Extracellular vesicles (EVs) carry a rich repertoire of glycan structures that exhibit crucial functions in diverse biological processes. Currently, the deciphering of EV glycans is predominantly conducted using bulk methods, which only yield ensemble-averaged information about a population of EV particles. This kind of deciphering manner suffers from limited sensitivity (particularly in detecting specific EV populations within complex biological matrices) and is inadequate for effectively elucidating fundamental characteristics (e.g., heterogeneity) of EV glycans, thereby impeding the exploitation of EV glycans. To overcome these challenges, we proposed a droplet-based strategy to achieve the deep analysis of EV glycans down to the single-particle level. Named Droplet-EVG, this assay leveraged polydisperse droplets formed through facile shaking as reaction units to compartmentalize distinct EV particles, and transferred the glycan signatures into fluorescence signals by integrating nanoagent-assisted EV manipulation, lectin-glycan affinity, and enzyme-mediated signal amplification. Compared to conventional bulk assays (ELISA and MAEG), this assay demonstrated a significantly enhanced detection sensitivity (∼107 particles/mL) and, more importantly, systematically revealed the heterogeneity widely present in diverse EV glycan signatures. Moreover, its excellent performance in mock samples, particularly at low target EV concentrations, conclusively substantiated the assay’s capability for directly distinguishing specific EV glycan signatures from complex biological backgrounds. With its advantages of user-friendly operation, minimal requirement for complex instrumentation, high accessibility, and good practicality in complex samples, this assay is envisioned to offer a robust deciphering tool for deepening the understanding of EV glycoscience and advancing EV glycan-based biomedical applications.
{"title":"Droplet-Based Facile Deciphering of Heterogeneous Glycans in Extracellular Vesicles down to the Single-Particle Level","authors":"Yufei Yan,Ying Zhu,Yifan Wang,Yifan Luo,Junyan Zhang,Wenlong Chen,Jiale Song,Yangfan Zhou,Sipeng Yang,Yulin Wang,Jing Liu,Yunqing Tang,Linglong Zou,Luru Dai,Zhigang Wang","doi":"10.1021/acs.analchem.5c07013","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c07013","url":null,"abstract":"Extracellular vesicles (EVs) carry a rich repertoire of glycan structures that exhibit crucial functions in diverse biological processes. Currently, the deciphering of EV glycans is predominantly conducted using bulk methods, which only yield ensemble-averaged information about a population of EV particles. This kind of deciphering manner suffers from limited sensitivity (particularly in detecting specific EV populations within complex biological matrices) and is inadequate for effectively elucidating fundamental characteristics (e.g., heterogeneity) of EV glycans, thereby impeding the exploitation of EV glycans. To overcome these challenges, we proposed a droplet-based strategy to achieve the deep analysis of EV glycans down to the single-particle level. Named Droplet-EVG, this assay leveraged polydisperse droplets formed through facile shaking as reaction units to compartmentalize distinct EV particles, and transferred the glycan signatures into fluorescence signals by integrating nanoagent-assisted EV manipulation, lectin-glycan affinity, and enzyme-mediated signal amplification. Compared to conventional bulk assays (ELISA and MAEG), this assay demonstrated a significantly enhanced detection sensitivity (∼107 particles/mL) and, more importantly, systematically revealed the heterogeneity widely present in diverse EV glycan signatures. Moreover, its excellent performance in mock samples, particularly at low target EV concentrations, conclusively substantiated the assay’s capability for directly distinguishing specific EV glycan signatures from complex biological backgrounds. With its advantages of user-friendly operation, minimal requirement for complex instrumentation, high accessibility, and good practicality in complex samples, this assay is envisioned to offer a robust deciphering tool for deepening the understanding of EV glycoscience and advancing EV glycan-based biomedical applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"24 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139073","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.5c07844
