybrid is prepared for the selective adsorption of acidic and/or basic proteins. The solidification of the POM moiety P8W48 is firstly achieved through dehydration condensation between the –OH group on the P8W48 surface and the Si–OH of aminopropyltriethoxysilane (APTS), and thereafter further condensation of the P8W48O184–APTS intermediate with poly(acrylic acid) (PAA) produces a hybrid, by linking carboxyl groups in PAA with –NH2 groups in P8W48O184–APTS via the formation of an amide bond. The P8W48–APTS–PAA hybrid surface is negatively charged due to abundant COO− groups from PAA, which provides electrostatic interactions with positively charged proteins by varying pHs. Meanwhile, the d–p π bond in P8W48 offers strong affinity to other proteins via π–π stacking interaction. The hybrid thus offers potential for achieving selective adsorption of either acidic or basic proteins by simply controlling the adsorption conditions, i.e., pH value or ionic strength of the adsorption medium. With ovalbumin (Ova) and lysozyme (Lys) as the models of acidic and basic proteins, their adsorption behaviors fit the Langmuir model, with adsorption capacities of 367.0 mg g−1 and 74.0 mg g−1, respectively. The retained proteins are readily recovered with 0.01 mol L−1 CTAB, providing recoveries of 89.0% for Ova and 93.0% for Lys. The P8W48–APTS–PAA hybrid is further applied for the isolation of Ova and Lys from real biological samples, egg white.
Co-reporter:Xin Lin, Xin Hai, Ning Wang, Xu-Wei Chen, Jian-Hua Wang
Analytica Chimica Acta 2017 Volume 992(Volume 992) pp:
Publication Date(Web):1 November 2017
DOI:10.1016/j.aca.2017.09.006
•A novel dual-signal model array sensor is developed for sensitive discrimination of proteins.•The protein concentration for complete discrimination is low down to 50 nM.•This dual-signal model array sensor can be applied to sample of complicated matrices.•Discriminations and identifications of microorganisms originated from same species are achieved.The accurate differentiation and identification of proteins play a vital role in many areas. Herein a novel array sensor is developed for sensitive discrimination of proteins, based on the various optical responses of GQDs/AuNPs system towards different protein species. The simultaneously generated distinct variations of fluorescence and absorbance of GQDs/AuNPs system resulted from the interactions between protein species and sensing units contribute to a dual-signal strategy for protein discrimination. The protein concentration for complete discrimination is low down to 50 nM, and accurate discriminations of protein mixture of different concentrations/molar ratio are achieved. The complementary fluorescence and absorbance response makes this dual-signal model array sensor practicable to sample of complicated matrices, demonstrated by the accurate discrimination of protein species in human urine. Moreover, six strains of microorganisms originated from three different species are also successfully discriminated with 100% accuracy (OD600 = 1.0).A dual-signal model array sensor is developed and applied for the highly sensitive discrimination of proteins and microorganisms based on GQDs stabilized AuNPs sensing system.Download high-res image (179KB)Download full-size image
Co-reporter:Yue Zhang, Zhiyong Guo, Lu Han, Yang Zhang, Xuwei Chen, Jianhua Wang
Carbon 2017 Volume 122(Volume 122) pp:
Publication Date(Web):1 October 2017
DOI:10.1016/j.carbon.2017.06.051
We report the self-assembly of monolayer polyhedral oligomeric silsesquioxane (POSS) on graphene oxide (GO), where GO acts as a directing template along with the assembly of POSS into a three-dimensional porous framework structure, shortly termed as PPG. The PPG framework contains ultrathin nanopetals with a thickness of ca. 1.95 nm, giving rise to reduced restacking and high surface area. The PPG framework exhibits a high adsorption capacity of up to 1570.3 mg g−1 towards β-lactoglobulin, in addition to a favorable selectivity against other protein species with similar isoelectric points to that of β-lactoglobulin. This might be attributed to the specific hydrogen-bonding donor-acceptor interaction between the calyx structure of β-lactoglobulin and the PPG framework. Satisfactory separation performance of PPG is confirmed by the selective discrimination and isolation of β-lactoglobulin from complex biological sample matrixes, e.g., milk whey. This observation provides a promising approach for the construction of monolayer polymer-modified three-dimensional graphene oxide composites with specific biological application potentials.Download high-res image (262KB)Download full-size image
Co-reporter:Chang Xia, Xin Hai, Xu-Wei Chen, Jian-Hua Wang
Talanta 2017 Volume 168(Volume 168) pp:
Publication Date(Web):1 June 2017
DOI:10.1016/j.talanta.2017.03.040
•Bi-morphological N, S-GQDs are simultaneously fabricated via a fast, facile and eco-friendly procedure.•The doping of N, S brings the free N, S-GQDs high fluorescence quantum yield and improves the affinity of GQDs with Fe3+.•The cross-linking among L-cysteine molecules and graphene nucleus prevent the aggregation of GQDs efficiently.A facile one-step solvent-free synthesis approach is proposed for the simultaneous fabrication of free and solidified N, S-doped graphene quantum dots (N, S-GQDs) by using citric acid as precursor and L-cysteine as dopant. Graphene nucleus is firstly formed via the intermolecular dehydration of citric acid. N and S are then incorporated into the graphene structure by attacking the margin of graphene nucleus. The cross-linking among the graphene nucleus via the intermolecular condensation leads to the generation of free N, S-GQDs, while the intermolecular amidation between L-cysteine molecules and graphene nucleuses contributes to the solid-state fluorescence graphene quantum dots (SSF-GQDs). The free N, S-GQDs exhibit favorable photoluminescence behaviors such as high fluorescent quantum yield of 74.5%, stable photoluminescence within a wide range of pH and high tolerance to external ionic strength of up to 1.0 mol L−1 NaCl, making it excellent fluorescence probe for the sensitive detection of Fe3+ with a linear range of 0.01–3 μM and a detection limit of 3.3 nM. The solidification of GQDs prevents the aggregation of GQDs efficiently and offers the solidified N, S-GQDs yellow-green fluorescence, with a fluorescence quantum yield of 10.6%. This proposed protocol provides a novel avenue to fabricate diverse fluorescent graphene materials for different practical applications.The simultaneous fabrication of free N, S-doped GQDs and solidified N, S-doped GQDs are achieved via the intermolecular dehydration and intermolecular amidation; the obtained GQDS can be used as excellent fluorescence probes for sensitive detection of Fe3+ and fingermarks.Download high-res image (292KB)Download full-size image
Co-reporter:Yue Zhang, Hui-Yan Shen, Xin Hai, Xu-Wei Chen, and Jian-Hua Wang
Analytical Chemistry 2017 Volume 89(Issue 2) pp:
Publication Date(Web):December 12, 2016
DOI:10.1021/acs.analchem.6b04407
The rapid and accurate detection of hydrogen sulfide is of great concern due to its unique role on environmental pollution and signal transmission in physiological systems. Herein, we report a smart colorimetric probe for the selective detection of H2S. The probe is prepared via a surfactant-free route with cross-linked polyhedral oligomeric silsesquioxane (POSS) polymer cage as capping ligand and reducing agent under microwave irradiation, called poly-POSS-formaldehyde polymer (PPF) cage-AgNPs or PPF-AgNPs for short. The caged silver nanoparticles are well-dispersed with narrow size distribution within 6.0–8.4 nm. Chloride ions and aldehyde groups in PPF make the nucleation and growth of Ag nanoparticles accomplished within a very short time of 1 min. The positively charged PPF-AgNPs exhibit excellent selectivity to H2S against other anionic species and thiols due to the specific Ag–H2S interaction, where the favorable protection effect of PPF polymer cage from the nanoparticle aggregation is demonstrated. The colorimetric probe presents a quick response to H2S (<3 min) and favorable sensitivity within a linear range of 0.7–10 μM along with a detection limit of 0.2 μM. The probe is well demonstrated by analysis of H2S in various water and biological samples.
Co-reporter:Yue Zhang;Yuting Zhuang;Huiyan Shen;Xuwei Chen;Jianhua Wang
Microchimica Acta 2017 Volume 184( Issue 4) pp:1037-1044
Publication Date(Web):2017 April
DOI:10.1007/s00604-017-2100-z
The authors have prepared a super-hydrophilic polymer consisting of a poly-polyhedral oligomeric silsesquioxane (POSS)-formaldehyde (PPF) composite. The polymerization process does not require a catalyst and results in a material with excellent hydrophilic properties and abundant functional groups. The PFF composite, even if not chemically modified, can selectively bind glycoproteins due to strong hydrophilic interactions. It is shown that glycoproteins can be selectively captured by the composite that has a binding capacity as large as 542 mg g−1 for the model protein ovalbumin. The PPF was applied to the selective capture and isolation of ovalbumin from complex biological samples.
Co-reporter:Jie Xia;Yu-Ting Zhuang;Yong-Liang Yu
Microchimica Acta 2017 Volume 184( Issue 4) pp:1109-1116
Publication Date(Web):2017 April
DOI:10.1007/s00604-017-2104-8
Carbon polymer dots (CPDs) were prepared by a one-pot aqueous synthetic route from ascorbic acid and diethylenetriamine at room-temperature. The CPDs under 350-nm excitation exhibit blue fluorescence peaking at 430 nm with a quantum yield of 47%. Other features include an average diameter of 5 nm, a fluorescence that is independent of the excitation wavelength, good water dispersibility and photostability, and excellent biocompatibility. The CPDs are shown to be viable fluorescent probes for ferric ion which acts as a strong quencher. The response to Fe(III) is linear in the 0.2 to 10 μM concentration range, and the detection limit is 0.1 μM. The probe was applied to the determination of Fe(III) in environmental waters and to intracellular imaging of ferric ions in HeLa cells.
Co-reporter:Yang Zhang, Lu Han, Lin-Lin Hu, Yan-Qin Chang, Rong-Huan He, Ming-Li Chen, Yang Shu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 vol. 4(Issue 30) pp:5178-5184
Publication Date(Web):11 Jul 2016
DOI:10.1039/C6TB00987E
A pH and redox responsive bi-trigger continuous drug release nanocarrier is developed by capping mesoporous carbon nanoparticles (MCNs) with polyacrylic acid (PAA), termed as PAA-ss-MCN. The nanocarrier contains disulfide bond units and exhibits pH responsive behavior. It provides promising potential for drug loading due to the internal uniform channels and large surface area of MCNs. PAA grafted on the exterior surface of MCNs acts as a gating layer, generating a novel nano-container and a pH-responsive intelligent nanovalve. By loading doxorubicin (DOX) in PAA-ss-MCN, its sequential release is achieved via two approaches: (1) the intracellular acidic environment induces partial release from the surface of the PAA gating layer, (2) release of the drug sealed in nanochannels via disruption of the integrity of the nanocarrier by glutathione (GSH) caused dissociation of disulfide bonds in the physiological environment. As a result, release of 62% loaded drug is readily achieved. After culturing with HeLa cells, DOX transports into the cell interior and therein exhibits pH- and GSH-sensitive release. As most tumor sites exhibit more acidic environments or high redox potential, the pH- and GSH-sensitive releasing capability of PAA-ss-MCN is particularly useful for controllable drug delivery by taking advantage of the inherent characteristics of tumor cells.
Co-reporter:Ji Feng, Wen-Jing Wang, Xin Hai, Yong-Liang Yu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 vol. 4(Issue 3) pp:387-393
Publication Date(Web):23 Nov 2015
DOI:10.1039/C5TB01999K
Carbon dots (CDs) with a high quantum yield have been synthesized by a facile and green one-pot approach under microwaves with silkworm chrysalis (SC) as the natural carbon source, without using any other chemicals/reagents. The morphology and optical properties of the resultant CDs are characterized by TEM, XRD, FT-IR, XPS, UV-vis and photoluminescence (PL). The SC-CDs have an average size of 19 nm, and contain C, O and N with relative contents of ca. 71.32%, 22.96% and 5.72%, respectively. A significant emission at 420 nm at an excitation wavelength of 350 nm is recorded, resulting in a quantum yield of 46% with quinine sulfate (quantum yield 54%) as a reference. In addition to excellent solubility and stability in aqueous medium, the SC-CDs exhibit excitation-dependent photoluminescence with a large Stokes shift of 70 nm. It is further demonstrated that the SC-CDs exhibit a low cytotoxicity at a higher concentration of 15 mg mL−1 and they are able to display bright blue, green and red colors under an inverted fluorescence microscope during cell imaging experiments, showing their vast potential in bioimaging.
Co-reporter:Lu Han, Yang Zhang, Xu-Wei Chen, Yang Shu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 vol. 4(Issue 1) pp:105-112
Publication Date(Web):17 Nov 2015
DOI:10.1039/C5TB02002F
A novel phototherapy nanoplatform is prepared by coating hollow CuS nanoparticles with a bovine serum albumin–folic acid (BSA–FA) complex. The obtained CuS–BSA–FA nanoparticles are used as drug-delivery vehicles to transport a near-infrared-absorbing phototherapeutic agent (indocyanine green, ICG) into HeLa cells, after loading ICG onto CuS–BSA–FA. In this manner, a combined therapy approach is established consisting of photothermal therapy (by CuS–BSA–FA nanocarriers) and cytotoxic effects of photodynamic and photothermal therapy (by ICG upon 808 nm laser irradiation). The encapsulation of ICG onto CuS–BSA–FA significantly improves the stability and reduces the dark toxicity of free ICG. This therapeutic system exhibits an obviously higher photothermal heating effect and capability of 1O2 generation under laser irradiation compared with bare nanocarriers. In addition, the grafted FA segments on the surface of CuS–BSA–FA are proved to enhance the internalization of nanoparticles by FA-receptor-mediated endocytosis.
Co-reporter:Zhi-Yong Guo, Yue Zhang, Dan-Dan Zhang, Yang Shu, Xu-Wei Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 43) pp:29734
Publication Date(Web):October 12, 2016
DOI:10.1021/acsami.6b11158
A novel strategy for the preparation of magnetic nanospheres encapsulated by mesoporous copper oxide shell, shortly termed as Fe3O4@mCuO, is reported via the calcination of Cu(NH3)4(NO3)2 into continuous mesoporous CuO shell onto the surface of Fe3O4 nanoparticles. The magnetic nanospheres are characterized to possess stable core–shell structure with a crystalline mesoporous CuO layer, exhibiting a CuO loading content of 25.2 ± 1.1% along with a favorable magnetic susceptibility. Fe3O4@mCuO nanospheres exhibit favorable selectivity on the adsorption of hemoglobin with a high adsorption capacity of up to 1162.5 mg g–1. After adsorption, the high magnetic susceptibility allows convenient separation of the nanospheres by an external magnet. The retained hemoglobin could be readily recovered by using 0.5% (m/v) sodium dodecyl sulfate (SDS) as stripping reagent, providing a recovery of 78%. Circular dichroism spectra illustrate virtually no change in the conformation of hemoglobin after the process of adsorption/desorption. Fe3O4@mCuO nanospheres are further applied for the selective isolation of hemoglobin from human whole blood, achieving high-purity hemoglobin as demonstrated by SDS-PAGE (polyacrylamide gel electrophoresis) assays.Keywords: core−shell structure; hemoglobin; isolation; magnetic Fe3O4 nanospheres; mesoporous CuO
Co-reporter:Yu-Ting Zhuang, Wei Gao, Yong-Liang Yu, Jian-Hua Wang
Carbon 2016 Volume 108() pp:190-198
Publication Date(Web):November 2016
DOI:10.1016/j.carbon.2016.06.107
A novel three-dimensional (3D) magnetic carbon framework (MCF) is developed and applied as an efficient absorbent for the removal of lead from aqueous medium. The MCF adsorbent was designed with Prussian blue (PB), amylopectin and polyurethane (PU) sponge serving as iron and carbon precursors at a calcination temperature of 450 °C. The framework is characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), thermogravimetric analysis (TGA), Fourier-transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS) and surface charge analysis to elucidate the mechanism for the formation of the framework structure and its performance in Pb (II) removal. The 3D network structure of PU sponge provides an ideal support for the magnetic PB. Meanwhile, a better porous network structure obtained by the introduction of amylopectin endows MCF with a high specific surface area and a large number of active adsorption sites. An adsorption capacity of up to 386 mg g−1 for Pb (II) is achieved in aqueous medium at pH 7. MCF provides excellent features of regeneration and ease of magnetic separation, thus it shows a vast potential for water remediation.
Co-reporter:Yi Cai, Ya-Jie Zhang, De-Fu Wu, Yong-Liang Yu, and Jian-Hua Wang
Analytical Chemistry 2016 Volume 88(Issue 8) pp:4192
Publication Date(Web):March 31, 2016
DOI:10.1021/acs.analchem.6b00830
The low atomization and excitation capability of nonthermal microplasma, e.g., dielectric barrier discharge (DBD), has greatly hampered its potential applications for the determination of metals in solution. In the present work, an inspiring development is reported for direct atomization and excitation of cadmium in aqueous solution by DBD and facilitates highly sensitive determination. A DBD microplasma is generated on the nozzle of a pneumatic micronebulizer to focus the DBD energy on a confined space and atomize/excite metals in the spray. Meanwhile, an appropriate sample matrix and nebulization in helium further improves the atomization and excitation capability of DBD. With cadmium as a model, its emission is recorded by a CCD spectrometer at 228.8 nm. By using an 80 μL sample solution nebulized at 3 μL s–1, a linear range of 5–1000 μg L–1 along with a detection limit of 1.5 μg L–1 is achieved, which is comparable to those obtained by commercial bulky inductively coupled plasma (ICP)-based instrumentations.
Co-reporter:Mingli Chen, Chunbao Huo, Yikun Li, and Jianhua Wang
ACS Sustainable Chemistry & Engineering 2016 Volume 4(Issue 3) pp:1296
Publication Date(Web):December 29, 2015
DOI:10.1021/acssuschemeng.5b01324
A three-dimensional adsorbent, i.e., lanthanum oxide decorated graphene composite (3D graphene–La2O3 composite), is prepared. The composite exhibits favorable adsorption performance to phosphate, providing a sorption capacity of 82.6 mg g–1 at pH 6.2. The adsorption behavior for phosphate fits the Langmuir model, and the adsorption kinetics fit a pseudo-second-order model, with rate constants of 0.1847 and 0.007 969 g mg–1 min–1 at phosphate concentrations of 35 and 142 mg L–1, respectively. For the removal of 25 mg L–1 phosphate in 1.0 mL aqueous medium, the commonly encountered anionic species in waters, e.g., Cl–, SO42–, and NO3–, pose no interfering effect at 8000 mg L–1, providing a favorable removal efficiency of 100% by 2.0 mg of composite. When 142 mg L–1 phosphate solution is treated, 100% and >80% adsorption efficiencies are achieved respectively in the presence of 1000 and 8000 mg L–1 of Cl–, SO42–, and NO3–. The high tolerance capacity against coexisting anionic species by the graphene–La2O3 composite makes it suitable for water cleanup by selective and fast adsorption/removal of phosphate.Keywords: Adsorption; Graphene composite; Lanthanum oxide; Phosphate; Removal
Co-reporter:Xuwei Chen, Xin Hai, Jianhua Wang
Analytica Chimica Acta 2016 Volume 922() pp:1-10
Publication Date(Web):30 May 2016
DOI:10.1016/j.aca.2016.03.050
•This review provides an updated overview of G/GO-materials in the separation, isolation/preconcentration of protein species.•The strategies to improve protein extraction performance by G/GO-materials are summarized.•The challenges and future perspectives in the related research fields are discussed.The distinctive/unique electrical, chemical and optical properties make graphene/graphene oxide-based materials popular in the field of analytical chemistry. Its large surface offers excellent capacity to anchor target analyte, making it an powerful sorbent in the adsorption and preconcentration of trace level analyte of interest in the field of sample preparation. The large delocalized π-electron system of graphene framework provides strong affinity to species containing aromatic rings, such as proteins, and the abundant active sites on its surface offers the chance to modulate adsorption tendency towards specific protein via functional modification/decoration. This review provides an overview of the current research on graphene/graphene oxide-based materials as attractive and powerful adsorption media in the separation/isolation and preconcentration of protein species from biological sample matrixes. These practices are aiming at providing protein sample of high purity for further investigations and applications, or to achieve certain extent of enrichment prior to quantitative assay. In addition, the challenges and future perspectives in the related research fields have been discussed.
Co-reporter:Deng-Ji Zhang, Yi Cai, Ming-Li Chen, Yong-Liang Yu and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2016 vol. 31(Issue 2) pp:398-405
Publication Date(Web):27 Aug 2015
DOI:10.1039/C5JA00266D
Dielectric barrier discharge (DBD) micro-plasma as a radiation source has been investigated for the excitation of chlorine, bromine and iodine and their simultaneous determination by vapor generation-DBD optical emission spectrometry (OES). Chloride and bromide in 6 mol L−1 H2SO4 were on-line vaporized by reaction with 0.1 mol L−1 KMnO4, while bromide and iodide in 0.5 mol L−1 H2SO4 were on-line vaporized by reaction with 0.02 mol L−1 KMnO4. The vapor species of halogens were subsequently transferred into a tubular DBD excitation chamber by a helium stream for performing multi-element optical emission and detection with a small charge-coupled device (CCD) spectrometer. Special attention has been paid to the simultaneous vapor generation introduction of halogens and subsequent multi-element DBD optical emission. With the characteristic emission lines of Cl 837 nm, Br 827 nm and I 905 nm as the analytical lines for quantification, the detection limits for the simultaneous determination of Cl and Br were 15 and 11 μg L−1, respectively, while those for Br and I were 10 and 95 μg L−1, respectively. The accuracy of the present DBD-OES system was confirmed by the determination of halide contents in a few certified reference materials and real samples.
Co-reporter:Ting Yang, Dong-Xue Gao, Yong-Liang Yu, Ming-Li Chen, Jian-Hua Wang
Talanta 2016 Volume 146() pp:603-608
Publication Date(Web):1 January 2016
DOI:10.1016/j.talanta.2015.07.074
•A portable acetone analyzer is constructed based on a planar dielectric barrier discharge-optical emission spectrometric system.•519 nm emission line attributes to CO fragments can eliminate potential interferences from non-oxygen containing species.•Breath acetone has been analyzed for diabetic patients and healthy volunteers.Acetone is a predominant volatile organic compound (VOC) in the exhaled breath and a promising biomarker for diabetes and ketoacidosis. A non-thermal micro-plasma generated in a planar dielectric barrier discharge (DBD) is used as a radiation source for the excitation of gaseous acetone followed by its quantification with optical emission spectrometry (OES). Gaseous acetone can be directly sampled, while liquid acetone is evaporated by heated tungsten coil and then introduced into the DBD micro-plasma by a helium carrier flow for performing optical emission and detection at a 519 nm emission line. In the present study, the exhaled breath is collected and transferred into aqueous medium for sampling. With a sampling volume of 7 μL in a micro-drop, a linear range of 40–1600 mg L−1 is obtained along with a detection limit of 44 ng and a precision of 5.7% RSD. The present system is successfully applied to the determination of breath acetone for both diabetic patients and healthy volunteers.Download full-size image
Co-reporter:Xing Wei, Lin-Lin Hu, Ming-Li Chen, Ting Yang, and Jian-Hua Wang
Analytical Chemistry 2016 Volume 88(Issue 24) pp:
Publication Date(Web):November 22, 2016
DOI:10.1021/acs.analchem.6b03810
The patterning of distribution models for specific heavy metal species in biological cells is highly important for elucidating their effect on single cells or in a living organism. For this purpose, the variation of chromium levels and the distribution patterns of chromium species in single-cell subjects are investigated by culturing two kinds of native cells (i.e., HeLa cells and MCF-7 cells) in the presence of either Cr(III) or Cr(VI). The analysis of single cells is performed with time-resolved inductively coupled plasma mass spectrometry. We found that the total chromium level in the single cells after culturing in a Cr(VI)-enriched medium is higher than that for those single cells cultured in a Cr(III)-reinforced medium. It is interesting to see that at certain culturing conditions, the chromium level in single individual cells increases linearly with Cr(III) concentration in the culture medium, whereas it increases exponentially with Cr(VI) concentration. This indicated that Cr(VI) is more prone to penetrate the cells with respect to Cr(III), and after a concentration threshold, considerably more Cr(VI) enters into the interior of HeLa cells or MCF-7 cells.
Co-reporter:Ning Wang, Yiting Wang, Tingting Guo, Ting Yang, Mingli Chen, Jianhua Wang
Biosensors and Bioelectronics 2016 Volume 85() pp:68-75
Publication Date(Web):15 November 2016
DOI:10.1016/j.bios.2016.04.089
•A green approach is developed for preparing water and ethanol soluble carbon dots.•The CDs facilitate fluorescence detection of Fe3+ and cell imaging.•Water soluble CDs offer a promising probe for fluorescence sensing of E.coli.A simple one-step hydrothermal green approach was reported for the preparation of carbon dots (CDs) without any further decoration or modification with papaya powder as natural carbon source. In this economical and eco-friendly system, deionized water or 90% ethanol was used as solvent to produce water-soluble or ethanol-soluble CDs, respectively, termed as W-CDs and E-CDs. The quantum yield (QY) for W-CDs was 18.98%, while that for E-CDs was 18.39%. The potentials of the prepared carbon dots toward diverse applications were thoroughly investigated. W-CDs and E-CDs provide promising probes for fluorescence detection of Fe3+, offering limits of detection of 0.48 μmol L−1 and 0.29 μmol L−1, respectively. W-CDs was further demonstrated to be a promising probe for fluorescence sensing of Escherichia coli O157: H7, along with a limit of detection of 9.5×104 cfu mL−1. Meanwhile, both W-CDs and E-CDs exhibit favorable biocompatibility, and demonstrated to be efficient for Hela cell imaging.
