Pub Date : 2026-10-05DOI: 10.1021/acssensors.6c04626
{"title":"Why Do I Reject So Many?","authors":"","doi":"10.1021/acssensors.6c04626","DOIUrl":"https://doi.org/10.1021/acssensors.6c04626","url":null,"abstract":"","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":""},"PeriodicalIF":10.9,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149100928","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}
Abstract Rapid and accurate diagnostics are essential for controlling emerging infectious diseases and antimicrobial resistance, yet CRISPR assays with exceptional analytical sensitivity often remain difficult to translate into deployable tests. Existing reviews have commonly organized CRISPR diagnostics by Cas effector, biosensor format, or application, offering limited guidance on how design decisions interact across complete workflows or why promising systems remain at the proof-of-concept stage. We introduce an integrated framework that connects five coupled design layers with five levels of translational evidence. The design layers comprise guide RNA engineering, signal amplification circuits, molecular adaptors, computational design support, and specimen and intended-use implementation. The evidence levels progress from purified-target characterization and spiked-matrix testing to retrospective specimen evaluation, prospective integrated-workflow evaluation, and intended-use operation by target users supported by controls, usability assessment, real-time stability, manufacturing consistency, cost per valid result, and claim-specific regulatory preparation. This dual framework shows how improvements at one layer can shift the dominant bottleneck to another. For example, preamplification can lower the analytical limit of detection while increasing contamination risk and workflow burden, whereas guide designs that improve sequence discrimination may reduce cognate-target activation. The framework supports bottleneck-guided selection of effectors, signal-gain strategies, adaptors, computational tools, and multiplexing formats according to target type and abundance, specimen matrix, intended decision, target users, and deployment setting. High analytical sensitivity or single-nucleotide discrimination under controlled conditions does not establish clinical utility unless such performance improves classification at the intended decision threshold within the complete workflow. Translation requires standardized benchmarking, matrix-aware validation, appropriate controls, stability and manufacturability assessment, prospective intended-use studies, and economic evaluation suited to the intended claim and setting. This framework shifts the evaluation of CRISPR diagnostics from isolated analytical performance toward evidence-based workflow co-design.
{"title":"Molecular Programming of CRISPR Diagnostics: From Target Recognition to Field Deployment","authors":"Hengyu Wang,Meiyou Chen,Qiurun He,Zuohao Wu,Junjie Zheng,Xiaoyi He,Ling Deng,Xuhu Mao,Yong Sheng","doi":"10.1021/acssensors.6c02636","DOIUrl":"https://doi.org/10.1021/acssensors.6c02636","url":null,"abstract":"Abstract Rapid and accurate diagnostics are essential for controlling emerging infectious diseases and antimicrobial resistance, yet CRISPR assays with exceptional analytical sensitivity often remain difficult to translate into deployable tests. Existing reviews have commonly organized CRISPR diagnostics by Cas effector, biosensor format, or application, offering limited guidance on how design decisions interact across complete workflows or why promising systems remain at the proof-of-concept stage. We introduce an integrated framework that connects five coupled design layers with five levels of translational evidence. The design layers comprise guide RNA engineering, signal amplification circuits, molecular adaptors, computational design support, and specimen and intended-use implementation. The evidence levels progress from purified-target characterization and spiked-matrix testing to retrospective specimen evaluation, prospective integrated-workflow evaluation, and intended-use operation by target users supported by controls, usability assessment, real-time stability, manufacturing consistency, cost per valid result, and claim-specific regulatory preparation. This dual framework shows how improvements at one layer can shift the dominant bottleneck to another. For example, preamplification can lower the analytical limit of detection while increasing contamination risk and workflow burden, whereas guide designs that improve sequence discrimination may reduce cognate-target activation. The framework supports bottleneck-guided selection of effectors, signal-gain strategies, adaptors, computational tools, and multiplexing