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BIOSENSORS & BIOELECTRONICS · 2021 · IF 10.618

Bipolar electrode ratiometric electrochemiluminescence biosensing analysis based on boron nitride quantum dots and biological release system

Xue-yun Yang,Yin-zhu Wang,Ling-ling Wang,Jia wan Zhu,Jie Zhao,Hui-long Zong,Chuan-xiang Chen

In this article, we developed a novel ECL ratiometry on a closed bipolar electrode (BPE) for the sensitively and accurately detection of miRNA-21. High quantum yield and low toxicity BNQDs was synthesized and coated at BPE cathode as an ECL emitter, while the anode of BPE was calibrated via another ECL material, Ir(df-ppy) 2 (pic) (Firpic). The electron neutrality at both ends of the BPE electrically coupled the reactions on each pole of the BPE. Therefore, one electrochemical sensing reaction could be quantified at one end of the BPE. By the hybridization of target miRNA-21 and hairpin, the glucose blocked in MSNs by the hairpin was released and reacted with glucose oxidase (GOD) to generate H 2 O 2 , thereby reducing the ECL signal of the cathode BNQDs/K 2 S 2 O 8 system and promoting ECL signal of anode Firpic/TPrA. Further, the G-quadruplex formed by unreacted hairpin bases consumed H 2 O 2 , which not only recovered the ECL of BNQDs, but also further improved the ECL emission of Firpic. Therefore, the concentration of miRNA-21 could be measured by the ECL ratio of BNQDs and Firpic. The data showed that the detection limit was 10 −15  M (S/N = 3) with the linear range of 10 −15  M to 10 −9  M. The strategy of the BPE-ECL ratio method based on BNQDs showed a good prospect in clinical application.

CAS / MDL: 16009-13-5
研究领域: 分析化学 · 生物化学 · 纳米技术 · 分子生物学 · 临床诊断
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BIOSENSORS & BIOELECTRONICS · 2016 · IF 7.476

Spatial-resolved electrochemiluminescence ratiometry based on bipolar electrode for bioanalysis

Yin-Zhu Wang,Wei Zhao,Pan-Pan Dai,Hai-Jie Lu,Jing-Juan Xu,Jing Pan,Hong-Yuan Chen

Herein, a spatial-resolved electrochemiluminescene (ECL) ratiometry based on a closed biopolar electrode (BPE) is reported for the highly sensitive detection of prostate specific antigen (PSA). [email protected] 3 N 4 NCs as one ECL emitter were firstly coated on the cathode of BPE, while the anode of the BPE served for calibration via another ECL substance, Ru(bpy) 3 2+ . The electroneutrality across the BPE makes the reactions on each pole of BPE electrically coupled. Thus one electrochemical sensing reaction at one pole of BPE could be quantified at both ends. A composite, Pt-PAMAM-DNAzyme was assembled on the surface of cathode via DNA hybridization between probe DNA and PSA aptamer . It acted as an ECL quencher of g-C 3 N 4 via resonance energy transfer (RET) and catalyzing the reduction of O 2 , the co-reactant of g-C 3 N 4 . Meanwhile, it could promote the ECL of Ru(bpy) 3 2+ at anode, since the catalytic reduction of O 2 at the cathode increased the faradiac current flowing through the BPE. Based on this signal composite , an ECL “off-on” phenomenon was observed at the cathode, after Pt-PAMAM-DNAzyme was “peeled off” by PSA. Conversely, at the anode, an “on-off” ECL changing was obtained. Therefore, a sensitive ratiometry for PSA detection was achieved with a linear range from 0.10 to 200   ng/mL. Since the two ECL emitters were physically separated, the ratiometric system was relatively simple and neither optical filters nor spectrometer were required. The strategy combining the ECL ratiometry and BPE broadens the applications of BPE-ECL and shows good perspective in clinical application.

