Potent and selective alpha-ketoheterocycle-based inhibitors of the anandamide and oleamide catabolizing enzyme, fatty acid amide hydrolase

J Med Chem. 2007 Mar 8;50(5):1058-68. doi: 10.1021/jm0611509. Epub 2007 Feb 6.

Abstract

A study of the structure-activity relationships (SAR) of 2f (OL-135), a potent inhibitor of fatty acid amide hydrolase (FAAH), is detailed, targeting the 5-position of the oxazole. Examination of a series of substituted benzene derivatives (12-14) revealed that the optimal position for substitution was the meta-position with selected members approaching or exceeding the potency of 2f. Concurrent with these studies, the effect of substitution on the pyridine ring of 2f was also examined. A series of small, nonaromatic C5-substituents was also explored and revealed that the K(i) follows a well-defined correlation with the Hammett sigma(p) constant (rho = 3.01, R2 = 0.91) in which electron-withdrawing substituents enhance potency, leading to inhibitors with K(i)s as low as 400 pM (20n). Proteomic-wide screening of the inhibitors revealed that most are exquisitely selective for FAAH over all other mammalian proteases, reversing the 100-fold preference of 20a (C5 substituent = H) for the enzyme TGH.

Publication types

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

MeSH terms

  • Amidohydrolases / antagonists & inhibitors*
  • Amidohydrolases / chemistry
  • Animals
  • Arachidonic Acids / metabolism*
  • Benzene Derivatives / chemical synthesis*
  • Benzene Derivatives / chemistry
  • Benzene Derivatives / pharmacology
  • COS Cells
  • Chlorocebus aethiops
  • Endocannabinoids
  • Humans
  • Oleic Acids / metabolism*
  • Oxazoles / chemical synthesis*
  • Oxazoles / chemistry
  • Oxazoles / pharmacology
  • Polyunsaturated Alkamides / metabolism*
  • Proteomics
  • Rats
  • Recombinant Proteins / antagonists & inhibitors
  • Recombinant Proteins / chemistry
  • Structure-Activity Relationship

Substances

  • Arachidonic Acids
  • Benzene Derivatives
  • Endocannabinoids
  • Oleic Acids
  • Oxazoles
  • Polyunsaturated Alkamides
  • Recombinant Proteins
  • oleylamide
  • Amidohydrolases
  • fatty-acid amide hydrolase
  • anandamide