Chiral nonsteroidal affinity ligands for the androgen receptor. 1. Bicalutamide analogues bearing electrophilic groups in the B aromatic ring

J Med Chem. 2000 Feb 24;43(4):581-90. doi: 10.1021/jm990027x.

Abstract

A series of chiral analogues of bicalutamide bearing electrophilic groups (isothiocyanate, N-chloroacetyl, and N-bromoacetyl) on aromatic ring B of the parent molecule were synthesized. These compounds were designed as affinity ligands for the androgen receptor (AR). We prepared the (R)- and (S)-optical isomers of these compounds as pure enantiomers. The AR binding affinities of these compounds were measured in a competitive binding assay with the radiolabeled high-affinity AR ligand, [(3)H]mibolerone. In accordance with our previous results for the enantiomers of bicalutamide, we found that all (R)-isomers demonstrated much higher binding affinity to the AR as compared to their corresponding (S)-isomers. The para-substituted affinity ligands in ring B bound the AR with higher affinities than the corresponding meta-substituted analogues. Oxidation of thioester affinity ligands to their sulfonyl analogues for the para-substituted compounds decreased AR binding affinities and similar modification increased binding affinities for corresponding meta-analogues. The least potent para-substituted sulfonyl compounds had higher AR binding affinities than the most potent meta-substituted sulfonyl compounds. Overall, the para-substituted unoxidized molecules demonstrated the highest AR binding affinity. Subsequent research using AR exchange assays and Scatchard analyses showed that the isothiocyanate affinity ligands (R)-7, (R)-9, and (R)-10 reported herein are the first specific chemoaffinity ligands for the AR.

Publication types

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

MeSH terms

  • Androgen Antagonists / chemical synthesis*
  • Androgen Antagonists / chemistry
  • Androgen Antagonists / metabolism
  • Androgen Receptor Antagonists
  • Anilides / chemical synthesis*
  • Anilides / chemistry
  • Anilides / metabolism
  • Animals
  • Disulfides / chemical synthesis*
  • Disulfides / chemistry
  • Disulfides / metabolism
  • In Vitro Techniques
  • Isothiocyanates / chemical synthesis*
  • Isothiocyanates / chemistry
  • Isothiocyanates / metabolism
  • Ligands
  • Male
  • Nitriles
  • Prostate / metabolism
  • Radioligand Assay
  • Rats
  • Rats, Sprague-Dawley
  • Receptors, Androgen / metabolism*
  • Stereoisomerism
  • Structure-Activity Relationship
  • Sulfones / chemical synthesis*
  • Sulfones / chemistry
  • Sulfones / metabolism
  • Tosyl Compounds

Substances

  • Androgen Antagonists
  • Androgen Receptor Antagonists
  • Anilides
  • Disulfides
  • Isothiocyanates
  • Ligands
  • N1-(4-cyano--3-(trifluoromethyl)phenyl)-2-hydroxy-3-((3-isothiocyanatophenyl)sulfanyl)-2-methylpropanamide
  • N1-(4-cyano-3-(trifluoromethyl)phenyl)-2-hydroxy-3-((4-isothiocyanatophenyl)sulfanyl)-2-methylpropanamide
  • N1-(4-cyano-3--(trifluoromethyl)phenyl)-2-hydroxy-3-((4-isothiocyanatophenyl)sulfonyl)-2-methylpropanamide
  • Nitriles
  • Receptors, Androgen
  • Sulfones
  • Tosyl Compounds
  • bicalutamide