An alkyne hydrosilylation-oxidation strategy for the selective installation of oxygen functionality

J Am Chem Soc. 2005 Jul 20;127(28):10028-38. doi: 10.1021/ja051578h.

Abstract

Alkynes bearing propargylic, homopropargylic, and bishomopropargylic hydroxyl groups are shown to serve as precursors for ketone or alpha-hydroxy ketone functionality. The approach hinges on the intermediacy of vinylsilanes created through regioselective hydrosilylation catalyzed by the complex [Cp*Ru(MeCN)3]PF6. Several oxidative pathways of linear and cyclic vinylsilanes are studied, and the possibility of diastereoselective epoxidation of cyclic vinylsilanes is demonstrated. The sequences constitute the equivalent of stereoselective aldol, homo-aldol, and bishomo-aldol type processes. The method is applied to a short synthesis of the piperidine alkaloid, spectaline.

Publication types

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

MeSH terms

  • Aldehydes / chemistry
  • Alkynes / chemistry*
  • Molecular Structure
  • Organosilicon Compounds / chemical synthesis*
  • Organosilicon Compounds / chemistry
  • Oxidation-Reduction
  • Oxygen / chemistry*
  • Oxygen / physiology
  • Piperidines / chemical synthesis
  • Piperidines / chemistry
  • Stereoisomerism

Substances

  • Aldehydes
  • Alkynes
  • Organosilicon Compounds
  • Piperidines
  • spectaline
  • 3-hydroxybutanal
  • Oxygen