Analytical Chemistry最新文献

{"title":"Cocktail Chemical Labeling for In-Depth Surfaceome Profiling of Bone-Marrow-Derived Dendritic Cells","authors":"Shiming Sun, Siyang Liu, Tao Deng, Yudi Hu, Rong Yang, Jie P. Li, Yun Ge","doi":"10.1021/acs.analchem.5c02734","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02734","url":null,"abstract":"Cell surface proteins (CSPs) are crucial identifiers for cell types and states, especially in dendritic cells (DCs). Current proteomic methods for profiling CSPs are limited by their hydrophobic nature and low abundance, which often require genetic or cell surface engineering and exhibit biased and insufficient labeling efficiency. Herein, we report [Ru(bpy)₃]Cl₂ (Ru) for effective biotinylation on the cell surfaceome via a simple “mix and lighten” method. The versatile photoredox pathways of Ru are leveraged using a probe cocktail of biotin-phenol and biotin-hydrazide for improved substrate coverage. The “cocktail” labeling strategy results in reproducible identification of up to 733 plasma membrane proteins on HeLa cells and is further applied to map dynamic changes in the surfaceome during the differentiation of primary bone-marrow-derived dendritic cells, which demonstrates a user-friendly and deep-surfaceome-coverage tool for profiling dynamic changes in primary cells, with potential implications for cell identities, functional states, and novel drug targets.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"12 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216209","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}

{"title":"One Assay, Nine Targets: Advancing Viral Surveillance with Multiplex RT-ddPCR.","authors":"Anastasia Zafeiriadou,Georgia Georgakopoulou,Foteini Pitaouli,Nikolaos Thomaidis,Athina Markou","doi":"10.1021/acs.analchem.5c04372","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04372","url":null,"abstract":"Viral infections continue to pose a major global health challenge, driven by factors such as population growth, migration, and environmental change, all of which contribute to the emergence and reemergence of infectious viruses. Advances in technology now enable the detection of multiple targets from a limited sample volume; however, few studies have fully leveraged these capabilities. In this study, we developed and analytically validated a highly sensitive and specific 9-plex one-step RT-ddPCR assay for the detection of high-risk viruses, including SARS-CoV-2 (N1 and N2 genes), Influenza A and B, Respiratory Syncytial Virus, Hepatitis A and E, along with both endogenous and exogenous controls. Initial validation was conducted using synthetic DNA, followed by application to 38 wastewater samples─complex and heterogeneous matrices that often harbor multiple viral targets. The assay demonstrated excellent analytical performance in terms of sensitivity, linearity, specificity, and reproducibility with detection limits ranging from 1.4 to 2.9 copies/μL depending on the viral target. A direct comparison with singleplex ddPCR assays revealed high concordance (Mann-Whitney test, p > 0.1), indicating no statistically significant differences and highlighting the efficiency of the multiplex format. To the best of our knowledge, this is the first study to simultaneously quantify nine targets in a single RT-ddPCR reaction. The developed assay shows a strong potential for application across various sample types, including wastewater.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"214 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209199","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}

{"title":"Multi-Path High Electrochemiluminescence Activation Induced by SnO2/g-C3N4 Heterojunction for Ultrasensitive Bioanalysis Using SDA-Mediated Reticular DNA Structure as Signal Amplifier.","authors":"Yuxin Dai,Jinli Yang,Zhigang Yu,Huijun Wang,Xinya Jiang,Ruo Yuan,Haijun Wang","doi":"10.1021/acs.analchem.5c04598","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04598","url":null,"abstract":"Here, an ultrasensitive electrochemiluminescence (ECL) biosensor for miRNA-222 detection was fabricated using a heterojunction nanomaterial composed of stannic oxide decorated graphitic carbon nitride (SnO2/g-C3N4) as an efficient emitter and strand displacement amplification (SDA) mediated reticular 3D DNA structure for dual-output signal amplification. The construction of the SnO2/g-C3N4 heterojunction could efficiently improve the ECL performance through multiple paths. First, it could drive the high-energy electrons in g-C3N4 to migrate the SnO2 conduction band, preventing the g-C3N4 conduction band from accumulating excessive electrons and thereby suppressing material passivation under high-potential conditions. Moreover, the Sn2+/Sn4+ redox pair could provide additional charge transport channels, accelerating electron transfer and significantly enhancing the ECL emission efficiency. Meanwhile, SnO2 could catalyze the decomposition of the coreactant H2O2, promoting the production of hydroxyl radicals (OH•) and further enhancing the ECL intensity of the material. Leveraging the synergistic effects of improved electron transfer and radical generation, the ECL intensity of the SnO2/g-C3N4 heterojunction exhibited 6 times enhancement in comparison with pure g-C3N4. Then, a simple and efficient SDA reaction was employed to construct a reticular 3D DNA structure for signal amplification. This 3D DNA structure functioned as an ideal molecular scaffold with high loading capacity, and excellent structural stability could provide abundant Nb.BbvCI restriction enzyme cleavage sites, enabling the effective release of a large amount of dual-output DNA, significantly improving signal amplification efficiency and detection accuracy. Finally, the proposed biosensor exhibited excellent detection performance, achieving a sensitive detection limit for miRNA-222 as low as 41.3 aM.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"10 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209203","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}

