Analytical Chemistry最新文献

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Highly Sensitive Hyperpolarized Multiplexed Single-Scan 2D 13C−1H NMR of Complex Mixtures at Natural 13C Abundance 高灵敏度超极化多路单扫描二维13C−1H核磁共振在自然13C丰度复杂混合物
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-17 DOI: 10.1021/acs.analchem.6c04662
Wiktor Adamski,Yuliia Horbenko,Benoît Charrier,Aurélie Bernard,Patrick Giraudeau
{"title":"Highly Sensitive Hyperpolarized Multiplexed Single-Scan 2D 13C−1H NMR of Complex Mixtures at Natural 13C Abundance","authors":"Wiktor Adamski,Yuliia Horbenko,Benoît Charrier,Aurélie Bernard,Patrick Giraudeau","doi":"10.1021/acs.analchem.6c04662","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c04662","url":null,"abstract":"Abstract Hyperpolarization provides a major sensitivity boost in NMR spectroscopy, and dissolution Dynamic Nuclear Polarization (d-DNP) has emerged as a particularly well-suited approach to analyze complex mixtures at natural 13C abundance. However, it only allows single-scan NMR detection due to the irreversible nature of hyperpolarized magnetization decay in solution. This precludes the acquisition of heteronuclear 2D NMR spectra, which are highly needed to obtain information on the identity and concentration of mixture components. To overcome this issue, ultrafast (UF) 2D NMR has been the method of choice for the last two decades, but it suffers from limited resolution and sensitivity, which restrains its application to 13C-labeled or highly concentrated molecular mixtures. Herein, we propose a new concept coined Selective Multiplexed Acquisition by Sequential Harnessing (SMASH), which when combined with d-DNP allows us to retrieve 13C−1H correlations of small-molecule mixtures at low mM concentrations (in d-DNP juice) and natural 13C abundance. This new method improves the sensitivity of single-scan heteronuclear 2D NMR by a factor of 10 to 20 compared to UF experiments, thus considerably lowering the limit of detection of d-DNP-hyperpolarized 2D NMR experiments. The potential of SMASH NMR is illustrated on d-DNP hyperpolarized metabolite mixtures, showing that it will complement UF 2D NMR methods in the future to reveal the 13C−1H correlations of hyperpolarized small-molecule mixtures at 13C natural abundance.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"39 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209959","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
Synergistic Vacancy-Mediated Adsorption-Activation Strategy and Spatial Confinement Effect for Enhanced Electrochemiluminescence Sensing of Isocarbophos 协同空位介导的吸附活化策略及空间限制效应增强异硫磷的电化学发光传感
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c04668
Chenxi Yang,Ying Wang,Xiaojiao Du,Xueling Shan,Wenchang Wang,Haijiao Xie,Ding Jiang
{"title":"Synergistic Vacancy-Mediated Adsorption-Activation Strategy and Spatial Confinement Effect for Enhanced Electrochemiluminescence Sensing of Isocarbophos","authors":"Chenxi Yang,Ying Wang,Xiaojiao Du,Xueling Shan,Wenchang Wang,Haijiao Xie,Ding Jiang","doi":"10.1021/acs.analchem.6c04668","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c04668","url":null,"abstract":"Abstract Exploring advanced strategies to overcome the sluggish activation kinetics of co-reactants and insufficient radical generation is pivotal for boosting electrochemiluminescence (ECL) sensing performance. Herein, an active radical-enriched ECL sensing platform for the ultrasensitive detection of isocarbophos (ICP) was fabricated by utilizing a synergistic vacancy-mediated adsorption-activation strategy coupled with a spatial confinement effect. Specifically, an oxygen-deficient titanium metal−organic framework (D-Ti MOF) was integrated as a robust co-reaction accelerator to trigger the emission of a pyrene-based hydrogen-bonded organic framework (PSA-HOF). Mechanistic studies revealed that abundant oxygen vacancies in D-Ti MOF served as catalytic sites, lowering the activation barrier of peroxydisulfate (K2S2O8) and promoting targeted adsorption and O−O bond cleavage to generate a high flux of sulfate radicals (SO4•−). Meanwhile, the porous MOF architecture imposed