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<p>Designing efficient acidic oxygen evolution catalysts for proton exchange membrane water electrolyzers is challenging due to a trade-off between activity and stability. In this work, we construct high-density microcrystalline grain boundaries (GBs) with V-dopant in RuO<sub>2</sub> matrix (GB-V-RuO<sub>2</sub>). Our theoretical and experimental results indicate this is a highly active and acid-resistant OER catalyst. Specifically, the GB-V-RuO<sub>2</sub> requires low overpotentials of 159, 222, and 300 mV to reach 10, 100, and 1500 mA cm<sup>-2</sup><sub>geo</sub> in 0.5 M H<sub>2</sub>SO<sub>4</sub>, respectively. Operando EIS, ATR-SEIRAS FTIR and DEMS measurements reveal the importance of GBs in stabilizing lattice oxygen and thus inhibiting the lattice oxygen mediated OER pathway. As a result, the adsorbate evolution mechanism pathway becomes dominant, even at high current densities. Density functional theory analyses confirm that GBs can stabilize V dopant and that the synergy between them modulates the electronic structure of RuO<sub>2</sub>, thus optimizing the adsorption of OER intermediate species and enhancing electrocatalyst stability. Our work demonstrates a rational strategy for overcoming the traditional activity/stability dilemma, offering good prospects of developing high-performance acidic OER catalysts.</p>

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Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月14日

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  • Han Wu,
  • Zhanzhao Fu,
  • Jiangwei Chang,
  • Zhiang Hu,
  • Jian Li,
  • Siyang Wang,
  • Jingkun Yu,
  • Xue Yong,
  • Geoffrey I. N. Waterhouse,
  • Zhiyong Tang,
  • Junbiao Chang,
  • Siyu Lu

摘要

Designing efficient acidic oxygen evolution catalysts for proton exchange membrane water electrolyzers is challenging due to a trade-off between activity and stability. In this work, we construct high-density microcrystalline grain boundaries (GBs) with V-dopant in RuO2 matrix (GB-V-RuO2). Our theoretical and experimental results indicate this is a highly active and acid-resistant OER catalyst. Specifically, the GB-V-RuO2 requires low overpotentials of 159, 222, and 300 mV to reach 10, 100, and 1500 mA cm-2geo in 0.5 M H2SO4, respectively. Operando EIS, ATR-SEIRAS FTIR and DEMS measurements reveal the importance of GBs in stabilizing lattice oxygen and thus inhibiting the lattice oxygen mediated OER pathway. As a result, the adsorbate evolution mechanism pathway becomes dominant, even at high current densities. Density functional theory analyses confirm that GBs can stabilize V dopant and that the synergy between them modulates the electronic structure of RuO2, thus optimizing the adsorption of OER intermediate species and enhancing electrocatalyst stability. Our work demonstrates a rational strategy for overcoming the traditional activity/stability dilemma, offering good prospects of developing high-performance acidic OER catalysts.