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<p>The increasing demand for green hydrogen production requires the development of advanced ruthenium (Ru)-based oxide catalysts for the anodic oxygen evolution reaction (OER). Here, we report the development of a Ga-doped RuO<sub>2</sub> catalyst (Ga-RuO<sub>2</sub>) that demonstrates enhanced OER performance attributed to modulated Ru–O bond covalency. The fully occupied 3<i>d</i> orbital of Ga stabilizes its oxidation state during OER, while its atomic radius, similar to Ru, helps maintain the initial crystal lattice structure upon doping. <i>In-situ</i> characterization, kinetic analysis and theoretical calculations reveal that the weakened Ru–O bond covalency lowers the energy barriers for *OH and *OOH formation, thus contributing to an enhanced OER performance. The resultant Ga-RuO<sub>2</sub> achieves a current density of 10 mA cm<sup>−2</sup> at a low overpotential of 203 mV and demonstrates durable operation for 500 h in acid. This work provides valuable insights into the electronic structure engineering of Ru-based catalysts for practical water electrolysis applications.</p>

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Modulating Ru–O bond covalency via Ga-doping for enhanced oxygen evolution reaction in acid

  • 期刊论文

  • 发表日期：

    2025年5月28日

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  • Zhongliang Liu,
  • Heng Liu,
  • Kai Zhou,
  • Miaomiao Liu,
  • Tianrui Xue,
  • Yongjun Shen,
  • Hao Li,
  • Huihui Li,
  • Chunzhong Li

摘要

The increasing demand for green hydrogen production requires the development of advanced ruthenium (Ru)-based oxide catalysts for the anodic oxygen evolution reaction (OER). Here, we report the development of a Ga-doped RuO2 catalyst (Ga-RuO2) that demonstrates enhanced OER performance attributed to modulated Ru–O bond covalency. The fully occupied 3d orbital of Ga stabilizes its oxidation state during OER, while its atomic radius, similar to Ru, helps maintain the initial crystal lattice structure upon doping. In-situ characterization, kinetic analysis and theoretical calculations reveal that the weakened Ru–O bond covalency lowers the energy barriers for *OH and *OOH formation, thus contributing to an enhanced OER performance. The resultant Ga-RuO2 achieves a current density of 10 mA cm−2 at a low overpotential of 203 mV and demonstrates durable operation for 500 h in acid. This work provides valuable insights into the electronic structure engineering of Ru-based catalysts for practical water electrolysis applications.