A well-designed 3D metal-organic framework with accessible Lewis acid-base sites,[Zn_(2)(PZDC)(1/2ATZ)_(2)(H_(2)O)2·2.5H_(2)O](H_(2)PZDC=3,5-pyrazoledicarboxylic acid,5-ATZ=5-aminoterazole)abbreviated as Zn(PZDC)...A well-designed 3D metal-organic framework with accessible Lewis acid-base sites,[Zn_(2)(PZDC)(1/2ATZ)_(2)(H_(2)O)2·2.5H_(2)O](H_(2)PZDC=3,5-pyrazoledicarboxylic acid,5-ATZ=5-aminoterazole)abbreviated as Zn(PZDC)(ATZ),was successfully prepared by incorporating zinc(II)ions,3,5-pyrazoledicarboxylic acid and nitrogen-rich 5-aminoterazole.The existence of abundant Lewis bases can increase the chemical affinity to carbon dioxide,thus resulting in their high CO_(2)capture ability.Additionally,the heterogeneous Zn(PZDC)(ATZ)catalyst facilitated the CO_(2)coupling reaction of various epoxides into cyclic carbonates with the aid of Bu_(4)NBr under solvent-free conditions(90℃,1 MPa,6 h);besides,a high TON(131.0)and TOF(21.8 h^(−1))of propylene carbonates were obtained.Furthermore,the Zn(PZDC)(ATZ)catalyst also showed good chemical stability and recyclability for seven cycles without a significant catalytic loss.What’s more,a plausible catalytic mechanism of synergistic effects derived from Zn(PZDC)(ATZ)/Bu4NBr catalysts for CO_(2)conversion to cyclic carbonate was proposed.展开更多
基金the National Natural Science Foundation of China(21673060)the State Key Lab of Urban Water Resource and Environment of Harbin Institute of Technology(HIT2017DX10).
文摘A well-designed 3D metal-organic framework with accessible Lewis acid-base sites,[Zn_(2)(PZDC)(1/2ATZ)_(2)(H_(2)O)2·2.5H_(2)O](H_(2)PZDC=3,5-pyrazoledicarboxylic acid,5-ATZ=5-aminoterazole)abbreviated as Zn(PZDC)(ATZ),was successfully prepared by incorporating zinc(II)ions,3,5-pyrazoledicarboxylic acid and nitrogen-rich 5-aminoterazole.The existence of abundant Lewis bases can increase the chemical affinity to carbon dioxide,thus resulting in their high CO_(2)capture ability.Additionally,the heterogeneous Zn(PZDC)(ATZ)catalyst facilitated the CO_(2)coupling reaction of various epoxides into cyclic carbonates with the aid of Bu_(4)NBr under solvent-free conditions(90℃,1 MPa,6 h);besides,a high TON(131.0)and TOF(21.8 h^(−1))of propylene carbonates were obtained.Furthermore,the Zn(PZDC)(ATZ)catalyst also showed good chemical stability and recyclability for seven cycles without a significant catalytic loss.What’s more,a plausible catalytic mechanism of synergistic effects derived from Zn(PZDC)(ATZ)/Bu4NBr catalysts for CO_(2)conversion to cyclic carbonate was proposed.
