N-1 and C-3 substituted indole Schiff bases as selective COX-2 inhibitors: synthesis and biological evaluation

Bioorg Med Chem Lett. 2012 Mar 15;22(6):2154-9. doi: 10.1016/j.bmcl.2012.01.130. Epub 2012 Feb 6.

Abstract

A group of N-1 and C-3 disubstituted-indole Schiff bases bearing an indole N-1 (R'=H, CH(2)Ph, COPh) substituent in conjunction with a C-3 -C=HN-C(6)H(4)-4-X (X=F, Me, CF(3), Cl) substituent were synthesized and evaluated as inhibitors of cyclooxygenase (COX) isozymes (COX-1/COX-2). Within this group of Schiff bases, compounds 15 (R(1)=CH(2)Ph, X=F), 17 (R(1)=CH(2)Ph, X=CF(3)), 18 (R(1)=COPh, X=F) and 20 (R(1)=COPh, X=CF(3)) were identified as effective and selective COX-2 inhibitors (COX-2 IC(50)'s=0.32-0.84 μM range; COX-2 selectivity index (SI)=113 to >312 range). 1-Benzoyl-3-[(4-trifluoromethylphenylimino)methyl]indole (20) emerged as the most potent (COX-1 IC(50) >100 μM; COX-2 IC(50)=0.32 μM) and selective (SI >312) COX-2 inhibitor. Furthermore, compound 20 is a selective COX-2 inhibitor in contrast to the reference drug indomethacin that is a potent and selective COX-1 inhibitor (COX-1 IC(50)=0.13 μM; COX-2 IC(50)=6.9 μM, COX-2 SI=0.02). Molecular modeling studies employing compound 20 showed that the phenyl CF(3) substituent attached to the CN spacer is positioned near the secondary pocket of the COX-2 active site, the CN nitrogen atom is hydrogen bonded (N···NH=2.85 Å) to the H90 residue, and the indole N-1 benzoyl is positioned in a hydrophobic pocket of the COX-2 active site near W387.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Catalytic Domain
  • Cyclooxygenase 1 / chemistry*
  • Cyclooxygenase 1 / metabolism
  • Cyclooxygenase 2 / chemistry*
  • Cyclooxygenase 2 / metabolism
  • Cyclooxygenase Inhibitors / chemical synthesis*
  • Cyclooxygenase Inhibitors / pharmacology
  • Drug Design
  • Humans
  • Indoles / chemical synthesis*
  • Indoles / pharmacology
  • Indomethacin / pharmacology
  • Kinetics
  • Models, Molecular
  • Recombinant Proteins / chemistry
  • Recombinant Proteins / metabolism
  • Schiff Bases / chemical synthesis*
  • Schiff Bases / pharmacology
  • Sheep
  • Solutions
  • Structure-Activity Relationship

Substances

  • Cyclooxygenase Inhibitors
  • Indoles
  • Recombinant Proteins
  • Schiff Bases
  • Solutions
  • Cyclooxygenase 1
  • Cyclooxygenase 2
  • Indomethacin