Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 27, Issue 60, Pages 14947-14963Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202102408
Keywords
DFT; In-situ DRIFTS; NBO; Lewis acid; Spn Topology
Categories
Funding
- National Natural Science Foundation of China [21968002]
- Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, Guangxi University [2019k006]
- high-performance computing platform of Guangxi University
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The series of MOFs with a 6-connected spn topology were synthesized and characterized for their Lewis acidity properties. The mesoporous structure MOFs showed higher catalytic activity, with MOF-818 having a higher acid site density. The density functional theory proposed the mechanism for the cycloaddition reaction of carbon dioxide and styrene oxide.
A series of MOFs with a 6-connected spn topology were synthesized (MOF-808-(Zr, Hf), PCN-777-(Zr, Hf), MOF-818-(Zr, Hf)). Through the in situ DRIFTS of NH3 adsorption-desorption, we found that the activated catalyst mainly contains Lewis acid sites. The effects of different organic ligands on the Lewis acid of the Zr-6 cluster were analyzed by XPS and NH3-TPD, and the relative Lewis acidity of the same metal was obtained: PCN-777>MOF-808>MOF-818. In the Py-FTIR results, we confirmed that MOF-818 has a higher acid site density. In the activity test, MOFs with mesoporous structure showed better catalytic activity under normal temperature and pressure. Among them, MOF-818 can still maintain a high degree of crystallinity after catalysis. Finally, we use density functional theory to propose the mechanism of the cycloaddition reaction of carbon dioxide and styrene oxide. The results show that the metal is coordinated with styrene oxide and halogens attack the beta carbon of the epoxide.
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