Lead optimization studies on FimH antagonists: discovery of potent and orally bioavailable ortho-substituted biphenyl mannosides

J Med Chem. 2012 Apr 26;55(8):3945-59. doi: 10.1021/jm300165m. Epub 2012 Apr 13.

Abstract

Herein, we describe the X-ray structure-based design and optimization of biaryl mannoside FimH inhibitors. Diverse modifications to the biaryl ring to improve druglike physical and pharmacokinetic properties of mannosides were assessed for FimH binding affinity based on their effects on hemagglutination and biofilm formation along with direct FimH binding assays. Substitution on the mannoside phenyl ring ortho to the glycosidic bond results in large potency enhancements several-fold higher than those of corresponding unsubstituted matched pairs and can be rationalized from increased hydrophobic interactions with the FimH hydrophobic ridge (Ile13) or "tyrosine gate" (Tyr137 and Tyr48) also lined by Ile52. The lead mannosides have increased metabolic stability and oral bioavailability as determined from in vitro PAMPA predictive model of cellular permeability and in vivo pharmacokinetic studies in mice, thereby representing advanced preclinical candidates with promising potential as novel therapeutics for the clinical treatment and prevention of recurring urinary tract infections.

Publication types

  • Research Support, American Recovery and Reinvestment Act
  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Adhesins, Escherichia coli
  • Animals
  • Bacterial Adhesion / drug effects
  • Biofilms / drug effects
  • Biphenyl Compounds / chemical synthesis
  • Biphenyl Compounds / pharmacokinetics
  • Biphenyl Compounds / pharmacology*
  • Fimbriae Proteins / antagonists & inhibitors*
  • Hemagglutination Inhibition Tests
  • Mannosides / chemical synthesis
  • Mannosides / chemistry
  • Mannosides / pharmacokinetics
  • Mannosides / pharmacology*
  • Mice
  • Structure-Activity Relationship
  • Urinary Tract Infections

Substances

  • Adhesins, Escherichia coli
  • Biphenyl Compounds
  • Mannosides
  • fimH protein, E coli
  • Fimbriae Proteins