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ACS Applied Materials & Interfaces · 2015 · IF 6.723

Label-Free Electrochemiluminescent Immunosensor for Detection of Carcinoembryonic Antigen Based on Nanocomposites of GO/MWCNTs-COOH/Au@CeO2

Xuehui Pang,Jianxiu Li,Yongbei Zhao,Dan Wu,Yong Zhang,Bin Du,Hongmin Ma,Qin Wei

A high-sensitivity electrochemiluminescence (ECL) sensor was conducted to detect carcinoembryonic antigen (CEA). Nanocomposites of graphene oxide/carboxylated multiwall carbon nanotubes/gold/cerium oxide nanoparticles (GO/MWCNTs-COOH/Au@CeO2) were used as antibody carriers and sensing platforms to modify on glassy carbon electrodes (GCE). CeO2 nanoparticles were first exploited as an ECL luminescent material and the possible ECL mechanism was proposed in this work. GO/MWCNTs-COOH was used as a loading matrix for CeO2 nanoparticles because of the superior conductivity and large specific surface area. Au nanoparticles were further deposited on this matrix to attach anti-CEA and enhance the sensitivity of immunosensor. The proposed sensing platform showed excellent cathodic ECL performance and sensitive response to CEA. The effects of experimental conditions on the ECL performance were investigated. The proposed immunosensor showed the broad linear range (0.05–100 ng/mL) and the low detection limit (LOD, 0.02 ng/mL, signal-to-noise ratio = 3) according to the selected experimental conditions. The excellent analysis performance for determination of CEA in the human serum samples simplied this immunosensor displayed high sensitivity and excellent repeatability. More importantly, this conducted immunosensor broadens the use scope of CeO2 nanoparticles.

CAS / MDL: 10294-41-4
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ANALYST · 2017 ·Vol. 142 ·期 16 ·2936-2944 · IF 3.885

An intrinsic internal standard substrate of Au@PS-b-P4VP for rapid quantification by surface enhanced Raman scattering

Jiamin Gao,Cheng Zhao,Zhuomin Zhang,Gongke Li

Reliable quantification by surface enhanced Raman scattering (SERS) highly depends on the development of a reproducible substrate with excellent anti-interference capability. In this work, an intrinsic internal standard (IS) SERS substrate based on a diblock copolymer, polystyrene-block-poly-4-vinylpyridine (PS-b-P4VP), as a template was developed by a modified block copolymer lithography (BCL) technique of reserving the diblock copolymer template. This substrate generated a stable vibration peak at 1066 cm−1 attributed to poly(4-vinylpyridine) (P4VP) which could be used as an intrinsic IS for precise SERS quantification. A series of characterization results showed that the diblock copolymer template endowed this substrate with homogeneous distribution of Au nanoparticles, excellent stability and reproducibility. A minor relative standard deviation (RSDs) of SERS responses at 1066 cm−1 was measured and calculated to be 4.3% from ten different substrates in the same batch, which suggested good substrate-to-substrate reproducibility of this substrate. Finally, this intrinsic IS substrate was successfully applied for the rapid quantification of a trace banned dye, chrysoidine, in food samples with complicated matrices by SERS. It was proved that chrysoidine could be found and quantified to be 0.50 and 0.41 mg L−1 in a positive dried bean curd stick and chilli powder sample respectively with good recoveries by this substrate coupled with SERS. The development of intrinsic IS substrates would benefit rapid and accurate quantification of trace targets in complex samples coupled with SERS analysis.

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LANGMUIR · 2017 · IF 3.833

Synthesis of Gold Nanoparticles from Au(I) Ions That Shuttle To Solidify: Application on the Sensor Array Design

Yumin Leng,Kai Jiang,Wentai Zhang,Yuhui Wang

Metal-mediated interlocking rings won the 2016 Nobel Prize in Chemistry. The metal-directed interlocking rings in macromolecular systems (e.g., proteins) may be similar to the form of Maxwell’s electromagnetic waves; the metal ions may shuttle among the rings in the special environment. To verify this hypothesis, we designed a general approach to synthesize the multicolored gold nanoparticles (GNPs) mediated by Au(I)-directed interlocking rings in proteins. The Au(I) ions shuttled among these interlocking rings in the strong alkaline solution. Through the rapid nucleation method, the multicolored GNPs of different morphology and sizes were synthesized in the multiple honeycombed templates. On the basis of the “three-color” principle of Thomas Young, we extracted the red, green, and blue (RGB) alterations of GNPs to fabricate a visual sensor array for protein discrimination. The fingerprints (ΔRGB) were obtained from the target proteins and fed into computer programs. The proposed sensing platform was also applied to detect lysozyme in human tears with satisfactory results. Importantly, we forecasted that lysozyme could be the effective drug for curing dacryocystitis and nasolacrimal duct obstruction diseases.

