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research article

Electrosorption at metal surfaces from first principles

Hoermann, Nicolas G.
•
Marzari, Nicola  
•
Reuter, Karsten
September 8, 2020
Npj Computational Materials

Electrosorption of solvated species at metal electrodes is a most fundamental class of processes in interfacial electrochemistry. Here, we use its sensitive dependence on the electric double layer to assess the performance of ab initio thermodynamics approaches increasingly used for the first-principles description of electrocatalysis. We show analytically that computational hydrogen electrode calculations at zero net-charge can be understood as a first-order approximation to a fully grand canonical approach. Notably, higher-order terms in the applied potential caused by the charging of the double layer include contributions from adsorbate-induced changes in the work function and in the interfacial capacitance. These contributions are essential to yield prominent electrochemical phenomena such as non-Nernstian shifts of electrosorption peaks and non-integer electrosorption valencies. We illustrate this by calculating peak shifts for H on Pt electrodes and electrosorption valencies of halide ions on Ag electrodes, obtaining qualitative agreement with experimental data already when considering only second order terms. The results demonstrate the agreement between classical electrochemistry concepts and a first-principles fully grand canonical description of electrified interfaces and shed new light on the widespread computational hydrogen electrode approach.

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Type
research article
DOI
10.1038/s41524-020-00394-4
Web of Science ID

WOS:000566966200001

Author(s)
Hoermann, Nicolas G.
Marzari, Nicola  
Reuter, Karsten
Date Issued

2020-09-08

Publisher

NATURE PUBLISHING GROUP

Published in
Npj Computational Materials
Volume

6

Issue

1

Start page

136

Subjects

Chemistry, Physical

•

Materials Science, Multidisciplinary

•

Chemistry

•

Materials Science

•

generalized gradient approximation

•

partial charge-transfer

•

ab-initio

•

evolution reaction

•

exchange current

•

valency

•

water

•

adsorption

•

reduction

•

alignment

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
Available on Infoscience
September 23, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/171838
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