Structural optimization of pyrazolo[1,5-a]pyrimidine derivatives as potent and highly selective DPP-4 inhibitors

Eur J Med Chem. 2020 Dec 15:208:112850. doi: 10.1016/j.ejmech.2020.112850. Epub 2020 Sep 19.

Abstract

Our previous discovery of pyrazolo [1,5-a]pyrimidin-7(4H)-one scaffold-based DPP-4 inhibitors yielded two potent compounds b2 (IC50 = 79 nM) and d1 (IC50 = 49 nM) but characterized by cytotoxicity. Herein, with scaffold hopping and fragment-based drug design strategies, highly potent and selective pyrazolo [1,5-a]pyrimidine DPP-4 inhibitors were found featured by reduced or diminished cytotoxicity. Specifically, c24 (IC50 = 2 nM) exhibits a 25 to 40-fold increase of inhibitory activity respect to those of b2 and d1, respectively, 2-fold from Alogliptin (IC50 = 4 nM), and remarkable selectivity over DPP-8 and DPP-9 (>2000 fold). Further docking studies confirmed that the pyrazolo [1,5-a]pyrimidine core interacts with the S1 pocket whereas its substituted aromatic ring interacts with the sub-S1 pocket. The interactive mode in this case resembles that of Alogliptin and Trelagliptin. Further in vivo IPGTT assays in diabetic mice demonstrated that c24 effectively reduces glucose excursion by 48% at the dose of 10 mg/kg, suggesting that c24 is worthy of further development as a potent anti-diabetes agent.

Keywords: DPP-4 inhibitor; Fragment-based drug design; Pyrazolo[1,5-a]pyrimidine derivatives; Scaffold hopping; Type 2 diabetes mellitus (T2DM).

MeSH terms

  • Animals
  • Diabetes Mellitus, Experimental / drug therapy*
  • Dipeptidyl Peptidase 4 / metabolism*
  • Dipeptidyl-Peptidase IV Inhibitors / chemical synthesis
  • Dipeptidyl-Peptidase IV Inhibitors / metabolism
  • Dipeptidyl-Peptidase IV Inhibitors / therapeutic use*
  • Drug Design
  • Hep G2 Cells
  • Humans
  • Hypoglycemic Agents / chemical synthesis
  • Hypoglycemic Agents / metabolism
  • Hypoglycemic Agents / therapeutic use*
  • Male
  • Mice, Inbred C57BL
  • Molecular Docking Simulation
  • Molecular Structure
  • Pyrazoles / chemical synthesis
  • Pyrazoles / metabolism
  • Pyrazoles / therapeutic use*
  • Pyrimidines / chemical synthesis
  • Pyrimidines / metabolism
  • Pyrimidines / therapeutic use*
  • Structure-Activity Relationship

Substances

  • Dipeptidyl-Peptidase IV Inhibitors
  • Hypoglycemic Agents
  • Pyrazoles
  • Pyrimidines
  • DPP4 protein, human
  • Dipeptidyl Peptidase 4