Co-reporter:Quan-Xing Mao, Lu Han, Yang Shu, Xu-Wei Chen, Jian-Hua Wang
Talanta 2016 Volume 161() pp:54-61
Publication Date(Web):1 December 2016
DOI:10.1016/j.talanta.2016.08.031
•Ionic liquids modified carbon nanodots is prepared at ambient temperature via covalent conjugation interaction.•The biocompatibility of carbon nanodots is significantly improved with the modification of ionic liquid moiety.•The prepared carbon nanodots show potentials in two-color cell imaging.In the practice of in vivo imaging with carbon nanodots (CNDs) as probe, the volume of CNDs solution introduced into living body should be kept at minimum, and a higher concentration is needed to ensure sufficient quantity of the probe for obtaining bright image. Therefore, the improvement on biocompatibility of the CNDs is among the most important and critical issues. We report herein the improvement on the biocompatibility of CNDs with modification by ionic liquid. Amide group functionalization of carbon nanodots is first conducted through microwave irradiation, followed by coupling the ionic liquid 1-carboxymethyl-3-methyl imidazolium bromide on the surface of the Amide-CNDs via covalent conjunction to produce the modified carbon nanodots (IL-CNDs). This modification process significantly improved the biocompatibility of CNDs, as demonstrated by cell imaging at a higher concentration of CNDs. Both Amide-CNDs and IL-CNDs exhibit abundant surface functional groups, resulting in tunable fluorescent emission feature and potential applications in two-color cell imaging.Ionic liquid modified carbon nanodots are prepared via covalent conjugation between carboxyl and amide groups functionalized carbon nanodots which exhibit significant improvement on the biocompatibility.
Co-reporter:Dan-Dan Zhang, Lin-Lin Hu, Qing Chen, Xu-Wei Chen, Jian-Hua Wang
Talanta 2016 Volume 159() pp:23-28
Publication Date(Web):1 October 2016
DOI:10.1016/j.talanta.2016.06.005
•A novel biocompatible polyoxometalates-based hybrid is developed by solidification of super-lacunary P8W48O18440- polyoxoanions.•The hybrid exhibits favorable adsorption selectivity toward hemoglobin through π-π stacking interaction.•Selective isolation of hemoglobin is achieved from a complex biological sample matrix, human whole blood.A novel polyoxometalate (POM)-based hybrid P8W48-APTS is prepared by the solidification of super-lacunary P8W48O18440- polyoxoanions with APTS in an acidic medium. The oxygen (O−) atoms in P8W48O18440- are bound to silicon atoms in APTS by the formation of Si-O linkage through dehydration condensation. The solidification is confirmed by characterizations with XRD, FT-IR, TGA, SEM and EDXS. Selective isolation of proteins of interest, hemoglobin (Hb) in this case, from complex sample matrices is achieved by using P8W48-APTS hybrid as adsorbent under controlled conditions. 5.0 mg of P8W48-APTS hybrid results in an adsorption efficiency of 93% for 100 mg L−1 hemoglobin in 1.0 mL sample solution at pH 7. The adsorption behavior of Hb onto P8W48-APTS hybrid fits Langmuir adsorption model, corresponding to an adsorption capacity of 355.0 mg g−1. The retained Hb could be readily recovered with either a SDS solution (0.1 mol L−1) or a Na3PO4 (0.1 mol L−1) solution as stripping reagent, providing recoveries of 94.6% or 83.9%, respectively. The biological activity of Hb remains 96.7% after an adsorption/desorption process (with elution by SDS), which illustrates virtually no change on the conformation of hemoglobin. The P8W48-APTS hybrid has been applied for the selective adsorption of Hb from human whole blood, and the results are demonstrated by SDS-PAGE assay.A novel polyoxometalate-based hybrid is developed by solidification of super-lacunary P8W48O18440- polyoxoanions which exhibits favorable selectivity to hemoglobin adsorption.
Co-reporter:Quan-Xing Mao, Shuang E, Jun-Mei Xia, Ru-Sheng Song, Yang Shu, Xu-Wei Chen, and Jian-Hua Wang
Langmuir 2016 Volume 32(Issue 46) pp:12221-12229
Publication Date(Web):November 2, 2016
DOI:10.1021/acs.langmuir.6b03331
Tunable fluorescent emission and applications in both in vitro and in vivo imaging of hydrophobic carbon nanodots (CNDs) with rapid penetration capability are reported. The hydrophobic CNDs are prepared via hydrothermal treatment of ionic liquid 1-ethyl-3-methylimidazolium bromide and exhibit excitation-dependent photoluminescence behavior along with a red-shift in the excitation/emission maxima with concentration. The quantum yields of the as-prepared CNDs are in the range of 2.5–4.8% at an excitation wavelength of 300–600 nm. The rapid penetration behavior (within 1 min) of CNDs into the cell membrane significantly reduces the sample treatment time and avoids potential fluorescence quenching induced by the interaction between CNDs and samples. A co-location study reveals that the hydrophobic CNDs are distributed mainly in the lysosome. The potentials of the hydrophobic CNDs as fluorescent probe in in vitro and in vivo imaging are well demonstrated by the labeling of HeLa cells, MCF-7 cells, A549 cells, and Kunming mice.
Co-reporter:Yue Zhang, Jia-Wei Liu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 6) pp:983-989
Publication Date(Web):23 Dec 2014
DOI:10.1039/C4TB01792G
A three-dimensional graphene oxide framework is prepared via a simple and cost-effective one-pot approach through the hydrogen-bonding interaction between amylopectin and graphene oxide in the presence of hydrazine hydrate acting as a reducing reagent. The framework is shortly termed as AP-rGO and it is characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), surface charge analysis and thermogravimetric analysis (TGA). The obtained AP-rGO framework exhibits excellent adsorption performance toward hemoglobin in the presence of other protein species. It provides a maximum adsorption capacity of 1010 mg g−1. In a neutral medium (at pH 7), 70 mg L−1 of Hb in 1.0 mL of aqueous solution could be effectively adsorbed by 1.0 mg of the AP-rGO framework, giving rise to an adsorption efficiency of 92.7%. The practical application of the AP-rGO framework is demonstrated by the removal of a highly abundant protein, i.e., hemoglobin, from complex biological sample matrices, e.g., human whole blood. The removal efficiency is well confirmed by sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) assay.
Co-reporter:Dan-Dan Zhang, Qing Chen, Lin-Lin Hu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 21) pp:4363-4369
Publication Date(Web):21 Apr 2015
DOI:10.1039/C5TB00544B
A Keggin-type cobalt mono-substituted silicotungstic acid doped with aniline (SiW11Co–PANI composite, where PANI denotes polyaniline) is prepared by a liquid phase method at room temperature. The obtained SiW11Co–PANI composite possesses a porous framework structure and has proven to be a promising adsorbent for the retention of proteins, which exhibits favorable selectivity toward the adsorption of ovalbumin from egg whites. 5.0 mg of SiW11Co–PANI composite gives rise to an adsorption efficiency of >70% for 100 mg L−1 ovalbumin in 1.0 mL of sample solution within a wide pH range of 3–9, and a maximum adsorption efficiency of 92% is achieved at pH 9. The adsorption behavior of ovalbumin onto the SiW11Co–PANI composite fits the Langmuir adsorption model, corresponding to a sorption capacity of 200.0 mg g−1. The retained ovalbumin could be readily recovered by using a 0.1 mol L−1 phosphate buffer at pH 5.6 as a stripping reagent, providing a recovery of 84.4%. Circular dichroism (CD) spectra illustrate virtually no change in the conformation of ovalbumin after the process of adsorption–desorption. The SiW11Co–PANI composite has been applied for the selective adsorption of ovalbumin from the chicken egg white, and SDS-PAGE assay demonstrates that high purity of ovalbumin is obtained.
Co-reporter:Quan-Xing Mao, Wen-Jing Wang, Xin Hai, Yang Shu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 29) pp:6013-6018
Publication Date(Web):22 Jun 2015
DOI:10.1039/C5TB00963D
The regulation of hydrophilicity/hydrophobicity of carbon dots (CDs) at will is most important. One pot simultaneous preparation of hydrophilic and/or hydrophobic CDs is herein reported, via a hydrothermal process with 1-butyl-3-methylimidazolium hexafluorophosphate as the carbon source in a H3PO4–ethanol medium. The hydrophilicity or hydrophobicity of CDs (or their proportions) is simply regulated by varying the H3PO4/ethanol molar ratio. Hydrophilic and hydrophobic CDs are obtained simultaneously with H3PO4/ethanol molar ratios within 0–1.72, while hydrophilic or hydrophobic CDs are the sole product obtained from H3PO4–BmimPF6 or BmimPF6-only systems. The CDs exhibit excitation-dependent maximum fluorescence at 360/440 nm (hydrophilic) and 430/510 nm (hydrophobic), with quantum yields of 17.0% and 7.7%, respectively. Both hydrophilic and hydrophobic CDs obtained by this approach exhibit favorable biocompatibility and offer great potential in bio-imaging as demonstrated for the fluorescent labeling and imaging of live HeLa cells.
Co-reporter:Qing Chen, Dan-Dan Zhang, Meng-Meng Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 34) pp:6964-6970
Publication Date(Web):28 Jul 2015
DOI:10.1039/C5TB01298H
A novel polyoxometalate (POM)-based organic–inorganic hybrid [C33H24O4]H3PMo12O40, namely, TPPA–PMo12, is prepared via a one-pot hydrothermal reaction between a Keggin POM (H3PMo12O40, PMo12) and a star-like N-donor ligand (tri(4-pyridylphenyl)amine, TPPA). The hybrid polyoxometalate is confirmed by characterization with XRD, FT-IR, TGA, SEM and EDS. It exhibits excellent adsorption performance towards β-lactoglobulin, and thus a solid-phase extraction procedure was established for the efficient and selective isolation of β-lactoglobulin from complex sample matrices. At pH 5.0, an adsorption efficiency of 99.2% is achieved for processing 100 μg mL−1 β-lactoglobulin in 1.0 mL aqueous solution with 0.5 mg TPPA–PMo12 as an adsorbent. The adsorption behavior of β-lactoglobulin fits the Langmuir model, corresponding to a theoretical adsorption capacity of 1428 mg g−1. The retained β-lactoglobulin could be readily recovered by rinsing with 0.05 mol L−1 Tris-HCl buffer, facilitating a recovery of 91.5%. The hybrid polyoxometalate was practically applied to the selective isolation of β-lactoglobulin from milk whey, and SDS-PAGE assay results clearly indicate that β-lactoglobulin of high-purity is obtained.
Co-reporter:Xin Hai, Quan-Xing Mao, Wen-Jing Wang, Xiao-Feng Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 47) pp:9109-9114
Publication Date(Web):02 Nov 2015
DOI:10.1039/C5TB01954K
Boron-doped graphene quantum dots (B-GQDs) are prepared via a one-pot acid-free microwave approach with graphene oxide as the carbon source and borax as the boron source. Boron atoms are incorporated into the graphene framework by attacking the defects in the graphene structure, deriving an atomic percentage of 1.44% in the final product. Boron atom doping into the graphene structure and restoration of defects in the graphene structure bring the obtained B-GQDs favorable photoluminescence behaviors. The as-prepared B-GQDs exhibit excitation-independent photoluminescence behaviors with an excitation/emission maximum at 320/430 nm, and a fluorescence quantum yield of 21.1%. Moreover, stable photoluminescence is observed within a wide range of pH 3.0–11.0. A tolerance to an external ionic strength of up to 2.0 mol L−1 KCl along with an excellent anti-photobleaching capability is achieved. The standard MTT assay suggests that the B-GQDs are of low cytotoxicity with favorable biocompatibility, and a cell viability of 87% could be achieved at 4.0 mg mL−1 of B-GQDs. The practical application of B-GQDs in bio-analysis is demonstrated by bio-imaging of HeLa cells.
Co-reporter:Yang Zhang, Li-Gang Xing, Xu-Wei Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 9) pp:5116
Publication Date(Web):February 18, 2015
DOI:10.1021/am508836m
Assembly of nano-objects with tunable size, morphology and function into integrated nanostructures is critical for the development of a novel nanosystem in adsorption, sensing and drug/gene delivery. We demonstrate herein the fabrication of ordered mesoporous carbon by assembling uniform and highly dispersed copper-oxide (CuxOy) nanoparticles into the mesopores via evaporation of solvent from the mixture of triblock copolymer, carbon source and metal nitrate hydrate. The ordered 2D hexagonal mesoporous carbon composite possesses a large surface area of 580.8 cm2/g, a uniform pore size of 5.4 nm, a large pore volume of 0.64 cm3/g and a high metal content of 3.32 wt %. The mesoporous composite exhibits excellent adsorption selectivity and high adsorption capacity to hemoglobin (Hb) under the synergistic effect of hydrophobic and metal-affinity interactions as well as size exclusion. This facilitates multimode adsorption of hemoglobin fitting Langmuir adsorption model and offers an adsorption capacity of 1666.7 mg g–1 for hemoglobin. The mesoporous composite is used for the isolation of hemoglobin from human whole blood with high purity. It demonstrates the potential of the copper-oxide nanoparticle-embedded mesoporous carbon composite in selective isolation/removal of specific protein species from biological sample matrixes.Keywords: copper-oxide nanoparticles; hemoglobin; mesoporous carbon; multimodal adsorption
Co-reporter:Wen-Jing Wang, Xin Hai, Quan-Xing Mao, Ming-Li Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 30) pp:16609
Publication Date(Web):July 14, 2015
DOI:10.1021/acsami.5b04172
In the present study, octa-aminopropyl polyhedral oligomeric silsesquioxane hydrochloride salt (OA-POSS) functionalized carbon dots (CDs/POSS) are prepared by a one-pot approach with glycerol as carbon source and solvent medium. OA-POSS serves as a passivation agent, and it is obtained via hydrolytic condensation of 3-aminopropyltriethoxysilane (APTES). During the functionalization process, the amino groups on OA-POSS combine with carboxylic groups on the bare CDs via formation of amide bond to construct organic–inorganic hybrid carbon dots. The obtained CDs/POSS are well dispersed in aqueous medium with a diameter of ca. 3.6 nm. It is demonstrated that CDs/POSS provide favorable photoluminescent property with a quantum yield of 24.0%. They also exhibit resistance to photobleaching and excellent photoluminescence stability in the presence of biological sample matrix (characterized by heavy metals and organic molecules), which facilitate cell imaging in biological systems. Both the photoluminescent emission wavelength and the fluorescence intensity depend closely on the excitation wavelength, and thus, it provides a potential for multicolor imaging as demonstrated with HeLa cells and MCF-7 cells.Keywords: carbon dots; cell imaging; functionalization; organic−inorganic hybrid; polyhedral oligomeric silsesquioxane
Co-reporter:Ting Yang, Xiao-Yu Zhang, Xiao-Xiao Zhang, Ming-Li Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 38) pp:21287
Publication Date(Web):September 8, 2015
DOI:10.1021/acsami.5b05606
The screening of suitable sorption medium is the key for highly selective solid phase extraction (SPE) of heavy metals. Herein, we demonstrate a universal protocol for producing selective SPE adsorbent through an evolutional approach based on phage display peptide library. By choosing chromium(III) as the model target, immobilized Cr(III) resins are first prepared using Ni-NTA affinity resins for the interaction with NEB heptapeptide phage library. After three rounds of positive biopanning against target Cr(III) and negative biopanning against foreign metal species, Cr(III) binding phages with high selectivity are obtained. The binding affinity and selectivity are further assessed with ELISA. The phages bearing peptide (YKASLIT) is finally chosen and immobilized on cytopore beads for Cr(III) preconcentration. The retained Cr(III) is efficiently recovered by 0.10 mol L–1 HNO3 and quantified with ICP-MS. By loading 4000 μL of sample solution at pH 7.0 for 2 h and stripping with 400 μL of 0.10 mol L–1 HNO3, a linear range of 0.05–0.50 μg L–1 is achieved along with an enrichment factor of 7.1. The limit of detection is derived to be 15 ng L–1 (3σ, n = 7) with a RSD of 3.6% (0.25 μg L–1, n = 7). The procedure is validated by analyzing chromium content in a certified reference material GBW08608 (simulate water). In addition, chromium speciation in real water samples is demonstrated. Cr(VI) is first converted into Cr(III), and the latter subjected to the sorption onto the Cr(III) binding phage, followed by elution and quantification of the total chromium amount, and finally speciation is achieved by difference.Keywords: Cr(III); metal binding peptide; phage display peptide library; preconcentration; solid phase extraction
Co-reporter:Shuai Chen, Ling Wei, Xu-Wei Chen, and Jian-Hua Wang
Analytical Chemistry 2015 Volume 87(Issue 21) pp:10902
Publication Date(Web):October 1, 2015
DOI:10.1021/acs.analchem.5b02453
It is of great importance to develop novel and sensitive sensing materials for the detection of proteins and microorganisms to fulfill the demand of disease diagnosis. As the selectivity and sensitivity of sensing systems are highly dependent on the receptor, the fluorescent sensor array with imidazolium ionic liquids (ILs) and ionic liquid–quantum dots conjugates as semiselective receptors is developed for protein/bacteria differential sensing or discrimination. The IL sensing system formed by 1,3-dibutylimidazolium chloride (BBimCl), 1,3-diethylimidazolium bromine (EEimBr), 1,3-dibutylimidazolium bromine (BBimBr), 1,3-dihexylimidazolium bromine (HHimBr), and 1,3-dioctylimidazolium bromine (OOimBr) and the IL@QDs/QDs sensing system formed by CdTe, BBimCl@CdTe, EEimBr@CdTe, BBimBr@CdTe, and HHimBr@CdTe are tested, by transferring the interaction binding difference between receptors and proteins to the fluorescent response pattern. The IL sensing system is applied to the identification of 48 samples (8 proteins at 500 nM) with an accuracy of 91.7%. For the IL@QDs/QDs sensing system, 8 proteins are completely distinguished with 100% accuracy at a very low concentration level of 10 nM. Remarkably, 36 training cases (6 strains of bacteria from 3 different species) are discriminated with 100% (OD600 of 0.1).
Co-reporter:Mei-Ling Chen, Hui Wang, Quan-Xing Mao, Xu-Wei Chen, Jian-Hua Wang
Carbon 2015 Volume 85() pp:335-343
Publication Date(Web):April 2015
DOI:10.1016/j.carbon.2014.12.108
A ferrate functionalized graphene-based composite is prepared by growth of hydrous ferric oxide (FeOOH) on the polyethylene glycol (PEG) modified graphene oxide (GO) sheets. The obtained GO–PEG–FeOOH composite is characterized by ATR-FTIR, TEM, AFM, XPS and ICP-MS. The PEGylation significantly changes the surface property of the bare graphene oxide, which not only generates a nano-bio-interface for protein interaction but also reduces the non-specific adsorption of proteins. The PEGylation and growth of FeOOH nanorods on GO sheets obviously enhanced the selectivity toward the adsorption of albumin through strong hydrogen bonding interaction, exhibiting an ultra-high adsorption capacity of 1377.4 mg g−1 for bovine serum albumin (BSA). It is obviously higher than those achieved by any hitherto reported graphene based materials and other carbon nanomaterials. Albumin retained by the composite could be effectively recovered with a 4.0 mM B–R buffer through the affinity of boronic acid toward protein, giving rise to a recovery of 70%. Circular dichroism (CD) spectra indicate no conformational change for BSA during the process of adsorption/desorption. The practical applicability of the GO nanocomposite is further demonstrated by the selective adsorption/isolation of albumin from complex biological samples matrixes, e.g., human whole blood.
Co-reporter:Bo Hu, Ning Wang, Lu Han, Ming-Li Chen, Jian-Hua Wang
Acta Biomaterialia 2015 Volume 11() pp:511-519
Publication Date(Web):1 January 2015
DOI:10.1016/j.actbio.2014.09.005
Abstract
A novel bactericidal material comprising rod-shaped core–shell–shell Au–Ag–Au nanorods is constructed as a nanoheater in the near-infrared (NIR) region. The outer Au shell melts under laser irradiation and results in exposure of the inner Ag shell, facilitating the controlled release of the antibacterial Ag shell/layer or Ag+. This results in the Au–Ag–Au nanorods having a favorable bactericidal ability as it combines the features of physical photothermal ablation sterilization of the outer Au shell and the antibacterial effect of the inner Ag shell or Ag+ to the surrounding bacteria. The sterilizing ability of Au–Ag–Au nanorods is investigated with Escherichia coli O157:H7 as a model bacterial strain. Under low-power NIR laser irradiation (785 nm, 50 mW cm−2), the Au–Ag–Au nanoheater exhibits a higher photothermal conversion efficiency (with a solution temperature of 44 °C) with respect to that for the Au–Ag nanorods (39 °C). Meanwhile, a much improved stability with respect to Au–Ag nanorods is observed, i.e., 16 successive days of monitoring reveal virtually no change in the ultraviolet–visible spectrum of Au–Ag–Au nanorods, while a significant drop in absorption along with a 92 nm red shift of Localized Surface Plasmon Resonance is recorded for the Au–Ag nanorods. This brings an increasing bactericidal efficiency and long-term stability for the Au–Ag–Au nanorods. At a dosage of 10 μg ml−1, a killing rate of 100% is reached for the E. coli O157:H7 cells under 20 min of irradiation. The use of Au–Ag–Au nanorods avoids the abuse of broad-spectrum antibiotics and reduces the damage of tissues by alleviating the toxicity of silver under controlled release and by the use of low-power laser irradiation. These features could make the bimetallic core–shell–shell nanorods a favorable nanoheater for in vivo biomedical applications.
Co-reporter:Yi Cai, Shao-Hua Li, Shuai Dou, Yong-Liang Yu, and Jian-Hua Wang
Analytical Chemistry 2015 Volume 87(Issue 2) pp:1366
Publication Date(Web):December 16, 2014
DOI:10.1021/ac5042457
The scope of dielectric barrier discharge (DBD) microplasma as a radiation source for optical emission spectrometry (OES) is extended by nickel carbonyl vapor generation. We proved that metal carbonyl completely avoids the extinguishing of plasma, and it is much more suitable for matching the DBD excitation and OES detection with respect to significant DBD quenching by concomitant hydrogen when hydride generation is used. A concentric quartz UV reactor allows sample solution to flow through the central channel wherein to efficiently receive the uniformly distributed UV irradiation in the confined cylindrical space between the concentric tubes, which facilitates effective carbonyl generation in a nickel solution. The carbonyl is transferred into the DBD excitation chamber by an argon stream for nickel excitation, and the characteristic emission of nickel at 232.0 nm is detected by a charge-coupled device (CCD) spectrometer. A 1.0 mL sample solution results in a linear range of 5–100 μg L–1 along with a detection limit of 1.3 μg L–1 and a precision of 2.4% RSD at 50 μg L–1. The present DBD–OES system is validated by nickel in certified reference materials.
Co-reporter:Ting Yang, Lin-Yu Ma, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2015 vol. 30(Issue 4) pp:929-935
Publication Date(Web):11 Feb 2015
DOI:10.1039/C4JA00418C
Metallothioneins (MTs) are low molecular weight, cysteine-rich proteins widely distributed in nature. Two isoforms of MT, e.g., metallothionein isolated from rabbit liver (rMT) and recombined cyanobacteria metallothionein (SmtA), were immobilized on spherical SiO2 particles to evaluate their biosorption behaviors for cadmium. We found that cadmium binding on both MT isoforms is pH dependent and follows Langmuir adsorption, and their adsorption dynamic fits the pseudo-second-order kinetics model. The affinity of cadmium on rMT is higher than that on SmtA, which is in accordance with the HSAB theory. On the other hand, however, SmtA exhibits a higher cadmium sorption capacity than rMTs both statically and dynamically. The SmtA–SiO2 composite was thus used to pack a mini-column for the evaluation of cadmium preconcentration. The cadmium retained on the SmtA surface was recovered with a small amount of thiourea in nitric acid and quantified by graphite furnace atomic absorption spectrometry (GFAAS). Within a range of 5–100 ng L−1 and a sample volume of 1 mL, an enrichment factor of 13.8 was achieved along with a detection limit of 1.4 ng L−1, and a precision of 3.2% RSD at 50 ng L−1. The procedure was validated by analyzing cadmium in certified reference materials and a series of environmental water samples.
Co-reporter:Xiao-Feng Wang, Yue Zhang, Yang Shu, Xu-Wei Chen and Jian-Hua Wang
RSC Advances 2015 vol. 5(Issue 40) pp:31496-31501
Publication Date(Web):27 Mar 2015
DOI:10.1039/C5RA00036J
A novel polymeric ionic liquid, poly(3-n-dodecyl-1-vinylimidazolium) bromide (poly(C12vim)Br), is prepared via solution polymerization. The poly(C12vim)Br exhibits excellent adsorption performance toward hemoglobin in the presence of other protein species. It is shown that favorable adsorption of hemoglobin is achieved at pH 8.0, and the variation of ionic strength has virtually no effect on the adsorption of hemoglobin at a NaCl concentration up to 0.4 mol L−1. A maximum adsorption capacity of 205.4 mg g−1 is derived for hemoglobin. An adsorption efficiency of 93.8% is obtained by processing 80 μg mL−1 of hemoglobin in 1.0 mL of solution with 2 mg of poly(C12vim)Br, and afterwards the use of 1.0 mL of sodium dodecyl sulfate (SDS, 0.5%, m/v) provides a recovery of ca. 86.3%. It is indicated that the process of adsorption/desorption causes a slight conformational change for hemoglobin, while its structure remains predominantly α-helix. The poly(C12vim)Br has been used for the adsorption of hemoglobin from complex biological sample matrixes, e.g., human whole blood, and the favorable separation and purification performance is demonstrated by SDS-PAGE assays.
