Novel pyrazoles and pyrazolo[1,2-a]pyridazines as selective COX-2 inhibitors; Ultrasound-assisted synthesis, biological evaluation, and DFT calculations

Bioorg Med Chem Lett. 2017 Jun 1;27(11):2377-2383. doi: 10.1016/j.bmcl.2017.04.020. Epub 2017 Apr 8.

Abstract

COX-2 is an inducible enzyme mediating inflammatory responses. Selective targeting of COX-2 is useful for developing anti-inflammatory agents devoid of ulcerogenic activity. Herein, we report the design and synthesis of a series of pyrazoles and pyrazolo[1,2-a]pyridazines with selective COX-2 inhibitory activity and in vivo anti-inflammatory effect. Both series were accessed through acid-catalyzed ultrasound-assisted reactions. The most active compounds in this study are two novel molecules, 11 and 16, showing promising selectivity and decent IC50 of 16.2 and 20.1nM, respectively. These compounds were also docked into the crystal structure of COX-2 enzyme (PDB ID: 3LN1) to understand their mode of binding. Finally, Mulliken charges and electrostatic surface potential were calculated for both compound 11 and celecoxib using DFT method to get insights into the molecular determinants of activity of this compound. These results could lead to the development of novel COX-2 inhibitors with improved selectivity.

Keywords: Anti-inflammatory; COX-2; DFT calculations; Pyrazole; Pyrazolo[1,2-a]pyridazine; Ultrasound-assisted reactions.

MeSH terms

  • Animals
  • Anti-Inflammatory Agents, Non-Steroidal / chemical synthesis
  • Anti-Inflammatory Agents, Non-Steroidal / pharmacology*
  • Binding Sites / drug effects
  • Celecoxib / chemistry
  • Cyclization
  • Cyclooxygenase 2 Inhibitors / chemical synthesis
  • Cyclooxygenase 2 Inhibitors / pharmacology*
  • Enzyme Assays
  • Hydrophobic and Hydrophilic Interactions
  • Molecular Docking Simulation
  • Pyrazoles / chemical synthesis
  • Pyrazoles / pharmacology*
  • Pyridazines / chemical synthesis
  • Pyridazines / pharmacology*
  • Quantum Theory
  • Quinones / chemical synthesis
  • Quinones / pharmacology*
  • Spodoptera
  • Ultrasonic Waves*

Substances

  • (2-hydroxyphenyl)(5-(2-hydroxyphenyl)-3-(phenylamino)-1H-pyrazol-1-yl)methanone
  • 9-amino-7-(2-hydroxyphenyl)-5,11-dioxo-7,11-dihydro-5H-pyrazolo(1,2-a)pyrido(2,3-d)pyridazine-8-carboxylate
  • Anti-Inflammatory Agents, Non-Steroidal
  • Cyclooxygenase 2 Inhibitors
  • Pyrazoles
  • Pyridazines
  • Quinones
  • Celecoxib