Substrate-Inspired Fragment Merging and Growing Affords Efficacious LasB Inhibitors

Angew Chem Int Ed Engl. 2022 Jan 26;61(5):e202112295. doi: 10.1002/anie.202112295. Epub 2021 Dec 13.

Abstract

Extracellular virulence factors have emerged as attractive targets in the current antimicrobial resistance crisis. The Gram-negative pathogen Pseudomonas aeruginosa secretes the virulence factor elastase B (LasB), which plays an important role in the infection process. Here, we report a sub-micromolar, non-peptidic, fragment-like inhibitor of LasB discovered by careful visual inspection of structural data. Inspired by the natural LasB substrate, the original fragment was successfully merged and grown. The optimized inhibitor is accessible via simple chemistry and retained selectivity with a substantial improvement in activity, which can be rationalized by the crystal structure of LasB in complex with the inhibitor. We also demonstrate an improved in vivo efficacy of the optimized hit in Galleria mellonella larvae, highlighting the significance of this class of compounds as promising drug candidates.

Keywords: Antibiotic resistance; Antivirulence; Fragment merging; Mercaptoacetamides; Pseudomonas aeruginosa.

MeSH terms

  • Animals
  • Anti-Bacterial Agents / chemical synthesis
  • Anti-Bacterial Agents / chemistry
  • Anti-Bacterial Agents / pharmacology
  • Bacterial Proteins* / antagonists & inhibitors
  • Bacterial Proteins* / chemistry
  • Bacterial Proteins* / metabolism
  • Larva / drug effects
  • Microbial Sensitivity Tests
  • Models, Molecular
  • Molecular Structure
  • Moths
  • Pancreatic Elastase / antagonists & inhibitors
  • Pancreatic Elastase / metabolism
  • Pseudomonas aeruginosa* / drug effects
  • Structure-Activity Relationship

Substances

  • Bacterial Proteins
  • Anti-Bacterial Agents
  • Pancreatic Elastase