期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 7, 页码 2795-2803出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c08466
关键词
crab-like Zn-2PDC MOF; flexible linker; open metal sites; CO2 transform; cyclic carbonates
资金
- National Natural Science Foundation of China [21972034, 21673060]
- State Key Lab of Urban Water Resource and Environment of Harbin Institute of Technology [HIT2019DX12]
A new tetratopic bridging ligand was designed and reacted with zinc centers to form a framework with high density zinc sites and coordinated water molecules, showing exceptional catalytic performance in CO2 cycloaddition to bulky styrene oxide. The catalyst also demonstrated good performance in cyclic use, retaining its catalytic activity after six cycles.
A new tetratopic bridging ligand 1,1'-(propane-1,3diyl)bis(1H-pyrazole-3,5-dicarboxylic acid) (PDC) with functional pyrazole groups was designed and used for reacting with environmentally friendly zinc centers in mixed solvents; the resulting framework [Zn3.5(PDC)2( H2O)10] (abbreviated as MOF Zn-2PDC) contained numerous organic-inorganic crablike blocks and had high density of zinc sites and coordinated water molecules. Abundant open metal sites (OMSs) were generated after the removal of coordinated water molecules by vacuum drying, which produced exceptionally catalytic performance for CO2 cycloaddition to bulky styrene oxide, and the produced styrene carbonate yield and selectivity reached up to 86 and 97% under mild conditions of 55 degrees C, 12 h, and 1 MPa. Moreover, MOF Zn- 2PDC also showed general applicability to other bulky epoxides. Meanwhile, the MOF Zn-2PDC catalyst remained with good catalytic performance after six cycles.
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