Synthesis, structure-property relationships and pharmacokinetic evaluation of ethyl 6-aminonicotinate sulfonylureas as antagonists of the P2Y₁₂ receptor

Eur J Med Chem. 2013 Jul:65:360-75. doi: 10.1016/j.ejmech.2013.04.007. Epub 2013 May 15.

Abstract

The present paper describes the development of a new series of P2Y12 receptor antagonists based on our previously reported piperazinyl urea series 1 (IC50 binding affinity = 0.33 μM, aq solubility <0.1 μM, microsomal CLint (HLM) ≥300 μM/min/mg). By replacement of the urea functionality with a sulfonylurea group we observed increased affinity along with improved stability and solubility as exemplified by 47 (IC50 binding affinity = 0.042 μM, aq solubility = 90 μM, microsomal CLint (HLM) = 70 μM/min/mg). Further improvements in affinity and metabolic stability were achieved by replacing the central piperazine ring with a 3-aminoazetidine as exemplified by 3 (IC50 binding affinity = 0.0062 μM, aq solubility = 83 μM, microsomal CLint (HLM) = 28 μM/min/mg). The improved affinity observed in the in vitro binding assay also translated to the potency observed in the WPA aggregation assay (47: 19 nM and 3: 9.5 nM) and the observed in vitro ADME properties translates to the in vivo PK properties observed in rat. In addition, we found that the chemical stability of the sulfonylureas during prolonged storage in solution was related to the sulfonyl urea linker and depended on the type of solvent and the substitution pattern of the sulfonyl urea functionality.

Keywords: 1-hydroxybenzotriazole; 2,2,2-trichloroethyl chloroformate; 2-morpholinoethanesulphonic acid monohydrate; 3-amino-azetidinyl; 3-aze; 4-amino-piperidinyl; 4-dimethylamino-pyridine; 4-pip; Anti-platelet; CDI; CLint; Caco-2; DIPEA; DMA; DMAP; DSC; EDCI; GTPγS; HLM; HOBT; LC; MES; MW; N,N-diisopropylethylamine; N,N′-carbonyl diimidazole; N,N′-disuccinimide carbonate; N-(3-dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride; P2Y(12) receptor; PS; RLM; Solubility; Stability; Sulfonylureas; TEA; TEER; TEG; Troc-Cl; WPA; adenocarcinoma cells from human colon; cy-Pr; cyclopropyl; dimethylacetamide; guanosine 5′-O-[γ-thio]triphosphate; human liver microsomes; intrinsic clearance; liquid chromatography; paz; piperazinyl; polymer-supported; rat liver microsomes; room temperature; rt; single node heating in a microwave oven; transepithelial electrical resistance; triethylamine; triethyleneglycol; washed platelet assay.

MeSH terms

  • Animals
  • Molecular Structure
  • Nicotinic Acids / chemical synthesis
  • Nicotinic Acids / chemistry
  • Nicotinic Acids / pharmacology*
  • Purinergic P2Y Receptor Antagonists / chemical synthesis
  • Purinergic P2Y Receptor Antagonists / chemistry
  • Purinergic P2Y Receptor Antagonists / pharmacology*
  • Rats
  • Receptors, Purinergic P2Y12 / metabolism*
  • Structure-Activity Relationship
  • Urea / analogs & derivatives*
  • Urea / chemical synthesis
  • Urea / chemistry
  • Urea / pharmacology

Substances

  • Nicotinic Acids
  • Purinergic P2Y Receptor Antagonists
  • Receptors, Purinergic P2Y12
  • ethyl 6-aminonicotinate sulfonylurea
  • Urea