研究领域: 生物分析 · 医学检测 · 电化学传感
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ChemElectroChem · 2015 ·Vol. 3 ·期 3 ·480-486 · IF 0

Vertically Ordered Silica Mesochannel Modified Bipolar Electrode for Electrochemiluminescence Imaging Analysis

Weiliang Guo,Xingyu Lin,Fei Yan,Bin Su

Graphical Enhanced and antifouling bipolar ECL analysis : An indium tin oxide bipolar electrode modified by vertical silica mesochannels (SMCs) is prepared for ECL imaging analysis. The SMCs offer not only a significant enhancement effect on the Ru(bpy) 3 2+ ECL intensity but also the molecular sieving ability against surface biofouling. The sensor can be used for sensitive ECL analysis in real media, such as human blood serum. This paper describes a miniaturized bipolar electrode (BPE) sensor that is constructed with an indium tin oxide (ITO) microband and a slice of poly(dimethylsioxane) (PDMS). The ITO microband modified by vertically ordered silica mesochannels (SMCs) functions as the BPE. Owing to the uniform pore size of ≈2–3 nm in diameter and negatively charged surface, the SMCs can significantly accelerate the mass transport of positively charged species via strong electrostatic interactions. Thus, an increase of more than two orders of magnitude in sensitivity for tri- n -propylamine (TPrA) analysis was achieved for the electrochemluminescence (ECL) of tris(2,2′-bipyridyl)ruthenium(II) (Ru(bpy) 3 2+ ) at a relatively low concentration (10 μ m ). Moreover, the SMC film with ultrasmall channels can effectively serve as an antifouling layer of the underlying ITO electrode to prevent the access of undesired large molecules, allowing the electrochemical detection in real complex media, such as atropine and l -proline in human blood serum.

研究领域: 分析化学 · 生物医学工程
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FOOD CHEMISTRY · 2024 · IF 8.5

Visual detection of ochratoxin a based on GPE-PET bipolar electrode-electrochemiluminescence platform

Fengyang Wang,Yan Qi,Lei Ji,Fanglin Qiao,Yin Chen,Xiaohui Xiong,Yuanjian Liu

A GPE-PET (graphene-polyethylene terephthalate) bipolar electrode-electrochemiluminescence (BPE-ECL) platform was developed for ochratoxin A (OTA) detection. PET served as the electrode sheet substrate, and GPE was drop-coated onto the surface of PET to form a conductive line. On the functional sensing interface, the thiol (-SH) modified OTA aptamer (OTA-Aptamer) are fixed on the surface of the gold-plated cathode through Au S bonds. The efficient electron transfer ability of methylene blue (MB) made the anode ECL signal strong. Due to competition between OTA and MB with OTA-Aptamer, leading to a decrease in ECL intensity of the [Ru(bpy) 3 ] 2+ /TPA system on the BPE anode. Under optimized conditions, the GPE-PET BPE-ECL biosensor displayed superior sensitivity for OTA with a detection limit of 2 ng mL −1 and a wide linear concentration range of 5–100 ng mL −1 . This method could be further applied to detect various toxins and had broad application prospects.

研究领域: 分析化学 · 食品安全 · 生物传感
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ANALYST · 2020 ·Vol. 145 ·期 10 ·3569-3574 · IF 3.978

A portable electrochemiluminescence bipolar electrode array for the visualized sensing of Cas9 activity

Rui Guo,Shanwen Hu,Zonghua Wang

CRISPR/Cas9 has become a powerful tool for genomic manipulation, and the evaluation of the Cas9 activity is essential for the precise control of the CRISPR system. Herein, we develop a point-of-care platform for the rapid and visible determination of the Cas9 activity. A bipolar electrochemiluminescence (ECL) biosensor platform comprises an Au electric circuit fabricated on a glass substrate and the PDMS layer acts as a reservoir. DNA probes are then modified on electrodes and hybridization chain reaction (HCR) is applied to introduce ferrocene-labeled DNA. The CRISPR/Cas9 system can recognize the immobilized DNA probes and cleave them from the electrode surface as well as the labeled H1 and H2. Therefore, the cleavage activity is closely related to the labeled ferrocene. The modified electrode is then embodied in a closed bipolar system such that the oxidation reaction on sensing poles could be detected by the anodic ECL reactions on isolated luminescent poles due to charge balance, leading to the changes in ECL signals. This portable, integrated and convenient platform may become a meaningful tool for the discovery of a new CRISPR/Cas9 system or additional Cas9 inhibitors.

