Signal-On Photoelectrochemical Immunoassay for Aflatoxin B1 Based on Enzymatic Product-Etching MnO2 Nanosheets for Dissociation of Carbon Dots.

Aflatoxin B1 (AFB1) monitoring has attracted extensive attention because food safety is a worldwide public health problem. Herein, we design a novel simultaneously visual and photoelectrochemical (PEC) immunosensing system for rapid sensitive detection of AFB1 in foodstuff. The immunoreaction was carried out on anti-AFB1 antibody-modified magnetic beads by using glucose oxidase (GOx)-labeled AFB1-bovine serum albumin (AFB1-BSA) conjugates as the tags with a competitive-type immunoassay format, while the visual and PEC evaluation was performed via carbon quantum dots (CQDs)-functionalized MnO2 nanosheets. Accompanying the formation of immunocomplexes, the carried GOx initially oxidized the substrate (glucose) for the generation of H2O2, which reduced/etched MnO2 nanosheets into Mn2+ ions, thereby resulting in the dissociation of CQDs from the electrode. Within the applied potentials, the photocurrent of MnO2-CQDs-modified electrode decreased with the increasing H2O2 level in the detection cell. Meanwhile, a visual detection could be performed according to the change in the color of MnO2-CQDs-coated electrode. To elaborate, this system was aggregated into a high-throughput microfluidic device to construct a semiautomatic detection cell. Under optimal conditions, the photocurrent increased with the increasing target AFB1 within a dynamic working range from 0.01 to 20 ng mL-1 with a limit of detection (LOD) of 2.1 pg mL-1 (ppt). The developed immunoassay exhibited good reproducibility and acceptable accuracy. In addition, the method accuracy relative to AFB1 ELISA kit was evaluated for analyzing naturally contaminated or spiked peanut samples, giving the well-matched results between two methods. Although our strategy was focused on the detection of target AFB1, it is easily extended to screen other small molecules or mycotoxins, thereby representing a versatile immunosensing scheme.

[1]  S. Mallakpour,et al.  Bio-functionalizing of α-MnO2 nanorods with natural l-amino acids: A favorable adsorbent for the removal of Cd(II) ions , 2017 .

[2]  E. Pereira-Filho,et al.  Recent advances on determination of milk adulterants. , 2017, Food chemistry.

[3]  Ang Li,et al.  Surviving High-Temperature Calcination: ZrO2 -Induced Hematite Nanotubes for Photoelectrochemical Water Oxidation. , 2017, Angewandte Chemie.

[4]  M. G. Sethuraman,et al.  Biological and catalytic applications of green synthesized fluorescent N-doped carbon dots using Hylocereus undatus. , 2017, Journal of photochemistry and photobiology. B, Biology.

[5]  Liqun Zhang,et al.  The synthesis of rhodium/carbon dots nanoparticles and its hydrogenation application , 2017 .

[6]  A. Lemaître,et al.  Scalable high-precision tuning of photonic resonators by resonant cavity-enhanced photoelectrochemical etching , 2015, Nature Communications.

[7]  Xu Zhao,et al.  Facile Electrospinning Synthesis of Carbonized Polyvinylpyrrolidone (PVP)/g-C3 N4 Hybrid Films for Photoelectrochemical Applications. , 2017, Chemistry.

[8]  D. Tang,et al.  Semiautomated Support Photoelectrochemical Immunosensing Platform for Portable and High-Throughput Immunoassay Based on Au Nanocrystal Decorated Specific Crystal Facets BiVO4 Photoanode. , 2016, Analytical chemistry.

[9]  C. Tung,et al.  Smart Utilization of Carbon Dots in Semiconductor Photocatalysis , 2016, Advanced materials.

[10]  Jun‐Jie Zhu,et al.  Cathode Photoelectrochemical Immunosensing Platform Integrating Photocathode with Photoanode. , 2016, Analytical chemistry.

[11]  Zhihui Dai,et al.  Dual Signal Amplification Using Gold Nanoparticles-Enhanced Zinc Selenide Nanoflakes and P19 Protein for Ultrasensitive Photoelectrochemical Biosensing of MicroRNA in Cell. , 2016, Analytical chemistry.

[12]  Hong Dai,et al.  A Potentiometric Addressable Photoelectrochemical Biosensor for Sensitive Detection of Two Biomarkers. , 2016, Analytical chemistry.

[13]  Mingkui Wang,et al.  Significant enhancement of the photoelectrochemical activity of WO3 nanoflakes by carbon quantum dots decoration , 2016 .

[14]  Jinghua Yu,et al.  An enhanced photoelectrochemical platform: graphite-like carbon nitride nanosheet-functionalized ZnO nanotubes. , 2016, Journal of materials chemistry. B.

[15]  R. Niessner,et al.  Silver Nanolabels-Assisted Ion-Exchange Reaction with CdTe Quantum Dots Mediated Exciton Trapping for Signal-On Photoelectrochemical Immunoassay of Mycotoxins. , 2016, Analytical chemistry.

[16]  Xiue Jiang,et al.  Synthesis of cell-penetrated nitrogen-doped carbon dots by hydrothermal treatment of eggplant sepals , 2016, Science China Chemistry.

[17]  W. Tan,et al.  A Smart Photosensitizer-Manganese Dioxide Nanosystem for Enhanced Photodynamic Therapy by Reducing Glutathione Levels in Cancer Cells. , 2016, Angewandte Chemie.

[18]  Jinghua Yu,et al.  Paper-Based Device for Colorimetric and Photoelectrochemical Quantification of the Flux of H2O2 Releasing from MCF-7 Cancer Cells. , 2016, Analytical chemistry.

