{"title":"A Minimally Invasive Diagnostic Platform Compatible with Tissue and Serum Analysis for Early Detection of Non-Alcoholic Fatty Liver Disease","authors":"Yongchuang Li,Haiyue Liu,Zhenwen Guo,Junping Wang,Fangjun Huo,Caixia Yin","doi":"10.1021/acs.analchem.6c05155","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c05155","url":null,"abstract":"Non-alcoholic fatty liver disease (NAFLD), one of the most prevalent chronic liver diseases, initially manifests as simple hepatic steatosis. Without timely intervention, it can progress to cirrhosis and ultimately hepatocellular carcinoma. Early diagnosis and intervention are therefore essential for slowing disease progression and reducing the risk of complications. However, effective minimally invasive methods for the early diagnosis of NAFLD remain limited in clinical practice, posing substantial challenges to large-scale screening. Emerging evidence indicates that during NAFLD progression, the mitochondrial membrane potential in hepatocytes gradually declines, accompanied by increasing spatial disorganization and pronounced alterations in the polarity of the mitochondrial microenvironment. Inspired by these findings, we developed a mitochondria-targeted, polarity-sensitive near-infrared fluorescent diagnostic system for the early detection of NAFLD. A series of probes (BS-X) were designed and synthesized based on a hemicyanine−triphenylamine fluorescent scaffold. Through comprehensive evaluation combining in vitro experiments and theoretical calculations, BS-1 was identified as the optimal probe, exhibiting excellent photophysical properties, low cytotoxicity, and high sensitivity to polarity variations. BS-1 efficiently targeted mitochondria (R = 0.89) and enabled real-time monitoring of dynamic changes in mitochondrial microenvironmental polarity. Notably, BS-1 enabled the detection of distinct disease-associated signals in both liver tissue and serum samples from NAFLD mice as early as one week after disease induction, achieving synchronous detection in hepatic tissue and serum and providing a novel molecular diagnostic tool for the early diagnosis of NAFLD.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"44 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218837","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":"High-Gain Bacterial RNA Imaging via High-Density Protein Fluorescence In Situ Hybridization","authors":"Qiuyu Luo,Jiemei Zhuang,Sha Deng,Qiang He,Yong Zhang,Ruijie Deng,Xuhan Xia","doi":"10.1021/acs.analchem.6c01963","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c01963","url":null,"abstract":"Fluorescence in situ hybridization (FISH) is important for bacterial genotypic analysis; however, the limited number of labels per probe results in insufficient signal gain, compromising the detection of low-abundance RNAs. Here, we present high-density protein FISH (HD-FISH) for high-gain bacterial RNA imaging. Instead of fluorophore-modified probes, this method employs a fluorescently tagged, catalytically inactive ribonuclease H1 for multi-site labeling of target RNAs. Compared to traditional FISH and hybridization chain reaction-based FISH, HD-FISH suppresses background noise while enhancing positive signals, achieving 7.43-fold and 1.89-fold increases in signal gain, respectively, thereby enabling high-gain imaging. We showed that HD-FISH can precisely quantify quinolone-resistant Salmonella enterica strains within complex microbial communities, with a recovery rate of 97.78−131.40%, and allows us to detect and identify quinolone-resistant bacteria in fecal samples. The method provides a robust tool for profiling bacterial genotypes at the single-cell level, facilitating the elucidation of microbial heterogeneity and its roles in complex populations.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"3 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218838","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}
Lydia A. Rush,Matthew A. Coble,Carmen S. Menoni,Andrew M. Duffin
