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@PHDTHESIS{Cheong:989043,
author = {Cheong, Oskar},
othercontributors = {Eikerling, Michael and Schneider, Jochen M.},
title = {{C}omputational investigation of solvation phenomena at
metal-electrolyte interfaces},
volume = {631},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH, Zentralbibliothek, Verlag},
reportid = {RWTH-2024-06567},
isbn = {978-3-95806-759-2},
series = {Schriften des Forschungszentrums Jülich. Reihe Energie
$\&$ Umwelt = Energy $\&$ environment},
pages = {xvii, 142 Seiten : Illustrationen},
year = {2024},
note = {Druckausgabe: 2024. - Onlineausgabe: 2024. - Auch
veröffentlicht auf dem Publikationsserver der RWTH Aachen
University; 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 initio molecular dynamics (AIMD) calculations are
considered to be more accurate than CMD calculations, the
latter allows for exploration of much longer time- and
length- scales, which results in better equilibrated water
structures. This work demonstrates the 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. Another problem investigated
in this thesis is to account for solvation entropy effects
on surface chemical reactions. In that context, the Two
Phase Thermodynamic (2PT) model is applied and tested to
evaluate solute entropy effects in bulk solvent and at the
metal-electrolyte interface. Since entropy contributions to
Gibbs energies of chemical reactions at the metal-solvent
interface are usually either neglected or modeled using the
ideal gas approximation, solvent effects on the reaction
free energies are often insufficiently or incorrectly
accounted for. The 2PT method offers a solution to obtain
computationally efficient and accurate estimates of solvent
entropy effects, resulting in a more realistic description
of chemical reactions at metal-electrolyte interfaces. The
presented research aims to pave the way towards efficient
computation of electrochemical interfaces under realistic
conditions, which is an essential ability in the context of
accelerating computer-aided design of novel and efficient
electrocatalysts.},
cin = {526810 / 520000},
ddc = {620},
cid = {$I:(DE-82)526810_20191118$ / $I:(DE-82)520000_20140620$},
pnm = {120 - Materialien und Technologien für die Energiewende
(MTET) (POF4-100) / Forschungsbereich Energie (POF4-100) /
Programmorientierte Förderung IV (POF4) /
Programmorientierte Förderung (POF)},
pid = {G:(DE-HGF)POF4-120 / G:(DE-HGF)POF4-100 / G:(DE-HGF)POF4 /
G:(DE-HGF)POF},
typ = {PUB:(DE-HGF)11 / PUB:(DE-HGF)3},
doi = {10.18154/RWTH-2024-06567},
url = {https://publications.rwth-aachen.de/record/989043},
}
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