Shengjun Yang , Tingting Du , Yunhua He , Chencen Lai , Min Zhang , Wen-Chao Yang , Xiuli Gao
{"title":"Dual-site 19F NMR/colorimetric probe with chemical shift encoding for multiplexed detection of biothiols and SO2 derivatives","authors":"Shengjun Yang , Tingting Du , Yunhua He , Chencen Lai , Min Zhang , Wen-Chao Yang , Xiuli Gao","doi":"10.1016/j.aca.2025.344726","DOIUrl":"10.1016/j.aca.2025.344726","url":null,"abstract":"<div><h3>Background</h3><div>Biological substances and its metabolites, such as reactive sulfur species (e.g., biothiols, SO<sub>2</sub> derivatives), play pivotal roles in physiological processes through interdependent interactions. Their precise detection is critical for elucidating functional dynamics. However, their overlapping coexistence, structural similarity, and mutual interference pose significant challenges for simultaneous discrimination. Thus, it is imperative to develop a novel analytical approach enabling multiplexed discrimination in complex systems.</div></div><div><h3>Result</h3><div>We herein report a dual-site <sup>19</sup>F NMR/colorimetric probe to detect RSS species by ‘naked’ eye and then simultaneously resolve them in mixed solution through <sup>19</sup>F NMR spectroscopy. This innovative platform exhibits rapid responsiveness towards biothiols and SO<sub>2</sub> derivatives, manifesting distinct color change alongside characteristic <sup>19</sup>F NMR chemical shifts. The produced distinguishable <sup>19</sup>F NMR signatures permit simultaneous detection and resolution of biothiols and SO<sub>2</sub> derivatives in mixtures.</div></div><div><h3>Significance</h3><div>We report a fluorinated dual-site probe enabling multiplexed analysis via <sup>19</sup>F NMR and colorimetry. This strategy overcomes structural analog discrimination challenges in biomolecules, exemplified with sulfur-containing species. The design establishes a generalizable platform for resolving complex mixtures and advances chemosensory systems for simultaneous detection of coexisting bioactive analytes.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344726"},"PeriodicalIF":6.0,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183180","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanni Ma , Xiaolei Zhang , Longrun Shi , Jiayang Yan , Keyun Wang , Mingliang Ye
{"title":"Sequential denaturation and protein precipitation assay (SDPP) improves the sensitivity for ligand target identification at the proteome level","authors":"Yanni Ma , Xiaolei Zhang , Longrun Shi , Jiayang Yan , Keyun Wang , Mingliang Ye","doi":"10.1016/j.aca.2025.344722","DOIUrl":"10.1016/j.aca.2025.344722","url":null,"abstract":"<div><h3>Background</h3><div>Proteins can be denatured and precipitated under different denaturation conditions, and ligand bound proteins are more resistant to denaturing induced precipitation. Consequently, ligand target proteins can be identified by measuring solubility shifts. Nowadays, numerous methods have been developed to screen ligand target proteins based on different denaturation mechanisms. However, due to the different responses of proteins to different denaturation conditions, there is a significant complementary between these methods. Direct pooling of the denatured supernatants from different denaturation strategies can utilize this complementary, however, the pooling procedure inevitably averages the ligand-induced solubility shift across conditions, significantly compromising target identification sensitivity.</div></div><div><h3>Results</h3><div>To avoid pooling-induced signal compression and enhance identification sensitivity, we developed a novel solubility shift-based approach, termed Sequential Denaturation and Protein Precipitation assay (SDPP). In this strategy, multi-step sequential denaturation of individual sample was conducted, which greatly improves the identification sensitivity. We evaluated the performance of this method by screening the target proteins of Staurosporine, SDPP with thermal treatment followed by organic solvent treatment (TEMP-SL) performs better than other sequential denaturation and one-step denaturation approach. The number of kinase targets identified by SDPP (TEMP-SL) increased by 54 %, 38 %, 48 % and 21 %, respectively compared with the TEMP, SL, and pH experiments and IPSSA. We further applied this approach to identify the target proteins of endogenous metabolite cAMP. Except for revealing the known cAMP-PRKAR1A/PRKAR1B interaction, we also observed that the solubility shift of the C2orf88 responds to the cAMP binding.