Copper-Catalyzed Double Additions and Radical Cyclization Cascades in the Re-Engineering of the Antibacterial Pleuromutilin

Chemistry. 2016 Jan 4;22(1):116-9. doi: 10.1002/chem.201504343. Epub 2015 Nov 26.

Abstract

A general synthetic sequence involving simply prepared starting materials provides rapid access to diverse, novel tricyclic architectures inspired by pleuromutilin. Sm(II) -mediated radical cyclization cascades of dialdehydes, prepared using a new, one-pot, copper-catalyzed double organomagnesium addition to β-chlorocyclohexenone, proceed with complete sequence selectivity and typically with high diastereocontrol to give analogues of the target core. Our expedient approach (ca. 7 steps) allows non-traditional, de novo synthetic access to analogues of the important antibacterial that can't be prepared from the natural product by semisynthesis.

Keywords: cyclization; domino reactions; electron-transfer; radical reactions; samarium.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-Bacterial Agents / chemical synthesis*
  • Anti-Bacterial Agents / chemistry*
  • Biological Products
  • Catalysis
  • Copper / chemistry*
  • Cyclization
  • Cyclohexanones / chemical synthesis*
  • Cyclohexanones / chemistry
  • Cyclohexenes / chemistry*
  • Diterpenes / chemistry
  • Lanthanoid Series Elements / chemistry*
  • Molecular Structure
  • Pleuromutilins
  • Polycyclic Compounds / chemical synthesis*
  • Polycyclic Compounds / chemistry*
  • Samarium / chemistry*
  • Stereoisomerism

Substances

  • Anti-Bacterial Agents
  • Biological Products
  • Cyclohexanones
  • Cyclohexenes
  • Diterpenes
  • Lanthanoid Series Elements
  • Polycyclic Compounds
  • beta-chlorocyclohexenone
  • Samarium
  • Copper