{"title":"更好地结合:双通道分子印迹电化学传感器中金纳米粒子和双功能单体的协同增效作用,用于同时检测杀草隆和噻草隆","authors":"Yi He, Chunyuan Tang, Yue Ren, Bingzheng Yuan, Libo Li, Tianyan You, Xuegeng Chen","doi":"10.1021/acs.analchem.4c06793","DOIUrl":null,"url":null,"abstract":"The combination of diuron (DU) and thidiazuron (TDZ) is commonly used in cotton production for its excellent adaptability to low temperatures, which may lead to increased crop and soil pollution. The simultaneous detection of DU and TDZ poses significant challenges due to their weak and overlapping signals, along with an unclear electrochemical detection mechanism for TDZ. This study developed a dual-channel multifunctional molecularly imprinted electrochemical (MMIP-EC) sensing platform by optimizing the substrate material and MIP layer for high performance. First, amino-functionalized graphene-based poly(pyrrole)-poly(3,4-ethylenedioxythiophene) (NH<sub>2</sub>-rGO/PPy-PEDOT) with high conductivity was synthesized as the substrate. Subsequently, MMIPs were prepared in one step using electropolymerization by introducing chloroauric acid (HAuCl<sub>4</sub>) and bifunctional monomers (dopamine and thiophene). This method not only enhanced specific binding capacity of the MMIP layer but also amplified the signal through the synergistic effect of reduced AuNPs and bifunctional monomers. Furthermore, two independent modules (MMIP-DU and MMIP-TDZ) were integrated into a dual-channel EC platform for simultaneous transmission of DU and TDZ responses to separate windows. Finally, based on high-performance liquid chromatography–mass spectrometry (HPLC-MS) and electrochemical kinetics studies, it was speculated that the electrochemical oxidation of TDZ via the carbonylation of a secondary amine under strongly acidic conditions, followed by hydrolysis to form a carboxyl group, reveals the electrochemical oxidation mechanism of TDZ. The developed sensor exhibited excellent performance in selectivity and sensitivity, with low detection limits of 26.6 pg/mL (DU) and 39.2 pg/mL (TDZ). In conclusion, this sensing platform presents a novel perspective for the cost-effective and highly efficient detection of diverse environmental pollutants.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"23 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Better Together: Synergistic Enhancement of AuNPs and Bifunctional Monomers in a Dual-Channel Molecularly Imprinting Electrochemical Sensor for Simultaneous Detection of Diuron and Thidiazuron\",\"authors\":\"Yi He, Chunyuan Tang, Yue Ren, Bingzheng Yuan, Libo Li, Tianyan You, Xuegeng Chen\",\"doi\":\"10.1021/acs.analchem.4c06793\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The combination of diuron (DU) and thidiazuron (TDZ) is commonly used in cotton production for its excellent adaptability to low temperatures, which may lead to increased crop and soil pollution. The simultaneous detection of DU and TDZ poses significant challenges due to their weak and overlapping signals, along with an unclear electrochemical detection mechanism for TDZ. This study developed a dual-channel multifunctional molecularly imprinted electrochemical (MMIP-EC) sensing platform by optimizing the substrate material and MIP layer for high performance. First, amino-functionalized graphene-based poly(pyrrole)-poly(3,4-ethylenedioxythiophene) (NH<sub>2</sub>-rGO/PPy-PEDOT) with high conductivity was synthesized as the substrate. Subsequently, MMIPs were prepared in one step using electropolymerization by introducing chloroauric acid (HAuCl<sub>4</sub>) and bifunctional monomers (dopamine and thiophene). This method not only enhanced specific binding capacity of the MMIP layer but also amplified the signal through the synergistic effect of reduced AuNPs and bifunctional monomers. Furthermore, two independent modules (MMIP-DU and MMIP-TDZ) were integrated into a dual-channel EC platform for simultaneous transmission of DU and TDZ responses to separate windows. Finally, based on high-performance liquid chromatography–mass spectrometry (HPLC-MS) and electrochemical kinetics studies, it was speculated that the electrochemical oxidation of TDZ via the carbonylation of a secondary amine under strongly acidic conditions, followed by hydrolysis to form a carboxyl group, reveals the electrochemical oxidation mechanism of TDZ. The developed sensor exhibited excellent performance in selectivity and sensitivity, with low detection limits of 26.6 pg/mL (DU) and 39.2 pg/mL (TDZ). In conclusion, this sensing platform presents a novel perspective for the cost-effective and highly efficient detection of diverse environmental pollutants.\",\"PeriodicalId\":27,\"journal\":{\"name\":\"Analytical Chemistry\",\"volume\":\"23 1\",\"pages\":\"\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2025-04-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Analytical Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.analchem.4c06793\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.analchem.4c06793","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Better Together: Synergistic Enhancement of AuNPs and Bifunctional Monomers in a Dual-Channel Molecularly Imprinting Electrochemical Sensor for Simultaneous Detection of Diuron and Thidiazuron
The combination of diuron (DU) and thidiazuron (TDZ) is commonly used in cotton production for its excellent adaptability to low temperatures, which may lead to increased crop and soil pollution. The simultaneous detection of DU and TDZ poses significant challenges due to their weak and overlapping signals, along with an unclear electrochemical detection mechanism for TDZ. This study developed a dual-channel multifunctional molecularly imprinted electrochemical (MMIP-EC) sensing platform by optimizing the substrate material and MIP layer for high performance. First, amino-functionalized graphene-based poly(pyrrole)-poly(3,4-ethylenedioxythiophene) (NH2-rGO/PPy-PEDOT) with high conductivity was synthesized as the substrate. Subsequently, MMIPs were prepared in one step using electropolymerization by introducing chloroauric acid (HAuCl4) and bifunctional monomers (dopamine and thiophene). This method not only enhanced specific binding capacity of the MMIP layer but also amplified the signal through the synergistic effect of reduced AuNPs and bifunctional monomers. Furthermore, two independent modules (MMIP-DU and MMIP-TDZ) were integrated into a dual-channel EC platform for simultaneous transmission of DU and TDZ responses to separate windows. Finally, based on high-performance liquid chromatography–mass spectrometry (HPLC-MS) and electrochemical kinetics studies, it was speculated that the electrochemical oxidation of TDZ via the carbonylation of a secondary amine under strongly acidic conditions, followed by hydrolysis to form a carboxyl group, reveals the electrochemical oxidation mechanism of TDZ. The developed sensor exhibited excellent performance in selectivity and sensitivity, with low detection limits of 26.6 pg/mL (DU) and 39.2 pg/mL (TDZ). In conclusion, this sensing platform presents a novel perspective for the cost-effective and highly efficient detection of diverse environmental pollutants.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.