{"title":"Multi-Collector Extreme Ultraviolet Laser Mass Spectrometry (MC-EUV-MS): Using High-Energy Photoionization for High-Spatial-Resolution Isotope Ratio Mapping of Actinide Materials","authors":"Lydia A. Rush,Matthew A. Coble,Carmen S. Menoni,Andrew M. Duffin","doi":"10.1021/acs.analchem.6c03668","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c03668","url":null,"abstract":"Isotope maps are typically collected with a multi-collector mass spectrometer (MC-MS) coupled to a high-spatial-resolution ionization source, yet few ionization sources compatible with MC-MS systems can operate robustly at the submicron scale. To meet this need, we couple an extreme ultraviolet (EUV) laser photon-based ionization source to a modified Thermo Scientific NeptunePlus MC-MS by removing and replacing the inductively coupled plasma (ICP) with the EUV laser system, herein called the MC-EUV-MS. The 46.9 nm EUV laser light is focused to sub-micrometer spots for sample ablation while simultaneously realizing high-energy photoionization using 26.4 eV photons. Thus, the EUV probe combines ablation and ionization in a single pulse. We characterize the newly built MC-EUV-MS by analyzing different actinide-bearing materials. We achieve a sample utilization efficiency (SUE) of 0.006% for 238U using the NIST 610 and 612 glasses at a low +2 kV extraction voltage for accelerating ions off the sample. Higher extraction voltages up to +5 kV point to increased ion yields. We measure 235U/238U isotope ratios from three uranium samples ranging from natural to low enriched. We demonstrate the high spatial resolution of the MC-EUV-MS by mapping uranium oxide microparticles using 500 nm ablation spots. Compared to isotope maps collected over the same sample area using large geometry secondary ion mass spectrometry, the MC-EUV-MS shows significantly higher spatial resolution within the scope of this study.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"65 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218853","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":"Band-Pass Fluorescence Activation via Dual-Responsive Molecular Design in the NIR-II Window for In Vivo pH Sensing","authors":"Xin Zhang,Chunyan Liu,Baofeng Yun,Benhao Li,Zuhai Lei,Mengyao Zhao,Fan Zhang","doi":"10.1021/acs.analchem.6c04399","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c04399","url":null,"abstract":"Real-time monitoring of physiological pH in living systems is essential for accurate disease evaluation and therapeutic guidance. However, conventional pH-responsive probes typically operate through monotonic activation and lack window selectivity, limiting their capacity to report further microenvironmental changes after crossing the activation threshold. Here, we report a NIR-II molecularly engineered band-pass pH (BPpH) sensing strategy that exhibits a non-monotonic “off-on-off” fluorescence response. By integrating an acid-responsive spirolactam switch with an alkaline-sensitive phenolic regulator, the BPpH probes enable window-restricted signal output within a defined pH range. BPpH-3 displays fluorescence activation from pH 3.6 to 5.2 and deactivation from pH 5.2 to 8.0, affording dual apparent pKa values of 4.16 and 7.42 and establishing a response window. Unlike conventional monotonic turn-on probes, this band-pass response enables continuous tracking of pH changes across the therapeutic process, and BPpH-3 further enables dynamic evaluation of therapeutic efficacy in a skin inflammation model, allowing timely assessment of treatment progression and dosing sufficiency. Moreover, its window-constrained response mitigates signal over-amplification under extreme acidification, facilitating improved tumor margin delineation for precision resection under NIR-II imaging guidance. The band-pass sensing strategy presented here provides a transferable framework for window-regulated detection of diverse physiological parameters and holds promise for integration with multiple diagnostic imaging modalities.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"14 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218878","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":"Valence-Engineered Regulation of Built-In Electric Field in Hollow CuS@CeO2 Heterojunction for Photoelectrochemical Immunoassay","authors":"Jiao Qin,Yang Yang,Di Wu,Shuo Tian,Man Xu,Yu He,Dianping Tang","doi":"10.1021/acs.analchem.6c06355","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c06355","url":null,"abstract":"Abstract Work function (Φ) strongly affects interfacial charge distribution and built-in electric field (BIEF) formation, fundamentally determining the photoelectric conversion efficiency of photoelectrochemical (PEC) sensors. Exploring