Chemoselective and Diastereoselective Synthesis of C-Aryl Nucleoside Analogues by Nickel-Catalyzed Cross-Coupling of Furanosyl Acetates with Aryl Iodides

Angew Chem Int Ed Engl. 2022 Jan 3;61(1):e202110391. doi: 10.1002/anie.202110391. Epub 2021 Nov 23.

Abstract

Canonical nucleosides are vulnerable to enzymatic and chemical degradation, yet their stable mimics-C-aryl nucleosides-have demonstrated potential utility in medicinal chemistry, chemical biology, and synthetic biology, although current synthetic methods remain limited in terms of scope and selectivity. Herein, we report a cross-electrophile coupling to prepare C-aryl nucleoside analogues from readily available furanosyl acetates and aryl iodides. This nickel-catalyzed modular approach is characterized by mild reaction conditions, broad substrate scope, excellent β-selectivity, and high functional-group compatibility. The exclusive chemoselectivity with respect to the aryl iodide enables efficient preparation of a variety of C-aryl halide furanosides suitable for various downstream transformations. The practicality of this transformation is demonstrated through the synthesis of a potent analogue of a naturally occurring NF-κB activator.

Keywords: arylation; nucleoside analogues; radical reactions; reductive cross-coupling; synthetic methods.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acetates / chemistry*
  • Catalysis
  • Furans / chemistry*
  • Hydrocarbons, Iodinated / chemistry*
  • Molecular Structure
  • Nickel / chemistry*
  • Nucleosides / chemical synthesis*
  • Nucleosides / chemistry
  • Stereoisomerism

Substances

  • Acetates
  • Furans
  • Hydrocarbons, Iodinated
  • Nucleosides
  • Nickel