Characterization of the metabolic activation of hepatitis C virus nucleoside inhibitor beta-D-2'-Deoxy-2'-fluoro-2'-C-methylcytidine (PSI-6130) and identification of a novel active 5'-triphosphate species

J Biol Chem. 2007 Oct 12;282(41):29812-20. doi: 10.1074/jbc.M705274200. Epub 2007 Aug 13.

Abstract

beta-D-2'-Deoxy-2'-fluoro-2'-C-methylcytidine (PSI-6130) is a potent inhibitor of hepatitis C virus (HCV) replication in the subgenomic HCV replicon system, and its corresponding 5'-triphosphate is a potent inhibitor of the HCV RNA polymerase in vitro. In this study the formation of PSI-6130-triphosphate was characterized in primary human hepatocytes. PSI-6130 and its 5'-phosphorylated derivatives were identified, and the intracellular concentrations were determined. In addition, the deaminated derivative of PSI-6130, beta-d-2'-deoxy-2'-fluoro-2'-C-methyluridine (RO2433, PSI-6026) and its corresponding phosphorylated metabolites were identified in human hepatocytes after incubation with PSI-6130. The formation of the 5'-triphosphate (TP) of PSI-6130 (PSI-6130-TP) and RO2433 (RO2433-TP) increased with time and reached steady state levels at 48 h. The formation of both PSI-6130-TP and RO2433-TP demonstrated a linear relationship with the extracellular concentrations of PSI-6130 up to 100 mum, suggesting a high capacity of human hepatocytes to generate the two triphosphates. The mean half-lives of PSI-6130-TP and RO2433-TP were 4.7 and 38 h, respectively. RO2433-TP also inhibited RNA synthesis by the native HCV replicase isolated from HCV replicon cells and the recombinant HCV polymerase NS5B with potencies comparable with those of PSI-6130-TP. Incorporation of RO2433-5'-monophosphate (MP) into nascent RNA by NS5B led to chain termination similar to that of PSI-6130-MP. These results demonstrate that PSI-6130 is metabolized to two pharmacologically active species in primary human hepatocytes.

MeSH terms

  • Antiviral Agents / pharmacology*
  • Cells, Cultured
  • Chromatography, High Pressure Liquid
  • DNA-Directed RNA Polymerases / metabolism
  • Deoxycytidine / analogs & derivatives*
  • Deoxycytidine / pharmacology
  • Hepacivirus / enzymology
  • Hepacivirus / metabolism*
  • Hepatocytes / metabolism
  • Humans
  • Inhibitory Concentration 50
  • Models, Biological
  • Models, Chemical
  • Phosphates / chemistry
  • Phosphorylation
  • RNA-Dependent RNA Polymerase / metabolism
  • Virus Replication

Substances

  • Antiviral Agents
  • Phosphates
  • 2'-deoxy-2'-fluoro-2'-C-methylcytidine
  • Deoxycytidine
  • RNA-Dependent RNA Polymerase
  • DNA-Directed RNA Polymerases