Shunda Qiao,Bangyu Liu,Ziheng Lv,Ying He,Xiyang Zhi,Lixian Liu,Andreas Mandelis,Yufei Ma
This paper presents a dual-quartz-enhanced photoacoustic spectroscopy (D-QEPAS) sensor based on an elliptical acoustic resonator (EAR) for the first time. The sensor, leveraging the acoustic focusing characteristics of the EAR and a synchronous detection mechanism with dual quartz tuning forks (QTFs), effectively resolves the low acoustic energy utilization issue in traditional QEPAS systems. Dual QTFs were positioned at the two focal points within the EAR to achieve efficient acoustic energy collection and signal superposition. An EAR theoretical model was established and calculated using the finite element analysis method for performance optimization. With acetylene (C2H2) as the target gas, results demonstrate that the signal intensity of the EAR-based D-QEPAS system exhibits an approximately 13.05x enhancement compared with the traditional QEPAS system. Allan deviation analysis indicates that this system achieves a detection limit of 134 ppb at an average time of 500 s
{"title":"Elliptical Acoustic Resonator-Based Dual-Quartz-Enhanced Photoacoustic Spectroscopy Sensing","authors":"Shunda Qiao,Bangyu Liu,Ziheng Lv,Ying He,Xiyang Zhi,Lixian Liu,Andreas Mandelis,Yufei Ma","doi":"10.1021/acs.analchem.5c07844","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c07844","url":null,"abstract":"This paper presents a dual-quartz-enhanced photoacoustic spectroscopy (D-QEPAS) sensor based on an elliptical acoustic resonator (EAR) for the first time. The sensor, leveraging the acoustic focusing characteristics of the EAR and a synchronous detection mechanism with dual quartz tuning forks (QTFs), effectively resolves the low acoustic energy utilization issue in traditional QEPAS systems. Dual QTFs were positioned at the two focal points within the EAR to achieve efficient acoustic energy collection and signal superposition. An EAR theoretical model was established and calculated using the finite element analysis method for performance optimization. With acetylene (C2H2) as the target gas, results demonstrate that the signal intensity of the EAR-based D-QEPAS system exhibits an approximately 13.05x enhancement compared with the traditional QEPAS system. Allan deviation analysis indicates that this system achieves a detection limit of 134 ppb at an average time of 500 s","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"295 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139084","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.5c05171
Deepak Dabur,Jie Li,Priyanka Rana,Hui-Fen Wu
This study introduces highly stable photoluminescent CeF3 nanocrystals as a first ratiometric fluorescent probe for the selective detection of the neurotoxic alkaloid anabasine in environmental water matrices. The hexagonal-phase CeF3 nanocrystals (40–50 nm) exhibit dual-emission bands at 322 (quenched) and 433 nm (enhanced) upon anabasine binding, enabling sensitive (LOD: 0.17 μM) and matrix-resistant quantification. Structural (XRD, TEM, EDS) and optical (pH and thermal stability: pH 4–10, 30–90 °C) characterizations confirm robustness for real-world applications. Recovery assays (95–103%) in lake, river, and tap water demonstrate minimal matrix interference, outperforming LC-MS/MS and GC-FID methods that require derivatization or complex sample pretreatment. The cost-effectiveness, simplicity, and ratiometric self-calibration of the method highlight its potential for on-site environmental monitoring of tobacco-derived contaminants.