Co-reporter:Xiao-Feng Wang, Xin Hai, Yang Shu, Xu-Wei Chen and Jian-Hua Wang
Analytical Methods 2015 vol. 7(Issue 22) pp:9529-9534
Publication Date(Web):05 Oct 2015
DOI:10.1039/C5AY02308D
A novel cross-linked co-polymeric ionic liquid is prepared via mini-emulsion polymerization by using N-vinyl-3-(2-methoxy-2-oxyl ethyl) imidazolium chloride as a monomer and 1,4-butanediyl-3,3′-bis-l-vinylimidazoliurn dibromide as a crosslinker. The as-synthesized material is used as an adsorbent for the solid-phase extraction of curcuminoids. Ion-exchange and hydrogen-bonding interactions contribute to a highly efficient adsorption of curcuminoids onto the cross-linked co-polymeric ionic liquid, and a maximum adsorption capacity of 108.7 μg mg−1 is achieved. Both the adsorption and desorption of curcuminoids could be achieved within 15 s, giving rise to a fast extraction process. This developed extraction protocol is applied to the isolation of curcuminoids from Curcuma longa Linn, and HPLC analysis demonstrates obvious improvement in extraction efficiency as compared with conventional extraction methodologies.
Co-reporter:Yong-Liang Yu, Yu-Ting Zhuang and Jian-Hua Wang
Analytical Methods 2015 vol. 7(Issue 5) pp:1660-1666
Publication Date(Web):04 Feb 2015
DOI:10.1039/C5AY00003C
During the last few years, various miniaturized optical emission spectrometry (OES) systems based on dielectric barrier discharge (DBD) micro-plasma as a radiation source have gained novel advances and exhibited powerful capability in the field of trace elemental analysis. At the heart of such analytical systems, DBD micro-plasma possesses a series of unique features and it is a promising technique for the development of miniaturized atomic spectrometric instruments, including OES spectrometers. This mini-review presents and discusses the progress of DBD-OES systems in the analysis of gaseous species and those in an aqueous medium. In the case of gaseous species, the approaches are focused on direct detection by DBD-OES after appropriate sample introduction. For the case of analyzing target species in an aqueous medium, the entire analytical process includes a DBD-OES detection unit, electrothermal vaporization or a chemical vapor generation unit. Special emphasis has been focused on the novel applications of DBD-OES systems and its hyphenation with various analytical techniques. Future perspectives of DBD-OES systems for trace elemental analysis are described.
Co-reporter:Yang Shu, Ying Meng, Ming-Li Chen, Jian-Hua Wang
Chinese Chemical Letters 2015 Volume 26(Issue 12) pp:1460-1464
Publication Date(Web):December 2015
DOI:10.1016/j.cclet.2015.10.013
The hierarchical metal–organic frameworks (MOFs), such as Y(BTC)(H2O)6, are prepared with yttrium nitrate and benzene-1,3,5-tricarboxylic acid at room temperature. The product is characterized by Fourier transform infrared (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) and thermogravimetric analysis (TGA). The Y(BTC)(H2O)6 particles are sufficiently rigid for performing solid phase extraction and they exhibit favorable selectivity toward the adsorption of hemoglobin. The adsorption behavior of hemoglobin onto the Y(BTC)(H2O)6 fits the Langmuir adsorption model with a theoretical adsorption capacity of 555.6 mg g−1. An adsorption efficiency of 87.7% for 100 μg mL−1 hemoglobin in 1 mL sample solution (at pH 6.0) is achieved with 0.40 mg Y(BTC)(H2O)6. 77.3% of the retained hemoglobin is readily recovered using a 0.5% (m/v) SDS solution as the stripping reagent. Circular dichroism spectra indicated that the conformation of hemoglobin is maintained during the adsorption–desorption process. The MOFs material is applied for the isolation of hemoglobin from human blood and the purity of the obtained hemoglobin is further verified by sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS–PAGE).The metal–organic frameworks, Y(BTC)(H2O)6, exhibits favorable adsorption toward hemoglobin that is attributed to the coordination interactions between the metal cations and the histidine residues in proteins.
Co-reporter:Ting Yang, Ming-Li Chen, Jian-Hua Wang
TrAC Trends in Analytical Chemistry 2015 Volume 66() pp:90-102
Publication Date(Web):March 2015
DOI:10.1016/j.trac.2014.11.016
•We review biosorption of heavy-metal species by microbes or biological cells.•Genetic modifications for selective sorption and speciation of heavy-metal species.•Chemical modifications for selective sorption and speciation of heavy-metal species.•Bioaccumulation of heavy-metal species and their analysis and speciation.Bioaccumulation describes the ability for microbes or other biological cells to accumulate heavy-metal species from the ambient environment. It has attracted extensive attention in the field of heavy metal remediation and precious metal recovery. Bioaccumulation has also shown great potential for adsorption and preconcentration of ultra-trace levels of heavy metals for their analysis and speciation. Genetic engineering and chemical modification of biological cells open up new avenues for bioaccumulative preconcentration of heavy-metal species for selective analysis and speciation of such metals in combination with spectrometric techniques. We focus on recent progress in genetic and chemical approaches to bioremediation and their applications in selective preconcentration and speciation of heavy-metal species. We also outline the uptake mechanisms of bioaccumulation and key issues in the biosorption of heavy metals and their analysis and speciation. Finally, we discuss future perspectives in the bioaccumulation of heavy-metal species and their analysis and speciation.
Co-reporter:Shuai Chen, Xin Hai, Xu-Wei Chen, and Jian-Hua Wang
Analytical Chemistry 2014 Volume 86(Issue 13) pp:6689
Publication Date(Web):May 26, 2014
DOI:10.1021/ac501497d
We report a facile green approach for in situ growth of silver nanoparticles (AgNPs) on the surface of graphene quantum dots (GQDs). GQDs serve as both reducing agent and stabilizer, and no additional reducing agent and stabilizer is necessary. The GQDs/AgNPs hybrid exhibits a superior absorbance fading response toward the reduction of H2O2. A simple colorimetric procedure is thus proposed for ultrasensitive detection of H2O2 without additional chromogenic agent. It provides a record detection limit of 33 nM for the detection of H2O2 by the AgNPs-based sensing system. This colorimetric sensing system is further extended to the detection of glucose in combination with the specific catalytic effect of glucose oxidase for the oxidation of glucose and formation of H2O2, giving rise to a detection limit of 170 nM. The favorable performances of the GQDs/AgNPs hybrid are due to the peroxidase-like activity of GQDs.
Co-reporter:Li-Ming Shen, Qing Chen, Zheng-Yue Sun, Xu-Wei Chen, and Jian-Hua Wang
Analytical Chemistry 2014 Volume 86(Issue 10) pp:5002
Publication Date(Web):April 28, 2014
DOI:10.1021/ac500601k
Recently, the development of optical probes for the assay of thiols, e.g., cysteine (Cys), homocysteine (Hcy), and glutathione (GSH), has been an active research area due to their biological significance. We have found that carbon dots (C-dots) exhibit direct reduction of Ag+ to elemental silver (Ag0) and the resulting Ag0 formed a silver nanoparticle (Ag-NP) spontaneously. The excessive C-dots consume free Ag+ in the solution by binding Ag+ with functional groups on the C-dots surface and thus inhibits the growth of Ag-NPs. Biothiols can coordinate with Ag+ through thiol groups, and afterward, the Ag+-biothiol complex gradually releases free Ag+ to ensure its reduction by C-dots and thus facilitates the growth of Ag-NPs on C-dots surface. A colorimetric assay procedure is thus developed for fast detection of biothiols based on Ag-NPs plasmon absorption. The linear calibration range can be regulated by controlling the concentration of Ag+. Two linear ranges were obtained for the biothiols assay at different levels, which offer ultrahigh sensitivity for the assay of an ultratrace amount of biothiols with detection limits of 1.5, 2.6, and 1.2 nM for Cys, Hcy, and GSH, respectively. The precisions for the assay of Cys, Hcy, and GSH at 20 nM are achieved as 3.1%, 3.1%, and 2.4%. In addition, the sensing system exhibits good selectivity toward biothiols in the presence of other amino acids, the major metal cations, and biomolecules in biological fluids. For the assay of 20 nM Cys, 150-fold of coexisting amino acids, 2500-fold of Ca2+, Mg2+, glucose, and ascorbic acid, and 38-fold of HSA are tolerated. In the assay of Cys in human plasma, spiking recoveries of 94% to 108% are obtained at 100 μM.
Co-reporter:Xiaofeng Wang, Ligang Xing, Yang Shu, Xuwei Chen, Jianhua Wang
Analytica Chimica Acta 2014 Volume 837() pp:64-69
Publication Date(Web):21 July 2014
DOI:10.1016/j.aca.2014.06.002
•Polymeric ionic liquid (PIL) microspheres are adopted for DNA isolation.•Fast adsorption equilibrium of DNA on PIL is achieved within 1 min.•The adsorption capacity of the PIL is much higher than that of the reported adsorbents.A novel polymeric ionic liquid (PIL) microsphere, poly(1-vinyl-3-(2-methoxy-2-oxyl ethyl)imidazolium) hexafluorophosphate, is prepared via W/O emulsion polymerization. Rapid ion-exchange between the anionic moieties of PIL and DNA fragments is demonstrated facilitating the exchange equilibrium to be reached within 1 min. The PIL microspheres exhibit a high capacity of 190.7 μg mg−1 for DNA adsorption. A fast DNA isolation protocol is thus developed with the PIL microspheres as solid phase adsorbent. It is feasible to facilitate DNA adsorption or stripping from the microspheres by simply regulating the concentration of salt. DNA adsorption is facilitated at low salt concentration, while higher concentration of salt entails DNA recovery from the microspheres. In practice, the retained DNA could be readily recovered with 1.0 mol L−1 NaCl as stripping reagent, giving rise to a recovery of ca. 80.7%. The PIL microspheres are used for the adsorption/isolation of plasmid DNA from E. coli cell culture, demonstrating a superior adsorption performance with respect to that achieved by a commercial Plasmid Miniprep Kit.
Co-reporter:Yong-Liang Yu, Yi Cai, Ming-Li Chen, Jian-Hua Wang
Analytica Chimica Acta 2014 Volume 809() pp:30-36
Publication Date(Web):27 January 2014
DOI:10.1016/j.aca.2013.11.054
•Dielectric barrier discharge (DBD) is for the first time used as a radiation source for the excitation of bromine and its emission.•A DBD–optical emission spectrometric (OES) system was developed for the detection of bromide and bromate.•The DBD–OES system has been demonstrated by screening trace bromide and bromate in a series of environmental water samples.Dielectric barrier discharge (DBD) at atmospheric pressure provides an efficient radiation source for the excitation of bromine and it is used for the first time for optical emission spectrometric (OES) detection of bromide and bromate. A portable DBD–OES system is developed for screening potential pollution from bromide and bromate in environmental waters. Bromide is on-line oxidized to bromine for in-situ generation of volatile bromine. Meanwhile, a helium stream carries bromine into the DBD micro-plasma for its excitation at a discharging voltage of 3.7 kV and optical emission spectrometric detection with a QE65000 charge-coupled device (CCD) spectrometer in the near-infrared spectral region. Similarly, the quantification of bromate is performed by its pre-reduction into bromide and then oxidized to bromine. The spectral characteristics and configuration of the DBD micro-plasma excitation source in addition to the oxidation vapor generation of bromine have been thoroughly investigated. With a sampling volume of 1 mL, a linear range of 0.05–10.0 mg L−1 is obtained with a detection limit of 0.014 mg L−1 by measuring the emission at 827 nm. A precision of 2.3% is achieved at 3 mg L−1 bromide. The system is validated by bromine detection in certified reference material of laver (GBW10023) at mg L−1 level, giving rise to satisfactory agreement. In addition, it is further demonstrated by screening trace bromide and bromate as well as spiking recoveries in a series of environmental water samples.
Co-reporter:Jia-Wei Liu, Meng-Meng Wang, Yue Zhang, Lu Han, Xu-Wei Chen and Jian-Hua Wang
RSC Advances 2014 vol. 4(Issue 106) pp:61936-61943
Publication Date(Web):12 Nov 2014
DOI:10.1039/C4RA09808K
Polymeric ionic liquid (PIL), poly(1-vinyl-3-ethylimidazolium bromide) (P(ViEtIm+Br−)), modified reduced graphene oxide (rGO) nanosheets (PIL–rGO) are prepared during the reduction process using hydrazine hydrate. The as-prepared PIL–rGO is further self-assembled onto the surface of SiO2 nanoparticles through electrostatic interactions as demonstrated by TEM & SEM images. The obtained PIL–rGO@SiO2 nano-hybrid exhibits highly selective adsorption toward acidic protein, i.e., ovalbumin (Ova) as a model in the present case. The strong electrostatic attractions and π–π interactions between Ova and the nano-hybrid are the main driving forces for protein adsorption. An adsorption efficiency of ca. 95% is achieved for 150 mg L−1 Ova in a 4 mM B–R buffer at pH 5, along with an ultra-high adsorption capacity of ca. 917.4 mg g−1 as compared to those adsorbents for similar purposes. The adsorbed Ova could be effectively recovered from the surface of the nano-hybrid by using a 0.4% (w/v) SDS solution, giving rise to a recovery of ca. 70%. The practical applicability of the PIL–rGO@SiO2 nano-hybrid is demonstrated by selective isolation and removal of Ova from a complex biological sample matrix, i.e., chicken egg white.
Co-reporter:Quan-Xing Mao, Hui Wang, Yang Shu, Xu-Wei Chen and Jian-Hua Wang
RSC Advances 2014 vol. 4(Issue 16) pp:8177-8182
Publication Date(Web):14 Jan 2014
DOI:10.1039/C3RA46736H
A novel dual-ionic liquid (IL) microemulsion system is developed with IL 1-decyl-3-methylimidazolium bromide (DmimBr) as the surfactant and IL 1-butyl-3-methylimidazolium hexaflourophosphate (BmimPF6) as a substitute for organic solvent. The phase diagram of this dual-IL microemulsion system clearly shows the formation of a single phase within a wide range of BmimPF6 (1.76–98.3%, wt) and in the presence of an appropriate amount of DmimBr and water. The microemulsion is characterized by means of FT-IR spectra, dynamic light scattering and molecular probe. The dual-IL microemulsion system has been demonstrated to be effective for the extraction of proteins, and exhibited an obvious improvement in extraction efficiency for hemoglobin in comparison with pure BmimPF6. When 100 μL microemulsion is used to extract 100 μg mL−1 of proteins in an equal volume of sample solution, high selective extraction of hemoglobin (Hb) has been observed at pH 5. This might be attributed to the coordination interaction between the heme group of Hb and the imidazolium cationic moiety in the ionic liquids. Hb transferred into the microemulsion can be readily recovered by back extraction with Britton–Robinson buffer at pH 12, giving rise to a recovery of 55.6%. The dual-IL microemulsion system is practically applied to the isolation of Hb from human whole blood and the SDS-PAGE indicates that hemoglobin has been selectively isolated from human blood in the presence of co-existing protein species.
Co-reporter:Jia-Wei Liu, Ting Yang, Shuai Chen, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2013 vol. 1(Issue 6) pp:810-818
Publication Date(Web):30 Nov 2012
DOI:10.1039/C2TB00334A
A novel functionalized graphene-based composite is prepared by successive modification of graphene oxide (GO) with epichlorohydrin (ECH), iminodiacetic acid (IDA) and 1-phenylboronic acid (1-PBA) through covalent functionalization and then chelating with nickel ions. Characterizations by FT-IR, XRD, SEM, TGA and ICP-MS demonstrate the successful modification of the graphene surface, resulting in a GO–PBA–IDA–Ni composite with a Ni2+ immobilization amount of 3.01 × 10−3 mol g−1. The composite shows favorable selectivity for the adsorption of lysozyme (Lys). In practice, a homogeneous GO–PBA–IDA–Ni film with a thickness of ca. 1.0 μm is fabricated by filtering the composite through a cellulose membrane with a pore aperture of 1.2 μm. The GO–PBA–IDA–Ni film is subsequently fastened into a rounded membrane cartridge and incorporated into a sequential injection system for on-line selective isolation of Lys. An adsorption efficiency of ca. 96% is achieved for 25 μg ml−1 Lys in 500 μl of sample solution at a loading rate of 5 μl s−1. Metal affinity and electrostatic interactions are the main driving forces for governing the protein adsorption behaviors. The retained Lys is readily recovered by a borate buffer (pH 10) containing 1.0 mol l−1 NaCl and 20 mmol l−1 imidazole, giving rise to a recovery of ca. 90%. The practical applicability of the composites is demonstrated by selective isolation of Lys from chicken egg white, and SDS-PAGE assay indicates that Lys is selectively isolated with high purity from complex matrices.
Co-reporter:Mei-Ling Chen, Li-Ming Shen, Shuai Chen, Hui Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2013 vol. 1(Issue 20) pp:2582-2589
Publication Date(Web):25 Mar 2013
DOI:10.1039/C3TB20234H
β-FeOOH has shown promise as a new contrast agent in magnetic resonance imaging (MRI), however, sensitive and accurate MR imaging is largely limited by its low transverse relaxivity (r2). Herein, for the first time we report in situ growth of β-FeOOH nanorods onto PEGylated graphene oxide (GO) sheets to produce a nanocomposite, e.g., GO-PEG–β-FeOOH. This nanocomposite exhibits a record ultra-high transverse relaxivity (r2) value of 303.81 mM−1 s−1, that is, >60 times higher than those achieved by hitherto reported β-FeOOH based MRI contrast agents. This well facilitates its practical use as a contrast agent for in vivo MR imaging. PEG on the surface of the GO nanocomposite improved the colloidal stability in aqueous medium. In addition, in vitro cell viability tests demonstrated that GO-PEG–β-FeOOH has minimal cellular toxicity. GO-PEG–β-FeOOH has been used for loading doxorubicin hydrochloride (DOX) with a capacity of 1.35 mg mg−1, which exhibits high efficiency in Hela cell apoptosis. These results indicated that GO-PEG–β-FeOOH provides an effective alternative to the existing nanoparticle-based contrast agents for non-invasive in vivo MR imaging and cancer therapy.
Co-reporter:Bo Hu, Li-Pei Zhang, Xu-Wei Chen and Jian-Hua Wang
Nanoscale 2013 vol. 5(Issue 1) pp:246-252
Publication Date(Web):25 Oct 2012
DOI:10.1039/C2NR32457A
A hybrid bactericidal material, gold nanorod-covered kanamycin-loaded hollow SiO2 (HSKAurod) nanocapsules, is constructed. The hybrid material combines the features of a chemical drug with photothermal physical sterilization which decreases the dosage of broad-spectrum antibiotic and the physical damage of biological systems. Hollow SiO2 nanocapsules are used as carriers for drug delivery. The nanocapsules load a model drug, kanamycin, and are covered with gold nanorods to avoid drug leakage and realize photothermal treatment. The sterilizing effect on the bacterial strain is investigated by incubating E. coli BL21 with the hybrid nanocapsules and irradiating under near-infrared light (NIR) for 20 min. A bactericidal effect, i.e., a sterilizing rate of 53.47%, is achieved for the HSKAurod nanocapsules under NIR irradiation, with respect to a net sum sterilizing rate of 34.49% for the individual components of the HSKAurod nanocapsules, e.g., carrier nanocapsules, chemical sterilization of kanamycin and physical sterilization due to the gold nanorods under NIR irradiation. It is demonstrated that the combination of chemical drug and physical sterilization results in an obvious synergistic effect and makes the sterilization more effective. This novel hybrid has great potential as an adjuvant therapeutic alternative material for sterilization or even for the control of disease.
Co-reporter:Yang Shu, Lu Han, Xiaofeng Wang, Xuwei Chen, and Jianhua Wang
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 22) pp:12156
Publication Date(Web):October 28, 2013
DOI:10.1021/am404069f
A hydrophilic ionic liquid (methylimidazolium chloride, NmimCl)-polyvinyl chloride ionomer (NmimCl-PVC) was prepared by immobilizing and confining N-methylimidazole onto PVC chains. The NmimCl-PVC ionomer exhibits a 4-fold enhancement on the fluorescence intensity with respect to that of NmimCl, attributing to the confinement of ionic liquid by the PVC chain. The fluorescence is excitation-dependent with a maximum at λem 430 nm when excited at 325 nm. In addition, the fluorescence intensity of NmimCl-PVC ionomer increases remarkably with the loading ratio of N-methylimidazole in the range of 4.3–15.1%. The fluorescence quantum yield and lifetime were derived to be 0.112/7.1 ns for the NmimCl-PVC ionomer and 0.063/8.8 ns for NmimCl. Furthermore, hemoglobin is selectively adsorbed by NmimCl-PVC and causes significant fluorescence quenching of the ionomer via dynamic quenching and energy transfer between NmimCl-PVC and hemoglobin. A solid surface fluorimetric procedure was developed for surface adsorption and preconcentration of hemoglobin followed by in situ detection. A linear dynamic range of 0.3–26.2 μg mg–1 is achieved with a detection limit of 0.1 μg mg–1. Regarding hemoglobin in aqueous solution, the linear range 5–300 μg mL–1 is achieved along with a detection limit of 2 μg mL–1.Keywords: fluorescence enhancement; hemoglobin; immobilization/confinement; ionic liquid;
Co-reporter:Ting Yang, Jia-Wei Liu, Cuibo Gu, Ming-Li Chen, and Jian-Hua Wang
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 7) pp:2767
Publication Date(Web):March 13, 2013
DOI:10.1021/am400578y
ArsR is a metalloregulatory protein with high selectivity and affinity toward arsenic. We hereby report the expression of ArsR in Escherichia coli by cell engineering, which significantly enhances the adsorption/accumulation capacity of methylated arsenic species. The ArsR-expressed E. coli cells (denoted as E. coli-ArsR) give rise to 5.6-fold and 3.4-fold improvements on the adsorption/accumulation capacity for monomethylarsonic acid (MMA) and dimethylarsinic acid (DMA), with respect to native E. coli cells. The uptake of MMA and DMA by the E. coli-ArsR is a fast process fitting Langmuir adsorption model. It is interesting to note that the accumulation of methylated arsenic is virtually not affected by the presence of competing heavy-metal species, at least 10 times of Cd(II) and Pb(II) are tolerated for the adsorption of 1 mg L–1 methylated arsenic. In addition, an ionic strength of up to 2 g L–1 Na+ poses no obvious effect on the sorption of 1 mg L–1 MMA and DMA. Furthermore, the accumulation of MMA and DMA is less sensitive to the variation of pH value, with respect to the blank control cells. Consequently, 82.4% of MMA and 96.3% of DMA at a concentration of 50 μg L–1 could be readily removed from aqueous medium by 12 g L–1 of E. coli-ArsR. This illustrates a great potential for the E. coli-ArsR for selective remediation of methylated arsenic species in waters, even in the presence of a high concentration of salts.Keywords: accumulation; ArsR; genetically engineering; metalloregulatory protein; methylated arsenic; remediation;
Co-reporter:Liming Shen, Lipei Zhang, Meiling Chen, Xuwei Chen, Jianhua Wang
Carbon 2013 Volume 55() pp:343-349
Publication Date(Web):April 2013
DOI:10.1016/j.carbon.2012.12.074
A cationic branched polyelectrolyte of large molecular weight, i.e., polyethylenimine (PEI) of 25,000 Da, was used as both a carbon source and a passivating agent to prepare photoluminescent carbon nanoparticles (CNPs) in one step. In contrast to the previously reported pH-insensitive CNPs, these CNPs have a distinct pH-sensitive feature that gives them the potential to serve as a proton sensor in monitoring cell metabolization process with proton release. When incubated with HeLa cells, the CNPs could readily penetrate the cell membrane and exhibit low cytotoxicity and favorable biocompatibility. The CNPs have been used for HeLa cell imaging.
Co-reporter:Mei-Ling Chen, Ye-Ju He, Xu-Wei Chen, and Jian-Hua Wang
Bioconjugate Chemistry 2013 Volume 24(Issue 3) pp:387
Publication Date(Web):February 21, 2013
DOI:10.1021/bc3004809
We report a novel quantum-dot-conjugated graphene, i.e., hybrid SiO2-coated quantum dots (HQDs)-conjugated graphene, for targeted cancer fluorescent imaging, tracking, and monitoring drug delivery, as well as cancer therapy. The hybrid SiO2 shells on the surface of QDs not only mitigate its toxicity, but also protect its fluorescence from being quenched by graphene. By functionalizing the surface of HQDs-conjugated graphene (graphene-HQDs) with transferrin (Trf), we developed a targeted imaging system capable of differential uptake and imaging of cancer cells that express the Trf receptor. The widely used fluorescent antineoplastic anthracycline drug, doxorubicin (DOX), is adsorbed on the surface of graphene and results in a large loading capacity of 1.4 mg mg–1. It is advantageous that the new delivery system exhibits different fluorescence color in between graphene-HQDs and DOX in the aqueous core upon excitation at a same wavelength for the purpose of tracking and monitoring drug delivery. This simple multifunctional nanoparticle system can deliver DOX to the targeted cancer cells and enable us to localize the graphene-HQDs and monitor intracellular DOX release. The specificity and safety of the nanoparticle conjugate for cancer imaging, monitoring, and therapy has been demonstrated in vitro.
