Hydrophobic *BEA-Type Zeolite Membranes on Tubular Silica Supports for Alcohol/Water Separation by Pervaporation
by
Kyohei Ueno 1,2
, Saki Yamada 3, Toshinari Watanabe 4, Hideyuki Negishi 5, Takuya Okuno 6, Hiromasa Tawarayama 6, Shinji Ishikawa 6, Manabu Miyamoto 2, Shigeyuki Uemiya 2 and 
Yasunori Oumi 7,*
, Saki Yamada 3, Toshinari Watanabe 4, Hideyuki Negishi 5, Takuya Okuno 6, Hiromasa Tawarayama 6, Shinji Ishikawa 6, Manabu Miyamoto 2, Shigeyuki Uemiya 2 and Yasunori Oumi 7,*
1
Department of Oral Biochemistry, Division of Oral Structure, Function and Development, Asahi University School of Dentistry, 1851 Hozumi, Mizuho, Gifu 501-0296, Japan
2
Faculty of Engineering, Gifu University, 1-1 Yanagido, Gifu, Gifu 501-1193, Japan
3
Graduate School of Natural Science and Technology, Gifu University, 1-1 Yanagido, Gifu, Gifu 501-1193, Japan
4
Graduate School of Engineering, Gifu University, 1-1 Yanagido, Gifu, Gifu 501-1193, Japan
5
Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology (AIST), AIST Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan
6
Frontier Technologies Laboratory, Sumitomo Electric Industries, Ltd., 1, Taya-cho, Sakae-ku, Yokohama, Kanagawa 244-8588, Japan
7
Organization for Research and Community Development, Gifu University, 1-1 Yanagido, Gifu, Gifu 501-1193, Japan
*
Author to whom correspondence should be addressed.
Membranes 2019, 9(7), 86; https://doi.org/10.3390/membranes9070086
Received: 24 May 2019 / Revised: 25 June 2019 / Accepted: 14 July 2019 / Published: 17 July 2019
(This article belongs to the Special Issue Preparation, Characterization and Application of Silica-Based Membranes)
Hydrophobic pure-silica *BEA-type zeolite membranes with large pores were prepared on tubular silica supports by hydrothermal synthesis using a secondary growth method and were applied to the separation of alcohol/water mixtures by pervaporation (PV), an alternative energy-efficient process for production of biofuels. Amorphous pure-silica tubular silica supports, free of Al atoms, were used for preparing the membranes. In this study, the effects of the synthesis conditions, such as the H2O/SiO2 and NH4F/SiO2 ratios in the synthetic gel, on the membrane formation process and separation performance were systematically investigated. The successfully prepared dense and continuous membranes exhibited alcohol selectivity and high flux for the separation of ethanol/water and butanol/water mixtures. The pure-silica *BEA membranes obtained under optimal conditions (0.08SiO2:0.5TEAOH:0.7NH4F:8H2O) showed high PV performance with a separation factor of 229 and a flux of 0.62 kg·m−2·h−1 for a 1 wt % n-butanol/water mixture at 318 K. This result was attributed to the hydrophobicity and large pore size of the pure-silica *BEA membrane. This was the first successful synthesis of hydrophobic large-pore zeolite membranes on tubular supports with alcohol selectivity, and the obtained results could provide new insights into the research on hydrophobic membranes with high permeability.
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Keywords:
*BEA-type zeolite; hydrophobic zeolite membrane; electrophoretic deposition; tubular silica support; secondary growth; hydrothermal synthesis; ethanol; butanol; pervaporation separation; alcohol selectivity
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MDPI and ACS Style
Ueno, K.; Yamada, S.; Watanabe, T.; Negishi, H.; Okuno, T.; Tawarayama, H.; Ishikawa, S.; Miyamoto, M.; Uemiya, S.; Oumi, Y. Hydrophobic *BEA-Type Zeolite Membranes on Tubular Silica Supports for Alcohol/Water Separation by Pervaporation. Membranes 2019, 9, 86.
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