Xiaojuan Yan, Sen Yang, Xinglun Kou, Tongxin Fu, Jiaqi Yang, Gang Zhao, Weiguang Ma
{"title":"Correction to “Optical-Feedback Cavity-Enhanced Raman Spectroscopy with Continuous Laser-to-Cavity Locking for Multigas Detection”","authors":"Xiaojuan Yan, Sen Yang, Xinglun Kou, Tongxin Fu, Jiaqi Yang, Gang Zhao, Weiguang Ma","doi":"10.1021/acs.analchem.5c03987","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03987","url":null,"abstract":"The power spectral density data in Figure 3 (published on page 11122) should be the measurement results of the transmission measurement system. Figure 3. Corrected Figure 3. Additionally, one textual modification is required: Original: “The locking technology has an obvious suppression effect on the low-frequency noise within 1 kHz.” Revised: “The locking technology has an obvious suppression effect on the low-frequency noise within 330 Hz.” This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"115 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145234969","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 Fully Integrated Wearable Microfluidic Electrochemical Sensor with Ultrasonic Connecting and Hot-Pressing Bonded Multilayer Structure for Sweat Biomarker Analysis","authors":"Guodong Liu, Xianyang Guan, Pingna Zhang, Qifeng Tan, Tianlong Li, Xin Jin, Huiqing Xu, Chaojiang Li, Jieliang Zhao","doi":"10.1021/acs.analchem.5c04641","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04641","url":null,"abstract":"Wearable microfluidic sweat sensors serve as critical devices for the continuous monitoring of human biomarkers. This research has developed a fully integrated wearable microfluidic electrochemical sensor (FIWMES) for noninvasive, continuous monitoring of glucose, Na<sup>+</sup>, K<sup>+</sup>, and Ca<sup>2+</sup> in human sweat. To address challenges including sample leakage, structure damage, and difficulties of multiple-biomarker detection, a hybrid bonding process that combines ultrasonic connecting and hot-pressing procedures is presented for structural integration of the FIWMES. The bonding process ensures high interfacial bonding strength (>65 N), excellent sealing performance (no leakage after 200 bends), and precise temperature control (<51 °C) inside the microfluidic chamber. By integrating the dendritic sweat-collecting module, microfluidic chamber, and 3D-arranged sensing units, the FIWMES can achieve efficient sweat capture, sample manipulation, and simultaneous biomarker detection. The glucose sensor exhibits a sensitivity of 6.4 μA/mM with strong anti-interference capability, while the Na<sup>+</sup>, K<sup>+</sup>, and Ca<sup>2+</sup> sensors display near-Nernstian responses with sensitivities of 65.3, 64.3, and 38.2 mV/decade, respectively. On-body trials confirm the practical wearability and its ability to accurately track dynamic metabolic changes, such as postprandial increases in sweat glucose and electrolyte variation under water deficiency. With its stability and monitoring capabilities, FIWMES offers a technical platform for the effective management of chronic diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"108 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235013","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}
Klaus Welters, Christian Thoben, Julius Schwieger, Alexander Nitschke, Tim Ostermeier, Stefan Zimmermann, Detlev Belder
{"title":"Fast Chemical Analysis of Droplets Unlocked by Ultra-Fast Ion Mobility Spectrometry","authors":"Klaus Welters, Christian Thoben, Julius Schwieger, Alexander Nitschke, Tim Ostermeier, Stefan Zimmermann, Detlev Belder","doi":"10.1021/acs.analchem.5c05025","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05025","url":null,"abstract":"This study presents the first coupling of high-throughput droplet microfluidics to an ultra-fast ion mobility spectrometer (IMS), providing a method for the label-free and comprehensive analysis of droplet contents at very high speeds. Building on the core strengths of IMS ─ compactness, simplicity, and cost-effectiveness ─ the added ability to capture full spectra at exceptionally short cycle times of less than 2 ms positions the technique as an exceptional platform for spectrometric analysis. The combination of a custom electrospray interface, a purpose-built monolithic fused-silica droplet generator chip, and an ultra-fast IMS enabled the chemical analysis of individual droplets in segmented flow at speeds of up to 120 Hz. The approach of droplet-based high-throughput ion mobility spectrometry (DHT-IMS) was also applied for reaction screening in nanoliter-sized droplets, exemplified by a hydrazone formation reaction between 5-methylisatin and phenylhydrazine.