{"title":"Highly Stable Photoluminescent CeF3 Nanocrystal as a Versatile Probe for Neurotoxic Alkaloid (Anabasine) Sensing via Fluorescence Modulation","authors":"Deepak Dabur,Jie Li,Priyanka Rana,Hui-Fen Wu","doi":"10.1021/acs.analchem.5c05171","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05171","url":null,"abstract":"This study introduces highly stable photoluminescent CeF3 nanocrystals as a first ratiometric fluorescent probe for the selective detection of the neurotoxic alkaloid anabasine in environmental water matrices. The hexagonal-phase CeF3 nanocrystals (40–50 nm) exhibit dual-emission bands at 322 (quenched) and 433 nm (enhanced) upon anabasine binding, enabling sensitive (LOD: 0.17 μM) and matrix-resistant quantification. Structural (XRD, TEM, EDS) and optical (pH and thermal stability: pH 4–10, 30–90 °C) characterizations confirm robustness for real-world applications. Recovery assays (95–103%) in lake, river, and tap water demonstrate minimal matrix interference, outperforming LC-MS/MS and GC-FID methods that require derivatization or complex sample pretreatment. The cost-effectiveness, simplicity, and ratiometric self-calibration of the method highlight its potential for on-site environmental monitoring of tobacco-derived contaminants.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"108 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138735","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}
Fibroblast activation protein-α (FAPα), with restricted biological distribution and cleavage site specificity, is an attractive biomarker and target for diseases diagnosis and therapy, especially for cancers. However, effective analytical tools for in vivo FAPα detection are lacking. In this work, based on classic hemicyanine and cyanine fluorophores, we developed two novel FAPα-activated fluorescent probes, Sulfo-OHDF and Sulfo-FQCy7, with improved water solubility by introducing a sulfonic acid group into the fluorophore scaffold. Consequently, these probes exhibited much higher signal-to-noise ratios and sensitivity toward FAPα than the control probes. Among them, Sulfo-OHDF, featuring near infrared exciation/emssion, displayed superior fluorescence enhancement (113.2-fold), excellent sensitivity (limit of detection of 1.59 ng/mL) toward FAPα, and improved biocompatibility. Furthermore, using this probe, overexpressed FAPα in cells, tumor tissues, the wound-healing process, and tumor-bearing mice was successfully detected. Overall, our work may provide a powerful tool for in vivo imaging of FAPα-relevant physiological and pathological processes.
{"title":"FAPα-Activated NIR-I Fluorescent Probe with Improved Water Solubility for Tumor Imaging","authors":"Cheng Xie,Jing-Jie Wu,Yurong Feng,Tian-Bing Ren,Lin Yuan,Shuang-Yan Huan,Xiao-Bing Zhang","doi":"10.1021/acs.analchem.5c07190","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c07190","url":null,"abstract":"Fibroblast activation protein-α (FAPα), with restricted biological distribution and cleavage site specificity, is an attractive biomarker and target for diseases diagnosis and therapy, especially for cancers. However, effective analytical tools for in vivo FAPα detection are lacking. In this work, based on classic hemicyanine and cyanine fluorophores, we developed two novel FAPα-activated fluorescent probes, Sulfo-OHDF and Sulfo-FQCy7, with improved water solubility by introducing a sulfonic acid group into the fluorophore scaffold. Consequently, these probes exhibited much higher signal-to-noise ratios and sensitivity toward FAPα than the control probes. Among them, Sulfo-OHDF, featuring near infrared exciation/emssion, displayed superior fluorescence enhancement (113.2-fold), excellent sensitivity (limit of detection of 1.59 ng/mL) toward FAPα, and improved biocompatibility. Furthermore, using this probe, overexpressed FAPα in cells, tumor tissues, the wound-healing process, and tumor-bearing mice was successfully detected. Overall, our work may provide a powerful tool for in vivo imaging of FAPα-relevant physiological and pathological processes.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"10 9 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139072","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}
Herein, a novel electrochemiluminescence (ECL) sensing platform was constructed by the DNA hybridization correctional immunoreaction as the target recognition element and ZnO nanostars (ZnO NSs) as an electron accelerator for Au nanoclusters (Au NCs) emitters for ultrasensitive and specific detection of the low expression of glial fibrillary acidic protein (GFAP) related to glioblastoma. Compared with traditional sandwich immunoreactions with low accuracy, the DNA hybridization correctional immunoreaction not only achieved high specificity of target recognition by the cross-correction between the conformational correspondence of the antibody–antigen and the spatial position of strand DNAs but also enhanced the target recognition efficiency by the modulation of thermodynamic stability via adjustment of the DNA stem length. Impressively, ZnO NSs as an electron accelerator could rapidly transfer the electrons of emitter Au NCs to the vacancy defects of ZnO NSs during electroexcitation, generating more excited-state Au NCs for strong ECL emission. The ECL efficiency of Au NCs@ZnO NSs (12.89%) was significantly higher than that of pure Au NCs (2.69%) versus standard [Ru(bpy)3]2+. As a result, the sensing platform achieved trace analysis of GFAP with a detection limit as low as 60 fg/mL, surpassing existing ECL biosensors for protein detection. Meanwhile, it displayed a higher positive/negative predictive value and a lower false positive/negative rate compared to those of the traditional sandwich immunoassay method. This strategy proposed a new electron accelerator-enhanced ECL emission of metal NCs for ultrasensitive protein detection through DNA hybridization correctional immunoreaction, displaying promising potential for applications in clinical diagnostics.