CAS / MDL: 6461-04-7
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TALANTA · 2016 · IF 4.035

Electrochemiluminescence biosensor for determination of organophosphorous pesticides based on bimetallic Pt-Au/multi-walled carbon nanotubes modified electrode

Shan Shan Miao,Mei Sheng Wu,Li Ya Ma,Xiao Jing He,Hong Yang

A novel and highly sensitive electrochemiluminescence (ECL) biosensing system was designed and developed for individual detection of different organophosphorous pesticides (OPs) in food samples. Bimetallic Pt-Au nanoparticles were electrodeposited on multi-walled carbon nanotubes (MWNTs)-modified glass carbon electrode (GCE) to increase the surface area of electrode and ECL signals of luminol. Biocomposites of enzymes from acetylcholinesterase and choline oxidase (AChE and ChOx) were immobilized onto the electrode surface to produce massive hydrogen peroxides (H 2 O 2 ), thus amplifying ECL signals. Based on the dual-amplification effects of nanoparticles and H 2 O 2 produced by enzymatic reactions , the proposed biosensor exhibits highly sensitivity. The proposed biosensing approach was then used for detecting OPs by inhibition of OPs on AChE. Under optimized experimental conditions, the ECL intensity decreased accordingly with the increase in concentration of OPs, and the inhibition rates of OPs were proportional to their concentrations in the range of 0.1–50   nmol   L −1 for malathion , methyl parathion and chlorpyrifos, with detection limit of 0.16   nmol   L −1 , 0.09   nmol   L −1 and 0.08   nmol   L −1 , respectively. The linearity range of the biosensor for pesticide dufulin varied from 50 to 500   nmol   L −1 , with the detection limit of 29.7   nmol   L −1 . The resulting biosensor was further validated by assessment of OPs residues in cabbage, which showed a fine applicability for the detection of OPs in the realistic sample.

CAS / MDL: 16941-12-1 16961-25-4
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TALANTA · 2017 · IF 4.162

Colorimetric detection of thiocyanate based on inhibiting the catalytic activity of cystine-capped core-shell Au@Pt nanocatalysts

Chi-Fang Peng,Na Pan,Qian Zhi-Juan,Xin-Lin Wei,Guang Shao

In this work, core-shell Au@Pt nanocatalysts (Au@Pt NCs) with ultrathin Pt shell were synthesized and demonstrated high peroxidase-like activity. Thiocyanate ions (SCN - ) were found to effectively inhibit the peroxidase-like activity of Au@Pt NCs, and the mechanism was discussed by the characterization of TEM , DLS, EPR and XPS, etc. The inhibition of the catalytic activity of Au@Pt NCs by SCN - was mainly due to the decreased ability of the Au@Pt NCs for capturing • OH radicals and the increased ratio of Pt 2+ to Pt° on the surface of the Au@Pt NCs. A sensitive colorimetric detection of thiocyanate (SCN - ) was developed, based on the activity inhibition of Au@Pt NCs by SCN - . Interestingly, cystine modification of Au@Pt NCs was found to significantly improve the selectivity of SCN - recognition. After optimization, a colorimetric assay for SCN - was established with a detection limit of 5.0   nM and a broad linear calibration over the range of 20   nM to 40   µM. This assay has the advantages of highly sensitive, selective and low-cost. Moreover, this assay demonstrated highly potential application in the quantitative determination of SCN - in water and raw milk samples.

CAS / MDL: 540-72-7 54827-17-7
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SENSORS AND ACTUATORS B-CHEMICAL · 2017 · IF 5.401

Direct reduction of HAuCl4 for the visual detection of intracellular hydrogen peroxide based on Au-Pt/SiO2 nanospheres

Long Wu,Wenmin Yin,Xuecai Tan,Pan Wang,Fan Ding,Huan Zhang,Biru Wang,Weiyun Zhang,Heyou Han

It is attractive but remains challenging to develop nanomaterials-based methods to realize the colorimetric detection of ultratrace biological analytes. In this work, an HAuCl 4 -H 2 O 2 system was developed for the visual detection of intracellular hydrogen peroxide (H 2 O 2 ) based on the Au-Pt/SiO 2 sensing platform. Owing to their excellent intrinsic peroxidase-like activity, Au-Pt/SiO 2 nanospheres were introduced to catalyze the decomposition of H 2 O 2 and then directly reduce HAuCl 4 into gold nanoparticles (Au NPs) for the naked-eye detection. The produced Au NPs behaved color variations from light purple to wine red as H 2 O 2 concentration increased. Under the optimal conditions, this strategy showed excellent sensitivity for H 2 O 2 with a detection limit of 0.1   nM by naked-eye readout and 0.1 pM by UV–vis spectrometer (S/N   =   3), as well as acceptable selectivity for H 2 O 2 , which could meet the demand for the detection of H 2 O 2 in biological systems. The method was further validated by the determination of H 2 O 2 in HeLa cells with low cellular cytotoxicity. Thus, this strategy would provide simple and sensitive detection of H 2 O 2 in biological systems, revealing the potential application in clinical, biological and environmental researches.

