Analytical Chemistry最新文献

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Deciphering the Mechanism of Interactions between Polyubiquitin Chains and Caspase Activation and Recruitment Domains Using Protein-Polymer-Engineering-Assisted Native Mass Spectrometry. 利用蛋白质-聚合物工程辅助天然质谱法解读多泛素链与Caspase激活和募集结构域之间相互作用的机制。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-13 DOI: 10.1021/acs.analchem.5c01898
Bin Song,Qingrong Chen,Rongrong Dai,Guanbo Wang,Jie Zheng
{"title":"Deciphering the Mechanism of Interactions between Polyubiquitin Chains and Caspase Activation and Recruitment Domains Using Protein-Polymer-Engineering-Assisted Native Mass Spectrometry.","authors":"Bin Song,Qingrong Chen,Rongrong Dai,Guanbo Wang,Jie Zheng","doi":"10.1021/acs.analchem.5c01898","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01898","url":null,"abstract":"Polyubiquitin (polyUb) chain topology plays important roles in determining Ub chain conformation and therefore directs specific cellular signal transductions. However, little is known about the conformational dynamics of polyUb chains and their complex topology. A major challenge lies in the inherent heterogeneity of native polyUb chains, which often exist as mixtures of different lengths and linkage types, making it difficult to achieve molecular-level characterization. Herein, we synthesized a panel of Lys63(K63)-linkage-specific polyUb chain ladders via E1-E2 cascade reactions as a platform for complexation with K63-linkage-specific binding proteins, including RNA sensors RIG-I, MDA5, and their adaptor MAVS, which govern the antiviral-signaling pathways in innate immunity. Taking advantage of precise stoichiometry control, we used native mass spectrometry to decipher their dynamic signaling mechanisms. The flexible range of polyUb chain lengths allowed polyUb to populate mono-, di-, and trimeric states and the corresponding conformations in solutions. Hexamer and undecamer were identified as the minimum-length polyUb chains adopting conformers enabling stable binding to RIG-ICARDs and MDA5CARDs at a 1:4 stoichiometry, respectively, demonstrating that a single Ub6 or Ub11 chain can stabilize the tetrameric structures of these antiviral-signaling complexes. Alternatively, polyUb chains enable the flexible accommodation of alternative stoichiometric constraints to regulate the tetramerizing events by RIG-ICARDs and MDA5CARDs. Further in-depth analysis of RIG-I/MDA5CARDs-MAVSCARD-K63-polyUb14+ complexes uncovered the assembly of macromolecular complexes featuring over 9 layers of MAVSCARD filaments. These findings elucidate the intricate interplay between the length of K63-polyUb chains and their dynamic binding stoichiometries and topologies during signaling transductions.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"28 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043838","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
Gap-Controlled Infrared Absorption Spectroscopy: A Unique Interface-Sensitive Spectroscopy Based on the Combination of Linear Spectroscopy and Multivariate Curve Resolution. 间隙控制红外吸收光谱:一种独特的基于线性光谱和多元曲线分辨率相结合的界面敏感光谱。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-13 DOI: 10.1021/acs.analchem.5c02765
Shoichi Maeda,Shunta Chikami,Subin Song,Maria Vanessa Balois-Oguchi,Airi Katase,Glenn Villena Latag,Takuo Tanaka,Tomohiro Hayashi
{"title":"Gap-Controlled Infrared Absorption Spectroscopy: A Unique Interface-Sensitive Spectroscopy Based on the Combination of Linear Spectroscopy and Multivariate Curve Resolution.","authors":"Shoichi Maeda,Shunta Chikami,Subin Song,Maria Vanessa Balois-Oguchi,Airi Katase,Glenn Villena Latag,Takuo Tanaka,Tomohiro Hayashi","doi":"10.1021/acs.analchem.5c02765","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02765","url":null,"abstract":"We present an interface-sensitive spectroscopy method that integrates attenuated total reflection infrared absorption (ATR-IR) spectroscopy, a distance control system, and multivariate curve resolution (MCR). In this approach, we adjust the distance between the sample and the ATR prism while collecting a series of spectra that reflect various contributions from both bulk and interfacial regions. Subsequently, we utilize MCR to extract the spectral components specific to the interfacial region. Here, we validate this method through the analysis of interfacial water adjacent to self-assembled monolayers (SAMs), quartz, polymers, and polymer brush films. Our findings are compared with results from other interface-sensitive spectroscopic techniques, confirming the interface sensitivity of our approach. This method does not necessitate surface enhancement or nonlinear optical effects and imposes virtually no restrictions on the types of samples suitable for analysis. Furthermore, it allows us to assess the thickness of the interfacial region using a spectral component distinct from the bulk region, revealing insights into the relationship between the interfacial behavior of molecules and related phenomena. Additionally, this method can be seamlessly integrated into standard ATR-IR spectroscopes, offering a straightforward solution for interface-sensitive spectroscopy.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"34 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043765","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