研究领域: 生物技术 · 分子生物学 · 分析化学
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TALANTA · 2023 · IF 6.1

Novel electrochemiluminescence biosensor of fumonisin B1 detection using MWCNTs-PDMS flexible bipolar electrode

Huihui Yu,Haijian Yang,Weishuai Liu,Longsheng Jin,Bing Jin,Meisheng Wu

A novel portable and disposable bipolar electrode (BPE)-electrochemiluminescence (ECL) device was fabricated for fumonisin B 1 (FB 1 ) detection. BPE was fabricated by using MWCNTs and polydimethylsiloxane (PDMS) due to their excellent electrical conductivity and good mechanical stiffness. After the deposition of Au NPs on the cathode of BPE, the ECL signal could be improved 89-fold. Then a specific aptamer-based sensing strategy was constructed by grafting capture DNA on Au surface, followed by hybridizing with aptamer . Meanwhile, an excellent catalyst, Ag NPs was labeled on aptamer to activate oxygen reduction reaction , leading to a 13.8-fold enhancement in ECL signal at the anode of BPE. Under the optimal conditions, the biosensor exhibited a wide linear range of 0.10 pg/mL to 10 ng/mL for FB 1 detection. Meanwhile, it demonstrated satisfactory recoveries for real sample detection with good selectivity , making it to be a convenient and sensitive device for mycotoxin assay.

研究领域: 分析化学 · 食品安全 · 生物技术 · 毒理学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2018 · IF 3.235

High-efficient preparation and screening of electrocatalysts using a closed bipolar electrode array system

Jia-Dong Zhang,Nan Hao,Lei Lu,Shan Yun,Xiu-Fang Zhu,Kun Hong,Liang-Dong Feng

High-efficient preparation and screening of electrocatalysts for oxygen reduction reaction (ORR) was realized by a three electrode driving closed bipolar electrode (BPE) array system. As high concentrations of Fe(CN) 6 3−/4− (both 200 mM) existed in the anodic cell of the BPE system and same electrode material was adopted by the BPE anodic pole and driving electrode in anodic cell, the anodic cell performed similar to “good conductor” and the electrochemical behavior of the closed BPE system approximately equal to that of the three-electrode system in cathodic cell. Based on the above property and the parallel array, electrocatalysts containing bimetallic Pt Au and reduced graphene oxide (PtAu-rGO) with varying metal proportion were successfully prepared on the cathodic BPE poles by a two-step reduction process. Graphene oxide was firstly reduced to reduced graphene oxide (rGO) in each cathodic pole by cyclic voltammetry , and then Pt Au with different metal proportion were electrodeposited on the surface of rGO. Afterward, in-situ and high-throughput screening of these electrocatalysts for ORR was carried out based on the electrochemiluminescence (ECL) imaging on the corresponding anodic BPE poles. The screening results were consistent with those of the conventional electrochemical method by testing the catalytic performance one by one very well. This closed BPE array system with one potentiostat not only can prepare multiple catalyst candidates at the same time, but also can evaluate them, simultaneously, which is of great immediate significance to the field of fuel cell.

研究领域: 材料科学 · 电化学
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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Visual Electrofluorochromic Detection of Cancer Cell Surface Glycoprotein on a Closed Bipolar Electrode Chip

Zhaoyan Tian,Li Mi,Yafeng Wu,Fengying Shao,Mingqiang Zou,Zhenxian Zhou,Songqin Liu

