Precision-Engineered Co-N4−x-Cx 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 limi...
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| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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American Association for the Advancement of Science (AAAS)
2025-01-01
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| Series: | Research |
| Online Access: | https://spj.science.org/doi/10.34133/research.0842 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Ziqi Kang |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-8f33fa6c52d74775b819f2702eab810d |
| institution | Kabale University |
| issn | 2639-5274 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | American Association for the Advancement of Science (AAAS) |
| record_format | Article |
| series | Research |
| spelling | doaj-art-8f33fa6c52d74775b819f2702eab810d2025-08-20T03:36:59ZengAmerican Association for the Advancement of Science (AAAS)Research2639-52742025-01-01810.34133/research.0842Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen SpeciesZiqi Kang0Shu Zhu1Shijun Wang2Zhizhi Xiang3Zixin Deng4Xuehao Tong5Zixu Wang6Yanghan Sun7Xiancheng Liu8Guangchao Zang9Chenzhong Li10Guixue Wang11Yuchan Zhang12Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Key Laboratory for Biorheological Science and Technology of Ministry of Education, National Local Joint Engineering Lab for Vascular Implants, College of Bioengineering, Chongqing University, Chongqing 400044, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.Bioelectronics and Biosensors Center, School of Medicine, Chinese University of Hong Kong, Shenzhen, Shenzhen 518172, China.Key Laboratory for Biorheological Science and Technology of Ministry of Education, National Local Joint Engineering Lab for Vascular Implants, College of Bioengineering, Chongqing University, Chongqing 400044, China.Biomedical Innovation and Entrepreneurship Practice Base, Lab Teaching & Management Center, Chongqing Medical University, Chongqing 400016, China.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.https://spj.science.org/doi/10.34133/research.0842 |
| spellingShingle | 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 Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species Research |
| title | Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species |
| title_full | Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species |
| title_fullStr | Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species |
| title_full_unstemmed | Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species |
| title_short | Precision-Engineered Co-N4−x-Cx Single Atoms Enhance Potential-Resolved Ru(bpy)32+ Electrochemiluminescence via Reactive Oxygen Species |
| title_sort | precision engineered co n4 x cx single atoms enhance potential resolved ru bpy 32 electrochemiluminescence via reactive oxygen species |
| url | https://spj.science.org/doi/10.34133/research.0842 |
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