The Impact of Rare Adsorption Site Clustering on Peak Broadening in Chromatography. 稀有吸附位点聚类对色谱峰展宽的影响。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-13 DOI: 10.1021/acs.analchem.5c03108
Nikita Kovalenko,Christy F Landes
{"title":"The Impact of Rare Adsorption Site Clustering on Peak Broadening in Chromatography.","authors":"Nikita Kovalenko,Christy F Landes","doi":"10.1021/acs.analchem.5c03108","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03108","url":null,"abstract":"Peak broadening is one of the most important phenomena in chromatography, leading to a decrease in the separation efficiency. It is well-known that the presence of rare sites on the adsorption surface, which have different kinetic characteristics compared to the majority sites, may result in peak broadening and tailing. Here, we extended a Monte Carlo model of chromatography, based on stochastic theory, and included an intermediate layer between the stationary and mobile phases to delve deeper into the study of this phenomenon. We discover that not only the fraction of rare sites and their individual characteristics are important, but also their distribution on the adsorption surface. Our results demonstrate that the spatial distribution of adsorption sites impacts peak broadening; specifically, the clustering of slow, rare adsorption sites broadens the peak, and this effect remains evident even considering longitudinal and eddy diffusion in the simulation of advective-diffusive transport.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"77 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043840","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
Ultra-Sensitive Near-Infrared Imaging of Micro-Neuroinflammation with Surface-Engineered Silver Indium Selenide Quantum Dots. 表面工程硒化银铟量子点微神经炎症的超灵敏近红外成像。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-13 DOI: 10.1021/acs.analchem.5c04255
Wanru Tian,Xin Zhao,Yao Li,Xuan Cheng,Zheng Yang,Peisen Zhang,Mingxia Jiao,Xiliang Luo
{"title":"Ultra-Sensitive Near-Infrared Imaging of Micro-Neuroinflammation with Surface-Engineered Silver Indium Selenide Quantum Dots.","authors":"Wanru Tian,Xin Zhao,Yao Li,Xuan Cheng,Zheng Yang,Peisen Zhang,Mingxia Jiao,Xiliang Luo","doi":"10.1021/acs.analchem.5c04255","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04255","url":null,"abstract":"Encephalitis, a severe inflammatory brain condition, poses significant diagnostic challenges due to its heterogeneous symptoms and the limitations of conventional imaging techniques, such as magnetic resonance imaging (MRI), which often fail to detect early or subtle lesions. To address this clinical need, herein, a near-infrared (NIR) optical imaging strategy using engineered silver indium selenide quantum dots (QDs) was developed for precise and early detection of microencephalitic lesions. The QDs were synthesized via a robust aqueous-phase method with optimized NIR emission intensity through suppression of nonradiative recombination pathways. Surface modification with carboxyl-terminated poly(ethylene glycol) (carboxyl-PEG) enhanced colloidal stability, biocompatibility, and selective uptake capabilities by disease-associated M1 macrophages, improving localization at inflammatory sites. In vivo studies demonstrated the outstanding imaging performance of QDs, with encephalitis lesions clearly delineated at ultrahigh spatial resolution, enabling reliable detection of microinflammatory foci as small as 4.6 mm × 5.3 mm. This breakthrough capability facilitates early diagnosis by resolving sub-5 mm lesions, surpassing the sensitivity and resolution of conventional methods for the first time. By providing a noninvasive, high-resolution diagnostic tool, this technology holds potential for improving clinical decision-making and patient outcomes in encephalitis and other neuroinflammatory disorders, particularly in resource-limited settings where early diagnosis remains challenging.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043843","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
