Mechanism of the electrochemical hydrogenation of graphene
The electrochemical hydrogenation of graphene induces a robust and reversible conductor-insulator transition, of strong interest in logic-and-memory applications. However, its mechanism remains unknown. Here we show that it proceeds as a reduction reaction in which proton adsorption competes with the formation of H<sub>2</sub> molecules via an Eley-Rideal process. Graphene's electrochemical hydrogenation is up to 10<sup>6</sup> times faster than alternative hydrogenation methods and is fully reversible via the oxidative desorption of protons. We demonstrate that the proton reduction rate in defect-free graphene can be enhanced by an order of magnitude by the introduction of nanoscale corrugations in its lattice, and that the substitution of protons for deuterons results both in lower potentials for the hydrogenation process and in a more stable compound. Our results pave the way to investigating the chemisorption of ions in 2D materials at high electric fields, opening a new avenue to control these materials' electronic properties.
Authors
- Shiqi Huang (ORCID: https://orcid.org/0000-0001-8644-0020)
- Cem Sevik (ORCID: https://orcid.org/0000-0002-2412-9672)
- Daniel Bahamón (ORCID: https://orcid.org/0000-0001-5473-1202)
- Eli Hoenig
- Lourdes F. Vega (ORCID: https://orcid.org/0000-0002-7609-4184)
- Yu-Chian Soong (ORCID: https://orcid.org/0000-0001-6940-321X)
- Jincheng Tong (ORCID: https://orcid.org/0000-0001-7762-1460)
- Erik C. Neyts (ORCID: https://orcid.org/0000-0002-3360-3196)
- M. Lozada-Hidalgo (ORCID: https://orcid.org/0000-0003-3216-7537)
- R. N. Costa Filho (ORCID: https://orcid.org/0000-0002-4654-8691)
- Xun Zhang (ORCID: https://orcid.org/0000-0002-8545-6263)
- François Maria Peeters (ORCID: https://orcid.org/0000-0003-3507-8951)
- Alex Summerfield (ORCID: https://orcid.org/0000-0001-6091-3969)
- E. Griffin (ORCID: https://orcid.org/0000-0002-1246-0333)
- Roman Gorbachev (ORCID: https://orcid.org/0000-0003-3604-5617)
- Yi Li (ORCID: https://orcid.org/0000-0002-2092-4505)
- Zhong Jin (ORCID: https://orcid.org/0000-0001-8860-8579)
- Yang Ming Fu (ORCID: https://orcid.org/0000-0002-6688-5388)
- M. Alhashmi
Institutions
- University of Antwerp (BE)
- Khalifa University of Science and Technology (AE)
- Nanjing University of Information Science and Technology (CN)
- Universidade Federal do Ceará (BR)
- University of Manchester (GB)
- Henry Royce Institute (GB)
- University of Bath (GB)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-11-28
- DOI
- https://doi.org/10.1038/s41467-025-65771-3
- Citations
- 2
- Primary Topic
- Graphene research and applications
- Type
- article
- Field-Weighted Citation Impact
- 1.04
Funders
- UK Research and Innovation
- Royal Society
- Fonds Wetenschappelijk Onderzoek
- Conselho Nacional de Desenvolvimento Científico e Tecnológico
- Khalifa University of Science, Technology and Research
- Fundação Cearense de Apoio ao Desenvolvimento Científico e Tecnológico
- U.S. Army Combat Capabilities Development Command
- Army Research Office