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@ARTICLE{vanGestel:10140,
author = {van Gestel, T. and Sebold, D. and Hauler, F. and
Meulenberg, W. A. and Buchkremer, H. P.},
title = {{P}otentialities of microporous membranes for
{H}(2)/{CO}(2) separation in future fossil fuel power
plants: {E}valuation of {S}i{O}(2), {Z}r{O}(2),
{Y}(2){O}(3)-{Z}r{O}(2) and {T}i{O}(2)-{Z}r{O}(2) sol-gel
membranes},
journal = {Journal of membrane science},
volume = {359},
issn = {0376-7388},
address = {New York, NY [u.a.]},
publisher = {Elsevier},
reportid = {PreJuSER-10140},
pages = {64 - 79},
year = {2010},
note = {Financial support from the Helmholtz Association of German
Research Centres (Initiative and Networking Fund) through
the MEM-BRAIN Helmholtz Alliance is gratefully acknowledged.
Stephan Roitsch (Ernst Ruska-Centre, FZ-Julich) and
Christoph Somsen (Institut fur Werkstoffe,
Werkstoffwissenschaft, Ruhr-Universitat Bochum) are thanked
for providing the TEM results.},
abstract = {In this work, an experimental study is made on the
preparation, the morphological characterization and the gas
permeation of graded ceramic multilayer membranes with
silica and non-silica toplayers. The membranes were prepared
on porous alpha-Al2O3 or 8Y(2)O(3)-ZrO2 supports by
dip-coating methods, where sols with different particle
sizes were used as coating liquids. In a first step,
mesoporous alumina or graded zirconia sublayers with a pore
size of 7-3 nm were deposited, starting from sols with a
particle size in the range 60-30 nm. The active toplayer of
the membrane is a SiO2, ZrO2, 8Y(2)O(3)-ZrO2 or
50TiO(2)-50ZrO(2) thin film with a thickness in the range
50-200 nrn. Nano-particles of these materials were prepared
by a precipitate-free hydrolysis-condensation synthesis
method, starting from metal-organic precursors. An important
consideration is that the properties of the novel zirconia
based sublayers and toplayers, which are developed for
typical higher steam pressure areas, are comparable to the
commonly used -y-Al2O3 and silica layers. Gas permeation
tests showed a decrease of permeation in the order He > H-2
> CO2 > N-2 and suggested that the membranes with silica
toplayers are microporous. Moreover, optimising all
conditions in the membrane manufacturing procedure in our
lab, such as the properties of the support and the sols and
the use of cleanroom coating, resulted in a $100\%$ H-2/CO2
selectivity for a few samples. The formation of crack-free
non-silica toplayers was initially experienced as very
difficult, but after optimization of the sol synthesis and
coating methodology and by restricting the layer thickness
below 100 nm, comparable ultra-thin toplayers are obtained.
Further, extensive gas permeation testing confirmed that
each of these toplayers posses a very low number of defects
and a comparable low or zero CO2 permeation is obtained. On
the other hand, extremely low He and H-2 permeation -
especially for the samples fired at 400 and 500 degrees C -
suggested the formation of thin dense toplayers. This
behaviour is found for the crystalline ZrO2 and
8Y(2)O(3)-ZrO2 layers as well as the amorphous
50TiO(2)-50ZrO(2) layers and indicates the presence of a
totally different structure in the non-silica material. The
amorphous silica toplayer is probably formed of 5-, 6-, 7-,
8- and also larger Si-O bonded rings which enable H-2
permeation, while our results suggest that the non-silica
toplayers are characterized by a more dense atomic packing
hindering H-2 permeation. For future H-2/CO2 separation in a
power plant, membranes will however need to out-perform the
discussed materials. Amorphous silica toplayers hold the
potential to combine an excellent selectivity with a
relatively high gas permeation, but lack the required
stability to operate over a wide range of conditions, and
the discussed non-silica toplayers which are considered as
the best until now in the literature - based on their zero
CO2 permeation - are to dense to allow the passage of H-2.
(C) 2010 Elsevier B.V. All rights reserved.},
keywords = {J (WoSType)},
cin = {IEF-1},
ddc = {570},
cid = {I:(DE-Juel1)VDB809},
pnm = {Rationelle Energieumwandlung},
pid = {G:(DE-Juel1)FUEK402},
shelfmark = {Engineering, Chemical / Polymer Science},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000279953300008},
doi = {10.1016/j.memsci.2010.04.002},
url = {https://juser.fz-juelich.de/record/10140},
}