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Formal total synthesis of (-)-taxol through Pd-catalyzed eight-membered carbocyclic ring formation

Chemistry. 2015 Jan 2;21(1):355-9. doi: 10.1002/chem.201404295. Epub 2014 Oct 24.

Abstract

A formal total synthesis of (-)-taxol by a convergent approach utilizing Pd-catalyzed intramolecular alkenylation is described. Formation of the eight-membered carbocyclic ring has been a problem in the convergent total synthesis of taxol but it was solved by the Pd-catalyzed intramolecular alkenylation of a methyl ketone affording the cyclized product in excellent yield (97 %), indicating the high efficiency of the Pd-catalyzed intramolecular alkenylation. Rearrangement of the epoxy benzyl ether through a 1,5-hydride shift, generating the C3 stereogenic center and subsequently forming the C1-C2 benzylidene, was discovered and utilized in the preparation of a substrate for the Pd-catalyzed reaction.

Keywords: cyclization; enantioselectivity; natural products; palladium; total synthesis.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Catalysis
  • Crystallography, X-Ray
  • Cyclization
  • Molecular Conformation
  • Paclitaxel / chemical synthesis*
  • Paclitaxel / chemistry
  • Palladium / chemistry*
  • Stereoisomerism

Substances

  • Palladium
  • Paclitaxel