Discovery and Optimization of DNA Gyrase and Topoisomerase IV Inhibitors with Potent Activity against Fluoroquinolone-Resistant Gram-Positive Bacteria

J Med Chem. 2021 May 13;64(9):6329-6357. doi: 10.1021/acs.jmedchem.1c00375. Epub 2021 Apr 30.

Abstract

Herein, we describe the discovery and optimization of a novel series that inhibits bacterial DNA gyrase and topoisomerase IV via binding to, and stabilization of, DNA cleavage complexes. Optimization of this series led to the identification of compound 25, which has potent activity against Gram-positive bacteria, a favorable in vitro safety profile, and excellent in vivo pharmacokinetic properties. Compound 25 was found to be efficacious against fluoroquinolone-sensitive Staphylococcus aureus infection in a mouse thigh model at lower doses than moxifloxacin. An X-ray crystal structure of the ternary complex formed by topoisomerase IV from Klebsiella pneumoniae, compound 25, and cleaved DNA indicates that this compound does not engage in a water-metal ion bridge interaction and forms no direct contacts with residues in the quinolone resistance determining region (QRDR). This suggests a structural basis for the reduced impact of QRDR mutations on antibacterial activity of 25 compared to fluoroquinolones.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Anti-Bacterial Agents / chemistry
  • Anti-Bacterial Agents / pharmacology*
  • DNA Gyrase / metabolism*
  • DNA Topoisomerase IV / antagonists & inhibitors*
  • Drug Design*
  • Drug Resistance, Bacterial / drug effects
  • Fluoroquinolones / pharmacology*
  • Mice
  • Staphylococcus aureus / drug effects*
  • Topoisomerase II Inhibitors / chemistry
  • Topoisomerase II Inhibitors / pharmacology*

Substances

  • Anti-Bacterial Agents
  • Fluoroquinolones
  • Topoisomerase II Inhibitors
  • DNA Topoisomerase IV
  • DNA Gyrase