<p>Developing durable acidic oxygen evolution reaction catalysts is critical for industrial proton exchange membrane water electrolyzers. We incorporate high-entropy atoms (Co, Ni, Cu, Mn, Sm) into RuO<sub>2</sub> (RuO<sub>2</sub>-HEAE) via annealing, achieving remarkably high stability (&gt;1500 h at 100 mA cm<sup>−</sup><sup>2</sup>). In situ differential electrochemical mass spectrometry and <i>operando</i> Attenuated Total Reflection Surface-Enhanced Infrared Absorption Spectroscopy reveal RuO<sub>2</sub>-HEAE follows a dual-site oxide path mechanism instead of the conventional adsorbate evolution mechanism. Quantitative Fourier-transformed extended X-ray absorption fine structure fitting and density functional theory calculations show this mechanistic shift stems from an elongated Ru-M distance in second coordination shell of RuO<sub>2</sub>-HEAE, enabling direct O-O coupling. This OPM-type catalyst delivers ~1500 h of stable operation at 1 A cm<sup>−</sup><sup>2</sup> and 50 °C, demonstrating superior durability versus most reported RuO<sub>2</sub>-based catalysts. This work provides fundamental insights for designing highly stable proton exchange membrane water electrolysis.</p>

错误:搜索内容不能为空,请输入英文关键词
错误:关键词超出字数限制,请精简
高级检索

High-entropy RuO2 catalyst with dual-site oxide path for durable acidic oxygen evolution reaction

  • Fangren Qian,
  • Dengfeng Cao,
  • Shuangming Chen,
  • Yalong Yuan,
  • Kai Chen,
  • Peter Joseph Chimtali,
  • Hengjie Liu,
  • Wei Jiang,
  • Beibei Sheng,
  • Luocai Yi,
  • Jiabao Huang,
  • Chengsi Hu,
  • Huxu Lei,
  • Xiaojun Wu,
  • Zhenhai Wen,
  • Qingjun Chen,
  • Li Song

摘要

Developing durable acidic oxygen evolution reaction catalysts is critical for industrial proton exchange membrane water electrolyzers. We incorporate high-entropy atoms (Co, Ni, Cu, Mn, Sm) into RuO2 (RuO2-HEAE) via annealing, achieving remarkably high stability (>1500 h at 100 mA cm2). In situ differential electrochemical mass spectrometry and operando Attenuated Total Reflection Surface-Enhanced Infrared Absorption Spectroscopy reveal RuO2-HEAE follows a dual-site oxide path mechanism instead of the conventional adsorbate evolution mechanism. Quantitative Fourier-transformed extended X-ray absorption fine structure fitting and density functional theory calculations show this mechanistic shift stems from an elongated Ru-M distance in second coordination shell of RuO2-HEAE, enabling direct O-O coupling. This OPM-type catalyst delivers ~1500 h of stable operation at 1 A cm2 and 50 °C, demonstrating superior durability versus most reported RuO2-based catalysts. This work provides fundamental insights for designing highly stable proton exchange membrane water electrolysis.