Route to Prolonged Residence Time at the Histamine H1 Receptor: Growing from Desloratadine to Rupatadine

J Med Chem. 2019 Jul 25;62(14):6630-6644. doi: 10.1021/acs.jmedchem.9b00447. Epub 2019 Jul 5.

Abstract

Drug-target binding kinetics are an important predictor of in vivo drug efficacy, yet the relationship between ligand structures and their binding kinetics is often poorly understood. We show that both rupatadine (1) and desloratadine (2) have a long residence time at the histamine H1 receptor (H1R). Through development of a [3H]levocetirizine radiolabel, we find that the residence time of 1 exceeds that of 2 more than 10-fold. This was further explored with 22 synthesized rupatadine and desloratadine analogues. Methylene-linked cycloaliphatic or β-branched substitutions of desloratadine increase the residence time at the H1R, conveying a longer duration of receptor antagonism. However, cycloaliphatic substituents directly attached to the piperidine amine (i.e., lacking the spacer) have decreased binding affinity and residence time compared to their methylene-linked structural analogues. Guided by docking studies, steric constraints within the binding pocket are hypothesized to explain the observed differences in affinity and binding kinetics between analogues.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cyproheptadine / analogs & derivatives*
  • Cyproheptadine / chemistry
  • Cyproheptadine / pharmacology
  • Histamine H1 Antagonists / chemistry
  • Histamine H1 Antagonists / pharmacology*
  • Humans
  • Kinetics
  • Loratadine / analogs & derivatives*
  • Loratadine / chemistry
  • Loratadine / pharmacology
  • Molecular Docking Simulation
  • Protein Binding
  • Receptors, Histamine H1 / metabolism*
  • Time Factors

Substances

  • Histamine H1 Antagonists
  • Receptors, Histamine H1
  • rupatadine
  • Cyproheptadine
  • Loratadine
  • desloratadine