Rational design of Lewis acid-base bifunctional nanopolymers with high performance on CO2/epoxide cycloaddition without a cocatalyst

被引:54
|
作者
Zhang, Wenwen [1 ]
Ping, Ran [1 ]
Lu, Xueyu [1 ]
Shi, Huibing [2 ]
Liu, Fusheng [1 ]
Ma, Jingjing [3 ]
Liu, Mengshuai [1 ]
机构
[1] Qingdao Univ Sci & Technol, Coll Chem Engn, State Key Lab Base Ecochem Engn, Qingdao 266042, Peoples R China
[2] Shandong Chambroad Petrochem Co Ltd, Binzhou 256500, Peoples R China
[3] Ningxia Univ, State Key Lab High Efficiency Utilizat Coal & Gree, Yinchuan 750021, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2 activation and conversion; Zwitterionic porous organic polymer; Green medium; Multifunctional catalyst; Cyclic carbonate; METAL-ORGANIC FRAMEWORK; CO2; CAPTURE; CYCLIC CARBONATES; CATALYST; EPOXIDES; FIXATION; POLYMERS; CONVERSION; DIOXIDE;
D O I
10.1016/j.cej.2022.138715
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Based on the Schiff base reaction and post-modification strategy, novel nanocomposites of pyridine-zinc-based ionic porous organic polymers (Py-Zn@IPOPx, X = Br, I, Ac) were constructed and structurally characterized. Various Py-Zn@IPOPx were applied to the transformation of CO2 and epoxides into cyclic carbonates, and their catalytic activities were studied and discussed in detail. The results showed that Py-Zn@IPOP] possesses Lewis acid-base bifunctional features, and also modified with superior nucleophilic active groups, which exerted an important synergistic effect on activation of CO2 and epoxide, and ring-opening of epoxide. Under co-catalyst/ solvent-free conditions, Py-Zn@IPOP] could afford 96 % PC yield and 99 % selectivity at 120 degrees C and 2.0 MPa CO2 pressure for 6 h, and turnover frequency (TOF) was high to 230 h(-1). Moreover, the reusability and versatility of the catalyst were examined, and the catalytic mechanism was speculated according to the obtained results. Compared with previously reported porous polymer catalysts, Py-Zn@IPOP ] requires much greener and milder reaction conditions while avoids the use of a co-catalyst, displaying bright prospects for the design and synthesis of ionic porous organic polymers for CO2 activation and utilization.
引用
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页数:10
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