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      Control of proton transport and hydrogenation in double-gated graphene

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          Abstract

          The basal plane of graphene can function as a selective barrier that is permeable to protons 1, 2 but impermeable to all ions 3, 4 and gases 5, 6 , stimulating its use in applications such as membranes 1, 2, 7, 8 , catalysis 9, 10 and isotope separation 11, 12 . Protons can chemically adsorb on graphene and hydrogenate it 13, 14 , inducing a conductor–insulator transition that has been explored intensively in graphene electronic devices 1317 . However, both processes face energy barriers 1, 12, 18 and various strategies have been proposed to accelerate proton transport, for example by introducing vacancies 4, 7, 8 , incorporating catalytic metals 1, 19 or chemically functionalizing the lattice 18, 20 . But these techniques can compromise other properties, such as ion selectivity 21, 22 or mechanical stability 23 . Here we show that independent control of the electric field, E, at around 1 V nm −1, and charge-carrier density, n, at around 1 × 10 14 cm −2, in double-gated graphene allows the decoupling of proton transport from lattice hydrogenation and can thereby accelerate proton transport such that it approaches the limiting electrolyte current for our devices. Proton transport and hydrogenation can be driven selectively with precision and robustness, enabling proton-based logic and memory graphene devices that have on–off ratios spanning orders of magnitude. Our results show that field effects can accelerate and decouple electrochemical processes in double-gated 2D crystals and demonstrate the possibility of mapping such processes as a function of E and n, which is a new technique for the study of 2D electrode–electrolyte interfaces.

          Abstract

          Independent control of the electric field and charge-carrier density in double-gated graphene allows the decoupling of proton transport and lattice hydrogenation, enabling both accelerated proton transport and proton-based logic operations.

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          Generalized Gradient Approximation Made Simple

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            Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis set

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              Projector augmented-wave method

              P. Blöchl (1994)
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                Author and article information

                Contributors
                tongjincheng@outlook.com
                marcelo.lozadahidalgo@manchester.ac.uk
                Journal
                Nature
                Nature
                Nature
                Nature Publishing Group UK (London )
                0028-0836
                1476-4687
                19 June 2024
                19 June 2024
                2024
                : 630
                : 8017
                : 619-624
                Affiliations
                [1 ]Department of Physics and Astronomy, University of Manchester, ( https://ror.org/027m9bs27) Manchester, UK
                [2 ]National Graphene Institute, University of Manchester, ( https://ror.org/027m9bs27) Manchester, UK
                [3 ]Yusuf Hamied Department of Chemistry, University of Cambridge, ( https://ror.org/013meh722) Cambridge, UK
                [4 ]Research and Innovation Center on CO2 and Hydrogen (RICH Center) and Chemical Engineering Department, Khalifa University, ( https://ror.org/05hffr360) Abu Dhabi, United Arab Emirates
                [5 ]Research and Innovation Center for Graphene and 2D materials (RIC2D), Khalifa University, ( https://ror.org/05hffr360) Abu Dhabi, United Arab Emirates
                [6 ]Departamento de Física, Universidade Federal do Ceará, ( https://ror.org/03srtnf24) Fortaleza, Brazil
                [7 ]Departement Fysica, Universiteit Antwerpen, ( https://ror.org/008x57b05) Antwerp, Belgium
                Author information
                http://orcid.org/0000-0001-7762-1460
                http://orcid.org/0000-0002-6202-2550
                http://orcid.org/0000-0003-3909-0093
                http://orcid.org/0000-0002-7524-8903
                http://orcid.org/0000-0001-5473-1202
                http://orcid.org/0000-0001-8644-0020
                http://orcid.org/0000-0002-4654-8691
                http://orcid.org/0000-0002-7609-4184
                http://orcid.org/0000-0001-5991-7778
                http://orcid.org/0000-0003-3507-8951
                http://orcid.org/0000-0002-9169-169X
                http://orcid.org/0000-0003-3216-7537
                Article
                7435
                10.1038/s41586-024-07435-8
                11186788
                38898294
                f2fdd4ec-c3d6-4b0f-b8f6-62dae94bb810
                © The Author(s) 2024

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 1 December 2023
                : 17 April 2024
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                © Springer Nature Limited 2024

                Uncategorized
                chemical physics,electronic properties and devices
                Uncategorized
                chemical physics, electronic properties and devices

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