{"title":"精密工程Co-N4-x -C x单原子通过活性氧增强电位分辨Ru(bpy) 32 +电化学发光。","authors":"Ziqi Kang, Shu Zhu, Shijun Wang, Zhizhi Xiang, Zixin Deng, Xuehao Tong, Zixu Wang, Yanghan Sun, Xiancheng Liu, Guangchao Zang, Chenzhong Li, Guixue Wang, Yuchan Zhang","doi":"10.34133/research.0842","DOIUrl":null,"url":null,"abstract":"<p><p>Electrochemiluminescence (ECL) immunoassays based on tris(bipyridine)ruthenium [Ru(bpy)<sub>3</sub> <sup>2+</sup>] is the luminophore representing the most advanced and widely adopted approach in the field of in vitro diagnostics (IVD). However, the scarcity of potential-resolved ECL promoters for Ru(bpy)<sub>3</sub> <sup>2+</sup> markedly limits its application in clinical diagnostics. Here, we report the first application of cobalt single-atom catalysts (SACs) designed via density functional theory (DFT) calculations to boost the multi-signal ECL of Ru(bpy)<sub>3</sub> <sup>2+</sup>. Mechanism investigations unveil that \"ROS accumulation\" induced by CoC<sub>4</sub> and \"ROS surge\" driven by CoN<sub>4</sub> are the key factors governing the cathodic and anodic ECL. As a proof of concept, a sandwich ratiometric immunosensor was developed to detect tumor marker CEA and demonstrated excellent clinical feasibility. This work provides insights into the development of tailored ECL promoters by introducing DFT prediction and elucidating the relationships between ORR/HPRR/OER processes and Ru(bpy)<sub>3</sub> <sup>2+</sup> ECL behavior, paving the way for designing precise immunoassays and advancing IVD techniques.</p>","PeriodicalId":21120,"journal":{"name":"Research","volume":"8 ","pages":"0842"},"PeriodicalIF":10.7000,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12351920/pdf/","citationCount":"0","resultStr":"{\"title\":\"Precision-Engineered Co-N<sub>4-<i>x</i></sub> -C <i><sub>x</sub></i> Single Atoms Enhance Potential-Resolved Ru(bpy)<sub>3</sub> <sup>2+</sup> Electrochemiluminescence via Reactive Oxygen Species.\",\"authors\":\"Ziqi Kang, Shu Zhu, Shijun Wang, Zhizhi Xiang, Zixin Deng, Xuehao Tong, Zixu Wang, Yanghan Sun, Xiancheng Liu, Guangchao Zang, Chenzhong Li, Guixue Wang, Yuchan Zhang\",\"doi\":\"10.34133/research.0842\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Electrochemiluminescence (ECL) immunoassays based on tris(bipyridine)ruthenium [Ru(bpy)<sub>3</sub> <sup>2+</sup>] is the luminophore representing the most advanced and widely adopted approach in the field of in vitro diagnostics (IVD). However, the scarcity of potential-resolved ECL promoters for Ru(bpy)<sub>3</sub> <sup>2+</sup> markedly limits its application in clinical diagnostics. Here, we report the first application of cobalt single-atom catalysts (SACs) designed via density functional theory (DFT) calculations to boost the multi-signal ECL of Ru(bpy)<sub>3</sub> <sup>2+</sup>. Mechanism investigations unveil that \\\"ROS accumulation\\\" induced by CoC<sub>4</sub> and \\\"ROS surge\\\" driven by CoN<sub>4</sub> are the key factors governing the cathodic and anodic ECL. As a proof of concept, a sandwich ratiometric immunosensor was developed to detect tumor marker CEA and demonstrated excellent clinical feasibility. This work provides insights into the development of tailored ECL promoters by introducing DFT prediction and elucidating the relationships between ORR/HPRR/OER processes and Ru(bpy)<sub>3</sub> <sup>2+</sup> ECL behavior, paving the way for designing precise immunoassays and advancing IVD techniques.</p>\",\"PeriodicalId\":21120,\"journal\":{\"name\":\"Research\",\"volume\":\"8 \",\"pages\":\"0842\"},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2025-08-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12351920/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Research\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.34133/research.0842\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/1/1 0:00:00\",\"PubModel\":\"eCollection\",\"JCR\":\"Q1\",\"JCRName\":\"Multidisciplinary\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Research","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.34133/research.0842","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/1/1 0:00:00","PubModel":"eCollection","JCR":"Q1","JCRName":"Multidisciplinary","Score":null,"Total":0}
Precision-Engineered Co-N4-x -C x Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species.
Electrochemiluminescence (ECL) immunoassays based on tris(bipyridine)ruthenium [Ru(bpy)32+] is the luminophore representing the most advanced and widely adopted approach in the field of in vitro diagnostics (IVD). However, the scarcity of potential-resolved ECL promoters for Ru(bpy)32+ markedly limits its application in clinical diagnostics. Here, we report the first application of cobalt single-atom catalysts (SACs) designed via density functional theory (DFT) calculations to boost the multi-signal ECL of Ru(bpy)32+. Mechanism investigations unveil that "ROS accumulation" induced by CoC4 and "ROS surge" driven by CoN4 are the key factors governing the cathodic and anodic ECL. As a proof of concept, a sandwich ratiometric immunosensor was developed to detect tumor marker CEA and demonstrated excellent clinical feasibility. This work provides insights into the development of tailored ECL promoters by introducing DFT prediction and elucidating the relationships between ORR/HPRR/OER processes and Ru(bpy)32+ ECL behavior, paving the way for designing precise immunoassays and advancing IVD techniques.
期刊介绍：
Research serves as a global platform for academic exchange, collaboration, and technological advancements. This journal welcomes high-quality research contributions from any domain, with open arms to authors from around the globe.
Comprising fundamental research in the life and physical sciences, Research also highlights significant findings and issues in engineering and applied science. The journal proudly features original research articles, reviews, perspectives, and editorials, fostering a diverse and dynamic scholarly environment.
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