Discovery of 5-Chloro-1-(5-chloro-2-(methylsulfonyl)benzyl)-2-imino-1,2-dihydropyridine-3-carboxamide (TAK-259) as a Novel, Selective, and Orally Active α1D Adrenoceptor Antagonist with Antiurinary Frequency Effects: Reducing Human Ether-a-go-go-Related Gene (hERG) Liabilities

J Med Chem. 2016 Apr 14;59(7):2989-3002. doi: 10.1021/acs.jmedchem.5b01528. Epub 2016 Mar 17.

Abstract

A novel structural class of iminopyridine derivative 1 was identified as a potent and selective human α1D adrenoceptor (α1D adrenergic receptor; α1D-AR) antagonist against α1A- and α1B-AR through screening of an in-house compound library. From initial structure-activity relationship studies, we found lead compound 9m with hERG K(+) channel liability. To develop analogues with reduced hERG K(+) channel inhibition, a combination of site-directed mutagenesis and docking studies was employed. Further optimization led to the discovery of (R)-9s and 9u, which showed antagonistic activity by a bladder strip test in rats with bladder outlet obstruction, as well as ameliorated cystitis-induced urinary frequency in rats. Ultimately, 9u was selected as a clinical candidate. This is the first study to show the utility of iminopyridine derivatives as selective α1D-AR antagonists and evaluate their effects in vivo.

MeSH terms

  • Administration, Oral
  • Adrenergic alpha-1 Receptor Antagonists / administration & dosage
  • Adrenergic alpha-1 Receptor Antagonists / chemistry*
  • Adrenergic alpha-1 Receptor Antagonists / pharmacokinetics
  • Adrenergic alpha-1 Receptor Antagonists / pharmacology*
  • Animals
  • Chemistry Techniques, Synthetic
  • Cystitis / chemically induced
  • Cystitis / drug therapy
  • Disease Models, Animal
  • Drug Discovery
  • Drug Evaluation, Preclinical / methods
  • ERG1 Potassium Channel
  • Ether-A-Go-Go Potassium Channels / antagonists & inhibitors*
  • Ether-A-Go-Go Potassium Channels / genetics
  • Ether-A-Go-Go Potassium Channels / metabolism
  • Humans
  • Imines / administration & dosage
  • Imines / chemistry*
  • Imines / pharmacology*
  • Molecular Docking Simulation
  • Mutagenesis, Site-Directed
  • Niacinamide / administration & dosage
  • Niacinamide / analogs & derivatives*
  • Niacinamide / chemistry
  • Niacinamide / pharmacology
  • Rats
  • Receptors, Adrenergic, alpha-1 / metabolism*
  • Structure-Activity Relationship
  • Urinary Bladder / drug effects
  • Urinary Bladder / physiology
  • Urinary Bladder Neck Obstruction / drug therapy
  • Urinary Bladder Neck Obstruction / physiopathology
  • Urinary Bladder, Overactive / drug therapy

Substances

  • ADRA1D protein, human
  • Adrenergic alpha-1 Receptor Antagonists
  • ERG1 Potassium Channel
  • Ether-A-Go-Go Potassium Channels
  • Imines
  • KCNH2 protein, human
  • Receptors, Adrenergic, alpha-1
  • TAK-259
  • Niacinamide