Book/Dissertation / PhD Thesis

FZJ-2024-04538

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Computational Investigation of Solvation Phenomena at Metal-Electrolyte Interfaces

Cheong, O. (Corresponding author)FZJ*

2024
Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag Jülich
ISBN: 978-3-95806-759-2

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Please use a persistent id in citations: urn:nbn:de:0001-20240724104044222-8032640-0  doi:10.34734/FZJ-2024-04538

Abstract: The interplay between metal catalyst surfaces and its surrounding solvent environment has a considerable impact on interfacial electrochemical processes, affecting both activity and selectivity of electrochemical reactions, e.g., the carbon dioxide (CO2) reduction reaction. While atomistic simulations are useful to gain advanced insight into the metal-electrolyte interface, many challenging problems exist for a realistic, computational description of the complex electrochemical interface. Especially, a computationally feasible scheme for description of solvation effects at the metal-electrolyte interface has yet to be established. This thesis explores several computational improvements that enable accounting for solvation effects when modelling a metal-electrolyte interface. The first part of the thesis focuses on testing the ability of a classical molecular dynamics (CMD) simulation approach based on the interface force field (IFF) to efficiently model water structures on metal surfaces, using the lead (Pb) surface as a test case. While ab initiomolecular dynamics (AIMD) calculations are considered to be more accurate than CMD calculations, the latter allows for exploration of much longer time- and lengthscales, which results in better equilibrated water structures. This work demonstratesthe potential of using IFF-based CMD simulations for statistically complete sampling water structures on metal surfaces. In the second part of the thesis the impact of different solvation models on the CO2 reduction reaction on both silver (Ag) and lead (Pb) catalysts towards formic acid (HCOOH) and carbon monoxide (CO) products are investigated. The systematic analysis indicates that accounting for explicit solvation has a crucial impact on the CO2 reduction reaction, correctly predicting primary products on both metal catalysts, which was not achieved by simplified computation assuming vacuum environment. Furthermore, the performance of implicit, explicit and hybrid solvation schemes are discussed in that subproject.

Note: Dissertation, RWTH Aachen University, 2024

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Contributing Institute(s):

1. IEK-13 (IEK-13)

Research Program(s):

1. 899 - ohne Topic (POF4-899) (POF4-899)

Appears in the scientific report 2024

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