Mtb-Selective 5-Aminomethyl Oxazolidinone Prodrugs: Robust Potency and Potential Liabilities

ACS Infect Dis. 2024 May 10;10(5):1679-1695. doi: 10.1021/acsinfecdis.4c00025. Epub 2024 Apr 6.

Abstract

Linezolid is a drug with proven human antitubercular activity whose use is limited to highly drug-resistant patients because of its toxicity. This toxicity is related to its mechanism of action─linezolid inhibits protein synthesis in both bacteria and eukaryotic mitochondria. A highly selective and potent series of oxazolidinones, bearing a 5-aminomethyl moiety (in place of the typical 5-acetamidomethyl moiety of linezolid), was identified. Linezolid-resistant mutants were cross-resistant to these molecules but not vice versa. Resistance to the 5-aminomethyl molecules mapped to an N-acetyl transferase (Rv0133) and these mutants remained fully linezolid susceptible. Purified Rv0133 was shown to catalyze the transformation of the 5-aminomethyl oxazolidinones to their corresponding N-acetylated metabolites, and this transformation was also observed in live cells of Mycobacterium tuberculosis. Mammalian mitochondria, which lack an appropriate N-acetyltransferase to activate these prodrugs, were not susceptible to inhibition with the 5-aminomethyl analogues. Several compounds that were more potent than linezolid were taken into C3HeB/FeJ mice and were shown to be highly efficacious, and one of these (9) was additionally taken into marmosets and found to be highly active. Penetration of these 5-aminomethyl oxazolidinone prodrugs into caseum was excellent. Unfortunately, these compounds were rapidly converted into the corresponding 5-alcohols by mammalian metabolism which retained antimycobacterial activity but resulted in substantial mitotoxicity.

Keywords: antibacterial; nonhuman primate; oxazolidinone; pro-drug; tuberculosis.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Antitubercular Agents* / chemistry
  • Antitubercular Agents* / pharmacology
  • Drug Resistance, Bacterial
  • Humans
  • Linezolid / chemistry
  • Linezolid / pharmacology
  • Mice
  • Microbial Sensitivity Tests
  • Mitochondria / drug effects
  • Mitochondria / metabolism
  • Mycobacterium tuberculosis* / drug effects
  • Oxazolidinones* / chemistry
  • Oxazolidinones* / pharmacology
  • Prodrugs* / chemistry
  • Prodrugs* / pharmacology

Substances

  • Prodrugs
  • Antitubercular Agents
  • Oxazolidinones
  • Linezolid