Design and synthesis of a novel and potent series of inhibitors of cytosolic phospholipase A(2) based on a 1,3-disubstituted propan-2-one skeleton

J Med Chem. 2002 Mar 14;45(6):1348-62. doi: 10.1021/jm011050x.

Abstract

Using knowledge of the substrate specificity of cPLA(2) (phospholipases A(2)), a novel series of inhibitors of this enzyme were designed based upon a three point model of inhibitor binding to the enzyme active site comprising a lipophilic anchor, an electrophilic serine "trap", and an acidic binding moiety. The resulting 1,3-diheteroatom-substituted propan-2-ones were evaluated as inhibitors of cPLA(2) in both aggregated bilayer and soluble substrate assays. Systematic variation of the lipophilic, electrophilic, and acidic groups revealed a well-defined structure-activity relationship against the enzyme. Optimization of each group led to compound 22 (AR-C70484XX), which contains a decyloxy lipophilic side chain, a 1,3-diaryloxypropan-2-one moiety as a unique serine trap, and a benzoic acid as the acidic binding group. AR-C70484XX was found to be among the most potent in vitro inhibitors of cPLA(2) described to date being more than 20-fold more active against the isolated enzyme (IC(50) = 0.03 microM) than the standard cPLA(2) inhibitor, arachidonyl trifluoromethyl ketone (AACOCF(3)), and also greater than 10-fold more active than AACOCF(3) against the cellular production of arachidonic acid by HL60 cells (IC(50) = 2.8 microM).

MeSH terms

  • Arachidonic Acid / analysis
  • Arachidonic Acid / biosynthesis
  • Cytosol / enzymology
  • Drug Design
  • Enzyme Inhibitors / chemical synthesis*
  • Enzyme Inhibitors / pharmacology
  • HL-60 Cells / drug effects
  • HL-60 Cells / metabolism
  • Humans
  • Ketones / chemical synthesis
  • Ketones / pharmacology
  • Lipid Bilayers / metabolism
  • Phospholipases A / antagonists & inhibitors*
  • Propane / analogs & derivatives*
  • Structure-Activity Relationship

Substances

  • Enzyme Inhibitors
  • Ketones
  • Lipid Bilayers
  • Arachidonic Acid
  • Phospholipases A
  • Propane