Design and synthesis of diazatricyclodecane agonists of the G-protein-coupled receptor 119

J Med Chem. 2013 Jan 10;56(1):301-19. doi: 10.1021/jm301626p. Epub 2012 Dec 31.

Abstract

A series of GPR119 agonists based on a 2,6-diazatricyclo[3.3.1.1∼3,7∼]decane ring system is described. Also provided is a detailed account of the development of a multigram scale synthesis of the diazatricyclic ring system, which was achieved using a Hofmann-Löffler-Freytag reaction as the key step. The basis for the use of this complex framework lies in an attempt to constrain one end of the molecule in the "agonist conformation" as was previously described for 3-oxa-7-aza-bicyclo[3.3.1]nonanes. Optimization of carbamate analogues of the diazatricylic compounds led to the identification of 32i as a potent agonist of the GPR119 receptor with low unbound human liver microsomal clearance. The use of an agonist response weighted ligand lipophilic efficiency (LLE) termed AgLLE is discussed along with the issues of applying efficiency measures to agonist programs. Ultimately, solubility limited absorption and poor exposure reduced further interest in these molecules.

MeSH terms

  • Animals
  • Aza Compounds / chemical synthesis*
  • Aza Compounds / chemistry
  • Aza Compounds / pharmacology
  • Biological Availability
  • Bridged-Ring Compounds / chemical synthesis*
  • Bridged-Ring Compounds / chemistry
  • Bridged-Ring Compounds / pharmacology
  • Crystallography, X-Ray
  • Cyclodecanes / chemical synthesis*
  • Cyclodecanes / chemistry
  • Cyclodecanes / pharmacology
  • Dogs
  • Drug Design
  • Humans
  • Male
  • Microsomes, Liver / metabolism
  • Molecular Structure
  • Pyrimidines / chemical synthesis
  • Pyrimidines / chemistry
  • Pyrimidines / pharmacology
  • Rats
  • Rats, Sprague-Dawley
  • Receptors, G-Protein-Coupled / agonists*
  • Receptors, G-Protein-Coupled / chemistry
  • Solubility
  • Stereoisomerism
  • Structure-Activity Relationship

Substances

  • Aza Compounds
  • Bridged-Ring Compounds
  • Cyclodecanes
  • GPR119 protein, human
  • Pyrimidines
  • Receptors, G-Protein-Coupled