Jun-Ye Zhang, Kaihang Yue, Yuqi Zhao, Rongyao Li, Qi Li, Yanjie Hu, Wendi Wang, Lu Liu, Jialong Li, Hao Zhao, Ya Yan, Zhe Xu, Lianhai Zu, Hui Yang, Kun Lan, Dongyuan Zhao
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. Developing robust anode catalysts that can operate at industrial-level current densities is essential for efficient hydrogen production. Here, the authors report a mesoporous ruthenium–titanium oxide solid solution with an engineered three-phase reaction interface for stable water electrolysis.