Ab initio study of water dissociation on a charged Pd(111) surface

Fidanyan, Karen; Liu, Guoyuan; Rossi, Mariana

doi:10.1063/5.0139082

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Ab initio study of water dissociation on a charged Pd(111) surface

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Rossi, Mariana
NOMAD, Fritz Haber Institute, Max Planck Society;

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arXiv:2212.08855.pdf
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Citation

Fidanyan, K., Liu, G., & Rossi, M. (2023). Ab initio study of water dissociation on a charged Pd(111) surface. The Journal of Chemical Physics, 158(9): 094707. doi:10.1063/5.0139082.

Cite as: https://hdl.handle.net/21.11116/0000-000C-224B-A

Abstract

Interactions between molecules and electrode surfaces play a key role in
electrochemical processes and are a subject of extensive research, both
experimental and theoretical. In this manuscript, we address the water
dissociation reaction on a Pd(111) electrode surface, modelled as a slab
embedded in an external electric field. We aim at unraveling the relationship
between surface charge and zero-point-energy in aiding or hindering this
reaction. We calculate energy barriers with dispersion-corrected
density-functional theory and an efficient parallel implementation of the
nudged-elastic-band method. We show that the lowest dissociation barrier, and
consequently highest reaction rate, takes place when the field reaches a
strength that induces a geometric frustration of the water molecule adsorbed on
the surface. Zero-point energy contributions to the this reaction, on the other
hand, remain nearly constant across a wide range of electric field strengths,
despite significant changes in the reactant state.