二次水热合成法制备ZSM-5分子筛膜及其渗透汽化性能

doi:10.16085/j.issn.1000-6613.2016.09.033

化工进展 ›› 2016, Vol. 35 ›› Issue (09): 2885-2891.DOI: 10.16085/j.issn.1000-6613.2016.09.033

二次水热合成法制备ZSM-5分子筛膜及其渗透汽化性能

朱美华, 夏水莲, 刘永生, 袁晓蕾, 李羚, 桂田, 张飞, 刘鑫, 陈祥树

江西师范大学化学化工学院, 江西南昌 330022

收稿日期:2015-12-16 修回日期:2016-05-16 出版日期:2016-09-05 发布日期:2016-09-05
通讯作者: 陈祥树,教授,博士生导师。E-mail:cxs66cn@jxnu.edu.cn。
作者简介:朱美华(1985-),女,讲师。
基金资助:
国家自然科学基金面上项目（21476099）、国家国际科技合作专项（2015DFA50190）、国家自然科学基金青年基金（21503100）、江西省教育厅科学技术研究项目（14240）及江西省科技厅对外合作科技项目（20141BDH80011）。

Secondary hydrothermal synthesis of ZSM-5 zeolite membrane and its pervaporation performance

ZHU Meihua, XIA Shuilian, LIU Yongsheng, YUAN Xiaolei, LI Ling, GUI Tian, ZHANG Fei, LIU Xin, CHEN Xiangshu

College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, Jiangxi, China

Received:2015-12-16 Revised:2016-05-16 Online:2016-09-05 Published:2016-09-05

摘要/Abstract

摘要： 采用二次水热合成法在管状多孔莫来石支撑体上制备高耐酸性ZSM-5分子筛膜，系统地研究分子筛晶种和合成溶胶中H₂O/SiO₂摩尔比率对ZSM-5分子筛膜生长与渗透汽化性能的影响，采用X射线衍射、冷场扫描电子显微镜和电子能谱等表征技术分别对制备的ZSM-5分子筛及其ZSM-5分子筛膜的结构、形貌和Si/Al比进行表征。针对分离75℃、90% HAc/H₂O的水溶液，最优化条件下制备的ZSM-5分子筛膜表现出优良的渗透汽化性能，渗透通量和分离因子分别为0.98kg/(m²·h)和890。此外，本研究所采用制备耐酸性ZSM-5分子筛膜的方法表现出良好的重现性，重复制备的12根ZSM-5分子筛膜在75℃下分离90% HAc/H₂O的水溶液时，平均通量和分离系数分别为（0.85±0.15）kg/(m²·h)和650±290。再者，ZSM-5分子筛膜在45～75℃的温度范围内分离50%～95% HAc/H₂O水溶液时都表现出优良的渗透汽化性能。

关键词: 耐酸性ZSM-5分子筛膜, 晶种, H₂O/SiO₂比率, 渗透汽化, 重复性

Abstract: The high acid-proof ZSM-5 zeolite membranes are prepared on tubular porous mullite supports by secondary hydrothermal synthesis,and the effects of seed crystals,H₂O/SiO₂ molar ratio of the precursor synthesis gel on the growth and pervaporation performance of ZSM-5 zeolite membranes are studied systematically. The structure,morphology,and Si/Al ratio of the ZSM-5 zeolite crystals and membranes are characterized by XRD,FE-SEM,and EDX. For the separation of 90% HAc/H₂O mixture at 75℃,the flux and separation factor (H₂O over HAc) of ZSM-5 zeolite membrane prepared with the optimum synthesis condition has a well dehydration performance,and the total flux and separation factor are 0.98kg/(m²·h) and 890,respectively. Besides,the prepared ZSM-5 zeolite membranes show good reproducibility,and the average flux and separation factor of the 12 pieces of ZSM-5 zeolite membranes are(0.85±0.15) kg/(m²·h) and 650±290 for dehydration of 90% HAc/H₂O mixture at 75℃. Moreover,the ZSM-5 zeolite membrane presents excellent dehydration performance for 50%~95% HAc/H₂O at 45~75℃.

Key words: acid-stable ZSM-5 zeolite membrane, seed crystals, H₂O/SiO₂ ratio, pervaporation, reproducibility

中图分类号:

TQ028.8

朱美华, 夏水莲, 刘永生, 袁晓蕾, 李羚, 桂田, 张飞, 刘鑫, 陈祥树. 二次水热合成法制备ZSM-5分子筛膜及其渗透汽化性能[J]. 化工进展, 2016, 35(09): 2885-2891.