sEV-ICP-TOF-MS for Multiparametric Single-EV Analysis via Nanoparticle-Conjugated Antibodies and Isotope Ratio Filtering. sEV-ICP-TOF-MS用于纳米颗粒偶联抗体和同位素比值过滤的多参数单ev分析。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-12 DOI: 10.1021/acs.analchem.5c02801
Minseop Kim,Seung Min Ha,Eunyong Ha,Yewon Han,Zayakhuu Gerelkhuu,Tae Hyun Yoon
{"title":"sEV-ICP-TOF-MS for Multiparametric Single-EV Analysis via Nanoparticle-Conjugated Antibodies and Isotope Ratio Filtering.","authors":"Minseop Kim,Seung Min Ha,Eunyong Ha,Yewon Han,Zayakhuu Gerelkhuu,Tae Hyun Yoon","doi":"10.1021/acs.analchem.5c02801","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02801","url":null,"abstract":"Extracellular vesicles (EVs) play a vital role in cell-to-cell communication and hold great promise for diagnostics and therapy. However, their small size, heterogeneity, and interference with other nanoparticles make them difficult to detect and characterize using traditional methods. In this study, we introduce a single-EV inductively coupled plasma time-of-flight mass spectrometry (sEV-ICP-TOF-MS) technique that integrates mass cytometry with nanoparticle-conjugated antibodies and isotope ratio filtering to improve EV detection and quantification. The application of nanoparticle-conjugated antibodies significantly increased the detection sensitivity compared to metal isotope-conjugated antibodies, allowing for reliable identification of EVs with low-abundance surface markers. The implementation of isotope ratio filtering enhanced signal specificity by distinguishing EV signals from background noise based on the distinct natural isotopic abundance patterns of the nanoparticles. Quantitative analysis of calibration curves revealed that applying isotope ratio filtering enhanced the limit of detection (LOD) by more than 36-fold, reducing it to 2.07 × 104 particles/mL, resulting in an extension of linear range by 2 orders of magnitude toward lower concentrations. Multiparametric profiling of surface proteins uncovered a bimodal distribution of CD9+CD63+ coexpression, indicating further heterogeneity in CD9+CD63+ EV subpopulations. This novel sEV-ICP-TOF-MS technique enhances both the sensitivity and specificity of single-EV detection and enables high-resolution, multiparametric EV profiling. It presents a scalable approach with strong potential for biomarker discovery, disease diagnostics, and advancing our understanding of EV biology.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"35 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036045","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
Probing the Growth Kinetics of Bioinspired Phenolic Nanocoating via Evanescent Wave Excited by Fiber-Optic Modal Interferometry. 利用光纤模态干涉法激发倏逝波探测仿生酚醛纳米涂层生长动力学。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-12 DOI: 10.1021/acs.analchem.5c04029
Xin Xin,Junjun Wu,Qiang Ling,Xun Zhu,Qiang Liao
{"title":"Probing the Growth Kinetics of Bioinspired Phenolic Nanocoating via Evanescent Wave Excited by Fiber-Optic Modal Interferometry.","authors":"Xin Xin,Junjun Wu,Qiang Ling,Xun Zhu,Qiang Liao","doi":"10.1021/acs.analchem.5c04029","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04029","url":null,"abstract":"Bioinspired polydopamine (PDA) nanocoating poses one important measure to precisely customize functionalized surfaces, while its dynamic growth characteristics are still not fully understood. Herein, we develop a high-sensitivity and rapid-response fiber-optic modal interferometer (FMI) to operando probe the growth dynamics of PDA nanocoating at the solid-liquid interface. The proposed FMI was treated with HF corrosion to enhance the surface evanescent field, thereby improving the surface refractive index sensitivity. Thus, the FMI successfully monitored the adhesion behavior of the polydopamine coating on the surface of the optical fiber and the subsequent adsorption of biomolecules. Through further analysis of surface evanescent wave field, a model was established to correlate FMI's interference spectra with PDA nanocoating's thickness. The accuracy of these results was validated through multiple ex situ characterization and spectroscopic techniques. Finally, the fiber-optic modal interferometer successfully revealed growth kinetic characteristics of the PDA coating induced by CuSO4/H2O2 under diverse operational conditions. This work may advance the evolution of surface-sensitive measurement technologies and surface phenolic chemistry.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"60 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036046","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 Dual-Enhancement Fiber-Optic Photoacoustic Spectroscopy Sensor Based on a Spherical-Cylindrical Coupled Resonator with an Integrated Multipass Cell for Sub-ppb C2H2 Detection. 基于球-柱耦合谐振腔集成多通单元的双增强光纤光声光谱传感器用于亚ppb C2H2检测。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-12 DOI: 10.1021/acs.analchem.5c04171
