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Atomically Dispersed Co-N/C Catalyst for Divergent Synthesis of Nitrogen-Containing Compounds from Alkenes

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 7, 页码 4142-4149

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c12344

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A Co-N/C catalyst derived from a bimetal-organic framework with an atomically dispersed cobalt center is reported to show good activity in the chemoselective aziridination/oxyamination reactions of alkene and hydroxylamine, as well as late-stage functionalization of complex alkenes and diversified synthetic transformations of the aziridine product. This system operates without external oxidants and exhibits mild, atom-economic, and recyclable characteristics. Detailed spectroscopic characterizations and mechanistic studies reveal the structure of the catalytic center and possible intermediates involved in the mechanism cycle.
Alkene functionalization with a single-atom catalyst (SAC) which merges homogeneous and heterogeneous catalysis is a fascinating route to obtain high-value-added molecules. However, C-N bond formation of alkene with SAC is still unexplored. Herein, a bimetal-organic framework-derived Co-N/C catalyst with an atomically dispersed cobalt center is reported to show good activity of chemoselective aziridination/oxyamination reactions from alkene and hydroxylamine, and late-stage functionalization of complex alkenes and diversified synthetic transformations of the aziridine product further expand the utility of this method. Moreover, this system proceeds without external oxidants and exhibits mild, atom-economic, and recyclable characters. Detailed spectroscopic characterizations and mechanistic studies revealed the structure of the catalytic center and possible intermediates involved in the mechanism cycle.

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