Co-reporter:Yong-Liang Yu, Shuai Dou, Ming-Li Chen and Jian-Hua Wang
Analyst 2013 vol. 138(Issue 6) pp:1719-1725
Publication Date(Web):08 Jan 2013
DOI:10.1039/C2AN36780G
A low temperature micro-plasma generated in a dielectric barrier discharge (DBD) was used as a radiation source for the excitation of iodine and its determination by vapor generation-optical emission spectrometry. A piece of ceramic tube served as an excitation chamber to provide a small gas path for introducing a helium stream to generate a DBD micro-plasma by using a neon power supply. Iodine was on-line vaporized by reaction of iodide in sample solution (or iodate pre-reduced to iodide by ascorbic acid) with H2O2. The vapor was subsequently separated and transferred into the DBD excitation chamber by a helium stream for performing optical emission and detection at a 905 nm emission line. The emission spectra were measured with a QE65000 charge-coupled device spectrometer. A few important issues governing the performance of the entire system, e.g., selection of the analytical emission line, elimination of the DBD micro-plasma background variation and optimization of the experimental parameters, were investigated. With a sampling volume of 1.0 mL, a linear range of 0.1–10.0 mg L−1 was obtained along with a detection limit of 0.03 mg L−1. A precision of 2.1% RSD was achieved at the concentration level of 2 mg L−1 iodine. The present system was applied in the determination of trace iodine in real samples, i.e., GBW10023 laver, table salt and cydiodine buccal tablets, giving rise to satisfactory results.
Co-reporter:Mingli Chen, Yueming Lin, Cuibo Gu, Jianhua Wang
Talanta 2013 Volume 104() pp:53-57
Publication Date(Web):30 January 2013
DOI:10.1016/j.talanta.2012.11.034
Multi-wall carbon nanotubes (MWNTs) are modified with branched cationic polyethyleneimine (BPEI). The MWNTs–BPEI nanocomposites serve as a novel adsorbent and exhibit favorable selectivity toward adsorption of As(V). Appropriate amount of MWNTs–BPEI suspension containing ca. 5 mg of the composites is used to pack a mini-column for on-line solid phase extraction preconcentration of inorganic arsenic in a sequential injection system, following detection by hydride generation atomic fluorescence spectrometry. At pH 5.8, an sorption efficiency of 80% is achieved for As(V) at 10 μg L−1, resulting in a sorption capacity of 26.18 mg g−1. Meanwhile, the sorption efficiency for As(III) is <5%. The retained As(V) is readily recovered by 100 μL NH4HCO3 (0.6%, m/v). With a sample volume of 2.0 mL, an enrichment factor of 16.3 for As(V) is obtained along with a detection limit of 14 ng L−1 within a linear range of 0.05–1.50 μg L−1. A RSD of 3.6% is derived at 0.5 μg L−1. Total amount of arsenic is obtained by converting As(III) to As(V) and following the same procedure. The speciation of inorganic arsenic is realized by difference. This procedure is validated by analyzing a certified reference material of human hair (GBW09101), achieving satisfactory agreements between the certified and the obtained values. Speciation of As(V) and As(III) is also performed in snow water and rain water samples.Highlights► A novel sorbent for arsenic by modifying carbon nanotubes (MWNTs) with polyethyleneimine (BPEI). ► The MWNTs–BPEI nanocomposites exhibit favorable selectivity to As(V) adsorption. ► It facilitates speciation of As(V) and As(III) by coupling to atomic fluorescence spectrometry.
Co-reporter:Bo Hu, Lin-Lin Hu, Ming-Li Chen, Jian-Hua Wang
Biosensors and Bioelectronics 2013 Volume 49() pp:499-505
Publication Date(Web):15 November 2013
DOI:10.1016/j.bios.2013.06.004
•A ratiometric fluorescence FRET sensor is developed with N-acetyl-L-cysteine functionalized QDs as donor and Rhodamine 6G derivative-mercury conjugate as acceptor.•The FRET sensor generates colorimetric images for mercury within and facilitates visual detection of mercury with a distinguishing ability of 50 μg L−1.•The intracellular imaging of mercury has been demonstrated in live Hela cells.The detection of mercury in biological systems and its imaging is of highly importance. In this work, a ratiometric fluorescence sensor is developed based on fluorescence resonance energy transfer (FRET) with N-acetyl-L-cysteine functionalized quantum dots (NAC-QDs) as donor and Rhodamine 6G derivative-mercury conjugate (R6G-D-Hg) as acceptor. Mercury annihilates the fluorescence of NAC-QDs at 508 nm and meanwhile interacts with R6G derivative to form a fluorescent conjugate giving rise to emission at 554 nm. Resonance energy transfer from NAC-QDs to R6G-D-Hg is triggered by mercury resulting in concentration-dependent variation of fluorescence ratio F508/F554. A linear calibration of F508/F554 versus mercury concentration is obtained within 5–250 μg L−1, along with a detection limit of 0.75 μg L−1 and a RSD of 3.2% (175 μg L−1). The sensor generates colorimetric images for mercury within 0–250 μg L−1, facilitating visual detection of mercury with a distinguishing ability of 50 μg L−1. This feature is further demonstrated by colorimetric imaging of intracellular mercury. On the other hand, the NAC-QDs/R6G-D FRET sensing system is characterized by a combination of high sensitivity and selectivity. The present study provides an approach for further development of ratiometric sensors dedicated to selective in vitro or in vivo sensing some species of biologically interest.
Co-reporter:Xuwei Chen, Linlin Hu, Jiawei Liu, Shuai Chen, Jianhua Wang
TrAC Trends in Analytical Chemistry 2013 Volume 48() pp:30-39
Publication Date(Web):July–August 2013
DOI:10.1016/j.trac.2013.03.010
•Applications of nanoscale carbon-based materials in protein isolation are reviewed.•Carbon-based materials with various morphologies are discussed.•Future perspectives in protein isolation and separation are discussed.This review provides an overview of the current research on nanoscale carbon-based materials as new adsorption materials in the isolation and preconcentration of protein species from biological sample matrices for ensuing bioscience investigations, or achieving enrichment prior to detection. In addition, we discuss future perspectives in related research fields.
Co-reporter:Liming Shen, Meiling Chen, Linlin Hu, Xuwei Chen, and Jianhua Wang
Langmuir 2013 Volume 29(Issue 52) pp:16135-16140
Publication Date(Web):2017-2-22
DOI:10.1021/la404270w
Carbon dots (C-dots) have been proven to show the capability for direct reduction of Ag+ to elemental silver (Ag0) without additional reducing agent or external photoirradiation by incubating Ag+ with C-dots for 5 min in a water bath at 50 °C. Silver nanoparticles (Ag-NPs) are simultaneously formed with an average size of 3.1 ± 1.5 nm and grew on carbon dots. This process involves the oxidation of amine or phenol hydroxyl groups on the aromatic ring of C-dots. Meanwhile C-dots protect and stabilize the Ag-NPs from aggregation in aqueous medium; that is, the Ag-NPs are stable at least for 45 days in aqueous medium. The formed Ag-NPs cause significant resonance light scattering (RLS), which correlates closely with the concentration of silver cation, and this facilitates quantitative detection of silver in aqueous medium.
Co-reporter:Dr. Shuai Chen;Xin Hai;Chang Xia;Dr. Xu-Wei Chen;Dr. Jian-Hua Wang
Chemistry - A European Journal 2013 Volume 19( Issue 47) pp:15918-15923
Publication Date(Web):
DOI:10.1002/chem.201302207
Abstract
We report the first pyrrole-ring surface-functionalized graphene quantum dots (p-GQDs) prepared by a two-step hydrothermal approach under microwave irradiation in an ammonia medium. The most distinct feature of the functionalized GQDs is that both the excitation and emission wavelengths fall into the visible-light region. The p-GQDs are excited by visible light at λex 490 nm (2.53 eV) to emit excitation-independent photoluminescence at a maximum wavelength of λem 550 nm. This is thus far the longest emission wavelength reported for GQDs. Stable photoluminescence is achieved at pH 4–10 with an ionic strength of 1.2 mol L−1 KCl. These features make the p-GQDs excellent probes for bio-imaging and bio-labeling, which is demonstrated by imaging live HeLa cells.
Co-reporter:Xin Wang;XiuFeng Ma;LanLan An;XiangWei Kong;ZhangRun Xu
Science China Chemistry 2013 Volume 56( Issue 6) pp:799-805
Publication Date(Web):2013 June
DOI:10.1007/s11426-012-4808-2
A novel fluid micromixer based on pneumatic perturbation and passive structures was developed. This micromixer facilitates integration and is applicable to fluid mixing over a wide range of flow rates. The microfluidic mixing device consists of an S-shaped structure with two mixing chambers and two barriers, and two pneumatic chambers designed over the S-shaped channel. The performance of the micromixer for fluids with wide variation of flow rates was significantly improved owing to the integration of the pneumatic mixing components with the passive mixing structures. The mixing mechanism of the passive mixing structures was explored by numerical simulation, and the influencing factors on the mixing efficiency were investigated. The results showed that when using a gas pressure of 0.26 MPa and a 100 μm-thick polydimethylsiloxane (PDMS) pneumatic diaphragm, the mixing of fluids with flow rates ranging from 1 to 650 μL/min was achieved with a pumping frequency of 50 Hz. Fast synthesis of CdS quantum dots was realized using this device. Smaller particles were obtained, and the size distribution was greatly improved compared with those obtained using conventional methods.
Co-reporter:YongLiang Yu;JianHua Wang
Science Bulletin 2013 Volume 58( Issue 17) pp:1992-2002
Publication Date(Web):2013 June
DOI:10.1007/s11434-013-5666-9
During the last few years, various flow-based separation/preconcentration methodologies have gained pertinent novel advances and exhibited powerful capability in the field of sample pretreatment and their hyphenation with detection by atomic spectrometry. The present mini-review presents and discusses the progress of flow-based sample processing approaches commonly used for the assay of trace elemental species with detection by atomic spectrometry, including preliminary sample pretreatment, solid phase extraction (including solid phase microextraction), liquid-liquid extraction, vapor generation and dialysis techniques. Special emphasis has been paid on the novel applications and analytical procedures hyphenated with atomic spectrometry. The future perspectives of flow-based sample pretreatment protocols in the determination of trace elements and their speciation are also discussed.
Co-reporter:Ting Yang, Lan-hua Liu, Jia-wei Liu, Ming-Li Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2012 vol. 22(Issue 41) pp:21909-21916
Publication Date(Web):05 Sep 2012
DOI:10.1039/C2JM34712A
Graphene oxide (GO) nanosheets were decorated with a cysteine-rich metal-binding protein, cyanobacterium metallothionein (SmtA). The SmtA–GO composites were characterized by means of FT-IR, AFM and TGA, giving rise to a SmtA binding amount of 867 mg g−1. The SmtA–GO composites exhibit ultra-high selectivity toward the adsorption of cadmium, i.e., the tolerant concentrations for the coexisting metal and anionic species were 1–800000 fold improved after SmtA decoration with respect to bare GO. The SmtA–GO composites were then assembled onto the surface of cytopore microbeads and used for highly selective adsorption and preconcentration of ultra-trace cadmium. In comparison with bare GO (carboxyl-rich GO) loaded cytopore (GO@cytopore), SmtA–GO loaded cytopore (SmtA–GO@cytopore) shows a 3.3-fold improvement over the binding capacity of cadmium, i.e. 7.70 mg g−1 for SmtA–GO@cytopore compared to 2.34 mg g−1 for that by GO@cytopore. A novel procedure for selective cadmium preconcentration was developed using SmtA–GO@cytopore beads as a renewable sorption medium incorporated into a sequential injection lab-on-valve system, with detection by graphite furnace atomic absorption spectrometry (GFAAS). The cadmium retained on the SmtA–GO surface was eluted with a small amount of nitric acid. An enrichment factor of 14.6 and a detection limit of 1.2 ng L−1 were achieved within a linear range of 5–100 ng L−1 by using a sample volume of 1 mL. The procedure was validated by analyzing cadmium in certified reference materials and a series of environmental water samples.
Co-reporter:Shuai Chen, Jia-Wei Liu, Mei-Ling Chen, Xu-Wei Chen and Jian-Hua Wang
Chemical Communications 2012 vol. 48(Issue 61) pp:7637-7639
Publication Date(Web):13 Jun 2012
DOI:10.1039/C2CC32984K
Graphene quantum dots prepared by a one-step hydrothermal procedure in a microwave exhibit an unusual emission transformation in strong acidic media and at high concentration, induced by self-assembled J-type aggregation under restrained π–π interactions.
Co-reporter:Ting Yang, Ming-Li Chen, Lan-Hua Liu, Jian-Hua Wang, and Purnendu K. Dasgupta
Environmental Science & Technology 2012 Volume 46(Issue 4) pp:2251-2256
Publication Date(Web):January 19, 2012
DOI:10.1021/es204034z
Bacillus subtilis is a spore forming bacterium that takes up both inorganic As(III) and As(V). Incubating the bacteria with Fe(III) causes iron uptake (up to ∼0.5% w/w), and some of the iron attaches to the cell membrane as hydrous ferric oxide (HFO) with additional HFO as a separate phase. Remarkably, 30% of the Bacillus subtilis cells remain viable after treatment by 8 mM Fe(III). At pH 3, upon metalation, As(III) binding capacity becomes ∼0, while that for As(V) increases more than three times, offering an unusual high selectivity for As(V) against As(III). At pH 10 both arsenic forms are sorbed, the As(V) sorption capacity of the ferrated Bacillus subtilis is at least of 11 times higher than that of the native bacteria. At pH 8 (close to pH of most natural water), the arsenic binding capacity per mole iron for the ferrated bacteria is greater than those reported for any iron containing sorbent. A sensitive arsenic speciation approach is thus developed based on the binding of inorganic arsenic species by the ferrated bacteria and its unusual high selectivity toward As(V) at low pH.
Co-reporter:Li-Pei Zhang, Bo Hu, Jian-Hua Wang
Analytica Chimica Acta 2012 Volume 717() pp:127-133
Publication Date(Web):2 March 2012
DOI:10.1016/j.aca.2011.12.037
A label-free strategy based on Fenton reaction with unmodified gold nanoparticles (AuNPs) as probe is demonstrated for ascorbic acid (AA) sensing. AuNPs is stable in the presence of single stranded DNA (ssDNA) which prevents salt-induced aggregation of AuNPs in solution. The hydroxyl free radicals generated by Fenton reaction lead to ssDNA cleavage into different sequence fragments which induce aggregation of AuNPs to produce a red-to-blue color change. As an efficient biological antioxidant, AA could effectively scavenge free radicals to avoid the cleavage of ssDNA, so that it prevents color change of the AuNPs solution. Thus, the color change of AuNPs in the presence and absence of AA provides a new approach for the detection of AA. The absorbance ratio at two wavelengths, A670/A520, decreases linearly with AA content within 1–15 μM, giving rise to a detection limit of 0.3 μM and a RSD of 2.8% (10 μM). The color display of AuNPs solution makes it feasible for the estimation of AA content by naked eye visualization. Moreover, based on Fenton reaction and unmodified gold nanoparticles, a multiple logic gate system includes two logic operations, i.e., INHIBIT and NOR, has been designed with small molecules (AA, l-cysteine, glutathione) as inputs and the colorimetric changes of AuNPs solution as outputs.Graphical abstractAscorbic acid is detected based on its prevention on the color change of ssDNA–AuNPs system, by using both naked eye visualization and visible absorption spectroscopy.Highlights► Ascorbic acid (AA) prevents ssDNA cleavage and prohibits color change of ssDNA–AuNPs system, deriving a novel approach for AA detection. ► Ascorbic acid is assayed by visible spectroscopy and naked eye visualization, facilitating fast detection of AA in biological samples. ► A multiple logic gate system is designed with small molecules as inputs and the colorimetric changes in the AuNPs solution as outputs.
Co-reporter:Li-Pei Zhang, Xiao-Xing Zhang, Bo Hu, Li-Ming Shen, Xu-Wei Chen and Jian-Hua Wang
Analyst 2012 vol. 137(Issue 21) pp:4974-4980
Publication Date(Web):28 Aug 2012
DOI:10.1039/C2AN36049G
A label-free strategy based on the Fenton reaction with DNA-templated silver nanoclusters (DNA-Ag NCs) as a probe is demonstrated for the sequential detection of Cu2+, ascorbic acid (AA) and H2O2. Cu2+ causes a structural change of the DNA template in DNA-Ag NCs to resist the environmental quenching and emit stronger fluorescence. The addition of AA in the presence of Cu2+ results in a further fluorescence increase of the DNA-Ag NCs. Interestingly, an even higher fluorescence enhancement is recorded by introducing Cu2+ into the DNA-Ag NCs–AA probing system. The fluorescence turn-on probe offers detection limits of 3 nM for Cu2+ and 7 nM for AA. Thereafter, the addition of H2O2 generates hydroxyl radicals from the Fenton reaction, which induces cleavage of the DNA template, leading to fluorescence quenching of the DNA-Ag NCs. This facilitates H2O2 detection. Moreover, based on the DNA-templated fluorescent silver nanoclusters and Fenton reaction, a multiple logic gate system, including AND and a three-input logic gate, is constructed, with Cu2+, AA and H2O2 as inputs, and the fluorescence intensity of the DNA-Ag NCs probe as output.
Co-reporter:Ting Yang, Xiao-Xing Zhang, Ming-Li Chen and Jian-Hua Wang
Analyst 2012 vol. 137(Issue 18) pp:4193-4199
Publication Date(Web):05 Jul 2012
DOI:10.1039/C2AN35755K
The potential of selective cell-sorption for separation/preconcentration of ultra-trace heavy metals was exploited by surface engineering of Saccharomyces cerevisiae cells. The general idea is to display the cadmium-binding peptide on the cell surface in order to enhance the covalent interaction between cadmium and the yeast cells. By immobilizing the surface-engineered yeast cells onto cytopore® microcarrier beads for cadmium adsorption, we demonstrated that with respect to the native yeast 600-fold and 25–1000-fold improvements were observed respectively for the tolerance of ionic strength and the tolerant capability toward various metal cations after surface engineering. Based on these observations, a novel procedure for selective cadmium preconcentration was developed with detection by graphite furnace atomic absorption spectrometry (GFAAS), employing the engineered S. cerevisiae cell-loaded cytopore® beads as a renewable sorption medium incorporated into a sequential injection lab-on-valve system. The cadmium retained on the yeast cell surface was eluted with a small amount of nitric acid and quantified with GFAAS. Within a range of 5–100 ng L−1 and a sample volume of 1 mL, an enrichment factor of 30 was achieved along with a detection limit of 1.1 ng L−1, a sampling frequency of 20 h−1 and a precision of 3.3% RSD at 50 ng L−1. The procedure was validated by analyzing cadmium in certified reference materials and a series of environmental water samples.
Co-reporter:Zhongchen Wu, Mingli Chen, Lin Tao, Duo Zhao and Jianhua Wang
Journal of Analytical Atomic Spectrometry 2012 vol. 27(Issue 10) pp:1709-1714
Publication Date(Web):16 Jul 2012
DOI:10.1039/C2JA30144J
A simple device was constructed for the on-site sequential monitoring of emitted elemental mercury (Hg0) in coal-fired stack gas. The device integrates on-line gold amalgam preconcentration, external thermal desorption and cold excitation in an enclosed atmospheric-pressure dielectric-barrier discharge (DBD) micro-plasma chamber. The emission was monitored by using a charge coupled device spectrometer. The Hg0 emission at 253.7 nm was well separated from the emission spectra of the Ar-DBD-plasma which eliminates the spectral interferences of ambient air and gaseous inorganic small molecular pollutants in the stack gas, e.g., NOx, SO2, H2S and HCl. Quantification was based on first derivative spectra. Among the three mercury species, Hg0 is efficiently and selectively trapped on the gold amalgam at <220 °C, the threshold temperature for thermal desorption of the trapped Hg0 is ca. 420 °C above which the gold amalgam releases the enriched Hg0 rapidly and gives rise to a high concentration of Hg0 in the flowing Ar stream in a very short period of time which significantly improves the detection sensitivity. A linear calibration graph was achieved within 8–256 ng (the mass of enriched Hg0 on the gold trapping micro-column) with a detection limit of 2.3 ng and an RSD of 4.0% at 32 ng. A spiking recovery of 96.1% was achieved at a spiking mass level of 50 ng Hg0. For real sample analysis (stack gas from a honeycomb briquette stove), a calibration range of 2.7–60.8 ppt was achieved after 5 min preconcentration with a 0.5 L min−1 sampling flow rate.
Co-reporter:Xiaoxing Zhang, Lipei Zhang, Ting Yang, Liming Shen, Mingli Chen and Jianhua Wang
Journal of Analytical Atomic Spectrometry 2012 vol. 27(Issue 10) pp:1680-1687
Publication Date(Web):19 Jun 2012
DOI:10.1039/C2JA30099K
Multi-walled carbon nanotubes (MWNTs) were functionalized by incubating in Fe3+ solution for the purpose of improving its selectivity and sorption capacity to cadmium. High resolution transmission electron microscopy, Raman spectroscopy, X-ray diffraction and surface charge analysis demonstrated that the MWNTs were decorated by a layer of iron phosphate. In a neutral medium (pH 6), the iron phosphate coated carbon nanotubes (NT-FP) offer a much improved sorption capacity of 32.68 mg g−1 for cadmium over 6.72 mg g−1 by bare carbon nanotubes after oxidation. The bare carbon nanotubes generally exhibit non-specific adsorption for various species, while the NT-FP composites provide very high selectivity to cadmium against complex sample matrix components, i.e., the tolerant limit for coexisting species were 5–100 fold improved. The NT-FP composites were packed into a mini-column for on-line selective preconcentration of cadmium with detection by electrothermal atomic absorption spectrometry. A 100% sorption was achieved at pH 6, and 50 μL of aqueous mixture of 0.002 mol L−1 H3PO4 and 0.1 mol L−1 NH4NO3 gives rise to a recovery of 77%. With a sample volume of 1000 μL, an enhancement factor of 31.2 is obtained, along with a detection limit of 1.3 ng L−1 (3σ, n = 11) and a RSD of 2.2% (0.1 μg L−1, n = 11) within a linear calibration range of 0.003–0.2 μg L−1. The procedure is validated by determining cadmium in two certified reference materials (GBW08608 and GBW07404) and environmental water samples.
Co-reporter:Xiao-Xing Zhang, Shi-Song Tang, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2012 vol. 27(Issue 3) pp:466-472
Publication Date(Web):25 Jan 2012
DOI:10.1039/C2JA10292G
Iron phosphate (FePO4) is for the first time used as a novel sorbent for chromium(III) adsorption. The prepared FePO4 was characterized by means of FT-IR, SEM and surface charge analysis, and used for selective adsorption of chromium(III). At pH 5.9, ca.100% of Cr(III) (<5 μg L−1) was retained on the surface of the adsorbent, while at the same conditions the adsorption of Cr(VI) was negligible (<2%). Cr(III) was adsorbed with an ca. 62/1 selectivity over Cr(VI). The adsorption of Cr(III) fits Langmuir model, corresponding to a maximum adsorption capacity of 8.12 mg g−1. The retained Cr(III) could be readily recovered by 200 μL of aqueous mixture of 0.1% H2O2 + 0.05 mol L−1 NH3 as stripping reagent, giving rise to a recovery of 96.5%. The chromium in the eluate is quantified with detection by electrothermal atomic absorption spectrometry. A sample volume of 2000 μL creates an enrichment factor of 8.7, along with a detection limit of 0.02 μg L−1 (3σ, n = 9) and a RSD of 2.5% (0.5 μg L−1) within a linear calibration range of 0.05–2.5 μg L−1. Total chromium was determined after reduction of Cr(VI) to Cr(III) by hydroxylamine hydrochloride as a reducing reagent. The content of Cr(VI) was achieved by difference. The method was validated by analyzing chromium content in a certified reference material (GBW08608, Trace Elements in Water) and speciation of Cr(III) and Cr(VI) in sea water, tap water, spring water and ground water samples was conducted.
Co-reporter:Myong-Il An;Xiaoxing Zhang;Ting Yang;Mingli Chen;Jianhua Wang
Chinese Journal of Chemistry 2012 Volume 30( Issue 9) pp:2225-2231
Publication Date(Web):
DOI:10.1002/cjoc.201200580
Abstract
A novel adsorbent was developed by coating yttrium hydroxide precipitate layer on cellulose fibre. This material takes up ca. 98% of 5 µg·L−1 As(III) and As(V) at low pH (pH<7), while a favorable selectivity for As(V) was achieved within pH 11–12. In practice, a mini-column packed with Y(OH)3 precipitate layer coated cellulose fibre particles was incorporated into a sequential injection system for selective uptake of arsenate at pH 11.5. The retained arsenate was afterwards recovered with 50 µL of 0.8 mol·L−1 NaOH solution as eluent, followed by hydride generation in a reaction medium of 2.0 mol·L−1 HCl and 1.0% NaBH4 solution (W/V, in 0.5% NaOH) after pre-reduction of arsenate to arsenite by KI-ascorbic acid (5%, W/V), with detection by atomic fluorescence spectrometry. Total inorganic arsenic was quantitatively taken up at pH 6.0 by following the same procedure and arsenic speciation was performed by difference. With a sample volume of 1.0 mL, an enrichment factor of 16.4 was derived with a detection limit of 17 ng·L−1 within a linear range of 0.05–2.0 µg·L−1. A relative standard deviation (RSD) of 2.6% (0.5 µg·L−1, n=11) was achieved. The procedure was validated by analyzing arsenic in a certified reference material GBW 09101 (human hair), and speciation of inorganic arsenic in natural water samples. The entire process requires no organic solvents, thus Y(OH)3 coated cellulose fibre provides a green adsorbent.
Co-reporter:Yong-Liang Yu, Ying Jiang, Shuai Dou and Jian-Hua Wang
Analytical Methods 2012 vol. 4(Issue 6) pp:1718-1724
Publication Date(Web):23 Mar 2012
DOI:10.1039/C2AY25159K
An approach for the immobilization of a chromogenic reagent on solid phase micro-beads is performed via a sulfonation reaction. The product as an optical sensor is applied in lab-on-valve bead injection spectroscopy. The benzene ring structure exists in various chromogenic reagents, which facilitates the introduction of a sulfonic acid group via sulfonation. Chromogenic reagents ranging from neutral to anionic can be immobilized on anion exchanger micro-beads. As a model of application, micro-beads of Sephadex QAE A-25 loaded with the chromogenic reagent 1-(2-pyridylazo)-2-naphthol-sulfonic acid (PAN-S) are employed for the determination of trace cobalt by lab-on-valve bead injection spectroscopy. The characteristics of the micro-beads and some important parameters governing the performance of the method are investigated. With a sample volume of 1.0 mL, a detection limit of 8 μg L−1 and a linear range of 20–500 μg L−1 are obtained for cobalt, along with a RSD value of 2.8% (at the 200 μg L−1 level). The accuracy and practical applicability of the present method are validated by analysing a certified reference material of soil GBW07404, vitamin B12 injection and mecobalamin tablets, and further demonstrated by spiking recovery of cobalt in two water samples.
