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@PHDTHESIS{Cheong:1028357,
author = {Cheong, Oskar},
title = {{C}omputational {I}nvestigation of {S}olvation {P}henomena
at {M}etal-{E}lectrolyte {I}nterfaces},
volume = {631},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2024-04538},
isbn = {978-3-95806-759-2},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {xvii, 142},
year = {2024},
note = {Dissertation, RWTH Aachen University, 2024},
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.},
cin = {IEK-13},
cid = {I:(DE-Juel1)IEK-13-20190226},
pnm = {899 - ohne Topic (POF4-899)},
pid = {G:(DE-HGF)POF4-899},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-20240724104044222-8032640-0},
doi = {10.34734/FZJ-2024-04538},
url = {https://juser.fz-juelich.de/record/1028357},
}