Analytical Chemistry最新文献

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Encodable DNA Hairpin Probes for Nanopore Multiplexed Target Detection 用于纳米孔多重目标检测的可编码 DNA 发夹探针
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-21 DOI: 10.1021/acs.analchem.4c03469
Feifei Sun, Jinde Liu, Zhuoqun Su, Di Wu, Shaoqi Qu, Yongning Wu, Lin Li, Guoliang Li
{"title":"Encodable DNA Hairpin Probes for Nanopore Multiplexed Target Detection","authors":"Feifei Sun, Jinde Liu, Zhuoqun Su, Di Wu, Shaoqi Qu, Yongning Wu, Lin Li, Guoliang Li","doi":"10.1021/acs.analchem.4c03469","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03469","url":null,"abstract":"Owing to the co-occurrence of hazardous compounds, it is crucial to build multiple highly discriminative probe libraries for simultaneous determination. Drawing inspiration from nucleic acid barcodes, we developed a probe system that is exclusively based on the nucleic acid secondary structure’s hairpin structure, which can be directly read by nanopores. The highly distinguishable hairpin probes were constructed, and a detailed explanation of the possible patterns in their design was provided. These probe-representative events measured through the α-hemolysin (α-HL) nanopores were both distinguished, either through visual observation or comparison of the nanopore parameters. Besides, the potential design pattern for probes with unique telegraphic switching between the two levels was also unveiled. Finally, these probes were utilized to realize simultaneous, ultrasensitive mycotoxin multiple-detection, and their prospective applications for the detection of proteins and microRNAs were presented, indicating their suitability for a wide range of sensing applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Improved Standard Addition Method for Measuring Stable Isotopic Compositions and Its Application to Sulfur Isotope Composition 测量稳定同位素组成的改进标准添加法及其在硫同位素组成中的应用
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-21 DOI: 10.1021/acs.analchem.4c02960
Guangliang Wu, Wenjing Liu, Jian-Ming Zhu, Di Liu, Jiangyi Zhang, Zhifang Xu
{"title":"Improved Standard Addition Method for Measuring Stable Isotopic Compositions and Its Application to Sulfur Isotope Composition","authors":"Guangliang Wu, Wenjing Liu, Jian-Ming Zhu, Di Liu, Jiangyi Zhang, Zhifang Xu","doi":"10.1021/acs.analchem.4c02960","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c02960","url":null,"abstract":"The standard addition method (SAM) is widely used to measure the isotopic compositions of natural samples, particularly those with a complex matrix. However, traditional SAM has limitations for isotope systems with significant variations in isotope composition due to its reliance on approximation in calculation and the requirement for <i>a priori</i> estimates of analyte isotopic compositions and accurate concentrations. To overcome the issues, our work proposes an improved SAM that explicitly calculates isotope ratio <i>R</i> (i.e., <sup>X</sup>E/<sup>Y</sup>E, <sup>34</sup>S/<sup>32</sup>S for example) instead of approximating <i>R</i>* (mass number of isotope X divided by total mass number of all isotopes of an element) with <i>R</i> in SAM. Additionally, the sample fraction within standard-sample mixture in improved SAM is determined using the isotope compositions of standards, sample–standard mixtures, and the mixtures of both standards, rather than relying on sample concentrations and volumes. Both improvements not only overcome the shortcomings of traditional SAM but also empowered the approach’s ability to accurately determine sample concentrations. To validate its effectiveness, we applied the improved SAM to natural samples with substantial sulfur (S) isotope variation (1.94 to 27.19‰) and low S concentration (0.81 to 3.47 μg g<sup>–1</sup>). The calculated δ<sup>34</sup>S values and concentrations of these samples are consistent with direct measurements within the error ranges while reducing sample sizes to 20% of those required for direct measurement. Moreover, our method achieves higher accuracy in δ<sup>34</sup>S values compared with traditional SAM. Both comparisons affirm the reliability and superiority of improved SAM.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Glycan-Evocated Metallization for Amplification-Free Electrochemical Detection of Glycoproteins at Low Concentration Levels 用于低浓度糖蛋白免放大电化学检测的糖诱导金属化技术
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-21 DOI: 10.1021/acs.analchem.4c04054
Junpeng Lv, Di Wu, Yingming Ma, Xiyao Zhang, Wenhui Xu, Mengge Wang, Songmin Chen, Qiong Hu, Dongxue Han, Li Niu
