Synthesis of a Multilayer Ceramic Membrane Used for Hydrogen Separation at High Temperature

Document Type: Research Paper

Authors

1 Chemical Engineering Department, Sharif university of Technology, Tehran, Iran

2 Gas Department, Research Institute of petroleum Industry, Tehran, Iran

Abstract

A multilayer composite ceramic membrane was prepared by depositing a nano-scale layer of SiO2 on top of a modified porous alumina support by chemical vapor deposition (CVD) method. The modification of the support was carried out by adding a graded layer of Al2O3 (γ-alumina phase), using sol-gel method. An optimized temperature of 700 K for intermediate layer calcination was gained by XRD analysis. Cross-sectional images obtained from SEM showed that the intermediate γ-alumina layer had a thickness of about 2 μm and the top selective silica layer was quite dense and uniform with a thickness of about 90-100 nm. Permeation tests showed a very good flux of 10-6-10-7 mol m-2 s-2 Pa-1 for H2 with selectivities over CO2, N2 and CH4 up to 500. By performing different tests with various deposition times, it was concluded that by changing CVD time from 3 h to 6 h H2/CO2 selectivity increased from 32 to 573, although H2  permeation flux reduced about 50 percent.

Keywords


[1] R. Ramachandran, R.K. Menon, An overview of industrial uses of hydrogen, Int. J. Hydrogen Energy 23 (1998) 593.

[2] R.W. Van Gemert, F.Petrus-Cuperus, Newly developed ceramic membranes for dehydration and separation of organic mixtures by pervaporation, J. Membr. Sci. 105 (1995) 287–291.

[3] N. Wynn, Dehydration with silica pervaporation membranes, Membr. Technol. 2001 (2001) 10–11.

[4] Yasushi Yoshino, Takehiro S., Development of tubular substrates, silica based membranes and membrane modules for hydrogen separation at high temperature, J.Membr. Sci. 267 (2005) 8–17.

[5] J. Lin, I. Kumakiri, B.N. Nair, H. Alsyouri, Microporous ceramic membranes: review, Sep. Purif. Meth. 31 (2) (2002) 229.

[6] R.J.R. Uhlhorn, Ceramic Membranes For Gas Separation, PhD Thesis,University of Twente, Cap. 2, 1990, ISBN 90-9003618-0.

[7] R.M. De Vos, H. Verweij, High-selectivity, high-flux silica membranes for gas separation, Science 279 (1998) 1710–1711.

[8] L.J.P. Van Den Broeke, W.J.W. Bakker, F. Kapteijn, J.A. Moulijn, Binary permeation through a silicalite-1 membrane, AIChE J. 45 (1999) 976–985.

[9] J. Sekulic, M.W.J. Luiten, J.E. Ten Elshof, N.E. Benes, K. Keizer, Microporous silica and doped silica membrane for alcohol dehydration by pervaporation, Desalination 148 (2002) 19–23.

[10] M. Tsapatsis, S. Kim, S.W. Nam, G.R. Gavalas, Synthesis of hydrogen permselective SiO2, TiO2, Al2O3 and B2O3 membranes from the chloride precursors, Ind. Eng. Chem. Res. 30 (1991) 2152.

[11] T. Okubo, H. Inoue, Introduction of specific gas selectivity to porous glass membranes by treatment with tetraethoxysilane, J. Membr. Sci. 42 (1989) 109.

[12] A.K. Prabhu, S.T. Oyama, Highly hydrogen selective ceramic membranes: application to the transformation of gr

[13] G.J. Hwang, K. Onuki, S. Shimizu, H. Ohya, Hydrogen separation in H2–H2O–HI gaseous mixture using the silica membrane prepared by chemical vapor deposition, J. Membr. Sci. 162 (1999) 83.

[14] Y. Yoshino, T. Suzuki, B.N. Nair, H. Taguchi, N. Itoh, Development of tubular substrates, silica based membranes and membrane modules for hydrogen separation at high temperature, J. Membr., Sci. 267, 2005 8.

[15] S. Yan, H. Maeda, K. Kusakabe, S. Morooka, Y. Akiyama, Hydrogenpermselective SiO2 membrane formed in pores of alumina support tube by chemical vapor deposition with tetraethyl orthosilicate, Ind. Eng. Chem.Res. 33 (1994) 2096.

[16] Yunfeng Gu, S. Ted Oyama, Ultrathin, hydrogen-selective silica membranes deposited on alumina-graded structures prepared from size-controlled boehmite sols, J. Memb. Sci. 306 (2007) 216–227.

[17] Yunfeng Gu, Pelin Hacarlioglu, S. Ted Oyama, Hydrothermally stable silica–alumina composite membranes for hydrogen separation, J. Memb. Sci. 310 (2008) 28–37.

eenhouse gases, J. Membr. Sci. 176 (2000) 233.