Abstract
The unexpected oxyamination reaction of O, ω-unsaturated alkoxyamines was found experimentally. The mechanistic issues were studied by DFT calculations. It is suggested that the reaction undergoes [3 + 2] cyclic addition, ON bond cleavage, CN reductive elimination, and the RhN unit protonation, generating the product and regenerating the active catalyst. The nitrene Rh(V) species containing a RhC bond rather than a RhO bond was suggested to be involved in the reaction mechanism. Why the substrate A with X = O but not X = C undergoes oxyamination reaction was rationalized based on the suggested reaction mechanism.
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