nanoscale spatial confinement, enriching reactive intermediates at the electrode interface and reducing diffusional loss. Such a confinement-enabled interfacial microenvironment was further substantiated by kinetic analyses, which revealed that D-Ti MOF promoted S2O82− reduction and redirected the process from predominantly diffusion-controlled behavior toward an adsorption- and confinement-coupled pathway, thereby increasing the local availability and productive utilization of reactive intermediates. Leveraging an isocarbophos-specific split aptamer recognition strategy, the proposed ECL biosensor exhibited a broad linear range (10 fM to 0.1 μM), an ultralow detection limit (8.38 fM), excellent stability, remarkable selectivity and reproducibility, making it highly applicable for practical sample monitoring. This work offers a new perspective for advancing co-reactant-based ECL biosensors and proposes a novel design strategy for ultrasensitive ECL sensing platforms.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209328","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
Synergistic Integration of Water-Stable 2D Perovskite Heterojunctions and Self-Priming DNA Walkers for Sensitive Photoelectrochemical Biosensing 水稳定的二维钙钛矿异质结和自吸DNA助行器的协同集成用于敏感的光电化学生物传感
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c05016
Chaomin Gao,Haihan Yu,Shenguang Ge,Jinghua Yu
{"title":"Synergistic Integration of Water-Stable 2D Perovskite Heterojunctions and Self-Priming DNA Walkers for Sensitive Photoelectrochemical Biosensing","authors":"Chaomin Gao,Haihan Yu,Shenguang Ge,Jinghua Yu","doi":"10.1021/acs.analchem.6c05016","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c05016","url":null,"abstract":"Abstract Two-dimensional Ruddlesden−Popper (2D RP) perovskites hold immense promise as light-harvesting photoactive materials for photoelectrochemical (PEC) bioanalysis, yet their poor aqueous durability and suboptimal charge-carrier dynamics severely restrict PEC sensing implementation. Herein, we report a dual-functional strategy that simultaneously addresses both challenges through the in-situ construction of a Z-scheme heterojunction, (BA)2PbI4−Pb(OH)2 (BA = butylammonium), via Lewis base vapor diffusion. The Pb(OH)2 barrier formed during synthesis acts as a robust protective shield that preserves the perovskite’s structural integrity, while the intimate Z-scheme heterointerface constructed in the heterojunction remains functional and continues to accelerate spatial charge separation even after three years of immersion in ultrapure water, as corroborated by electron paramagnetic resonance spectroscopy, photo-assisted Kelvin probe force microscopy, and density functional theory calculations. To further amplify the PEC signal, we engineer a circular DNA scaffold-supported tripedal DNA walker powered by self-priming polymerization, eliminating the requirement for exogenous primers in traditional polymerase-driven DNA nanomachines. Target-triggered autonomous walking of the tripedal DNA nanomachine continuously disassembles surface-tethered hairpin tracks, drastically mitigating interfacial steric hindrance and yielding prominent photocurrent enhancement. Synergizing the ultra-stable Z-scheme RP perovskite photoelectrode with the primer-free DNA walker, the integrated PEC sensing platform achieves ultrasensitive quantification of acetamiprid with a wide linear range spanning 10−13 to 10−6 M. This work establishes a new paradigm for rationally designing aqueous-stable perovskites and coupling them with intelligent molecular devices, paving the way for high-performance PEC sensing platforms.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"64 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210006","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
When Two Interfaces Meet: A Unified Theory for Thin-Membrane Voltammetric Ion Selective Electrodes 当两个界面相遇:薄膜伏安离子选择电极的统一理论
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c03127
Javier López-Asanza,Edward Zamudio,Angela Molina,Gastón A. Crespo,María Cuartero,Eduardo Laborda