</div></div><div><h3>Significance</h3><div>This method conducts sequential denaturation on individual samples to induce stepwise protein precipitation, preserving and progressively accumulating the solubility shifts generated at each denaturation step. This cumulative effect amplifies the overall detectable solubility shift signal and greatly improves identification sensitivity, demonstrating great potential as an efficient and high-throughput strategy for proteome-wide ligand target identification.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344722"},"PeriodicalIF":6.0,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xing Liu , Wenjing Ji , Yulin Tao , Yuxiang Gong , Qiannan Zhang , Ruoyao Lin , Yang Yang , Yiting Wang , Shasha Li , Yu Zhang , Hongli Liu , Zhixiang Du , Bin Liu , Jiamin Qin , Guangqiao Liu , Kai Zhang , Yongfeng Yang
{"title":"A novel Halo Tag-based photo-crosslinking system for efficient drug target identification via chemoproteomic profiling","authors":"Xing Liu , Wenjing Ji , Yulin Tao , Yuxiang Gong , Qiannan Zhang , Ruoyao Lin , Yang Yang , Yiting Wang , Shasha Li , Yu Zhang , Hongli Liu , Zhixiang Du , Bin Liu , Jiamin Qin , Guangqiao Liu , Kai Zhang , Yongfeng Yang","doi":"10.1016/j.aca.2025.344720","DOIUrl":"10.1016/j.aca.2025.344720","url":null,"abstract":"<div><h3>Background</h3><div>Target discovery of natural products is critical for novel drug development. However, it remains challenging due to the risk of disrupting bioactive molecule integrity during chemical modification. Moreover, many current methods for identifying drug targets rely on chemical synthesis to design the probes and enrichment systems. This is not friendly to researchers lacking experience in chemical synthesis, which limits their large-scale applications. To address these limitations, we present a novel chemoproteomic strategy to identify drug targets by integrating Halo Tag technology with photo-crosslinking chemistry.</div></div><div><h3>Results</h3><div>A bifunctional probe was synthesized by conjugating the Halo Tag ligand with a photo-crosslinker, 3-Phenyl-3-(trifluoromethyl)-3H-diazirine (TAD). TAD induced UV-triggered covalent binding with drug molecules. And Halo Tag ligand was enriched by Halo Protein magnetic beads, with less structural bias and reduced activity impairment. Taking sweroside (SWE) as an example, 159 target proteins were screened using this probe, and yin-yang 1 (YY1) was selected as the most potential target of SWE. Furtherly, <em>in vitro</em> small molecule-protein interaction analysis, including cell thermal shift assays (CETSA), surface plasmon resonance (SPR) and molecular docking were performed. These results demonstrated the strong binding affinity of YY1 and SWE. Moreover, SWE was demonstrated to relieve bile acid (BA) induced hepatocyte apoptosis by targeting YY1 to regulate its transcriptional activity to enhance Farnesoid X Receptor (FXR) expression. Furthermore, <em>in vivo</em> assays showed that SWE administration effectively ameliorated 3,5-diethoxycarbonyl-1,4-dihydro-collidine (DDC) induced cholestatic liver injury in mice. It was evidenced by markedly reducing the serum biochemical biomarkers and liver pathological change. Notably, SWE decreased YY1 expression and promoted FXR and BSEP expression. Thus, SWE exerted hepatoprotective effects by regulating YY1/FXR pathway.</div></div><div><h3>Significance</h3><div>In conclusion, our method without pre-derivatization simplifies workflows and preserves native pharmacophores. It is compatible with routine laboratory equipment and can be widely used in drug target discovery.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344720"},"PeriodicalIF":6.0,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaqiong Fan , Lijin Shang , Shuo Zhao , Jixing Fan , Senlin Zhang , Qiong Yang , Chengyang Wu , Yulin Liu , Tiejun Yang , Hongchao Ji