the inherent correlation between Φ and BIEF is therefore essential to guide the rational design of PEC sensors. In this work, a PEC sensing platform was fabricated based on hollow CuS@CeO2 heterojunctions, where BIEF intensity was precisely regulated by cerium valence-state engineering. A robust BIEF was formed in high-valence CuS@CeO2(IV), which facilitates efficient photogenerated carrier separation and yields a high initial PEC signal. Following the sandwich-type immunoassay recognition of carcinoembryonic antigen (CEA), hydrogen peroxide (H2O2) generated by enzymatic reactions was used to react with high-valence CuS@CeO2(IV). After CuS@CeO2(IV) underwent a reduction reaction with H2O2, the Ce atoms in the heterojunction were reduced to form low-valence CuS@CeO2(III). The reduction in Ce valence states was accompanied by a decrease in work function difference (ΔΦ) values, which weakened the BIEF intensity. The weakened BIEF is unfavorable for the photogenerated carrier separation, thereby inducing an obvious decline in the PEC signal. Relying on this distinct signal variation, sensitive CEA detection is successfully realized by the PEC platform, which exhibits a linear detection range of 0.02−50 ng/mL and a low detection limit of 0.53 pg/mL. This study validates the efficacy of valence engineering in BIEF regulation, offering a promising strategy for the development of advanced PEC sensors for clinical diagnostic applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"168 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209908","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}
Connor Beveridge,Prageeth R. Wijewardhane,Matthew Muhoberac,Nicolás M. Morato,Andreas Kaerner,Li-Kang Zhang,Douglas Richardson,Ayanna Shoulds,Jeffrey R. Gilbert,Christopher J. Welch,Shane Tichy,Gaurav Chopra
{"title":"Instrument-Agnostic Machine Learning Framework for Accurate Prediction of Functional Groups from Tandem Mass Spectrometry","authors":"Connor Beveridge,Prageeth R. Wijewardhane,Matthew Muhoberac,Nicolás M. Morato,Andreas Kaerner,Li-Kang Zhang,Douglas Richardson,Ayanna Shoulds,Jeffrey R. Gilbert,Christopher J. Welch,Shane Tichy,Gaurav Chopra","doi":"10.1021/acs.analchem.5c05945","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05945","url":null,"abstract":"Abstract Structural elucidation of unknown compounds using tandem mass spectrometry (MS/MS) is an ongoing challenge. Expert chemists will often use common product ion peaks and neutral losses or peak matching software to predict structural aspects from MS/MS spectra, a process which is time consuming and limited by the molecular entries in the database. We introduce an instrument-agnostic machine learning (ML) framework that predicts functional groups directly from MS/MS spectra, eliminating the need for conventional database searches. The ML models are trained on data from different sources, the MassBank of North America (MONA), a public database, and a custom MS/MS database acquired using a single high throughput desorption electrospray ionization (DESI) MS/MS platform to showcase transferability of model predictions independent of instrument acquisition. Additionally, a novel spectral representation is developed for ML use by standardizing the spectra to the precursor ion m/z. We utilized molecular metrics, specifically, average molecular F1 score of 87% (MONA) and 76% (DESI) and average molecular accuracy of 94% (MONA) and 87% (DESI), indicating similar model performance when trained on different databases to validate the ML framework. To further illustrate the robustness and transferability of our ML framework, models trained on DESI-generated data successfully predicted functional groups, using spectral data generated from a blind test set of molecules using two different company laboratories using distinct mass spectrometry instruments (Orbitrap and TOF) operated in positive-ion mode electrospray ionization. We believe that such an approach, where models trained on data from one instrument can reliably make accurate predictions on spectra acquired using different instruments in a database-free manner, will significantly expand the practical applications of ML to mass spectrometry.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"4 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210136","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}