{"title":"Glycan-Evocated Metallization for Amplification-Free Electrochemical Detection of Glycoproteins at Low Concentration Levels","authors":"Junpeng Lv, Di Wu, Yingming Ma, Xiyao Zhang, Wenhui Xu, Mengge Wang, Songmin Chen, Qiong Hu, Dongxue Han, Li Niu","doi":"10.1021/acs.analchem.4c04054","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04054","url":null,"abstract":"Glycoproteins have become the most often screened tumor markers in the in vitro diagnostics. Although a large number of electrochemical methods have been proposed to sensitively detect glycoproteins, most of them involve the aid of laborious signal amplification. Herein, we report the use of glycan-evocated metallization (GlyMetal) for the amplification-free electrochemical detection of glycoproteins at low concentration levels. Briefly, the glycoproteins of interest are captured by an aptamer recognition layer, and then the glycans of targets are oxidized by NaIO<sub>4</sub> to convert the 1,2-diol sites into aldehyde groups for the silver deposition-based metallization, followed by the electrochemical stripping assay of the deposited metallic silver for glycoprotein quantification via the established solid-state Ag/AgCl voltammetric process. As GlyMetal can enable the deposition of a large amount of metallic silver and a high signal-to-background ratio can be obtained for the solid-state Ag/AgCl voltammetric stripping assay, the developed GlyMetal-based electrochemical method is applicable to the amplification-free detection of glycoproteins. As a proof of concept, a detection limit of 1.65 pg/mL has been achieved for carcinoembryonic antigen (CEA) detection. In addition to the high selectivity, desirable results have been obtained with respect to the use of the method for CEA detection in serum samples. In consideration of the desirable simplicity, short assay time, and cost-effectiveness of the amplification-free approach, the GlyMetal-based electrochemical method shows great promise in the point-of-care detection of glycoproteins.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Long-Term Stable and Multifeature Microfluidic Impedance Flow Cytometry Based on a Constricted Channel for Single-Cell Mechanical Phenotyping 基于收缩通道的长期稳定多特征微流体阻抗流式细胞仪用于单细胞机械表型分析
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-21 DOI: 10.1021/acs.analchem.4c04097
Shan-Shan Li, Chun-Dong Xue, Si-Yu Hu, Yong-Jiang Li, Xiao-Ming Chen, Yan Zhao, Kai-Rong Qin
{"title":"Long-Term Stable and Multifeature Microfluidic Impedance Flow Cytometry Based on a Constricted Channel for Single-Cell Mechanical Phenotyping","authors":"Shan-Shan Li, Chun-Dong Xue, Si-Yu Hu, Yong-Jiang Li, Xiao-Ming Chen, Yan Zhao, Kai-Rong Qin","doi":"10.1021/acs.analchem.4c04097","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04097","url":null,"abstract":"The microfluidic impedance flow cytometer (m-IFC) using constricted microchannels is an appealing choice for the high-throughput measurement of single-cell mechanical properties. However, channels smaller than the cells are susceptible to irreversible blockage, extremely affecting the stability of the system and the throughput. Meanwhile, the common practice of extracting a single quantitative index, i.e., total cell passage time, through the constricted part is inadequate to decipher the complex mechanical properties of individual cells. Herein, this study presents a long-term stable and multifeature m-IFC based on a constricted channel for single-cell mechanical phenotyping. The blockage problem is effectively overcome by adding tiny xanthan gum (XG) polymers. The cells can pass through the constricted channel at a flow rate of 500 μL/h without clogging, exhibiting high throughput (∼240 samples per second) and long-term stability (∼2 h). Moreover, six detection regions were implemented to capture the multiple features related to the whole process of a single cell passing through the long-constricted channel, e.g., creep, friction, and relaxation stages. To verify the performance of the multifeature m-IFC, cells treated with perturbations of microtubules and microfilaments within the cytoskeleton were detected, respectively. It suggests that the extracted features provide more comprehensive clues for single-cell analysis in structural and mechanical transformation. Overall, our proposed multifeature m-IFC exhibits the advantages of nonclogging and high throughput, which can be extended to other cell types for nondestructive and real-time mechanical phenotyping in cost-effective applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452413","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
