Preparation and catalytic properties of TS-1 zeolite membranes |
Authors: ZHU Meihua, LI Ling, DING Wenjuan, CHEN Le, LI Yuqin, GUI Tian*, Chen Xiangshu* |
Units: Institute of Advanced Materials, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang, 330022, P.R. China State-Province Joint Engineering Laboratory of Zeolite Membrane Materials, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang, 330022, P.R. China |
KeyWords: TS-1 zeolite membrane; H2O2 oxidation; Pervaporation |
ClassificationCode:O6,TQ,G3 |
year,volume(issue):pagination: 2018,38(2):45-51 |
Abstract: |
The TS-1 zeolite membrane was synthesized on a tubular mullite support by secondary hydrothermal synthesis. Influences of the concentration of seed crystal suspension, H2O2/SiO2 ratio and crystal seed content in the precursor synthesis solution on growth and catalytic performance of TS-1 zeolite membrane were investigated by XRD and SEM characterization. When the molar ratio of the initial synthesis solution, concentration of seed crystal suspension, H2O2/SiO2 molar ratio and crystal seed content in the precursor synthesis solution, synthesis temperature and synthesis time were SiO2:0.03TiO2:0.2TPAOH:120H2O, 5 wt%, 6, 1 wt%, 150 ℃ and 24 h, respectively, the as-synthesized TS-1 zeolite membrane showed an excellent catalytic performance in the oxidation of iso-propanol and hydrogen peroxide by pervaporation. Besides, when isopropanol/H2O2 molar ratio and reaction temperature in the pervaporation-catalytic oxidation process, were 1:2 and 70 ℃, the iso-propanol conversion and flux of the TS-1 zeolite membrane were 81.14% and 2.23 kg·m-2·h-1, respectively. |
Funds: |
国家自然科学基金面上项目(21476099),国家国际科技合作专项(2015DFA50190),江西省科技厅科技项目((20171BCB24005) |
AuthorIntro: |
第一作者简介:朱美华(1985年8月),女,江西景德镇人,工学博士,副教授,研究方向为分子筛膜的制备与应用,E-mail:zhumeihua@jxnu.edu.cn 通讯作者:陈祥树,E-mail: cxs66cn@jxnu.edu.cn |
Reference: |
[1] Chen X S, Chen P, Kita H. Pervaporation through TS-1 membrane[J]. Microporous Mesoporous Mater, 2008, 115(1-2): 164-169. [2] Chen P, Chen X B, Chen X S, et al. Preparation and catalytic activity of titanium silicalite-1 zeolite membrane with TPABr as template[J]. J Membr Sci, 2009, 330(1-2): 369-378. [3] 刘秀凤, 张宝泉, 林跃生. 无模板剂二次生长法制备取向MFI型分子筛膜[J]. 无机化学学报, 2008, 24(10): 1679-1683. [4] 王正宝, 路晓飞, 彭勇. 一种二次生长法制备高度取向性MFI型分子筛膜的方法,CN104891519A[P]. 2015. [5] Zhang X F, Yao J F, Yang X X. Effects of crystal size and pore structure on catalytic performance of TS-1 in the isomerization of styrene oxide to phenyl acetaldehyde[J]. Microporous Mesoporous Mater, 2017, 247: 16-22. [6] 王晓东, 张宝泉, 刘秀凤. 不同载体上TS-1分子筛膜的制备与表征[J]. 中国科技论文, 2009, 4(3): 175-178. [7] 古玲, 王莅. TS-1分子筛膜合成及其催化氯丙烯环氧化性能[J]. 中国炼油与石油化工, 2013. [8] 王晓东, 延静, 黄伟. 小晶粒TS-1分子筛膜的制备及表征[J]. 