Porous Zn(Bmic)(AT) MOF with Abundant Amino Groups and Open Metal Sites for Efficient Capture and Transformation of CO2

被引:73
作者
Li, Yixing [1 ]
Zhang, Xiao [1 ]
Lan, Jianwen [1 ]
Xu, Ping [1 ]
Sun, Jianmin [1 ]
机构
[1] Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, MIIT Key Lab Crit Mat Technol New Energy Convers, Sch Chem & Chem Engn, Harbin 150080, Heilongjiang, Peoples R China
基金
中国国家自然科学基金;
关键词
CARBON-DIOXIDE CAPTURE; ORGANIC FRAMEWORK; CHEMICAL FIXATION; CYCLIC CARBONATES; CATALYTIC CONVERSION; ADSORPTION; CYCLOADDITION; EPOXIDES;
D O I
10.1021/acs.inorgchem.9b01762
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
An efficient Zn(Bmic)(AT) MOF with available Lewis acid-base blocks was prepared by a solvothermal method combining the mixed ligands 5-aminotetrazole (HAT) and 1-benzimidazole-5-carboxylic acid (H(2)Bmic). The prepared Zn(Bmic)(AT) catalyst is rich in amino groups, uncoordinated oxygen atoms, and multiple open metal sites (OMSs), which contribute to CO2 adsorption of 79 cm(3)/g at 273 K and 52 cm(3)/g at 298 K, with high adsorption enthalpy (28 kJ mol(-1)). Furthermore, its multiple functional sites facilitate CO2 cycloaddition to various small-molecule epoxides to give five-ring cyclic carbonates with the assistance of a Bu4NBr cocatalyst, achieving a high TON of 170 for propylene carbonates (PC) under solvent-free, mild conditions (80 degrees C, 5 bar). In addition, the Zn(Bmic)(AT) catalyst exhibits good recyclability for six consecutive cycles. Moreover, a feasible synergistic mechanism of Zn(Bmic)(AT)/Bu4NBr catalysts for CO2 conversion into cyclic carbonate is proposed.
引用
收藏
页码:13917 / 13926
页数:10
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