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@PHDTHESIS{Winterhalder:1038889,
author = {Winterhalder, Franziska Elisabeth},
title = {{E}ntwicklung alternativer {B}renngaselektroden für die
{H}ochtemperatur-{E}lektrolyse},
volume = {655},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2025-01700},
isbn = {978-3-95806-805-6},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {vii, 161},
year = {2025},
note = {Dissertation, RWTH Aachen University, 2024},
abstract = {The production of hydrogen is vital for a CO2-neutral,
hydrogen-based energy system, essential for achieving
national and international climate goals. Solid oxide
electrolysis cells (SOECs) powered by renewable energy are
key to producing green hydrogen and can achieve electrical
efficiencies over $100\%$ when coupled with waste heat.
However, there are challenges concerning long-term stability
and cost efficiency. Current materials used in these cells
degrade significantly under SOEC conditions, leading to
reduced performance. In particular, the commonly used Ni-YSZ
fuel electrode shows considerable degradation due to Ni
agglomeration and migration. A potential solution is using
alternative fuel electrodes. This study aimed to develop
alternative perovskite-based fuel electrodes for steam
electrolysis in SOECs. Five alternative perovskite materials
were synthesized and characterized:
La0.6Sr0.38Fe0.8Mn0.2O3-δ – LSFM, La0.35Sr0.63TiO3-δ –
LST, Sr0.98Ti0.7Fe0.3O3-δ – STF30, Sr0.98Ti0.5Fe0.5O3-δ
– STF50 and Sr1.98FeNbO6-δ – SFN. In particular, the
stability under reducing conditions and the compatibility of
the perovskites with 8YSZ under the production conditions of
fuel electrode-supported SOECs were investigated. It was
found that SFN exhibits the highest stability in a reducing
atmosphere as well as low reactivity with 8YSZ under the
tested conditions. Based on the results of the
characterizations, SFN and STF50 were selected as fuel
electrode materials for all subsequent experiments. First,
the stability of the perovskites under realistic SOEC
conditions was tested. The results showed that both
materials can be considered chemically stable, although a
small amount of Fe3O4 secondary phase formation was observed
in STF50. Furthermore, the compatibility of SFN/STF50 with
8YSZ and GDC under SOEC conditions and the manufacturing
conditions for electrolyte-supported cells was investigated.
SFN showed no interactions with 8YSZ or GDC, while STF50 was
compatible only with GDC under the tested conditions.
Overall, a barrier layer between the perovskite electrode
and the 8YSZ electrolyte is beneficial for preventing or
reducing chemical reactions. Electrochemical measurements of
cells with SFN and STF50 fuel electrodes at different
temperatures (650–800 °C) and varying H2O content in the
fuel gas (3–90 $vol.-\%)$ indicated that the contact layer
significantly impacts resistance values. It was also
observed that both the ohmic resistance (RΩ) and the
polarization resistance (RPol) decrease with increasing
temperature but increase with a higher water vapor content.
A degradation study of a full cell with an STF50 fuel
electrode and an LSCF oxygen electrode over approximately
1700 h at 800 °C in 50 $vol.-\%$ H2O + H2 and a current of
i = -0.43 A∙cm-2 revealed comparatively high degradation
rates of 0.195 V kh-1, 0.162 Ω∙cm2 kh-1, and 0.361
Ω∙cm2 kh-1 for voltage, RPol, and RΩ, respectively. A
subsequent SEM analysis of the microstructure of the STF50
fuel electrode before and after the degradation study showed
no significant changes in the electrode microstructure,
except for diffused Ni particles. Whether the Ni particles
that diffused from the NiO/Ni contact layer into the STF50
fuel electrode and the GDC barrier layer have an impact on
the cell's performance cannot be confirmed or ruled out at
the current stage. In addition to producing
electrolyte-supported cells, the integration of STF50 and
SFN into the manufacturing route for fuel
electrode-supported cells (FESCs) was investigated. Planar
half-cells with STF50 fuel electrodes were successfully
produced, though they did not meet the required gas
tightness. In general, integrating perovskite-based
alternative fuel electrodes into the FESC manufacturing
process is not feasible without modifications. In summary,
this work demonstrates that STF50 and SFN have considerable
potential as alternative fuel electrodes in steam SOECs.
Although they exhibit a certain degree of stability and, in
the case of STF50, sufficient baseline performance, further
optimizations and long-term studies are necessary to
establish these materials as potential replacements for
Ni-YSZ fuel electrodes.},
cin = {IMD-2},
cid = {I:(DE-Juel1)IMD-2-20101013},
pnm = {1231 - Electrochemistry for Hydrogen (POF4-123)},
pid = {G:(DE-HGF)POF4-1231},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
doi = {10.34734/FZJ-2025-01700},
url = {https://juser.fz-juelich.de/record/1038889},
}