Total synthesis and study of 6-deoxyerythronolide B by late-stage C-H oxidation

Nat Chem. 2009 Oct;1(7):547-51. doi: 10.1038/nchem.351. Epub 2009 Aug 30.

Abstract

Among the frontier challenges in chemistry in the twenty-first century are the interconnected goals of increasing synthetic efficiency and diversity in the construction of complex molecules. Oxidation reactions of C-H bonds, particularly when applied at late stages of complex molecule syntheses, hold special promise for achieving both these goals. Here we report a late-stage C-H oxidation strategy in the total synthesis of 6-deoxyerythronolide B (6-dEB), the aglycone precursor to the erythromycin antibiotics. An advanced intermediate is cyclized to give the 14-membered macrocyclic core of 6-dEB using a late-stage (step 19 of 22) C-H oxidative macrolactonization reaction that proceeds with high regio-, chemo- and diastereoselectivity (>40:1). A chelate-controlled model for macrolactonization predicted the stereochemical outcome of C-O bond formation and guided the discovery of conditions for synthesizing the first diastereomeric 13-epi-6-dEB precursor. Overall, this C-H oxidation strategy affords a highly efficient and stereochemically versatile synthesis of the erythromycin core.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Crystallography, X-Ray
  • Cyclization
  • Erythromycin / analogs & derivatives*
  • Erythromycin / chemical synthesis
  • Erythromycin / chemistry
  • Models, Molecular
  • Molecular Structure
  • Oxidation-Reduction
  • Stereoisomerism

Substances

  • 6-deoxyerythronolide B
  • Erythromycin

Associated data

  • PubChem-Substance/85098522
  • PubChem-Substance/85098523
  • PubChem-Substance/85098524
  • PubChem-Substance/85098525
  • PubChem-Substance/85098526
  • PubChem-Substance/85098527
  • PubChem-Substance/85098528
  • PubChem-Substance/85098529
  • PubChem-Substance/85098530
  • PubChem-Substance/85098531
  • PubChem-Substance/85098532
  • PubChem-Substance/85098533
  • PubChem-Substance/85098534
  • PubChem-Substance/85098535
  • PubChem-Substance/85098536