Hailin Zhang,SuXuan Liao,Jiakuan Wu,Yunzhe Tang,Tianhui Huang,Zhiheng Su,Mei Li
{"title":"Deep Learning-Enabled Plasmonic-Catalytic Au@PBA Array for Simultaneous SERS/Colorimetric Quantification of Exhaled Benzene-Related VOCs","authors":"Hailin Zhang,SuXuan Liao,Jiakuan Wu,Yunzhe Tang,Tianhui Huang,Zhiheng Su,Mei Li","doi":"10.1021/acs.analchem.6c04396","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c04396","url":null,"abstract":"Abstract Accurate determination of benzene-related volatile organic compounds (B-VOCs) in exhaled breath is of considerable importance for disease screening and occupational exposure assessment. However, the simultaneous identification and quantification of structurally similar B-VOCs remain a challenge due to severe cross-interference and nonlinear signal coupling in multicomponent matrices. Herein, we report a deep learning-enabled plasmonic-catalytic sensor array based on core−shell Au@PBA(M) (M = Co, Ni, Mn) nanozymes featuring an ultrathin PBA shell for the multiplexed analysis of five B-VOCs (toluene, ethylbenzene, xylene, styrene, and phenol). The dual-response core−shell Au@PBA nanoparticles provide both strong plasmonic enhancement and peroxidase-mimicking activity, enabling the catalytic oxidation of TMB with concurrent surface-enhanced Raman scattering (SERS) and colorimetric readouts. In the presence of different B-VOCs, the oxidation process is inhibited to different extents due to the differential binding affinities of the B-VOCs to the Au@PBA nanoparticles, generating highly characteristic dual-mode fingerprints. Based on this mechanism, linear discriminant analysis enabled reliable discrimination of the five B-VOCs. Notably, quantitative analysis of single-component systems demonstrated broad quantitative ranges of 0.001−500 ppm for ethylbenzene and phenol and 0.005−500 ppm for toluene, xylene, and styrene. More importantly, the integration of multichannel SERS fingerprints with an artificial neural network enabled simultaneous quantification of five B-VOCs in 25 complex breath-relevant samples, yielding excellent predictive accuracy (R2 > 0.97) and low root-mean-square errors (0.27−0.30 in log10 scale). These results demonstrate that the proposed strategy effectively resolves the cross-responsiveness of complex gas mixtures, providing a robust and noninvasive platform for intelligent breath analysis and environmental monitoring.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209907","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":"Immunophenotypic Profiles of General Chinese Population during Natural Aging","authors":"Yiyang Li,Boqian Wang,Xuling Han,Jingqi Dang,Jian-Ge Qiu,Bingjie Liu,Wei Wang,Fengmei Zhou,Yiran Zhao,Xiaobei Zhang,Liangshi Hao,Lezhong Ding,Xiaoxiang Chen,Quanhong Zhou,Wenqiong Su,Binghua Jiang,Feng Qian,Xianting Ding","doi":"10.1021/acs.analchem.6c03408","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c03408","url":null,"abstract":"Abstract Understanding the interplay between the immune system’s dynamics and the natural aging process is crucial for developing potential strategies to mitigate age-related health challenges. Here, we investigated how immunophenotypic profiles vary with the natural aging process, daily practices, and physiological characteristics within a general population of 605 healthy individuals from the Central China Cohort. Utilizing mass cytometry on peripheral blood mononuclear cell (PBMC) samples, we acquired over 57 million single-cell data in total from this cohort. These cells were clustered into 50 distinct immune cell subsets. Additionally, we gathered detailed questionnaires from every participant with 764 questions concerning their physical and physiological metrics, lifestyles, and socioeconomic status. By leveraging bootstrap lasso and logit regression models, we endeavored to forecast age and gender based on immunophenotypic profiles. Our investigations unveiled significant correlations between chronological age and specific immune cell clusters such as CD27+CD28+ naïve T and γδ T cells and CD38+ pDCs, showcasing discernible age-related patterns. Furthermore, we established immune ages through the regression models and calculated the age differentials relative to the chronological age, which shed light on the relationships between younger or older immune ages and various body metrics and lifestyles. By offering a comprehensive overview of immune cell profiles in a sizable healthy cohort through mass cytometry, this data resource advances our comprehension of the roles played by immune systems and lifestyles in the aging process.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210487","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}