无机材料学报, 2011,26(1): 85-90 [9] Sebastian V, Motuzas J, Dirrix R W J, et al. Synthesis of capillary titanosilicalite TS-1 ceramic membranes by MW-assisted hydrothermal heating for pervaporation application[J]. Sep Purif Technol, 2010, 75(3): 249-256. [10] Wang X B, Zhang X F, Liu H O, et al. Preparation of titanium silicalite-1 catalytic films and application as catalytic membrane reactors[J]. Chem Eng J, 2010, 156(3): 562-570. [11] Xia S X, Peng Y, Lu H B, et al. The influence of nanoseeds on the pervaporation performance of MFI-type zeolite membranes on hollow fibers[J]. Microporous Mesoporous Mater, 2016, 222(4): 128-137. [12] Peng Y, Zhan Z Y, Shan L J, et al. Preparation of zeolite MFI membranes on defective macroporous alumina supports by a novel wetting–rubbing seeding method: Role of wetting agent[J]. J Membr Sci, 2013, 444(444): 60-69. [13] Guo Y, Jin Y J, Hong-Mei W U, et al. Preparation and Characterization of TS-1 Zeolite Membrane Supported on Alumina Tube[J]. Bulletin of the Chinese Ceramic Society, 2014. [14] Motuzas J, Mikutaviciute R, Gerardin E, et al. Controlled growth of thin and uniform TS-1 membranes by MW-assisted heating[J]. Microporous Mesoporous Mater, 2010, 128(1-3): 136-143. [15] Liu X G, Liu Y, Xu L, et al. Spreading-wetting method for highly reproducible tertiary growth of perfective bilayer TS-1 membranes[J]. Appl Surf Sci, 2015, 343: 77-87. [16] Wang X D, Yan J, Huang W. Synthesis of b-oriented TS-1 zeolite membranes with high performance in the oxyfunctionalization of n-hexane[J]. Thin Solid Films, 2013, 534(5): 40-44. [17] Xue J, Zhuang Z, Feng X. Hydrothermal crystallization of b-oriented TS-1 films on PVAc-modified glass[J]. Microporous Mesoporous Mater, 2013, 172(19): 141-145. [18] Shibata M, Gérard J, Gabelica Z. Rapid synthesis of MFI titanosilicates using in situ seeding method[J]. Microporous Mater, 1997, 12(1): 141-148. [19] Engström V, Mihailova B, Hedlund J, et al. The effect of seed size on the growth of silicalite-1 films on gold surfaces[J]. Microporous Mesoporous Mater, 2000, 38(1): 51-60. [20] Tuel A. Crystallization of titanium silicalite-1 (TS-1) from gels containing hexanediamine and tetrapropylammonium bromide[J]. Zeolites, 1996, 16(2-3): 108-117. [21] Xia Q H, Gao Z. Crystallization kinetics of pure TS-1 zeolite using quaternary ammonium halides as templates[J]. Mater Chem Phys, 1997, 47(2): 225-230. [22] Treacy M M J, Princeton, NJ. Collection of simulated XRD powder patterns for zeolites, Elsevier, 2001. [23] Koningsveld H V, Jansen J C, Bekkum H V. The monoclinic framework structure of zeolite H-ZSM-5. Comparison with the orthorhombic framework of as-synthesized ZSM-5[J]. Zeolites, 1990, 10(4): 235-242. [24] Qiu F R, Wang X B, Zhang X F, et al. Preparation and properties of TS-1 zeolite and film using Sil-1 nanoparticles as seeds[J]. Chem Eng J, 2009, 147(2-3): 316-322. [25] 张海燕. 无有机模板晶种导向合成沸石分子筛[D]. 吉林大学, 2013. [26] 任利敏, 宋江伟, 纪研研等. 无有机模板剂合成Beta分子筛的方法,CN 101249968 A [P]. 2008. [27] Guo Y, Jin Y J, Wu H M, et al. Direct synthesis of propylene oxide using hydrogen peroxide in a membrane reactor[J]. Chem Pap, 2016, 71(1): 49-57. [28] Kwon S, Schweitzer N M, Park S, et al. A kinetic study of vapor-phase cyclohexene epoxidation by H2O2 over mesoporous TS-1[J]. J Catal, 2015, 326: 107-115. |
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