Co-reporter:Mei-Ling Chen, Ye-Ju He, Xu-Wei Chen, and Jian-Hua Wang
Langmuir 2012 Volume 28(Issue 47) pp:16469-16476
Publication Date(Web):November 6, 2012
DOI:10.1021/la303957y
A novel and specific nanoplatform for in vitro simultaneous cancer-targeted optical imaging and magnetically guided drug delivery is developed by conjugating CdTe quantum dots with Fe3O4-filled carbon nanotubes (CNTs) for the first time. Fe3O4 is filled into the interior of the CNTs, which facilitates magnetically guided delivery and improves the synergetic targeting efficiency. In comparison with that immobilized on the external surface of CNTs, the magnetite nanocrystals inside the CNTs protect it from agglomeration, enhance its chemical stability, and improve the drug loading capacity. It also avoids magnetic nanocrystals-induced quenching of fluorescence of the quantum dots. The SiO2-coated quantum dots (HQDs) attached on the surface of CNTs exhibit favorable fluorescence as the hybrid SiO2 shells on the QDs surface prevent its fluorescence quenching caused by the CNTs. In addition, the hybrid SiO2 shells also mitigate the toxicity of the CdTe QDs. By coating transferrin on the surface of the herein modified CNTs, it provides a dual-targeted drug delivery system to transport the doxorubicin hydrochloride (DOX) into Hela cells by means of an external magnetic field. The nanocarrier based on the multifunctional nanoplatform exhibits an excellent drug loading capability of ca. 110%, in addition to cancer-targeted optical imaging as well as magnetically guided drug delivery.
Co-reporter:Xu-Wei Chen, Quan-Xing Mao, Jia-Wei Liu, Jian-Hua Wang
Talanta 2012 Volume 100() pp:107-112
Publication Date(Web):15 October 2012
DOI:10.1016/j.talanta.2012.07.095
Hemoglobin (Hb) modified magnetic nanocomposites are prepared by immobilization of Hb onto the surface of amino-functionalized Fe3O4@SiO2 magnetic nanoparticles via covalent bonding with glutaraldehyde as cross-linker. The obtained nanocomposites are characterized with FT-IR, SEM, XRD and surface charge analysis. A direct solid-phase extraction procedure for the isolation/separation of plasmid DNA using this nanocomposite as a novel adsorbent is thus developed. Some important experimental parameters governing the sorption efficiency, i.e., the pH of sample solution and the ionic strength, are investigated. The Hb modified magnetic nanocomposites provide a sorption capacity of 27.86 mg g−1 for DNA. By using 2.0 mg of the nanocomposites as sorption medium and a suitable acidity of pH 6.1, a sorption efficiency of 93% is achieved for 25 μg mL−1 of DNA in 1.0 mL of sample solution. Afterwards, the absorbed DNA could be readily recovered by using 1.0 mL of Tris–HCl buffer (pH 8.9, 0.01 mol L−1), giving rise to a recovery of ca. 68.3%. The present solid-phased extraction protocol is applied for the isolation of plasmid DNA from Escherichia coli culture, resulting in comparable yield and purity of plasmid DNA with respect to those obtained by using commercial kits.Highlights► Hemoglobin (Hb) modified magnetic nanocomposites were prepared as a novel adsorbent. ► Hb was immobilized onto the surface of amino-functionalized Fe3O4@SiO2 magnetic nanoparticles. ► The composites provide comparable yield of plasmid DNA with respect to those obtained by commercial kits.
Co-reporter:Bo Hu, Li-Pei Zhang, Mei-Ling Chen, Ming-Li Chen, Jian-Hua Wang
Biosensors and Bioelectronics 2012 Volume 32(Issue 1) pp:82-88
Publication Date(Web):15 February 2012
DOI:10.1016/j.bios.2011.11.031
Fluorescence resonance energy transfer (FRET) between two quantum dots of different sizes causes fluorescence quenching. Hereby a binding site pre-blocking approach is proposed to avoid this effect. Pre-binding of glucose on the donor occupies the binding sites and thus blocks resonance energy transfer between the two quantum dots, protecting the fluorescence from being quenched. A glucose assay is developed based on this approach. The glucose content is correlated with the fluorescence difference in the absence and in the presence of glucose. In practice, Green QDs–Con A conjugates are used as donors and Red QDs–NH2-glu conjugates as acceptors to form FRET system. The inhibition of fluorescence quenching is then measured in the presence of glucose. A linear calibration graph is achieved within 0.1–2.0 mmol L−1, along with a detection limit of 0.03 mmol L−1 and a RSD of 2.1% (1.0 mmol L−1). 91–105% of glucose in serum and urine samples is recovered. It is worth mentioning that the present glucose assay approach also generates a fluorescence chromatic difference imaging, and the color display clearly identifies the glucose contents by visual detection with a distinguishing ability of ca. 0.5 mmol L−1. The present approach can potentially be used for the clinical determination of glucose in biological samples which can be further developed into a glucose sensor.Highlights► FRET between two quantum dots causes fluorescence quenching. A binding site pre-blocking assay approach for avoiding this phenomenon is proposed. ► Pre-binding of glucose on the donor occupies the binding sites and blocks resonance energy transfer between quantum dots, protecting the fluorescence from being quenched. ► A glucose assay approach is developed based on this approach. ► This system generates a fluorescence chromatic difference image, which can identify glucose contents by visual detection with a distinguishing ability of ca. 0.5 mM.
Co-reporter:Yan-Yan Song;Zhi-Da Gao;Xing-Hua Xia;Robert Lynch
Advanced Functional Materials 2011 Volume 21( Issue 10) pp:1941-1946
Publication Date(Web):
DOI:10.1002/adfm.201002258
Abstract
WO3 nanoparticles loaded in TiO2 nanotube arrays, fabricated by a chemical bath deposition (CBD) technique in combination with a pyrolysis process, is uniform and the diameter can be easily adjusted by the deposition times. The resultant hybrid nanotubes array shows a multistage coloring electrochromic response at different potential bias. The formation of a 3-dimensional WO3/TiO2 junction promotes unidirectional charge transport due to the one-dimensional features of the tubes, which leads to the significant positive-shift onset potential of the cathodic reaction (ion insertion) and the highly increased proton storage capacity. Compared to non-decorated nanotube arrays, the enhanced electrochromic properties of longer lifetime, higher contrast ratio (bleaching time/coloration time), and improved tailored electrochromic behavior could be achieved using the composite films.
Co-reporter:Hao Meng, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2011 vol. 21(Issue 38) pp:14857-14863
Publication Date(Web):18 Aug 2011
DOI:10.1039/C1JM11918D
A novel one-pot procedure for the synthesis of ionic liquid N,N-bis[2-methylbutyl] imidazolium hexafluorophosphate (PPimPF6/TiO2) nanocomposites is reported for the first time. During the in situ formation of TiO2 nanoparticles via hydrolysis of tetrabutyl titanate (TBOT), the ionic liquid PPimPF6 is simultaneously incorporated into the TiO2 nanostructure via H-bonding. The PPimPF6/TiO2 nanocomposites are characterized by means of TEM, FT-IR and XRD, showing that they possess the structure of anatase and exhibit selective adsorption for neutral proteins, hemoglobin (Hb) in this particular case, under controlled experimental conditions. At pH 8, an adsorption efficiency of 88.3% for 150 μg mL−1 Hb is achieved by 2.0 mg of PPimPF6/TiO2 nanocomposites, while virtually no adsorption is observed for the basic protein cytochrome c (cyt-c) and the acidic protein bovine serum albumin (BSA). An adsorption capacity of 122.3 μg mg−1 is obtained for Hb by calculation on the amount of the incorporated ionic liquid, corresponding to a 5-fold improvement with respect to that achieved by pure PPimPF6. The retained Hb on the PPimPF6/TiO2 nanocomposites could be readily collected by stripping with 0.5% SDS, giving rise to a recovery of ca. 73%. The circular dichroism (CD) spectra indicate no conformational change of Hb after the adsorption/elution process. The selective isolation of Hb from human whole blood is achieved by the nanocomposites.
Co-reporter:Chun-Guang Yang, Ying-Fan Wu, Zhang-Run Xu and Jian-Hua Wang
Lab on a Chip 2011 vol. 11(Issue 19) pp:3305-3312
Publication Date(Web):15 Aug 2011
DOI:10.1039/C1LC20123A
An integrated microfluidic concentration gradient chip was developed for generating stepwise concentrations in high-density channels and applied to high-throughput apoptosis analysis of human uterine cervix cancer (HeLa) cells. The concentration gradient was generated by repeated splitting-and-mixing of the source solutions in a radial channel network which consists of multiple concentric circular channels and an increasing number of branch channels. The gradients were formed over hundreds of branches with predictable concentrations in each branch channel. This configuration brings about some distinctive advantages, e.g., more compact and versatile design, high-density of channels and wide concentration ranges. This concentration gradient generator was used in perfusion culture of HeLa cells and a drug-induced apoptosis assay, demonstrated by investigating the single and combined effects of two model anticancer drugs, 5-fluorouracil and Cyclophosphamide, which were divided into 65 concentrations of the two drugs respectively and 65 of their combinatorial concentrations. The gradient generation, the cell culture/stimulation and staining were performed in a single chip. The present device offers a unique platform to characterize various cellular responses in a high-throughput fashion.
Co-reporter:Zhongchen Wu, Mingli Chen, Ping Li, Qianqian Zhu and Jianhua Wang
Analyst 2011 vol. 136(Issue 12) pp:2552-2557
Publication Date(Web):10 May 2011
DOI:10.1039/C0AN00938E
Dielectric-barrier discharge (DBD) in argon as a cold source is used for the excitation of gaseous inorganic small molecules at atmospheric pressure. By choosing ammonia as a model molecule, the excitation process and the characteristics of the emission spectra are investigated. The emission spectra are recorded by designing either an open-end or an enclosed DBD excitation/emission source. The enclosed excitation mode effectively eliminates the background emissions arising from the ambient air components, especially those from nitrogen. Two emission lines attributed to the excitation of ammonia, i.e., 326.2 and 336.5 nm, are clearly isolated from the background emission spectra of argon, providing the basis for quantitative analysis. A detection limit of 0.37 ppm is achieved within a linear range of 1.2–35 ppm by monitoring at 326.2 nm. In practice, gaseous samples containing ammonia collected in a public toilet are excited in an enclosed excitation source and the emission at 326.2 nm is monitored for quantitative analysis. An ammonia concentration of 2.4 ppm is derived in the original atmospheric sample, and a spiking recovery of 94.7% is achieved at a 10 ppm ammonia level. This study shows that DBD cold excitation in combination with optical emission spectrometry (OES) offers a promising approach for the detection of ammonia pollution.
Co-reporter:Yong Tian, Zhao-Ming Xie, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2011 vol. 26(Issue 7) pp:1408-1413
Publication Date(Web):28 Mar 2011
DOI:10.1039/C0JA00265H
A novel green/biodegradable adsorbent, mungbean-coat, has been investigated for the adsorption of ultra-trace amounts of cadmium. Carboxylic groups on the bean-coat effectively retain the cadmium ions via coordinative interactions. This well facilitates the adsorption of cadmium ions which can readily be recovered by acid elution. In practice, bean-coat is used to pack a mini-column for on-line adsorption and preconcentration of cadmium from environmental samples with detection by electrothermal atomic absorption spectrometry. By using a sample loading volume of 1.4 mL and an eluent volume of 70 μL, an enrichment factor of 19.8 along with a detection limit of 1.4 ng L−1 are achieved. A precision of 2.4% RSD at the level of 0.05 μg L−1 is derived. The present procedure has been applied for the determination of cadmium in certified reference materials (GBW08608 Trace Elements in Water and CRM 176 Trace Elements in a City Waste Incineration Ash) and a snow water sample. Fair agreements are reached between the certified values and the experimental results, in addition to a satisfactory spiking recovery for the snow water sample. In the present work, the use of green and biodegradable adsorbent as well as the elimination of use of organic solvent/eluent facilitates the development of a green analytical protocol.
Co-reporter:Ming-Li Chen, Hui-Juan Ma, Si-Qi Zhang and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2011 vol. 26(Issue 3) pp:613-617
Publication Date(Web):14 Feb 2011
DOI:10.1039/C0JA00185F
The functionalization of cellulose fibre by grafting L-cysteine on the surface (Cys-fibre) significantly improves the sorption capacity toward mercury and methyl-mercury. The Cys-fibre is used to pack a mini-column for on-line separation and preconcentration of mercury species in a sequential injection system. The retained mercury and methyl-mercury could readily be recovered by a mixture of L-cysteine and nitric acid. The inorganic mercury is selectively quantified using the cold atomization mode with vapor generation atomic fluorescence spectrometry. The total amount of mercury is determined by adopting the flame/heat atomization mode, and thus the concentration of methyl-mercury is achieved by the difference. When 1000 μL of sample solution is processed followed by elution with 100 μL of eluent, detection limits of 1 ng L−1 (3σ, n = 9) for inorganic mercury and 3 ng L−1 (3σ, n = 9) for methyl-mercury are obtained within linear ranges of 0.01–0.7 μg L−1Hg2+ and 0.03–2.0 μg L−1MeHg, respectively. The precisions for Hg2+ and MeHg of 1.5% RSD (n = 11) and 2.6% RSD (n = 9) are recorded at 0.1 μg L−1 and 1.0 μg L−1, respectively. The procedure has been validated by analyzing mercury in certified reference material of BCR176 and a cosmetic sample. Speciation of mercury and methyl-mercury in a series of water samples and the extracts of cosmetic and seaweed samples are performed, and favorable spiking recoveries have been demonstrated.
Co-reporter:Yong Tian, Ming-Li Chen, Xu-Wei Chen, Jian-Hua Wang, Yoshihiro Hirano, Hideyuki Sakamoto and Toshihiro Shirasaki
Journal of Analytical Atomic Spectrometry 2011 vol. 26(Issue 1) pp:133-140
Publication Date(Web):16 Nov 2010
DOI:10.1039/C0JA00091D
A novel method for arsenic speciation is developed by interfacing solid phase preconcentration-liquid chromatography (LC) separation-gradient hydride generation (GHG)-quartz flame atomic absorption spectrometry (QFAAS). A MnO2 mini-column is used to preconcentrate the arsenic species of As(III), As(V), MMA and DMA, during which process, As(III) is converted to As(V)viaoxidation by MnO2, while other species remain unchanged. The recovery of As(V) (i.e., the total amount of arsenate and arsenite in the original sample), MMA and DMA from the MnO2 mini-column is facilitated by tetramethylammonium hydroxide (TMAH). After LC separation with C30 columns, arsenic species in the eluate are subject to gradient hydride generation with detection by QFAAS. On the other hand, cellulose fibre selectively adsorbs the chelating complex between As(III) and ammonium pyrrolidine dithiocarbamate (APDC). After elution with HNO3, As(III) in the original sample is quantified by graphite furnace atomic absorption spectrometry (GFAAS), and the amount of As(V) is obtained by subtraction. A sample volume of 2.0 mL derives enrichment factors of 14.0–19.2 for the arsenic species. By injecting 20 μL of eluate into the LC system (the eluate of As(III)-PDC complex is injected into the GFAAS), detection limits of 0.019, 0.33, 0.39, 0.62 μg L−1 are obtained for As(III), As(V), MMA and DMA respectively. RSDs of less than 4.2% are achieved at the level of 2 μg L−1 for As(V), MMA, DMA and 1 μg L−1 for As(III). The procedure is evaluated by speciating arsenic in snow water and Hijiki samples.
Co-reporter:Xuwei Chen, Wenjing Wang, Zhining Song and Jianhua Wang
Analytical Methods 2011 vol. 3(Issue 8) pp:1769-1773
Publication Date(Web):15 Jun 2011
DOI:10.1039/C1AY05130J
A cross-linked chitosan/multi-wall carbon nanotube (MWCNTs) nanocomposite is prepared via surface deposition-cross linking. The nanocomposite is characterized by means of FT-IR, SEM and TGA analysis, indicating that a chitosan layer is well coated on the surfaces of the MWCNTs, weighing about 35% of the total mass. Investigations on the performance of the chitosan/MWCNTs nanocomposite to the adsorption or loading of hemoglobin indicated that the adsorption equilibrium time is reduced from a few hours in the conventional protocols to 25 min in the present case. A theoretical adsorption capacity of 15.41 μg mg−1 is achieved, corresponding to a 6-fold improvement when compared to that obtained by using conventional chitosan particles in the micrometre range at a same mass condition. The nanocomposite is used as an adsorbent for the isolation of hemoglobin from human whole blood, the SDS-PAGE results indicated that successful separation of hemoglobin is obtained in the presence of large amount of abundant protein, e.g., human serum albumin.
Co-reporter:Xiaoxing Zhang, Mingli Chen, Yongliang Yu, Ting Yang and Jianhua Wang
Analytical Methods 2011 vol. 3(Issue 2) pp:457-462
Publication Date(Web):06 Jan 2011
DOI:10.1039/C0AY00621A
Multi-walled carbon nanotubes (MWNTs) are noncovalently wrapped by a cationic polyelectrolyte of poly(diallyldimethylammonium chloride) (PDDA) via π–π interactions between the unsaturated impurity in PDDA and MWNTs. The modified PDDA-MWNTs are characterized by FT-IR and surface charge analysis. The PDDA-MWNTs are packed into a mini-column and used for the adsorption of Cr(VI) in a sequential injection system with detection by electrothermal atomic absorption spectrometry (ETAAS). A 32% improvement on the adsorption efficiency of Cr(VI) by the PDDA-MWNTs at pH 6 is achieved with respect to that obtained by the bare MWNTs. The retained Cr(VI) is afterwards recovered by using 80 μL of ammonium nitrate solution (0.1 mol L−1) as stripping reagent producing an elution efficiency of 81%. The presence of a certain amount of Cr(III) within a Cr(III)/Cr(VI) concentration ratio of 6:1 causes no interfering effect for the adsorption of Cr(VI) by the PDDA-MWNTs mini-column. A sample loading volume of 1000 μL creates an enrichment factor of 8.6, along with a detection limit of 0.016 μg L−1 (3σ, n = 7) and a RSD of 3.9% (0.5 μg L−1) within a linear calibration range of 0.05–1.5 μg L−1. The procedure has been validated by analyzing a certified reference material of GBW08608 and a series of water samples.
Co-reporter:Xin Wang, Xuemin Chen, Xiufeng Ma, Xiangwei Kong, Zhangrun Xu, Jianhua Wang
Talanta 2011 Volume 84(Issue 2) pp:565-571
Publication Date(Web):15 April 2011
DOI:10.1016/j.talanta.2011.01.065
A novel fluid mixing strategy was developed which significantly enhanced the efficiency of DNA hybridization. A pneumatic micro-mixing device consisting of two pneumatic chambers and an underneath DNA microarray chamber was built up. The fluid in the array chamber was pneumatically pumped alternately by the two pneumatic chambers. The chaotic oscillatory flow caused by the pumping greatly intensified the fluidic mixing. A homogeneous distribution of the tracer dye solution in the microarray chamber was observed after 2 s mixing with a pumping frequency of 24 Hz. Microarray DNA hybridization was substantially accelerated using this device, and the fluorescence intensity showed a plateau after oscillating 30 s at room temperature. The corresponding signal level of the dynamic hybridization was 12.5-fold higher than that of the static hybridization performed at 42 °C. A signal-to-noise ratio of 117 was achieved and the nonspecific adsorption of the targets to the sample array was minimized, which might be attributed to the strong shearing force generated during the pneumatic mixing process.
Co-reporter:Jia-Wei Liu;Dr. Qian Zhang;Dr. Xu-Wei Chen; Jian-Hua Wang
Chemistry - A European Journal 2011 Volume 17( Issue 17) pp:4864-4870
Publication Date(Web):
DOI:10.1002/chem.201003361
Abstract
Graphene oxide (GO) nanosheets have been immobilized onto SiO2 particles through electrostatic interactions by surface assembly. The surface-assembled composite material was characterized by means of SEM and FTIR and UV/Vis spectroscopy to reveal an assembling ratio of 2.3 % (w/w, GO/SiO2). The GO/SiO2 composites were subsequently used, for the first time, as adsorbents for the adsorption/isolation of proteins. Selective isolation of proteins of interest, namely, hemoglobin (Hb) in this case, from complex sample matrices, for example, human whole blood, could be obtained by carefully manipulating the adsorption/desorption process. At pH 7, an adsorption of 85 % was achieved for Hb (70 mg L−1) in sample solution (1.0 mL) by the GO/SiO2 composites (3.0 mg). The adsorption behavior was consistent with the Langmuir adsorption model, corresponding to a theoretical adsorption capacity of 50.5 mg g−1 for Hb. The retained Hb could be readily recovered by using a Tris-HCl buffer at pH 8.9 to give a recovery of 80 %. Circular dichroism and specific activity investigations indicated that the GO/SiO2 composites exhibited favorable biocompatibility, characterized by virtually no effect on the conformation and activity of Hb after adsorption/desorption. The composites were used for the selective isolation of Hb from human whole blood and achieved satisfactory results by assaying with sodium dodecyl sulfate polyacrylamide gel electrophoresis.
Co-reporter:Yang Shu, Menglin Liu, Shuai Chen, Xuwei Chen, and Jianhua Wang
The Journal of Physical Chemistry B 2011 Volume 115(Issue 42) pp:12306-12314
Publication Date(Web):September 15, 2011
DOI:10.1021/jp2071925
The interactions of imidazolium ionic liquids (ILs), i.e., dibutylimidazolium chloride, 1-butyl-3-methylimidazolium chloride, and 1-butyl-3-methylimidazolium nitrate, with bovine serum albumin (BSA) were studied by monitoring the spectral behaviors of IL–BSA aqueous systems. The intrinsic fluorescence of BSA at 340 nm excited at 230 nm is obviously quenched by these ILs due to complex dynamic collision and their quenching constants are at the order of 102 L mol–1. However, no fluorescence quenching is observed within the same region when excited at 280 nm, which is widely used for probing protein conformations. Thermodynamic investigations reveal that the combination between ILs and BSA is entropy driven by predominantly hydrophobic and electrostatic interactions, leading to the unfolding of polypeptides within BSA. The influence of the ILs on the conformation of BSA follows a sequence of BmimNO3 > BmimCl ≈ BbimCl. Molecular docking shows that cationic imidazolium moieties of ILs enter the subdomains of protein and interact with the hydrophobic residues of domain III. An agreement between fluorescence spectroscopic investigations and molecular docking is reached. It is found that the fluorescence of BSA at λex 230 nm arising from aromatic amino acids Trp and Tyr is almost as sensitive as that achieved at λex 280 nm for elucidating the protein conformational changes, which provides a valid and new probe for the investigation of binding kinetics between molecules/ions and proteins.
Co-reporter:Xu-Wei Chen, Jia-Wei Liu, and Jian-Hua Wang
The Journal of Physical Chemistry B 2011 Volume 115(Issue 6) pp:1524-1530
Publication Date(Web):January 26, 2011
DOI:10.1021/jp109121h
With respect to the conventional imidazolium ionic liquids which generally create very weak fluorescence with quantum yields at extremely low levels of 0.005−0.02, a symmetrical hydrophilic ionic liquid 1,3-butylimidazolium chloride (BBimCl) was found to be highly fluorescent with λem at 388 nm when excited at λex < 340 nm. The very high quantum yield of BBimCl in aqueous medium, derived to be 0.523 when excited at 315 nm, was attributed to its symmetrical plane conjugating structure. In the presence of hemoglobin, the fluorescence of BBimCl could be significantly quenched, resulting from the coordinating interaction between the iron atom in the heme group of hemoglobin and the cationic imidazolium moiety. This feature of the present hydrophilic ionic liquid makes it a promising fluorescence probe candidate for the sensitive sensing of hemoglobin. A linear regression was observed within 3 × 10−7 to 5 × 10−6 mol L−1 for hemoglobin, and a detection limit of 7.3 × 10−8 mol L−1 was derived.
Co-reporter:Xuwei Chen, Yanpei Ji and Jianhua Wang
Analyst 2010 vol. 135(Issue 9) pp:2241-2248
Publication Date(Web):08 Jul 2010
DOI:10.1039/C0AN00244E
The crystallization of lysozyme with hydrophilic ionic liquid 1,3-butylimidazolium chloride (BBimCl) as an additive was investigated with hanging-drop vapor diffusion crystallization protocol. The elevated threshold to super-saturation caused by the increased solubility of lysozyme in the presence of BBimCl and the slower super-saturation process of lysozyme induced by the negligible vapor pressure of BBimCl contributed to a lower super-saturation degree, offering a promoted ambient circumstance for nucleation and providing a controlled velocity for the growth of lysozyme crystal. These eventually offer a prominent promotion to the crystallization of lysozyme, i.e., less crystal polymorphism and precipitation while larger crystals and significantly improved the tolerance to the concomitant impurities or sample matrices for the crystallization of lysozyme. Therefore, the presence of BBimCl enables the direct crystallization of lysozyme from a real complex sample matrix, i.e., egg-white, which opens a promising avenue for the development of protein crystallization methodology with ionic liquids as an additive and offers vast potentials for the practical separation/purification of proteins of interest from complex real sample matrices.
