Computational elucidation of the origins of reactivity and selectivity in non-aldol aldol rearrangements of cyclic epoxides

Org Lett. 2011 Jun 17;13(12):3238-41. doi: 10.1021/ol2011488. Epub 2011 May 13.

Abstract

The non-aldol aldol reaction of the isomeric epoxy silyl ethers is controlled by the conformation of the transition states leading to an internal hydride shift. One isomer rearranges to the β-silyloxy ketone whereas the other isomer gives a β-elimination product. Theoretical calculations show that the substrates with substituents that favor the formation of the chairlike transition state rearrange normally while those that do not undergo elimination instead.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Aldehydes / chemistry*
  • Epoxy Compounds / chemistry*
  • Ketones / chemistry*
  • Models, Theoretical*
  • Molecular Structure
  • Silanes / chemistry
  • Stereoisomerism

Substances

  • Aldehydes
  • Epoxy Compounds
  • Ketones
  • Silanes
  • 3-hydroxybutanal