Lyngbyastatin 1 and Ibu-epilyngbyastatin 1: synthesis, stereochemistry, and NMR line broadening

J Nat Prod. 2002 Dec;65(12):1824-9. doi: 10.1021/np020117w.

Abstract

The synthesis of a lyngbyastatin 1-Ibu-epilyngbyastatin 1 mixture combined with NMR and molecular modeling studies proved that natural lyngbyastatin 1 was only one Ibu epimer rather than a mixture of both and that the configuration of this epimer in the Ibu unit was R. The substance isolated with lyngbyastatin 1 was Ibu-epidolastatin 12. The extreme broadness in the proton NMR spectra of lyngbyastatin 1 and Ibu-epidolastatin 12 was exchange broadening due to rotation about the Ibu-Ala amide bond. It was a consequence of (1) a small energy difference between the cis and trans forms of this bond, (2) a substantial difference in conformation between these forms, and (3) a lowered barrier between them compared to most amide bonds (due to steric hindrance). The synthetic lyngbyastatin 1-Ibu-epilyngbyastatin 1 mixture had significant activities against cancer cells and in stimulating actin polymerization, but was less active than dolastatin 11 in all assays.

Publication types

  • Comparative Study
  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Actins / antagonists & inhibitors
  • Actins / drug effects
  • Antineoplastic Agents / chemical synthesis*
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology
  • Depsipeptides*
  • Drug Screening Assays, Antitumor
  • Humans
  • Lung Neoplasms
  • Male
  • Molecular Structure
  • Nuclear Magnetic Resonance, Biomolecular
  • Oligopeptides / chemical synthesis*
  • Oligopeptides / chemistry
  • Oligopeptides / pharmacology
  • Peptides, Cyclic / chemical synthesis*
  • Peptides, Cyclic / chemistry
  • Peptides, Cyclic / pharmacology
  • Prostatic Neoplasms
  • Seaweed / chemistry*
  • Stereoisomerism
  • Structure-Activity Relationship
  • Tumor Cells, Cultured / drug effects

Substances

  • Actins
  • Antineoplastic Agents
  • Depsipeptides
  • Ibu-epilyngbyastatin 1
  • Oligopeptides
  • Peptides, Cyclic
  • dolastatin 11
  • lyngbyastatin 1