Targeting the Src Homology 2 (SH2) Domain of Signal Transducer and Activator of Transcription 6 (STAT6) with Cell-Permeable, Phosphatase-Stable Phosphopeptide Mimics Potently Inhibits Tyr641 Phosphorylation and Transcriptional Activity

J Med Chem. 2015 Nov 25;58(22):8970-84. doi: 10.1021/acs.jmedchem.5b01321. Epub 2015 Nov 9.

Abstract

Signal transducer and activator of transcription 6 (STAT6) transmits signals from cytokines IL-4 and IL-13 and is activated in allergic airway disease. We are developing phosphopeptide mimetics targeting the SH2 domain of STAT6 to block recruitment to phosphotyrosine residues on IL-4 or IL-13 receptors and subsequent Tyr641 phosphorylation to inhibit the expression of genes contributing to asthma. Structure-affinity relationship studies showed that phosphopeptides based on Tyr631 from IL-4Rα bind with weak affinity to STAT6, whereas replacing the pY+3 residue with simple aryl and alkyl amides resulted in affinities in the mid to low nM range. A set of phosphatase-stable, cell-permeable prodrug analogues inhibited cytokine-stimulated STAT6 phosphorylation in both Beas-2B human airway cells and primary mouse T-lymphocytes at concentrations as low as 100 nM. IL-13-stimulated expression of CCL26 (eotaxin-3) was inhibited in a dose-dependent manner, demonstrating that targeting the SH2 domain blocks both phosphorylation and transcriptional activity of STAT6.

Publication types

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

MeSH terms

  • Animals
  • Asthma / genetics
  • CD4-Positive T-Lymphocytes / drug effects
  • Cell Line
  • Dose-Response Relationship, Drug
  • Gene Expression Regulation / drug effects
  • Interleukin-13 / biosynthesis
  • Interleukin-4 / biosynthesis
  • Mice
  • Mice, Inbred C57BL
  • Models, Molecular
  • Phosphopeptides / pharmacology*
  • Phosphoric Monoester Hydrolases / chemistry
  • Phosphoric Monoester Hydrolases / metabolism
  • Phosphorylation
  • Prodrugs
  • Rats
  • Receptors, Interleukin-3 / drug effects
  • Receptors, Interleukin-4 / drug effects
  • STAT6 Transcription Factor / drug effects*
  • Structure-Activity Relationship
  • Transcriptional Activation / drug effects
  • Tyrosine / chemistry
  • Tyrosine / metabolism
  • src Homology Domains / drug effects*

Substances

  • Interleukin-13
  • Phosphopeptides
  • Prodrugs
  • Receptors, Interleukin-3
  • Receptors, Interleukin-4
  • STAT6 Transcription Factor
  • Interleukin-4
  • Tyrosine
  • Phosphoric Monoester Hydrolases