Unprecedented catalytic asymmetric reduction of N-H imines

Org Lett. 2005 Jan 20;7(2):355-8. doi: 10.1021/ol047431x.

Abstract

[Reaction: see text] Addition of lithium bis(trimethylsilyl)amide to perfluorinated ketones 1a-j affords (E)-N-TMS-ketimines 2a-j that are reduced in situ to afford racemic perfluoromethylated amine hydrochloride salts 3a-j in 54-97% yields. Solvolysis of the N-Si bond in MeOH leads to formation of bench-stable, isolable N-H imine Z/E isomer mixtures along with a methanol adduct. Enantioselective reduction of these three-component mixtures provides the first catalytic asymmetric synthesis of trifluoromethylated amines in 72-95% yields and 75-98% ee.

MeSH terms

  • Amines / chemistry*
  • Catalysis
  • Hydrogen / chemistry*
  • Hydrogen / metabolism
  • Hydrogen Bonding
  • Imines / chemistry*
  • Nitrogen / chemistry*
  • Nitrogen / metabolism
  • Oxidation-Reduction
  • Stereoisomerism

Substances

  • Amines
  • Imines
  • Hydrogen
  • Nitrogen