Post-oxidation of all-organic electrocatalysts to promote O−O coupling in water oxidation
Abstract 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...
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| Main Authors: | , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59771-6 |
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| Summary: | Abstract 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. |
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| ISSN: | 2041-1723 |