This work reports an electrofluorochromic strategy on the basis of electric field control of fluorescent signal generation on bipolar electrodes (BPEs) for visualizing cancer cell surface glycoprotein (mucin 1). The device included two separate cells: anodic sensing cell and cathodic reporting cell, which were connected by a screen-printing electrode patterned on poly(ethylene terephthalate) (PET) membrane. In the sensing cell, anti-MUC1 antibody immobilized on a chitosan-multiwalled carbon nanotube (CS-MWCNT)-modified anodic BPE channel was used for capturing mucin-1 (MUC1) or MCF-7 cancer cells. Then ferrocene (Fc)-labeled mucin 1 aptamers were introduced through hybridization. Under an applied voltage, the ferrocene was oxidized and the electroactive molecules of 1,4-benzoquinone (BQ) in the cathodic reporting cell were reduced according to electroneutrality. This produced a strongly basic 1,4-benzoquinone anion radical (BQ•–), which turned on the fluorescence of pH-responsive fluorescent molecules of (2-(2-(4-hydroxystyryl)-6-methyl-4H-pyran-4-ylidene)malononitrile) (SPM) coexisting in the cathode reporting cell for both spectrophotometric detection and imaging. This strategy allowed sensitive detection of MUC1 at a concentration down to 10 fM and was capable of detecting a minimum of three MCF-7 cells. Furthermore, the amount of MUC1 on MCF-7 cells was calculated to be 6.02 × 104 molecules/cell. Our strategy also had the advantages of high temporal and spatial resolution, short response time, and high luminous contrast and is of great significance for human health and the promotion of life science development.

研究领域: 生物化学 · 生物医学工程 · 分析化学 · 癌症研究
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ANALYTICAL CHEMISTRY · 2016 · IF 5.886

Visual Color-Switch Electrochemiluminescence Biosensing of Cancer Cell Based on Multichannel Bipolar Electrode Chip

Huai-Rong Zhang,Yin-Zhu Wang,Wei Zhao,Jing-Juan Xu,Hong-Yuan Chen

In this work, we developed a visual electrochemiluminescence (ECL) sensing platform based on a dual-bipolar electrode (D-BPE) array chip. The chip was composed of two arrays of BPEs and three separated arrays of reservoirs filled with buffer, Ru(bpy)32+-TPrA and luminol solutions, respectively. Both BPEs served as ECL reporting platforms. By applying 6.0 V voltage, an array of orange electrochemiluminescence (ECL) signals belonging to Ru(bpy)32+ turned on. After adding DNAzyme and H2O2 in Ru(bpy)32+ and luminol reservoirs, the orange Ru(bpy)32+ signals decreased until vanished due to the quenching effect; meanwhile, a new array of blue ECL signals turned on because of the luminol-H2O2 ECL reaction. The designed D-BPE owns superior properties compared with the three-electrode system benefiting from the quantitative relation of bipolar systems, which greatly enhanced the ECL detection sensitivity. Meanwhile, the visual color-switch ECL and the ratiometric detecting principle made the results easier to evaluate and more accurate. Quantitative detection of HL-60 cancer cells from 320 cells/mL to 2.5 × 105 cells/mL with two linear ranges was achieved. The detection limit was down to 80 cells/mL. Finally, this D-BPE chip could distinguish the tumor cells from normal cells and provide a prospect for cancer diagnosis in a high-throughput, visual way.

CAS / MDL: 16009-13-5
研究领域: 生物传感 · 医学诊断 · 分析化学
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 11 ·1-12 · IF 5.3

Detection of pathogenic gram-negative bacteria using an antimicrobial peptides-modified bipolar electrode-electrochemiluminescence platform

