Chiral Cyclic Aliphatic Linkers as Building Blocks for Selective Dopamine D2 or D3 Receptor Agonists

J Med Chem. 2021 Nov 11;64(21):16088-16105. doi: 10.1021/acs.jmedchem.1c01433. Epub 2021 Oct 26.

Abstract

Linkers are emerging as a key component in regulating the pharmacology of bitopic ligands directed toward G-protein coupled receptors (GPCRs). In this study, the role of regio- and stereochemistry in cyclic aliphatic linkers tethering well-characterized primary and secondary pharmacophores targeting dopamine D2 and D3 receptor subtypes (D2R and D3R, respectively) is described. We introduce several potent and selective D2R (rel-trans-16b; D2R Ki = 4.58 nM) and D3R (rel-cis-14a; D3R Ki = 5.72 nM) agonists while modulating subtype selectivity in a stereospecific fashion, transferring D2R selectivity toward D3R via inversion of the stereochemistry around these cyclic aliphatic linkers [e.g., (-)-(1S,2R)-43 and (+)-(1R,2S)-42]. Pharmacological observations were supported with extensive molecular docking studies. Thus, not only is it an innovative approach to modulate the pharmacology of dopaminergic ligands described, but a new class of optically active cyclic linkers are also introduced, which can be used to expand the bitopic drug design approach toward other GPCRs.

Publication types

  • Research Support, N.I.H., Intramural

MeSH terms

  • Dopamine Agonists / chemistry
  • Dopamine Agonists / pharmacology*
  • HEK293 Cells
  • Humans
  • Ligands
  • Molecular Docking Simulation
  • Radioligand Assay
  • Receptors, Dopamine D2 / drug effects*
  • Receptors, Dopamine D3 / drug effects*
  • Stereoisomerism

Substances

  • Dopamine Agonists
  • Ligands
  • Receptors, Dopamine D2
  • Receptors, Dopamine D3