{"title":"PLSELM: A lightweight modeling approach for low-data calibration in near-infrared spectroscopy","authors":"Xiaqiong Fan , Lijin Shang , Shuo Zhao , Jixing Fan , Senlin Zhang , Qiong Yang , Chengyang Wu , Yulin Liu , Tiejun Yang , Hongchao Ji","doi":"10.1016/j.aca.2025.344728","DOIUrl":"10.1016/j.aca.2025.344728","url":null,"abstract":"<div><h3>Background</h3><div>Near infrared (NIR) spectroscopy is widely used as a rapid analytical technique in various fields for its advantages of on-line monitoring and non-destructive testing. It can provide rich chemical information and is of great significance for studying the structure, composition and changes of substances. Reliable calibration remains a major challenge in near-infrared (NIR) spectroscopy, especially under low-data conditions or across instruments with varying configurations. To address this, we propose PLSELM, a lightweight modeling calibration method, which combines Partial Least Squares (PLS) score matrices and Ensemble Extreme Learning Machine (ELM).</div></div><div><h3>Results</h3><div>To address this, we propose PLSELM, a lightweight modeling calibration method, which combines Partial Least Squares (PLS) score matrices and Ensemble Extreme Learning Machine (ELM). By modeling the relationship between latent PLS features and concentration values, PLSELM provides a fast, robust, and transferable calibration framework. To evaluating the performance, five diverse NIR spectral data, including 21 sets of concentration indicators from 10 different spectrometers, were used for benchmarking comparison. These NIR spectra have different wavelength ranges, resolutions, lengths, and a wide range of concentrations. Results demonstrate that PLSELM has excellent calibration performance, outperforming conventional <span>PLS</span>, Support Vector Regression, and deep learning-based models. PLSELM also has great suitability in low-data learning and calibration transfer analysis. In addition, PLSELM model has good robustness, which is manifested in that it is not sensitive to the randomness of sample division and the randomness of hidden layer nodes. PLSELM only took 0.5 s to finished the PLSELM and PLS models on corn data.</div></div><div><h3>Significance</h3><div>The comprehensive comparison results indicate that the PLSELM method is a robust NIR calibration method, which performs well in various spectral wavelength ranges, resolutions, lengths, and a wide range of concentrations. In summary, PLSELM offers a practical and scalable solution for NIR calibration, with excellent potential for use in real-world analytical applications involving limited data or heterogeneous instruments.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344728"},"PeriodicalIF":6.0,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188816","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kelly H. Lu , Hua Zhang , Gargey B. Yagnik , Mark J. Lim , Kenneth J. Rothschild , Wei Li , Andrew J. Schneider , Luigi Puglielli , Lingjun Li
{"title":"Deciphering the three-dimensional biomolecular distribution in the Alzheimer's disease brain: A multiomic approach integrating immunohistochemistry with MALDI MS imaging","authors":"Kelly H. Lu , Hua Zhang , Gargey B. Yagnik , Mark J. Lim , Kenneth J. Rothschild , Wei Li , Andrew J. Schneider , Luigi Puglielli , Lingjun Li","doi":"10.1016/j.aca.2025.344721","DOIUrl":"10.1016/j.aca.2025.344721","url":null,"abstract":"<div><div>Alzheimer's disease (AD) is characterized by complex and distinct spatial and molecular changes in the brain that contribute to its onset and progression, which includes disruptions in proteins, lipids, and neuroinflammatory pathways. In this study, we introduce a three-dimensional (3D) spatial multi-omics imaging approach that integrates lipid mass spectrometry imaging (MSI) with targeted proteomic analysis using 10-plex photo-cleavable mass tag (PC-MT) probes. Brain tissues from wild-type (WT) and AD model mice were sectioned at four coronal levels, spaced 1500 μm apart, enabling the reconstruction of a depth-resolved molecular atlas. Lipid MSI revealed region- and depth-specific alterations in phosphatidylcholine (PC), phosphatidylethanolamine (PE), and other lipid classes between AD and WT brains. In parallel, protein MSI using PC-MT probes identified spatially distinct changes in neuroinflammatory and neurodegenerative markers across the cortex, hippocampus, and thalamus at different depths. This integrative platform uncovered co-localization patterns of lipid dysregulation and protein overexpression unique to AD pathology, highlighting vulnerable brain subregions. Our findings demonstrate that combining targeted protein and untargeted lipid imaging in 3D enables the discovery of spatially coordinated molecular signatures in neurodegeneration, offering a powerful framework for biomarker discovery and therapeutic development.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344721"},"PeriodicalIF":6.0,"publicationDate":"2025-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183233","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Robin Joshi , Soon Yew Tang , Ujjalkumar Subhash Das , Daniel J. Boehmler , Antonijo Mrčela , Ronan Lordan , E. James Petersson , Aalim M. Weljie , Garret A. FitzGerald