{"title":"When Two Interfaces Meet: A Unified Theory for Thin-Membrane Voltammetric Ion Selective Electrodes","authors":"Javier López-Asanza,Edward Zamudio,Angela Molina,Gastón A. Crespo,María Cuartero,Eduardo Laborda","doi":"10.1021/acs.analchem.6c03127","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c03127","url":null,"abstract":"Abstract Voltammetric solid-contact ion-selective electrodes (SC-ISEs) exhibit electrochemical responses that arise from the coupling of heterogeneous electron transfer at the electrode−membrane interface with ion transfer at the membrane−sample boundary. In this work, a novel theoretical framework is developed for voltammetric SC-ISEs based on thin membranes, capturing the intrinsic consequences of coupling two polarized interfaces in series under markedly different mass-transport conditions in the membrane and solution phases. The theory describes the current/charge−potential−time responses and the corresponding interfacial potentials and dynamic ion and redox-species concentrations, accounting for the effects of membrane and solution composition, membrane thickness, and experimental timescale. Besides, the theory enables quantitative analysis of experimental voltammetric outcomes. A systematic classification of cyclic voltammetry (CV) responses is obtained in terms of three dimensionless parameters that quantify ion availability in the sample solution relative to the confined membrane. Simple relationships for peak positions and practical diagnostic criteria based on CV shape and scan-rate dependence are derived to verify thin-membrane conditions and the absence of kinetic or ohmic limitations, identifying indeed whether charge compensation proceeds via ion release or uptake.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"626 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209963","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
AND-Gated Intramolecular Confined CHA Converts Forked DNA Probes into Brushlike Assemblies for Tumor-Cell Imaging and门控分子内受限CHA将叉形DNA探针转化为用于肿瘤细胞成像的刷状组件
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c05499
Shui Qin Chai,Xin Hou,Jiu Mao Zhao,Wan Lin Sun,Shu Chen Pei,Yun Ying Cheng,Wen Yi Lv,Chun Mei Li
{"title":"AND-Gated Intramolecular Confined CHA Converts Forked DNA Probes into Brushlike Assemblies for Tumor-Cell Imaging","authors":"Shui Qin Chai,Xin Hou,Jiu Mao Zhao,Wan Lin Sun,Shu Chen Pei,Yun Ying Cheng,Wen Yi Lv,Chun Mei Li","doi":"10.1021/acs.analchem.6c05499","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c05499","url":null,"abstract":"Abstract Sensitive and selective imaging of low-abundance intracellular biomarkers is important for cellular analysis and disease-related biomarker evaluation, but it is often hampered by insufficient sensitivity and false-positive signals from single-target analysis. Herein, we developed a dual-locked forked DNA fluorescent probe (DL-forked probe) that integrated intramolecular confined catalytic hairpin assembly (intra-CHA) with AND-logic gating. The probe facilitated cellular uptake in the tested tumor cells via the AS1411 aptamer, without transfection reagents. APE1 and miRNA-21, two biomarkers overexpressed in tumor cells, served as the dual inputs. APE1 first cleaved the AP site in H2 to expose a toehold for miRNA-21, which then triggered a rapid intra-CHA cycle, converting the forked structure into brushlike DNA assemblies with fluorescence recovery. The spatial confinement effect restricted the reactants within ∼13 nm, with the geometric local concentration approximately 9.2 × 103-fold higher than the nominal concentration of the free-CHA system, thereby drastically accelerating reaction kinetics. The DL-forked probe exhibited a detection limit of 29 pM for miRNA-21 and 7.0 × 10−3 U/mL for APE1, with outstanding selectivity. In live-cell imaging, the probe generated 2.2-fold stronger fluorescence than the free-CHA control and produced distinct fluorescence responses among the tested tumor cells (MDA-MB-231, MCF-7, A549) and normal AML12 cells, with signal enhancements of 14.7- to 33.0-fold. These results agreed well with the independent reference methods of ELISA and RT-qPCR. This AND-gated, confinement-accelerated CHA platform provides a potential strategy for dual-biomarker-gated intracellular imaging and warrants further evaluation in clinically relevant models.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210009","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
