Synthesis, experimental evaluation and molecular modelling of hydroxamate derivatives as zinc metalloproteinase inhibitors

Eur J Med Chem. 2016 Jan 27:108:141-153. doi: 10.1016/j.ejmech.2015.11.019. Epub 2015 Nov 28.

Abstract

Enzymes of the M4 family of zinc-metalloproteinases are virulence factors secreted from gram-positive or gram-negative bacteria, and putative drug targets in the treatment of bacterial infections. In order to have a therapeutic value such inhibitors should not interfere with endogenous zinc-metalloproteinases. In the present study we have synthesised a series of hydroxamate derivatives and validated the compounds as inhibitors of the M4 enzymes thermolysin and pseudolysin, and the endogenous metalloproteinases ADAM-17, MMP-2 and MMP-9 using experimental binding studies and molecular modelling. In general, the compounds are stronger inhibitors of the MMPs than of the M4 enzymes, however, an interesting exception is LM2. The compounds bound stronger to pseudolysin than to thermolysin, and the molecular modelling studies showed that occupation of the S2(') subpocket by an aromatic group is favourable for strong interactions with pseudolysin.

Keywords: Adamalysins; Bacterial virulence factors; Docking and scoring; Enzyme selective inhibition; M4 family; Matrix metalloproteinases; Molecular dynamics simulations; Zinc-metalloproteinases.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • ADAM Proteins / antagonists & inhibitors
  • ADAM Proteins / metabolism
  • ADAM17 Protein
  • Humans
  • Hydroxamic Acids / chemical synthesis
  • Hydroxamic Acids / chemistry
  • Hydroxamic Acids / pharmacology*
  • Matrix Metalloproteinase 2 / metabolism*
  • Matrix Metalloproteinase 9 / metabolism*
  • Matrix Metalloproteinase Inhibitors / chemical synthesis
  • Matrix Metalloproteinase Inhibitors / chemistry
  • Matrix Metalloproteinase Inhibitors / pharmacology*
  • Models, Molecular
  • Molecular Structure
  • Thermolysin / antagonists & inhibitors
  • Thermolysin / metabolism

Substances

  • Hydroxamic Acids
  • Matrix Metalloproteinase Inhibitors
  • ADAM Proteins
  • Matrix Metalloproteinase 2
  • Thermolysin
  • Matrix Metalloproteinase 9
  • ADAM17 Protein
  • ADAM17 protein, human