Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence
Abstract Electrochemiluminescence (ECL) is a light-emitting process in which the stability of electrochemically generated radicals has a crucial impact on the efficiency and durability of excited state generation. Therefore, deciphering a relationship between radical stability and ECL performance is...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56009-3 |
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| author | Haocheng Xu Rengan Luo Haifeng Lv Tianrui Liu Qiaobo Liao Yandong Wang Ziyan Zhong Xiaojun Wu Jianping Lei Kai Xi |
| author_facet | Haocheng Xu Rengan Luo Haifeng Lv Tianrui Liu Qiaobo Liao Yandong Wang Ziyan Zhong Xiaojun Wu Jianping Lei Kai Xi |
| author_sort | Haocheng Xu |
| collection | DOAJ |
| description | Abstract Electrochemiluminescence (ECL) is a light-emitting process in which the stability of electrochemically generated radicals has a crucial impact on the efficiency and durability of excited state generation. Therefore, deciphering a relationship between radical stability and ECL performance is highly appealing. In this work, three sp2 carbon-conjugated covalent organic framework (COF) reticular nanoemitters compositing of same pyrene luminophores but different acrylonitrile linkers are designed with progressive electron affinities, named as CN-COF-1, 2, and 3. By precisely modulating the electron affinity of CN-COFs, a volcano relationship between ECL and radical stability is discovered with 78 folds enhancement in ECL intensity. Density functional theoretical calculations indicate that CN-COF-2 exhibits moderate radical stabilization capacity as well as efficient electron transport between the pyrene cores, facilitating ECL generation. Significantly, the appropriate radical stability of CN-COF-2 not only achieves the self-enhanced cathodic ECL but also promotes durability of the ECL intensity. The rational regulation of radical stability paves the way for developing efficient reticular nanoemitters and decoding the ECL fundamentals. |
| format | Article |
| id | doaj-art-91dbfe09f2b04606b7e3aeb7f5706b66 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-91dbfe09f2b04606b7e3aeb7f5706b662025-08-20T02:16:49ZengNature PortfolioNature Communications2041-17232025-02-011611910.1038/s41467-025-56009-3Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescenceHaocheng Xu0Rengan Luo1Haifeng Lv2Tianrui Liu3Qiaobo Liao4Yandong Wang5Ziyan Zhong6Xiaojun Wu7Jianping Lei8Kai Xi9State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Material Sciences, CAS Key Laboratory of Materials for Energy Conversion, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory, University of Science and Technology of ChinaState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Material Sciences, CAS Key Laboratory of Materials for Energy Conversion, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory, University of Science and Technology of ChinaState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityState Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing UniversityAbstract Electrochemiluminescence (ECL) is a light-emitting process in which the stability of electrochemically generated radicals has a crucial impact on the efficiency and durability of excited state generation. Therefore, deciphering a relationship between radical stability and ECL performance is highly appealing. In this work, three sp2 carbon-conjugated covalent organic framework (COF) reticular nanoemitters compositing of same pyrene luminophores but different acrylonitrile linkers are designed with progressive electron affinities, named as CN-COF-1, 2, and 3. By precisely modulating the electron affinity of CN-COFs, a volcano relationship between ECL and radical stability is discovered with 78 folds enhancement in ECL intensity. Density functional theoretical calculations indicate that CN-COF-2 exhibits moderate radical stabilization capacity as well as efficient electron transport between the pyrene cores, facilitating ECL generation. Significantly, the appropriate radical stability of CN-COF-2 not only achieves the self-enhanced cathodic ECL but also promotes durability of the ECL intensity. The rational regulation of radical stability paves the way for developing efficient reticular nanoemitters and decoding the ECL fundamentals.https://doi.org/10.1038/s41467-025-56009-3 |
| spellingShingle | Haocheng Xu Rengan Luo Haifeng Lv Tianrui Liu Qiaobo Liao Yandong Wang Ziyan Zhong Xiaojun Wu Jianping Lei Kai Xi Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence Nature Communications |
| title | Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence |
| title_full | Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence |
| title_fullStr | Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence |
| title_full_unstemmed | Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence |
| title_short | Deciphering a volcano-shaped relationship between radical stability and reticular electrochemiluminescence |
| title_sort | deciphering a volcano shaped relationship between radical stability and reticular electrochemiluminescence |
| url | https://doi.org/10.1038/s41467-025-56009-3 |
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