COLMAR1d: A Web Server for Automated, Quantitative One-Dimensional Nuclear Magnetic Resonance-Based Metabolomics at Arbitrary Magnetic Fields COLMAR1d:任意磁场下基于一维核磁共振的自动定量代谢组学网络服务器
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-20 DOI: 10.1021/acs.analchem.4c02688
Da-Wei Li, Rodrigo Cabrera Allpas, Munki Choo, Lei Bruschweiler-Li, Alexandar L. Hansen, Rafael Brüschweiler
{"title":"COLMAR1d: A Web Server for Automated, Quantitative One-Dimensional Nuclear Magnetic Resonance-Based Metabolomics at Arbitrary Magnetic Fields","authors":"Da-Wei Li, Rodrigo Cabrera Allpas, Munki Choo, Lei Bruschweiler-Li, Alexandar L. Hansen, Rafael Brüschweiler","doi":"10.1021/acs.analchem.4c02688","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c02688","url":null,"abstract":"The field of metabolomics, which is quintessential in today’s omics research, involves the large-scale detection, identification, and quantification of small-molecule metabolites in a wide range of biological samples. Nuclear magnetic resonance spectroscopy (NMR) has emerged as a powerful tool for metabolomics due to its high resolution, reproducibility, and exceptional quantitative nature. One of the key bottlenecks of metabolomics studies, however, remains the accurate and automated analysis of the resulting NMR spectra with good accuracy and minimal human intervention. Here, we present the COLMAR1d platform, consisting of a public web server and an optimized database, for one-dimensional (1D) NMR-based metabolomics analysis to address these challenges. The COLMAR1d database comprises more than 480 metabolites from GISSMO enabling a database query of spectra measured at arbitrary magnetic field strengths, as is demonstrated for spectra acquired between <sup>1</sup>H resonance frequencies of 80 MHz and 1.2 GHz of mouse serum, DMEM cell growth medium, and wine. COLMAR1d combines the GISSMO metabolomics database concept with the latest tools for automated processing, spectral deconvolution, database querying, and globally optimized mixture analysis for improved accuracy and efficiency. By leveraging advanced computational algorithms, COLMAR1d offers a user-friendly, automated platform for quantitative 1D NMR-based metabolomics analysis allowing a wide range of applications, including biomarker discovery, metabolic pathway elucidation, and integration with multiomics strategies.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Solid-Phase Microextraction Mediated Solid-Phase Dielectric Barrier Discharge Vapor Generation–Atomic Fluorescence Spectrometry for Sensitive Determination of Mercury in Seawater 固相微萃取介导的固相介质势垒放电蒸汽发生-原子荧光光谱法用于灵敏测定海水中的汞
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-20 DOI: 10.1021/acs.analchem.4c04340
Runyan Wang, Shanshan Chen, Qian He, Shengrui Xu
{"title":"Solid-Phase Microextraction Mediated Solid-Phase Dielectric Barrier Discharge Vapor Generation–Atomic Fluorescence Spectrometry for Sensitive Determination of Mercury in Seawater","authors":"Runyan Wang, Shanshan Chen, Qian He, Shengrui Xu","doi":"10.1021/acs.analchem.4c04340","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04340","url":null,"abstract":"A novel method coupling solid-phase microextraction (SPME) to solid-phase dielectric barrier discharge (SPDBD) vapor generation was proposed and used for the sensitive detection of trace mercury (Hg) in seawater with atomic fluorescence spectrometry (AFS) in this work. The method proposed herein offers the unique advantages of integrating desorption and chemical vapor generation into one step, eliminating the use of elution reagents, and reducing the analysis time. SPME with multiwalled carbon nanotubes (MWCNTs) coated on the glass tube was used to extract Hg<sup>2+</sup> in seawater. The Hg<sup>2+</sup> was then desorbed and reduced to Hg<sup>0</sup> vapor by SPDBD, which was detected by cold vapor AFS. The parameters affecting Hg<sup>2+</sup> extraction, desorption, and vapor generation were studied. The detection limit of Hg<sup>2+</sup> was 0.0003 μg L<sup>–1</sup>, and the relative standard deviation at a Hg<sup>2+</sup> concentration of 0.05 μg L<sup>–1</sup> was 4.4%. This method also has excellent antimatrix interference ability for Hg<sup>2+</sup> determination with recoveries between 91.8% and 101.1% in the presence of extremely high concentrations (two million times excess) of coexisting ions. The practicality of this method was also evaluated by analyzing two different certified reference materials of Hg<sup>2+</sup> in water and several seawater samples with good spike recoveries (94.0%–107.4%). Compared with solid-phase photothermo-induced vapor generation, this method has higher extraction efficiency and higher desorption efficiency without the assistance of heating as well as a lower detection limit of Hg<sup>2+</sup>, which is capable of performing trace Hg analysis in seawater.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
