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Preparation and hydrogen separation of microporous silica membranesmodified by isobutylgroup
Authors: ZHANG Shaokang, WEI Qi, LI Qunyan, NIE Zuoren, LIU Yajun
Units: College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China
KeyWords: isobutyl groups; organic-inorganic hybrid microporous silica membranes; pore structure; hydrogen separation
ClassificationCode:O613.72
year,volume(issue):pagination: 2016,36(4):46-53

Abstract:
An isobutyl-modified silica sol was synthesized by the co-hydrolysis and condensation of tetraethyl orthosilicate(TEOS) and isobutyltriethoxysilane(iTES) under acidic condition and the sol was deposited on the ?-Al2O3/?-Al2O3 support by dip-coating in clean room(Grade 100).The particle size distribution of silica sol, the hydrophobic properties and the pore size distribution of the silica membranes were characterized by means of dynamic light scattering(DLS), water contact angle measurement, Fourier translation infrared spectroscopy(FT-IR), solid state 29Si magic-angle spinning nuclear magnetic resonance(29Si MAS NMR) and N2 adsorption-desorption. The hydrogen permeation and separation performance of modified silica membranes were also investigated in detail. The results show that the particle size of silica sol increases with increasing iTES/TEOS molar ratio, reaching 5.1nm at an iTES/TEOS molar ratio of 0.6. Isobutyl groups have been successfully incorporated into silica membranes, leading to an enhanced hydrophobic property with a water contact angle as high as (114.0±0.5)° for the modified membranes. The modified silica membranes possess a microporous structure with a pore size centered at 0.45~0.8nm.The hydrogen permeance increases with increasing temperatures, indicating that the hydrogen transport in modified silica membranes complies predominantly with activated diffusion mechanism. At a temperature of 300°C, the modified membranes exhibit a significantly high H2permeance of 9.07×10-7 mol•m-2•s-1•Pa-1, a H2/CO2 and H2/COpermselectivity of 6.79 and 15.37, a H2/CO2and H2/CObinary gas mixture separation factor of 7.09 and 15.72, respectively, both higher than that of Knudsen diffusion.Under a humid condition with a temperature of 250°C and a water vapor molar ratio of 5% for at least 200 hours, the modified membranes possess an outstanding hydrothermal stability.

Funds:
国家自然科学基金(21171014),北京市教委科技计划重点项目(KZ201410005006)

AuthorIntro:
第一作者简介:张少康(1988-),男,河北石家庄人,硕士生,从事用于气体分离的二氧化硅膜材料的制备与表征.*通讯作者,E-mail:qiwei@bjut.edu.cn

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