Carbon dioxide(CO_2) capture and catalytic conversion has become an attractive and challenging strategy for CO_2 utilization since it is an abundant, inexpensive, and renewable C1 resource and a main greenhouse gas....Carbon dioxide(CO_2) capture and catalytic conversion has become an attractive and challenging strategy for CO_2 utilization since it is an abundant, inexpensive, and renewable C1 resource and a main greenhouse gas. Herein, a novel hydrazine-bridged covalent triazine polymer(HB-CTP) was first designed and synthesized through simple polymerization of cyanuric chloride with 2,4,6-trihydrazinyl-1,3,5-triazine. The resultant HB-CTP exhibited good CO_2 capture capacity(8.2 wt%, 0 °C, and 0.1 MPa) as well as satisfactory recyclability after five consecutive adsorption-desorption cycles. Such a polymer was subsequently employed as a metal-free heterogeneous catalyst for the cyclo-addition of CO_2 with various epoxides under mild and solvent-free conditions,affording cyclic carbonates with good to excellent yields(67%–99%) and high functional-group tolerance. The incorporation of hydrazine linkages into HB-CTP's architecture was suggested to play the key role in activating epoxides through hydrogen bonding. Moreover, HB-CTP can be reused at least five times without significant loss of its catalytic activity.展开更多
基金supported by the National Natural Science Foundation of China(21406025)the China Postdoctoral Science Foundation(2014M551067)the Start-Up Foundation of Dalian University of Technology(DUT13RC(3)58)~~
文摘Carbon dioxide(CO_2) capture and catalytic conversion has become an attractive and challenging strategy for CO_2 utilization since it is an abundant, inexpensive, and renewable C1 resource and a main greenhouse gas. Herein, a novel hydrazine-bridged covalent triazine polymer(HB-CTP) was first designed and synthesized through simple polymerization of cyanuric chloride with 2,4,6-trihydrazinyl-1,3,5-triazine. The resultant HB-CTP exhibited good CO_2 capture capacity(8.2 wt%, 0 °C, and 0.1 MPa) as well as satisfactory recyclability after five consecutive adsorption-desorption cycles. Such a polymer was subsequently employed as a metal-free heterogeneous catalyst for the cyclo-addition of CO_2 with various epoxides under mild and solvent-free conditions,affording cyclic carbonates with good to excellent yields(67%–99%) and high functional-group tolerance. The incorporation of hydrazine linkages into HB-CTP's architecture was suggested to play the key role in activating epoxides through hydrogen bonding. Moreover, HB-CTP can be reused at least five times without significant loss of its catalytic activity.