DMF-Bimol: Counting mRNA and Protein Molecules in Single Cells with Digital Microfluidics DMF-Bimol:利用数字微流控技术计算单细胞中的 mRNA 和蛋白质分子
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-20 DOI: 10.1021/acs.analchem.4c03277
Shanshan Liang, Chong Li, Yu Ning, Rui Su, Mingyin Li, Yihao Huang, Yuning Zou, Liu Yang, Xing Xu, Chaoyong Yang
{"title":"DMF-Bimol: Counting mRNA and Protein Molecules in Single Cells with Digital Microfluidics","authors":"Shanshan Liang, Chong Li, Yu Ning, Rui Su, Mingyin Li, Yihao Huang, Yuning Zou, Liu Yang, Xing Xu, Chaoyong Yang","doi":"10.1021/acs.analchem.4c03277","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03277","url":null,"abstract":"Analyzing single-cell protein and mRNA levels yields invaluable insights into cellular functions and the intricacies of biologically heterogeneous systems. Current joint mRNAs and protein analysis methodologies suffer from relative quantification, low sensitivity, possible background interference, and tedious manual manipulation. Therefore, we propose DMF-Bimol that leverages addressable digital microfluidics to automate digital counting of single-cell mRNA and protein based on proximity ligation assay (PLA) and one-step RT-droplet digital PCR (RT-ddPCR). Through an engineered hydrophilic–hydrophobic interface, DMF-Bimol enables efficient single-cell isolation and lossless protein and nucleic acid processing. The closed droplet reaction system enhances the protein concentration and isolates exogenous contaminants, thereby dramatically improving the efficiency of the PLA reaction. The limit of detection of this approach achieves 3313 protein copies, marking a significant 17-fold enhancement in sensitivity over traditional benchtop PLA. This heightened sensitivity also uncovers a lower correlation between mRNA and protein levels in individual cells (Spearman <i>r</i> = 0.255) than bulk results, reflecting the complex relationship in heterogeneous cells. Using DMF-Bimol, we observed a significant upsurge of CD147 protein in CD138<sup>+</sup> myeloma cells but consistent levels of CD147 mRNAs compared with normal leukocytes. This discovery indicates a possible consequence of CD147 oncogenic activation that tends to harness protein translation to bolster tumor cell survival and enhance invasiveness, highlighting the potential of DMF-Bimol in unveiling intricate dynamics in translation processes at the single-cell level.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Comprehensive Coverage of Glycolysis and Pentose Phosphate Metabolic Pathways by Isomer-Selective Accurate Targeted Hydrophilic Interaction Liquid Chromatography-Tandem Mass Spectrometry Assay 通过异构体选择性精确靶向亲水相互作用液相色谱-串联质谱分析法全面覆盖糖酵解和五糖磷酸代谢途径
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-19 DOI: 10.1021/acs.analchem.4c03490
Kristian Serafimov, Michael Lämmerhofer
{"title":"Comprehensive Coverage of Glycolysis and Pentose Phosphate Metabolic Pathways by Isomer-Selective Accurate Targeted Hydrophilic Interaction Liquid Chromatography-Tandem Mass Spectrometry Assay","authors":"Kristian Serafimov, Michael Lämmerhofer","doi":"10.1021/acs.analchem.4c03490","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03490","url":null,"abstract":"The accurate liquid chromatography-tandem mass spectrometry analysis of phosphorylated isomers from glycolysis and pentose phosphate pathways is a challenging analytical problem in metabolomics due to extraction problems from the biological matrix, adherence to stainless steel surfaces leading to tailing in LC, and incomplete separation of hexose and pentose phosphate isomers. In this study, we present a targeted HILIC-ESI-MS/MS method based on a BEH amide fully porous 1.7 μm particle column with an inert surface coating of column hardware and multiple reaction monitoring (MRM) acquisition fully covering the glycolysis and pentose phosphate pathway metabolites. To minimize contact of the phosphorylated analytes with stainless steel surfaces, a μ-ESI-MS probe with a hybrid electrode made of PEEKsil was employed. Optimized HILIC gradient elution conditions with 100 mM ammonium formate (pH 11) provided the separation of hexose monophosphate and pentose phosphate isomers. To ensure good retention time repeatability in HILIC, perfluoroalkoxy alkane bottles were used for the mobile phase (with sd over 60 runs between 0.01 and 0.02 min). For the quantitative assay, the U-<sup>13</sup>C-labeled cell extract was spiked prior to extraction by metal oxide-based affinity chromatography (MOAC) with TiO<sub>2</sub> beads. The concentrations of the 24 targets were quantified in HeLa and human embryonic kidney (HEK293) cells. Erastin-induced ferroptosis in HEK293 cells was accompanied by enhanced levels of fructose-1,6-bis-phosphate, 2- and 3-phosphoglycerate, and 2,3-bis-phosphoglycerate.