The structural basis of endocannabinoid oxygenation by cyclooxygenase-2

J Biol Chem. 2011 Jun 10;286(23):20736-45. doi: 10.1074/jbc.M111.230367. Epub 2011 Apr 13.

Abstract

The cyclooxygenases (COX-1 and COX-2) oxygenate arachidonic acid (AA) in the committed step of prostaglandin biogenesis. Substitutions of I434V, H513R, and I523V constitute the only differences in residues lining the cyclooxygenase channel between COX-1 and COX-2. These changes create a hydrophobic pocket in COX-2, with Arg-513 located at the base of the pocket, which has been exploited in the design of COX-2-selective inhibitors. Previous studies have shown that COX-2, but not COX-1, can oxygenate endocannabinoid substrates, including 2-arachidonoyl glycerol (2-AG). To investigate the isoform-specific structural basis of endocannabinoid binding to COX-2, we determined the crystal structure of the 2-AG isomer 1-arachidonoyl glycerol (1-AG) in complex with wild type and R513H murine (mu) COX-2 to 2.2 and 2.35 Å, respectively, and R513H muCOX-2 in complex with AA to 2.45 Å resolution. The 2,3-dihydroxypropyl moiety of 1-AG binds near the opening of the cyclooxygenase channel in the space vacated by the movement of the Leu-531 side chain, validating our previous hypothesis implicating the flexibility of the Leu-531 side chain as a determinant for the ability of COX-2 to oxygenate endocannabinoid substrates. Functional analyses carried out to compliment our structural findings indicated that Y355F and R513H muCOX-2 constructs had no effect on the oxygenation of 1-AG and 2-AG, whereas substitutions that resulted in a shortened side chain for Leu-531 had only modest effects. Both AA and 1-AG bind to R513H muCOX-2 in conformations similar to those observed in the co-crystal structures of these substrates with wild type enzyme.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Amino Acid Substitution
  • Animals
  • Arachidonic Acids / chemistry*
  • Arachidonic Acids / metabolism
  • Cannabinoid Receptor Modulators / chemistry*
  • Cannabinoid Receptor Modulators / metabolism
  • Crystallography, X-Ray
  • Cyclooxygenase 2 / chemistry*
  • Cyclooxygenase 2 / genetics
  • Cyclooxygenase 2 / metabolism
  • Endocannabinoids*
  • Glycerides / chemistry*
  • Glycerides / metabolism
  • Mice
  • Mutation, Missense
  • Oxidation-Reduction
  • Protein Binding
  • Protein Structure, Tertiary
  • Substrate Specificity

Substances

  • Arachidonic Acids
  • Cannabinoid Receptor Modulators
  • Endocannabinoids
  • Glycerides
  • glyceryl 2-arachidonate
  • Ptgs2 protein, mouse
  • Cyclooxygenase 2

Associated data

  • PDB/3MDL
  • PDB/3OLT
  • PDB/3OLU