期刊
INORGANIC CHEMISTRY
卷 60, 期 12, 页码 9122-9131出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c01104
关键词
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资金
- National Natural Science Foundation of China [21701039]
- Hebei Natural Science Foundation [B2017201055]
- Priority Strategy Project of Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of Ministry of Education [ts2020005]
- Postgraduate's Innovation Fund Project of Hebei University [HBU2021ss018]
The newly synthesized porous copper-organic framework compound 1 exhibits a porous structure capable of adsorbing harmful dyes, and demonstrates high selectivity in CO2 absorption and catalyzing cycloaddition reactions. The CO2 cycloaddition mechanism was revealed through DFT calculations, providing important insights for the design of efficient MOFs catalysts.
A new porous copper-organic framework assembled from 12-nuclear [Cu-12] nanocages {[Cu-2(L4-)(H2O)(2)]center dot 4DMA center dot 2H(2)O}(n) (1) (H4L = 5,5'-(butane-1,4-diyl)-bis(oxy)-diisophthalic acid) was successfully prepared and structurally characterized. Compound 1 feathering of a 3D framework with two types of 1D nanotubular channels and a large specific surface area can effectively enrich various harmful dyes. Additionally, due to the carbon dioxide (CO2) interactions with open Cu(II) sites and the electron-rich ether oxygen atoms of ligand in 1, it exhibits a highly selective CO2 uptake. Interestingly, 1 can effectively catalyze the cycloaddition reaction of CO2 with various epoxides under mild conditions, which is ascribed to the Lewis acid Cu(II) sites in the framework of 1. Importantly, 1 acting as a heterogeneous catalyst can be recycled at least 10 times without an obvious loss of catalytic activity, and the CO2 cycloaddition mechanism was further uncovered by density functional theory (DFT) calculations. This study can greatly enrich the MOF catalysts system of CO2 conversion and also provide a valuable guidance for the design of efficient MOFs catalysts.
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