Structure-based design, synthesis, and biological evaluation of indomethacin derivatives as cyclooxygenase-2 inhibiting nitric oxide donors

J Med Chem. 2007 Dec 13;50(25):6367-82. doi: 10.1021/jm0611861. Epub 2007 Nov 10.

Abstract

Indomethacin, a nonselective cyclooxygenase (COX) inhibitor, was modified in three distinct regions in an attempt both to increase cyclooxygenase-2 (COX-2) selectivity and to enhance drug safety by covalent attachment of an organic nitrate moiety as a nitric oxide donor. A human whole-blood COX assay shows the modifications on the 3-acetic acid part of the indomethacin yielding an amide-nitrate derivative 32 and a sulfonamide-nitrate derivative 61 conferred COX-2 selectivity. Along with their respective des-nitrate analogs, for example, 31 and 62, the nitrates 32 and 61 were effective antiinflammatory agents in the rat air-pouch model. After oral dosing, though, only 32 increased nitrate and nitrite levels in rat plasma, indicating that its nitrate tether served as a nitric oxide donor in vivo. In a rat gastric injury model, examples 31 and 32 both show a 98% reduction in gastric lesion score compared to that of indomethacin. In addition, the nitrated derivative 32 inducing 85% fewer gastric lesions when coadministered with aspirin as compared to the combination of aspirin and valdecoxib.

MeSH terms

  • Animals
  • Aspirin / adverse effects
  • Celecoxib
  • Cyclooxygenase 2 Inhibitors / adverse effects
  • Cyclooxygenase 2 Inhibitors / chemical synthesis*
  • Cyclooxygenase 2 Inhibitors / pharmacology
  • Drug Design
  • Drug Synergism
  • Female
  • Gastric Mucosa / pathology
  • Humans
  • Hydroxamic Acids / adverse effects
  • Hydroxamic Acids / chemical synthesis
  • Hydroxamic Acids / pharmacology
  • Indomethacin / adverse effects
  • Indomethacin / analogs & derivatives*
  • Indomethacin / chemical synthesis*
  • Indomethacin / pharmacology
  • Male
  • Nitric Oxide Donors / adverse effects
  • Nitric Oxide Donors / chemical synthesis*
  • Nitric Oxide Donors / pharmacology
  • Pyrazoles / pharmacology
  • Rats
  • Rats, Sprague-Dawley
  • Stomach Ulcer / chemically induced
  • Stomach Ulcer / pathology
  • Structure-Activity Relationship
  • Sulfonamides / pharmacology

Substances

  • Cyclooxygenase 2 Inhibitors
  • Hydroxamic Acids
  • Nitric Oxide Donors
  • Pyrazoles
  • Sulfonamides
  • Celecoxib
  • Aspirin
  • Indomethacin