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Optimal Stapling of a Helical Peptide‐Foldamer Hybrid Using a C‐Terminal 4‐Mercaptoproline Enhances Protein Surface Recognition and Cellular Activity

2025/03/11 by Maxime Neuville, Mathieu Bourgeais, Jérémie Buratto +11 · 1 voice
Biochemistry, Genetics and Molecular Biology · #Cancer-related gene regulation #Chemical Synthesis and Analysis #Glycosylation and Glycoproteins Research

paper · pdf · doi:10.1002/chem.202403330

openalex publication_date 2025/03/11 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/30

Abstract

Structural analysis of a co-crystal of a helically-folded peptide-foldamer hybrid in complex with hDM2 E3 ubiquitin ligase, revealed a unique orientation for the C-terminal proline with the pyrrolidine ring pointing backwards in the sequence, and suggested new opportunities for macrocyclization. In particular, we found that the C-terminal prolyl residue could be replaced by its (2S,4S)-4-mercaptoprolyl analogue for optimal bisthioether crosslinking with a cysteine residue installed at position 4 in the sequence. The resulting i,i+7 stapled peptide-foldamer is a high-affinity binder to hDM2, is cell permeable and restores the p53 signalling pathway in p53wt cancer cells. The co-crystal structure of hDM2 and the stapled peptide-foldamer hybrid was determined at 1.84 Å, fully validating the original design and further highlighting the potential of cis-4-mercaptoproline in the context of peptide and foldamer stapling.

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