Structural Encoding-decoupled Universal RecognitionEnables Amplification-free Multiplex miRNA Detection 结构编码解耦通用识别实现无放大的多重miRNA检测
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c03760
Chang Zhang,Hao Wang,Yingying Zhu,Haifeng Dong,Huiting Lu
{"title":"Structural Encoding-decoupled Universal Recognition\u0000Enables Amplification-free Multiplex miRNA Detection","authors":"Chang Zhang,Hao Wang,Yingying Zhu,Haifeng Dong,Huiting Lu","doi":"10.1021/acs.analchem.6c03760","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c03760","url":null,"abstract":"Abstract Accurate multiplex analysis of microRNAs (miRNAs) remains constrained by enzymatic amplification, spectral crosstalk, and instrumental complexity. Herein, we report a conceptually distinct PhC-SQ platform that integrates photonic crystal (PhC) structural encoding with S9.6-mediated universal recognition for amplification-free multiplex miRNA detection. PhC microspheres act as structural color barcodes for target encoding, while quantum dots (QDs) enriched at the microsphere interface serve as fluorescent reporters. Target miRNAs hybridize with surface-bound DNA probes to form DNA/RNA duplexes, which are recognized by the S9.6 antibody. Subsequent biotin–streptavidin assembly recruits QDs, enabling interfacial fluorescence enrichment and enhanced sensitivity without enzymatic amplification. By decoupling encoding from readout, the platform eliminates spectral crosstalk and enables accurate multiplexing. A dual-mode readout, combining confocal quantification with direct UV visualization, further supports point-of-care applicability. Validation in cellular samples shows good agreement with RT-PCR. Overall, this work establishes a structural encoding-universal recognition-interfacial signal enrichment strategy for robust and field-deployable multiplex miRNA detection.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210014","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
A Novel sMRMHR Pseudotargeted Method for Rapid Chemome Comparison Among Herbal Medicines: from Metabolome to Exposome 一种新的sMRMHR伪靶向方法用于草药间快速化学组比较:从代谢组到暴露组
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c01533
Xing Wang,Chen-Xi Shen,Si-Min Shao,Tian-Bo Ma,Jing Cui,Qing-Xuan Ren,Hua Yang,Wen Gao
{"title":"A Novel sMRMHR Pseudotargeted Method for Rapid Chemome Comparison Among Herbal Medicines: from Metabolome to Exposome","authors":"Xing Wang,Chen-Xi Shen,Si-Min Shao,Tian-Bo Ma,Jing Cui,Qing-Xuan Ren,Hua Yang,Wen Gao","doi":"10.1021/acs.analchem.6c01533","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c01533","url":null,"abstract":"Abstract The metabolomic comparison of closely related herbal species, both the intrinsic plant metabolome and the subsequent in vivo exposome, is vital for ensuring drug safety and elucidating therapeutic mechanisms. However, such a comparison is challenging because medicinal plants within the same genus share similar chemical profiles with minor chemical or abundance differences, and their in vivo exposure levels are typically low and are affected by complex biological matrices. In this study, Curcumae Radix (CR), a traditional Chinese medicine derived from the roots of four Curcuma species, was used as a case study. A pseudotargeted workflow based on scheduled high-resolution multiple reaction monitoring (sMRMHR) was established to compare the metabolites and plasma exposure profiles of these species, using a transition library constructed from the four plant species. The sMRMHR pseudotargeted method showed acceptable linearity, repeatability, and stability in QC samples and 12 reference standards, with performance comparable to that of SWATH and TOF MS1 while maintaining stable coefficients of variation (CVs) at low concentrations. Specifically, 95.2% of metabolomic features showed linearity with R2 ≥ 0.8, 98.16% showed a CV ≤ 30%. In exposomics, 83.14% of exposures had matrix effect factor (MF) CVs below 30%, and over 300 exposures showed MFs within 70%−130%. Finally, the application results of CR demonstrate its capability for chemome comparison of metabolites and exposures. In conclusion, this approach provides a practical HRMS-based strategy for the integrated comparison of plant metabolite profiles and plasma exposure-related profiles across closely related medicinal species, and may support subsequent studies of interspecies chemical differences and in vivo exposure characteristics after oral administration.