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<p>The performance of electrocatalytic oxygen evolution reaction is governed by molecular evolution pathways, yet their regulation remains a significant experimental and theoretical hurdle. Herein, we propose the construction of asymmetric non-metallic dual-active sites through engineering hydroxyl groups in an all-organic electrocatalyst, thereby triggering an uncommon asymmetric oxide pathway mechanism. This reaction pathway reduces the requirement of strict equilibrium on adsorption energies at dual-active sites for traditional oxide pathway mechanism, and also avoids the limitation of the linear scaling relationship for adsorbate evolution mechanism. Therefore, the proposed metal-free electrocatalyst shows competitive oxygen evolution reaction performance with an overpotential of 364.3 ± 4.5 mV at 1.0 A·cm<sup>−2</sup>. Combining operando spectroscopic/mass spectrometry and theoretical calculations unveils that the asymmetric oxide pathway mechanism undergoes the critical step of *OH intramolecular nucleophilic attack to neighboring *O, forming *OOH with drastically reducing energy barriers. This work shows the diversity of oxygen evolution pathways in all-organic electrocatalysts and offers a viewpoint for optimizing the electrocatalytic performances of metal-free solids.</p>

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Engineering all-organic electrocatalysts with asymmetric dual-active sites for uncommon oxygen-evolving pathway

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月7日

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  • Li-Hong Yu,
  • Li-Ming Cao,
  • Xue-Feng Zhang,
  • Li-Dong Wang,
  • Jian Yang,
  • Zhiwei Hu,
  • Yuhai Dou,
  • Shu-Chih Haw,
  • Chun-Ting He

摘要

The performance of electrocatalytic oxygen evolution reaction is governed by molecular evolution pathways, yet their regulation remains a significant experimental and theoretical hurdle. Herein, we propose the construction of asymmetric non-metallic dual-active sites through engineering hydroxyl groups in an all-organic electrocatalyst, thereby triggering an uncommon asymmetric oxide pathway mechanism. This reaction pathway reduces the requirement of strict equilibrium on adsorption energies at dual-active sites for traditional oxide pathway mechanism, and also avoids the limitation of the linear scaling relationship for adsorbate evolution mechanism. Therefore, the proposed metal-free electrocatalyst shows competitive oxygen evolution reaction performance with an overpotential of 364.3 ± 4.5 mV at 1.0 A·cm−2. Combining operando spectroscopic/mass spectrometry and theoretical calculations unveils that the asymmetric oxide pathway mechanism undergoes the critical step of *OH intramolecular nucleophilic attack to neighboring *O, forming *OOH with drastically reducing energy barriers. This work shows the diversity of oxygen evolution pathways in all-organic electrocatalysts and offers a viewpoint for optimizing the electrocatalytic performances of metal-free solids.