Remarkable reactivity difference in oxygen-substituted versus non-oxygen-substituted bromoalkynes in Cu(I)-catalyzed cross-coupling reactions: total synthesis of (-)-S-18-hydroxyminquartynoic acid

J Org Chem. 2003 Jul 25;68(15):5956-60. doi: 10.1021/jo0344900.

Abstract

The conjugated tetraacetylenic natural product (S)-18-hydroxyminquartynoic acid (2) is synthesized in five linear steps and 17.7% overall yield from commercially available 1,2,5,6-O-diisopropylidene mannitol. The key step is a one-pot three-component Cadiot-Chodkiewicz reaction affording the tetrayne unit. The oxygen-substituted bromoalkyne 10 was found to react at a much faster rate than the non-oxygen-substituted bromoalkyne 6 in the key step. The undesired symmetric cross-coupling by 10 generates a symmetric tetrayne intermediate, which undergoes a nucleophilic addition by 1 equiv of ethylamine. This side reaction is suppressed by controlling the order and rate of addition of each component and by reducing the amount of ethylamine.

Publication types

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

MeSH terms

  • Alkynes / chemical synthesis*
  • Alkynes / chemistry
  • Bromine*
  • Catalysis
  • Copper*
  • Fatty Acids, Unsaturated / chemical synthesis*
  • Fatty Acids, Unsaturated / chemistry
  • Magnetic Resonance Spectroscopy
  • Molecular Conformation
  • Oxygen

Substances

  • (S)-18-hydroxyminquartynoic acid
  • Alkynes
  • Fatty Acids, Unsaturated
  • Copper
  • Oxygen
  • Bromine