ZHU Meihua, XIA Shuilian, LIU Yongsheng, YUAN Xiaolei, LI Ling, GUI Tian, ZHANG Fei, LIU Xin, CHEN Xiangshu. Secondary hydrothermal synthesis of ZSM-5 zeolite membrane and its pervaporation performance[J]. Chemical Industry and Engineering Progree, 2016, 35(09): 2885-2891.

参考文献

[1] 张欢欢,葛志强,郭翔海,等. 从工业废水中回收乙酸的方法研究进展[J]. 化工进展,2015,34(6):1768-1778.
[2] YANG Jianhua,LI Liangqing,LI Wanze,et al. Tuning aluminum spatial distribution in ZSM-5 membranes:a new strategy to fabricate high performance and stable zeolite membranes for dehydration of acetic acid[J]. Chemical Communications,2014,50:14654-14657.
[3] 由涛,陈龙祥,张庆文,等. 渗透汽化分离乙酸的研究进展[J]. 化工进展,2009,28(2):187-213.
[4] GAO Xue,ZOU Xiaoqin,ZHANG Feng,et al. Eco-friendly fabrication of hydrophilic ZSM-5 membranes for alcohol upgrading[J]. Chemical Communications,2013,49:8839-8841.
[5] 周荣飞,胡娜,袁慧,等. T型分子筛膜的合成、表征与渗透汽化性能[J]. 无机化学学报,2009,25(8):1439-1446.
[6] MORIGAMI Yoshio,KONDO Masakazu,ABE Jun,et al. The first large-scale pervaporation plant using tubular-type module with zeolite NaA membrane[J]. Separation and Purification Technology,2001, 25:251-260.
[7] ZHU Meihua,XIA Shuilian,HUA Xuemei,et al. Rapid preparation of acid-stable and high dehydration performance Mordenite membranes[J]. Industrial & Engineering Chemistry Research,2014, 53:19168-19174.
[8] LI Xiansen,KITA Hidetoshi,ZHU Hua,et al. Synthesis of long-term acid-stable zeolite membranes and their potential application to esterification reactions[J]. Journal of Membrane Science,2009,339:224-232.
[9] KITA Hidetoshi,HORⅡ Kohji,TANAKA Kazuhiro,et al. Synthesis of a zeolite NaA membrane for pervaperation of water/organic liquid mixtures[J]. Journal of Material Science Letters,1995,14:206.
[10] LIPNIZKI Frank,FIELD Robertw,TEN Po-kiong. Pervaporation based hydrid process:a review of process design,applications and economics[J]. Journal of Membrane Science,1999,153:183-210.
[11] 杨丽君,殷德宏,王金渠,等. 采用复合晶种法在大孔载体上制备高性能ZSM-5沸石膜[J]. 硅酸盐通报,2012,31:1212-1217.
[12] 金鸽,周志辉,刘红,等. 无模板剂ZSM-5沸石膜在乙酸乙酯渗透汽化脱水中的应用[J]. 石油学报,2015, 31:31-37.
[13] ZHU Meihua,LU Zhanghui,KUMAKIRI Izumi,et al. Preparation and characterization of high water perm-selectivity ZSM-5 membrane without organic template[J]. Journal of Membrane Science,2012, 415-416:57-65.
[14] ZHU Meihua,KUMAKIRI Izumi,TANAKA Kazuhiro,et al. Dehydration of acetic acid and esterification product by acid-stable ZSM-5 membrane[J]. Microporous and Mesoporous Materials,2013, 181:47-53.
[15] 张雄福,王金渠,刘海鸥,等. ZSM-5沸石膜的合成及成膜因素研究[J]. 石油学报,2001,17:9-14.
[16] HU Na,ZHENG Yihong,YANG Zhen,et al. Mircowave synthesis of high-flux NaY zeolite membranes in fluoride media[J]. The Royal Society of Chemistry Advance,2015,5:87556-87563.
[17] 张飞,郑艺鸿,桂田,等. 含氟体系中高性能T型分子筛膜的合成[J]. 无机化学学报,2014,30:1845-1854.
[18] SUN Weiguo,WANG Xianwu,YANG Jianhua,et al. Pervaporation separation of acetic acid-water mixtures through Sn-substituted ZSM-5 zeolite membranes[J]. Journal of Membrane Science,2009, 335:83-88.

二次水热合成法制备ZSM-5分子筛膜及其渗透汽化性能

Secondary hydrothermal synthesis of ZSM-5 zeolite membrane and its pervaporation performance

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