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Design of N-Benzoxaborole Benzofuran GSK8175-Optimization of Human Pharmacokinetics Inspired by Metabolites of a Failed Clinical HCV Inhibitor

J Med Chem. 2019 Apr 11;62(7):3254-3267. doi: 10.1021/acs.jmedchem.8b01719. Epub 2019 Mar 7.

Abstract

We previously described the discovery of GSK5852 (1), a non-nucleoside polymerase (NS5B) inhibitor of hepatitis C virus (HCV), in which an N-benzyl boronic acid was essential for potent antiviral activity. Unfortunately, facile benzylic oxidation resulted in a short plasma half-life (5 h) in human volunteers, and a backup program was initiated to remove metabolic liabilities associated with 1. Herein, we describe second-generation NS5B inhibitors including GSK8175 (49), a sulfonamide- N-benzoxaborole analog with low in vivo clearance across preclinical species and broad-spectrum activity against HCV replicons. An X-ray structure of NS5B protein cocrystallized with 49 revealed unique protein-inhibitor interactions mediated by an extensive network of ordered water molecules and the first evidence of boronate complex formation within the binding pocket. In clinical studies, 49 displayed a 60-63 h half-life and a robust decrease in viral RNA levels in HCV-infected patients, thereby validating our hypothesis that reducing benzylic oxidation would improve human pharmacokinetics and lower efficacious doses relative to 1.

MeSH terms

  • Animals
  • Antiviral Agents / chemistry
  • Antiviral Agents / pharmacokinetics
  • Antiviral Agents / pharmacology*
  • Boronic Acids / chemistry
  • Boronic Acids / pharmacokinetics
  • Boronic Acids / pharmacology*
  • Crystallography, X-Ray
  • Dogs
  • Drug Design*
  • Half-Life
  • Hepacivirus / drug effects*
  • Humans
  • Macaca fascicularis
  • Mice
  • Molecular Structure
  • Nucleic Acid Synthesis Inhibitors / chemistry
  • Nucleic Acid Synthesis Inhibitors / pharmacokinetics
  • Nucleic Acid Synthesis Inhibitors / pharmacology*
  • Rats

Substances

  • Antiviral Agents
  • Boronic Acids
  • GSK8175
  • Nucleic Acid Synthesis Inhibitors