期刊
ADVANCED SUSTAINABLE SYSTEMS
卷 6, 期 3, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adsu.202100380
关键词
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资金
- National Natural Science Foundation of China [21908033]
- Fok Ying-Tong Education Foundation [161030]
- Program of Introducing Talents of Discipline to Universities of China (111 Program) [D20023]
- Guizhou Frontiers Science Center for Asymmetric Synthesis and Medicinal Molecules [[2020]004]
This study successfully utilizes the carboxylate-functionalized zeolitic imidazolate framework (F-ZIF-90) as a heterogeneous catalyst for the reductive N-functionalization of various amines with CO2. The catalyst exhibits good catalytic performance, thermodynamic stability, and adsorption capacity towards CO2, leading to the high-yield production of N-formyl compounds. This strategy provides a new avenue for the development of heterogeneous catalysts for the reductive upgrading of CO2.
Catalytic upgrading of CO2 into value-added chemicals to build the excess carbon cycle is of great significance. In this work, carboxylate-functionalized zeolitic imidazolate framework (F-ZIF-90) with good crystallinity and porosity is constructed from ZIF-90 and employed as a robust heterogeneous catalyst to boost the reductive N-functionalization of various amines with CO2 to furnish N-formyl compounds (up to 99% yield) in the presence of PhSiH3 under an ambient environment. The imidazole carboxylate species (-COO ) can not only activate hydrosilane and CO(2 )to form the key intermediate formoxysliane but also activate amines to participate in the N-formylation reaction to obtain the target product. Moreover, it can enhance the catalyst capture and exchange ability toward ambient CO2. The powerful adsorption capacity of the F-ZIF-90 catalyst toward CO2 is conducive to elevating CO2 concentration around the active species. Theoretical calculations show that the carboxylatemediated conversion path undergoes the transition state of hydrosilane activation with a relatively lower energy barrier (Delta G = 26.9 kcal mot(-1)). F-ZIF-90 exhibits good thermochemical stability with no obvious activity attenuation after repeated use 5 times. This strategy opens a new avenue based on ZIFs to develop heterogeneous catalysts for reductive upgrading of CO2.
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