CAS / MDL: 148504-34-1
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2017 · IF 3.012

Synthesis of monodispersed PEDOT/Au hollow nanospheres and its application for electrochemical determination of dopamine and uric acid

Ahmat Ali,Ruxangul Jamal,Tursun Abdiryim,Xueli Huang

Poly(3,4-ethylenedioxythiophene)/Gold (PEDOT/Au) hollow nanospheres with the ratio of EDOT and HAuCl 4 from 2:1 to 1:2 were synthesized by in-situ polymerization method. The synergism between the PEDOT and Au explored for detection of Dopamine (DA) and Uric acid (UA) in neutral phosphate buffer solutions (PBS 7.0). It was found that the monodispersed PEDOT and PEDOT/Au hollow nanospheres had been successfully prepared. Electrochemical experiments showed that the PEDOT/Au(1:1) modified electrode revealed excellent electrocatalytic activity with faster electron charge transfer kinetics. The results from differential pulse voltammetry (DPV) experiments revealed that the PEDOT/Au(1:1) electrode has excellent linear response with 0.15   μμ–330   μM and 1.5   μM–150   μM for the determination of DA and UA, respectively. The detection limits(S/N   =   3) were found to be 0.07   μM and 0.08   μM for determination of DA and UA, respectively. The PEDOT/Au(1:1) modified electrode also had good reproducibility, repeatability and excellent stability.

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Scientific Reports · 2016 ·Vol. 6 ·期 1 ·1-9 · IF 5.228

Efficient double-quenching of electrochemiluminescence from CdS:Eu QDs by hemin-graphene-Au nanorods ternary composite for ultrasensitive immunoassay

Liu Jing,Cui Meirong,Zhou Hong,Zhang Shusheng

A novel ternary composite of hemin-graphene-Au nanorods (H-RGO-Au NRs) with high electrocatalytic activity was synthesized by a simple method. And this ternary composite was firstly used in construction of electrochemiluminescence (ECL) immunosensor due to its double-quenching effect of quantum dots (QDs). Based on the high electrocatalytic activity of ternary complexes for the reduction of H 2 O 2 which acted as the coreactant of QDs-based ECL, as a result, the ECL intensity of QDs decreased. Besides, due to the ECL resonance energy transfer (ECL-RET) strategy between the large amount of Au nanorods (Au NRs) on the ternary composite surface and the CdS:Eu QDs, the ECL intensity of QDs was further quenched. Based on the double-quenching effect, a novel ultrasensitive ECL immunoassay method for detection of carcinoembryonic antigen (CEA) which is used as a model biomarker analyte was proposed. The designed immunoassay method showed a linear range from 0.01 pg mL −1 to 1.0 ng mL −1 with a detection limit of 0.01 pg mL −1 . The method showing low detection limit, good stability and acceptable fabrication reproducibility, provided a new approach for ECL immunoassay sensing and significant prospect for practical application.

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ACS Sustainable Chemistry & Engineering · 2016 · IF 5.267

Synthesis of TiO2@WO3/Au Nanocomposite Hollow Spheres with Controllable Size and High Visible-Light-Driven Photocatalytic Activity

Jiabai Cai,Xueqing Wu,Shunxing Li,Fengying Zheng

A new nanocomposite was reported as a good-performance photocatalyst, i.e., double-shelled, positively and negatively charged, nanostructured hollow spheres with supported Au nanoparticles (NPs). TiO2, WO3, and Au NPs were coated successively onto the functionalized polystyrene (PS) template spheres. The as-synthesized product PS@TiO2@WO3/Au nanocomposites were calcined at elevated temperature and then intact double-shelled TiO2@WO3/Au hollow spheres were obtained. The dispersity, morphology, size, and lattice of TiO2@WO3/Au hollow spheres were investigated by SEM and TEM. The presence of TiO2 hollow sphere and WO3/Au shell was proved by HAADF-STEM and XRD images. The photodegradation activity for rhodamine B and trimesic acid (i.e., color and colorless aromatic pollutants) in decreasing order were TiO2@WO3/Au, TiO2–WO3, P25. Under visible-light irradiation, the photodegradation rate of rhodamine B and trimesic acid for TiO2@WO3/Au was 94% and 95%, respectively, which exhibited a significant increase of 62% and 80% as compared with P25. The synergistic effect of coupling TiO2 hollow spheres with WO3 shell and Au NPs on photocatalytic performance was proved by this article. First, Au NPs deposited in WO3 shell and loaded on TiO2 shell separately act as electron trap site and surface plasmon resonance-sensitizer, respectively, and hence the photogenerated electron–hole separation rate was improved. Second, the visible-light absorption of TiO2 hollow spheres was increased by the coexistence of WO3 and Au and unique hierarchical mesoporous architectures of TiO2@WO3/Au. Finally, the surface charge of TiO2@WO3/Au and rhodamine B was negative and positive, respectively, the affinity between them could be improved by electrical attractions, and then the major bottleneck in heterogeneous photocatalysis (i.e., poor affinity between pollutants and photocatalyst) could be broken. The optimal hollow sphere size of TiO2@WO3/Au was 450 nm, which was proved by the photodegradation of aromatic pollutants and photoreduction of Cr(VI).

