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@PHDTHESIS{Karaca:912054,
author = {Karaca, Ali},
title = {{E}ignung von nickelhaltigen {K}atalysatorsystemen in
sauren {M}edien zur {N}utzung im {B}etrieb von
{B}rennstoffzellen},
volume = {594},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2022-05281},
isbn = {978-3-95806-663-2},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {iv, 249},
year = {2022},
note = {Dissertation, RWTH Aachen University, 2022},
abstract = {Catalysts for the oxygen reduction reaction in fuel cells
are more favorable when platinum is replaced by alternative
materials such as non-precious metals and their catalytic
activity is increased. This work addresses a reduction of
platinum in the cathode of a direct methanol fuel cell by
using nickel. Two approaches are investigated:
platinum-nickel alloys and core-shell structures. Automated
ultrasonic spraycoating was used to produce mechanically
stable electrodes with reproducible electrochemical
properties. In addition, whole catalyst-coated membranes
(CCMs) were integrally fabricated using ultrasonic spray
technology. The ionomer to carbon ratio (I/C) in the
electrode was shown to have a significant effect on the
electrochemically active surface area (44.7 (I/C 0.87) and
53.0 m2 g-1 (I/C 0.5)). Core-shell catalysts have lower
powerdensities than the alloys. Long-term stability of at
least 1000 hours of operation with increase in performance
is given for both. Both catalyst types experience
significant nickel discharge from the surface of the
particles, which explains the performance increases. Both
alloy and core-shell catalysts exhibit increased methanol
tolerance compared to commercial platinum particles. In
addition, fabrication of membraneelectrode assemblies has
been demonstrated as an integral process by ultrasonic
spraying of the electrode and membrane. Thermal modification
could be used toimprove the conductivity of the membranes
but is not practical in real processes and results in
performance losses under the selected conditions.
Modification of the membranes with high-boiling solvents
also does not result in any improvements. Trace amounts or
degradation products of the solvents (DMAc, DMF) lead to
membrane poisoning and higher ionic resistivities (0.18
untreated, 0.30 with DMAc and 2.18 Ω cm2 with DMF).
Membranes with very good protonic conductivity and low
permeations are obtained using graphene oxide as an
additive. Thin membranes (20 30 μm) with graphene oxide
have up to $20\%$ better protonic conductivity and $50\%$
lower hydrogen permeation. However, the methanol permeation
does not decrease. In the long term, the results and
findings obtained in this work can lead to a significant
reduction in theplatinum content in fuel cells, a
simplification of the manufacturing process and an
improvement in the properties in terms of permeation,
performance, and stability of the membrane-electrode
assemblies},
cin = {IEK-14},
cid = {I:(DE-Juel1)IEK-14-20191129},
pnm = {1231 - Electrochemistry for Hydrogen (POF4-123)},
pid = {G:(DE-HGF)POF4-1231},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2023013169},
url = {https://juser.fz-juelich.de/record/912054},
}