含氟体系下高性能丝光沸石分子筛膜的制备及其性能

doi:10.3724/SP.J.1088.2012.20436

催化学报 ›› 2012, Vol. 33 ›› Issue (9): 1558-1564.DOI: 10.3724/SP.J.1088.2012.20436

含氟体系下高性能丝光沸石分子筛膜的制备及其性能

任秀秀, 杨建华a, 陈赞, 杨兴宝, 鲁金明, 张艳, 王金渠b

大连理工大学化工学院吸附与无机膜研究所, 辽宁大连 116012

收稿日期:2012-04-18 修回日期:2012-06-07 出版日期:2012-09-11 发布日期:2012-09-11

Preparation and Performance of Mordenite Zeolite Membrane Using Fluoride Route

REN Xiuxiu, YANG Jianhuaa, CHEN Zan, YANG Xingbao, LU Jinming, ZHANG Yan, WANG Jinqub

Institute of Adsorption and Inorganic Membrane, School of Chemical Engineering, Dalian University of Technology, Dalian 116012, Liaoning, China

Received:2012-04-18 Revised:2012-06-07 Online:2012-09-11 Published:2012-09-11

摘要/Abstract

摘要： 采用热涂-浸渍法在大孔 α-Al₂O₃ 载体上形成薄且致密的晶种层, 然后在不添加有机模板剂的含氟条件下二次水热生长法制备了高性能丝光沸石分子筛膜, 考察了 NaF 含量、硅/铝比对丝光沸石分子筛膜形貌和性能的影响. 将摩尔组成为 6Na₂O:1.2Al₂O₃:30SiO₂:780H₂O:1.5NaF 条件下合成的丝光沸石分子筛膜用于渗透汽化分离 91.5% 乙醇/水体系, 在渗透汽化温度 70 °C、真空度为 400 Pa 条件下, 分离因子和通量分别达到了 6872 和 0.51 kg/(m²•h); 另外, 在分离异丙醇/水、乙酸/水体系时, 渗透侧水浓度达到了 100% (在色谱检测极限范围内), 该分离系数是目前报道的丝光沸石分子筛膜分离的最佳值, 并在乙酸浓度为 1 mol/L 的乙醇水溶液中表现出良好的耐酸性. 该膜有望作为膜反应器在乙酸乙酯等酯类的生产中大大提高转化率.

关键词: 丝光沸石分子筛膜, 渗透汽化, 热涂-浸渍法, 耐酸性, 氟体系

Abstract: High performance mordenite zeolite membranes in fluoride media with organic-free template were prepared on macroporous α-Al₂O₃ tubes by secondary growth. The seeding method was used hot dip-coating and could form a thin and compact layer. The effects of NaF content and Si/Al ratio on the morphology and pervaporation properties of the as-synthesized membranes were studied. The prepared membranes with a molar composition 6Na₂O:1.2Al₂O₃:30SiO₂:780H₂O:1.5NaF for pervaporation experiments were carried out at 70 °C and vacuum pressure 400 Pa in a 91.5% EtOH/H₂O system. The results indicated that the separation factor reached 6872 with flux 0.51 kg/(m²·h). The H₂O concentration of permeation side for pervaporation of IPA/H₂O, acetic acid/H₂O systems can reach 100% (limit in GC detection). The membranes almost keep high selectivity as before after acid test with 1 mol/L acetic acid in the H₂O/EtOH system. The membranes may have potential applications as membrane reactors in acetic ether production with a higher transformation ratio.

Key words: mordenite zeolite membrane, pervaporation, hot dip-coating, acid-resistance, fluoride route

任秀秀, 杨建华, 陈赞, 杨兴宝, 鲁金明, 张艳, 王金渠. 含氟体系下高性能丝光沸石分子筛膜的制备及其性能[J]. 催化学报, 2012, 33(9): 1558-1564.

REN Xiu-Xiu, YANG Jian-Hua, CHEN Zan, YANG Xing-Bao, LU Jin-Ming, ZHANG Yan, WANG Jin-Qu. Preparation and Performance of Mordenite Zeolite Membrane Using Fluoride Route[J]. Chinese Journal of Catalysis, 2012, 33(9): 1558-1564.