{"title":"A Benign Protocol for the Simultaneously Specific Extraction of Acidic and Basic Pollutants in Environmental Samples under the Assistance of Electric Field.","authors":"Lingxin Zheng,Yan-Yun Li,Baomin Liu,Xiaojia Huang","doi":"10.1021/acs.analchem.5c05335","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05335","url":null,"abstract":"Simultaneously specific extraction of acidic and basic organic pollutants (A&BOPs) is significant in the enhancement of analytical efficiency but is challenging due to their strong and opposite polarity. In the current study, a benign protocol was proposed for the simultaneously selective capture of A&BOPs with the assistance of electric field. Selecting 4-nitrophenol and 2,4-dinitroaniline as the model templates of acidic and basic compounds, respectively, two molecularly imprinted monolith (MIM)-based microelectrodes (MEs) were in situ synthesized and acted as the anode and cathode of the electro-assisted solid-phase microextraction (EA/SPME) technique, respectively. Results revealed that the application of an electric field during the extraction procedure significantly improved the specific recognition capability toward templates and their structural analogues. For phenols, the imprinted factors (α) were increased from 1.37 to 1.45 (absence of electric field) to 2.76-2.92 (presence of electric field) and enhanced from 1.47 to 1.69 to 2.35-2.85 for anilines. Studies about extraction behaviors revealed that the specific recognition of imprinting materials and electric field force co-contributed to the simultaneously selective capture of phenols and anilines. Under the beneficial extraction parameters, the practicality of MIM@MEs-EA/SPME was well demonstrated by simultaneously selective extraction of trace phenols and anilines in various environmental water and soil samples prior to chromatographic analysis. The present work not only supplies a feasible strategy for the simultaneously and effectively specific extraction of A&BOPs but also expands the application scopes of EA/SPME and MIM.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"18 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209204","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}

{"title":"PLANTA Protocol for the Direct Detection and Identification of Bioactive Compounds in Complex Mixtures via Combined NMR-HPTLC-Based Heterocovariance.","authors":"Vaios Amountzias,Evagelos Gikas,Nektarios Aligiannis","doi":"10.1021/acs.analchem.5c02192","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02192","url":null,"abstract":"The assignment of bioactivity to compounds within complex natural product (NPs) mixtures remains a significant challenge in NPs research. The present research introduces a comprehensive protocol, named \"PLANTA (PhytochemicaL Analysis for NaTural bioActives)\" protocol, for the detection and identification of bioactive compounds in complex natural extracts prior to isolation combining the NMR-HeteroCovariance Approach (NMR-HetCA), high-performance thin-layer chromatography (HPTLC), and chemometric techniques. This study emphasizes two novel components: STOCSY-guided targeted spectral depletion, adapted to resolve overlapping NMR signals in complex matrices, improve minor component detection, and facilitate identification through NMR databases, as well as a new SHY variant termed SH-SCY (Statistical Heterocovariance - SpectroChromatographY), a new cross-correlation method linking orthogonal datasets by identifying the corresponding HPTLC spot from a single NMR peak and reconstructing of the 1H NMR spectrum from a specific HPTLC spot, enhancing dereplication confidence. In this proof-of-concept study, an artificial extract (ArtExtr) composed of 59 standard compounds was evaluated for the detection of compounds active against the free radical 2,2-diphenyl-1-picrylhydrazyl (DPPH). Statistical approaches were applied to the spectral, chromatographic, and bioactivity data to identify the highly correlated bioactive compounds. The PLANTA protocol achieved an 89.5% detection rate of active metabolites and 73.7% correct identification of them. The integration of NMR and HPTLC with HetCA provides a robust and sensitive strategy for preisolation identification of bioactive constituents. This methodology addresses core challenges in metabolite profiling of complex mixtures and offers a streamlined, reproducible workflow for natural product dereplication and discovery.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"98 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209205","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}