{"title":"Electron Accelerator-Enhanced Au Nanoclusters Electrochemiluminescence for Ultrasensitive Detection of Low-Expression Protein Based on DNA Hybridization Correctional Immunoreaction","authors":"Furong Ran,Xiaochun Zhu,Yaqin Chai,Ying Zhou,Ruo Yuan","doi":"10.1021/acs.analchem.5c04129","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c04129","url":null,"abstract":"Herein, a novel electrochemiluminescence (ECL) sensing platform was constructed by the DNA hybridization correctional immunoreaction as the target recognition element and ZnO nanostars (ZnO NSs) as an electron accelerator for Au nanoclusters (Au NCs) emitters for ultrasensitive and specific detection of the low expression of glial fibrillary acidic protein (GFAP) related to glioblastoma. Compared with traditional sandwich immunoreactions with low accuracy, the DNA hybridization correctional immunoreaction not only achieved high specificity of target recognition by the cross-correction between the conformational correspondence of the antibody–antigen and the spatial position of strand DNAs but also enhanced the target recognition efficiency by the modulation of thermodynamic stability via adjustment of the DNA stem length. Impressively, ZnO NSs as an electron accelerator could rapidly transfer the electrons of emitter Au NCs to the vacancy defects of ZnO NSs during electroexcitation, generating more excited-state Au NCs for strong ECL emission. The ECL efficiency of Au NCs@ZnO NSs (12.89%) was significantly higher than that of pure Au NCs (2.69%) versus standard [Ru(bpy)3]2+. As a result, the sensing platform achieved trace analysis of GFAP with a detection limit as low as 60 fg/mL, surpassing existing ECL biosensors for protein detection. Meanwhile, it displayed a higher positive/negative predictive value and a lower false positive/negative rate compared to those of the traditional sandwich immunoassay method. This strategy proposed a new electron accelerator-enhanced ECL emission of metal NCs for ultrasensitive protein detection through DNA hybridization correctional immunoreaction, displaying promising potential for applications in clinical diagnostics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"7 9 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139074","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.5c06654
Bo Wang,Xinyi Luo,Wenting Guo,Ping Hu,Yong Wang,Guohua Qi,Yongdong Jin
Hydrogen sulfide (H2S) is the third gasotransmitter after nitrogen oxide and carbon monoxide, playing vital roles in physiological controls, such as angiogenesis, vascular homeostasis, thrombosis, inflammation, and remodeling. Monitoring the content level and dynamic variations of H2S within cells will help understand its involvement and relationship in cancer proliferation and may also lead to new cancer therapy options. Herein, we developed a simple and effective approach for ionic rectification sensing detection of H2S in single living cells using p-azidobenzoic acid (PA)-functionalized glass nanopores (PA-nanopores), in which the glass nanopores were successively functionalized with 3-aminopropyltrimethoxysilane and PA, and the exposed azido groups on the inner wall of the nanopore caused a negative rectification ratio (R) and varied upon reaction with the intracellular H2S. In the presence of H2S, azido groups could be reduced to amino groups, leading to a shift in the rectification ratio. The developed H2S nanopore sensing platform showed high resolution and excellent selectivity, making it reliable for the quantification of H2S in individual cells. The H2S concentrations in individual HeLa cells, MCF-7 cells, and HL7702 cells were effectively quantified using the approach.
