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<p>The dynamic reconstruction of oxygen evolution electrocatalysts dictates their performance, yet conventional Ir-based materials face an inherent activity-stability trade-off due to surface amorphization into hydrous IrO<sub>x</sub> phases accompanied by lattice oxygen mechanisms. Here, we uncover a distinct reconstruction pathway for supported Ir nanoparticles, where a TiO<sub>x</sub>@Ti substrate drives a bulk phase transition from metallic Ir to crystalline rutile IrO<sub>2</sub> during electrocatalysis. Unlike surface-limited amorphization, this support-guided crystallization shifts the reaction mechanism from involving lattice oxygen mechanism to the complete adsorbate evolution mechanism, as confirmed by mechanistic and structural analyses. Consequently, the Ir/TiO<sub>x</sub>@Ti catalyst achieves both high activity and durability in acidic media, demonstrated in three-electrode systems and proton exchange membrane water electrolyzers. This work redefines support roles in electrocatalyst reconstruction, demonstrating that bulk phase engineering—rather than surface modification—resolves the long-standing efficiency-durability conflict in acidic oxygen evolution.</p>

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Support-tuned iridium reconstruction with crystalline phase dominating acidic oxygen evolution

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年9月1日

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  • Kexin Zhang,
  • Xiao Liang,
  • Yucheng Wang,
  • Yongcun Zou,
  • Xiao Zhao,
  • Hui Chen,
  • Xiaoxin Zou

摘要

The dynamic reconstruction of oxygen evolution electrocatalysts dictates their performance, yet conventional Ir-based materials face an inherent activity-stability trade-off due to surface amorphization into hydrous IrOx phases accompanied by lattice oxygen mechanisms. Here, we uncover a distinct reconstruction pathway for supported Ir nanoparticles, where a TiOx@Ti substrate drives a bulk phase transition from metallic Ir to crystalline rutile IrO2 during electrocatalysis. Unlike surface-limited amorphization, this support-guided crystallization shifts the reaction mechanism from involving lattice oxygen mechanism to the complete adsorbate evolution mechanism, as confirmed by mechanistic and structural analyses. Consequently, the Ir/TiOx@Ti catalyst achieves both high activity and durability in acidic media, demonstrated in three-electrode systems and proton exchange membrane water electrolyzers. This work redefines support roles in electrocatalyst reconstruction, demonstrating that bulk phase engineering—rather than surface modification—resolves the long-standing efficiency-durability conflict in acidic oxygen evolution.