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

Author

Listed:
  • 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)

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.

Suggested Citation

  • 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 & Xiao-Ming Chen, 2025. "Post-oxidation of all-organic electrocatalysts to promote O−O coupling in water oxidation," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-59771-6
    DOI: 10.1038/s41467-025-59771-6
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