基于两性离子型季铵盐-KI的温度控制自分离离子液体(IL)催化体系用于二氧化碳固定反应

doi:10.1016/S1872-2067(18)63101-8

催化学报 ›› 2018, Vol. 39 ›› Issue (11): 1854-1860.DOI: 10.1016/S1872-2067(18)63101-8

• 论文 • 上一篇

基于两性离子型季铵盐-KI的温度控制自分离离子液体(IL)催化体系用于二氧化碳固定反应

付西英^a, 谢鹏涛^b, 连一苇^a, 何乐芹^a, 赵伟^c, 常涛^a, 秦身钧^a

a 河北工程大学材料科学与工程学院, 河北邯郸 056038;
b 邯郸学院化学化工与材料学院, 河北邯郸 056005;
c 南阳师范学院化学与制药工程学院, 河南南阳 473061

收稿日期:2018-03-31 修回日期:2018-05-14 出版日期:2018-11-18 发布日期:2018-09-01
通讯作者: 常涛, 秦身钧
基金资助:
国家自然科学基金（41330317，21403051）；河北省自然科学基金（B2016402030，B2017402079）；河北省高等学校科学研究项目（ZD2015113）；邯郸市科学技术研究与发展计划（1621211041-3，1622201049-2）；河北省高校百名创新人才项目（BR2-204）.

Temperature-responsive self-separation ionic liquid system of zwitterionic-type quaternary ammonium-KI for CO₂ fixation

Xiying Fu^a, Pengtao Xie^b, Yiwei Lian^a, Leqin He^a, Wei Zhao^c, Tao Chang^a, Shenjun Qin^a

a College of Material Science and Engineering, Hebei University of Engineering, Handan 056038, Hebei, China;
b College of Chemical Engineering and Materials, Handan College, Handan 056005, Hebei, China;
c College of Chemistry and Pharmaceutical Engineering, Nanyang Normal University, Nanyang 473061, Henan, China

Received:2018-03-31 Revised:2018-05-14 Online:2018-11-18 Published:2018-09-01
Contact: 10.1016/S1872-2067(18)63101-8
Supported by:
This work was supported by the National Natural Science Foundation of China (41330317, 21403051), the Natural Science Foundation of Hebei province (B2016402030, B2017402079), the Science and Technology Foundation of Universities of Hebei Province (ZD2015113), the Science and Technology Research Development Program of Handan (1621211041-3, 1622201049-2), and the Program for One Hundred Innovative Talents in Universities of Hebei Province (BR2-204).

摘要/Abstract

摘要：

随着在世界各国工业化进程不断加快，人类对煤、石油、天然气等化石燃料的需求越来越大，既加速了能源短缺，又排放了大量CO₂.CO₂又成为分布最广、价格便宜和储量丰富的碳资源.人类除了努力做到CO₂减排，又可将其转化为能源、材料和各种化工产品.CO₂与环氧化合物发生偶联反应生成环碳酸酯，具有原子经济性，符合绿色化学的观点，是最有前景的方法之一.CO₂可以与三元环氧化合物发生偶联反应生成五元环状碳酸酯，它是当今合成环碳酸酯比较成熟的方法.已经被设计合成并应用的高效催化体系有离子液体催化剂、金属盐或氧化物催化剂、有机催化剂、希夫碱金属配合物催化剂以及大环金属配合物催化剂等等，但最有效的催化剂还是均相催化剂，其最大的缺点在于催化剂和产物分离困难.既有均相催化剂高的催化活性，又能像多相催化剂易于分离，是人们设计新催化剂的目标.
本文设计合成了一系列含有不同烷基链长度的两性离子型季铵盐（ZTQAs），可以与KI协同催化CO₂与环氧化合物偶联反应.随着烷基链的增长，ZTQAs在碳酸丙烯酯中表现出温度调控的自分离特性.通过X射线光电子能谱和量子化学计算证实，ZTQAs与KI之间存在明显的相互作用，从而增强了碘离子的亲核能力.当反应条件为125℃，CO₂压力1.5MPa以及1mol%催化剂用量下，DTPS/KI催化剂取得了良好的收率（95.1%）.并且该催化剂可以从催化系统中自发的析出，因而既表现出均相催化剂的高活性，又可以像非均相催化剂那样循环使用.该催化剂催化各种环氧化合物与CO₂偶联反应中均显示出良好的催化性能.

关键词: 二氧化碳, 自分离, 环碳酸酯, 两性离子型季铵盐, 碘化钾

Abstract:

A series of zwitterionic-type quaternary ammoniums (ZTQAs) with varying lengths of alkyl chains combined with KI were synthesized and considered as catalysts for the coupling reaction of CO₂ and various terminal epoxides. The prolonged alkyl chain of ZTQAs exhibited temperature-responsive self-separation in propylene carbonate (PC). The interaction between ZTQAs and KI was confirmed by X-ray photoelectron spectroscopy and quantum chemical calculations. This interaction strengthened the nucleophilicity of the I^- ion, favoring the catalytic reaction. The 3-(dimethyltetradecylammonium) propane sulfonate (DTPS)/KI showed an excellent yield of PC (95.1%) at 125℃, 1.5 MPa, and 1 mol% loading of catalyst. The precipitate formed spontaneously from the catalytic system, providing high catalytic activity of the homogeneous catalyst, as well as easy recovery of the heterogeneous catalyst.

Key words: Carbon dioxide, Self-separation, Cyclic carbonate, Zwitterionic-type quaternary ammonium, KI

付西英, 谢鹏涛, 连一苇, 何乐芹, 赵伟, 常涛, 秦身钧. 基于两性离子型季铵盐-KI的温度控制自分离离子液体(IL)催化体系用于二氧化碳固定反应[J]. 催化学报, 2018, 39(11): 1854-1860.

Xiying Fu, Pengtao Xie, Yiwei Lian, Leqin He, Wei Zhao, Tao Chang, Shenjun Qin. Temperature-responsive self-separation ionic liquid system of zwitterionic-type quaternary ammonium-KI for CO₂ fixation[J]. Chinese Journal of Catalysis, 2018, 39(11): 1854-1860.

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基于两性离子型季铵盐-KI的温度控制自分离离子液体(IL)催化体系用于二氧化碳固定反应

Temperature-responsive self-separation ionic liquid system of zwitterionic-type quaternary ammonium-KI for CO₂ fixation

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基于两性离子型季铵盐-KI的温度控制自分离离子液体(IL)催化体系用于二氧化碳固定反应

Temperature-responsive self-separation ionic liquid system of zwitterionic-type quaternary ammonium-KI for CO2 fixation

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Temperature-responsive self-separation ionic liquid system of zwitterionic-type quaternary ammonium-KI for CO₂ fixation