Co-reporter:Mei-Ling Chen;Ming-Li Chen;Xu-Wei Chen
Macromolecular Bioscience 2010 Volume 10( Issue 8) pp:906-915
Publication Date(Web):
DOI:10.1002/mabi.200900444
Co-reporter:Xuwei Chen, Shuai Chen and Jianhua Wang
Analyst 2010 vol. 135(Issue 7) pp:1736-1741
Publication Date(Web):17 May 2010
DOI:10.1039/C000465K
A pH-responsive poly(N-isopropylacrylamide-co-acrylic acid) hydrogel was prepared by an aqueous dispersion polymerization process. The number of carboxylic groups distributed on the surface of the hydrogel was found to be 1.89 mmol g−1. The hydrogel exhibits excellent binding selectivity to the protein species of interest within certain pH regions. In the present work, it was applied to the selective isolation of hemoglobin from human whole blood. Some important experimental parameters governing the sorption property, including the pH of sample solution, the ionic strength and sorption time, were investigated. Using 2.0 mg of the hydrogel as a sorption medium and suitable acidity of pH 6.0, a sorption efficiency of 93% was achieved for 200 μg mL−1 of hemoglobin in 1.0 mL of sample solution. Afterwards, the absorbed hemoglobin could be readily recovered using 1.0 mL of Tris-HCl buffer (pH 8.6, 0.01 mol L−1), giving rise to recovery of ca. 76%. The practical applicability of this system was further demonstrated by processing human whole blood for the isolation of hemoglobin, and satisfactory results were obtained by assay with SDS-PAGE.
Co-reporter:Ming-Li Chen, Ya-Nan Zhao, Da-Wei Zhang, Yong Tian and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2010 vol. 25(Issue 11) pp:1688-1694
Publication Date(Web):19 Aug 2010
DOI:10.1039/C0JA00026D
The immobilization of N-methylimidazolium (Nmim) onto PVC surface forms bonded hydrophilic ionic liquid 1-chlorovinyl-3-methylimidazolium chloride (PVC-NmimCl), which entails anion exchange nature and positively charged surface, facilitating favorable retention of Cr(VI) with a retention capacity of 23.2 mg g−1 for Cr(VI) at pH 5.6. A novel on-line solid phase extraction approach for the separation and preconcentration of Cr(VI) is developed in a sequential injection system with a PVC-NmimCl mini-column, and an extra mini-column of strong acidic styrene type cation exchange resin is incorporated for pre-eliminating Cr(III) in sample solution before entering the PVC-NmimCl mini-column. The retained Cr(VI) is effectively recovered with elution by 0.2 mol l−1 NH4NO3 solution, and the eluate is quantified by electrothermal atomic absorption spectrometry (ETAAS) and inductively coupled plasma mass spectrometry (ICP-MS). With a sample volume of 2000 μl, a complete retention of Cr(VI) is obtained, giving rise to an enrichment factor of 23.4 and a sampling frequency of 9 h−1. A linear range of 0.01–1.0 μg l−1 for Cr(VI), along with a detection limit of 3 ng l−1 and a RSD of 2.9% at 0.5 μg l−1 is obtained. Total chromium in a certified reference material of reverine water (GBW08608) is determined after oxidation, which results in good agreement between the certified and the found values. The procedure is further demonstrated for chromium speciation in tap water and snow water samples.
Co-reporter:Yong Tian, Ming-Li Chen, Xu-Wei Chen, Jian-Hua Wang, Yoshihiro Hirano, Hideyuki Sakamoto and Ikumei Setsu
Journal of Analytical Atomic Spectrometry 2010 vol. 25(Issue 1) pp:48-54
Publication Date(Web):14 Oct 2009
DOI:10.1039/B913198A
Arsenic speciation was performed based on liquid chromatographic separation followed by gradient hydride generation (GHG) and quartz atomizer atomic absorption spectrometric detection. The arsenic species, i.e., arsenate (As(V)), arsenite (As(III)), monomethylarsonic acid (MMA), dimethylarsinic acid (DMA) and trimethylarsine oxide (TMAO), were separated on C30-5 columns, and the concept of gradient hydride generation facilitates high conversion efficiency of the arsenic species into corresponding hydrides. The use of 2% L-cysteine in the GHG process gives rise to further improvements on the hydride generation efficiency of 13% to 32% for the arsenic species. The hydrides were separated in a unique design of gas–liquid separator, which not only ensures a complete separation but minimizes the dispersion of hydrides when delivering into the atomizer, resulting in a maximum of 13-fold improvement on the sensitivity of As(V) compared to previous studies. A separation process was finished within 800 s by injecting 100 µL sample solution, achieving detection limits of 0.9, 1.4, 1.4, 1.6, 1.5 µg/L, respectively, for As(V), As(III), MMA, DMA and TMAO. Precisions of less than 3% and 6% RSD were obtained for the five arsenic species at 100 µg/L and 20 µg/L, respectively. Three arsenic species, i.e., As(V), DMA and TMAO, were identified in Hijiki samples by this procedure.
Co-reporter:Xuwei Chen, Jiawei Liu and Jianhua Wang
Analytical Methods 2010 vol. 2(Issue 9) pp:1222-1226
Publication Date(Web):10 Aug 2010
DOI:10.1039/C0AY00342E
As a group of novel green solvents, ionic liquids have attracted extensive attention and gained popularity in various applications including protein assays. Ionic liquids are not only an excellent reaction medium to replace the conventional organic solvents, but are also an efficient participant to achieve better performances. The aim of the present mini-review is to illustrate the state-of-the-art progress of implementing ionic liquids in protein assays, focusing on the investigations of protein stability/activity, protein extraction and isolation/purification, protein crystallization, separation of protein species and their detections.
Co-reporter:Zhang-Run Xu, Chun-Guang Yang, Cui-Hong Liu, Zhe Zhou, Jin Fang, Jian-Hua Wang
Talanta 2010 Volume 80(Issue 3) pp:1088-1093
Publication Date(Web):January 2010
DOI:10.1016/j.talanta.2009.08.031
A novel microfluidic chip integrating an osmosis-based micro-pump was developed and used for perfusion cell culture. The micro-pump includes two sealed chambers, i.e., the inner osmotic reagent chamber and the outer water chamber, sandwiching a semi-permeable membrane. The water in the outer chamber was forced to flow through the membrane into the inner chamber via osmosis, facilitating continuous flow of fluidic zone in the channel. An average flow rate of 0.33 μL min−1 was obtained within 50 h along with a precision of 4.3% RSD (n = 51) by using a 100 mg mL−1 polyvinylpyrrolidone (PVP) solution as the osmotic driving reagent and a flow passage area of 0.98 cm2 of the semi-permeable membrane. The power-free micro-pump has been demonstrated to be pulse-free offering stable flow rates during long-term operation. The present microfluidic chip has been successfully applied for the perfusion culture of human colorectal carcinoma cell by continuously refreshing the culture medium with the osmotic micro-pump. In addition, in situ cell immunostaining was also performed on the microchip by driving all the reagent zones with the integrated micro-pump.
Co-reporter:Yang Shu, Xu-Wei Chen, Jian-Hua Wang
Talanta 2010 Volume 81(1–2) pp:637-642
Publication Date(Web):15 April 2010
DOI:10.1016/j.talanta.2009.12.059
Hydrophilic ionic liquid–polyvinyl chloride (PVC) hybrids were prepared by immobilizing N-methylimidazole (N-mim) to PVC chains in toluene. The NmimCl–PVC hybrids were characterized by FT-IR, 1H NMR, surface charge analysis and elemental analysis. The immobilization ratio, i.e., the percentage of chloride on PVC chain reacting with N-mim to form the hybrid, varies from 4.3% to 15.1% by increasing the N-mim/PVC molar ratio. The most distinct feature of the hybrid is its excellent selectivity for adsorbing basic proteins by effective suppression of the non-specific protein adsorption by pure PVC, and a higher immobilization ratio facilitates better selectivity. In Tris–HCl buffer, 100 μg mL−1 of basic proteins, i.e., lysozyme (Lys), cytochrome c (cyt-c) and hemoglobin (Hb), were favorably adsorbed with efficiencies of 97%, 98% and 94% by the hybrid with an immobilization ratio of 15.1%, while the adsorption of acidic proteins, i.e., bovine albumin serum (BSA), transferring (Trf) and immunoglobulin G (IgG) were negligible. The retained Lys, cyt-c and Hb could be readily recovered by elution with phosphate buffer, carbonate buffer and SDS solution with efficiencies of 89%, 87% and 84%, respectively. Another feature of the hybrid is the significant improvement of the biocompatibility characterized by the maintenance of the activity of hemoglobin after adsorption and elution process. The practical usefulness of the hybrid was demonstrated by selective isolation of hemoglobin from human whole blood.
Co-reporter:Zhang-Run Xu;Xin Wang;Xiao-Feng Fan
Microchimica Acta 2010 Volume 168( Issue 1-2) pp:71-78
Publication Date(Web):2010 February
DOI:10.1007/s00604-009-0262-z
A novel extrusion driving protocol was developed based on micro-fabricated polydimethylsiloxane (PDMS) pneumatic valves. High efficiency liquid transfer was performed by using entirely overlapping control channels and fluid channels. A 0.5-s time is sufficient for the transfer of 9 μL sample solution between two chambers in the microchip with a nitrogen pressure of 70 kPa. The driving method was used in a microfluidic polymerase chain reaction (PCR) system, and rapid cycling of the PCR mixture in a closed loop was achieved. The amplification of DNA was demonstrated via both three-stage and two-stage PCR thermal cycling on the microchips resulting in significant reduction of the PCR time. The amplifications of 144-bp and 200-bp DNA fragments were achieved within 24 min using a three-stage protocol with 30 thermal cycles, and 130-bp DNA fragments within 12 min by using 20 thermal cycles in the two-stage system, compared to about 2 h in benchtop PCR with the same number of thermal cycles.
Co-reporter:Xu-Wei Chen, Ai-Mei Zou, Ming-Li Chen, Jian-Hua Wang and Purnendu K. Dasgupta
Analytical Chemistry 2009 Volume 81(Issue 3) pp:1291
Publication Date(Web):January 7, 2009
DOI:10.1021/ac802475b
Live HeLa cells immobilized on Sephadex G-50 beads were used as a medium for the preconcentration and speciation of inorganic arsenic. The sorption of arsenic species by live HeLa cells involves both surface uptake and bioaccumulation within the cells. At pH 3.0, the cells accumulate arsenate with high specificity over arsenite: 83.0 ± 1.3% of the arsenate was sorbed while the retention of arsenite was negligible at 2.1 ± 0.6%. The speciation of inorganic arsenic could thus be performed by direct determination of arsenate followed by quantifying total inorganic arsenic after conversion of arsenite to arsenate. We formed a disposable live cell preconcentration microcolumn with the live HeLa cells immobilized on Sephadex G-50 beads. After the sample was passed through the column for sorption to occur, the cells and any retained arsenate were stripped with 2 M HNO3. The arsenic in the 30 μL eluate was directly measured by graphite furnace atomic absorption spectrometry. A new microcolumn was used for each sample. With a sample volume of 450 μL, a S/N = 3 limit of detection (LOD) of 0.05 μg/L and a linear range of 0.15−2.5 μg/L were attained; the relative standard deviation (RSD) was 1.7% at 1.25 μg/L. The procedure was validated by arsenic speciation in certified reference river water.
Co-reporter:Mingli Chen, Ting Yang, Jianhua Wang
Analytica Chimica Acta 2009 Volume 631(Issue 1) pp:74-79
Publication Date(Web):5 January 2009
DOI:10.1016/j.aca.2008.10.019
Lanthanum hydroxide precipitate is for the first time coated onto cellulose fibre and serves as a novel sorption medium for separation and speciation of inorganic selenium. A micro-column packed with precipitate-layer-coated cellulose fibre is incorporated into a sequential injection system for selenite retention from a neutral aqueous solution, which is afterwards stripped with a NaBH4–NaOH solution as eluent. The hydride generation is actuated by merging the eluate and hydrochloric acid downstream, followed by the detection with atomic fluorescence spectrometry. Total inorganic selenium is derived by pre-reduction of selenate and speciation is estimated by difference. The coated precipitate layer can be used for 150 runs for selenium sorption, offering a clear advantage over the conventional precipitation protocols where a large amount of precipitate is dissolved into a small volume of eluent which might interfere with the detection. With a sample volume of 1.0 mL, an enrichment factor of 9.7 and a detection limit of 9 ng L−1 are obtained in a linear range of 0.05–2.5 μg L−1. A sampling frequency of 24 h−1 is achieved along with a R.S.D. of 1.7% at 0.5 μg L−1 Se(IV). The procedure is validated by analyzing selenium in a reference material GBW 10010 (rice) and a human hair sample. It is further demonstrated by speciation of inorganic selenium in surface water samples by pre-reduction of selenate.
Co-reporter:Zhuo Du;Yong-Liang Yu
Macromolecular Bioscience 2009 Volume 9( Issue 1) pp:55-62
Publication Date(Web):
DOI:10.1002/mabi.200800200
Co-reporter:Xuwei Chen;Shuai Chen;Jiawei Liu;Jianhua Wang
Microchimica Acta 2009 Volume 165( Issue 1-2) pp:
Publication Date(Web):2009 April
DOI:10.1007/s00604-008-0123-1
A direct solid-phase extraction procedure for the selective isolation of hemoglobin from complex matrices using lanthanum(III) modified zeolite (clinoptilolite) as sorbent was developed. The modified clinoptilolite provides a sorption capacity of 31.8 mg g-1 for hemoglobin (Hb). Experimental parameters governing the sorption efficiency, i.e., the pH of sample solution, the ionic strength and sorption time, were investigated. A sorption efficiency of 98% was achieved for 500 ng μL-1 Hb in 500 μL of sample solution. The absorbed Hb could be readily stripped by using 500 μL of a 0.01 mol L-1 orthophosphate solution, giving rise to a recovery of about 80%. The applicability of this method was demonstrated by processing human whole blood for the isolation of Hb, and satisfactory results were obtained by assay with SDS-PAGE.
Co-reporter:Mingli Chen, Yumei Huo, Jianhua Wang
Talanta 2009 Volume 78(Issue 1) pp:88-93
Publication Date(Web):15 April 2009
DOI:10.1016/j.talanta.2008.10.060
The separation and speciation of inorganic arsenic(III) and arsenic(V) are facilitated by employing a novel sequential injection system incorporating two mini-columns followed by detection with hydride generation atomic fluorescence spectrometry. An octadecyl immobilized silica mini-column is used for selective retention of the complex between As(III) and APDC, while the sorption of As(V) is readily accomplished by a 717 anion exchange resin mini-column. The retained As(III)–PDC complex and As(V) are effectively eluted with a 3.0 mol L−1 hydrochloric acid solution as stripping reagent, which well facilitates the ensuing hydride generation process via reaction with tetrahydroborate. With a sampling volume of 1.0 mL and an eluent volume of 100 μL for both species, linear ranges of 0.05–1.5 μg L−1 for As(III) and 0.1–1.5 μg L−1 for As(V) are obtained, along with enrichment factors of 7.0 and 8.2, respectively. Precisions of 2.8% for As(III) and 2.9% for As(V) are derived at the concentration level of 1.0 μg L−1. The practical applicability of the procedure has been demonstrated by analyzing a certified reference material of riverine water (SLRS-4), in addition to spiking recovery in a lake water sample matrix.
Co-reporter:Zhuo Du, Yong-Liang Yu, Xiao-Rui Yan and Jian-Hua Wang
Analyst 2008 vol. 133(Issue 10) pp:1373-1379
Publication Date(Web):11 Jul 2008
DOI:10.1039/B804347G
Multi-walled carbon nanotubes (MWNTs) were assembled on a silica surface using a polyelectrolyte-assisted layer-by-layer (LBL) assembly technique. The surface-assembled silica spheres with MWNTs (MWNTs/SiO2), which serve as a novel solid-phase extraction sorbent for separation/pre-concentration of basic proteins, was investigated. The adsorption behavior of cytochrome c (cyto-c) by MWNTs/SiO2 spheres agrees well with the Langmuir adsorption model. A thorough scrutiny of the experimental parameters affecting the adsorption of cyto-c from aqueous solution onto the MWNTs/SiO2 spheres and its subsequent desorption was carried out. A maximum adsorption capacity of cyto-c was derived as 112 mg (cyto-c) g−1 (MWNTs). A distinct feature of the MWNTs/SiO2-packed micro-column provides clear advantages of minimized flow impedance when operated in a flow system, in addition to better separation efficiency as well as the favorable enrichment capability of proteins, characterized by an enrichment factor of 30 by using 2.0 mL of aqueous solution. The practical applicability of the MWNTs/SiO2 spheres as a sorbent for the isolation of basic proteins from acidic protein species was demonstrated by effective separation of cyto-c from bovine serum albumin (BSA).
Co-reporter:Yang Shu, Dehong Cheng, Xuwei Chen, Jianhua Wang
Separation and Purification Technology 2008 Volume 64(Issue 2) pp:154-159
Publication Date(Web):17 December 2008
DOI:10.1016/j.seppur.2008.09.010
A water-in-ionic liquid reverse microemulsion prepared with water, sodium bis(2-ethylhexyl) sulfosuccinate (AOT) and ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate (BmimPF6) has been proved to entail selective extraction of hemoglobin. 96% of the hemoglobin in a 500-μL of aqueous solution (100 ng μL−1, pH 6.3) could be readily extracted by employing an equal volume of microemulsion (with an AOT concentration of 50 mmol L−1, and the molar ratios of water/AOT/BmimPF6 of 6/50/5). 73% of the hemoglobin transferred into the microemulsion system could afterwards be rapidly back extracted into an aqueous phase with a 6-mol L−1 urea as stripping reagent. The hemoglobin in the microemulsion system might exist either in the bulk of the ionic liquid phase or in the “water pools” of the microemulsion system. In addition, electrostatic interaction is among the main driving forces for the transfer of hemoglobin from aqueous phase into the microemulsion. The practical applicability of the present microemulsion system for sample pretreatment was demonstrated by the successful isolation of hemoglobin from human whole blood.
Co-reporter:Ming-Li Chen, Yong Tian and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 vol. 23(Issue 6) pp:876-880
Publication Date(Web):25 Apr 2008
DOI:10.1039/B802595A
A cellulose fibre packed micro-column was used for sorption preconcentration of ultra-trace cadmium and successive coating of a thin layer of sodium tetrahydroborate solution. The retained cadmium was stripped with hydrochloric acid and in-situ vapor generation on the cellulose surface was initiated by reaction with the coated layer of reducing reagent. The vapor was detected by atomic fluorescence spectrometry (AFS). The integration of preconcentration, reducing reagent immobilization, elution and in-situ vapor generation onto the cellulose surface significantly simplifies the entire operation, where a single syringe pump suffices fluids delivery, providing sufficient stability and long-term reliability indicated by an intra-day RSD <5%. In addition, the detection limit and precision were significantly improved with respect to those obtained by a conventional elution approach. With a sampling volume of 1.0 mL, a quantitative retention of cadmium was obtained within a linear range of 0.01–1.0 μg L−1, along with an enrichment factor of 19.5 and a sampling frequency of 12 h−1. A precision of 1.9% at 0.2 μg L−1 was obtained and a detection limit of 3 ng L−1 was derived. The procedure was validated by analyzing certified reference materials of Riverine Water (SLRS-4), and Trace Elements in Water (GBW 08608), in addition to spiking recovery in a coastal sea water.
Co-reporter:Yong-Liang Yu, Zhuo Du, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 vol. 23(Issue 4) pp:493-499
Publication Date(Web):25 Feb 2008
DOI:10.1039/B718977J
A miniaturized atomic fluorescence spectrometer (AFS) incorporating a dielectric barrier discharge (DBD) atomizer was developed in a lab-on-valve (LOV) configuration. The entire system integrates hydride generation, gas–liquid separation, in-situatomization and fluorescence detection. The hydride isolated from the gas–liquid separation chamber was swept by an argon flow into the atomization chamber, where free atoms of the analyte, i.e., arsenic, were formed in the DBD discharge area, which were afterwards immediately transported into the detection chamber to undergo excitation by an incident light from a hollow cathode lamp and the fluorescence was monitored using a side-on photomultiplier with its receiving window directly adhered onto one side of the detection chamber. Some important aspects concerning the performance of the entire system, i.e., the configurations of the atomization and detection chambers, the parameters governing the atomization process and the chemical and flow variables were investigated. When employing a 500 μl sample volume, a detection limit of 0.03 μg l−1(As) was derived within a linear range of 0.10–5.00 μg l−1. The detection limit of the present system is at the same level as that obtained by using a commercial AFS system. A sampling frequency of 80 h−1 was obtained along with an RSD value of 2.8% at the level of 2.0 μg l−1 As. The system was applied to the determination of arsenic in two certified reference materials, i.e., GBW10010 (rice) and GBW09101 (human hair), achieving satisfactory results.
Co-reporter:Ai-Mei Zou, Xu-Wei Chen, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 vol. 23(Issue 3) pp:412-415
Publication Date(Web):07 Dec 2007
DOI:10.1039/B714535G
Egg-shell membrane (ESM) is a unique cell surface with various functional groups, providing the potential for bio-sorption of metal species. We have demonstrated the selective retention of chromium(VI)via a reductive sorption process, while Cr(III) is virtually not retained. This includes adsorption of Cr(VI) onto the ESM surface while charge transfer on the ESM results in the reduction of Cr(VI) to Cr(III) through transient, unstable species of Cr(V) and Cr(IV). A novel procedure for chromium speciation was thus developed in a sequential injection system with detection by electrothermal atomic absorption spectrometry. The procedure includes the separation and preconcentration of Cr(VI) on ESM at pH 2 and its subsequent detection after elution, followed by conversion of Cr(III) to Cr(VI) and total chromium analysis, Cr(III) finally being obtained by subtraction. With a sampling volume of 1000 µl, an enrichment factor of 13.3 was achieved. A linear range of 0.05–1.25 µg l−1 for Cr(VI), along with a detection limit of 0.01 µg l−1 and a precision of 3.2% at the level of 0.5 µg l−1, were obtained. Chromium speciation was performed by using a certified reference material of riverine water (GBW08608) and cave water.
Co-reporter:Yongliang Yu Dr.;Zhuo Du;Mingli Chen ;Jianhua Wang
Angewandte Chemie 2008 Volume 120( Issue 41) pp:8027-8030
Publication Date(Web):
DOI:10.1002/ange.200802681
Co-reporter:De-Hong Cheng, Xu-Wei Chen, Yang Shu, Jian-Hua Wang
Talanta 2008 Volume 75(Issue 5) pp:1270-1278
Publication Date(Web):15 June 2008
DOI:10.1016/j.talanta.2008.01.044
Ionic liquid was for the first time employed for selective isolation of heme-protein species. Direct extraction of hemoglobin into ionic liquid without using any concomitant reagent or extractant was carried out. Hemoglobin at the level of 100 ng μL−1 could readily be quantitatively extracted into ionic liquid (IL) 1-butyl-3-trimethylsilylimidazolium hexafluorophosphate (BtmsimPF6) in the absence of any co-existing extractants/additives at pH 7, at the same time; however, the other protein species do not interfere and remain in the aqueous phase. A back extraction efficiency of ca. 80% for 20 ng μL−1 hemoglobin in ionic liquid phase was achieved with sodium dodecyl sulfate (SDS) solution as stripping reagent. 57Fe Mossbauer spectra and circular dichroism (CD) spectra indicated that the penta-coordinated ferrous atom in hemoglobin provide a vacant or free coordinating position, which could be occupied by the cationic Btmsim+ moiety. The interaction/coordination reaction between the iron atom in the heme group of hemoglobin and the cationic ionic liquid moiety furnishes the driving force for facilitating fast transfer of hemoglobin into BtmsimPF6. The present system was applied for selective isolation of heme-protein, i.e., hemoglobin from human whole blood without any pretreatment, giving rise to satisfactory results.
Co-reporter:Ai-Mei Zou, Xiao-Yan Tang, Ming-Li Chen, Jian-Hua Wang
Spectrochimica Acta Part B: Atomic Spectroscopy 2008 Volume 63(Issue 5) pp:607-611
Publication Date(Web):May 2008
DOI:10.1016/j.sab.2008.02.008
A procedure for chromium preconcentration and speciation with a dual mini-column sequential injection system coupled with electrothermal atomic absorption spectrometry (ETAAS) was developed. At pH 6, the sample solution was firstly aspirated to flow through a Chlorella vulgaris cell mini-column on which the Cr(III) was retained. The effluent was afterwards directed to flow through a 717 anion exchange resin mini-column accompanied by the retention of Cr(VI). Thereafter, Cr(III) and Cr(VI) were eluted by 0.04 mol L− 1 and 1.0 mol L− 1 nitric acid, respectively, and the eluates were quantified with ETAAS. Chemical and flow variables governing the performance of the system were investigated. By using a sampling volume of 600 µL, sorption efficiencies of 99.7% for Cr(III) and 99% for Cr(VI) were achieved along with enrichment factors of 10.5 for Cr(III) and 11.6 for Cr(VI), within linear ranges of 0.1–2.5 µg L− 1 for Cr(III) and 0.12–2.0 µg L− 1 for Cr(VI). Detection limits of 0.02 µg L− 1 for Cr(III) and 0.03 µg L− 1 for Cr(VI) along with RSD values of 1.9% for Cr(III) and 2.5% for Cr(VI) (1.0 µg L− 1, n = 11) were obtained. The procedure was validated by analyzing a certified reference material of GBW08608 and further demonstrated by chromium speciation in river and tap water samples.
