Synthesis and Diversification of Macrocyclic Alkynediyl Sulfide Peptides

Chemistry. 2020 Nov 17;26(64):14575-14579. doi: 10.1002/chem.202003655. Epub 2020 Oct 6.

Abstract

The synthesis of rare macrocyclic alkynediyl sulfides by a Cu-catalyzed Csp -S cross-coupling is presented. The catalytic protocol (Cu(MeCN)4 PF6 /dtbbpy) promotes macrocyclization of peptides, dipeptides and tripeptides at ambient temperature (14 examples, 23→73 % yields) via thiols and bromoalkynes, and is chemoselective with regards to terminal alkynes. Importantly, the underexplored alkynediyl sulfide functionality incorporates a rigidifying structural element and opens new opportunities for diversification of macrocyclic frameworks through S oxidation, halide addition and azide-alkyne cycloaddition chemistries to integrate sulfones, halides or valuable fluorophores (7 examples, 37→92 % yields).

Keywords: alkynyl sulfides; copper catalysis; cycloaddition; macrocycles; peptides.

MeSH terms

  • Alkynes / chemistry
  • Azides*
  • Catalysis
  • Coordination Complexes / chemistry*
  • Copper*
  • Molecular Structure
  • Peptides / chemistry*
  • Sulfides / chemistry*

Substances

  • Alkynes
  • Azides
  • Coordination Complexes
  • Peptides
  • Sulfides
  • Copper