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

Chun-Ting He (), Li-Hong Yu, Haiming Liu, Qing Wang, Zi-Ming Ye, Jia Zhang (), Li-Dong Wang, Mei-Qian He, Xue-Feng Zhang, Hong-Gang Du, Zi-Wei Lu, Jian Yang, Hai-Hua Huang and Xiao-Ming Chen
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Chun-Ting He: Jiangxi Normal University
Li-Hong Yu: Jiangxi Normal University
Haiming Liu: ShanghaiTech University
Qing Wang: ShanghaiTech University
Zi-Ming Ye: Fujian Normal University
Jia Zhang: Jiangxi Normal University
Li-Dong Wang: Jiangxi Normal University
Mei-Qian He: Jiangxi Normal University
Xue-Feng Zhang: Jiangxi Normal University
Hong-Gang Du: Jiangxi Normal University
Zi-Wei Lu: Jiangxi Normal University
Jian Yang: Jiangxi Normal University
Hai-Hua Huang: Jiangxi Normal University
Xiao-Ming Chen: Sun Yat-Sen University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-59771-6

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