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参考文献

1 王金渠, 杨建华, 陈赞, 殷德宏. 膜科学与技术 (Wang J Q, Yang J H, Chen Z, Yin D H. Membr Sci Technol), 2011, 31(3): 118
2 Morigami Y, Kondo M, Abe J, Kita H, Okamoto K. Sep Purif Technol, 2001, 25: 251
3 Hasegawa Y, Nagase T, Kiyozumi Y, Hanaoka T, Mizu-kami F. J Membr Sci, 2010, 349: 189
4 Zhou H, Li Y Sh, Zhu G Q, Liu J, Yang W Sh. Sep Purif Technol, 2009, 65: 164
5 Tanaka K, Yoshikawa R, Ying C, Kita H, Okamoto K. Catal Today, 2001, 67: 121
6 徐如人, 庞文琴, 于吉红, 霍启升, 陈接胜. 分子筛与多孔材料化学. 北京: 科学出版社 (Xu R R, Pang W Q, Yu J H, Huo Q Sh, Chen J Sh. Chemsitry of Zeolites and Porous Materials. Beijing: Sci Press), 2004. 39
7 肖强, 李自运, 孙昕, 项寿鹤. 催化学报 (Xiao Q, Li Z Y, Sun X, Xiang Sh H. Chin J Catal), 2005, 26: 243
8 刘俊龙, 薛会福, 黄秀敏, 吴培豪, 黄信灵, 刘尚斌, 申文杰. 催化学报 ( Liu J L, Xue H F, Huang X M, Wu P H, Huang X L, Liu Sh B, Shen W J. Chin J Catal), 2010, 31: 729
9 Cora L, Thompson R W. Zolites, 1997, 18: 132
10 Huang A Sh, Lin Y Sh, Yang W Sh. J Membr Sci, 2004, 245: 41
11 Lin X, Kikuchi E, Matsukata M. Chem Commun, 2000: 957
12 Casado L, Mallada R, Téllez C, Coronas J, Menéndez M, Santamaría J. J Membr Sci, 2003, 216: 135
13 Sastre G, Fornes V, Corma A. J Phys Chem B, 2002, 106: 701
14 Kato M, Itabashi K, Matsumoto A, Kazuo T. J Phy Chem B, 2003, 107: 1788
15 Lu B W, Tsuda T, Sasaki H, Oumi Y, Itabashi K, Teranishi T, Sano T. Chem Mater, 2004, 16: 286
16 Arichia J, Louis B. Cryst Growth Des, 2008, 8: 3999
17 张延风, 许中强, 陈庆龄. 催化学报 (Zhang Y F, Xu Zh Q, Chen Q L. Chin J Catal), 2002, 23: 235
18 Sato K, Sugimoto K, Kyotani T, Shimotsuma N, Kurata T. J Membr Sci, 2011, 385-386: 20
19 Li X S, Kita H, Zhu H, Zhang Zh J, Tanak K. J Membr Sci, 2009, 339: 224
20 陈祥树, 周荣飞, 胡娜, 胡中丽, 段龙乔 (Chen X Sh, Zhou R F, Hu N, Hu Zh L, Duan L Q). CN 200910186437.8. 2009
21 Chen Z, Li Y H, Yin D H, Song Y M, Ren X X, Lu J M, Yang J H , Wang J Q. J Membr Sci, 2012, (in press). DOI: org/10.1016/j.memsci.2012.04.030
22 Xiao W, Chen Z, Zhou L, Yang J H, Lu J M, Wang J Q. Microporous Mesoporous Mater, 2011, 142: 154
23 Louis B, Kiwi-Minsker L. Microporous Mesoporous Mater, 2004, 74: 171
24 李宝宗, 徐文国, 裘式纶, 庞文琴, 徐如仁. 高等学校化学学报 (Li B Z, Xu W G, Qiu Sh L, Pang W Q, Xu R R. Chem J Chin Univ), 1998, 19: 930

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含氟体系下高性能丝光沸石分子筛膜的制备及其性能

Preparation and Performance of Mordenite Zeolite Membrane Using Fluoride Route

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