Total Synthesis and Structural Reassignment of the Antitubercular Natural Product Evybactin

Chemistry. 2025 Jan 2;31(1):e202403767. doi: 10.1002/chem.202403767. Epub 2024 Nov 14.

Abstract

The escalating threat posed by antibiotic resistance is a global concern and underscores the need for new antibiotics. In this context, the recent discovery of evybactin, a nonribosomal depsipeptide antibiotic that selectively and potently inhibits the growth of M. tuberculosis, is particularly noteworthy. Here, we present the first total synthesis of this natural product, along with a revision of its assigned structure. Our studies revealed a disparity between the structure originally proposed for evybactin and its actual configuration. Specifically, the 3-methylhistidine residue present in the evybactin core macrocycle was found to be of the d-configuration rather than the previously assigned l-His(Me). Having addressed this, we further optimized our solid-phase synthetic route to provide access to evybactin on a multi-hundred-milligram scale. Access to such quantities will allow for more comprehensive studies with this promising antibiotic.

Keywords: Antibiotic; Evybactin; Structural assignment; Total synthesis; Tuberculosis.

MeSH terms

  • Antitubercular Agents* / chemical synthesis
  • Antitubercular Agents* / chemistry
  • Antitubercular Agents* / pharmacology
  • Biological Products* / chemical synthesis
  • Biological Products* / chemistry
  • Biological Products* / pharmacology
  • Depsipeptides* / chemical synthesis
  • Depsipeptides* / chemistry
  • Depsipeptides* / pharmacology
  • Mycobacterium tuberculosis* / drug effects
  • Solid-Phase Synthesis Techniques
  • Stereoisomerism

Substances

  • Antitubercular Agents
  • Biological Products
  • Depsipeptides