Chuanxiu Yu,Ting Xie,Yuxuan Liao,Lin Tan,Song Chen,Zhimin Zhang,Hongmei Lu
{"title":"DeepCPR: UNet3+ and Multivariate Curve Resolution for Automated GC−MS Data Deconvolution","authors":"Chuanxiu Yu,Ting Xie,Yuxuan Liao,Lin Tan,Song Chen,Zhimin Zhang,Hongmei Lu","doi":"10.1021/acs.analchem.6c04440","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c04440","url":null,"abstract":"Abstract Resolving overlapping peaks in gas chromatography−mass spectrometry (GC−MS), especially for isomers and low-abundance compounds, remains challenging due to spectral similarity and noise. Traditional multivariate curve resolution (MCR) methods heavily rely on initial spectral estimates, often leading to biased results. Here we present DeepCPR, a deep learning framework integrating a UNet3+ architecture with multi-scale feature fusion and dynamic channel attention to predict chromatographic profiles as robust initializations for MCR. This design accurately resolves co-eluted peaks even at low signal-to-noise ratios (SNR of 3−10). On amino acid and fatty acid standard mixtures, DeepCPR achieves mean explained variances (R2) of 0.987 and concentration correlation coefficients (r) of 0.994, outperforming AMDIS and DeepResolution2. Crucially, DeepCPR resolves near-identical isomers (spectral similarity > 0.999) with 94.1% spectral match accuracy, an 18% improvement over spectral-based methods. DeepCPR automates untargeted GC−MS processing and peak-table generation. OPLS-DA of a fixed 53-variable matrix from 136 human plasma samples achieved 98.54% mean accuracy under repeated stratified 10-fold cross-validation (100 repetitions) and prioritized 16 variables as potential biomarkers. The open-source implementation (https://github.com/YuChuanxiu/DeepCPR) ensures reproducibility and adaptability across diverse analytical workflows for precision metabolomics and environmental analysis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"89 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209909","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}
Min Zhang,Feng Yuan,Sining Li,Yuxin Leng,Yupeng Li,Yuanji Gao
{"title":"Induced Nanoelectrospray Ionization for Spontaneous Singlet Oxygen Formation and Oxidative Transformation of Pollutants","authors":"Min Zhang,Feng Yuan,Sining Li,Yuxin Leng,Yupeng Li,Yuanji Gao","doi":"10.1021/acs.analchem.6c05080","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c05080","url":null,"abstract":"Abstract Induced nanoelectrospray ionization (induced nESI) is a noncontact, in situ spray methodology initiated by an externally applied high-voltage electric field. Within this setup, the mass spectrometer serves as a counter electrode that shapes the electric-field distribution and governs charge transport via electrostatic induction, thereby sustaining a stable spray containing positive and negative ions. Notably, the rapid transition from bulk solution into highly charged microdroplets triggers the spontaneous, in situ generation of singlet oxygen (1O2) at the μg mL−1 level, providing the first experimental evidence of spontaneous 1O2 generation within an induced nESI source. Mass spectrometric analysis confirmed this selective 1O2-mediated oxidation, revealing the characteristic signals of 9,10-diphenylanthracene oxidation products with a mass increase of 32 Da. 1O2 formation was further validated using multiple chemical probes, including 1,5-dihydroxynaphthalene, 1,3-diphenylisobenzofuran, and furfuryl alcohol, complemented by deuterium oxide−induced lifetime enhancement and radical-trapping experiments. Leveraging this highly selective oxidation mechanism, this platform enables the efficient transformation of six representative organic pollutants, including dibenzo-p-dioxin and bisphenol A. Collectively, these results establish induced nESI as a powerful new analytical and reaction platform for advanced oxidation processes.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"22 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209916","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}