{"title":"Quantification of Hydrogen Sulfide in Single Living Cells by Azido-Functionalized Glass Nanopores","authors":"Bo Wang,Xinyi Luo,Wenting Guo,Ping Hu,Yong Wang,Guohua Qi,Yongdong Jin","doi":"10.1021/acs.analchem.5c06654","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c06654","url":null,"abstract":"Hydrogen sulfide (H2S) is the third gasotransmitter after nitrogen oxide and carbon monoxide, playing vital roles in physiological controls, such as angiogenesis, vascular homeostasis, thrombosis, inflammation, and remodeling. Monitoring the content level and dynamic variations of H2S within cells will help understand its involvement and relationship in cancer proliferation and may also lead to new cancer therapy options. Herein, we developed a simple and effective approach for ionic rectification sensing detection of H2S in single living cells using p-azidobenzoic acid (PA)-functionalized glass nanopores (PA-nanopores), in which the glass nanopores were successively functionalized with 3-aminopropyltrimethoxysilane and PA, and the exposed azido groups on the inner wall of the nanopore caused a negative rectification ratio (R) and varied upon reaction with the intracellular H2S. In the presence of H2S, azido groups could be reduced to amino groups, leading to a shift in the rectification ratio. The developed H2S nanopore sensing platform showed high resolution and excellent selectivity, making it reliable for the quantification of H2S in individual cells. The H2S concentrations in individual HeLa cells, MCF-7 cells, and HL7702 cells were effectively quantified using the approach.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"244 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139078","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}
The dual challenges of accurately imaging cancer cells and selectively activating immune signaling pathways require innovative DNA nanomachines with targeted recognition and multistimulus response capabilities. In this study, we developed a dual tetrahedral DNA nanomachine (DTDN) with layered responsiveness, which integrated a cascaded AND logic gate driven by sequential activation of reconfigurable DNA modules for precise cancer cell imaging and selective activation of the cGAS-STING pathway. Through AS1411 aptamer modification, DTDN achieved selective targeting and efficient cancer cell internalization. The overexpression of apurinic/apyrimidinic endonuclease 1 (APE1) in cancer cells first triggered the release of functional hairpins H1 and H2, after which miR-21 initiated a hybridization chain reaction (HCR) to generate long fluorescent nicked double-stranded DNA (dsDNA). The dsDNA product was recognized by cGAS, thereby activating the cGAS-STING pathway. The design of DNA tetrahedra gate prevented signal leakage by blocking the HCR toehold sequences. Moreover, the dual-locked cascade strategy exhibited high specificity and anti-interference capability, ensuring the specificity of cancer cell recognition and the activation of downstream events. Furthermore, the generated long nicked dsDNA not only provided an amplified fluorescence signal for cancer cell imaging but also acted as potent cGAS activators, thereby triggering the cGAS-STING pathway. Hence, this work provides a programmable, safe, and reliable nucleic acid nanoplatform for cancer diagnosis and cGAS-STING pathway-based regulatory therapy.
