Biocatalytic asymmetric rearrangement of a methylene-interrupted bis-epoxide: simultaneous control of four asymmetric centers through a biomimetic reaction cascade

Chemistry. 2004 Jul 19;10(14):3467-78. doi: 10.1002/chem.200400061.

Abstract

Asymmetric enzyme-catalyzed hydrolysis of methylene-interrupted bis-epoxides 1 a and 1 b catalyzed by bacterial epoxide hydrolases furnished tetrahydrofuran derivatives 2 a and 2 b through a hydrolysis-rearrangement cascade. Whereas racemic bis-oxiranes 1 b-d underwent kinetic resolution with moderate stereoselectivities to yield products with up to 92 % ee and 66 % de: meso-bis-oxirane cis,cis-1 a was transformed into (6R,7R,9S,10S)-2 a in 94 % ee and 89 % de at high conversion (85 %) by Rhodococcus sp. CBS 717.73 as the major product. The reaction sequence resembles a biomimetic reaction cascade and provides an efficient entry into the structural core of annonaceous acetogenins with simultaneous control of four stereocenters.

MeSH terms

  • Actinomycetales / enzymology
  • Biomimetics*
  • Catalysis
  • Cyclization
  • Epoxide Hydrolases / metabolism*
  • Epoxy Compounds / chemistry*
  • Epoxy Compounds / metabolism*
  • Hydrocarbons / chemistry
  • Hydrocarbons / metabolism
  • Hydrolysis
  • Methane / analogs & derivatives*
  • Methane / chemistry
  • Methane / metabolism
  • Molecular Structure
  • Stereoisomerism

Substances

  • Epoxy Compounds
  • Hydrocarbons
  • carbene
  • Epoxide Hydrolases
  • Methane