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449887","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacial Conductor-Modulated Low-Triggered Potential Electrochemiluminescence from Conjugated Polymers for Bioanalysis 用于生物分析的共轭聚合物的界面导体调制低触发电位电化学发光
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-19 DOI: 10.1021/acs.analchem.4c04146
Ying He, Jinwen Zhao, Guomin Yang, Ruo Yuan, Shihong Chen
{"title":"Interfacial Conductor-Modulated Low-Triggered Potential Electrochemiluminescence from Conjugated Polymers for Bioanalysis","authors":"Ying He, Jinwen Zhao, Guomin Yang, Ruo Yuan, Shihong Chen","doi":"10.1021/acs.analchem.4c04146","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04146","url":null,"abstract":"Polyfluorene and its derivatives (PFs) are extremely appealing electrochemiluminescence (ECL) illuminants thanks to their easy modification, high quantum yield, excellent photostability, and nontoxicity, exhibiting great application potential in ECL sensing and imaging. Unfortunately, most reported PFs-based ECL bioanalysis generally exhibited high triggering potential (&gt;1.0 V vs Ag/AgCl), which introduced undesirable electrochemical interference to adversely affect the sensitivity and accuracy of biological analysis. This work innovatively exploited poly(3,4-ethylenedioxythiophene) (PEDOT) as an interfacial conductor to modulate the low ECL triggering potential of poly[(9,9-dioctylfluorenyl-2,7-diyl)-<i>co</i>-(1,4-benzo-{2,1′,3}-thiadazole)] (PFBT) nanoparticles (NPs). The unique conductivity of in situ electrodeposited PEDOT promoted electron transfer between PFBT NPs and coreactant tripropylamine (TPrA), negatively shifting the ECL triggering potential of PFBT NPs from +1.22 to +0.78 V. The PFBT NPs/PEDOT coupled the localized hybridization chain reaction (LHCR) circuits to achieve a specific and sensitive ECL detection of malathion (MAL), and a low limit of detection (LOD) of 22 fg/mL was obtained. The interfacial conductor provides inspiration for creating the low ECL triggering potential. PFBT NPs-coupled PEDOT builds a low ECL triggering potential of the PFs-based platform for pesticide residue analysis with low interference and high sensitivity.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-Coverage Disulfide Mapping Enabled by Programmable Disulfide-Ene Reaction Integrated onto a Bottom-Up Protein Analysis Workflow 将可编程二硫-炔反应集成到自下而上的蛋白质分析工作流程中,实现高覆盖率二硫绘图
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2024-10-19 DOI: 10.1021/acs.analchem.4c04257
Keting Zhou, Yu Xia
{"title":"High-Coverage Disulfide Mapping Enabled by Programmable Disulfide-Ene Reaction Integrated onto a Bottom-Up Protein Analysis Workflow","authors":"Keting Zhou, Yu Xia","doi":"10.1021/acs.analchem.4c04257","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04257","url":null,"abstract":"Mapping disulfide linkages is crucial for characterizing pharmaceutical proteins during drug development and quality control. Traditional bottom-up protein analysis workflows often suffer from incomplete mapping for tryptic peptides consisting of multiple disulfide bonds. Although the employment of a partial reduction of disulfide bonds can improve disulfide mapping, it becomes a bottleneck of analysis because individual tuning is often needed. Herein, we have developed an online disulfide-ene reaction system in which the composition of the reaction solvent can be programmed to achieve optimal partial reduction of tryptic disulfide peptides after liquid chromatography separation. By coupling this system onto a bottom-up protein analysis workflow, high coverage for sequencing (71–83%) and disulfide mapping (84–100%) was achieved for standard proteins consisting of 4–19 disulfide bonds. The analytical capability was further demonstrated by mapping 13 scrambled disulfide bonds in lysozyme and achieving compositional analysis of IgG isotypes (κ and λ) and subclasses (IgG1–IgG4) from human plasma.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":null,"pages":null},"PeriodicalIF":7.4,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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