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@INPROCEEDINGS{Kadyk:1022607,
author = {Kadyk, Thomas and Olbrich, Wolfgang and Bernhard, David and
Kirsch, Sebastian and Krewer, Ulrike and Eikerling, Michael},
title = {{B}ridging {M}icrostructure {D}egradation and {M}acroscopic
{P}erformance {M}odeling in {P}olymer {E}lectrolyte {F}uel
{C}ell {C}atalyst {L}ayers},
reportid = {FZJ-2024-01573},
year = {2023},
abstract = {Electrochemical energy devices like fuel cells,
electrolyzers or batteries harness porous electrodes with
complex heterogeneous microstructures to optimize the
interplay between the transport processes and
electrochemical reaction. The use of nano-to-microstructured
electrodes increases performance as well as catalyst
utilization. However, such electrode structures are also
more susceptible to degradation and performance decline.
Statistical-physical models for microstructure degradation
must be interlinked to macrohomogeneous performance models.
This talk outlines the challenges in establishing this link,
as depicted in Fig. 1, and discusses possible solutions.The
catalyst layer of a PEFC is a complex composite electrode of
Pt-based catalyst nanoparticles on a carbon substrate,
ionically connected by ionomer and water as the active
reaction medium. During operation, catalyst nanoparticles
undergo changes due to dissolution, re-deposition of
dissolved catalyst (i.e., Ostwald ripening), coagulation or
inactivation of catalyst particles. The carbon substrate can
undergo corrosion and the ionomer can undergo restructuring,
which could affect the water retention behavior of the
electrode. The changes in catalyst particle properties,
especially the particle radius distribution, lead to a
decrease of the overall catalyst surface available for the
reaction, and thus to a performance decline. At a first
glance, the coupling between microstructure and performance
could be achieved by using the catalyst surface area as a
scaling factor for the exchange current density. However,
difficulties arise when incorporating degradation mechanisms
that alter structural properties and conditions other than
the catalyst particle size. For example, dealloying of
catalysts like PtCo or PtNi changes both particles size and
materials composition. When deconvoluting both effects in
accelerated stress tests on automotive cells, we found that
the change in catalyst activity, described by Tafel slope
and exchange current density, correlates with the change in
active surface area [1]. Changes in the ionomer morphology
can lead to altered wetting behavior and liquid water
retention, leaving the catalyst layer more prone to flooding
[2]. Additionally, proton conductivity changes, but its
description needs to take structural features of the ionomer
morphology into account [3]. Overall, linking structural
degradation effects to device-level performance requires
finding and tailoring appropriate descriptors and structure
property relationships.References: [1] D. Bernhard, T.
Kadyk, S. Kirsch, H. Scholz, U. Krewer. J. Power Sources
562:232771 (2023)[2] W. Olbrich, T. Kadyk, U. Sauter, M.
Eikerling. Electrochim. Acta 431:140850 (2022)[3] W.
Olbrich, T. Kadyk, U. Sauter, M. Eikerling, J. Gostick.
Scientific Reports 13:14127 (2023)Keywords: polymer
electrolyte fuel cell, solid oxide cell, catalyst
degradation, modelling, voltage loss prediction.},
month = {Dec},
date = {2023-12-11},
organization = {World Fuel Cell Conference 2023,
London (UK), 11 Dec 2023 - 13 Dec 2023},
subtyp = {After Call},
cin = {IEK-13},
cid = {I:(DE-Juel1)IEK-13-20190226},
pnm = {1231 - Electrochemistry for Hydrogen (POF4-123)},
pid = {G:(DE-HGF)POF4-1231},
typ = {PUB:(DE-HGF)6},
doi = {10.34734/FZJ-2024-01573},
url = {https://juser.fz-juelich.de/record/1022607},
}