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<p>High valence metal species are essential for driving electrocatalytic acidic water oxidation, but suffer from intrinsic thermodynamic instability. This activity-stability paradox is particularly severe for ruthenium-based catalysts, where highly active Ru(&gt;IV) species are also precursors for rapid dissolution. Here we show that a cooperative host-guest architecture circumvents this trade-off through dynamic, hydroxyl-mediated charge buffering. By anchoring isolated ruthenium atoms at β-MnO<sub>2</sub> edge sites, we demonstrate that host-derived surface hydroxyls govern both kinetics and robustness. These hydroxyls optimize intermediate binding to facilitate ideal O-O coupling, accelerating the reaction. Concurrently, the specific coordination environment allows the manganese host to reversibly accommodate excess oxidative charge, preventing irreversible structural degradation and ruthenium dissolution. The resulting Ru<sub>0.03</sub>Mn<sub>0.97</sub>O<sub>2</sub> catalyst achieves a mass activity 223-fold higher than RuO<sub>2</sub> and increases the stability number by three orders of magnitude. As an anode in a proton exchange membrane electrolyzer, it sustains an industrial-level current density of 1 A cm<sup>−2</sup> for over 1000 h, comparing favorably to IrO<sub>2</sub> while reducing precious metal usage by 80%.</p>

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Dynamic hydroxyl mediated charge buffering stabilizes high valence ruthenium edge sites for acidic water oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月17日

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  • Tianqing Yan,
  • Kang Xue,
  • Shishi Zhang,
  • Huayang Wang,
  • Zhen-Feng Huang,
  • Minhua Ai,
  • Ruijie Gao,
  • Chengxiang Shi,
  • Wanliang Mi,
  • Xiangwen Zhang,
  • Lun Pan,
  • Ji-Jun Zou

摘要

High valence metal species are essential for driving electrocatalytic acidic water oxidation, but suffer from intrinsic thermodynamic instability. This activity-stability paradox is particularly severe for ruthenium-based catalysts, where highly active Ru(>IV) species are also precursors for rapid dissolution. Here we show that a cooperative host-guest architecture circumvents this trade-off through dynamic, hydroxyl-mediated charge buffering. By anchoring isolated ruthenium atoms at β-MnO2 edge sites, we demonstrate that host-derived surface hydroxyls govern both kinetics and robustness. These hydroxyls optimize intermediate binding to facilitate ideal O-O coupling, accelerating the reaction. Concurrently, the specific coordination environment allows the manganese host to reversibly accommodate excess oxidative charge, preventing irreversible structural degradation and ruthenium dissolution. The resulting Ru0.03Mn0.97O2 catalyst achieves a mass activity 223-fold higher than RuO2 and increases the stability number by three orders of magnitude. As an anode in a proton exchange membrane electrolyzer, it sustains an industrial-level current density of 1 A cm−2 for over 1000 h, comparing favorably to IrO2 while reducing precious metal usage by 80%.