{"title":"Manipulation of Electrochemical Enantioselective Sensing of Chiral Metal Organic Frameworks Using the Charge Reconstruction Strategy.","authors":"Xing Yang,Yongqi Liu,Mei Yuan,Ke Chu","doi":"10.1021/acs.analchem.5c04446","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04446","url":null,"abstract":"The surface charge state has a significant effect on the process of chiral recognition. Charged surfaces can selectively adsorb specific chiral molecules through electrostatic interactions. Herein, the surface charge state of coordination polymer particles (CPPs) was transformed from negative to positive by changing the dosage of acetic acid. By combination of the chiral properties of zirconium-based metal-organic frameworks (L-PCN-224) with the surface advantages of oppositely charged CPP-1 and CPP-5 (CPP-1@L-PCN-224 and CPP-5@L-PCN-224), a chiral composite material with oppositely charged surfaces has been constructed. Systematic studies indicate that the polarity of surface charges under varying pH conditions significantly influences the selective adsorption of tryptophan (Trp) enantiomers. Our findings reveal a clear structure-property relationship between the charge polarity and chiral recognition performance in chiral metal-organic frameworks (CMOFs), offering an alternative approach to traditional chiral site-dependent materials. This study reveals the correlation between the altered charge polarity of CMOFs and their chiral recognition properties, offering an alternative to conventional materials. This study focuses on the transformation patterns of supramolecular interactions driven by charge alterations in materials under specific pH conditions. While grounded in conventional paradigms, it elucidates the role of charge polarity in determining dominant interaction types, offering novel insights into traditional chiral recognition.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"124 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203674","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}

{"title":"Self-Assembled Plasmonic Magnifier: A New Platform for Ultra-Sensitive Detection of Respiratory Viruses Using Surface-Enhanced Raman Spectroscopy.","authors":"Lixin Guo,Qiuying Wang,Yaowen Xing,Xiaojiao Zhao,Rongheng Ma,Danping Liu,Peng Gao,Yang Li","doi":"10.1021/acs.analchem.5c02722","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02722","url":null,"abstract":"Accurate and sensitive pathogen detection is critical for the prevention and control of respiratory viral infections, which pose significant threats to global health, particularly for vulnerable populations such as children, the elderly, and immunocompromised individuals. Here, we present a novel detection platform, Surface-Enhanced Raman Scattering combined with Artificial Intelligence (SERS-AI). At the core of this platform lies the independently developed self-assembled plasmonic magnifier (SPM), an enhanced substrate. Unlike traditional SERS substrates that rely on random aggregation or prefabricated nanostructures, this platform employs a virus-triggered self-assembly mechanism. Through the electrostatic attraction of C12 DNA molecules and the aggregation regulation of calcium ions, the self-assembled plasmonic magnifier (SPM) can significantly increase the probability of forming highly localized plasmonic \"hotspots\" near viral particles. This virus-associated hotspot formation strategy, which enhances the correlation between hotspot distribution and viral particles, significantly improves the specificity, intensity, and reproducibility of signals. Integrating surface-enhanced Raman spectroscopy (SERS) with artificial intelligence (AI) technology, the platform enables rapid, accurate, and label-free identification and quantitative analysis of respiratory viruses. The platform demonstrated exceptional sensitivity and reproducibility in detecting respiratory syncytial virus, human adenovirus type 5, influenza B virus, and H1N1 virus, with unique SERS fingerprints showing strong linear correlations with viral concentrations. The AI-driven spectral analysis allowed accurate differentiation of these viruses in serum and saliva samples, achieving detection within 2 min. Detection limits reached as low as 5 × 10-5 copies/mL demonstrating robustness and reliability even in complex biological matrices. This SERS-AI-SPM platform represents a significant breakthrough in SERS technology by integrating advanced nanomaterial engineering with AI-powered data analysis. Its rapid, sensitive, and reliable performance underscores its transformative potential in clinical diagnostics, large-scale epidemic prevention, and personalized medicine. This innovation provides a powerful tool for real-time infectious disease monitoring and public health management.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"76 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203681","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}

