Preparation of macrocyclic Z-enoates and (E,Z)- or (Z,E)-dienoates through catalytic stereoselective ring-closing metathesis

J Am Chem Soc. 2014 Nov 26;136(47):16493-6. doi: 10.1021/ja510768c. Epub 2014 Nov 17.

Abstract

The first examples of catalyst-controlled stereoselective macrocyclic ring-closing metathesis reactions that generate Z-enoates as well as (E,Z)- or (Z,E)-dienoates are disclosed. Reactions promoted by 3.0-10 mol % of a Mo-based monoaryloxide pyrrolide complex proceed to completion within 2-6 h at room temperature. The desired macrocycles are formed in 79:21 to >98:2 Z/E selectivity; stereoisomerically pure products can be obtained in 43-75% yield after chromatography. Utility is demonstrated by application to a concise formal synthesis of the natural product (+)-aspicilin.

Publication types

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

MeSH terms

  • Catalysis
  • Cyclization
  • Ketones / chemical synthesis*
  • Ketones / chemistry
  • Macrocyclic Compounds / chemical synthesis*
  • Macrocyclic Compounds / chemistry
  • Molecular Structure
  • Stereoisomerism

Substances

  • Ketones
  • Macrocyclic Compounds