Rh-catalyzed formation of dioxolanes from alpha-alkyl diazoesters: diastereoselective cycloadditions of carbonyl ylides with selectivity over beta-hydride elimination

J Org Chem. 2008 Feb 15;73(4):1435-9. doi: 10.1021/jo702308f. Epub 2008 Jan 12.

Abstract

Described here is a diastereoselective Rh-catalyzed method for the preparation of dioxolanes from alpha-alkyl-alpha-diazoesters. This represents the first general method for generating carbonyl ylides from alpha-diazoesters that possess beta-hydrogens, as such diazo compounds typically give rise to alkenes via beta-hydride elimination. Subsequent cycloaddition with aromatic aldehydes gives tetrasubstituted dioxolanes with unusually high diastereoselectivity. A model is set forth to explain the diastereoselectivity of the cycloaddition.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Catalysis
  • Cyclization
  • Dioxolanes / chemistry*
  • Esters
  • Hydrogen / chemistry
  • Ketones / chemistry*
  • Magnetic Resonance Spectroscopy
  • Rhenium / chemistry*
  • Spectrometry, Mass, Electrospray Ionization
  • Spectrophotometry, Infrared

Substances

  • Dioxolanes
  • Esters
  • Ketones
  • Rhenium
  • Hydrogen