Lattice-hydrogen cycling mechanism enables pH-universal hydrogen evolution at ampere-level current densities
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.
Authors
- Lijun Yang (ORCID: https://orcid.org/0000-0002-5392-558X)
- Zheng Hu (ORCID: https://orcid.org/0000-0002-4847-899X)
- Shiqi Zhou (ORCID: https://orcid.org/0000-0003-1220-3342)
- Xizhang Wang (ORCID: https://orcid.org/0000-0001-5084-2482)
- Luming Peng (ORCID: https://orcid.org/0000-0003-1935-1620)
- Xiaoli Xia
- Changkai Zhou (ORCID: https://orcid.org/0000-0003-0675-069X)
- Jingyi Tian (ORCID: https://orcid.org/0009-0002-6444-7381)
- Yan Zhang (ORCID: https://orcid.org/0000-0002-6607-0509)
- Yiqun Chen (ORCID: https://orcid.org/0000-0002-4979-0117)
- Qiang Wu (ORCID: https://orcid.org/0000-0001-6858-1719)
- Biao Feng (ORCID: https://orcid.org/0000-0002-8266-5326)
- Hongwen Huang (ORCID: https://orcid.org/0000-0003-3967-6182)
Institutions
- Ministry of Education and Child Care (CA)
- Nanjing University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-12-03
- DOI
- https://doi.org/10.1038/s41467-025-65909-3
- Citations
- 3
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 1.09
Funders
- Salt Science Research Foundation
- National Natural Science Foundation of China
- Government of Jiangsu Province
- Nanjing University
- Science and Technology Support Program of Jiangsu Province
- National Key Research and Development Program of China