Nitrogen Arylation for Macrocyclization of Unprotected Peptides

We describe an efficient and mild method for the synthesis of macrocyclic peptides via nitrogen arylation from unprotected precursors. Various electrophiles and lysine-based nucleophiles were investigated and showed high-yielding product formation, even for a macrocyclization scan with 14 variants....

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Veröffentlicht in:Journal of the American Chemical Society 2016-07, Vol.138 (27), p.8340-8343
Hauptverfasser: Lautrette, Guillaume, Touti, Fayçal, Lee, Hong Geun, Dai, Peng, Pentelute, Bradley L
Format: Artikel
Sprache:eng
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Zusammenfassung:We describe an efficient and mild method for the synthesis of macrocyclic peptides via nitrogen arylation from unprotected precursors. Various electrophiles and lysine-based nucleophiles were investigated and showed high-yielding product formation, even for a macrocyclization scan with 14 variants. We found that nitrogen-linked aryl products were more stable to base and oxidation when compared to thiol arylated species, thereby highlighting the utility of this methodology. Finally, N-aryl macrocyclization was performed on a p53 peptide inhibitor of MDM2 and resulted in identification of a nanomolar binder with improved proteolytic stability and cell permeability.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.6b03757