{"title":"Multimodal landscape of atherosclerotic plaques: A spatial omics approach with mass spectrometry imaging","authors":"Robin Joshi , Soon Yew Tang , Ujjalkumar Subhash Das , Daniel J. Boehmler , Antonijo Mrčela , Ronan Lordan , E. James Petersson , Aalim M. Weljie , Garret A. FitzGerald","doi":"10.1016/j.aca.2025.344723","DOIUrl":"10.1016/j.aca.2025.344723","url":null,"abstract":"<div><div>Atherosclerotic plaques are complex and heterogeneous structures, originating as fatty streaks in the vasculature and formed by the accumulation of lipids and foam cells. Over time, these lesions progress as inflammation, smooth muscle cell proliferation and phenotypic switching, and extracellular matrix deposition contribute to plaque growth, culminating in their fracture, reactive thrombogenesis, and a cardiovascular event such as myocardial infarction and stroke. Traditional bulk mass spectrometry (MS) analysis has yielded critical insights into the molecular mechanisms of plaque formation and disease progression, but it is unable to determine the spatial heterogeneity and microenvironmental complexity within the lesion. Recent advances in mass spectrometry imaging (MSI) based omics, including spatial lipidomics, proteomics, and metabolomics, have enabled unprecedented visualization of molecular distribution in atherosclerotic plaques at cellular resolution. These techniques promise to elucidate the distinct cellular crosstalk, lesion vulnerability, and sex-specific disease mechanisms that contribute to plaque development and rupture. This review examines the recent advances in MS-based spatial omics and their application to atherosclerotic plaques in both experimental models and human samples. We highlight recent findings, explore their implications for precision medicine and translational research, and discuss current challenges in sample preparation and data integration. Despite challenges, we suggest approaches for integration of MS-based spatial omics using artificial intelligence (AI) to enhance data integration, interpretation, and translational applications in atherosclerosis research. These advances promise to broaden our understanding of atherosclerosis and identify novel therapeutic targets to limit the burden of cardiovascular disease.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344723"},"PeriodicalIF":6.0,"publicationDate":"2025-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183354","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Zeeshan Asghar , Habibulla Imran , Ali shan , Baoyang Lu , Sooman Lim
{"title":"Development of a wireless vitamin B2 sensor by using flexible and disposable screen-printed electrode modified with g-C3N4 based ternary composite","authors":"Muhammad Zeeshan Asghar , Habibulla Imran , Ali shan , Baoyang Lu , Sooman Lim","doi":"10.1016/j.aca.2025.344702","DOIUrl":"10.1016/j.aca.2025.344702","url":null,"abstract":"<div><div>Water-soluble vitamin B<sub>2</sub> (riboflavin, RF) is essential for the metabolism and well-being of living things because it facilitates the synthesis of red blood cells, maintains the normal operation of the skin, eyes, and nerves, and helps turn food into energy. Consequently, creating a portable, wireless, and sensitive RF detection technique is crucial for clinical diagnosis as well as the food sector. In this work, we present a novel, flexible, and disposable homemade screen-printed electrode (HSPE) interfaced with a portable, wireless sensor system for selective and sensitive RF detection. The HSPE was fabricated using a cellulose-coated mulberry paper substrate, onto which a ternary composite of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) was deposited to enhance its electrochemical properties. The