Novel multi-target-directed ligands for Alzheimer's disease: Combining cholinesterase inhibitors and 5-HT6 receptor antagonists. Design, synthesis and biological evaluation

Eur J Med Chem. 2016 Nov 29:124:63-81. doi: 10.1016/j.ejmech.2016.08.016. Epub 2016 Aug 11.

Abstract

As currently postulated, a complex treatment may be key to an effective therapy for Alzheimer's disease (AD). Recent clinical trials in patients with moderate AD have shown a superior effect of the combination therapy of donepezil (a selective acetylcholinesterase inhibitor) with idalopirdine (a 5-HT6 receptor antagonist) over monotherapy with donepezil. Here, we present the first report on the design, synthesis and biological evaluation of a novel class of multifunctional ligands that combines a 5-HT6 receptor antagonist with a cholinesterase inhibitor. Novel multi-target-directed ligands (MTDLs) were designed by combining pharmacophores directed against the 5-HT6 receptor (1-(phenylsulfonyl)-4-(piperazin-1-yl)-1H-indole) and cholinesterases (tacrine or N-benzylpiperidine analogues). In vitro evaluation led to the identification of tacrine derivative 12 with well-balanced potencies against the 5-HT6 receptor (Kb = 27 nM), acetylcholinesterase and butyrylcholinesterase (IC50hAChE = 12 nM, IC50hBuChE = 29 nM). The compound also showed good in vitro blood-brain-barrier permeability (PAMPA-BBB assay), which was confirmed in vivo (open field study). Central cholinomimetic activity was confirmed in vivo in rats using a scopolamine-induced hyperlocomotion model. A novel class of multifunctional ligands with compound 12 as the best derivative in a series represents an excellent starting point for the further development of an effective treatment for AD.

Keywords: 5-HT(6) receptor antagonists; Acetylcholinesterase inhibitors; Alzheimer's disease; Butyrylcholinesterase inhibitors; Multi-target-directed ligands.

MeSH terms

  • Acetylcholinesterase / metabolism
  • Alzheimer Disease / diet therapy*
  • Alzheimer Disease / enzymology
  • Alzheimer Disease / metabolism
  • Animals
  • Blood-Brain Barrier / metabolism
  • Butyrylcholinesterase / metabolism
  • Catalytic Domain
  • Chemistry Techniques, Synthetic
  • Cholinesterase Inhibitors / chemical synthesis*
  • Cholinesterase Inhibitors / chemistry
  • Cholinesterase Inhibitors / metabolism
  • Cholinesterase Inhibitors / pharmacology*
  • Drug Design*
  • Humans
  • Kinetics
  • Ligands
  • Male
  • Models, Molecular
  • Molecular Targeted Therapy*
  • Protein Conformation
  • Rats
  • Rats, Wistar
  • Receptors, Serotonin / chemistry
  • Receptors, Serotonin / metabolism*

Substances

  • Cholinesterase Inhibitors
  • Ligands
  • Receptors, Serotonin
  • serotonin 6 receptor
  • Acetylcholinesterase
  • Butyrylcholinesterase