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"63 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209326","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
Physically Constrained Inverse-Gaussian Deconvolution of Diffusion-Broadened Drift-Tube Ion Mobility Spectra 扩散加宽漂管离子迁移谱的物理约束反高斯反卷积
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c05780
Haoran Huang,Zhicheng Li,Lu Chen,Jianna Yu,Wenjie Liu
{"title":"Physically Constrained Inverse-Gaussian Deconvolution of Diffusion-Broadened Drift-Tube Ion Mobility Spectra","authors":"Haoran Huang,Zhicheng Li,Lu Chen,Jianna Yu,Wenjie Liu","doi":"10.1021/acs.analchem.6c05780","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c05780","url":null,"abstract":"Abstract Peak overlap limits chemical assignment in drift-tube ion mobility spectrometry (DT-IMS). Diffusion broadening is commonly modeled with symmetric Gaussian kernels, although a fixed detector records ion first-passage times. We developed an inverse-Gaussian-Nernst-Townsend-Einstein (IG-NTE) deconvolution framework in which the point-spread function (PSF) follows an inverse-Gaussian distribution and its temporal width is constrained by instrument settings through the NTE relation. The resulting drift-time-dependent measurement operator was inverted by nonnegative Richardson-Lucy iteration without peak-width calibration or specification of component number. In simulations, relative to a Gaussian kernel, IG-NTE deconvolution reduced the average full-residual root-mean-square value by 11.4%, the right-tail residual by 18.1%, and the mean absolute peak-area deviation from 5.10% to 1.19%. Applied to a 63Ni DT-IMS instrument, the method separated ethyl 2-methylpentanoate and 1,8-cineole responses 0.040 ms apart while retaining 2,6-di-tert-butylpyridine (DTBP) as a single-component control. It also recovered paired alkyl-pyrazine mobility features consistent with protonation site- and hydration-dependent collision cross sections. In the negative mode, dichloromethane-derived chloride responses assigned to 35Cl− and 37Cl− exhibited a 3.08:1 area ratio and were supported by GC-TOF-MS. These results show that detector-domain transport modeling can improve the effective reconstructed resolution of diffusion-broadened DT-IMS spectra without hardware modification, provided that controls and forward residual analysis are used to assess reconstruction artifacts.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"57 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209327","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
In Situ Time-Weighted Average Monitoring of 11 Antiviral Drugs in Natural Waters Using Diffusive Gradients in Thin-Films with Graphitized Carbon Black and Mixed-Mode Resin Binding Gels 利用石墨化炭黑薄膜和混合模式树脂结合凝胶的扩散梯度对天然水体中11种抗病毒药物的原位时间加权平均监测
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c03524
Zhou Fang,Kefei Huang,Hao Zhang,Kevin C. Jones,Haitao Sun,Li Zhang,Lei Zhang,Jun Luo
