期刊
CHEMSUSCHEM
卷 15, 期 19, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202201386
关键词
carbon dioxide; formamides; heterogeneous catalysis; homogeneous catalysis; metal-organic frameworks
资金
- NSFC [22121005, 21875120]
- Fundamental Research Funds for the Central Universities [63223012]
Environmental problem caused by carbon emission has attracted widespread attention. This study developed a new dual-active site catalyst for converting CO2 into formamides, which has the advantages of high efficiency, low cost, and reusability. It provides a reliable approach to unify the advantages of homogeneous and heterogeneous catalysts, and has significant implications for synthetic chemistry and environmental protection.
Environmental problem caused by carbon emission is of widespread concern. Involving CO2 as C-1 resource into chemical synthesis is one of the most attractive ways for carbon recycling. Herein, the first example of host-guest composites featuring metal-organic framework (MOF)-encapsulated binuclear N-heterocyclic carbene (NHC) complex, Co-2@MIL101, was developed with the molecularly dispersed [Co(IPr)Br](2)(mu-Br)(2) (Co-2) loading in the cage of MIL-101(Cr) via a ligand-in-dimer-trap strategy, which was comprehensively investigated through various techniques including synchrotron X-ray absorption, electron microscopy, X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and others. The noble-metal-free double-sites catalyst Co-2@MIL101 exhibited promising stability, activity, efficiency, reusability, and substrate adaptability for converting CO2 into various formamides with amines and hydrosilanes and achieved the best performance for one of the most useful formamides, N-methyl-N-phenylformamide (MFA), among the recyclable catalysts at ambient conditions, providing a reliable approach to successfully unify the advantages of both homo- and heterogeneous catalysts. Density functional theory calculations were applied to illustrate the superior activity of the binuclear NHC complex center as double-sites catalyst toward the activation of CO2.
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