化工进展 ›› 2017, Vol. 36 ›› Issue (09): 3323-3328.DOI: 10.16085/j.issn.1000-6613.2017-0044

• 工业催化 • 上一篇    下一篇

离子液体催化转化CO2合成碳酸丙烯酯

郭立颖, 邓莉莉, 胡卫东, 金先超, 殷龙珠   

  1. 沈阳工业大学石油化工学院, 辽宁 辽阳 111003
  • 收稿日期:2017-01-09 修回日期:2017-03-21 出版日期:2017-09-05 发布日期:2017-09-05
  • 通讯作者: 郭立颖(1981-),女,博士,硕士生导师,主要从事离子液体结构设计与制备及其改性高分子材料或工业催化等方面的研究。
  • 作者简介:郭立颖(1981-),女,博士,硕士生导师,主要从事离子液体结构设计与制备及其改性高分子材料或工业催化等方面的研究。E-mail:lyguo1981@163.com
  • 基金资助:
    国家自然科学基金(21706163)、辽宁省科技厅自然科学基金(201602537)及大学生创新创业计划训练项目。

Ionic liquids as catalysts for conversion of CO2 to propylene carbonate

GUO Liying, DENG Lili, HU Weidong, JIN Xianchao, YIN Longzhu   

  1. School of Petrochemical Engineering, Shenyang University of Technology, Liaoyang 111003, Liaoning, China
  • Received:2017-01-09 Revised:2017-03-21 Online:2017-09-05 Published:2017-09-05

摘要: 首先采用7种离子液体分别催化二氧化碳与环氧丙烷合成碳酸丙烯酯,考察离子液体种类对催化性能的影响,确定最优催化剂是离子液体溴化1-乙胺基-3-甲基咪唑盐[AeMIM]Br。然后研究辅助催化剂Lewis酸与离子液体[AeMIM]Br复合体系对催化性能的影响,再将最优复合催化体系[AeMIM]Br/(ZnBr22与正硅酸乙酯通过溶胶-凝胶法制备硅胶负载型复合离子液体,实现催化剂的相态转变并有利于实现固定床催化工艺,研究硅胶负载的复合离子液体催化转化二氧化碳进行环加成反应的影响。结果表明,离子液体的结构特点对催化性能影响很大,对于烷基咪唑离子液体其侧链长度越长,催化性能越好;功能化离子液体催化性能要优于烷基咪唑离子液体,且Lewis酸ZnBr2的加入明显提高催化效果。当正硅酸乙酯与复合离子液体[AeMIM]Br/(ZnBr22配比为1:2时,所制备的硅胶负载复合离子液体催化性能最佳,其转化率为96.9%,选择性为94.8%,转化频率为3124h-1。该催化剂催化性能稳定,可多次循环使用。

关键词: 离子液体, 催化, 二氧化碳

Abstract: Seven kinds of ionic liquids were used in the reaction of carbon dioxide and propylene oxide to synthesize propylene carbonate,and 1-bromide ethylamine-3-methyl imidazolium ionic liquid[AeMIM]Br showed the best catalytic performance. Then the catalytic properties of ionic liquid[AeMIM]Br mediated Lewis acid was investigated. After that,the optimal composite catalytic system[AeMIM]Br/(ZnBr2)2 was reacted with the tetraethyl orthosilicate(TEOS)prepared ionic liquid catalyst supported on silica gel,which achieved the phase transition of the catalyst and was helpful to realize the catalytic progress in fixed bed reactor. The silica gel supported catalyst was applied to cycloaddition reaction with CO2 in order to investigate its catalytic efficiency. The results showed that the structure characteristics of ionic liquids had great influence on the catalytic properties. For alkyl imidazole ionic liquids,the longer the side chain,the better the catalytic properties. The catalytic activities of functionalized ionic liquids were superior to alkyl imidazole ionic liquids,and thus the addition of Lewis acid ZnBr2 to the catalytic system could improve the catalytic effect significantly. The best catalytic performance was obtained when the ratio of TEOS and[AeMIM]Br/(ZnBr2)2 was 1:2,giving rise to the conversion rate of 96.9%,selectivity of 94.8%,and the turnover frequency (TOF) of 3124h-1. The catalytic performance of this catalyst was stable and could be reused many times.

Key words: ionic liquids, catalysis, carbon dioxide

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