Discovery of novel PI3-kinase δ specific inhibitors for the treatment of rheumatoid arthritis: taming CYP3A4 time-dependent inhibition

J Med Chem. 2012 Jun 28;55(12):5887-900. doi: 10.1021/jm3003747. Epub 2012 Jun 11.

Abstract

PI3Kδ is a lipid kinase and a member of a larger family of enzymes, PI3K class IA(α, β, δ) and IB (γ), which catalyze the phosphorylation of PIP2 to PIP3. PI3Kδ is mainly expressed in leukocytes, where it plays a critical, nonredundant role in B cell receptor mediated signaling and provides an attractive opportunity to treat diseases where B cell activity is essential, e.g., rheumatoid arthritis. We report the discovery of novel, potent, and selective PI3Kδ inhibitors and describe a structural hypothesis for isoform (α, β, γ) selectivity gained from interactions in the affinity pocket. The critical component of our initial pharmacophore for isoform selectivity was strongly associated with CYP3A4 time-dependent inhibition (TDI). We describe a variety of strategies and methods for monitoring and attenuating TDI. Ultimately, a structure-based design approach was employed to identify a suitable structural replacement for further optimization.

MeSH terms

  • Arthritis, Rheumatoid / drug therapy*
  • Arthritis, Rheumatoid / enzymology
  • Benzimidazoles / chemistry
  • Benzimidazoles / pharmacology
  • Benzimidazoles / therapeutic use
  • Cell Line
  • Cytochrome P-450 CYP3A
  • Cytochrome P-450 CYP3A Inhibitors*
  • Drug Discovery*
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / pharmacology*
  • Enzyme Inhibitors / therapeutic use
  • Humans
  • Inhibitory Concentration 50
  • Models, Molecular
  • Phosphatidylinositol 3-Kinases / chemistry
  • Phosphoinositide-3 Kinase Inhibitors*
  • Protein Conformation
  • Substrate Specificity
  • Time Factors

Substances

  • Benzimidazoles
  • Cytochrome P-450 CYP3A Inhibitors
  • Enzyme Inhibitors
  • Phosphoinositide-3 Kinase Inhibitors
  • benzimidazole
  • Cytochrome P-450 CYP3A
  • CYP3A4 protein, human