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ZSM-5分子筛膜在乙酸异戊酯酯化反应中的应用

作者：薛淼，朱美华，钟彩君，杨一鸣，李玉琴，胡娜，张飞，陈祥树

单位：江西师范大学

关键词： ZSM-5分子筛膜；乙酸异戊酯；酯化反应；渗透汽化

DOI号：

分类号： O6，TQ， G3

出版年,卷(期):页码： 2018,38(4):107-112

摘要：

通过渗透汽化技术将高性能ZSM-5分子筛膜应用于原位脱除乙酸和异戊醇酯化反应产生的水，从而打破酯化反应的平衡和提高乙酸异戊酯的收率。本论文重点考察反应条件对乙酸异戊酯收率的影响，结果表明，当采用2.0 wt%硫酸氢钠为催化剂，反应温度为100 °C时，乙酸与异戊醇的初始摩尔比为3.0/1.0，乙酸异戊酯的收率达到98.39%，分子筛膜的通量和分离因子（水/有机物）分别为0.21 kg·m-2·h-1和1040。此外，分子筛膜在酯化反应中表现出良好的稳定性，间歇重复使用8次或连续经过160 h的长时间耦合酯化反应后，乙酸异戊酯收率仍可高达97.73%。

The high performance ZSM-5 zeolite membrane is in-situ removed H2O from the esterification of acetic acid and isoamyl alcohol by pervaporation. Influences of reaction conditions on the ethanol conversion are studied in details. Compared with the traditional esterification of acetic acid and isoamyl alcohol, the esterification with “membrane extractor” has a well isoamyl acetate yields at low reaction temperature. As the reaction temperature, acetic acid/ isoamyl alcohol molar ratio, and effective membrane surface area to esterification mixture ratio volume are 100 ºC, 3.0/1.0 and 0.26 cm2/cm3, the isoamyl acetate yields is 98.39%, and the corrseponding membrane total flux and separation factor (H2O to organic) are 0.21 kg·m-2·h-1 and 1040, respectively. Besides, the ZSM-5 zeolite membrane shows well long-term stablilty and reproducibility for the pervaporation-esterification, the isoamyl acetate yields of the esterification-pervaporation for intermittent 8 times or continuous 160 h are still kept 97.73%. In addition, the ZSM-5 zeolite membrane is still kept the MFI zeolite structure and morphology by XRD, SEM and EDX characterization results.

基金项目：

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)，江西省自然科学基金（20151BAB213037）

作者简介：

第一作者简介：薛淼（1994年4月），女，陕西咸阳，硕士研究生，研究方向为分子筛膜的制备与应用 E-mail：xuemiao0402@163.com 通讯作者，E-mail：zhumeihua@jxnu.edu.cn, cxs66cn@jxnu.edu.cn

参考文献：

[1]Yang Z H, Zhou C X, Zhang W X, et al. β-MnO2 nanorods: A new and efficient catalyst for isoamyl acetate synthesis[J]. Colloids Surf., A, 2010, 356: 134-139.
[2]Wilmar O-V, Harold N I-T, Izabela D-G, et al. Hybrid membrane and conventional processes comparison for isoamyl acetate production[J]. Chem Eng Process, 2014, 76: 70-82.
[3]Michael J. E, José I. R. Enhanced synthesis of isoamyl acetate using an ionic liquid-alcohol biphasic system at high hydrostatic pressure[J]. J Mol Catal B: Enzym. 2010, 76: 36-40.
[4]Su X, Zhang W D, Qing W H, et al. Modeling study of a pervaporation membrane reactor for improving oxime hydrolysis reaction[J]. J Membr Sci. 2016, 497: 410-420.
[5]Han Y, Lv E, Ma L L, ea al. Coupling membrane pervaporation with a fixed-bed reactor for enhanced esterification of oleic acid with ethanol[J]. Energy Convers Manage. 2015, 106: 1379-1386.
[6]Nigiz F U, Hilmioglu N D. Simultaneous separation performance of a catalytic membrane reactor for ethyl lactate production by using boric acid coated carboxymethyl cellulose membrane[J]. React Kinet Catal Lett. 2016, 118: 557-575.
[7]祝春芳, 王忠铭, 袁振宏等. 用于酯化反应的亲水性渗透汽化膜研究进展[J]. 膜科学与技术, 2011, 31(5): 94-99.
[8]章龙, 彭勇, 余立新等.己二酸和甲醇酯化反应与渗透汽化脱水耦合过程的研究[J]. 膜科学与技术, 2008, 28: 99-101.
[9]Tanaka K, Yoshikawa R, Cui Y, et al. Application of Zeolite T Membranes to Esterification Reactions[J]. Catal Today, 2001, 67(1/3): 121-125.
[10]张飞, 胡娜, 周荣飞等. T型分子筛膜的制备及其在酯化反应中的应用[C]// 中国膜科学与技术报告会. 中国膜工业协会, 2010.
[11]Hasegawa Y, Abe C, Mizukami F, et al. Application of a CHA-type zeolite membrane to the esterification of adipic acid with isopropyl alcohol using sulfuric acid catalyst[J]. J Membr Sci. 2012, 415-416: 368-374.
[12]Rathod A P, Wasewar K L, Sonawane S S. Intensification of esterification reaction of lactic acid with iso-propanol using pervaporation reactor[J]. Procedia Eng. 2013, 51: 456-460.
[13]Zhu M H, Feng Z J, Hua X M, et al. Application of a mordenite membrane to the esterification of acetic acid and alcohol using sulfuric acid catalyst[J]. Microporous Mesoporous Mater. 2016, 233:171-176.
[14]张富娟, 张翔宇, 盛淑玲. 硫酸氢钠催化合成乙酸异戊酯的研究[J]. 食品工业科技, 2004, 1: 48.
[15]吴春燕. 硫酸氢钠催化合成水杨酸正丁酯[J]. 化工技术与开发, 2015, 44(1): 21-22.
[16]Zhu M H, Lu Z H, Kumakiri I, et al. Preparation and characterization of high water perm-selectivity ZSM-5 membrane without organic template[J]. J Membr Sci. 2012, 415-416: 57-65.
[17]Zhu M H, Kumakiri I, Tanaka K, et al. Dehydration of acetic acid and esterification product by acid-stable ZSM-5 membrane[J]. Microporous Mesoporous Mater. 2013, 181: 47-53.
[18]Zhang J C, Meng X J, Cao W L. Preparation and catalytic performance of novel water-tolerant Zr(SO4)2/AC solid acid catalyst[J]. Chin J Catal, 2006, 27(2): 135-138.

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