Direct oxa-Pictet-Spengler cyclization to the natural (3a,5)-trans-stereochemistry in the syntheses of (+)-7-deoxyfrenolicin B and (+)-7-deoxykalafungin

J Org Chem. 2009 Jan 2;74(1):423-6. doi: 10.1021/jo801945n.

Abstract

The pyranonaphthoquinones (+)-7-deoxyfrenolicin B and (+)-7-deoxykalafungin were synthesized in four steps using an oxa-Pictet-Spengler cyclization that directly provided the natural (3a,5)-trans-substituted dihydronaphthopyrans with high diastereoselectivity. This outcome is in contrast to the unnatural (3a,5)-cis-substituted dihydronaphthopyrans reported under similar conditions for the syntheses of (+)-frenolicin B and (+)-kalafungin. Computational modeling is presented that provides insight into this unusual stereoselectivity.

MeSH terms

  • Cyclization
  • Molecular Conformation
  • Naphthoquinones / chemical synthesis*
  • Naphthoquinones / chemistry
  • Stereoisomerism

Substances

  • 7-deoxyfrenolicin B
  • 7-deoxykalafungin
  • Naphthoquinones