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<p>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<sub>x</sub>WO<sub>3</sub>, 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<sub>x</sub>WO<sub>3</sub> 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<sup>-2</sup>) alongside 500-hour stability.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月3日

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  • 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

摘要

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 HxWO3, we create a dynamic hydrogen reservoir, enabling efficient hydrogen supply. In-situ Raman spectroscopy, isotopic labeling, and theoretical simulations reveal the lattice hydrogen in HxWO3 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.