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"10 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235014","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":"IDSP-IA: Immunotriggered Double Stem-Loop Probe-Mediated Isothermal Amplification for Attomolar Protein Quantification.","authors":"Jiangyan Zhang,Yinuo Wang,Qing Li,Hailan Gao,Chunfang Wang,Tingting Cai,Yan Wang,Hui Wang,Zhengping Li,Yongqiang Cheng","doi":"10.1021/acs.analchem.5c04062","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04062","url":null,"abstract":"Ultrasensitive quantification of low-abundance proteins is critical for disease full-cycle management but remains a significant challenge. Herein, we present an immunotriggered double stem-loop probe-mediated isothermal amplification (IDSP-IA) assay for highly sensitive and specific protein detection. The IDSP-IA assay consists of three modular components: a monoclonal capture antibody (mAb1)-coated reaction tube for target capture, an aptamer-oligonucleotide switch (Apt-OS) for signal transduction, and a universal double stem-loop-mediated isothermal amplification module. After target protein capture and enrichment of mAb1-coated tubes, Apt-OS converts nonamplifiable protein signals to the nucleic acid triggers, initiating efficient exponential amplification. Benefiting from the modular design, the assay allows flexible adaptation to various proteins by simply replacing antibody/aptamer pairs while keeping amplification components unchanged. We have demonstrated that the IDSP-IA assay achieves a wide dynamic range (5 fg/mL to 50 pg/mL) with a limit of detection (LOD) of 1.3 fg/mL for α-fetoprotein (AFP) and 1.4 fg/mL for interleukin-6 (IL-6) detection without cross-reactivity from other common serum proteins. More importantly, clinical validation using human serum samples showed excellent correlation with routinely used electrochemiluminescence and chemiluminescence immunoassays. These advantages, including high specificity, ultrasensitivity, modular design, and universality, enable the IDSP-IA assay to provide a robust and flexible tool for accurate and attomolar protein biomarker quantification in diagnostic and biomedical settings.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"98 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229044","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":"Unsupervised Machine Learning for Differential Analysis in Proteomics","authors":"Guanyang Xu, Enhui Wu, Yuxiang Lin, Ling Lin, Liang Qiao","doi":"10.1021/acs.analchem.5c03117","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03117","url":null,"abstract":"Differential analysis in proteomics is pivotal for biomarker discovery and disease mechanism elucidation, yet traditional statistical methods are constrained by distributional assumptions and empirical fold change threshold dependencies. This study systematically evaluates 18 unsupervised anomaly detection machine learning (ML) algorithms against the established statistical frameworks for differential protein detection from proteomic data sets. Using <i>in silico</i> simulated data sets derived from experimental data, we enabled cross-algorithm comparability through a probability based transformation. Results demonstrated that ML methods, particularly the Minimum Covariance Determinant (MCD), outperformed statistical test in recall, precision, and accuracy, with superior robustness to intersample heterogeneity. Validation on real-world proteomic data further confirmed that the MCD-identified differentially expressed proteins comprehensively covered canonical pathways while uncovering novel tumor-associated functional biomolecules. This work establishes unsupervised ML methods as robust alternatives to traditional hypothesis-driven statistical approaches in proteomics differential analysis, offering enhanced reliability for precision medicine research.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"19 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235016","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}
Yan Pu, Qiong Zhang, Wenjie Zhou, Huiqing Li, Jinquan Liao, Yupeng Tian, Shengyu Shi, Yingcui Bu, Hongping Zhou
{"title":"A Highly Efficient Pyroptosis Activator for Three-Photon Fluorescence Imaging-Guided Phototherapy and Hypoxia Tumor Immunotherapy","authors":"Yan Pu, Qiong Zhang, Wenjie Zhou, Huiqing Li, Jinquan Liao, Yupeng Tian, Shengyu Shi, Yingcui Bu, Hongping Zhou","doi":"10.1021/acs.analchem.5c04817","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04817","url":null,"abstract":"Pyroptosis is a highly immunogenic form of programmed cell death capable of eliciting inflammation and enhancing antitumor immune responses. However, there remains a lack of effective visualization of pyroptosis processes and deep-penetrating organelle-targeted photosensitizers in cancer treatment strategies. Here, we develop two aggregation-induced emission (AIE) pyroptosis inducers (CM1-NIC@F127 and CM2-NIC@F127), which are found to proficiently generate reactive nitrogen species (RNS) under hypoxic tumor conditions. The visualization of cellular mitochondrial swelling and the formation of large vesicles throughout the pyroptosis process are achieved owing to their excellent three-photon fluorescence (3PF) properties. Mechanistically, the mitochondria experience dysfunction after phototherapy treatment because of their hypersensitivity to free radical active substances. Cleaved-caspase 1 activation is observed during pyroptosis, leading to the gasdermin D (GSDMD) cleavage fragment GSDMD-N and initiating an inflammatory response. CM1-NIC@F127 promotes dendritic cell (DC) maturation and cytotoxic T cell activation due to the enhanced immunogenic cell death (ICD) effect, leading to the inhibition of both primary and distant tumor growth. Thus, this study provides ideas and strategies for tumor immunotherapy mediated by RNS-induced pyroptosis that has a good therapeutic effect on tumors.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"53 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235020","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":"FePtCoNiCu High-Entropy Nanozymes Embedded in a Hydrogel Matrix as a Portable, Rapid, and Visual On-Site Biosensing Platform","authors":"Chaoyu Fan, , , Yimin Pan, , , Deshu Wu, , , Deshuai Yu, , , Hanqi Wang, , , Zhehao Han, , , Yonghua Tang*, , , Zhisen Zhang, , , Qiyu Zhang, , , Youhui Lin*, , and , Jie Zhang*, ","doi":"10.1021/acs.analchem.5c04893","DOIUrl":"10.1021/acs.analchem.5c04893","url":null,"abstract":"<p >High-entropy nanozymes (HEzymes) have garnered significant interest due to their multifunctional active sites and synergistic metal interactions, yet their applications in advanced biosensing, especially for portable on-site detection, remain underexplored. Herein, by integrating FePtCoNiCu HEzymes into a hydrogel matrix, we established aportable, cost-effective, and user-friendly system for on-site visual detection without complex instrumentation. Our HEzymes were facilely fabricated via a low-temperature oil-phase process and exhibit robust peroxidase-like (POD-like) activity through efficient conversion of H<sub>2</sub>O<sub>2</sub> to hydroxyl radicals. Density functional theory calculations indicate that strong electronic coupling among the metal components enhances catalytic efficiency by promoting charge transfer via d-orbital redistribution near the Fermi level. Leveraging these properties, we developed a colorimetric platform for rapid and sensitive detection of biothiols, acetylcholinesterase, and organophosphorus pesticides. Furthermore, by embedding HEzymes within an alginate hydrogel and integrating smartphone imaging, we further established a portable, rapid, and visual on-site biosensing platform. This approach expands the applicability of HEzymes in biosensing and medical diagnostics while offering new insights into their catalytic mechanisms and paving the way for next-generation biosensing technologies.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"97 40","pages":"22368–22379"},"PeriodicalIF":6.7,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229041","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}
Eirik Almklov Magnussen*, , , Boris Zimmermann, , , Simona Dzurendova, , , Ondrej Slany, , , Valeria Tafintseva, , , Kristian Hovde Liland, , , Kristin To̷ndel, , , Volha Shapaval, , and , Achim Kohler,
{"title":"Calibration for Quantitative Chemical Analysis in IR Microscopic Imaging","authors":"Eirik Almklov Magnussen*, , , Boris Zimmermann, , , Simona Dzurendova, , , Ondrej Slany, , , Valeria Tafintseva, , , Kristian Hovde Liland, , , Kristin To̷ndel, , , Volha Shapaval, , and , Achim Kohler, ","doi":"10.1021/acs.analchem.5c03049","DOIUrl":"10.1021/acs.analchem.5c03049","url":null,"abstract":"<p >Infrared spectroscopy of macroscopic samples can be calibrated against reference analysis, such as lipid profiles acquired by gas chromatography, and serve as a fast, low-cost, quantitative analytical method. Calibration of infrared microspectroscopic images against reference data is in general not feasible, and thus spatially resolved quantitative analysis from infrared spectral data has not been possible so far. In this work, we present a deep learning-based calibration transfer method to adapt regression models established for macroscopic infrared spectroscopic data to apply to microscopic pixel spectra of hyperspectral IR images. The calibration transfer is accomplished by transferring microspectroscopic infrared spectra to the domain of macroscopic spectra, which enables the use of models obtained for bulk measurements. This allows us to perform quantitative chemical analysis in the imaging domain based on infrared microspectroscopic measurements. We validate the suggested microcalibration approach on microspectroscopic data of oleaginous filamentous fungi, which is calibrated toward lipid profiles obtained by gas chromatography and measurements of glucosamine content to perform quantitative infrared microspectroscopy.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"97 40","pages":"21947–21955"},"PeriodicalIF":6.7,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.analchem.5c03049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229046","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Na Li,Jingui Chen,Yu Du,Dehao Jia,Hongying Jia,Dawei Fan,Qin Wei
