Analytical Chemistry最新文献_第2页

Back Isomerization Kinetics of Molecular Photoswitches: Complementary Insights from Liquid Chromatography and Ion Mobility Measurements

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-25 DOI: 10.1021/acs.analchem.5c00560

Thomas Robert, Gwendal Henrard, Benjamin Tassignon, Ari Serez, Julien De Winter, Philippe Dugourd, Jérôme Cornil, Fabien Chirot, Pascal Gerbaux

引用次数: 0

Monitoring Amphetamine and Methamphetamine Mixtures Based on Deep Learning Involves Colorimetric Sensing

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-25 DOI: 10.1021/acs.analchem.5c00915

Sifan Cao, Yuan Liu, Yuwan Du, Wenlong Li, Xincun Dou

{"title":"Monitoring Amphetamine and Methamphetamine Mixtures Based on Deep Learning Involves Colorimetric Sensing","authors":"Sifan Cao, Yuan Liu, Yuwan Du, Wenlong Li, Xincun Dou","doi":"10.1021/acs.analchem.5c00915","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00915","url":null,"abstract":"Precise recognition and discrimination of highly similar analytes (either in structure or property) with distinguishable sensing responses are challenging but significant in the practical application of drug seizing, food additive inspection, environmental monitoring, etc. Here, a colorimetric differentiation strategy was proposed by modulating the probe structure to influence the aggregate behaviors of the reaction products; thus, amphetamine (AMP) and methamphetamine (MA) with the sole structural difference of a methyl group were successfully discriminated. Specifically, upon recognition of the furan ring-opening reaction, the probe was screened out from a series of furan-based probes with different electron-withdrawing groups, which further facilitated the aggregate state difference of reaction products and then amplified the difference in colorimetric responses. In addition, the probe-embedded porous polymer substrate was fabricated to accelerate the response for trace AMP and MA, and the judgment of doping ratios of AMP and MA in the mixtures was realized for the first time by further combining with the self-developed Drugs Analyst as well as deep learning algorithms. Hence, we envisage that this structural-modulation-enabled colorimetric differentiation strategy will shine light on the multianalyte discrimination from aspects of optical sensing development and multidisciplinary fusion.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"68 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872937","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 Characterization of IgG2 Disulfide Isoforms Using Native Cation Exchange Chromatography-Mass Spectrometry and Peptide Mapping

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.5c00578

Yann Leblanc, Nicolas Cauquil, Valérie Pasteau, Fanny Duguet, Stéphane Bahraoui, Magali André, Emmanuel Nony

{"title":"Comprehensive Characterization of IgG2 Disulfide Isoforms Using Native Cation Exchange Chromatography-Mass Spectrometry and Peptide Mapping","authors":"Yann Leblanc, Nicolas Cauquil, Valérie Pasteau, Fanny Duguet, Stéphane Bahraoui, Magali André, Emmanuel Nony","doi":"10.1021/acs.analchem.5c00578","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00578","url":null,"abstract":"The IgG2 antibody subclass is unique in displaying complex disulfide bond connectivity in its hinge region, resulting in three distinct isoforms, namely, A, A/B, and B. Structural elucidation of these isoforms by liquid chromatography–mass spectrometry (LC-MS) is challenging and usually involves denaturing methodologies, such as reversed-phase chromatography or capillary electrophoresis. In this study, we developed a native cation exchange chromatography–mass spectrometry (CEX-MS) method using volatile salts to separate IgG2 disulfide isoforms. This approach was combined with a middle-up strategy focusing on F(ab′)2 fragments of the antibody, where IgG2 disulfide bond rearrangements are localized. By targeting F(ab′)2, this methodology achieves optimal chromatographic separation and high-quality MS spectra while excluding Fc-related heterogeneity. The elution order of IgG2 disulfide isoforms was determined by CEX-MS through redox treatment and site-directed mutagenesis. For the first time, native CEX-MS enabled the characterization of an IgG2 mutant designed to favor agonistic activity through a pseudoisoform B structure stabilized by noncovalent interactions between subunits. To further decipher hinge region disulfide linkage, we also developed an optimized nonreduced peptide mapping that limits missed cleavages. Peptide identification was enhanced by an isotope envelope confidence score, which compares theoretical and experimental isotope distributions. This scoring allowed for confident identification of complex hinge-related peptides, overcoming limitations of conventional peptide mapping methods for the elucidation of IgG2 interchain patterns.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"73 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872658","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

