3-substituted indazoles as configurationally locked 4EGI-1 mimetics and inhibitors of the eIF4E/eIF4G interaction

Chembiochem. 2014 Mar 3;15(4):595-611. doi: 10.1002/cbic.201300723. Epub 2014 Jan 23.

Abstract

4EGI-1, the prototypic inhibitor of eIF4E/eIF4G interaction, was identified in a high-throughput screening of small-molecule libraries with the aid of a fluorescence polarization assay that measures inhibition of binding of an eIF4G-derived peptide to recombinant eIF4E. As such, the molecular probe 4EGI-1 has potential for the study of molecular mechanisms involved in human disorders characterized by loss of physiological restraints on translation initiation. A hit-to-lead optimization campaign was carried out to overcome the configurational instability in 4EGI-1, which stems from the E-to-Z isomerization of the hydrazone function. We identified compound 1 a, in which the labile hydrazone was incorporated into a rigid indazole scaffold, as a promising rigidified 4EGI-1 mimetic lead. In a structure-activity relationship study directed towards probing the structural latitude of this new chemotype as an inhibitor of eIF4E/eIF4G interaction and translation initiation we identified 1 d, an indazole-based 4EGI-1 mimetic, as a new and improved lead inhibitor of eIF4E/eIF4G interaction and a promising molecular probe candidate for elucidation of the role of cap-dependent translation initiation in a host of pathophysiological states.

Keywords: eIF4E/eIF4G interaction; inhibitors; molecular probes; protein-protein interactions; translation initiation.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cell Line, Tumor
  • Cell Proliferation / drug effects
  • Eukaryotic Initiation Factor-4E / antagonists & inhibitors
  • Eukaryotic Initiation Factor-4E / metabolism*
  • Eukaryotic Initiation Factor-4G / antagonists & inhibitors
  • Eukaryotic Initiation Factor-4G / metabolism*
  • Humans
  • Hydrazones / chemistry
  • Hydrazones / metabolism*
  • Hydrazones / pharmacology
  • Indazoles / chemical synthesis
  • Indazoles / chemistry*
  • Indazoles / pharmacology
  • Protein Binding
  • Protein Interaction Domains and Motifs / drug effects
  • Stereoisomerism
  • Structure-Activity Relationship
  • Thiazoles / chemistry
  • Thiazoles / metabolism*
  • Thiazoles / pharmacology

Substances

  • 4EGI-1 compound
  • Eukaryotic Initiation Factor-4E
  • Eukaryotic Initiation Factor-4G
  • Hydrazones
  • Indazoles
  • Thiazoles