Inorganic Microporous Membranes for Gas Separation in Fossil Fuel ...

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5 Conclusions and recommendations mesoporous defects or intercrystalline channels between ZrO2 crystals that are in the same order as the layer thickness. It is expected that crystalline TiO2 or ZrO2 may not form ultramicroporous membranes with crystallisation temperatures of 500ºC and higher due to the relative large crystallinity of these layers. Defect free, TiO2 or ZrO2 membranes should be prepared and studied with gas permeability to confirm the absence of ultramicropores. H2/CO2 permselectivity higher than Knudsen factor is observed for Ti0.5Zr0.5O2 films calcined at 500 and 600ºC. He and H2 gas transport is thermally activated indicating the presence of micropore diffusion. Knudsen mass transport is obtained for gasses with kinetic diameter of CO2 and larger. These results show that Ti0.5Zr0.5O2 films calcined at 500 and 600ºC contain a pore size distribution of ~0.3 to ~0.5 nm in diameter. The He permeance of 1·10 -7 mol/m 2 sPa with a He/N2 permselectivity of 5.9 or the He permeance 2·10 -8 mol/m 2 sPa with a He/N2 permselectivity of 14 are lower than state of the art SiO2 membranes but are higher than TiO2-ZrO2 membranes found in literature. 80 These results fulfil the primary aim of achieving gas separation membranes from TiO2- ZrO2 material. The permeance might be increased by the formation of thinner or more porous γ-Al2O3 intermediate layers. The permselectivity might be improved using structure directing agents (SDAs) in the sols, avoiding larger pores or metal loading in the final membrane layer. The micropores in these membranes are stable for at least 1500 hours. Steam test results in reversible pore blocking without layer delamination or destruction while maintaining the He/N2 permselectivity of ~10. These gas separation membranes show the chemical stability at high temperatures in humid conditions fulfilling the aim of hydrothermally stable membrane preparation. This evidence indicates that binary oxide 50 mol % TiO2 in ZrO2 microporous thin layers could be alternatives to SiO2 membranes for precombustion applications. However, the permselectivity and permeability values of the prepared Ti0.5Zr0.5O2 membranes do not reach industrial targets and these membranes might not have sufficient hydrothermal stability. The hydrothermal stability might be improved by using SDAs used in hydrothermal stable SiO2 membranes. 113
6 References 6 References 1. Metz, B., Davidson, O., de Coninck, H., Loos, M. & Meyer, L. IPCC special report on carbon dioxide capture and storage (Cambridge university press, Cambridge, 2005). 2. Bernal, M. P., Coronas, J., Menendez, M. & Santamaria, J. Separation of CO2/N2 mixtures using MFI-type zeolite membranes. AICHE 50, 127-135 (2004). 3. Goettlicher, G. Energetik der Kohlendioxidrückhaltung in Kraftwerken. Fortschritt- Berichte VDI, Energietechnik (1999). 4. Bohnes, S., Van der Donk, G. J. W., Meulenberg, W. A., Scherer, V. & Stoever, D. in Proceeding of Porous Ceramic Materials (ed. Luyten, J.) (Brugge, Belgium, 2005). 5. Bhave, R. Inorganic Membranes, Synthesis, Characterization and Properties (Van Nostrand Reinhold, New York, 1991). 6. Lin, Y. S. Microporous and dense inorganic membranes: current status and prospective. Separation and Purification Technology 25, 39-55 (2001). 7. Bredesen, R., Jordal, K. & Bolland, O. High-temperature membranes in power generation with CO2 capture. Chemical Engineering and Processing 43, 1129 (2004). 8. Pex, P. et al. in Eight international conference on inorganic membranes (eds. Akin, F. T. & Lin, Y. S.) 524 (Cincinnati, Ohio, 2004). 9. Pan, X. L., Stroh, N., Brunner, H., Xiong, G. X. & Sheng, S. S. Pd/ceramic hollow fibers for H2 separation. Separation and Purification Technology 32, 265-270 (2003). 10. Jun, C. S. & Lee, K. H. Preparation of palladium membranes from the reaction of Pd(C3H3)(C5H5) with H2: wet-impregnated deposition. Journal of Membrane Science 157, 107-115 (1999). 11. Yeung, K. L. & Varma, A. Novel preparation techniques for thin metal-ceramic composite membranes. AICHE 41, 2131-2139 (1995). 12. Moss, T. S., Peachey, N. M., Wilson, M. S. & Dye, R. C. in Fourth international conference on inorganic membranes (ed. Fain, D. E.) 343 (Gatlinburg, Tennessee, 1996). 13. Edlund, D. J. & McCarthy, J. The Relationship between Intermetallic Diffusion and Flux Decline in Composite-Metal Membranes - Implications for Achieving Long Membrane Lifetime. Journal of Membrane Science 107, 147-153 (1995). 14. Morooka, S. & Kusakabe, K. Inorganic membranes for gas separation at elevated temperatures. Industrial Ceramics 20, 15-18 (2000). 