{"title":"A Layered-Responsive DNA Tetrahedral Nanomachine for Precise Cancer Cell Imaging and Selective cGAS-STING Signaling Activation","authors":"Yu-Wen Zhang,Tong Zhang,Xiao-Qiong Li,Bin Kang,Hong-Yuan Chen,Jing-Juan Xu","doi":"10.1021/acs.analchem.5c07640","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c07640","url":null,"abstract":"The dual challenges of accurately imaging cancer cells and selectively activating immune signaling pathways require innovative DNA nanomachines with targeted recognition and multistimulus response capabilities. In this study, we developed a dual tetrahedral DNA nanomachine (DTDN) with layered responsiveness, which integrated a cascaded AND logic gate driven by sequential activation of reconfigurable DNA modules for precise cancer cell imaging and selective activation of the cGAS-STING pathway. Through AS1411 aptamer modification, DTDN achieved selective targeting and efficient cancer cell internalization. The overexpression of apurinic/apyrimidinic endonuclease 1 (APE1) in cancer cells first triggered the release of functional hairpins H1 and H2, after which miR-21 initiated a hybridization chain reaction (HCR) to generate long fluorescent nicked double-stranded DNA (dsDNA). The dsDNA product was recognized by cGAS, thereby activating the cGAS-STING pathway. The design of DNA tetrahedra gate prevented signal leakage by blocking the HCR toehold sequences. Moreover, the dual-locked cascade strategy exhibited high specificity and anti-interference capability, ensuring the specificity of cancer cell recognition and the activation of downstream events. Furthermore, the generated long nicked dsDNA not only provided an amplified fluorescence signal for cancer cell imaging but also acted as potent cGAS activators, thereby triggering the cGAS-STING pathway. Hence, this work provides a programmable, safe, and reliable nucleic acid nanoplatform for cancer diagnosis and cGAS-STING pathway-based regulatory therapy.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"43 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138734","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.6c00210
Jing-Jing Chao,Li-Yuan Chen,Jing Chen,Yu-Xin Ding,Guo-Jiang Mao,Liufang Hu,Juan Ouyang,Chun-Yan Li
Hepatic ischemia-reperfusion (I/R) injury is a major cause of postoperative liver dysfunction and liver failure, leading to irreversible hepatocellular damage. The NLRP3 inflammasome and ferroptosis are recognized as key contributors to hepatic I/R injury, but their synergistic role in the underlying pathological mechanism remains unclear. Since dysregulated lipid droplets (LDs) metabolism is closely linked to oxidative stress and ferroptosis, real-time visualizing LDs dynamics offers a promising approach to study the interplay between NLRP3 inflammasome and ferroptosis during hepatic I/R injury. Herein, we designed and synthesized a dual-channel fluorescent probe, PX-P, based on a donor-π-acceptor-donor (D-π-A-D) structure, enabling specific targeting of LDs, a large Stokes shift (>120 nm), excellent photostability, and zero-crosstalk between two emission channels (Δλem = 363 nm). Using PX-P, we monitored LDs polarity changes in hepatocytes and mice during I/R injury, revealing distinct differences between normal and cancer cells, dynamic alterations in LDs polarity during inflammation and ferroptosis, and interactions between LDs and lysosomes, nucleolus, and nucleus in the processes of lipophagy and lipid homeostasis disruption. Visible/NIR-II dual-channel imaging revealed that LDs accumulation increased during ischemia and early stages of reperfusion, then gradually decreased with prolonged reperfusion. Notably, simultaneous inhibition of the NLRP3 inflammasome and ferroptosis pathways effectively alleviated hepatocellular injury. Collectively, PX-P provides a versatile cross-scale imaging platform for tracking LDs dynamics from cells to living organisms, offering insights into the pathogenic mechanism of hepatic I/R injury and potential therapeutic strategies for early intervention.