CAS / MDL: 140-22-7 13283-01-7
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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

Molybdenum disulfide nanosheets supported Au-Pd bimetallic nanoparticles for non-enzymatic electrochemical sensing of hydrogen peroxide and glucose

Xueyuan Li,Xuezhong Du

The molybdenum disulfide (MoS 2 ) nanosheets supported Au-Pd bimetallic nanoparticles were synthesized using a facile thermal co-reduction method. The Au-Pd/MoS 2 nanocomposites showed good electrocatalytic activities toward the reduction of hydrogen peroxide (H 2 O 2 ) in neutral solution and the oxidation of glucose in alkaline solution, attributed to the synergistic effects of the Au-Pd bimetallic nanoparticles and MoS 2 nanosheets. The fabricated non-enzymatic electrochemical sensors exhibited the linear responses of H 2 O 2 and glucose in the concentration ranges of 0.8   μM–10   mM and 0.5–20   mM with the detection limits of 0.16   μM and 0.40   mM (S/N   =   3), respectively, together with good stability and reproducibility. The Au-Pd/MoS 2 nanocomposites provide new potential materials for the development of other non-enzymatic sensors.

CAS / MDL: 103-90-2
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Semi-solid state electrochromic device based on deep eutectic solvent gel electrolyte and transparent Au modified FTO electrode

Rong Wang,Shengxia Zhang,Yun Su,Junxia Liu,Ye Ying,Feng Wang,Xiaowei Cao

A semi-solid state electrochromic device with deep eutectic solvent gel as the electrolyte, Ethyl-viologen as the electrochromic compound, and K 4 Fe(CN) 6 as the electron donor was reported. Four kinds of silica were simply mixed with ethaline for preparing the gel electrolyte, and the hydrophilic ones were found to be capable of being used as the gelling agent . To enhance the electron transfer at the electrode/gel interface and keep the transparency of the electrode, tiny amount of Au was electrochemically deposited on the FTO electrode. The as-prepared electrochromic device shows a coloration time of ca. 60 s at −0.7 V with the coloration efficiency of 91 cm 2 /C, and a bleaching time of ca. 150 s at 0 V with the efficiency of 194 cm 2 /C. The reversible response of the electrochromic device up to 820 cycles with Δ T max > 60% was also demonstrated.

CAS / MDL: 7440-57-5
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CRYSTENGCOMM · 2016 ·Vol. 19 ·期 4 ·675-683 · IF 3.849

Photo-reduction assisted synthesis of W-doped TiO2 coupled with Au nanoparticles for highly efficient photocatalytic hydrogen evolution

Bing Liu,Shuangyue Su,Wenhui Zhou,Yin Wang,Ding Wei,Lihua Yao,Yuanman Ni,Minhua Cao,Changwen Hu

The practical applications of TiO2 have been greatly suppressed by its low quantum yield, which arises from the rapid recombination of photo-induced electrons and holes, and poor solar efficiency, which is determined by its band gap. Herein, W-doped TiO2 coupled with Au nanoparticles (W-TiO2/Au) was designed and synthesized by a facile multi-step process. The W-doping in the TiO2 lattice, on the one hand, can hinder the phase transition of TiO2 from anatase to rutile structure, and the pure anatase structure is well preserved. On the other hand, W-doping can narrow the band gap of TiO2 and result in oxygen vacancies, which may act as trapping sites to retard charge recombination. Furthermore, Au loading on the surface of TiO2 can effectively suppress the recombination of photo-induced electrons and holes, leading to improvement in the quantum yields of TiO2. Benefiting from the unique dual-hybrid strategy, the W-TiO2/Au catalyst possesses a strong solar adsorption narrowed band gap, abundant active sites, strong synergetic coupling, enhanced electron transfer, and high efficiencies in H2 generation. Its maximum H2 generation rate can reach as high as 24 mmol g−1 h−1 under simulated solar light. A synergetic effect was proposed to explain the enhancement of the photocatalytic activity of TiO2.

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