Discovery of a Potent Adenine-Benzyltriazolo-Pleuromutilin Conjugate with Pronounced Antibacterial Activity against MRSA

J Med Chem. 2020 Dec 24;63(24):15693-15708. doi: 10.1021/acs.jmedchem.0c01328. Epub 2020 Dec 16.

Abstract

Conjugation of pleuromutilin is an attractive strategy for the development of novel antibiotics and the fight against multiresistant bacteria as the class is associated with low rates of resistance and cross-resistance development. Herein, the preparation of 35 novel (+)-pleuromutilin conjugates is reported. Their design was based on a synthetically more efficient benzyl adaption of a potent lead but still relied on the Cu(I)-catalyzed alkyne-azide [3 + 2] cycloaddition for conjugation onto pleuromutilin. Their antibacterial activity was evaluated against the multiresistant Staphylococcus aureus strain USA300 for which they displayed moderate to excellent activity. Compound 35, bearing a para-benzyladenine substituent, proved particularly potent against USA300 and additional strains of MRSA and displayed as importantly no cytotoxicity in four mammalian cell lines. Structure-activity relationship analysis revealed that the purine 6-amino is essential for high potency, likely because of strong hydrogen bonding with the RNA backbone of C2469, as suggested by a molecular model based on the MM-GBSA approach.

MeSH terms

  • Adenine / chemistry*
  • Animals
  • Anti-Bacterial Agents / chemistry
  • Anti-Bacterial Agents / pharmacology*
  • Binding Sites
  • Catalysis
  • Cell Line
  • Cell Survival / drug effects
  • Copper / chemistry
  • Cycloaddition Reaction
  • Diterpenes / chemistry*
  • Dogs
  • Humans
  • Methicillin-Resistant Staphylococcus aureus / drug effects*
  • Microbial Sensitivity Tests
  • Molecular Dynamics Simulation
  • Pleuromutilins
  • Polycyclic Compounds / chemistry*
  • Structure-Activity Relationship
  • Triazoles / chemistry*

Substances

  • Anti-Bacterial Agents
  • Diterpenes
  • Polycyclic Compounds
  • Triazoles
  • Copper
  • Adenine