{"title":"A Visible/NIR-II Dual-Channel Fluorescent Probe for Investigating the Roles of NLRP3 Inflammasome and Ferroptosis during Hepatic Ischemia-Reperfusion Injury","authors":"Jing-Jing Chao,Li-Yuan Chen,Jing Chen,Yu-Xin Ding,Guo-Jiang Mao,Liufang Hu,Juan Ouyang,Chun-Yan Li","doi":"10.1021/acs.analchem.6c00210","DOIUrl":"https://doi.org/10.1021/acs.analchem.6c00210","url":null,"abstract":"Hepatic ischemia-reperfusion (I/R) injury is a major cause of postoperative liver dysfunction and liver failure, leading to irreversible hepatocellular damage. The NLRP3 inflammasome and ferroptosis are recognized as key contributors to hepatic I/R injury, but their synergistic role in the underlying pathological mechanism remains unclear. Since dysregulated lipid droplets (LDs) metabolism is closely linked to oxidative stress and ferroptosis, real-time visualizing LDs dynamics offers a promising approach to study the interplay between NLRP3 inflammasome and ferroptosis during hepatic I/R injury. Herein, we designed and synthesized a dual-channel fluorescent probe, PX-P, based on a donor-π-acceptor-donor (D-π-A-D) structure, enabling specific targeting of LDs, a large Stokes shift (>120 nm), excellent photostability, and zero-crosstalk between two emission channels (Δλem = 363 nm). Using PX-P, we monitored LDs polarity changes in hepatocytes and mice during I/R injury, revealing distinct differences between normal and cancer cells, dynamic alterations in LDs polarity during inflammation and ferroptosis, and interactions between LDs and lysosomes, nucleolus, and nucleus in the processes of lipophagy and lipid homeostasis disruption. Visible/NIR-II dual-channel imaging revealed that LDs accumulation increased during ischemia and early stages of reperfusion, then gradually decreased with prolonged reperfusion. Notably, simultaneous inhibition of the NLRP3 inflammasome and ferroptosis pathways effectively alleviated hepatocellular injury. Collectively, PX-P provides a versatile cross-scale imaging platform for tracking LDs dynamics from cells to living organisms, offering insights into the pathogenic mechanism of hepatic I/R injury and potential therapeutic strategies for early intervention.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138738","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.5c07024
Qing Li,Wei Li,Liping Lu,Xiayan Wang
Cortisol is an important biomarker in response to psychological stress. Detecting its content in biological samples is crucial for gaining insights into individual stress and personalized healthcare. The limitations of traditional techniques for cortisol detection make them unsuitable for rapid and real-time analysis, thereby motivating the development of alternative sensing strategies. Herein, we report a molecularly imprinted polymer (MIP) electrochemical sensor based on laser-induced graphene (LIG), fabricated via a one-step electropolymerization that integrates a Cu2+-l-histidine metal complex as intrinsic redox probes and 3,4-ethylenedioxythiophene (EDOT) as a conductive scaffold. The morphology, structure, electrochemical performance, and adsorption kinetics of the MIP film were systematically characterized. This MIP/LIG has a wide linear range of 0.05 to 100 μM, covering its physiological concentration range, with a detection limit as low as 5.6 nM, which is far below the lowest cortisol level in human sweat. Furthermore, it shows good selectivity for structurally similar steroid hormones and common sweat metabolites. Its excellent reproducibility, renewability, and long-term stability make it suitable for the detection of cortisol in both artificial and real human sweat, and the results are consistent with the physiological circadian rhythm changes. Importantly, this work first proposes the redox-active MIP using metal complexes, providing a new strategy for the development of electrochemical sensors for nonelectroactive substances.
{"title":"Redox-Active Molecularly Imprinted Polymer: Synergistic Integration of Recognition and Signal Transduction for Sweat Cortisol Sensing","authors":"Qing Li,Wei Li,Liping Lu,Xiayan Wang","doi":"10.1021/acs.analchem.5c07024","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c07024","url":null,"abstract":"Cortisol is an important biomarker in response to psychological stress. Detecting its content in biological samples is crucial for gaining insights into individual stress and personalized healthcare. The limitations of traditional techniques for cortisol detection make them unsuitable for rapid and real-time analysis, thereby motivating the development of alternative sensing strategies. Herein, we report a molecularly imprinted polymer (MIP) electrochemical sensor based on laser-induced graphene (LIG), fabricated via a one-step electropolymerization that integrates a Cu2+-l-histidine metal complex as intrinsic redox probes and 3,4-ethylenedioxythiophene (EDOT) as a conductive scaffold. The morphology, structure, electrochemical performance, and adsorption kinetics of the MIP film were systematically characterized. This MIP/LIG has a wide linear range of 0.05 to 100 μM, covering its physiological concentration range, with a detection limit as low as 5.6 nM, which is far below the lowest cortisol level in human sweat. Furthermore, it shows good selectivity for structurally similar steroid hormones and common sweat metabolites. Its excellent reproducibility, renewability, and long-term stability make it suitable for the detection of cortisol in both artificial and real human sweat, and the results are consistent with the physiological circadian rhythm changes. Importantly, this work first proposes the redox-active MIP using metal complexes, providing a new strategy for the development of electrochemical sensors for nonelectroactive substances.