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

Yan Zhang, Biao Feng, Jingyi Tian, Shiqi Zhou, Changkai Zhou, Yiqun Chen, Xiaoli Xia, Xizhang Wang, Lijun Yang, Luming Peng, Qiang Wu (), Hongwen Huang () and Zheng Hu ()
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Yan Zhang: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Biao Feng: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Jingyi Tian: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Shiqi Zhou: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Changkai Zhou: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Yiqun Chen: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Xiaoli Xia: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Xizhang Wang: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Lijun Yang: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Luming Peng: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Qiang Wu: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Hongwen Huang: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering
Zheng Hu: Nanjing University, State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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 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.

Date: 2025
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DOI: 10.1038/s41467-025-65909-3

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