Sequence and Equivalent of Reagents Addition in NHC-Catalyzed Oxidative
Nonpolar Inversion Enable Conversion from Aldimine to Benzoxazole
Abstract
Mechanism of the oxidative nonpolar inversion reaction catalyzed by
N-heterocyclic carbenes (NHCs) to achieve benzoxazoles was investigated
in very details. The reaction was revealed to occur through five
processes, and for oxidation in the second process, two successive
tautomerizations followed by oxidation were demonstrated to be more
energetically favorable than the other two pathways. The
rate-determining step was disclosed to be the oxidation by
3,3’-5,5’-tetra-tert-butyl-4,4’-diphenoquinone (DQ). Afterwards,
mechanism calculations to the non-catalyzed reaction was conducted and
it was revealed that the excessive exothermic property of the initial
step should be the main reason for the extremely high barrier in the
following step. While with participation of NHC, this unfavorable
transformation can be deftly prevented according to the specific
sequence and amount of reagents addition, and therefore to enable the
reaction to occur under mild conditions.