Synthesis, modeling, and in vitro activity of (3'S)-epi-K-252a analogues. Elucidating the stereochemical requirements of the 3'-sugar alcohol on trkA tyrosine kinase activity

J Med Chem. 2005 Jun 2;48(11):3776-83. doi: 10.1021/jm040178m.

Abstract

Utilizing our recently published semisynthetic approach to the (3'S)-K-252a diastereomer, we report the first synthesis of the (3'R)-10 diastereomer and a set of related epimers, with the goal of defining the stereochemical role of the 3'-sugar hydroxyl group on trkA tyrosine kinase activity and selectivity. (3'R)-10 displayed potent trkA inhibitory activity with an IC50 value of 4 nM. The corresponding deshydroxy epimer (3'S)-14 was 7-fold more potent than its 3'R counterpart (natural stereochemistry) with a trkA IC50 value of 3 nM and demonstrated >280-fold selectivity over PKC (IC50 = 850 nM). In cells, (3'S)-14 displayed potent inhibition of trkA autophosphorylation with an IC50 < 10 nM. Molecular modeling studies revealed that the 3'-OH, due to the inverted geometry, forms significant H-bonding interactions with Glu27 and Arg195, an interaction that is not attainable with the natural isomers.

MeSH terms

  • Animals
  • Carbazoles / chemical synthesis*
  • Carbazoles / chemistry
  • Carbazoles / pharmacology
  • Hydrogen Bonding
  • Hydrophobic and Hydrophilic Interactions
  • Indole Alkaloids
  • Mice
  • Models, Molecular
  • Molecular Conformation
  • NIH 3T3 Cells
  • Phosphorylation
  • Protein Kinase C / antagonists & inhibitors
  • Receptor, trkA / antagonists & inhibitors*
  • Receptor, trkA / metabolism
  • Stereoisomerism
  • Structure-Activity Relationship
  • Sugar Alcohols / chemistry*
  • Thermodynamics

Substances

  • Carbazoles
  • Indole Alkaloids
  • Sugar Alcohols
  • staurosporine aglycone
  • Receptor, trkA
  • Protein Kinase C