Identification of determinants required for agonistic and inverse agonistic ligand properties at the ADP receptor P2Y12

Mol Pharmacol. 2013 Jan;83(1):256-66. doi: 10.1124/mol.112.082198. Epub 2012 Oct 23.

Abstract

The ADP receptor P2Y(12) belongs to the superfamily of G protein-coupled receptors (GPCRs), and its activation triggers platelet aggregation. Therefore, potent antagonists, such as clopidogrel, are of high clinical relevance in prophylaxis and treatment of thromboembolic events. P2Y(12) displays an elevated basal activity in vitro, and as such, inverse agonists may be therapeutically beneficial compared with antagonists. Only a few inverse agonists of P2Y(12) have been described. To expand this limited chemical space and improve understanding of structural determinants of inverse agonist-receptor interaction, this study screened a purine compound library for lead structures using wild-type (WT) human P2Y(12) and 28 constitutively active mutants. Results showed that ATP and ATP derivatives are agonists at P2Y(12). The potency at P2Y(12) was 2-(methylthio)-ADP > 2-(methylthio)-ATP > ADP > ATP. Determinants required for agonistic ligand activity were identified. Molecular docking studies revealed a binding pocket for the ATP derivatives that is bordered by transmembrane helices 3, 5, 6, and 7 in human P2Y(12,) with Y(105), E(188), R(256), Y(259), and K(280) playing a particularly important role in ligand interaction. N-Methyl-anthraniloyl modification at the 3'-OH of the 2'-deoxyribose leads to ligands (mant-deoxy-ATP [dATP], mant-deoxy-ADP) with inverse agonist activity. Inverse agonist activity of mant-dATP was found at the WT human P2Y(12) and half of the constitutive active P2Y(12) mutants. This study showed that, in addition to ADP and ATP, other ATP derivatives are not only ligands of P2Y(12) but also agonists. Modification of the ribose within ATP can result in inverse activity of ATP-derived ligands.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • CHO Cells
  • COS Cells
  • Chlorocebus aethiops
  • Cricetinae
  • Cricetulus
  • Cyclic AMP / metabolism
  • Databases, Factual
  • Drug Inverse Agonism
  • High-Throughput Screening Assays
  • Humans
  • Ligands
  • Molecular Docking Simulation*
  • Mutation
  • Purinergic P2Y Receptor Agonists / chemistry*
  • Purinergic P2Y Receptor Agonists / pharmacology
  • Purines / chemistry*
  • Purines / pharmacology
  • Receptors, Purinergic P2Y12 / chemistry*
  • Receptors, Purinergic P2Y12 / genetics
  • Receptors, Purinergic P2Y12 / metabolism
  • Saccharomyces cerevisiae / drug effects
  • Saccharomyces cerevisiae / metabolism
  • Structure-Activity Relationship

Substances

  • Ligands
  • P2RY12 protein, human
  • Purinergic P2Y Receptor Agonists
  • Purines
  • Receptors, Purinergic P2Y12
  • Cyclic AMP