{"title":"Developing Quinacridone-Based Long Fluorescent Lifetime Probes for Cell Membrane Heterogeneity Imaging","authors":"Tong Wu, Yifan Liu, Fei Yuan, Zhiyang An, Xiaoling Zhang, Jing Jing","doi":"10.1021/acs.analchem.5c03649","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03649","url":null,"abstract":"The nonuniform distribution of lipids and proteins in phospholipid bilayers forms distinct microdomains, leading to the structural and functional heterogeneity of cell membranes. Fluorescence lifetime imaging (FLIM) provides microenvironment-sensitive readouts that are independent of local fluorophore concentration. Conventional fluorescent probes for membrane microdomain imaging are limited by short fluorescence lifetimes (<6 ns), which may overlap with endogenous signals and hinder precise microenvironment discrimination. To overcome this limitation, we have designed and synthesized a series of polarity-sensitive fluorescent probes with exceptionally long lifetimes to resolve membrane heterogeneity. The optimized probe CMFL-QASAG (including CQSC6, CQSC8, and CQSC10) exhibits an unprecedented lifetime shift (Δτ ≈ 18 ns) linearly responding to membrane polarity changes and effectively decoupling from cellular autofluorescence. Cholesterol depletion experiments demonstrated a robust correlation between CMFL-QASAG’s extended lifetime and membrane polarity variations in glioma cells. Furthermore, we observed dynamic changes in membrane polarity during cell migration, enabling imaging analysis and tracking of heterogeneous functional microregions on the cell membrane surface.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"69 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209890","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}

{"title":"Dual-Trap “Brick” Miniature Mass Spectrometer with Enhanced Sensitivity and Fragmentation Capabilities","authors":"Ronghui Ma, Yongguang Han, Ting Jiang, Dayu Li, Yanbing Zhai, Wei Xu","doi":"10.1021/acs.analchem.5c04683","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04683","url":null,"abstract":"Although the miniaturization of mass spectrometry (MS) frequently compromises analytical performance due to size and power limitations, the direct on-site analysis of complex samples requires a miniature mass spectrometer (mini-MS) to have enhanced instrument capabilities. To resolve this challenge, we have developed our “Brick” mini-MS into a next-generation system incorporating a differential-pressure dual-trap configuration. Each trap functions at distinct pressures, enabling parallel and optimized operations: ion accumulation/cooling and dissociation at higher pressures, in conjunction with ion isolation and MS analysis at lower pressure. Efficient ion transfer between the two traps enables parallel ion manipulation and diverse fragmentation modes. The parallel ion accumulation mode boosted the sensitivity of the miniature instrument by ∼20-fold, down to 50 pg/mL. In addition to conventional in-trap collision induced dissociation (CID), transfer dissociation during the ion accelerating and shuttling process and high-pressure collisional dissociation (HpCD) in a higher-pressure trap were also investigated. The results demonstrate that HpCD can generate more extensive ion fragments, which are typically observed in beam-type collisional activation dissociation methods. This study significantly advances the capabilities of mini-MS for high-performance, field-deployable analytical applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"94 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209894","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}

{"title":"Elucidating the Correlation Between Nanozyme-Substrate Binding Constants and Catalytic Efficiency by Affinity Capillary Electrophoresis.","authors":"Yuxin Wu,Tong Xu,Xin Qian,Zhining Xia,Min Wang","doi":"10.1021/acs.analchem.5c03216","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03216","url":null,"abstract":"The correlation between the binding constants of nanozymes with their substrates and the catalytic efficiency of these nanozymes was investigated for the first time by using affinity capillary electrophoresis (ACE). As a demonstration, two types of oxidase-like nanoceria-based nanozymes (CeO2@PAA (PAA, poly(acrylic acid)) and CeO2@PEI (PEI, polyethylenimine)) with different surface charges were employed as models, and partially filled affinity capillary electrophoresis (PFACE) was chosen for determining the binding constants (Kb) between these nanozymes and their substrate 3,3',5,5'-tetramethylbenzidine (TMB). In PFACE, by variation of the filling length of the nanozyme in the capillary column, Kb was calculated to be 152.23 and 117.74 L/mol for CeO2@PAA and CeO2@PEI, respectively. Moreover, with increasing concentration of the effector F-, the Kb values between CeO2@PEI and TMB exhibited a linear increase. Interestingly, by exploring the relationship between Kb and the catalytic kinetic parameters of the nanozyme, a good linear correlation between Kb and the catalytic efficiency (kcat/Km) (r = 0.909) was observed. This work provides a new strategy for studying the binding interaction between nanozymes and their substrates, thereby offering insights into the elucidation of the catalytic performance of nanozymes through the understanding of the binding process.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203643","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}