developed sensor exhibited prominent analytical performance, with high selectivity, reproducibility, low detection limit (LOD, 2.78 nM), high sensitivity (1724.76 μA μM<sup>−1</sup> cm<sup>−2</sup>), rapid response time (5 s), and a wide linear detection range (0.01–0.8 μM, R<sup>2</sup> = 0.97). The HSPE demonstrated effective real-time RF detection in diverse food samples, including rice, beans, chicken, potatoes, and yogurt, achieving good recovery rates. Integrated with a portable, wireless sensor device based on the Arduino Nano 33 Internet of Things (IoT), the system detected RF via open-circuit potential (OCP) changes and transmitted data wirelessly for remote monitoring through an Android mobile application. The device successfully distinguished RF presence with a performance comparable to larger-scale systems, demonstrating high potential for commercial deployment.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1378 ","pages":"Article 344702"},"PeriodicalIF":6.0,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153903","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jin Yu , Jie Han , Qingxia Duan , Xiaoli Zhang , Jing Jing , Guangle Niu , Xiaoling Zhang
{"title":"An engineered single-wavelength-excitable dual-color fluorescent probe for simultaneous imaging of polarity and viscosity dynamics during ferroptosis","authors":"Jin Yu , Jie Han , Qingxia Duan , Xiaoli Zhang , Jing Jing , Guangle Niu , Xiaoling Zhang","doi":"10.1016/j.aca.2025.344710","DOIUrl":"10.1016/j.aca.2025.344710","url":null,"abstract":"<div><div>Understanding complex biological processes like ferroptosis requires simultaneous monitoring of microenvironmental parameters, particularly polarity and viscosity. However, existing fluorescent probes lack multifunctionality for independent, real-time tracking. To address this, we developed <strong>CouPy<sup>+</sup></strong>, the first single-molecule probe enabling dual-color imaging of polarity and viscosity dynamics during ferroptosis. Combining a twisted intramolecular charge transfer (TICT) mechanism with molecular rotors, <strong>CouPy <sup>+</sup></strong> emits distinct green (polarity-sensitive) and deep-red (viscosity-sensitive) signals under a single excitation. This design allows concurrent yet independent parameter visualization in live cells, overcoming limitations of traditional tools. <strong>CouPy <sup>+</sup></strong> exhibits dual-emission (green for polarity, deep-red for viscosity) under one excitation, enabling simultaneous, independent tracking in live cells. Mitochondria-localized, it discriminated cancer cells from normal cells via emission differences. During ferroptosis, <strong>CouPy <sup>+</sup></strong> achieved the first real-time, two-color visualization, revealing concurrent nuclear polarity decreases and viscosity increases. In vivo studies confirmed its utility by detecting ferroptosis-associated changes in zebrafish. Control experiments validated the probe's specificity, with no cross-interference between polarity and viscosity responses. In living cells, polarity-dependent green emission decreased to 25 % of baseline levels, while viscosity-dependent red emission increased by 15 % during ferroptosis. Time-lapse imaging captured dynamic parameter shifts, highlighting <strong>CouPy<sup>+</sup>’</strong>s sensitivity to microenvironmental changes. Additionally, the probe's photostability and low cytotoxicity ensured reliable long-term imaging. Its dual-response capability provides unprecedented insights into the spatiotemporal coupling of polarity and viscosity during ferroptosis, a previously unattainable feat with single-parameter probes. <strong>CouPy<sup>+</sup></strong> is the first single-molecule probe for dual-color imaging of polarity and viscosity during ferroptosis, addressing a critical gap in multifunctional tools. Its TICT-rotor design establishes a blueprint for future multi-parameter probes. <strong>CouPy <sup>+</sup></strong> provides a powerful tool for simultaneously tracking multiple microenvironmental parameters in live cells and zebrafish, facilitating a deeper mechanistic understanding of ferroptosis and related pathologies.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344710"},"PeriodicalIF":6.0,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chengxiang Li , Shujing Wang , Longfei Zhu , Kaiyue Liu , Liyuan Jing , Li Xie , Shenguang Ge , Jinghua Yu
