Pyridinylimidazoles as dual glycogen synthase kinase 3β/p38α mitogen-activated protein kinase inhibitors

Eur J Med Chem. 2019 Aug 1:175:309-329. doi: 10.1016/j.ejmech.2019.04.035. Epub 2019 Apr 24.

Abstract

Compounds simultaneously inhibiting two targets that are involved in the progression of the same complex disease may exhibit additive or even synergistic therapeutic effects. Here we unveil 2,4,5-trisubstituted imidazoles as dual inhibitors of p38α mitogen-activated protein kinase and glycogen synthase kinase 3β (GSK3β). Both enzymes are potential therapeutic targets for neurodegenerative disorders, like Alzheimer's disease. A set of 39 compounds was synthesized and evaluated in kinase activity assays for their ability to inhibit both target kinases. Among the synthesized compounds, potent dual-target-directed inhibitors showing IC50 values down to the low double-digit nanomolar range, were identified. One of the best balanced dual inhibitors presented in here is N-(4-(2-ethyl-4-(4-fluorophenyl)-1H-imidazol-5-yl)pyridin-2-yl)cyclopropanecarboxamide (20c) (p38α, IC50 = 16 nM; GSK3β, IC50 = 35 nM) featuring an excellent metabolic stability and an appreciable isoform selectivity over the closely related GSK3α. Our findings were rationalized by computational docking studies based on previously published X-ray structures.

Keywords: Alzheimer's disease; Dual inhibitors; Glycogen synthase kinase 3β; Kinase inhibitors; Pyridinylimidazoles; p38α MAP kinase.

MeSH terms

  • Amino Acid Sequence
  • Carbon-13 Magnetic Resonance Spectroscopy
  • Glycogen Synthase Kinase 3 beta / antagonists & inhibitors*
  • Humans
  • Imidazoles / chemistry
  • Imidazoles / pharmacology*
  • Inhibitory Concentration 50
  • Molecular Docking Simulation
  • Protein Kinase Inhibitors / pharmacology*
  • Proton Magnetic Resonance Spectroscopy
  • Pyridines / chemistry
  • Pyridines / pharmacology*
  • Sequence Homology, Amino Acid
  • Spectrometry, Mass, Electrospray Ionization
  • Structure-Activity Relationship
  • p38 Mitogen-Activated Protein Kinases / antagonists & inhibitors*

Substances

  • Imidazoles
  • Protein Kinase Inhibitors
  • Pyridines
  • GSK3B protein, human
  • Glycogen Synthase Kinase 3 beta
  • p38 Mitogen-Activated Protein Kinases
  • pyridine