Litcius/Paper detail

Carbene‐Catalyzed Activation of C−Si Bonds for Chemo‐ and Enantioselective Cross Brook–Benzoin Reaction

Chenghao Tang, Wei Wang, Guoyong Luo, Chaoyang Song, Zhaowei Bao, Pei Li, Ge‐Fei Hao, Yonggui Robin, Zhichao Jin

2022Angewandte Chemie International Edition23 citationsDOI

Abstract

The first carbene-catalyzed asymmetric chemoselective cross silyl benzoin (Brook-Benzoin) reaction has been developed. Key steps of this reaction involve activation of the carbon-silicon bond of an acylsilane by a chiral N-heterocyclic carbene (NHC) catalyst to form a silyl acyl anion intermediate. These acyl anions then undergo an addition reaction with indole aldehydes in a highly chemo- and enantioselective manner to afford α-silyloxy ketones with excellent optical purities. The reaction mechanism of this cross Brook-Benzoin reaction was investigated through both experimental and computational methods. The chiral α-hydroxy ketone derivatives obtained by this approach show promising, agrochemically interesting activity against harmful plant bacteria.

Topics & Concepts

CarbeneEnantioselective synthesisBenzoinChemistrySilylationCatalysisUmpolungKetoneReaction mechanismMedicinal chemistryCombinatorial chemistryOrganic chemistryNucleophileN-Heterocyclic Carbenes in Organic and Inorganic ChemistrySynthetic Organic Chemistry MethodsCatalytic Cross-Coupling Reactions