Ji Lei,Wang Fengyang,Qi Yan,Qiao Fanglin,Xiong Xiaohui,Liu Yuanjian

Real-time, label-free detection of gram-negative bacteria with high selectivity and sensitivity is demonstrated using a bipolar electrode-electrochemiluminescence (BPE-ECL) platform. This platform utilizes anode luminescence and cathode modification of antimicrobial peptides (AMPs) to effectively capture bacteria. Magainin I, basic AMP from Xenopus skin, boasting an α -helix structure, exhibits a preferential affinity for the surface of gram-negative pathogens. The covalent attachment of the peptide’s C-terminal carboxylic acid to the free amines of a previously thiolated linker ensures its secure immobilization onto the surface of the interdigitated gold-plated cathode of BPE. The AMP-modified BPE sensor, when exposed to varying concentrations of gram-negative bacteria, produces reproducible ECL intensities, allowing for the detection of peptide-bacteria interactions within the range 1 to 10 4  CFU mL −1 . Furthermore, this AMP-modified BPE sensor demonstrates a selective capacity to detect Escherichia coli O157:H7 amidst other gram-negative strains, even at a concentration of 1-CFU mL −1 . This study underscores the high selectivity of Magainin I in bacterial detection, and the AMP-modified BPE-ECL system holds significant promise for rapid detection of gram-negative bacteria in various applications. The AMP-modified BPE sensor generated reproducible ECL intensity that detected peptide-bacteria interactions in the range 1 to 10 4  CFU mL −1 . The AMP-modified BPE sensor also selectively detected E. coli O157:H7 from other gram-negative strains at a concentration of 1-CFU mL −1 . In this paper, AMP demonstrated high selectivity in bacterial detection. The AMP-modified BPE-ECL system prepared has a great potential for application in the field of rapid detection of gram-negative bacteria. Graphical Abstract

CAS / MDL: 156-57-0 25952-53-8
研究领域: 生物技术 · 微生物学 · 分析化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2020 · IF 3.807

Alternate reporting surfaces in closed bipolar electrode system: A strategy forelectrochemiluminescence sensing of both redox processes

Jiadong Zhang,Weijian Yu,Xingyu Jiang,Ye Gao,Guiming Peng

Bipolar electrode (BPE) combining with electrochemiluminescence (ECL) has been a very efficient tool for chemical and biological sensing, catalysts screening, etc. In general, however,These commonly used BPE-ECL sensing strategies could only monitor alternative oxidation or reduction behaviors of targets. To address this issue, a closed BPE system with alternate ECL reporting surfaces between BPE pole and driving electrode was constructed for monitoring both of the redox processes of targets. The feasibility and universality of this strategy were elaborated by studying the electrochemical (EC) and ECL behaviors of this closed BPE system. Then, based on the alternate ECL reporting surfaces, both of the redox processes were successfully detected by this closed BPE-ECL sensor, which had a good linear relationship between the concentrations and the corresponding ECL signals. Furthermore, take advantage of the visual ECL imaging, high-throughput determination of the redox of targets was successfully carried out by an array of the closed BPE system with alternate reporting surfaces.

研究领域: 分析化学 · 生物传感 · 电化学
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TALANTA · 2019 · IF 4.916

Combination of area controllable sensing surface and bipolar electrode-electrochemiluminescence approach for the detection of tetracycline

Longsheng Jin,Jingtang Qiao,Jinghan Chen,Ning Xu,Meisheng Wu

A novel area controllable biosensing interface is designed on glassy carbon bead (GCB) and used for measurement of tetracycline (TET) in closed bipolar electrode-electrochemiluminescence (ECL) device. One face of GCB is modified with Au particles and the covered area is varied from 0 to 45.3% by tuning the external voltage during bipolar electrodeposition process in a home-made open bipolar electrochemical cell . It enables the conjugation of various amounts of biomolecules on Au/GCB. Then DNA walker and methylene blue (MB) labeled DNA (MB-DNA) are conjugated on Au surface for the following combination of aptamer . In the presence of target, aptamer partially hybridized with DNA walker will be released from Au surface, leading to the formation of dsDNA between DNA walker and MB-DNA. As a result, MB-DNA with recognition site for nicking endonuclease (Nb. Bbv CI) in dsDNA is cleft into two segments by Nb. Bbv CI. Meanwhile, the liberated DNA walker is triggered to continue the degradation of many MB-DNA. Due to the excellent electrochemical performance of MB, it is reduced at the cathode of BPE to amplify the ECL signal at the anode of BPE in a closed BPE-ECL platform. When the covered area of GCB by Au particles is enlarged from 10.1 to 45.3%, the change of ECL intensity could be increased 2.7-fold. The linear range for the detection of tetracycline is from 1 × 10 −12 to 1 × 10 −5  M with the detection limit of 6.0 × 10 −13  M. Hence, controllable sensing area on a single glassy carbon bead, the amplification effect of DNA walker and MB make this approach possess many advantages over traditional biosensor.

CAS / MDL: 60-54-8
研究领域: 分析化学 · 生物传感技术
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