formats according to target type and abundance, specimen matrix, intended decision, target users, and deployment setting. High analytical sensitivity or single-nucleotide discrimination under controlled conditions does not establish clinical utility unless such performance improves classification at the intended decision threshold within the complete workflow. Translation requires standardized benchmarking, matrix-aware validation, appropriate controls, stability and manufacturability assessment, prospective intended-use studies, and economic evaluation suited to the intended claim and setting. This framework shifts the evaluation of CRISPR diagnostics from isolated analytical performance toward evidence-based workflow co-design.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"36 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091864","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}
Abstract Fiber‑optic hydrogen sensors offer intrinsic safety and remote operation, yet their application is constrained by expensive spectrometers and complex demodulation. Here, we present a self-powered all‑fiber hydrogen sensor (SAHS) that integrates optical excitation, electrical readout and gas detection on a single fiber tip, enabling remote and room‑temperature sensing at zero bias. By constructing a whispering gallery mode (WGM)-enhanced lateral ZnO/PEDOT:PSS n–p heterojunction on the fiber tip, we achieve synergy between the localized optical field and the built‑in electric field. The WGM microcavity confines and recycles incident light, markedly enhancing light-matter interaction and photogeneration on the tiny fiber tip. Meanwhile, the lateral built‑in field efficiently dissociates the photogenerated carriers, producing a substantial photocurrent without any external voltage. The self‑powered sensor exhibits outstanding room‑temperature H2 detection under 380 nm light excitation upon Pd functionalization, with a detection limit of ∼19 ppm and response/recovery times of 30 s and 7 s, respectively. This light‑activated, electrically‑read‑out architecture eliminates costly optical demodulation equipment, offering a low‑cost, user‑friendly and intrinsically safe solution for advanced hydrogen energy monitoring.
{"title":"Self‑Powered All‑Fiber Hydrogen Sensor via Whispering Gallery Mode Microcavity and Built‑in Electric Field Synergy","authors":"Ying Liu,Zhibo Li,Jie Mao,Yuansheng Yin,Wanjun Li,Liang Huang,Shuang Shang,Jianle Huang,Yiyang Qin,Daotong You,Minghui Du,Tuan Guo","doi":"10.1021/acssensors.6c03580","DOIUrl":"https://doi.org/10.1021/acssensors.6c03580","url":null,"abstract":"Abstract Fiber‑optic hydrogen sensors offer intrinsic safety and remote operation, yet their application is constrained by expensive spectrometers and complex demodulation. Here, we present a self-powered all‑fiber hydrogen sensor (SAHS) that integrates optical excitation, electrical readout and gas detection on a single fiber tip, enabling remote and room‑temperature sensing at zero bias. By constructing a whispering gallery mode (WGM)-enhanced lateral ZnO/PEDOT:PSS n–p heterojunction on the fiber tip, we achieve synergy between the localized optical field and the built‑in electric field. The WGM microcavity confines and recycles incident light, markedly enhancing light-matter interaction and photogeneration on the tiny fiber tip. Meanwhile, the lateral built‑in field efficiently dissociates the photogenerated carriers, producing a substantial photocurrent without any external voltage. The self‑powered sensor exhibits outstanding room‑temperature H2 detection under 380 nm light excitation upon Pd functionalization, with a detection limit of ∼19 ppm and response/recovery times of 30 s and 7 s, respectively. This light‑activated, electrically‑read‑out architecture eliminates costly optical demodulation equipment, offering a low‑cost, user‑friendly and intrinsically safe solution for advanced hydrogen energy monitoring.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"48 6 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091863","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 : 2026-10-02DOI: 10.1021/acssensors.6c02981
Jianle Wang,Qiuyun Tian,Yuling Li,Yaqi Qin,Xiaorong Xiong,Shijia Ding,Wenchun Xu,Meiying Shen,Changjin Liu
