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Pervaporation Separation and Catalysis Activity of Novel Zirconium Silicalite-1 Zeolite Membrane
Authors:CHEN Pei  CHEN Xinbing  CHEN Xiangshu  AN Zhongwei  KITA Hidetoshi
Institution:1. Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Materials Science, Shaanxi Normal University, Xi'an, Shannxi 710062, China;2. Department of Advanced Materials Science and Engineering, Faculty of Engineering, Yamaguchi University, Tokiwadai 2‐16‐1, Ube 755‐8611, Japan;3. Tel.: 0086‐029‐85308081;4. Fax: 086‐029‐85308090;5. College of Chemistry and Chemical Industry, Jiangxi Normal University, Nanchang, Jiangxi 330027, China
Abstract:Novel zirconium silicalite‐1 zeolite membrane was hydrothermally prepared on the mullite porous support at 150–185°C for 40–72 h by an "in situ" method using tetraethyl orthosilicate (TEOS), zirconium butoxide (ZBOT) and tetrapropylammonium hydroxide (TPAOH) as silica source, zirconium source and organic structure directing agent, respectively. X‐ray diffraction (XRD) patterns, fourier transformed infrared (FT‐IR) spectra, and inductively coupled plasma‐atomic emission spectrometry (ICP) of the accompanying zeolite powder confirmed that the zirconium was isomorphously incorporated into the zeolite framework. The surface chemical compositions of the obtained membrane were measured with an energy‐dispersive X‐ray spectral analyzer (EDS), and the membrane morphologies were observed by a scanning electron microscope (SEM). The results showed that the zeolite crystals growing on the support were zirconium silicalite‐1 zeolites, and the dense membrane layer was composed of the well inter‐growing zeolite crystals. The zirconium silicalite‐1 zeolite membrane, which was derived from the synthesis solution having a molar ratio of 1.00SiO2:0.01ZrO2:0.17TPAOH:120H2O, showed high ethanol permselectivity with a flux of 1.01 kg/(m2·h) accompanied with a separation factor of 73 for ethanol/water (5/95, w/w) system under a pervaporation condition at 60°C. Moreover, this membrane displayed pervaporation‐aided catalysis activity for iso‐propanol oxidation with hydrogen peroxide as oxidant, and the corresponding iso‐propanol conversion was 35%.
Keywords:zirconium silicalite‐1  zeolite membrane  pervaporation  catalysis activity
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