<p>The development of stable Ru-based anodes for acidic proton exchange membrane water electrolysis is promising, but strictly limited by Ru over-oxidation and structural collapse due to lattice oxygen participation under high current densities. Rational design of competitive Ru-based catalyst is, thereby, highly desired. Here, by exploring a customized self-assembly route, we report a type of mesoporous Ru-Ti-O solid solution catalyst delivering competitive performance (1 A cm<sup>-2</sup> for over 450 h at 0.4mg<sub>Ru</sub>cm<sup>-2</sup>). Mechanistic investigations reveal that the enhanced performance arises from the integration of atomic-scale electronic structure tuning and mesoscopic triple phase interface engineering. The electron delocalization forms a conductive network and suppresses Ru overoxidation through electron donation. Atomically dispersed Ru-O-Ti motifs favor the oxygen pathway mechanism over the lattice oxygen mechanism, suppressing lattice oxygen release and enhancing structural stability. Simultaneously, the ordered mesoporous architecture and radially aligned nanorod bundles establish a robust, super-hydrophilic triple phase interface, enabling effective water and gas exchange and mitigating concentration overpotentials. This cross-scale design strategy offers a possible route to non-Ir catalysts with measurable activity and long-term durability for scalable acidic water electrolysis.</p>

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Mesoporous ruthenium titanium oxide solid solution with efficient three phase reaction interface for water electrolysis

  • Jun-Ye Zhang,
  • Kaihang Yue,
  • Yuqi Zhao,
  • Rongyao Li,
  • Qixuan Li,
  • Yanjie Hu,
  • Wendi Wang,
  • Lu Liu,
  • Jialong Li,
  • Hao Zhao,
  • Ya Yan,
  • Zhe Xu,
  • Lianhai Zu,
  • Hui Yang,
  • Kun Lan,
  • Dongyuan Zhao

摘要

The development of stable Ru-based anodes for acidic proton exchange membrane water electrolysis is promising, but strictly limited by Ru over-oxidation and structural collapse due to lattice oxygen participation under high current densities. Rational design of competitive Ru-based catalyst is, thereby, highly desired. Here, by exploring a customized self-assembly route, we report a type of mesoporous Ru-Ti-O solid solution catalyst delivering competitive performance (1 A cm-2 for over 450 h at 0.4mgRucm-2). Mechanistic investigations reveal that the enhanced performance arises from the integration of atomic-scale electronic structure tuning and mesoscopic triple phase interface engineering. The electron delocalization forms a conductive network and suppresses Ru overoxidation through electron donation. Atomically dispersed Ru-O-Ti motifs favor the oxygen pathway mechanism over the lattice oxygen mechanism, suppressing lattice oxygen release and enhancing structural stability. Simultaneously, the ordered mesoporous architecture and radially aligned nanorod bundles establish a robust, super-hydrophilic triple phase interface, enabling effective water and gas exchange and mitigating concentration overpotentials. This cross-scale design strategy offers a possible route to non-Ir catalysts with measurable activity and long-term durability for scalable acidic water electrolysis.