Abstract CRISPR/Cas12a diagnostics have greatly advanced nucleic acid testing, yet their extension to non-nucleic acid targets remains constrained by the intricate preamplification process and by inefficient signal transduction. Herein, we present a non-nucleic acid detection platform that integrates a CRISPR/Cas12a positive-feedback cascade with a single-atom nanozyme. In this strategy, cleavage of the designed double-clasp transition probe (DCTP) activates additional Cas12a ribonucleoprotein (RNP) complexes, enabling cascade signal amplification without a preamplification treatment. Meanwhile, the created single-atom Pt-engineered PdCeB nanozyme (Pt1/PdCeB SAN) functions as an efficient electrochemiluminescence (ECL) nanolabel in the luminol/O2 system, converting dissolved oxygen (O2) into reactive oxygen species (ROS) to produce a robust ECL response without an external coreactant. Using human epidermal growth factor receptor 2 (HER2) as a clinically relevant non-nucleic acid target, the DCTP-driven Cas12a positive-feedback system shortened the cleavage time from 33 min in the conventional Cas12a system to 18 min and achieved a wide linear range from 10–3 to 104 ng/mL, with a low detection limit of 0.513 pg/mL. Furthermore, preliminary analysis of 31 clinical serum samples supported the feasibility of the strategy for quantitative serum HER2 (sHER2) determination, although validation in larger independent cohorts is required.
{"title":"Single-Atom Nanozyme Integrated Double-Clasp Transition Probe-Driven CRISPR/Cas12a Cascade for Preamplification-Free Detection of Non-Nucleic Acid Targets","authors":"Jianle Wang,Qiuyun Tian,Yuling Li,Yaqi Qin,Xiaorong Xiong,Shijia Ding,Wenchun Xu,Meiying Shen,Changjin Liu","doi":"10.1021/acssensors.6c02981","DOIUrl":"https://doi.org/10.1021/acssensors.6c02981","url":null,"abstract":"Abstract CRISPR/Cas12a diagnostics have greatly advanced nucleic acid testing, yet their extension to non-nucleic acid targets remains constrained by the intricate preamplification process and by inefficient signal transduction. Herein, we present a non-nucleic acid detection platform that integrates a CRISPR/Cas12a positive-feedback cascade with a single-atom nanozyme. In this strategy, cleavage of the designed double-clasp transition probe (DCTP) activates additional Cas12a ribonucleoprotein (RNP) complexes, enabling cascade signal amplification without a preamplification treatment. Meanwhile, the created single-atom Pt-engineered PdCeB nanozyme (Pt1/PdCeB SAN) functions as an efficient electrochemiluminescence (ECL) nanolabel in the luminol/O2 system, converting dissolved oxygen (O2) into reactive oxygen species (ROS) to produce a robust ECL response without an external coreactant. Using human epidermal growth factor receptor 2 (HER2) as a clinically relevant non-nucleic acid target, the DCTP-driven Cas12a positive-feedback system shortened the cleavage time from 33 min in the conventional Cas12a system to 18 min and achieved a wide linear range from 10–3 to 104 ng/mL, with a low detection limit of 0.513 pg/mL. Furthermore, preliminary analysis of 31 clinical serum samples supported the feasibility of the strategy for quantitative serum HER2 (sHER2) determination, although validation in larger independent cohorts is required.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"16 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092069","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 : 2026-10-02DOI: 10.1021/acssensors.6c02725
Minju Cho,Suyeon Kang,Joon Seup Hwang,Miyeon Jue,Jung Hyun Shin,Jun Ki Kim
Abstract Interstitial cystitis (IC) and overactive bladder (OAB) are chronic pelvic conditions with shared symptoms of urinary urgency, increased frequency, and nocturia with pain in the bladder. IC is characterized by bladder pain and inflammation without a clear etiology, whereas OAB involves detrusor overactivity in the absence of infection. Despite this symptomatic overlap, IC and OAB differ in underlying pathophysiology and require distinct treatment and medical care. A specific diagnostic strategy is currently lacking and highlights the need of a robust diagnostic method for effective treatment. Raman spectroscopy provides sensitive and nondestructive molecular fingerprints; when combined with artificial intelligence (AI)-driven analysis of spectral data, it offers a promising approach to overcoming the limitations of exclusion-based diagnoses. In this study, urinary samples were collected from healthy individuals (n = 117), IC patients (n = 19), and OAB patients (n = 45) for the acquisition of Raman spectra using Au-ZnO nanorod surface-enhanced Raman spectroscopy (SERS) chips. To obtain biological interpretable Raman spectra per group and high accuracy of classification performance, the linear models PCA-PLS-DA and PCA-LDA and tree-based nonlinear models XGBoost and LightGBM were applied and reached up to 92% accuracy with interpretable and pathologic relative Raman features for discriminating among healthy control, IC, and OAB. This approach suggests that urine-based SERS Raman spectra combined with machine learning could serve as a promising diagnostic platform to support disease-specific clinical decision.
