Toxicity modulation, resistance enzyme evasion, and A-site X-ray structure of broad-spectrum antibacterial neomycin analogs

ACS Chem Biol. 2014 Sep 19;9(9):2067-73. doi: 10.1021/cb5003416. Epub 2014 Jul 14.

Abstract

Aminoglycoside antibiotics are pseudosaccharides decorated with ammonium groups that are critical for their potent broad-spectrum antibacterial activity. Despite over three decades of speculation whether or not modulation of pKa is a viable strategy to curtail aminoglycoside kidney toxicity, there is a lack of methods to systematically probe amine-RNA interactions and resultant cytotoxicity trends. This study reports the first series of potent aminoglycoside antibiotics harboring fluorinated N1-hydroxyaminobutyryl acyl (HABA) appendages for which fluorine-RNA contacts are revealed through an X-ray cocrystal structure within the RNA A-site. Cytotoxicity in kidney-derived cells was significantly reduced for the derivative featuring our novel β,β-difluoro-HABA group, which masks one net charge by lowering the pKa without compromising antibacterial potency. This novel side-chain assists in evasion of aminoglycoside-modifying enzymes, and it can be easily transferred to impart these properties onto any number of novel analogs.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Aminoglycosides / chemistry*
  • Aminoglycosides / pharmacology*
  • Aminoglycosides / toxicity
  • Anti-Bacterial Agents / chemical synthesis
  • Anti-Bacterial Agents / chemistry*
  • Anti-Bacterial Agents / pharmacology*
  • Anti-Bacterial Agents / toxicity
  • Cell Line / drug effects
  • Chemistry Techniques, Synthetic
  • Crystallography, X-Ray
  • Drug Evaluation, Preclinical / methods
  • Drug Resistance, Bacterial / drug effects
  • Humans
  • Kidney / cytology
  • Kidney / drug effects
  • Microbial Sensitivity Tests
  • Molecular Structure
  • Neomycin / analogs & derivatives*
  • RNA / chemistry
  • RNA / metabolism
  • Structure-Activity Relationship

Substances

  • Aminoglycosides
  • Anti-Bacterial Agents
  • RNA
  • Neomycin

Associated data

  • PDB/3WRU