Guojie Wu,Yuchen Guan,Jing Jiang,Jiawei Xing,Zhenfeng Gong
{"title":"A Dual-Enhancement Fiber-Optic Photoacoustic Spectroscopy Sensor Based on a Spherical-Cylindrical Coupled Resonator with an Integrated Multipass Cell for Sub-ppb C2H2 Detection.","authors":"Guojie Wu,Yuchen Guan,Jing Jiang,Jiawei Xing,Zhenfeng Gong","doi":"10.1021/acs.analchem.5c04171","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04171","url":null,"abstract":"Although conventional spherical resonators are effective for photoacoustic spectroscopy (PAS), their sensitivities are fundamentally limited because the required detection apertures disrupt the optimal acoustic resonance. To address this limitation, this work presents a novel dual-enhancement fiber-optic PAS sensor that integrates a multipass cell (MPC) within a novel spherical-cylindrical (SC) coupled resonator for ultrahigh-sensitivity gas detection. The coupled resonator design is engineered to resolve the aperture conflict by incorporating a cylindrical waveguide, allowing noninvasive photoacoustic signal detection, yielding a 1.72-fold acoustic enhancement. Simultaneously, the optical enhancement is realized by integrating a two-mirror MPC into the coupled cavity, which extends the effective optical path length and enhances the photoacoustic signal by a factor of over 15. Together, these dual enhancements enable a 26-fold overall sensitivity improvement compared with conventional spherical resonator-based PAS systems. Consequently, the system achieves 223-parts-per-trillion (ppt) detection for C2H2, with a normalized noise equivalent absorption coefficient as low as 9.8 × 10-10 cm-1 W/Hz1/2. To the best of our knowledge, this performance represents the highest sensitivity and lowest detection limit reported to date for a spherical resonator-based PAS sensor. This work resolves the inherent design trade-off in spherical resonators between structural integrity and detection sensitivity. The proposed dual-enhancement fiber-optic PAS, featuring a compact, all-optical, and robust design, provides a powerful solution for ultrasensitive gas detection in complex or harsh environments, holding significant promise for broad engineering and practical applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036044","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 Structure-Guided Bifunctional Aptamer Mitigates Pseudomonas aeruginosa Virulence and Biofilms by Disrupting las and rhl Quorum Sensing Systems. 一种结构引导的双功能适体通过破坏las和rhl群体感应系统减轻铜绿假单胞菌的毒力和生物膜。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-12 DOI: 10.1021/acs.analchem.5c03245
Kuaile Wu,Yalin Mo,Mengxia Duan,Yan Zheng,Yuting Chang,Man Ding,Zhouping Wang,Shijia Wu,Nuo Duan
{"title":"A Structure-Guided Bifunctional Aptamer Mitigates Pseudomonas aeruginosa Virulence and Biofilms by Disrupting las and rhl Quorum Sensing Systems.","authors":"Kuaile Wu,Yalin Mo,Mengxia Duan,Yan Zheng,Yuting Chang,Man Ding,Zhouping Wang,Shijia Wu,Nuo Duan","doi":"10.1021/acs.analchem.5c03245","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03245","url":null,"abstract":"Quorum sensing (QS) is a microbial communication system that mediates the virulence factor synthesis and biofilm formation through signaling molecules. QS-targeted antivirulence strategies have emerged as a new approach to avoiding antibiotic resistance by weakening bacterial pathogenicity instead of directly killing bacteria, thereby reducing the selection pressure caused by traditional antibiotics. However, the molecular mechanisms that disrupt QS by blocking the binding of signaling molecules to receptor proteins remain elusive. Here, we engineered a bifunctional aptamer Cb-2 targeting the QS system of Pseudomonas aeruginosa─a canonical QS model organism─through structure-guided rational design integrating molecular docking with progressive truncation and sequence optimization. This aptamer specifically targeted both 3O-C12-HSL (the las system signal molecule) and C4-HSL (the rhl system signal molecule), achieving a dual blockade of QS cascade signaling. The intervention resulted in significant suppression of environmental virulence determinants (51.76% inhibition of rhamnolipid synthesis; 66.28% reduction in pyocyanin production) coupled with 74.46% attenuation of biofilm formation. This aptamer-targeted intervention strategy on the QS system exhibits significant potential for developing low environmental toxicity and highly targeted antimicrobial alternatives.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"35 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036047","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
