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<p>Developing efficient and stable oxygen evolution reaction electrocatalysts under acidic conditions is crucial for advancing proton-exchange membrane water electrolysers commercialization. Here, we develop a representative strategy through <i>p</i>-orbital atoms (N, P, S, Se) doping in RuO<sub>2</sub> to precisely regulate the lattice oxygen-mediated mechanism-oxygen vacancy site mechanism pathway. In situ and ex situ measurements along with theoretical calculations demonstrate that Se doping dynamically adjusts the band gap between the Ru-<i>e</i><sub>g</sub> and O<i>-p</i> orbitals during the oxygen evolution reaction process. This modulation accelerates electron diffusion to the external circuit, promotes the lattice oxygen-mediated process, and enhances catalytic activity. Additionally, it facilitates electron feedback and stabilizes oxygen vacancies, thereby promoting the oxygen vacancy site mechanism process and enhancing catalytic stability. The resulting Se-RuO<sub>x</sub> catalyst achieves efficient proton-exchange membrane water electrolysers performance under industrial conditions with a minimal charge overpotential of 1.67 V to achieve a current density of 1 A cm<sup>−2</sup> and maintain long-term cyclability for over 1000 h. This work presents a unique method for guiding the future development of high-performance metal oxide catalysts.</p>

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Orbital-level band gap engineering of RuO2 for enhanced acidic water oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月24日

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  • Xing Wang,
  • Wei Pi,
  • Zhaobing Li,
  • Sheng Hu,
  • Haifeng Bao,
  • Weilin Xu,
  • Na Yao

摘要

Developing efficient and stable oxygen evolution reaction electrocatalysts under acidic conditions is crucial for advancing proton-exchange membrane water electrolysers commercialization. Here, we develop a representative strategy through p-orbital atoms (N, P, S, Se) doping in RuO2 to precisely regulate the lattice oxygen-mediated mechanism-oxygen vacancy site mechanism pathway. In situ and ex situ measurements along with theoretical calculations demonstrate that Se doping dynamically adjusts the band gap between the Ru-eg and O-p orbitals during the oxygen evolution reaction process. This modulation accelerates electron diffusion to the external circuit, promotes the lattice oxygen-mediated process, and enhances catalytic activity. Additionally, it facilitates electron feedback and stabilizes oxygen vacancies, thereby promoting the oxygen vacancy site mechanism process and enhancing catalytic stability. The resulting Se-RuOx catalyst achieves efficient proton-exchange membrane water electrolysers performance under industrial conditions with a minimal charge overpotential of 1.67 V to achieve a current density of 1 A cm−2 and maintain long-term cyclability for over 1000 h. This work presents a unique method for guiding the future development of high-performance metal oxide catalysts.