Double Strain-Promoted Macrocyclization for the Rapid Selection of Cell-Active Stapled Peptides

Angew Chem Int Ed Engl. 2015 Dec 14;54(51):15410-3. doi: 10.1002/anie.201508416. Epub 2015 Nov 2.

Abstract

Peptide stapling is a method for designing macrocyclic alpha-helical inhibitors of protein-protein interactions. However, obtaining a cell-active inhibitor can require significant optimization. We report a novel stapling technique based on a double strain-promoted azide-alkyne reaction, and exploit its biocompatibility to accelerate the discovery of cell-active stapled peptides. As a proof of concept, MDM2-binding peptides were stapled in parallel, directly in cell culture medium in 96-well plates, and simultaneously evaluated in a p53 reporter assay. This in situ stapling/screening process gave an optimal candidate that showed improved proteolytic stability and nanomolar binding to MDM2 in subsequent biophysical assays. α-Helicity was confirmed by a crystal structure of the MDM2-peptide complex. This work introduces in situ stapling as a versatile biocompatible technique with many other potential high-throughput biological applications.

Keywords: bioorthogonal chemistry; click chemistry; macrocycles; peptide stapling; peptides.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Culture Media
  • Macrocyclic Compounds / chemistry*
  • Peptides / chemistry*
  • Protein Binding
  • Proto-Oncogene Proteins c-mdm2 / chemistry

Substances

  • Culture Media
  • Macrocyclic Compounds
  • Peptides
  • Proto-Oncogene Proteins c-mdm2