{"title":"Multiclass Diagnostic Improvement of Interstitial Cystitis (IC) and Overactive Bladder (OAB) via Machine Learning Pipeline on Surface-Enhanced Raman Spectroscopy (SERS)","authors":"Minju Cho,Suyeon Kang,Joon Seup Hwang,Miyeon Jue,Jung Hyun Shin,Jun Ki Kim","doi":"10.1021/acssensors.6c02725","DOIUrl":"https://doi.org/10.1021/acssensors.6c02725","url":null,"abstract":"Abstract Interstitial cystitis (IC) and overactive bladder (OAB) are chronic pelvic conditions with shared symptoms of urinary urgency, increased frequency, and nocturia with pain in the bladder. IC is characterized by bladder pain and inflammation without a clear etiology, whereas OAB involves detrusor overactivity in the absence of infection. Despite this symptomatic overlap, IC and OAB differ in underlying pathophysiology and require distinct treatment and medical care. A specific diagnostic strategy is currently lacking and highlights the need of a robust diagnostic method for effective treatment. Raman spectroscopy provides sensitive and nondestructive molecular fingerprints; when combined with artificial intelligence (AI)-driven analysis of spectral data, it offers a promising approach to overcoming the limitations of exclusion-based diagnoses. In this study, urinary samples were collected from healthy individuals (n = 117), IC patients (n = 19), and OAB patients (n = 45) for the acquisition of Raman spectra using Au-ZnO nanorod surface-enhanced Raman spectroscopy (SERS) chips. To obtain biological interpretable Raman spectra per group and high accuracy of classification performance, the linear models PCA-PLS-DA and PCA-LDA and tree-based nonlinear models XGBoost and LightGBM were applied and reached up to 92% accuracy with interpretable and pathologic relative Raman features for discriminating among healthy control, IC, and OAB. This approach suggests that urine-based SERS Raman spectra combined with machine learning could serve as a promising diagnostic platform to support disease-specific clinical decision.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"31 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091865","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 : 2026-10-01DOI: 10.1021/acssensors.6c02644
Joydip Dey,Linh Hua,Md Tawfiq Anik,Ravi F. Saraf
Abstract A promising approach for the electrochemical detection of nucleic acids is to measure changes in the redox behavior of methylene blue (MB) tethered to the free end of an ssDNA probe immobilized on an Au electrode via an Au–S bond. The change in redox current results from the modulation of MB proximity to the electrode due to conformational changes upon probe-target binding. A critical limitation of these electrochemical beacon methods is the intrinsic conformational heterogeneity of probes that are partly adsorbed (DN) and standing-up (UP), which limits sensitivity and reliability. An opto-electrochemical instrument called SEED has been developed, in which a fast scan at 400 V/s inhibits (diffusion-controlled) MB redox from the UP chains to deconvolute the heterogeneity effect. The optical contrast is due to color flip-flops between blue MB and colorless leucomethylene-blue; thus, the background, due to high capacitance from ion vibration at a fast scan rate, is eliminated. To evaluate sensing performance, irrespective of sample volume and binding conditions, the sensitivity to the percentage of probe binding is measured and compared with cyclic voltammetry (CV). A “reactivity amplification” was discovered where ∼2% binding produces a 27% change in the SEED signal, enabling detection of 250 zeptomoles of binding on a ∼20 µm spot. The study underscores and leverages the subtle effects of the interfacial ionic microenvironment, especially the local pH, to rationally identify the appropriate buffer chemistry. By measuring local redox, SEED allows combinatorial electrochemical sensing of binding across an array of different probe sequences on a monolithic electrode.
