Optimization of peptidomimetic boronates bearing a P3 bicyclic scaffold as proteasome inhibitors

Eur J Med Chem. 2014 Aug 18:83:1-14. doi: 10.1016/j.ejmech.2014.06.017. Epub 2014 Jun 10.

Abstract

A new series of pseudopeptide boronate proteasome inhibitors (2-3) was developed, through optimization of our previously described analogs of bortezomib, bearing a bicyclic 1,6-naphthyridin-5(6H)-one scaffold as P3 fragment (1). The biological evaluation on human 20S proteasome displayed a promising inhibition profile, especially for compounds bearing a P2 ethylene fragment, which exhibited Ki values in the nanomolar range for the ChT-L activity (e.g. 2a, Ki = 0.057 μM) and considerable selectivity for proteasome over bovine pancreatic α-chymotrypsin. Docking experiments into the yeast 20S proteasome revealed that the ligands are accommodated predominantly into the ChT-L site and that they covalently bind to the active site threonine residue via boron atom. Within the cellular assays performed against a 60 cancer cell line panel, compounds 3e and 3f demonstrated also good antiproliferative activity and compound 3f emerged as promising lead compound for the development of anticancer agents targeting melanoma and non-small cell lung cancer.

Keywords: Docking studies; Peptidomimetic boronates; Proteasome inhibitors.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / metabolism
  • Antineoplastic Agents / pharmacology
  • Boronic Acids / chemistry*
  • Bortezomib
  • Caspases / metabolism
  • Cattle
  • Cell Line, Tumor
  • Cell Proliferation / drug effects
  • Drug Design*
  • Endopeptidases / metabolism
  • Humans
  • Hydrolysis / drug effects
  • Molecular Docking Simulation
  • Peptidomimetics / chemistry*
  • Peptidomimetics / metabolism
  • Peptidomimetics / pharmacology*
  • Proteasome Endopeptidase Complex / chemistry
  • Proteasome Endopeptidase Complex / metabolism*
  • Proteasome Inhibitors / chemistry*
  • Proteasome Inhibitors / metabolism
  • Proteasome Inhibitors / pharmacology*
  • Protein Conformation
  • Proteolysis / drug effects
  • Pyrazines / chemistry*
  • Trypsin / metabolism

Substances

  • Antineoplastic Agents
  • Boronic Acids
  • Peptidomimetics
  • Proteasome Inhibitors
  • Pyrazines
  • Bortezomib
  • Endopeptidases
  • Trypsin
  • Caspases
  • Proteasome Endopeptidase Complex
  • peptidylglutamylpeptide hydrolase