Low-background Near-infrared Fluorescent Probe for Real-time Monitoring of β-Glucuronidase Activity in Inflammation and Therapy

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.5c00658

Dianfeng Dai, Zhimin Zhang, Mo Ma, Chen Zhao, Jingkang Li, Siqi Zhang, Pinyi Ma, Qiong Wu, Daqian Song

{"title":"Low-background Near-infrared Fluorescent Probe for Real-time Monitoring of β-Glucuronidase Activity in Inflammation and Therapy","authors":"Dianfeng Dai, Zhimin Zhang, Mo Ma, Chen Zhao, Jingkang Li, Siqi Zhang, Pinyi Ma, Qiong Wu, Daqian Song","doi":"10.1021/acs.analchem.5c00658","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00658","url":null,"abstract":"β-Glucuronidase (GUS) is an acidic hydrolase enzyme overexpressed in various inflammatory diseases, making it a promising biomarker for inflammation. However, current tools for real-time, in situ imaging of GUS activity are hindered by background interference, which reduces their effectiveness in dynamic biological environments. To address this challenge, we developed Ox-GUS, a GUS-specific fluorescent probe with a unique molecular design featuring a disrupted conjugated structure. This design provided Ox-GUS with near-zero background optical properties, a significantly enhanced signal-to-noise ratio, and a highly sensitive detection ability. The probe demonstrated a fluorescence enhancement of up to 400 folds in response to GUS activity, with a detection limit as low as 0.0035 U/mL. We successfully employed Ox-GUS to visualize GUS activity in real-time in mouse models of rheumatoid arthritis, autoimmune hepatitis, and inflammatory bowel disease, and effectively monitored therapeutic responses. This study highlights the potential of Ox-GUS as a robust tool for advancing research on GUS-related inflammatory mechanisms and for early diagnosis and treatment monitoring of inflammatory diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"69 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872838","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 Orientational Dynamics of Magnetic Nanoparticles in Opaque Samples Using Near-Infrared Magnetic Linear Birefringence

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.4c06781

Masayori Suwa, Maika Higuchi, Misato Takatsu, Yukihiro Okamoto, Satoshi Tsukahara

{"title":"Probing Orientational Dynamics of Magnetic Nanoparticles in Opaque Samples Using Near-Infrared Magnetic Linear Birefringence","authors":"Masayori Suwa, Maika Higuchi, Misato Takatsu, Yukihiro Okamoto, Satoshi Tsukahara","doi":"10.1021/acs.analchem.4c06781","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06781","url":null,"abstract":"We demonstrated the advantage of magnetic linear birefringence (MLB) measurement for studying the orientation dynamics of magnetic nanoparticles (MNPs) in various environments. It is expected that MNPs will be utilized as active probes of nanoscale measurements, such as nanorheology and homogeneous bioassay. The optical anisotropy induced in MNP suspensions under an AC magnetic field, including MLB, reflects the physical rotation of the MNP itself. MLB is measurable with near-infrared light, which can reduce undesirable extinction due to the scattering or absorption by the sample suspension. In this study, we built an apparatus for precise MLB measurement by refurbishing the previous one to measure magnetic linear dichroism under an AC magnetic field and confirmed the relationship between the MLB signal and the orientation of MNP. Then, two systems that were opaque for visible light were examined to show the unique advantage of the MLB measurement of MNPs: (1) MLB measurement applied to the MNP suspension with a wide concentration range, and the effect of the interparticle interaction on the orientation dynamics could be detected from MLB frequency spectra. (2) Magneto-liposomes (ML), small vesicles containing MNPs, could be measured, and the frequency spectra could provide information on the condition of MNPs in ML. Furthermore, it was possible to detect the phase transition of the lipid bilayer from the gel to the liquid crystal phase.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"5 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866157","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 Selective Determination of Cysteine in Crops Employing a Novel Colorimetric and NIR-Emitting Ratiometric Fluorescent Probe along with a Smartphone-Assisted Portable Detection Device

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.4c07073

Xiaodong Chen, Chenglu Zhao, Sanxiu Yang, Yunfei Yang, Yuqing Wang, Rumeng Zhang, Kun Wang, Jing Qian, Lingliang Long