{"title":"Tailoring the Interfacial Ionic Microenvironment of the ssDNA Brush to Quantify 250 Zeptomoles of Targets","authors":"Joydip Dey,Linh Hua,Md Tawfiq Anik,Ravi F. Saraf","doi":"10.1021/acssensors.6c02644","DOIUrl":"https://doi.org/10.1021/acssensors.6c02644","url":null,"abstract":"Abstract A promising approach for the electrochemical detection of nucleic acids is to measure changes in the redox behavior of methylene blue (MB) tethered to the free end of an ssDNA probe immobilized on an Au electrode via an Au–S bond. The change in redox current results from the modulation of MB proximity to the electrode due to conformational changes upon probe-target binding. A critical limitation of these electrochemical beacon methods is the intrinsic conformational heterogeneity of probes that are partly adsorbed (DN) and standing-up (UP), which limits sensitivity and reliability. An opto-electrochemical instrument called SEED has been developed, in which a fast scan at 400 V/s inhibits (diffusion-controlled) MB redox from the UP chains to deconvolute the heterogeneity effect. The optical contrast is due to color flip-flops between blue MB and colorless leucomethylene-blue; thus, the background, due to high capacitance from ion vibration at a fast scan rate, is eliminated. To evaluate sensing performance, irrespective of sample volume and binding conditions, the sensitivity to the percentage of probe binding is measured and compared with cyclic voltammetry (CV). A “reactivity amplification” was discovered where ∼2% binding produces a 27% change in the SEED signal, enabling detection of 250 zeptomoles of binding on a ∼20 µm spot. The study underscores and leverages the subtle effects of the interfacial ionic microenvironment, especially the local pH, to rationally identify the appropriate buffer chemistry. By measuring local redox, SEED allows combinatorial electrochemical sensing of binding across an array of different probe sequences on a monolithic electrode.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"21 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091916","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 : 2026-10-01DOI: 10.1021/acssensors.6c01817
Zhenghan Shi,Liya Ding,Li-ang Zhou,Ye Liu,Yuhang Wang,Yi Xu,Yunrui Cao,Zhinong Jiang,Qingjun Liu
Abstract Tumor necrosis factor-α (TNF-α) is an important inflammatory cytokine whose rapid and quantitative detection is essential for disease diagnosis and monitoring. However, conventional methods are often limited by bulky instrumentation and are not well suited for analysis in complex biological environments. Herein, a portable CRISPR/Cas12a-based aptasensor system was developed for detection of TNF-α by integrating aptamer recognition, Cas12a trans-cleavage signal amplification, and a miniaturized fluorescence detection device. An aptamer for TNF-α was designed to regulate the accessibility of the target sequence to the CRISPR RNA (crRNA), and the resulting change in Cas12a activity was converted into fluorescence signals. The portable device integrated light-emitting diode (LED) excitation and photodiode-based detection, with modulated signals wirelessly transmitted to a smartphone for readout. The aptasensor showed concentration-dependent responses, and the inhibition rate exhibited a linear relationship with TNF-α concentration. The applicability of the system was validated in cell culture supernatants and cervical tissue samples, including tumor and adjacent normal tissues. Distinct TNF-α levels were observed between these samples, showing good agreement with enzyme-linked immunosorbent assay (ELISA) results. This portable CRISPR/Cas12a aptasensor system provides a practical approach for point-of-care TNF-α detection and extends CRISPR-based sensing to protein biomarkers.