{"title":"Cs3Bi2Br9 QDs/BiOBr heterojunction photoelectrochemical biosensor with APE1 enzyme-driven bipedal DNA walker signal amplification for miRNA-320d detection","authors":"Chengxiang Li , Shujing Wang , Longfei Zhu , Kaiyue Liu , Liyuan Jing , Li Xie , Shenguang Ge , Jinghua Yu","doi":"10.1016/j.aca.2025.344713","DOIUrl":"10.1016/j.aca.2025.344713","url":null,"abstract":"<div><h3>Background</h3><div>MicroRNAs (miRNAs), as pivotal biomarkers, demonstrate critical significance in early cancer diagnosis through their sensitive detection. An ultrasensitive photoelectrochemical (PEC) sensing platform for miRNA-320d detection was developed by integrating apurinic/apyrimidinic endonuclease 1 (APE1) enzyme-driven bipedal DNA walker amplification strategy.</div></div><div><h3>Results</h3><div>The platform employed a Cs<sub>3</sub>Bi<sub>2</sub>Br<sub>9</sub> QDs/BiOBr Z-scheme heterojunction as the photoactive material, which generated a robust anodic photocurrent. Upon immobilizing alkaline phosphatase (ALP)-conjugated gold nanoparticles carrying apurine/pyrimidine (AP) site-modified L1 (ALP-Au NPs-L1) probes on the heterojunction surface, catalytic hairpin assembly (CHA)-generated 3D bipedal DNA walker walked in the presence of miRNA-320d, hybridizing with L1 to form duplex structures. The APE1 enzyme then selectively cleaved these duplexes, triggering the release of ALP-Au NPs from the electrode surface. This spatial separation deactivated the catalytic capacity of ALP, inducing a pronounced photocurrent attenuation. By synergizing the exceptional PEC performance of the Cs<sub>3</sub>Bi<sub>2</sub>Br<sub>9</sub> QDs/BiOBr heterojunction, specific recognition and efficient cleavage of APE1 enzyme, and 3D walker-mediated signal amplification, this platform achieved ultrasensitive miRNA-320d detection with a detection limit of 0.1 fM and a linear range spanning 1 fM to 1 nM.</div></div><div><h3>Significance</h3><div>This study established novel conceptual frameworks for implementing emerging perovskite materials in PEC biosensing platforms targeting microRNA detection.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1379 ","pages":"Article 344713"},"PeriodicalIF":6.0,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ya-Qian Xie , Ya-Shu Wei , Hang Du , Yu-Yi Zhou , Lin-Yi Liu , Fu-Cun Wei , Yan-Ni Luo , Xue-Cai Tan , Ke-Jing Huang , De-Fen Feng
{"title":"On-off-on electrochemiluminescence biosensor with dual-cycle amplification for ultrasensitive prenatal detection of thalassemia mutations using lanthanide europium nanorods","authors":"Ya-Qian Xie , Ya-Shu Wei , Hang Du , Yu-Yi Zhou , Lin-Yi Liu , Fu-Cun Wei , Yan-Ni Luo , Xue-Cai Tan , Ke-Jing Huang , De-Fen Feng","doi":"10.1016/j.aca.2025.344712","DOIUrl":"10.1016/j.aca.2025.344712","url":null,"abstract":"<div><div>Herein, we develop an on-off-on electrochemiluminescence (ECL) biosensor with dual-cycle amplification for ultrasensitive prenatal detection of thalassemia mutations. The biosensor utilizes hydrothermally synthesized lanthanide europium nanorods (EuBTC), which possess abundant active sites and exhibit a 3.2-fold improvement in electron transfer efficiency compared to conventional spherical MOFs. By integrating catalytic hairpin assembly and exonuclease-driven target recycling amplification, the biosensor achieves sequential detection of CD122 (β-globin IVS-II-654 mutation) and CD17 (β-globin codon 17 mutation) in a single assay. The CHA-triggered ferrocene quenching (signal-off) enables CD122 quantification with 0.739 fM detection limit, while T7 exonuclease-mediated strand displacement restores ECL signals (signal-on) for CD17 detection at 0.301 fM sensitivity, representing 2-3 orders of magnitude improvement over existing PCR-based methods. Validation using actual maternal serum samples showed recoveries ranging from 97.7 % to 108.0 %, with relative standard deviation (RSD) < 4.1 %, confirming its reliability in non-invasive prenatal diagnosis. This dual-signal modulation strategy, combines with the antenna effect of EuBTC, provides a universal platform for multiplexed gene analysis through programmable DNA sequence replacement.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1378 ","pages":"Article 344712"},"PeriodicalIF":6.0,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}