Discovery of potent and selective inhibitors of human platelet-type 12- lipoxygenase

J Med Chem. 2011 Aug 11;54(15):5485-97. doi: 10.1021/jm2005089. Epub 2011 Jul 8.

Abstract

We report the discovery of novel small molecule inhibitors of platelet-type 12-human lipoxygenase, which display nanomolar activity against the purified enzyme, using a quantitative high-throughput screen (qHTS) on a library of 153607 compounds. These compounds also exhibit excellent specificity, >50-fold selectivity vs the paralogues, 5-human lipoxygenase, reticulocyte 15-human lipoxygenase type-1, and epithelial 15-human lipoxygenase type-2, and >100-fold selectivity vs ovine cyclooxygenase-1 and human cyclooxygenase-2. Kinetic experiments indicate this chemotype is a noncompetitive inhibitor that does not reduce the active site iron. Moreover, chiral HPLC separation of two of the racemic lead molecules revealed a strong preference for the (-)-enantiomers (IC(50) of 0.43 ± 0.04 and 0.38 ± 0.05 μM) compared to the (+)-enantiomers (IC(50) of >25 μM for both), indicating a fine degree of selectivity in the active site due to chiral geometry. In addition, these compounds demonstrate efficacy in cellular models, which underscores their relevance to disease modification.

Publication types

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

MeSH terms

  • 12-Hydroxy-5,8,10,14-eicosatetraenoic Acid / antagonists & inhibitors
  • Animals
  • Arachidonate 12-Lipoxygenase / drug effects*
  • Blood Platelets / enzymology
  • Humans
  • Islets of Langerhans / drug effects
  • Kinetics
  • Lipoxygenase Inhibitors / chemical synthesis
  • Lipoxygenase Inhibitors / pharmacokinetics
  • Lipoxygenase Inhibitors / pharmacology*
  • Mice
  • Sheep
  • Stereoisomerism
  • Structure-Activity Relationship

Substances

  • Lipoxygenase Inhibitors
  • 12-Hydroxy-5,8,10,14-eicosatetraenoic Acid
  • Arachidonate 12-Lipoxygenase