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@PHDTHESIS{Niehoff:200847,
author = {Niehoff, Patrick},
title = {{E}ntwicklung planarer
{B}a$_{0,5}${S}r$_{0,5}${C}o$_{0,8}${F}e$_{0,2}${O}$_{3-δ}$
- {M}embranmodule zur {S}auerstoffabtrennung und {A}nalyse
ihres {T}ransportverhaltens},
volume = {256},
school = {Ruhr-Universität Bochum},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2015-03226},
isbn = {978-3-95806-044-9},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {VIII, 134 S.},
year = {2015},
note = {Dissertation, Ruhr-Universität Bochum, 2015},
abstract = {Oxygen transport membranes (OTMs) represent a promising
alternative for the extraction of oxygen compared to energy
intensive processes such as the cryogenic air separation.
Especially ceramic, mixed ionic-electronic conducting
membranes (MIECs) are of current interest. Due to their
ability to transport oxygen via vacancies in the crystal
lattice in case of sufficient high temperature and partial
pressure gradients, such membranes can theoretically achieve
a selectivity of $100\%$ assuming the absence of any
leakages. With respect to membrane material, mostly
perovskites are used, showing high ionic and electronic
conductance. In this context, the perovskite with the
highest oxygen permeability is
Ba$_{0,5}$Sr$_{0,5}$Co$_{0,8}$Fe$_{0,2}$O$_{3-\delta}$
(BSCF), which is also used in this work. Regarding the
technical implementation, different design and operational
concepts exist, whereas the respective oxygen transport is
governed by a complex set of different mechanisms depending
on each individual membrane system’s architecture. One
part of this work addresses the modeling of the oxygen
transport through a supported membrane. For this purpose,
different approaches for individual transport mechanisms
such as solid state diffusion, surface exchange, and
transport in the support and gas phase are combined to one
comprehensive model. With regard to the surface exchange, a
correction factor is introduced, which takes into account
the realistic topography of the membrane surfaces. This
approach was verified by permeation measurements of
supported samples with varying membrane layer thicknesses (8
- 400 $\mu$m), showing a good agreement between model and
experiment. Characteristic values (porosity, tortuosity,
spec. surface area) necessary for the modeling were
determined using x-ray computed tomography. Overall the
complete model allows the description of experimental data
with a deviation of only 7\%. Another focal point of this
work is the development and testing of a complete ceramic
membrane module. The manufacturing of planar compounds (20
mm diameter) consisting of membrane- (thickness 25 $\mu$m)
and support-layers (thickness 1.4 mm) was done by sequential
tape casting and lamination. Also, the adaption of the
sintering program allows the fabrication of samples with a
surface area of 110 x 110 cm$^{2}$, thus confirming the
scalability of this manufacturing process. The compound’s
outer surface is sealed by applying a ceramic layer. For
this purpose, a BSCF-paste was developed and optimized with
regard to a maximum green density, resulting in a gastight,
crack-free layer with low porosity (ca. 5\%). A gastight
connection between BSCF-tube and compound was successfully
achieved by garnishing and subsequent sintering under load.
A tape-cast BSCF-foil (green thickness ca. 60 $\mu$m) is
used as joining material, yielding a high mechanical
stability and gas-tightness of the established connection.
The membrane-module’s oxygen permeation was measured in
3-end mode undervarying conditions and is compared to
reference samples. In this context, the results of the
module, the reference samples and the developed transport
model are consistent to each other. The viscous gas
transport within the support layer was identified as the
limiting factor. Thus future research and development needs
to focus on the optimization of the support’s
microstructure.},
keywords = {Dissertation (GND)},
cin = {IEK-1},
cid = {I:(DE-Juel1)IEK-1-20101013},
pnm = {113 - Methods and Concepts for Material Development
(POF3-113) / HITEC - Helmholtz Interdisciplinary Doctoral
Training in Energy and Climate Research (HITEC)
(HITEC-20170406)},
pid = {G:(DE-HGF)POF3-113 / G:(DE-Juel1)HITEC-20170406},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
url = {https://juser.fz-juelich.de/record/200847},
}