Co-reporter:Yongliang Yu Dr.;Zhuo Du;Mingli Chen ;Jianhua Wang
Angewandte Chemie International Edition 2008 Volume 47( Issue 41) pp:7909-7912
Publication Date(Web):
DOI:10.1002/anie.200802681
Co-reporter:Xu-Wei Chen, Jian-Hua Wang
Analytica Chimica Acta 2007 Volume 602(Issue 2) pp:173-180
Publication Date(Web):29 October 2007
DOI:10.1016/j.aca.2007.09.019
Termed as the third generation of flow injection analysis, the lab-on-valve (LOV) system is closely related to the principle of sequential injection analysis and constructed aiming at facilitating various miniature analytical operations and downscaling sample/reagent consumption. The highly integrated configuration makes LOV system compatible with virtually all kinds of spectroscopic detection techniques and presents it an intelligent platform for bead-injection protocol. The minimized reagent consumption and precise fluidic manipulation also propose the LOV system an excellent candidate for the adaptation of sample processing in the macroscopic world with the microfluidic analysis system. After a few years development, it has been applied extensively in the miniaturization and automation of analytical procedures, especially in the field of bioassays. This review presents the up-to-date progress and some of the selected applications of the LOV system for bioanalytical assays. In addition, future perspectives are discussed.
Co-reporter:Yang Shu, Jun Lu, Quan-Xing Mao, Ru-Sheng Song, Xue-Ying Wang, Xu-Wei Chen, Jian-Hua Wang
Carbon (April 2017) Volume 114() pp:
Publication Date(Web):April 2017
DOI:10.1016/j.carbon.2016.12.038
By taking advantage of the structural tunability of ionic liquids (ILs), a series of imidazolium ILs were employed as precursors to prepare carbon dots (IL-CDs) and as regulators to control their properties. The simultaneous formation of hydrophilic CDs (IL-HCDs) and organophilic CDs (IL-OCDs) is achieved in hydrothermal reaction system by undergoing sulfuric acid carbonization. The quantum yields (QY) of IL-OCDs are closely correlated with both the cationic and anionic moieties of the ionic liquids, i.e., longer side chains of cations in the imidazolium ILs and weakly nucleophilic anions tend to produce highly fluorescent IL-OCDs. Both IL-HCDs and IL-OCDs exhibit low cytotoxicity, and that of IL-HCDs is even lower than IL-OCDs. A drug delivery system is constructed by combining anticancer drug curcumin (Cur) with IL-OCDs via hydrophobic interaction, among which 1,3-dibutylimidazolium nitrate derived IL-OCDs exhibit highest photoluminescence. In addition, it serves as a favorable drug carrier with high drug loading efficiency and facilitates rapid penetration/transportation of Cur into the cell interior, which significantly accelerates the apoptosis of HeLa cells. This process is further visualized by cell imaging.
Co-reporter:Jia-Wei Liu ; Yue Zhang ; Xu-Wei Chen
ACS Applied Materials & Interfaces () pp:
Publication Date(Web):
DOI:10.1021/am503298v
Graphene oxide-La(BTC)(H2O)6 (H3BTC=1,3,5-benzenetricarboxylic acid) metal organic framework composites (LaMOF-GOn, n = 1–6, corresponding to the percentage of GO at 1, 2, 3, 4, 5, and 10%) are prepared through a simple and large-scale method at room temperature. The obtained composites are characterized by ATR-FTIR spectra, SEM, XRD, TGA, and N2 adsorption–desorption isotherm. The presence of GO significantly changes the morphologies of the composites from spindly rectangular rods to irregular thick blocks and increases their surface area from 14.8 cm2 g–1 (LaMOFs) to 26.6 cm2 g–1 (LaMOF-GO3), whereas at the same time, the crystalline structure of La(BTC)(H2O)6 is maintained. As a novel solid-phase adsorbent the LaMOF-GO composite exhibits outstanding adsorption properties for proteins. The strong hydrophobic interaction, especially π–π interaction between protein and the composite, is the main driving force for protein adsorption. In particular, highly selective isolation of hemoglobin (Hb) is achieved by using LaMOF-GO3 composite as sorbent in 4 mM B-R buffer containing 0.05 mol L–1 NaCl at pH 8. The retained Hb could be effectively recovered with a 1 mM B-R buffer at pH 10, giving rise to a recovery of 63%. The practical applicability of the LaMOF-GO3 composite is demonstrated by the selective adsorption of Hb from human whole blood, and SDS-PAGE assays indicate that Hb could be selectively isolated with high purity from biological samples of complex matrixes.
Co-reporter:Xuwei Chen, Jiawei Liu and Jianhua Wang
Analytical Methods (2009-Present) 2010 - vol. 2(Issue 9) pp:
Publication Date(Web):
DOI:10.1039/C0AY00342E
Co-reporter:Shuai Chen, Jia-Wei Liu, Mei-Ling Chen, Xu-Wei Chen and Jian-Hua Wang
Chemical Communications 2012 - vol. 48(Issue 61) pp:NaN7639-7639
Publication Date(Web):2012/06/13
DOI:10.1039/C2CC32984K
Graphene quantum dots prepared by a one-step hydrothermal procedure in a microwave exhibit an unusual emission transformation in strong acidic media and at high concentration, induced by self-assembled J-type aggregation under restrained π–π interactions.
Co-reporter:Ting Yang, Lin-Yu Ma, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2015 - vol. 30(Issue 4) pp:NaN935-935
Publication Date(Web):2015/02/11
DOI:10.1039/C4JA00418C
Metallothioneins (MTs) are low molecular weight, cysteine-rich proteins widely distributed in nature. Two isoforms of MT, e.g., metallothionein isolated from rabbit liver (rMT) and recombined cyanobacteria metallothionein (SmtA), were immobilized on spherical SiO2 particles to evaluate their biosorption behaviors for cadmium. We found that cadmium binding on both MT isoforms is pH dependent and follows Langmuir adsorption, and their adsorption dynamic fits the pseudo-second-order kinetics model. The affinity of cadmium on rMT is higher than that on SmtA, which is in accordance with the HSAB theory. On the other hand, however, SmtA exhibits a higher cadmium sorption capacity than rMTs both statically and dynamically. The SmtA–SiO2 composite was thus used to pack a mini-column for the evaluation of cadmium preconcentration. The cadmium retained on the SmtA surface was recovered with a small amount of thiourea in nitric acid and quantified by graphite furnace atomic absorption spectrometry (GFAAS). Within a range of 5–100 ng L−1 and a sample volume of 1 mL, an enrichment factor of 13.8 was achieved along with a detection limit of 1.4 ng L−1, and a precision of 3.2% RSD at 50 ng L−1. The procedure was validated by analyzing cadmium in certified reference materials and a series of environmental water samples.
Co-reporter:Ji Feng, Wen-Jing Wang, Xin Hai, Yong-Liang Yu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 3) pp:NaN393-393
Publication Date(Web):2015/11/23
DOI:10.1039/C5TB01999K
Carbon dots (CDs) with a high quantum yield have been synthesized by a facile and green one-pot approach under microwaves with silkworm chrysalis (SC) as the natural carbon source, without using any other chemicals/reagents. The morphology and optical properties of the resultant CDs are characterized by TEM, XRD, FT-IR, XPS, UV-vis and photoluminescence (PL). The SC-CDs have an average size of 19 nm, and contain C, O and N with relative contents of ca. 71.32%, 22.96% and 5.72%, respectively. A significant emission at 420 nm at an excitation wavelength of 350 nm is recorded, resulting in a quantum yield of 46% with quinine sulfate (quantum yield 54%) as a reference. In addition to excellent solubility and stability in aqueous medium, the SC-CDs exhibit excitation-dependent photoluminescence with a large Stokes shift of 70 nm. It is further demonstrated that the SC-CDs exhibit a low cytotoxicity at a higher concentration of 15 mg mL−1 and they are able to display bright blue, green and red colors under an inverted fluorescence microscope during cell imaging experiments, showing their vast potential in bioimaging.
Co-reporter:Yue Zhang, Jia-Wei Liu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 6) pp:NaN989-989
Publication Date(Web):2014/12/23
DOI:10.1039/C4TB01792G
A three-dimensional graphene oxide framework is prepared via a simple and cost-effective one-pot approach through the hydrogen-bonding interaction between amylopectin and graphene oxide in the presence of hydrazine hydrate acting as a reducing reagent. The framework is shortly termed as AP-rGO and it is characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), surface charge analysis and thermogravimetric analysis (TGA). The obtained AP-rGO framework exhibits excellent adsorption performance toward hemoglobin in the presence of other protein species. It provides a maximum adsorption capacity of 1010 mg g−1. In a neutral medium (at pH 7), 70 mg L−1 of Hb in 1.0 mL of aqueous solution could be effectively adsorbed by 1.0 mg of the AP-rGO framework, giving rise to an adsorption efficiency of 92.7%. The practical application of the AP-rGO framework is demonstrated by the removal of a highly abundant protein, i.e., hemoglobin, from complex biological sample matrices, e.g., human whole blood. The removal efficiency is well confirmed by sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) assay.
Co-reporter:Dan-Dan Zhang, Qing Chen, Lin-Lin Hu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 21) pp:NaN4369-4369
Publication Date(Web):2015/04/21
DOI:10.1039/C5TB00544B
A Keggin-type cobalt mono-substituted silicotungstic acid doped with aniline (SiW11Co–PANI composite, where PANI denotes polyaniline) is prepared by a liquid phase method at room temperature. The obtained SiW11Co–PANI composite possesses a porous framework structure and has proven to be a promising adsorbent for the retention of proteins, which exhibits favorable selectivity toward the adsorption of ovalbumin from egg whites. 5.0 mg of SiW11Co–PANI composite gives rise to an adsorption efficiency of >70% for 100 mg L−1 ovalbumin in 1.0 mL of sample solution within a wide pH range of 3–9, and a maximum adsorption efficiency of 92% is achieved at pH 9. The adsorption behavior of ovalbumin onto the SiW11Co–PANI composite fits the Langmuir adsorption model, corresponding to a sorption capacity of 200.0 mg g−1. The retained ovalbumin could be readily recovered by using a 0.1 mol L−1 phosphate buffer at pH 5.6 as a stripping reagent, providing a recovery of 84.4%. Circular dichroism (CD) spectra illustrate virtually no change in the conformation of ovalbumin after the process of adsorption–desorption. The SiW11Co–PANI composite has been applied for the selective adsorption of ovalbumin from the chicken egg white, and SDS-PAGE assay demonstrates that high purity of ovalbumin is obtained.
Co-reporter:Qing Chen, Dan-Dan Zhang, Meng-Meng Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 34) pp:NaN6970-6970
Publication Date(Web):2015/07/28
DOI:10.1039/C5TB01298H
A novel polyoxometalate (POM)-based organic–inorganic hybrid [C33H24O4]H3PMo12O40, namely, TPPA–PMo12, is prepared via a one-pot hydrothermal reaction between a Keggin POM (H3PMo12O40, PMo12) and a star-like N-donor ligand (tri(4-pyridylphenyl)amine, TPPA). The hybrid polyoxometalate is confirmed by characterization with XRD, FT-IR, TGA, SEM and EDS. It exhibits excellent adsorption performance towards β-lactoglobulin, and thus a solid-phase extraction procedure was established for the efficient and selective isolation of β-lactoglobulin from complex sample matrices. At pH 5.0, an adsorption efficiency of 99.2% is achieved for processing 100 μg mL−1 β-lactoglobulin in 1.0 mL aqueous solution with 0.5 mg TPPA–PMo12 as an adsorbent. The adsorption behavior of β-lactoglobulin fits the Langmuir model, corresponding to a theoretical adsorption capacity of 1428 mg g−1. The retained β-lactoglobulin could be readily recovered by rinsing with 0.05 mol L−1 Tris-HCl buffer, facilitating a recovery of 91.5%. The hybrid polyoxometalate was practically applied to the selective isolation of β-lactoglobulin from milk whey, and SDS-PAGE assay results clearly indicate that β-lactoglobulin of high-purity is obtained.
Co-reporter:Jia-Wei Liu, Ting Yang, Shuai Chen, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 6) pp:NaN818-818
Publication Date(Web):2012/11/30
DOI:10.1039/C2TB00334A
A novel functionalized graphene-based composite is prepared by successive modification of graphene oxide (GO) with epichlorohydrin (ECH), iminodiacetic acid (IDA) and 1-phenylboronic acid (1-PBA) through covalent functionalization and then chelating with nickel ions. Characterizations by FT-IR, XRD, SEM, TGA and ICP-MS demonstrate the successful modification of the graphene surface, resulting in a GO–PBA–IDA–Ni composite with a Ni2+ immobilization amount of 3.01 × 10−3 mol g−1. The composite shows favorable selectivity for the adsorption of lysozyme (Lys). In practice, a homogeneous GO–PBA–IDA–Ni film with a thickness of ca. 1.0 μm is fabricated by filtering the composite through a cellulose membrane with a pore aperture of 1.2 μm. The GO–PBA–IDA–Ni film is subsequently fastened into a rounded membrane cartridge and incorporated into a sequential injection system for on-line selective isolation of Lys. An adsorption efficiency of ca. 96% is achieved for 25 μg ml−1 Lys in 500 μl of sample solution at a loading rate of 5 μl s−1. Metal affinity and electrostatic interactions are the main driving forces for governing the protein adsorption behaviors. The retained Lys is readily recovered by a borate buffer (pH 10) containing 1.0 mol l−1 NaCl and 20 mmol l−1 imidazole, giving rise to a recovery of ca. 90%. The practical applicability of the composites is demonstrated by selective isolation of Lys from chicken egg white, and SDS-PAGE assay indicates that Lys is selectively isolated with high purity from complex matrices.
Co-reporter:Mei-Ling Chen, Li-Ming Shen, Shuai Chen, Hui Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 20) pp:NaN2589-2589
Publication Date(Web):2013/03/25
DOI:10.1039/C3TB20234H
β-FeOOH has shown promise as a new contrast agent in magnetic resonance imaging (MRI), however, sensitive and accurate MR imaging is largely limited by its low transverse relaxivity (r2). Herein, for the first time we report in situ growth of β-FeOOH nanorods onto PEGylated graphene oxide (GO) sheets to produce a nanocomposite, e.g., GO-PEG–β-FeOOH. This nanocomposite exhibits a record ultra-high transverse relaxivity (r2) value of 303.81 mM−1 s−1, that is, >60 times higher than those achieved by hitherto reported β-FeOOH based MRI contrast agents. This well facilitates its practical use as a contrast agent for in vivo MR imaging. PEG on the surface of the GO nanocomposite improved the colloidal stability in aqueous medium. In addition, in vitro cell viability tests demonstrated that GO-PEG–β-FeOOH has minimal cellular toxicity. GO-PEG–β-FeOOH has been used for loading doxorubicin hydrochloride (DOX) with a capacity of 1.35 mg mg−1, which exhibits high efficiency in Hela cell apoptosis. These results indicated that GO-PEG–β-FeOOH provides an effective alternative to the existing nanoparticle-based contrast agents for non-invasive in vivo MR imaging and cancer therapy.
Co-reporter:Xin Hai, Quan-Xing Mao, Wen-Jing Wang, Xiao-Feng Wang, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 47) pp:NaN9114-9114
Publication Date(Web):2015/11/02
DOI:10.1039/C5TB01954K
Boron-doped graphene quantum dots (B-GQDs) are prepared via a one-pot acid-free microwave approach with graphene oxide as the carbon source and borax as the boron source. Boron atoms are incorporated into the graphene framework by attacking the defects in the graphene structure, deriving an atomic percentage of 1.44% in the final product. Boron atom doping into the graphene structure and restoration of defects in the graphene structure bring the obtained B-GQDs favorable photoluminescence behaviors. The as-prepared B-GQDs exhibit excitation-independent photoluminescence behaviors with an excitation/emission maximum at 320/430 nm, and a fluorescence quantum yield of 21.1%. Moreover, stable photoluminescence is observed within a wide range of pH 3.0–11.0. A tolerance to an external ionic strength of up to 2.0 mol L−1 KCl along with an excellent anti-photobleaching capability is achieved. The standard MTT assay suggests that the B-GQDs are of low cytotoxicity with favorable biocompatibility, and a cell viability of 87% could be achieved at 4.0 mg mL−1 of B-GQDs. The practical application of B-GQDs in bio-analysis is demonstrated by bio-imaging of HeLa cells.
Co-reporter:Hao Meng, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2011 - vol. 21(Issue 38) pp:NaN14863-14863
Publication Date(Web):2011/08/18
DOI:10.1039/C1JM11918D
A novel one-pot procedure for the synthesis of ionic liquid N,N-bis[2-methylbutyl] imidazolium hexafluorophosphate (PPimPF6/TiO2) nanocomposites is reported for the first time. During the in situ formation of TiO2 nanoparticles via hydrolysis of tetrabutyl titanate (TBOT), the ionic liquid PPimPF6 is simultaneously incorporated into the TiO2 nanostructure via H-bonding. The PPimPF6/TiO2 nanocomposites are characterized by means of TEM, FT-IR and XRD, showing that they possess the structure of anatase and exhibit selective adsorption for neutral proteins, hemoglobin (Hb) in this particular case, under controlled experimental conditions. At pH 8, an adsorption efficiency of 88.3% for 150 μg mL−1 Hb is achieved by 2.0 mg of PPimPF6/TiO2 nanocomposites, while virtually no adsorption is observed for the basic protein cytochrome c (cyt-c) and the acidic protein bovine serum albumin (BSA). An adsorption capacity of 122.3 μg mg−1 is obtained for Hb by calculation on the amount of the incorporated ionic liquid, corresponding to a 5-fold improvement with respect to that achieved by pure PPimPF6. The retained Hb on the PPimPF6/TiO2 nanocomposites could be readily collected by stripping with 0.5% SDS, giving rise to a recovery of ca. 73%. The circular dichroism (CD) spectra indicate no conformational change of Hb after the adsorption/elution process. The selective isolation of Hb from human whole blood is achieved by the nanocomposites.
Co-reporter:Wen-Jing Wang, Jun-Mei Xia, Xin Hai, Ming-Li Chen and Jian-Hua Wang
Environmental Science: Nano 2017 - vol. 4(Issue 5) pp:
Publication Date(Web):
DOI:10.1039/C7EN00027H
Co-reporter:Dan-Dan Zhang, Peng-Fei Guo, Lin-Lin Hu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2017 - vol. 5(Issue 4) pp:NaN756-756
Publication Date(Web):2016/12/08
DOI:10.1039/C6TB02733D
A novel polyoxometalate (POM)-based hybrid is prepared for the selective adsorption of acidic and/or basic proteins. The solidification of the POM moiety P8W48 is firstly achieved through dehydration condensation between the –OH group on the P8W48 surface and the Si–OH of aminopropyltriethoxysilane (APTS), and thereafter further condensation of the P8W48O184–APTS intermediate with poly(acrylic acid) (PAA) produces a hybrid, by linking carboxyl groups in PAA with –NH2 groups in P8W48O184–APTS via the formation of an amide bond. The P8W48–APTS–PAA hybrid surface is negatively charged due to abundant COO− groups from PAA, which provides electrostatic interactions with positively charged proteins by varying pHs. Meanwhile, the d–p π bond in P8W48 offers strong affinity to other proteins via π–π stacking interaction. The hybrid thus offers potential for achieving selective adsorption of either acidic or basic proteins by simply controlling the adsorption conditions, i.e., pH value or ionic strength of the adsorption medium. With ovalbumin (Ova) and lysozyme (Lys) as the models of acidic and basic proteins, their adsorption behaviors fit the Langmuir model, with adsorption capacities of 367.0 mg g−1 and 74.0 mg g−1, respectively. The retained proteins are readily recovered with 0.01 mol L−1 CTAB, providing recoveries of 89.0% for Ova and 93.0% for Lys. The P8W48–APTS–PAA hybrid is further applied for the isolation of Ova and Lys from real biological samples, egg white.
Co-reporter:Ting Yang, Lan-hua Liu, Jia-wei Liu, Ming-Li Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2012 - vol. 22(Issue 41) pp:NaN21916-21916
Publication Date(Web):2012/09/05
DOI:10.1039/C2JM34712A
Graphene oxide (GO) nanosheets were decorated with a cysteine-rich metal-binding protein, cyanobacterium metallothionein (SmtA). The SmtA–GO composites were characterized by means of FT-IR, AFM and TGA, giving rise to a SmtA binding amount of 867 mg g−1. The SmtA–GO composites exhibit ultra-high selectivity toward the adsorption of cadmium, i.e., the tolerant concentrations for the coexisting metal and anionic species were 1–800000 fold improved after SmtA decoration with respect to bare GO. The SmtA–GO composites were then assembled onto the surface of cytopore microbeads and used for highly selective adsorption and preconcentration of ultra-trace cadmium. In comparison with bare GO (carboxyl-rich GO) loaded cytopore (GO@cytopore), SmtA–GO loaded cytopore (SmtA–GO@cytopore) shows a 3.3-fold improvement over the binding capacity of cadmium, i.e. 7.70 mg g−1 for SmtA–GO@cytopore compared to 2.34 mg g−1 for that by GO@cytopore. A novel procedure for selective cadmium preconcentration was developed using SmtA–GO@cytopore beads as a renewable sorption medium incorporated into a sequential injection lab-on-valve system, with detection by graphite furnace atomic absorption spectrometry (GFAAS). The cadmium retained on the SmtA–GO surface was eluted with a small amount of nitric acid. An enrichment factor of 14.6 and a detection limit of 1.2 ng L−1 were achieved within a linear range of 5–100 ng L−1 by using a sample volume of 1 mL. The procedure was validated by analyzing cadmium in certified reference materials and a series of environmental water samples.
Co-reporter:Quan-Xing Mao, Wen-Jing Wang, Xin Hai, Yang Shu, Xu-Wei Chen and Jian-Hua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 29) pp:NaN6018-6018
Publication Date(Web):2015/06/22
DOI:10.1039/C5TB00963D
The regulation of hydrophilicity/hydrophobicity of carbon dots (CDs) at will is most important. One pot simultaneous preparation of hydrophilic and/or hydrophobic CDs is herein reported, via a hydrothermal process with 1-butyl-3-methylimidazolium hexafluorophosphate as the carbon source in a H3PO4–ethanol medium. The hydrophilicity or hydrophobicity of CDs (or their proportions) is simply regulated by varying the H3PO4/ethanol molar ratio. Hydrophilic and hydrophobic CDs are obtained simultaneously with H3PO4/ethanol molar ratios within 0–1.72, while hydrophilic or hydrophobic CDs are the sole product obtained from H3PO4–BmimPF6 or BmimPF6-only systems. The CDs exhibit excitation-dependent maximum fluorescence at 360/440 nm (hydrophilic) and 430/510 nm (hydrophobic), with quantum yields of 17.0% and 7.7%, respectively. Both hydrophilic and hydrophobic CDs obtained by this approach exhibit favorable biocompatibility and offer great potential in bio-imaging as demonstrated for the fluorescent labeling and imaging of live HeLa cells.
Co-reporter:Yang Zhang, Lu Han, Lin-Lin Hu, Yan-Qin Chang, Rong-Huan He, Ming-Li Chen, Yang Shu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 30) pp:NaN5184-5184
Publication Date(Web):2016/07/11
DOI:10.1039/C6TB00987E
A pH and redox responsive bi-trigger continuous drug release nanocarrier is developed by capping mesoporous carbon nanoparticles (MCNs) with polyacrylic acid (PAA), termed as PAA-ss-MCN. The nanocarrier contains disulfide bond units and exhibits pH responsive behavior. It provides promising potential for drug loading due to the internal uniform channels and large surface area of MCNs. PAA grafted on the exterior surface of MCNs acts as a gating layer, generating a novel nano-container and a pH-responsive intelligent nanovalve. By loading doxorubicin (DOX) in PAA-ss-MCN, its sequential release is achieved via two approaches: (1) the intracellular acidic environment induces partial release from the surface of the PAA gating layer, (2) release of the drug sealed in nanochannels via disruption of the integrity of the nanocarrier by glutathione (GSH) caused dissociation of disulfide bonds in the physiological environment. As a result, release of 62% loaded drug is readily achieved. After culturing with HeLa cells, DOX transports into the cell interior and therein exhibits pH- and GSH-sensitive release. As most tumor sites exhibit more acidic environments or high redox potential, the pH- and GSH-sensitive releasing capability of PAA-ss-MCN is particularly useful for controllable drug delivery by taking advantage of the inherent characteristics of tumor cells.
Co-reporter:Yong-Liang Yu, Zhuo Du, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 - vol. 23(Issue 4) pp:NaN499-499
Publication Date(Web):2008/02/25
DOI:10.1039/B718977J
A miniaturized atomic fluorescence spectrometer (AFS) incorporating a dielectric barrier discharge (DBD) atomizer was developed in a lab-on-valve (LOV) configuration. The entire system integrates hydride generation, gas–liquid separation, in-situatomization and fluorescence detection. The hydride isolated from the gas–liquid separation chamber was swept by an argon flow into the atomization chamber, where free atoms of the analyte, i.e., arsenic, were formed in the DBD discharge area, which were afterwards immediately transported into the detection chamber to undergo excitation by an incident light from a hollow cathode lamp and the fluorescence was monitored using a side-on photomultiplier with its receiving window directly adhered onto one side of the detection chamber. Some important aspects concerning the performance of the entire system, i.e., the configurations of the atomization and detection chambers, the parameters governing the atomization process and the chemical and flow variables were investigated. When employing a 500 μl sample volume, a detection limit of 0.03 μg l−1(As) was derived within a linear range of 0.10–5.00 μg l−1. The detection limit of the present system is at the same level as that obtained by using a commercial AFS system. A sampling frequency of 80 h−1 was obtained along with an RSD value of 2.8% at the level of 2.0 μg l−1 As. The system was applied to the determination of arsenic in two certified reference materials, i.e., GBW10010 (rice) and GBW09101 (human hair), achieving satisfactory results.
