General Methodologies Toward cis-Fused Quinone Sesquiterpenoids. Enantiospecific Synthesis of the epi-Ilimaquinone Core Featuring Sc-Catalyzed Ring Expansion

Molecules. 2017 Jun 24;22(7):1041. doi: 10.3390/molecules22071041.

Abstract

A stereocontrolled approach to the cis-decalin framework of clerodane diterpenes and biologically active quinone sesquiterpenes is reported. Starting from an inexpensive optically pure tetrahydroindanone, Birch reductive alkylation builds two new contiguous chiral centers-one of which is quaternary and all-carbon-substituted. Also featured is a highly regioselective diazoalkane-carbonyl homologation reaction to prepare the 6,6-bicyclic skeleton. Therein, the utility of Sc(OTf)₃ as a mild catalyst for formal 1C insertion in complex settings is demonstrated.

Keywords: (trimethylsilyl)diazomethane; 5-epi-ilimaquinone; 5-epi-isospongiaquinone; catalytic ring expansion; cis-decalin; hexahydroindanones; homologation; quaternary carbon synthesis; quinone natural products; scandium triflate.

MeSH terms

  • Catalysis
  • Diterpenes, Clerodane / chemistry*
  • Models, Chemical
  • Molecular Structure
  • Quinones / chemical synthesis*
  • Quinones / chemistry
  • Sesquiterpenes / chemical synthesis*
  • Sesquiterpenes / chemistry
  • Stereoisomerism

Substances

  • Diterpenes, Clerodane
  • Quinones
  • Sesquiterpenes
  • ilimaquinone