Lattice-hydrogen cycling mechanism enables pH-universal hydrogen evolution at ampere-level current densities

作者：Yan Zhang, Biao Feng, Jingyi Tian, Shiqi Zhou, Changkai Zhou, Yiqun Chen, Xiaoli Xia, Xizhang Wang, Lijun Yang, Luming Peng, Qiang Wu, Hongwen Huang, Zheng Hu · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-65909-3 · 被引用次数：10 · 研究领域：Electrocatalysts for Energy Conversion、Microbial Fuel Cells and Bioremediation、Advanced battery technologies research

Abstract Controllable supply of hydrogen intermediate across a wide pH range is crucial for electroreduction reactions, but is hindered by pH-dependent hydrogen species formation on conventional catalysts. We report a lattice-hydrogen cycling mechanism that dissociates hydrogen intermediate availability from electrolyte pH. By integrating proton-blocking Ru with thermally-hydrogenated H x WO 3 , we create a dynamic hydrogen reservoir, enabling efficient hydrogen supply. In-situ Raman spectroscopy, isotopic labeling, and theoretical simulations reveal the lattice hydrogen in H x WO 3 migrates swiftly to Ru active sites via low-energy-barrier pathways, while consumed hydrogen is spontaneously replenished via proton adsorption (acidic) or water dissociation (alkaline/neutral). Consequently, this catalyst achieves a competitive pH-universal performance for hydrogen evolution reaction, with low overpotentials (125 mV acidic, 142 mV alkaline, 219 mV neutral @1 A cm -2 ) alongside 500-hour stability.