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@PHDTHESIS{RojekWckner:825972,
author = {Rojek-Wöckner, Veronika Anna},
title = {{E}ntwicklung und {C}harakterisierung von {N}ickel /
{G}adolinium-{C}eroxid-basierten {A}noden für die
metallgestützte {F}estoxid-{B}rennstoffzelle},
volume = {343},
school = {Universität Bochum},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2017-00244},
isbn = {978-3-95806-182-8},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {XVI, 133 S.},
year = {2016},
note = {Dissertation, Universität Bochum, 2016},
abstract = {The present work aims at the development of an
ageing-resistant and sulfur-tolerant high-performance anode
for the metal supported solid oxide fuel cell (MSC). As a
starting point, the current MSC concept of Plansee with an
Ni/YSZ cermet as anode material, which is already
established in the fuel cell technology, is used. The
work’s main innovation is the replacement of the purely
ionic conducting YSZ phase by a mixed ionic/electronic
conducting oxide Ce$_{1-x}$Gd$_{x}$O$_{2-\delta}$ (GDC). In
the first part of the work, a comparison of the sintering
behavior between GDC and the reference material YSZ was
made. The results from studies on powder compacts and by
means of dilatometry indicate that the sintering atmosphere
(air/hydrogen) does not affect the shrinkage of YSZ, whose
maximum sintering rate is reached at T$_{max}$ = 1330 °C.
In contrast, GDC’s shrinkage is strongly increased in
reducing hydrogen atmosphere compared to the shrinkage in
air. The maximum sintering rate T$_{max}$ is noted at 1100
°C for GDC in hydrogen. In reducing atmospheres and at high
temperatures, the enhanced solid state diffusion of GDC is
caused, according to literature, by the following factors:
(i) an increased quantity of oxygen vacancies, (ii) a change
of valence from Ce$^{4+}$ to Ce$^{3+}$ and (iii) a reduced
Gd/Ce lattice mismatch induced by the valence change of
Cerium. Based on these findings, a series of cermet anode
layer samples with different Ni/GDC ratios and sintering
conditions was prepared and characterized, from which a set
of Best Choice manufacturing parameters (sintering at 1100
°C, +3 K/min, 3 h, H$_{2}$) with a cermet ratio 60/40 wt.\%
for Ni/GDC was derived. An impedance spectroscopical
characterization of symmetrical cells for partial decoupling
of particular electrode processes was performed in a
single-compartment system. The Ni/GDC anode stands out both
by a much lower polarization resistance and a small
temperature dependence as compared to the Ni/YSZ anode. For
both anode types two electrode processes could be decoupled,
which differ in their relaxation times. One of the processes
is associated with a limitation due to gas diffusion and the
second process is linked to a hydrogen surface reaction. The
entire polarization of the Ni/GDC anode is dominated by a
gas diffusion limitation, which additionally is superimposed
by a further unknown electro-catalytic process. The greatest
optimization potential of the Ni/GDC anode, according to
conducted experiments, lies therefore within the
optimization of the anode microstructure. Single cell
measurements served to demonstrate the functionality of the
Ni/GDC anode within the real MSC system, with comparing of
the cell performance to the Plansee MSC. At 700 °C, the MSC
based on a Ni/YSZ anode (with an anode layer thickness of d
= 3 $\mu$m) reached a current density of 0,55 A/cm$^{2}$ at
the operating point of 0,7 V. A subsequent variation of the
Best Choice Ni/GDC-based MSC with an increased anode layer
thickness of d = 8 $\mu$m led to an improvement of
performance by more than 100 \%, by achieving j0,7V = 1,12
A/cm$^{2}$ at 700 °C. Concluding from those results: (i)
compared to the Plansee Ni/YSZ anode, the electrochemical
reaction zone of Ni/GDC extends an electrode layer thickness
of 3 $\mu$m, (ii) the cell voltage of Ni/GDC based MSC is
only slightly reduced by an activation overvoltage, what
presumably can be attributed to a high catalytic activity
and a low temperature dependence of the Ni/GDC system, (iii)
the anode performance of Ni/GDC anodes is clearly limited by
gas diffusion, what was shown by means of symmetrical cells
as well as single cell measurements, which is why a high
optimization potential in terms of improved microstructure,
with attention to high porosity and enhanced catalytic
surface, is on hand.},
cin = {IEK-1},
cid = {I:(DE-Juel1)IEK-1-20101013},
pnm = {135 - Fuel Cells (POF3-135) / SOFC - Solid Oxide Fuel Cell
(SOFC-20140602)},
pid = {G:(DE-HGF)POF3-135 / G:(DE-Juel1)SOFC-20140602},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
url = {https://juser.fz-juelich.de/record/825972},
}