Discovery of potent and orally bioavailable 17β-hydroxysteroid dehydrogenase type 3 inhibitors

Bioorg Med Chem. 2012 May 15;20(10):3242-54. doi: 10.1016/j.bmc.2012.03.052. Epub 2012 Apr 1.

Abstract

We have previously reported the discovery of a new class of potent inhibitors of 17β-hydroxysteroid dehydrogenase type 3 (17β-HSD3) derived from benzylidene oxazolidinedione and thiazolidinedione scaffolds. In this study, these analogs were designed, synthesized, and evaluated in a human cell-based assay. The detailed structure-activity relationship (SAR) surrounding this pharmacophore were developed, and consequently a number of compounds from this series demonstrated single-digit nanomolar 17β-HDS3 inhibitory activity in vitro. Subsequent optimization work in pursuit of the improvement of oral bioavailability demonstrated in vivo proof-of-concept by prodrug strategy based on phosphate esters for these 17β-HSD3 inhibitors. When a phosphate ester 16 was administered orally at a high dose of 100mg/kg, 16 showed approximately two times more potent testosterone (T)-lowering effect against a positive control in the luteinizing hormone-releasing hormone (LH-RH)-induced T production assay. The T-lowering effect continued at ca 10% level of control over 4h after administration. The nonsteroidal molecules based on this series have the potential to provide unique and effective clinical opportunities for treatment of prostate cancer.

MeSH terms

  • 17-Hydroxysteroid Dehydrogenases / antagonists & inhibitors*
  • Administration, Oral
  • Animals
  • Antineoplastic Agents / chemical synthesis
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology
  • Drug Discovery*
  • Drug Screening Assays, Antitumor
  • Enzyme Activation / drug effects
  • Enzyme Inhibitors / chemical synthesis*
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / pharmacology*
  • Esters / chemical synthesis
  • Esters / chemistry
  • Esters / pharmacology
  • HeLa Cells
  • Humans
  • Inhibitory Concentration 50
  • Male
  • Phosphates / chemical synthesis
  • Phosphates / chemistry
  • Phosphates / pharmacology
  • Prostatic Neoplasms / drug therapy
  • Rats
  • Rats, Sprague-Dawley
  • Structure-Activity Relationship
  • Testosterone / blood

Substances

  • Antineoplastic Agents
  • Enzyme Inhibitors
  • Esters
  • Phosphates
  • Testosterone
  • 17-Hydroxysteroid Dehydrogenases
  • 17beta-hydroxysteroid dehydrogenase type 3