Selectively targeting the DNA-binding domain of the androgen receptor as a prospective therapy for prostate cancer

J Biol Chem. 2014 Sep 19;289(38):26417-26429. doi: 10.1074/jbc.M114.553818. Epub 2014 Aug 1.

Abstract

The androgen receptor (AR) is a transcription factor that has a pivotal role in the occurrence and progression of prostate cancer. The AR is activated by androgens that bind to its ligand-binding domain (LBD), causing the transcription factor to enter the nucleus and interact with genes via its conserved DNA-binding domain (DBD). Treatment for prostate cancer involves reducing androgen production or using anti-androgen drugs to block the interaction of hormones with the AR-LBD. Eventually the disease changes into a castration-resistant form of PCa where LBD mutations render anti-androgens ineffective or where constitutively active AR splice variants, lacking the LBD, become overexpressed. Recently, we identified a surfaced exposed pocket on the AR-DBD as an alternative drug-target site for AR inhibition. Here, we demonstrate that small molecules designed to selectively bind the pocket effectively block transcriptional activity of full-length and splice variant AR forms at low to sub-micromolar concentrations. The inhibition is lost when residues involved in drug interactions are mutated. Furthermore, the compounds did not impede nuclear localization of the AR and blocked interactions with chromatin, indicating the interference of DNA binding with the nuclear form of the transcription factor. Finally, we demonstrate the inhibition of gene expression and tumor volume in mouse xenografts. Our results indicate that the AR-DBD has a surface site that can be targeted to inhibit all forms of the AR, including enzalutamide-resistant and constitutively active splice variants and thus may serve as a potential avenue for the treatment of recurrent and metastatic prostate cancer.

Keywords: Androgen Receptor; DNA-binding Protein; Drug Discovery; Nuclear Receptor; Prostate Cancer.

Publication types

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

MeSH terms

  • Active Transport, Cell Nucleus
  • Amino Acid Sequence
  • Androgen Receptor Antagonists / pharmacology*
  • Animals
  • Binding Sites
  • Cell Nucleus / metabolism
  • Chromatin / metabolism
  • Gene Expression Regulation, Neoplastic
  • Humans
  • Imidazoles / pharmacology*
  • MCF-7 Cells
  • Male
  • Mice, Nude
  • Molecular Sequence Data
  • Molecular Targeted Therapy
  • Prostatic Neoplasms / drug therapy*
  • Prostatic Neoplasms / pathology
  • Protein Binding
  • Protein Isoforms / chemistry
  • Protein Isoforms / physiology
  • Receptors, Androgen / chemistry
  • Receptors, Androgen / physiology*
  • Thiazoles / pharmacology*
  • Transcription, Genetic
  • Transcriptional Activation
  • Tumor Burden / drug effects
  • Xenograft Model Antitumor Assays

Substances

  • 4-(4-(4,5-bromo-1H-imidazol-1-yl)thiazol-2-yl)morpholine
  • Androgen Receptor Antagonists
  • Chromatin
  • Imidazoles
  • Protein Isoforms
  • Receptors, Androgen
  • Thiazoles

Associated data

  • PDB/1R4I