15. Wagner, C. Beitrag zur Theorie des Anlaufvorganges. Zeitschrift fuer Physikalische Chemie B11, 25 (1930). 16. Van der Haar, L. M. Mixed-conducting perovskite membranes for oxygen separation (PhD Thesis, University of Twente, Enschede, 2001). 17. Vente, J., McIntosh, S., Haije, W. G. & Bouwmeester, H. J. M. Properties and performance of BaxSr1-xCo0.8Fe0.2O3 materials for oxygen transport membranes. Journal of Solid State electrochemistry 10, 581 (2006). 18. Vente, J., Haije, H. & Rak, Z. in Eight international conference on inorganic membranes (eds. Akin, F. T. & Lin, Y. S.) 595 (Cincinnati, Ohio, 2004). 19. Mertins, F. H. B. Perovskite-type ceramic membranes; Partial oxidation of methane in a catalytic membrane reactor (PhD Thesis, University of Twente, Enschede, 2005). 20. Bouwmeester, H. J. M., Kruidhof, H. & Burggraaf, A. J. Importance of the Surface Exchange Kinetics as Rate Limiting Step in Oxygen Permeation through Mixed- Conducting Oxides. Solid State Ionics 72, 185-195 (1994). 21. Buechler, O., Serra, J. M., Meulenberg, W. A. & Sebold, D. Preparatin of thin La1xSrxCo1-yFeyO3-delta membranes supported on tailored ceramic substrates. Solid State Ionics 178, 91-99 (2007). 114
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Mitglied der Helmholtz-Gemeinschaft
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Forschungszentrum Jülich GmbH Inst
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List of Abbreviations Ac Acetyl Ace
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Summary CO2 capture and storage mig
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Zusammenfassung Die Abtrennung und
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1 Introduction and aims 1 Introduct
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1 Introduction and aims Candidate m
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2 Theoretical background 2 Theoreti
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2 Theoretical background Table 2 Ox
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2 Theoretical background 2.1.2 Micr
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2 Theoretical background Poly-cryst
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2 Theoretical background membranes
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2 Theoretical background Dry or wet
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2 Theoretical background the materi
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2 Theoretical background Figure 11
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2 Theoretical background due to its
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2 Theoretical background 2.3.3.2 Mi
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2 Theoretical background 2.4 Microp
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2 Theoretical background Figure 15
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2 Theoretical background wall inter
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3 Experimental 3 Experimental The m
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3 Experimental vacuum sample holder
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3 Experimental o of as-made DOH cry
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3 Experimental Another solution was
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3 Experimental 3.4 Characterisation
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3 Experimental Element analysis The
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3 Experimental Additionally, the hy
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4 Results and discussion Abundance
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4 Results and discussion 4.2 Zeolit
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4 Results and discussion Table 14 D
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4 Results and discussion hours usin
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4 Results and discussion Intensity
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4 Results and discussion The carbon
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Page 102 and 103: 4 Results and discussion In pure Ti
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Page 106 and 107: 4 Results and discussion Intensity
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Page 126 and 127: 6 References 22. Shao, Z., Dong, H.
Page 128 and 129: 6 References 65. Van den Berg, A. W
Page 130 and 131: 6 References 108. Wen, T. L., Heber
Page 132 and 133: Curriculum Vitae - George van der D
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