Structure-activity relationships for inhibitors of Pseudomonas aeruginosa exoenzyme S ADP-ribosyltransferase activity

Eur J Med Chem. 2018 Jan 1:143:568-576. doi: 10.1016/j.ejmech.2017.11.036. Epub 2017 Nov 21.

Abstract

During infection, the Gram-negative opportunistic pathogen Pseudomonas aeruginosa employs its type III secretion system to translocate the toxin exoenzyme S (ExoS) into the eukaryotic host cell cytoplasm. ExoS is an essential in vivo virulence factor that enables P. aeruginosa to avoid phagocytosis and eventually kill the host cell. ExoS elicits its pathogenicity mainly via ADP-ribosyltransferase (ADPRT) activity. We recently identified a new class of ExoS ADPRT inhibitors with in vitro IC50 of around 20 μM in an enzymatic assay using a recombinant ExoS ADPRT domain. Herein, we report structure-activity relationships of this compound class by comparing a total of 51 compounds based on a thieno [2,3-d]pyrimidin-4(3H)-one and 4-oxo-3,4-dihydroquinazoline scaffolds. Improved inhibitors with in vitro IC50 values of 6 μM were identified. Importantly, we demonstrated that the most potent inhibitors block ADPRT activity of native full-length ExoS secreted by viable P. aeruginosa with an IC50 value of 1.3 μM in an enzymatic assay. This compound class holds promise as starting point for development of novel antibacterial agents.

Keywords: 2-Aminobenzamide; ADP-Ribosyltransferase; Bacterial exotoxins; ExoS; Pseudomonas aeruginosa; Quinazolines; Type III secretion.

MeSH terms

  • ADP Ribose Transferases / antagonists & inhibitors*
  • ADP Ribose Transferases / metabolism
  • Bacterial Toxins / antagonists & inhibitors*
  • Bacterial Toxins / metabolism
  • Dose-Response Relationship, Drug
  • Molecular Structure
  • Poly(ADP-ribose) Polymerase Inhibitors / chemical synthesis
  • Poly(ADP-ribose) Polymerase Inhibitors / chemistry
  • Poly(ADP-ribose) Polymerase Inhibitors / pharmacology*
  • Pseudomonas aeruginosa / enzymology*
  • Pyrimidinones / chemical synthesis
  • Pyrimidinones / chemistry
  • Pyrimidinones / pharmacology*
  • Quinazolines / chemical synthesis
  • Quinazolines / chemistry
  • Quinazolines / pharmacology*
  • Structure-Activity Relationship

Substances

  • 4-oxo-3,4-dihydroquinazoline
  • Bacterial Toxins
  • Poly(ADP-ribose) Polymerase Inhibitors
  • Pyrimidinones
  • Quinazolines
  • thieno(2,3-d)pyrimidin-4(3H)-one
  • ADP Ribose Transferases
  • exoenzyme S