Post-oxidation of all-organic electrocatalysts to promote O−O coupling in water oxidation
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| Publicat a: | Nature Communications vol. 16, no. 1 (2025), p. 4389 |
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| Publicat: |
Nature Publishing Group
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| Accés en línia: | Citation/Abstract Full Text - PDF |
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| Resum: | Covalently bonded metal-free electrocatalysts exhibit significant potential for sustainable energy technologies, yet their performances remain unsatisfactory compared with metal-based catalysts. Herein, we propose an all-organic electrocatalyst, MEC-2, that conforms to the infrequent oxide path mechanism in alkaline oxygen evolution reaction through post-oxidation modification. MEC-2 achieves an intrinsic overpotential of 257.7 ± 0.6 mV at 10 mA·cm−2 and possesses durability with negligible degradation over 100,000 CV cycles or 250 h of operation at 1.0 A·cm−2, being comparable to the advanced metal-based OER electrocatalysts. The 18O-labeled operando characterization and theoretical calculations unveil that post-oxidation modification enhances the electron affinity to OH intermediates, and adjusts the adsorption configuration and proximity distance of O intermediates, thereby promoting direct O−O radical coupling. In this work, we show a fresh perspective for understanding the role of non-metallic elements/functional groups in electrocatalysis, and to a certain extent, narrows the gap between all-organic electrocatalysts and metal-based electrocatalysts.Metal-free catalysts offer a sustainable option for water oxidation but typically underperform compared to metal-based ones. Here, the authors report an all-organic catalyst that uses a rare oxide pathway to achieve high efficiency and long-term stability, comparable to metal-based systems. |
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| ISSN: | 2041-1723 |
| DOI: | 10.1038/s41467-025-59771-6 |
| Font: | Health & Medical Collection |