{"title":"In Situ Time-Weighted Average Monitoring of 11 Antiviral Drugs in Natural Waters Using Diffusive Gradients in Thin-Films with Graphitized Carbon Black and Mixed-Mode Resin Binding Gels","authors":"Zhou Fang,Kefei Huang,Hao Zhang,Kevin C. Jones,Haitao Sun,Li Zhang,Lei Zhang,Jun Luo","doi":"10.1021/acs.analchem.6c03524","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c03524","url":null,"abstract":"Abstract The widespread occurrence of antiviral drugs in aquatic systems has raised concerns on their potential ecological risks, necessitating reliable monitoring techniques. This study introduces the first application of the diffusive gradients in thin-films (DGT) technique for the in situ measurement of 11 commonly used antiviral drugs from six therapeutic categories. Two complementary DGT configurations were developed, employing graphitized carbon black (ENVI-CARB) and a mixed-mode resin (MCX + HLB at a 6:4 mass ratio) embedded in agarose as the binding phases. Diffusion coefficients of all target compounds in the diffusive gel were determined for the first time using a diffusion cell, and stable elution efficiencies were obtained with acetonitrile/formic acid for ENVI-CARB and acetonitrile/ammonia for MCX + HLB. Both DGT devices performed robustly across wide environmental gradients: pH 3.16−9.74, ionic strength 0.1−500 mmol L−1 and dissolved organic matter up to 20 mg L−1. The total binding capacities exceeded 230 μg per disc, supporting deployments over several months in natural waters. Laboratory evaluations of diffusive layer thickness (0.515−2.015 mm), deployment time (10−168 h), storage stability (≥148 days) and competitive adsorption confirmed the reliability of the method. Field deployments at five river sites in Nanjing, China, during a 14 day period detected ribavirin (9−29 ng L−1) and lamivudine (12−29 ng L−1) as the predominant antivirals. The DGT-derived time-weighted average concentrations closely matched those from repeated grab sampling while effectively capturing episodic pollution events that individual grab samples missed. The developed DGT samplers thus provide a robust, cost-effective and sensitive tool for source tracking and long-term monitoring of antiviral drugs, overcoming the inherent limitations of conventional grab sampling in dynamic aquatic environments.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"292 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209965","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
Soft Wearable Aptamer Wristband Enables Real-Time Sweat Dual-Hormone Monitoring for Menstrual Cycle Tracking 柔软可穿戴的适体腕带使实时汗液双激素监测月经周期跟踪
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2026-10-16 DOI: 10.1021/acs.analchem.6c06397
Jiaqi Liu,Yuyang Yang,Renfeng Dong,Tailin Xu
{"title":"Soft Wearable Aptamer Wristband Enables Real-Time Sweat Dual-Hormone Monitoring for Menstrual Cycle Tracking","authors":"Jiaqi Liu,Yuyang Yang,Renfeng Dong,Tailin Xu","doi":"10.1021/acs.analchem.6c06397","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c06397","url":null,"abstract":"Abstract Noninvasive and longitudinal monitoring of female reproductive hormones could provide valuable information on individualized endocrine dynamics across the menstrual cycle. Here, we developed an integrated wearable electrochemical platform for simultaneous monitoring of estradiol (E2) and progesterone (P4), together with sweat pH and ionic strength. Competitive-displacement aptamer sensing interfaces were constructed for dual-hormone detection, while a Tesla-valve microfluidic network supported passive sweat transport and sequential sample replacement. A flexible wireless electronic system provided multiplexed signal acquisition and wireless data transmission. To improve quantitative reliability under variable sweat conditions, pH-dependent calibration was incorporated into hormone analysis. The platform was evaluated in two volunteers over approximately one complete menstrual cycle, and the longitudinal E2 and P4 profiles obtained by the wearable sensors showed similar temporal trends to those obtained by paired sweat enzyme-linked immunosorbent assay (ELISA) measurements. pH compensation further improved the correlation between sensor and ELISA measurements of hormone concentrations. These results demonstrate the feasibility of integrating dual-hormone sensing, pH-dependent calibration, microfluidic sweat management, and wireless electronics into a wearable platform for longitudinal monitoring of reproductive hormone dynamics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"64 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210062","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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