[19]  Hiroshi Nishihara,et al.  Manganese Compounds as Water-Oxidizing Catalysts: From the Natural Water-Oxidizing Complex to Nanosized Manganese Oxide Structures. , 2016, Chemical reviews.

[20]  Chun‐Sing Lee,et al.  A carbon dot-based fluorescence turn-on sensor for hydrogen peroxide with a photo-induced electron transfer mechanism. , 2015, Chemical communications.

[21]  Wenqiang Lai,et al.  Target-induced nano-enzyme reactor mediated hole-trapping for high-throughput immunoassay based on a split-type photoelectrochemical detection strategy. , 2015, Analytical chemistry.

[22]  R. Niessner,et al.  Enzymatic hydrolysate-induced displacement reaction with multifunctional silica beads doped with horseradish peroxidase-thionine conjugate for ultrasensitive electrochemical immunoassay. , 2015, Analytical chemistry.

[23]  Wenpei Fan,et al.  Intelligent MnO2 Nanosheets Anchored with Upconversion Nanoprobes for Concurrent pH‐/H2O2‐Responsive UCL Imaging and Oxygen‐Elevated Synergetic Therapy , 2015, Advanced materials.

[24]  Ru-Qin Yu,et al.  MnO2-Nanosheet-Modified Upconversion Nanosystem for Sensitive Turn-On Fluorescence Detection of H2O2 and Glucose in Blood. , 2015, ACS applied materials & interfaces.

[25]  Dianping Tang,et al.  Plasmonic AuNP/g-C3N4 Nanohybrid-based Photoelectrochemical Sensing Platform for Ultrasensitive Monitoring of Polynucleotide Kinase Activity Accompanying DNAzyme-Catalyzed Precipitation Amplification. , 2015, ACS applied materials & interfaces.

[26]  A. Schwartzberg,et al.  Rate and mechanism of the photoreduction of birnessite (MnO2) nanosheets , 2015, Proceedings of the National Academy of Sciences.

[27]  Zhiqiang Gao,et al.  Carbon quantum dots and their applications. , 2015, Chemical Society reviews.

[28]  Jun‐Jie Zhu,et al.  Ultrasensitive photoelectrochemical immunoassay for matrix metalloproteinase-2 detection based on CdS:Mn/CdTe cosensitized TiO2 nanotubes and signal amplification of SiO2@Ab2 conjugates. , 2014, Analytical chemistry.

[29]  R. Niessner,et al.  Low-cost and highly sensitive immunosensing platform for aflatoxins using one-step competitive displacement reaction mode and portable glucometer-based detection. , 2014, Analytical chemistry.

[30]  Guohua Zhao,et al.  A femtomolar level and highly selective 17β-estradiol photoelectrochemical aptasensor applied in environmental water samples analysis. , 2014, Environmental science & technology.

[31]  Jianrong Chen,et al.  B-doped carbon quantum dots as a sensitive fluorescence probe for hydrogen peroxide and glucose detection. , 2014, The Analyst.

[32]  Meng Li,et al.  Flexible paper-based ZnO nanorod light-emitting diodes induced multiplexed photoelectrochemical immunoassay. , 2014, Chemical communications.

[33]  Shenguang Ge,et al.  Photoelectrochemical lab-on-paper device based on an integrated paper supercapacitor and internal light source. , 2013, Analytical chemistry.

[34]  R. Niessner,et al.  Anodic-stripping voltammetric immunoassay for ultrasensitive detection of low-abundance proteins using quantum dot aggregated hollow microspheres. , 2013, Chemistry.

[35]  Xingyuan Liu,et al.  A biocompatible fluorescent ink based on water-soluble luminescent carbon nanodots. , 2012, Angewandte Chemie.

[36]  Reinhard Niessner,et al.  DNA-based hybridization chain reaction for amplified bioelectronic signal and ultrasensitive detection of proteins. , 2012, Analytical chemistry.

[37]  C. Shek,et al.  Recent advances in manganese oxide nanocrystals: fabrication, characterization, and microstructure. , 2012, Chemical reviews.

[38]  Juan Tang,et al.  Nanoparticle-based sandwich electrochemical immunoassay for carbohydrate antigen 125 with signal enhancement using enzyme-coated nanometer-sized enzyme-doped silica beads. , 2010, Analytical chemistry.

[39]  Yukihiro Yoshida,et al.  Room-temperature synthesis of manganese oxide monosheets. , 2008, Journal of the American Chemical Society.

[40]  C. Grimes,et al.  Photoelectrochemical Properties of Heterojunction CdTe/TiO2 Electrodes Constructed Using Highly Ordered TiO2 Nanotube Arrays , 2008 .

[41]  G. Sposito,et al.  Defect-induced photoconductivity in layered manganese oxides: a density functional theory study. , 2007, Physical review letters.

[42]  T. Sasaki,et al.  Photocurrent generation from semiconducting manganese oxide nanosheets in response to visible light. , 2005, The journal of physical chemistry. B.

[43]  Eric R. Ziegel,et al.  Statistics and Chemometrics for Analytical Chemistry , 2004, Technometrics.

[44]  Itamar Willner,et al.  Acetylcholine esterase-labeled CdS nanoparticles on electrodes: photoelectrochemical sensing of the enzyme inhibitors. , 2003, Journal of the American Chemical Society.

[45]  D. Guyomard,et al.  Study of structural defects in γ‐MnO2 by Raman spectroscopy , 2002 .

[46]  Tao Zhang,et al.  Efficient Electrochemical and Photoelectrochemical Water Splitting by a 3D Nanostructured Carbon Supported on Flexible Exfoliated Graphene Foil , 2017, Advanced materials.