Post-oxidation of all-organic electrocatalysts to promote O−O coupling in water oxidation

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Yayımlandı:Nature Communications vol. 16, no. 1 (2025), p. 4389
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Nature Publishing Group
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022 |a 2041-1723 
024 7 |a 10.1038/s41467-025-59771-6  |2 doi 
035 |a 3204003528 
045 2 |b d20250101  |b d20251231 
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245 1 |a Post-oxidation of all-organic electrocatalysts to promote O−O coupling in water oxidation 
260 |b Nature Publishing Group  |c 2025 
513 |a Journal Article 
520 3 |a 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. 
653 |a Intermediates 
653 |a Oxidation 
653 |a Electrocatalysts 
653 |a Metals 
653 |a Sustainable energy 
653 |a Clean technology 
653 |a Catalysts 
653 |a Electron affinity 
653 |a Oxygen evolution reactions 
653 |a Functional groups 
653 |a Energy technology 
653 |a Coupling 
653 |a Environmental 
773 0 |t Nature Communications  |g vol. 16, no. 1 (2025), p. 4389 
786 0 |d ProQuest  |t Health & Medical Collection 
856 4 1 |3 Citation/Abstract  |u https://www.proquest.com/docview/3204003528/abstract/embedded/6A8EOT78XXH2IG52?source=fedsrch 
856 4 0 |3 Full Text - PDF  |u https://www.proquest.com/docview/3204003528/fulltextPDF/embedded/6A8EOT78XXH2IG52?source=fedsrch