{"title":"Portable CRISPR/Cas12a-Based Aptasensor System for Point-of-Care Detection of Cytokine Tumor Necrosis Factor-Alpha (TNF-α)","authors":"Zhenghan Shi,Liya Ding,Li-ang Zhou,Ye Liu,Yuhang Wang,Yi Xu,Yunrui Cao,Zhinong Jiang,Qingjun Liu","doi":"10.1021/acssensors.6c01817","DOIUrl":"https://doi.org/10.1021/acssensors.6c01817","url":null,"abstract":"Abstract Tumor necrosis factor-α (TNF-α) is an important inflammatory cytokine whose rapid and quantitative detection is essential for disease diagnosis and monitoring. However, conventional methods are often limited by bulky instrumentation and are not well suited for analysis in complex biological environments. Herein, a portable CRISPR/Cas12a-based aptasensor system was developed for detection of TNF-α by integrating aptamer recognition, Cas12a trans-cleavage signal amplification, and a miniaturized fluorescence detection device. An aptamer for TNF-α was designed to regulate the accessibility of the target sequence to the CRISPR RNA (crRNA), and the resulting change in Cas12a activity was converted into fluorescence signals. The portable device integrated light-emitting diode (LED) excitation and photodiode-based detection, with modulated signals wirelessly transmitted to a smartphone for readout. The aptasensor showed concentration-dependent responses, and the inhibition rate exhibited a linear relationship with TNF-α concentration. The applicability of the system was validated in cell culture supernatants and cervical tissue samples, including tumor and adjacent normal tissues. Distinct TNF-α levels were observed between these samples, showing good agreement with enzyme-linked immunosorbent assay (ELISA) results. This portable CRISPR/Cas12a aptasensor system provides a practical approach for point-of-care TNF-α detection and extends CRISPR-based sensing to protein biomarkers.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"21 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091922","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}
Abstract Selective molecular recognition of trace volatile biomarkers in humid breath remains a fundamental coordination challenge at graphene interfaces. While exhaled breath contains a complex matrix of more than 3500 volatile organic compounds, clinical transition has been largely challenged by the selectivity-humidity paradox. This review traces the evolution of graphene transduction platforms from fundamental quantum phenomena to coordination-governed interfacial engineering strategies enabling selective molecular recognition. It critically analyzes the atomic-level interactions governing the interface, specifically how sublattice symmetry breaking, metal–ligand interactions, competitive water coordination, and 1/f noise spectroscopy enable detection limits at the parts-per-trillion level. It details nanoengineering strategies for superior performance, tracing the shift from pristine graphene to 2D/2D heterostructures and organic-functionalized scaffolds that introduce defined coordination environments to regulate analyte binding and suppress humidity interference. These coordination-engineered platforms are linked with clinical targets such as oncology and metabolic disorders, while machine intelligence serves as a supporting analytical layer within the sensor intelligence paradigm. Crucially, it addresses the path to clinical translation, emphasizing first-in-human safety milestones, green synthesis, and economic scalability afforded by adopting laser-induced graphene. By unifying 2D-material physics, coordination-driven selectivity, and sensor intelligence, graphene breathomics provides a chemically grounded framework for decentralized, personalized diagnostic technologies.
