Importance of ligand bioactive conformation in the discovery of potent indole-diamide inhibitors of the hepatitis C virus NS5B

J Am Chem Soc. 2010 Nov 3;132(43):15204-12. doi: 10.1021/ja101358s.

Abstract

Significant advances have led to receptor induced-fit and conformational selection models for describing bimolecular recognition, but a more comprehensive view must evolve to also include ligand shape and conformational changes. Here, we describe an example where a ligand's "structural hinge" influences potency by inducing an "L-shape" bioactive conformation, and due to its solvent exposure in the complex, reasonable conformation-activity-relationships can be qualitatively attributed. From a ligand design perspective, this feature was exploited by successful linker hopping to an alternate "structural hinge" that led to a new and promising chemical series which matched the ligand bioactive conformation and the pocket bioactive space. Using a combination of X-ray crystallography, NMR and modeling with support from binding-site resistance mutant studies and photoaffinity labeling experiments, we were able to derive inhibitor-polymerase complexes for various chemical series.

MeSH terms

  • Allosteric Regulation
  • Diamide / chemistry*
  • Diamide / metabolism
  • Diamide / pharmacology*
  • Drug Discovery*
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / metabolism
  • Enzyme Inhibitors / pharmacology
  • Hepacivirus*
  • Indoles / chemistry*
  • Inhibitory Concentration 50
  • Ligands
  • Models, Molecular
  • Molecular Conformation*
  • Viral Nonstructural Proteins / antagonists & inhibitors*
  • Viral Nonstructural Proteins / chemistry
  • Viral Nonstructural Proteins / metabolism

Substances

  • Enzyme Inhibitors
  • Indoles
  • Ligands
  • Viral Nonstructural Proteins
  • Diamide
  • NS-5 protein, hepatitis C virus