A1 Journal article (refereed)
Adiabatic versus non-adiabatic electron transfer at 2D electrode materials (2021)


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


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Publication details

All authors or editorsLiu, Dan-Qing; Kang, Minkyung; Perry, David; Chen, Chang-Hui; West, Geoff; Xia, Xue; Chaudhuri, Shayantan; Laker, Zachary P. L.; Wilson, Neil R.; Meloni, Gabriel N.; et al.

Journal or seriesNature Communications

eISSN2041-1723

Publication year2021

Volume12

Article number7110

PublisherNature Publishing Group

Publication countryUnited Kingdom

Publication languageEnglish

DOIhttps://doi.org/10.1038/s41467-021-27339-9

Publication open accessOpenly available

Publication channel open accessOpen Access channel

Publication is parallel published (JYX)https://jyx.jyu.fi/handle/123456789/79286

Publication is parallel publishedhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC8651748/


Abstract

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.


Keywordselectrochemistryelectrodesgraphenedensity functional theory


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Ministry reportingYes

Reporting Year2021

JUFO rating3


Last updated on 2024-03-04 at 19:45