{"title":"Graphene-Enabled Breathomics: A Translational Roadmap from Fundamental Physics to Non-Invasive Point-of-Care Diagnostics","authors":"Vishal Chaudhary,Harsh Sable,Sonu Sonu,Balkishan Choudhary,Balaram Pani,Ajit Khosla","doi":"10.1021/acssensors.6c02104","DOIUrl":"https://doi.org/10.1021/acssensors.6c02104","url":null,"abstract":"Abstract Selective molecular recognition of trace volatile biomarkers in humid breath remains a fundamental coordination challenge at graphene interfaces. While exhaled breath contains a complex matrix of more than 3500 volatile organic compounds, clinical transition has been largely challenged by the selectivity-humidity paradox. This review traces the evolution of graphene transduction platforms from fundamental quantum phenomena to coordination-governed interfacial engineering strategies enabling selective molecular recognition. It critically analyzes the atomic-level interactions governing the interface, specifically how sublattice symmetry breaking, metal–ligand interactions, competitive water coordination, and 1/f noise spectroscopy enable detection limits at the parts-per-trillion level. It details nanoengineering strategies for superior performance, tracing the shift from pristine graphene to 2D/2D heterostructures and organic-functionalized scaffolds that introduce defined coordination environments to regulate analyte binding and suppress humidity interference. These coordination-engineered platforms are linked with clinical targets such as oncology and metabolic disorders, while machine intelligence serves as a supporting analytical layer within the sensor intelligence paradigm. Crucially, it addresses the path to clinical translation, emphasizing first-in-human safety milestones, green synthesis, and economic scalability afforded by adopting laser-induced graphene. By unifying 2D-material physics, coordination-driven selectivity, and sensor intelligence, graphene breathomics provides a chemically grounded framework for decentralized, personalized diagnostic technologies.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"31 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091608","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}
Abstract Dendrite growth and parasitic reactions in aqueous zinc-ion batteries (AZIBs) are intrinsically driven by heterogeneous interfacial Zn2+ distribution, but conventional characterization techniques cannot achieve real-time, micron-scale quantitative tracking of dynamic Zn2+ evolution. Herein, we report a high-performance Zn2+-selective scanning electrochemical microscopy (SECM) probe based on a multiwalled carbon nanotube (MWCNT)-modified all-solid-state ion-selective membrane. The MWCNT-modified interface effectively suppresses the water-layer effect, reducing the fitted interfacial resistance component from 17,442 to 389 Ω. The optimized probe exhibits a wide linear response range of 10–5–1 × 10–1 M (R2 = 0.999, slope = –19.8 mV·dec–1), an ultrafast response time of <10 s, low potential drift (<10 mV/2000 s), excellent anti-interference against common interfering ions (Na+, K+, Mg2+, Al3+), and a long service life of 45 days. Notably, in situ SECM mapping reveals severe Zn2+ concentration fluctuations (0.178–0.303 M) at the Zn anode in blank electrolyte, which are effectively homogenized to a narrow range of 0.235–0.255 M by 0.01 M mesylacetone additive. This work provides a powerful in situ platform for deciphering AZIB interfacial dynamics and guiding advanced electrolyte design.