{"title":"In Situ Selective Determination of Cysteine in Crops Employing a Novel Colorimetric and NIR-Emitting Ratiometric Fluorescent Probe along with a Smartphone-Assisted Portable Detection Device","authors":"Xiaodong Chen, Chenglu Zhao, Sanxiu Yang, Yunfei Yang, Yuqing Wang, Rumeng Zhang, Kun Wang, Jing Qian, Lingliang Long","doi":"10.1021/acs.analchem.4c07073","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07073","url":null,"abstract":"Cysteine (Cys) is the first organic sulfur nutrient produced by crops. There is an urgent need to construct a reliable analytical method to quantitatively detect Cys in crops. Herein, a colorimetric and NIR-emitting ratiometric fluorescent probe for in situ quantitative detection of Cys in crops has been developed. The probe presented highly specific response to Cys over other biothiols including Hcy and GSH. The fluorescence ratios (I545/I655) exhibited a linearity with Cys concentration in the range of 0.113–300 μM, and the detection limit was measured to be 0.034 μM (S/N = 3). Importantly, the specific sensing reaction between the probe and Cys is achieved through a unique two-step recognition process. The probe was employed to detect Cys in living cells through fluorescence imaging. Additionally, alterations in Cys levels within Gynura cusimbua leaves, triggered by atmospheric H2S, have been monitored. Furthermore, the probe has been utilized to trace changes in the Cys concentration in G. cusimbua roots under external Cd stress. Notably, to facilitate in situ quantitative detection of Cys in crops, a smartphone-assisted portable detection device was made up. The probe and portable detection device were successfully employed for in situ quantitative detection of Cys in cabbage and apple.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"52 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866158","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

Phosphorothioate-Modified Hairpin G-Triplex Reporter-Assisted Split CRISPR/Cas12a-Powered Biosensor for “Turn-On” Fluorescent Detection of Nucleic Acid and Non-Nucleic Acid Targets

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.5c00140

Kai Shi, Wenjie Luo, Ying Cheng, Honglei Li, Liai Peng, Xiangrui Luo, Yu Hu, Jiaheng Zhang, Jiaxuan Chen

{"title":"Phosphorothioate-Modified Hairpin G-Triplex Reporter-Assisted Split CRISPR/Cas12a-Powered Biosensor for “Turn-On” Fluorescent Detection of Nucleic Acid and Non-Nucleic Acid Targets","authors":"Kai Shi, Wenjie Luo, Ying Cheng, Honglei Li, Liai Peng, Xiangrui Luo, Yu Hu, Jiaheng Zhang, Jiaxuan Chen","doi":"10.1021/acs.analchem.5c00140","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00140","url":null,"abstract":"CRISPR/Cas12a-powered biosensors with guanine (G)-rich sequence reporters (e.g., G-quadruplex and G-triplex) are widely used in detection applications due to their simplicity and sensitivity. However, when these biosensors are employed for molecular detection in complex samples, they may encounter difficulties such as high background signal and susceptibility to interference because of the “turn-off” signal output. Herein, we explore, for the first time, a set of phosphorothioate (ps)-modified G-quadruplex (G4) and G-triplex (G3) sequences that can bind with thioflavin T (ThT) in an active split CRISPR/Cas12a system (SCas12a) to generate a “turn-on” fluorescent signal. To apply this new phenomenon, we develop a universal SCas12a-powered biosensor for “turn-on” fluorescent detection of nucleic acid (miRNA-21) and non-nucleic acid (kanamycin) targets by using ps-modified hairpin G3 as a reporter (SCas12a/psHG3). Target recognition activates SCas12a’s trans-cleavage activity, leading to cleavage at the loop region of the psHG3 reporter. The released prelocked psG3 DNA binds ThT to produce a strong fluorescence signal. Without preamplification, this strategy can detect miRNA-21 with a detection limit of 100 fM. Moreover, the SCas12a/psHG3 system was further utilized for detecting kanamycin by incorporating its aptamers, enabling the detection of kanamycin at concentrations as low as 100 pM. This work is the first to develop a “turn-on” SCas12a/psHG3 system, showcasing its improved performance and wide range of applications in synthetic biology-based sensing technology.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"46 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866231","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