Co-reporter:Ai-Mei Zou, Xu-Wei Chen, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 - vol. 23(Issue 3) pp:NaN415-415
Publication Date(Web):2007/12/07
DOI:10.1039/B714535G
Egg-shell membrane (ESM) is a unique cell surface with various functional groups, providing the potential for bio-sorption of metal species. We have demonstrated the selective retention of chromium(VI)via a reductive sorption process, while Cr(III) is virtually not retained. This includes adsorption of Cr(VI) onto the ESM surface while charge transfer on the ESM results in the reduction of Cr(VI) to Cr(III) through transient, unstable species of Cr(V) and Cr(IV). A novel procedure for chromium speciation was thus developed in a sequential injection system with detection by electrothermal atomic absorption spectrometry. The procedure includes the separation and preconcentration of Cr(VI) on ESM at pH 2 and its subsequent detection after elution, followed by conversion of Cr(III) to Cr(VI) and total chromium analysis, Cr(III) finally being obtained by subtraction. With a sampling volume of 1000 µl, an enrichment factor of 13.3 was achieved. A linear range of 0.05–1.25 µg l−1 for Cr(VI), along with a detection limit of 0.01 µg l−1 and a precision of 3.2% at the level of 0.5 µg l−1, were obtained. Chromium speciation was performed by using a certified reference material of riverine water (GBW08608) and cave water.
Co-reporter:Yong Tian, Zhao-Ming Xie, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2011 - vol. 26(Issue 7) pp:NaN1413-1413
Publication Date(Web):2011/03/28
DOI:10.1039/C0JA00265H
A novel green/biodegradable adsorbent, mungbean-coat, has been investigated for the adsorption of ultra-trace amounts of cadmium. Carboxylic groups on the bean-coat effectively retain the cadmium ions via coordinative interactions. This well facilitates the adsorption of cadmium ions which can readily be recovered by acid elution. In practice, bean-coat is used to pack a mini-column for on-line adsorption and preconcentration of cadmium from environmental samples with detection by electrothermal atomic absorption spectrometry. By using a sample loading volume of 1.4 mL and an eluent volume of 70 μL, an enrichment factor of 19.8 along with a detection limit of 1.4 ng L−1 are achieved. A precision of 2.4% RSD at the level of 0.05 μg L−1 is derived. The present procedure has been applied for the determination of cadmium in certified reference materials (GBW08608 Trace Elements in Water and CRM 176 Trace Elements in a City Waste Incineration Ash) and a snow water sample. Fair agreements are reached between the certified values and the experimental results, in addition to a satisfactory spiking recovery for the snow water sample. In the present work, the use of green and biodegradable adsorbent as well as the elimination of use of organic solvent/eluent facilitates the development of a green analytical protocol.
Co-reporter:Yong Tian, Ming-Li Chen, Xu-Wei Chen, Jian-Hua Wang, Yoshihiro Hirano, Hideyuki Sakamoto and Toshihiro Shirasaki
Journal of Analytical Atomic Spectrometry 2011 - vol. 26(Issue 1) pp:NaN140-140
Publication Date(Web):2010/11/16
DOI:10.1039/C0JA00091D
A novel method for arsenic speciation is developed by interfacing solid phase preconcentration-liquid chromatography (LC) separation-gradient hydride generation (GHG)-quartz flame atomic absorption spectrometry (QFAAS). A MnO2 mini-column is used to preconcentrate the arsenic species of As(III), As(V), MMA and DMA, during which process, As(III) is converted to As(V)viaoxidation by MnO2, while other species remain unchanged. The recovery of As(V) (i.e., the total amount of arsenate and arsenite in the original sample), MMA and DMA from the MnO2 mini-column is facilitated by tetramethylammonium hydroxide (TMAH). After LC separation with C30 columns, arsenic species in the eluate are subject to gradient hydride generation with detection by QFAAS. On the other hand, cellulose fibre selectively adsorbs the chelating complex between As(III) and ammonium pyrrolidine dithiocarbamate (APDC). After elution with HNO3, As(III) in the original sample is quantified by graphite furnace atomic absorption spectrometry (GFAAS), and the amount of As(V) is obtained by subtraction. A sample volume of 2.0 mL derives enrichment factors of 14.0–19.2 for the arsenic species. By injecting 20 μL of eluate into the LC system (the eluate of As(III)-PDC complex is injected into the GFAAS), detection limits of 0.019, 0.33, 0.39, 0.62 μg L−1 are obtained for As(III), As(V), MMA and DMA respectively. RSDs of less than 4.2% are achieved at the level of 2 μg L−1 for As(V), MMA, DMA and 1 μg L−1 for As(III). The procedure is evaluated by speciating arsenic in snow water and Hijiki samples.
Co-reporter:Zhongchen Wu, Mingli Chen, Lin Tao, Duo Zhao and Jianhua Wang
Journal of Analytical Atomic Spectrometry 2012 - vol. 27(Issue 10) pp:NaN1714-1714
Publication Date(Web):2012/07/16
DOI:10.1039/C2JA30144J
A simple device was constructed for the on-site sequential monitoring of emitted elemental mercury (Hg0) in coal-fired stack gas. The device integrates on-line gold amalgam preconcentration, external thermal desorption and cold excitation in an enclosed atmospheric-pressure dielectric-barrier discharge (DBD) micro-plasma chamber. The emission was monitored by using a charge coupled device spectrometer. The Hg0 emission at 253.7 nm was well separated from the emission spectra of the Ar-DBD-plasma which eliminates the spectral interferences of ambient air and gaseous inorganic small molecular pollutants in the stack gas, e.g., NOx, SO2, H2S and HCl. Quantification was based on first derivative spectra. Among the three mercury species, Hg0 is efficiently and selectively trapped on the gold amalgam at <220 °C, the threshold temperature for thermal desorption of the trapped Hg0 is ca. 420 °C above which the gold amalgam releases the enriched Hg0 rapidly and gives rise to a high concentration of Hg0 in the flowing Ar stream in a very short period of time which significantly improves the detection sensitivity. A linear calibration graph was achieved within 8–256 ng (the mass of enriched Hg0 on the gold trapping micro-column) with a detection limit of 2.3 ng and an RSD of 4.0% at 32 ng. A spiking recovery of 96.1% was achieved at a spiking mass level of 50 ng Hg0. For real sample analysis (stack gas from a honeycomb briquette stove), a calibration range of 2.7–60.8 ppt was achieved after 5 min preconcentration with a 0.5 L min−1 sampling flow rate.
Co-reporter:Xiaoxing Zhang, Lipei Zhang, Ting Yang, Liming Shen, Mingli Chen and Jianhua Wang
Journal of Analytical Atomic Spectrometry 2012 - vol. 27(Issue 10) pp:NaN1687-1687
Publication Date(Web):2012/06/19
DOI:10.1039/C2JA30099K
Multi-walled carbon nanotubes (MWNTs) were functionalized by incubating in Fe3+ solution for the purpose of improving its selectivity and sorption capacity to cadmium. High resolution transmission electron microscopy, Raman spectroscopy, X-ray diffraction and surface charge analysis demonstrated that the MWNTs were decorated by a layer of iron phosphate. In a neutral medium (pH 6), the iron phosphate coated carbon nanotubes (NT-FP) offer a much improved sorption capacity of 32.68 mg g−1 for cadmium over 6.72 mg g−1 by bare carbon nanotubes after oxidation. The bare carbon nanotubes generally exhibit non-specific adsorption for various species, while the NT-FP composites provide very high selectivity to cadmium against complex sample matrix components, i.e., the tolerant limit for coexisting species were 5–100 fold improved. The NT-FP composites were packed into a mini-column for on-line selective preconcentration of cadmium with detection by electrothermal atomic absorption spectrometry. A 100% sorption was achieved at pH 6, and 50 μL of aqueous mixture of 0.002 mol L−1 H3PO4 and 0.1 mol L−1 NH4NO3 gives rise to a recovery of 77%. With a sample volume of 1000 μL, an enhancement factor of 31.2 is obtained, along with a detection limit of 1.3 ng L−1 (3σ, n = 11) and a RSD of 2.2% (0.1 μg L−1, n = 11) within a linear calibration range of 0.003–0.2 μg L−1. The procedure is validated by determining cadmium in two certified reference materials (GBW08608 and GBW07404) and environmental water samples.
Co-reporter:Ming-Li Chen, Yong Tian and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2008 - vol. 23(Issue 6) pp:NaN880-880
Publication Date(Web):2008/04/25
DOI:10.1039/B802595A
A cellulose fibre packed micro-column was used for sorption preconcentration of ultra-trace cadmium and successive coating of a thin layer of sodium tetrahydroborate solution. The retained cadmium was stripped with hydrochloric acid and in-situ vapor generation on the cellulose surface was initiated by reaction with the coated layer of reducing reagent. The vapor was detected by atomic fluorescence spectrometry (AFS). The integration of preconcentration, reducing reagent immobilization, elution and in-situ vapor generation onto the cellulose surface significantly simplifies the entire operation, where a single syringe pump suffices fluids delivery, providing sufficient stability and long-term reliability indicated by an intra-day RSD <5%. In addition, the detection limit and precision were significantly improved with respect to those obtained by a conventional elution approach. With a sampling volume of 1.0 mL, a quantitative retention of cadmium was obtained within a linear range of 0.01–1.0 μg L−1, along with an enrichment factor of 19.5 and a sampling frequency of 12 h−1. A precision of 1.9% at 0.2 μg L−1 was obtained and a detection limit of 3 ng L−1 was derived. The procedure was validated by analyzing certified reference materials of Riverine Water (SLRS-4), and Trace Elements in Water (GBW 08608), in addition to spiking recovery in a coastal sea water.
Co-reporter:Ming-Li Chen, Ya-Nan Zhao, Da-Wei Zhang, Yong Tian and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2010 - vol. 25(Issue 11) pp:NaN1694-1694
Publication Date(Web):2010/08/19
DOI:10.1039/C0JA00026D
The immobilization of N-methylimidazolium (Nmim) onto PVC surface forms bonded hydrophilic ionic liquid 1-chlorovinyl-3-methylimidazolium chloride (PVC-NmimCl), which entails anion exchange nature and positively charged surface, facilitating favorable retention of Cr(VI) with a retention capacity of 23.2 mg g−1 for Cr(VI) at pH 5.6. A novel on-line solid phase extraction approach for the separation and preconcentration of Cr(VI) is developed in a sequential injection system with a PVC-NmimCl mini-column, and an extra mini-column of strong acidic styrene type cation exchange resin is incorporated for pre-eliminating Cr(III) in sample solution before entering the PVC-NmimCl mini-column. The retained Cr(VI) is effectively recovered with elution by 0.2 mol l−1 NH4NO3 solution, and the eluate is quantified by electrothermal atomic absorption spectrometry (ETAAS) and inductively coupled plasma mass spectrometry (ICP-MS). With a sample volume of 2000 μl, a complete retention of Cr(VI) is obtained, giving rise to an enrichment factor of 23.4 and a sampling frequency of 9 h−1. A linear range of 0.01–1.0 μg l−1 for Cr(VI), along with a detection limit of 3 ng l−1 and a RSD of 2.9% at 0.5 μg l−1 is obtained. Total chromium in a certified reference material of reverine water (GBW08608) is determined after oxidation, which results in good agreement between the certified and the found values. The procedure is further demonstrated for chromium speciation in tap water and snow water samples.
Co-reporter:Yong Tian, Ming-Li Chen, Xu-Wei Chen, Jian-Hua Wang, Yoshihiro Hirano, Hideyuki Sakamoto and Ikumei Setsu
Journal of Analytical Atomic Spectrometry 2010 - vol. 25(Issue 1) pp:NaN54-54
Publication Date(Web):2009/10/14
DOI:10.1039/B913198A
Arsenic speciation was performed based on liquid chromatographic separation followed by gradient hydride generation (GHG) and quartz atomizer atomic absorption spectrometric detection. The arsenic species, i.e., arsenate (As(V)), arsenite (As(III)), monomethylarsonic acid (MMA), dimethylarsinic acid (DMA) and trimethylarsine oxide (TMAO), were separated on C30-5 columns, and the concept of gradient hydride generation facilitates high conversion efficiency of the arsenic species into corresponding hydrides. The use of 2% L-cysteine in the GHG process gives rise to further improvements on the hydride generation efficiency of 13% to 32% for the arsenic species. The hydrides were separated in a unique design of gas–liquid separator, which not only ensures a complete separation but minimizes the dispersion of hydrides when delivering into the atomizer, resulting in a maximum of 13-fold improvement on the sensitivity of As(V) compared to previous studies. A separation process was finished within 800 s by injecting 100 µL sample solution, achieving detection limits of 0.9, 1.4, 1.4, 1.6, 1.5 µg/L, respectively, for As(V), As(III), MMA, DMA and TMAO. Precisions of less than 3% and 6% RSD were obtained for the five arsenic species at 100 µg/L and 20 µg/L, respectively. Three arsenic species, i.e., As(V), DMA and TMAO, were identified in Hijiki samples by this procedure.
Co-reporter:Ming-Li Chen, Hui-Juan Ma, Si-Qi Zhang and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2011 - vol. 26(Issue 3) pp:NaN617-617
Publication Date(Web):2011/02/14
DOI:10.1039/C0JA00185F
The functionalization of cellulose fibre by grafting L-cysteine on the surface (Cys-fibre) significantly improves the sorption capacity toward mercury and methyl-mercury. The Cys-fibre is used to pack a mini-column for on-line separation and preconcentration of mercury species in a sequential injection system. The retained mercury and methyl-mercury could readily be recovered by a mixture of L-cysteine and nitric acid. The inorganic mercury is selectively quantified using the cold atomization mode with vapor generation atomic fluorescence spectrometry. The total amount of mercury is determined by adopting the flame/heat atomization mode, and thus the concentration of methyl-mercury is achieved by the difference. When 1000 μL of sample solution is processed followed by elution with 100 μL of eluent, detection limits of 1 ng L−1 (3σ, n = 9) for inorganic mercury and 3 ng L−1 (3σ, n = 9) for methyl-mercury are obtained within linear ranges of 0.01–0.7 μg L−1Hg2+ and 0.03–2.0 μg L−1MeHg, respectively. The precisions for Hg2+ and MeHg of 1.5% RSD (n = 11) and 2.6% RSD (n = 9) are recorded at 0.1 μg L−1 and 1.0 μg L−1, respectively. The procedure has been validated by analyzing mercury in certified reference material of BCR176 and a cosmetic sample. Speciation of mercury and methyl-mercury in a series of water samples and the extracts of cosmetic and seaweed samples are performed, and favorable spiking recoveries have been demonstrated.
Co-reporter:Xiao-Xing Zhang, Shi-Song Tang, Ming-Li Chen and Jian-Hua Wang
Journal of Analytical Atomic Spectrometry 2012 - vol. 27(Issue 3) pp:NaN472-472
Publication Date(Web):2012/01/25
DOI:10.1039/C2JA10292G
Iron phosphate (FePO4) is for the first time used as a novel sorbent for chromium(III) adsorption. The prepared FePO4 was characterized by means of FT-IR, SEM and surface charge analysis, and used for selective adsorption of chromium(III). At pH 5.9, ca.100% of Cr(III) (<5 μg L−1) was retained on the surface of the adsorbent, while at the same conditions the adsorption of Cr(VI) was negligible (<2%). Cr(III) was adsorbed with an ca. 62/1 selectivity over Cr(VI). The adsorption of Cr(III) fits Langmuir model, corresponding to a maximum adsorption capacity of 8.12 mg g−1. The retained Cr(III) could be readily recovered by 200 μL of aqueous mixture of 0.1% H2O2 + 0.05 mol L−1 NH3 as stripping reagent, giving rise to a recovery of 96.5%. The chromium in the eluate is quantified with detection by electrothermal atomic absorption spectrometry. A sample volume of 2000 μL creates an enrichment factor of 8.7, along with a detection limit of 0.02 μg L−1 (3σ, n = 9) and a RSD of 2.5% (0.5 μg L−1) within a linear calibration range of 0.05–2.5 μg L−1. Total chromium was determined after reduction of Cr(VI) to Cr(III) by hydroxylamine hydrochloride as a reducing reagent. The content of Cr(VI) was achieved by difference. The method was validated by analyzing chromium content in a certified reference material (GBW08608, Trace Elements in Water) and speciation of Cr(III) and Cr(VI) in sea water, tap water, spring water and ground water samples was conducted.
Co-reporter:Deng-Ji Zhang;Yi Cai;Ming-Li Chen;Yong-Liang Yu
Journal of Analytical Atomic Spectrometry 2016 - vol. 31(Issue 2) pp:NaN405-405
Publication Date(Web):2016/02/03
DOI:10.1039/C5JA00266D
Dielectric barrier discharge (DBD) micro-plasma as a radiation source has been investigated for the excitation of chlorine, bromine and iodine and their simultaneous determination by vapor generation-DBD optical emission spectrometry (OES). Chloride and bromide in 6 mol L−1 H2SO4 were on-line vaporized by reaction with 0.1 mol L−1 KMnO4, while bromide and iodide in 0.5 mol L−1 H2SO4 were on-line vaporized by reaction with 0.02 mol L−1 KMnO4. The vapor species of halogens were subsequently transferred into a tubular DBD excitation chamber by a helium stream for performing multi-element optical emission and detection with a small charge-coupled device (CCD) spectrometer. Special attention has been paid to the simultaneous vapor generation introduction of halogens and subsequent multi-element DBD optical emission. With the characteristic emission lines of Cl 837 nm, Br 827 nm and I 905 nm as the analytical lines for quantification, the detection limits for the simultaneous determination of Cl and Br were 15 and 11 μg L−1, respectively, while those for Br and I were 10 and 95 μg L−1, respectively. The accuracy of the present DBD-OES system was confirmed by the determination of halide contents in a few certified reference materials and real samples.
Co-reporter:
Analytical Methods (2009-Present) 2012 - vol. 4(Issue 6) pp:
Publication Date(Web):
DOI:10.1039/C2AY25159K
An approach for the immobilization of a chromogenic reagent on solid phase micro-beads is performed via a sulfonation reaction. The product as an optical sensor is applied in lab-on-valve bead injection spectroscopy. The benzene ring structure exists in various chromogenic reagents, which facilitates the introduction of a sulfonic acid group via sulfonation. Chromogenic reagents ranging from neutral to anionic can be immobilized on anion exchanger micro-beads. As a model of application, micro-beads of Sephadex QAE A-25 loaded with the chromogenic reagent 1-(2-pyridylazo)-2-naphthol-sulfonic acid (PAN-S) are employed for the determination of trace cobalt by lab-on-valve bead injection spectroscopy. The characteristics of the micro-beads and some important parameters governing the performance of the method are investigated. With a sample volume of 1.0 mL, a detection limit of 8 μg L−1 and a linear range of 20–500 μg L−1 are obtained for cobalt, along with a RSD value of 2.8% (at the 200 μg L−1 level). The accuracy and practical applicability of the present method are validated by analysing a certified reference material of soil GBW07404, vitamin B12 injection and mecobalamin tablets, and further demonstrated by spiking recovery of cobalt in two water samples.
Co-reporter:Yu-Ting Zhuang, Ting-Ting Zhu, Man Ruan, Yong-Liang Yu and Jian-Hua Wang
Journal of Materials Chemistry A 2017 - vol. 5(Issue 7) pp:NaN3455-3455
Publication Date(Web):2017/01/19
DOI:10.1039/C6TA09774J
A facile and green approach for the preparation of a multifunctional ternary Fe2O3/graphitic-C3N4/graphene (FeCNG) nanocomposite with a porous structure is reported. This entails the growth of Prussian blue (PB) and adsorption of urea on graphene oxide (GO), followed by thermal pyrolysis of PB and urea leading to in situ formation of a porous N-doped graphene/iron oxide architecture. This strategy for the generation of FeCNG requires no structure-directing surfactants and gives rise to an N-doped composite capable of separation for recycling. The FeCNG architecture is capable of both rapid reduction of p-nitrophenol (4-NP) and efficient scavenging of Cr(VI) in aqueous media. The reduction of 4-NP to p-aminophenol by NaBH4 could be achieved within 3 min at 25 °C, using catalyst loadings as low as 1 mg. Cr(VI) adsorption was evaluated by Langmuir and pseudo-second-order models, offering a maximum equilibrium adsorption capacity of 149 mg g−1. In particular, Cr(VI) could be effectively adsorbed by the FeCNG nanocomposite and thereby reduced to less toxic Cr(III). By virtue of the enhanced catalytic performance and highly efficient adsorption of Cr(VI) across a wide pH range, the FeCNG nanocomposite possesses a broad application potential in energy and environmental sciences.
Co-reporter:Lu Han, Yang Zhang, Xu-Wei Chen, Yang Shu and Jian-Hua Wang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 1) pp:NaN112-112
Publication Date(Web):2015/11/17
DOI:10.1039/C5TB02002F
A novel phototherapy nanoplatform is prepared by coating hollow CuS nanoparticles with a bovine serum albumin–folic acid (BSA–FA) complex. The obtained CuS–BSA–FA nanoparticles are used as drug-delivery vehicles to transport a near-infrared-absorbing phototherapeutic agent (indocyanine green, ICG) into HeLa cells, after loading ICG onto CuS–BSA–FA. In this manner, a combined therapy approach is established consisting of photothermal therapy (by CuS–BSA–FA nanocarriers) and cytotoxic effects of photodynamic and photothermal therapy (by ICG upon 808 nm laser irradiation). The encapsulation of ICG onto CuS–BSA–FA significantly improves the stability and reduces the dark toxicity of free ICG. This therapeutic system exhibits an obviously higher photothermal heating effect and capability of 1O2 generation under laser irradiation compared with bare nanocarriers. In addition, the grafted FA segments on the surface of CuS–BSA–FA are proved to enhance the internalization of nanoparticles by FA-receptor-mediated endocytosis.
Co-reporter:Xuwei Chen, Wenjing Wang, Zhining Song and Jianhua Wang
Analytical Methods (2009-Present) 2011 - vol. 3(Issue 8) pp:NaN1773-1773
Publication Date(Web):2011/06/15
DOI:10.1039/C1AY05130J
A cross-linked chitosan/multi-wall carbon nanotube (MWCNTs) nanocomposite is prepared via surface deposition-cross linking. The nanocomposite is characterized by means of FT-IR, SEM and TGA analysis, indicating that a chitosan layer is well coated on the surfaces of the MWCNTs, weighing about 35% of the total mass. Investigations on the performance of the chitosan/MWCNTs nanocomposite to the adsorption or loading of hemoglobin indicated that the adsorption equilibrium time is reduced from a few hours in the conventional protocols to 25 min in the present case. A theoretical adsorption capacity of 15.41 μg mg−1 is achieved, corresponding to a 6-fold improvement when compared to that obtained by using conventional chitosan particles in the micrometre range at a same mass condition. The nanocomposite is used as an adsorbent for the isolation of hemoglobin from human whole blood, the SDS-PAGE results indicated that successful separation of hemoglobin is obtained in the presence of large amount of abundant protein, e.g., human serum albumin.
Co-reporter:Xiaoxing Zhang, Mingli Chen, Yongliang Yu, Ting Yang and Jianhua Wang
Analytical Methods (2009-Present) 2011 - vol. 3(Issue 2) pp:NaN462-462
Publication Date(Web):2011/01/06
DOI:10.1039/C0AY00621A
Multi-walled carbon nanotubes (MWNTs) are noncovalently wrapped by a cationic polyelectrolyte of poly(diallyldimethylammonium chloride) (PDDA) via π–π interactions between the unsaturated impurity in PDDA and MWNTs. The modified PDDA-MWNTs are characterized by FT-IR and surface charge analysis. The PDDA-MWNTs are packed into a mini-column and used for the adsorption of Cr(VI) in a sequential injection system with detection by electrothermal atomic absorption spectrometry (ETAAS). A 32% improvement on the adsorption efficiency of Cr(VI) by the PDDA-MWNTs at pH 6 is achieved with respect to that obtained by the bare MWNTs. The retained Cr(VI) is afterwards recovered by using 80 μL of ammonium nitrate solution (0.1 mol L−1) as stripping reagent producing an elution efficiency of 81%. The presence of a certain amount of Cr(III) within a Cr(III)/Cr(VI) concentration ratio of 6:1 causes no interfering effect for the adsorption of Cr(VI) by the PDDA-MWNTs mini-column. A sample loading volume of 1000 μL creates an enrichment factor of 8.6, along with a detection limit of 0.016 μg L−1 (3σ, n = 7) and a RSD of 3.9% (0.5 μg L−1) within a linear calibration range of 0.05–1.5 μg L−1. The procedure has been validated by analyzing a certified reference material of GBW08608 and a series of water samples.
Co-reporter:
Analytical Methods (2009-Present) 2015 - vol. 7(Issue 22) pp:NaN9534-9534
Publication Date(Web):2015/10/05
DOI:10.1039/C5AY02308D
A novel cross-linked co-polymeric ionic liquid is prepared via mini-emulsion polymerization by using N-vinyl-3-(2-methoxy-2-oxyl ethyl) imidazolium chloride as a monomer and 1,4-butanediyl-3,3′-bis-l-vinylimidazoliurn dibromide as a crosslinker. The as-synthesized material is used as an adsorbent for the solid-phase extraction of curcuminoids. Ion-exchange and hydrogen-bonding interactions contribute to a highly efficient adsorption of curcuminoids onto the cross-linked co-polymeric ionic liquid, and a maximum adsorption capacity of 108.7 μg mg−1 is achieved. Both the adsorption and desorption of curcuminoids could be achieved within 15 s, giving rise to a fast extraction process. This developed extraction protocol is applied to the isolation of curcuminoids from Curcuma longa Linn, and HPLC analysis demonstrates obvious improvement in extraction efficiency as compared with conventional extraction methodologies.