多孔聚离子液体催化二氧化碳辅助环氧乙烷水合反应  

Porous Poly(ionic liquid)s-catalyzed Carbon Dioxide-promoted Hydration of Ethylene Oxide

作　　者：洪扬 李丹丹[1] 张景顺 章子旺 高国华[1] HONG Yang;LI Dandan;ZHANG Jingshun;ZHANG Ziwang;GAO Guohua(State Key Laboratory of Petroleum Molecular&Process Engineering,Shanghai Key Laboratory of Green Chemistry and Chemical Processes,School of Chemistry and Molecular Engineering,Institute of Eco-Chongming,East China Normal University,Shanghai 200062,China)

机构地区：[1]华东师范大学石油化工分子转化与反应工程全国重点实验室,上海市绿色化学与化工过程绿色化重点实验室,化学与分子工程学院,崇明生态研究院,上海200062

出　　处：《高等学校化学学报》2025年第5期100-108,共9页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:22172053);国家重点研发计划项目(批准号:2020YFA0710201)资助.

摘　　要：以刚性离子液体和有机碱为单体,通过自由基共聚法制备了一系列具有高比表面积和大孔结构的多孔聚离子液体.采用魔角旋转固体核磁共振波谱、傅里叶变换红外光谱、扫描电子显微镜、氮气吸附-脱附实验和热重分析对聚离子液体的结构、形貌和热稳定性进行了表征.结果表明,多孔聚离子液体的比表面积为100.9~374.7 m^(2)/g,孔容为0.41~0.86 cm^(3)/g,活性位点均匀分布在孔隙结构内.多孔聚离子液体同时具有离子液体与有机碱活性中心,能够协同催化CO_(2)辅助环氧乙烷水合反应,在低水合比(1.5∶1)条件下,乙二醇收率达到96.5%,选择性为96.5%,达到了与均相催化剂相当的催化性能;CO_(2)的助催化作用改变了水合反应的路径,极大地降低了反应的水合比,提高了乙二醇的选择性.该聚离子液体催化剂具有良好的底物适用性及可回收性,并且在烟气气氛下也具有良好的催化性能.As one of the energy-intensive processes,the production of ethylene glycol with high selectivity from ethylene oxide under low hydration ratios is a challenge in the industry.In this study,a series of porous poly(ionic liquid)s with high specific surface area and macroporous structure were synthesized through free radical copolymerization of rigid ionic liquids and organic base monomers.The structure,microscopic morphology,and thermal stability of the poly(ionic liquid)s were characterized by magic angle spinning nuclear magnetic resonance(MAS NMR)spectroscopy,Fourier transform infrared(FTIR)spectroscopy,scanning electron microscopy(SEM),N2 physical adsorption-desorption,and thermogravimetric analysis(TGA).These poly(ionic liquid)s have a specific surface area ranging from 100.9 m²/g to 374.7 m²/g,a pore volume ranging from 0.41 cm³/g to 0.86 cm³/g,with active sites uniformly distributed within the porous structure.Porous poly(ionic liquid)s possessing both the active centers of ionic liquids and organic bases could synergistically catalyze the CO_(2)-promoted hydration of ethylene oxide.Under a low hydration ratio of 1.5∶1,high yield(96.5%)and selectivity(96.5%)of ethylene glycol are achieved,which are comparable to the corresponding homogeneous catalysts.The CO 2-promoted catalysis alters the pathway of hydration reaction,significantly reducing the hydration ratio and improving the selectivity of ethylene glycol.In addition,the catalyst has good substrate applicability and recyclability,and it also shows good catalytic performance under the flue gas atmosphere.

关 键 词：乙二醇 环氧乙烷 多孔聚离子液体 二氧化碳辅助水合反应 

分 类 号：O643.2[理学—物理化学]