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Asymmetric boronate addition to o-quinone methides: ligand exchange, solvent effects, and Lewis acid catalysis.


Type

Article

Change log

Authors

Grayson, Matthew N 
Goodman, Jonathan M 

Abstract

Density functional theory calculations suggest that asymmetric boronate addition to o-quinone methides proceeds via a Lewis acid catalyzed process through a closed six-membered transition structure. The BINOL-derived catalyst undergoes an exchange process with the original ethoxide boronate ligands. This activation mode successfully accounts for the sense and level of enantioselectivity observed experimentally. A qualitative model which accurately predicts the observed enantioselectivity has been developed and is consistent with results from our study of ketone propargylation demonstrating the reaction model's generality. The effects of replacing the BINOL framework with H8-BINOL have been rationalized.

Description

Keywords

Boronic Acids, Catalysis, Indolequinones, Lewis Acids, Ligands, Models, Molecular, Molecular Structure, Quantum Theory, Solvents, Thermodynamics

Journal Title

J Org Chem

Conference Name

Journal ISSN

0022-3263
1520-6904

Volume Title

80

Publisher

American Chemical Society (ACS)
Sponsorship
We thank Girton College, Cambridge (Research Fellowship to M.N.G.), the EPSRC (studentship to M.N.G.), and Unilever for support.