Characterization of selective exosite-binding inhibitors of matrix metalloproteinase 13 that prevent articular cartilage degradation in vitro

J Med Chem. 2014 Nov 26;57(22):9598-611. doi: 10.1021/jm501284e. Epub 2014 Nov 11.

Abstract

Matrix metalloproteinase 13 (MMP-13) has been shown to be the main collagenase responsible for degradation of articular cartilage during osteoarthritis and therefore represents a target for drug development. As a result of high-throughput screening and structure-activity relationship studies, we identified a novel, highly selective class of MMP-13 inhibitors (compounds 1 (Q), 2 (Q1), and 3 (Q2)). Mechanistic characterization revealed a noncompetitive nature of these inhibitors with binding constants in the low micromolar range. Crystallographic analyses revealed two binding modes for compound 2 in the MMP-13 S1' subsite and in an S1/S2* subsite. Type II collagen- and cartilage-protective effects exhibited by compounds 1, 2, and 3 suggested that these compounds might be efficacious in future in vivo studies. Finally, these compounds were also highly selective when tested against a panel of 30 proteases, which, in combination with a good CYP inhibition profile, suggested low off-target toxicity and drug-drug interactions in humans.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Binding Sites
  • Cartilage / metabolism
  • Cartilage, Articular / drug effects*
  • Cartilage, Articular / metabolism
  • Cattle
  • Chemistry, Pharmaceutical / methods
  • Collagen / chemistry
  • Collagenases / chemistry
  • Crystallography, X-Ray / methods
  • Cytochrome P-450 Enzyme System / chemistry
  • Drug Design
  • Humans
  • Hydrolysis
  • Inhibitory Concentration 50
  • Kinetics
  • Matrix Metalloproteinase 13 / chemistry*
  • Matrix Metalloproteinase Inhibitors / chemistry*
  • Mice
  • Microsomes / drug effects
  • Molecular Conformation
  • Osteoarthritis / physiopathology
  • Protein Binding
  • Protein Conformation
  • Rats
  • Structure-Activity Relationship

Substances

  • Matrix Metalloproteinase Inhibitors
  • Collagen
  • Cytochrome P-450 Enzyme System
  • Collagenases
  • MMP13 protein, human
  • Matrix Metalloproteinase 13