Synthesis of novel nocathiacin-class antibiotics. Condensation of glycolaldehyde with primary amides and tandem reductive amination of amadori-rearranged 2-oxoethyl intermediates

J Org Chem. 2002 Dec 13;67(25):8789-93. doi: 10.1021/jo020385z.

Abstract

Nocathiacin I (1) and nocathiacin IV (2) are novel indole-containing thiazolyl peptide antibiotics, which exhibit potent activity against key Gram-positive bacterial pathogens, including multi drug-resistant Staphylococcus aureus, Streptococcus pneumoniae, and Enterococcus faecium. New nocathiacins 7-12 were prepared from 2 by a condensation with glycolaldehyde followed by tandem reductive amination of the 2-oxoethyl intermediate 4. The latter was formed via Amadori rearrangement from initial 2-hydroxyethylideneamide 3. This transformation readily tolerates the complex architecture of nocathiacins and allows selective incorporation of water solubilizing groups to the primary amide in 2 without protecting group manipulation.

MeSH terms

  • Acetaldehyde / analogs & derivatives*
  • Acetaldehyde / chemistry*
  • Amides / chemistry
  • Anti-Bacterial Agents / chemical synthesis*
  • Anti-Bacterial Agents / pharmacology
  • Catalysis
  • Combinatorial Chemistry Techniques*
  • Drug Resistance, Multiple, Bacterial
  • Enterococcus faecium / drug effects
  • Intercellular Signaling Peptides and Proteins
  • Microbial Sensitivity Tests
  • Molecular Structure
  • Peptides*
  • Peptides, Cyclic / chemical synthesis*
  • Peptides, Cyclic / pharmacology
  • Staphylococcus aureus / drug effects
  • Streptococcus pneumoniae / drug effects
  • Structure-Activity Relationship
  • Thiazoles / chemical synthesis*
  • Thiazoles / pharmacology
  • Water / chemistry

Substances

  • Amides
  • Anti-Bacterial Agents
  • Intercellular Signaling Peptides and Proteins
  • Peptides
  • Peptides, Cyclic
  • Thiazoles
  • nocathiacin I
  • nocathiacin IV
  • Water
  • Acetaldehyde
  • glycolaldehyde