Mechanism of the electrochemical hydrogenation of graphene

Y.-C. Soong, H. Li, Y. Fu (), J. Tong, S. Huang, X. Zhang, E. Griffin, E. Hoenig, M. Alhashmi, Y. Li, D. Bahamon, J. Zhong, A. Summerfield, R. N. Costa Filho, C. Sevik, R. Gorbachev, E. C. Neyts, L. F. Vega, F. M. Peeters and M. Lozada-Hidalgo ()
Additional contact information
Y.-C. Soong: The University of Manchester, Department of Physics and Astronomy
H. Li: The University of Manchester, Department of Physics and Astronomy
Y. Fu: The University of Manchester, Department of Physics and Astronomy
J. Tong: The University of Manchester, Department of Physics and Astronomy
S. Huang: The University of Manchester, Department of Physics and Astronomy
X. Zhang: The University of Manchester, Department of Physics and Astronomy
E. Griffin: The University of Manchester, Department of Physics and Astronomy
E. Hoenig: The University of Manchester, Department of Physics and Astronomy
M. Alhashmi: The University of Manchester, Department of Physics and Astronomy
Y. Li: Khalifa University of Science and Technology, Research and Innovation Center on CO2 and Hydrogen (RICH Center) and Chemical and Petroleum Engineering Department
D. Bahamon: Khalifa University of Science and Technology, Research and Innovation Center on CO2 and Hydrogen (RICH Center) and Chemical and Petroleum Engineering Department
J. Zhong: The University of Manchester, Department of Chemistry
A. Summerfield: The University of Manchester, National Graphene Institute
R. N. Costa Filho: Universidade Federal do Ceará, Departamento de Física
C. Sevik: Universiteit Antwerpen, Departement Fysica
R. Gorbachev: The University of Manchester, Department of Physics and Astronomy
E. C. Neyts: University of Antwerp, Department of Chemistry
L. F. Vega: Khalifa University of Science and Technology, Research and Innovation Center for Graphene and 2D Materials (RIC2D)
F. M. Peeters: Universidade Federal do Ceará, Departamento de Física
M. Lozada-Hidalgo: The University of Manchester, Department of Physics and Astronomy

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract 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 H2 molecules via an Eley-Rideal process. Graphene’s electrochemical hydrogenation is up to 106 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.

Date: 2025
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DOI: 10.1038/s41467-025-65771-3

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