Adiabatic versus non-adiabatic electron transfer at 2D electrode materials
Liu, D.-Q., Kang, M., Perry, D., Chen, C.-H., West, G., Xia, X., Chaudhuri, S., Laker, Z. P. L., Wilson, N. R., Meloni, G. N., Melander, M. M., Maurer, R. J., & Unwin, P. R. (2021). Adiabatic versus non-adiabatic electron transfer at 2D electrode materials. Nature Communications, 12, Article 7110. https://doi.org/10.1038/s41467-021-27339-9
Published inNature Communications
Xia, Xue |
DisciplineResurssiviisausyhteisöNanoscience CenterFysikaalinen kemiaSchool of Resource WisdomNanoscience CenterPhysical Chemistry
© 2021 the Authors
2D electrode materials are often deployed on conductive supports for electrochemistry and there is a great need to understand fundamental electrochemical processes in this electrode configuration. Here, an integrated experimental-theoretical approach is used to resolve the key electronic interactions in outer-sphere electron transfer (OS-ET), a cornerstone elementary electrochemical reaction, at graphene as-grown on a copper electrode. Using scanning electrochemical cell microscopy, and co-located structural microscopy, the classical hexaamineruthenium (III/II) couple shows the ET kinetics trend: monolayer > bilayer > multilayer graphene. This trend is rationalized quantitatively through the development of rate theory, using the Schmickler-Newns-Anderson model Hamiltonian for ET, with the explicit incorporation of electrostatic interactions in the double layer, and parameterized using constant potential density functional theory calculations. The ET mechanism is predominantly adiabatic; the addition of subsequent graphene layers increases the contact potential, producing an increase in the effective barrier to ET at the electrode/electrolyte interface. ...
PublisherNature Publishing Group
Publication in research information system
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Related funder(s)Academy of Finland
Funding program(s)Postdoctoral Researcher, AoF; Academy Project, AoF
Additional information about fundingD-Q.L. thanks the China Scholarship Council-University of Warwick joint scholarship programme. S.C. acknowledges funding by the EPSRC Centre for Doctoral Training in Diamond Science and Technology (EP/L015315/1). R.J.M. acknowledges funding via a UKRI Future Leaders Fellowship (MR/S016023/1) and computing resources provided by the Scientific Computing Research Technology Platform of the University of Warwick, the EPSRC-funded HPC Midlands Plus Centre for high-performance computing (EP/P020232/1) and the ARCHER2 UK National Supercomputing Service (https://www.archer2.ac.uk) via the EPSRC-funded High End Computing Materials Chemistry Consortium (EP/R029431/1). M.M.M. acknowledges funding by the Academy of Finland (projects 307853 and 317739) and the computational resources provided by CSC—IT Center for Science, Espoo, Finland (https://www.csc.fi/en/). P.R.U. thanks the Royal Society for a Wolfson Research Merit Award. M.K. acknowledges support from the Leverhulme Trust for an Early Career Fellowship. ...
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