Amplification by Polysaccharides for the Electrochemical Detection of Trypsin Activity. 多糖扩增法电化学检测胰蛋白酶活性。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-12 DOI: 10.1021/acs.analchem.5c04170
Junpeng Lv,Jingjing Xu,Yiting Chen,Wenqi Tang,Wenhui Xu,Mengge Wang,Xiyao Zhang,Ziluan Zhu,Songmin Chen,Qiong Hu,Li Niu
{"title":"Amplification by Polysaccharides for the Electrochemical Detection of Trypsin Activity.","authors":"Junpeng Lv,Jingjing Xu,Yiting Chen,Wenqi Tang,Wenhui Xu,Mengge Wang,Xiyao Zhang,Ziluan Zhu,Songmin Chen,Qiong Hu,Li Niu","doi":"10.1021/acs.analchem.5c04170","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04170","url":null,"abstract":"Although polysaccharides are ubiquitous in nature, biodegradable, and cheap, there is no report illustrating their use as functional materials for signal amplification in the biosensing of enzyme activities. Herein, we report the development of a polysaccharide-amplified electrochemical biosensor for the highly sensitive detection of trypsin activity. The substrate peptides without carboxyl sites are attached to the electrode surface via the N-terminus. Such that, the tryptic cleavage of the peptide layer gives rise to a free carboxyl site at the C-terminus of each truncated fragment, and the carboxyl-carrying polysaccharide chains are then recruited via the carboxylate-Zr(IV)-carboxylate linkage, followed by the decoration of redox labels via the cross-linking between the cis-diol sites of polysaccharide chains and the phenylboronic acid group. Through boronate cross-linking, each polysaccharide chain can be decorated with hundreds of redox labels, leading to the significantly amplified electrochemical detection of trypsin activity. The polysaccharide-based signal amplification is advantageous due to its simple operation, low cost, and mild reaction conditions. With alginic acid as the proof-of-concept polysaccharide, a detection limit of 103.5 μU/mL (∼0.41 ng/mL) has been obtained for trypsin detection. The cleavage-based recognition enabled the selective discrimination of trypsin against other proteases and proteins. In addition, the potential use of electrochemical biosensors in inhibitor screening, together with the interrogation of trypsin activity in urine samples, has been validated. Collectively, the results clearly show that the polysaccharide-amplified electrochemical biosensor is highly applicable to the highly sensitive detection of trypsin activity.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"72 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036051","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
Aptamer-Based Molecule-Responsive SERS System for Highly Efficient Detection of Cocaine. 基于适配体的分子响应SERS系统高效检测可卡因。
IF 7.4 1区 化学
Analytical Chemistry Pub Date : 2025-09-11 DOI: 10.1021/acs.analchem.5c03632
Tingting Xiao,Weiqiang Wang,Lingyi Zhao,Jian Xie,Weiping Cai
{"title":"Aptamer-Based Molecule-Responsive SERS System for Highly Efficient Detection of Cocaine.","authors":"Tingting Xiao,Weiqiang Wang,Lingyi Zhao,Jian Xie,Weiping Cai","doi":"10.1021/acs.analchem.5c03632","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03632","url":null,"abstract":"Illicit drug abuse has brought big challenges to public health, because it has caused severe damage to the human central nervous system. The development of a rapid, quantified, and on-site detection of illicit drugs is of key importance for the control of drug abuse. However, it remains challenging due to biological sample interference and difficulties in achieving specific recognition of the drug molecule. Here, we report a molecule-responsive two-component surface-enhanced Raman scattering (SERS) platform for the capture and detection of illicit drugs. Under optimized conditions, the system demonstrates a linear response to cocaine concentrations ranging from 1 ppb to 10 ppm (R2 > 0.99), with an ultralow detection limit of 1.5 ppb. Successful application in spiked bovine serum validates the method's robustness against complex biological matrices. This work establishes a novel paradigm for detecting trace-level illicit drugs with significant forensic potential. The design principle might be applied to other chemical detection.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"106 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145036052","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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