{"title":"A High-Performance Zn2+-Selective Scanning Electrochemical Microscopy Probe:\u0000 In Situ\u0000 Deciphering of Interfacial Zn2+ Heterogeneity for Aqueous Zinc-Ion Battery Engineering","authors":"Jun-Jie Qu,Ze-Jie Zhu,Jing-Yan Zhou,Hao-Ran Yuan,Quan Zong,Mei-Mei Zhang,Yue Li,Jia-Ning Yan,Jing-Ji Zhang,Guo-Ying Wei,Jiang-Ying Wang,Fa-He Cao","doi":"10.1021/acssensors.6c02953","DOIUrl":"https://doi.org/10.1021/acssensors.6c02953","url":null,"abstract":"Abstract Dendrite growth and parasitic reactions in aqueous zinc-ion batteries (AZIBs) are intrinsically driven by heterogeneous interfacial Zn2+ distribution, but conventional characterization techniques cannot achieve real-time, micron-scale quantitative tracking of dynamic Zn2+ evolution. Herein, we report a high-performance Zn2+-selective scanning electrochemical microscopy (SECM) probe based on a multiwalled carbon nanotube (MWCNT)-modified all-solid-state ion-selective membrane. The MWCNT-modified interface effectively suppresses the water-layer effect, reducing the fitted interfacial resistance component from 17,442 to 389 Ω. The optimized probe exhibits a wide linear response range of 10–5–1 × 10–1 M (R2 = 0.999, slope = –19.8 mV·dec–1), an ultrafast response time of &lt;10 s, low potential drift (&lt;10 mV/2000 s), excellent anti-interference against common interfering ions (Na+, K+, Mg2+, Al3+), and a long service life of 45 days. Notably, in situ SECM mapping reveals severe Zn2+ concentration fluctuations (0.178–0.303 M) at the Zn anode in blank electrolyte, which are effectively homogenized to a narrow range of 0.235–0.255 M by 0.01 M mesylacetone additive. This work provides a powerful in situ platform for deciphering AZIB interfacial dynamics and guiding advanced electrolyte design.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"405 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092142","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 : 2026-09-30DOI: 10.1021/acssensors.6c02504
Jingyao Peng,Xue Fan,Hongye Liu,Yanru Zhang,Ying Sun,Wenbo Song,Daqian Song
Abstract Simultaneously recognizing multiple targets and independently decoding their signals in food is critically demanded for safeguarding public health against antimicrobial resistance. Photoelectrochemical (PEC) sensors, promising for on-site detection, face a fundamental constraint: all targets generate unidimensional current signals at the electrode, rendering multiple target signals prone to overlap and difficult to distinguish. To address this issue, we developed a magnetic-bead-assisted dual-target distinguishable Y-shaped probe (MDDYP) based on orthogonal stimuli-responsive triggers, enabling independent detection of tobramycin (TOB) and tetracycline (TET) on a PEC sensor. Three DNA strands are assembled into a Y-shaped nanostructure bearing hydroquinone (HQ)-encapsulated liposomes, in which the PC-linker and C-rich sequence function as orthogonal stimulus-responsive modules, which are selectively activated after TOB or TET recognition events, respectively. Either UV-induced photocleavage at the PC-linker or acidification-induced i-motif formation at the C-rich sequence drives target-concentration-dependent liposome release into the supernatant, achieving solution-phase signal separation without electrode surface modification. HQ liberated from the lysed liposomes is oxidized at the ITO/ZIF-67/Fe3O4/Fe-COFBTC photoanode, altering the electron transfer pathway and reversing the photocurrent polarity as the quantitative readout. The platform demonstrates a wide linear range of 1 fM–100 nM for TOB and 10 fM–100 nM for TET, with detection limits of 0.62 and 2.27 fM, respectively. Featuring simple operation, rapid response, and dual-target detection, this work offers a promising strategy with potential for future integration into on-site platforms for multiplexed detection of antibiotic residues.
同时识别食品中的多个靶点并独立解码其信号对于保护公众健康免受抗菌素耐药性的侵害至关重要。光电化学（PEC）传感器有望用于现场检测，但它面临着一个基本的限制：所有目标在电极处产生一维电流信号，使得多个目标信号容易重叠且难以区分。为了解决这个问题，我们开发了一种基于正交刺激响应触发器的磁珠辅助双靶标可区分y形探针（MDDYP），可以在PEC传感器上独立检测妥布霉素（TOB）和四环素（TET）。三条DNA链被组装成一个y形的纳米结构，其中pc -连接子和富含c的序列作为正交刺激响应模块，分别在TOB或TET识别事件后被选择性激活。无论是紫外线诱导的pc -连接子的光裂解，还是酸化诱导的富含c序列的i基序形成，都可以驱动靶浓度依赖性脂质体释放到上清中，从而实现无需电极表面修饰的溶液相信号分离。从溶解的脂质体中释放的HQ在ITO/ZIF-67/Fe3O4/Fe-COFBTC光阳极氧化，改变电子传递途径并反转光电流极性作为定量读出。该平台显示TOB的线性范围为1 fM - 100 nM， TET的线性范围为10 fM - 100 nM，检出限分别为0.62和2.27 fM。该研究具有操作简单、反应迅速、双靶点检测等特点，为未来整合到现场平台进行多重抗生素残留检测提供了一种有前景的策略。
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