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000010140 0247_ $$2DOI$$a10.1016/j.memsci.2010.04.002
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000010140 084__ $$2WoS$$aEngineering, Chemical
000010140 084__ $$2WoS$$aPolymer Science
000010140 1001_ $$0P:(DE-Juel1)VDB61604$$avan Gestel, T.$$b0$$uFZJ
000010140 245__ $$aPotentialities of microporous membranes for H(2)/CO(2) separation in future fossil fuel power plants: Evaluation of SiO(2), ZrO(2), Y(2)O(3)-ZrO(2) and TiO(2)-ZrO(2) sol-gel membranes
000010140 260__ $$aNew York, NY [u.a.]$$bElsevier$$c2010
000010140 300__ $$a64 - 79
000010140 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article
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000010140 440_0 $$03536$$aJournal of Membrane Science$$v359$$x0376-7388$$y1-2
000010140 500__ $$aFinancial 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.
000010140 520__ $$aIn 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.
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000010140 65320 $$2Author$$aGas separation membrane
000010140 65320 $$2Author$$aCO2 separation
000010140 65320 $$2Author$$aSiO2
000010140 65320 $$2Author$$aZrO2
000010140 65320 $$2Author$$aSol-gel
000010140 65320 $$2Author$$aSEM
000010140 65320 $$2Author$$aTEM
000010140 7001_ $$0P:(DE-Juel1)129662$$aSebold, D.$$b1$$uFZJ
000010140 7001_ $$0P:(DE-Juel1)VDB68418$$aHauler, F.$$b2$$uFZJ
000010140 7001_ $$0P:(DE-Juel1)129637$$aMeulenberg, W. A.$$b3$$uFZJ
000010140 7001_ $$0P:(DE-Juel1)129594$$aBuchkremer, H. P.$$b4$$uFZJ
000010140 773__ $$0PERI:(DE-600)1491419-0$$a10.1016/j.memsci.2010.04.002$$gVol. 359, p. 64 - 79$$p64 - 79$$q359<64 - 79$$tJournal of membrane science$$v359$$x0376-7388$$y2010
000010140 8567_ $$uhttp://dx.doi.org/10.1016/j.memsci.2010.04.002
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000010140 9141_ $$y2010
000010140 915__ $$0StatID:(DE-HGF)0010$$aJCR/ISI refereed
000010140 9201_ $$0I:(DE-Juel1)VDB809$$d30.09.2010$$gIEF$$kIEF-1$$lWerkstoffsynthese und Herstellungsverfahren$$x0
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