Mechanism of the electrochemical hydrogenation of graphene

Fuente: arXiv
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Autori principali: Soong, Y. -C., Li, H., Fu, Y., Tong, J., Huang, S., Zhang, X., Griffin, E., Hoenig, E., Alhashmi, M., Li, Y., Bahamon, D., Zhong, J., Summerfield, A., Filho, R. N. Costa, Sevik, C., Gorbachev, R., Neyts, E. C., Vega, L. F., Peeters, F. M., Lozada-Hidalgo, M.
Natura: Preprint
Pubblicazione: 2025
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author Soong, Y. -C.
Li, H.
Fu, Y.
Tong, J.
Huang, S.
Zhang, X.
Griffin, E.
Hoenig, E.
Alhashmi, M.
Li, Y.
Bahamon, D.
Zhong, J.
Summerfield, A.
Filho, R. N. Costa
Sevik, C.
Gorbachev, R.
Neyts, E. C.
Vega, L. F.
Peeters, F. M.
Lozada-Hidalgo, M.
author_facet Soong, Y. -C.
Li, H.
Fu, Y.
Tong, J.
Huang, S.
Zhang, X.
Griffin, E.
Hoenig, E.
Alhashmi, M.
Li, Y.
Bahamon, D.
Zhong, J.
Summerfield, A.
Filho, R. N. Costa
Sevik, C.
Gorbachev, R.
Neyts, E. C.
Vega, L. F.
Peeters, F. M.
Lozada-Hidalgo, M.
contents 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 $10^6$ 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.
format Preprint
id arxiv_https___arxiv_org_abs_2510_19505
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Mechanism of the electrochemical hydrogenation of graphene
Soong, Y. -C.
Li, H.
Fu, Y.
Tong, J.
Huang, S.
Zhang, X.
Griffin, E.
Hoenig, E.
Alhashmi, M.
Li, Y.
Bahamon, D.
Zhong, J.
Summerfield, A.
Filho, R. N. Costa
Sevik, C.
Gorbachev, R.
Neyts, E. C.
Vega, L. F.
Peeters, F. M.
Lozada-Hidalgo, M.
Chemical Physics
Mesoscale and Nanoscale Physics
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 $10^6$ 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.
title Mechanism of the electrochemical hydrogenation of graphene
topic Chemical Physics
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2510.19505