{"title":"Co-CdO-Amplified Electrochemiluminescence of GSH-AuNCs Immobilized on Fe-MIL-88A for Ultrasensitive Immunosensing of Carbohydrate Antigen 15-3.","authors":"Na Li,Jingui Chen,Yu Du,Dehao Jia,Hongying Jia,Dawei Fan,Qin Wei","doi":"10.1021/acs.analchem.5c05119","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05119","url":null,"abstract":"Gold nanoclusters (AuNCs) protected by sulfhydryl ligands exhibit excellent optical properties and good biocompatibility. However, the inefficient charge transfer during redox reactions, stemming from free vibration and rotation of the ligands, limits their application in electrochemiluminescence (ECL). To address this, glutathione-protected AuNCs (GSH-AuNCs) were immobilized onto Fe-MIL-88A nanoparticles, serving as the ECL emitter. The GSH-AuNCs@Fe-MIL-88A composite effectively suppressed energy dissipation caused by ligand motion, while simultaneously enhancing charge transfer and reducing nonradiative decay pathways through structural stabilization. Furthermore, Co-doped CdO was employed as a co-reaction accelerator to promote the generation of radical intermediates from N,N-diisopropylethylamine, thereby amplifying the ECL signal. Leveraging this enhanced system, a highly sensitive ECL immunosensor was constructed for the detection of the glycan antigen CA15-3. This immunosensor demonstrated excellent stability, reproducibility, and selectivity. Meanwhile, it exhibited a wide linear range from 0.1 pM to 100 nM for CA15-3 detection, with an impressively low limit of detection of 0.02 pM (S/N = 3). This work provides a novel strategy for utilizing gold nanoclusters in ECL applications and can be readily extended to detect other disease biomarkers.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"8 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229035","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}
Peng-Kai Liu, Ting-Jia Gu, Shuling Xu, Alexander Nassar, Zicong Wang, Hung-Yu Chiang, Danqing Wang, Lingjun Li
{"title":"13-Plex DeAla Isobaric Reagents for High-Throughput Proteome Quantification","authors":"Peng-Kai Liu, Ting-Jia Gu, Shuling Xu, Alexander Nassar, Zicong Wang, Hung-Yu Chiang, Danqing Wang, Lingjun Li","doi":"10.1021/acs.analchem.5c03910","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03910","url":null,"abstract":"Isobaric labeling techniques are widely used in mass spectrometry-based quantitative proteomics to enable the simultaneous analysis of multiple samples. However, commercial isobaric tags are expensive due to complex synthesis and costly reagents, limiting their use in large-scale studies. Here, we introduce a novel, cost-effective diethylalanine-based isobaric reagent (DeAla), synthesized using diethylated alanine and β-alanine with <i>N</i>-hydroxysuccinimide. The DeAla tag offers several advantages, including improved peptide fragmentation, enhanced protein identification, and competitive pricing. We optimized labeling efficiency and collision energy parameters, demonstrating that DeAla-labeled peptides produce more backbone fragmentation ions and higher XCorr values compared to peptides labeled with <i>N</i>,<i>N</i>-dimethyl leucine (DiLeu) tags. By selectively incorporating stable isotopes, we expanded the multiplexing capacity to 13-plex without increasing structural complexity, achieving baseline resolution in Orbitrap MS/MS acquisition at 60k resolution. Comparative proteomic analyses of two cancer cell lines demonstrated that DeAla labeling outperformed DiLeu tags and showed comparable performance to label-free approaches in terms of protein and peptide identification. Additionally, DeAla provided accurate and reproducible quantification across a dynamic range with minimal technical variability. Overall, the 13-plex DeAla reagents are cost-effective, high-performance isobaric tagging tools that enhance peptide fragmentation and protein identification while ensuring high quantification accuracy, making them valuable for complex quantitative proteomic analyses.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"79 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235018","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}