Enhanced “Off–On” Electrochemiluminescent Biosensor Based on a Multivalent Aptamer-Induced Spatial Confinement Strategy for Ultrasensitive Detection of Membrane Protein (PTK-7)

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.4c06828

Yinbo Ban, Lin Zhang, Fu Zhou, Ruonan Qiao, Ruifen Tian, Baojuan Wang, Yanping He, Guangfeng Wang

{"title":"Enhanced “Off–On” Electrochemiluminescent Biosensor Based on a Multivalent Aptamer-Induced Spatial Confinement Strategy for Ultrasensitive Detection of Membrane Protein (PTK-7)","authors":"Yinbo Ban, Lin Zhang, Fu Zhou, Ruonan Qiao, Ruifen Tian, Baojuan Wang, Yanping He, Guangfeng Wang","doi":"10.1021/acs.analchem.4c06828","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06828","url":null,"abstract":"“Off–on” electrochemiluminescence (ECL) techniques have garnered considerable interest in the biosensing field owing to its high sensitivity, low background signal, high signal-to-noise ratio, and avoidance of false-positive signals. However, a significant hurdle that prevents its further application is the lack of nontoxic, label-free, and easily synthesized ECL luminophores. In addition, achieving high quenching efficiency on these luminophores still requires strategy renewal. In this study, we propose novel Tb-DNA nanoparticles (NPs) as an emerging luminophore with low environmental risk and easy synthesis, which were synthesized in a facile coordination-driven approach. Taking advantage of the sequence programmability of these luminophores conferred by DNA molecules, we further construct an ultralow background “off–on” ECL platform by anchoring a multivalent aptamer on these nanoparticles, which facilitates close proximity with electron acceptors (e.g., dopamine (DA) oxidized by K2S2O8, DAOx) and enables efficient electron transfer between the excited state of Tb-DNA NPs and DAOx. Using the membrane protein protein tyrosine kinase-7 (PTK-7) as a sensing target, our “off–on” ECL strategy of spatially confined electron acceptors by multivalent aptamer-anchored Tb-DNA NPs displayed good detection performance, exhibiting a detection range of 90 to 106 cells/mL and a detection limit as low as a single-digit number of cells. This work not only puts forward novel Tb-DNA-based ECL luminophores but also proposes a multivalent aptamer-recognized acceptor strategy with high sensitivity, low background noise, and high specificity, which might hold great potential for ultrasensitive membrane protein detection.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"2 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872657","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

Miniaturization of Mass Spectrometry Systems: An Overview of Recent Advancements and a Perspective on Future Directions

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.5c01223

Xiaomin Fan, Bin Jiao, Xiaoyu Zhou, Wenpeng Zhang, Zheng Ouyang

{"title":"Miniaturization of Mass Spectrometry Systems: An Overview of Recent Advancements and a Perspective on Future Directions","authors":"Xiaomin Fan, Bin Jiao, Xiaoyu Zhou, Wenpeng Zhang, Zheng Ouyang","doi":"10.1021/acs.analchem.5c01223","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01223","url":null,"abstract":"The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.5c01223. Data regarding the miniature mass spectrometry systems (Table S-1) (PDF) Miniaturization\u0000of Mass Spectrometry Systems: An Overview\u0000of Recent Advancements and a Perspective on Future Directions 0 views 0 shares 0 downloads Electronic Supporting Information files are available without a subscription to ACS Web Editions.\u0000The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting\u0000Information. Files available from the ACS website may be downloaded for personal use only. Users are\u0000not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information\u0000from the ACS website, either in whole or in part, in either machine-readable form or any other form\u0000without permission from the American Chemical Society. For permission to reproduce, republish and\u0000redistribute this material, requesters must process their own requests via the RightsLink permission\u0000system. Information about how to use the RightsLink permission system can be found at\u0000http://pubs.acs.org/page/copyright/permissions.html.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"91 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866233","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

Quantitative Characterization of Modified Lignin Using Solid-State 13C NMR Spectroscopy

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-24 DOI: 10.1021/acs.analchem.5c01084

Haruka Sotome-Yukisada, Kentaro Hiratsuka, Keiichi Noguchi, Jun Ashida, Toshiyo Kato, Kazuhiro Shikinaka, Yasuyuki Matsushita, Yuichiro Otsuka, Yoichi Tominaga

引用次数: 0