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"35 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138973","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.analchem.5c05437
Liping Dai,Yun Wang,Xiaosong Wu,Qian Wang,Zhigang Li,Yong Liu,Long Zhang,Shuai Zheng,Shu Wang
Healthcare-associated infection (HAI) pathogens cause severe nosocomial outbreaks, jeopardizing patient safety and straining healthcare systems. Conventional loop-mediated isothermal amplification–lateral flow immunoassay (LAMP-ICA) allows rapid pathogen detection but is constrained by low sensitivity, a high false-positive rate, and an extended detection time. To address these limitations, we present a dual-mode (colorimetric/fluorescent) microfluidic biosensing platform based on silicon–gold/quantum dot core–shell nanoprobes (Si@Au/DQD NPs). The platform incorporates two key innovations: (1) The colorimetric/fluorescent dual-signal Si@Au/DQD nanoprobe enhances detection reliability and sensitivity through dual-signal complementary verification and multilayered QD design, halving the LAMP amplification time compared to traditional colloidal gold systems, and (2) a modular microfluidic chip integrates LAMP amplification and ICA detection within a closed system, effectively preventing leakage and contamination of amplification products. Performance evaluation showed that the fluorescence detection limit of this system for Staphylococcus aureus (S. aureus), Legionella pneumophila (L. pneumophila), and Klebsiella pneumoniae (K. pneumoniae) reaches 82–140 CFU/mL, with the entire process completed within 30 min. In addition, the detection of 25 clinical environmental samples verifies the practicality of the designed integrated detection platform. With high sensitivity, strong specificity, and dual-mode capability for qualitative colorimetric screening and quantitative fluorescence analysis, this technology offers an efficient solution for point-of-care testing (POCT) of HAI pathogens, particularly in resource-limited settings and in on-site emergency diagnostics.
{"title":"Push-Button Microfluidic Platform with Dual-Signal Nanoprobes for Enhanced Sensitivity Detection of Healthcare-Associated Infection Pathogens at Point-of-Care","authors":"Liping Dai,Yun Wang,Xiaosong Wu,Qian Wang,Zhigang Li,Yong Liu,Long Zhang,Shuai Zheng,Shu Wang","doi":"10.1021/acs.analchem.5c05437","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c05437","url":null,"abstract":"Healthcare-associated infection (HAI) pathogens cause severe nosocomial outbreaks, jeopardizing patient safety and straining healthcare systems. Conventional loop-mediated isothermal amplification–lateral flow immunoassay (LAMP-ICA) allows rapid pathogen detection but is constrained by low sensitivity, a high false-positive rate, and an extended detection time. To address these limitations, we present a dual-mode (colorimetric/fluorescent) microfluidic biosensing platform based on silicon–gold/quantum dot core–shell nanoprobes (Si@Au/DQD NPs). The platform incorporates two key innovations: (1) The colorimetric/fluorescent dual-signal Si@Au/DQD nanoprobe enhances detection reliability and sensitivity through dual-signal complementary verification and multilayered QD design, halving the LAMP amplification time compared to traditional colloidal gold systems, and (2) a modular microfluidic chip integrates LAMP amplification and ICA detection within a closed system, effectively preventing leakage and contamination of amplification products. Performance evaluation showed that the fluorescence detection limit of this system for Staphylococcus aureus (S. aureus), Legionella pneumophila (L. pneumophila), and Klebsiella pneumoniae (K. pneumoniae) reaches 82–140 CFU/mL, with the entire process completed within 30 min. In addition, the detection of 25 clinical environmental samples verifies the practicality of the designed integrated detection platform. With high sensitivity, strong specificity, and dual-mode capability for qualitative colorimetric screening and quantitative fluorescence analysis, this technology offers an efficient solution for point-of-care testing (POCT) of HAI pathogens, particularly in resource-limited settings and in on-site emergency diagnostics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"90 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139076","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}
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