Metallaphotoredox-enabled deoxygenative arylation of alcohols

Nature. 2021 Oct;598(7881):451-456. doi: 10.1038/s41586-021-03920-6. Epub 2021 Aug 31.

Abstract

Metal-catalysed cross-couplings are a mainstay of organic synthesis and are widely used for the formation of C-C bonds, particularly in the production of unsaturated scaffolds1. However, alkyl cross-couplings using native sp3-hybridized functional groups such as alcohols remain relatively underdeveloped2. In particular, a robust and general method for the direct deoxygenative coupling of alcohols would have major implications for the field of organic synthesis. A general method for the direct deoxygenative cross-coupling of free alcohols must overcome several challenges, most notably the in situ cleavage of strong C-O bonds3, but would allow access to the vast collection of commercially available, structurally diverse alcohols as coupling partners4. We report herein a metallaphotoredox-based cross-coupling platform in which free alcohols are activated in situ by N-heterocyclic carbene salts for carbon-carbon bond formation with aryl halide coupling partners. This method is mild, robust, selective and most importantly, capable of accommodating a wide range of primary, secondary and tertiary alcohols as well as pharmaceutically relevant aryl and heteroaryl bromides and chlorides. The power of the transformation has been demonstrated in a number of complex settings, including the late-stage functionalization of Taxol and a modular synthesis of Januvia, an antidiabetic medication. This technology represents a general strategy for the merger of in situ alcohol activation with transition metal catalysis.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Alcohols / chemistry*
  • Bromides / chemistry*
  • Carbon / chemistry*
  • Catalysis
  • Chlorides / chemistry*
  • Metals / chemistry*
  • Methane / analogs & derivatives
  • Methane / chemistry
  • Nitrogen / chemistry
  • Oxidation-Reduction
  • Oxygen / chemistry*
  • Paclitaxel / chemistry
  • Photochemistry*
  • Simvastatin / chemical synthesis
  • Simvastatin / chemistry

Substances

  • Alcohols
  • Bromides
  • Chlorides
  • Metals
  • carbene
  • Carbon
  • Simvastatin
  • Nitrogen
  • Methane
  • Paclitaxel
  • Oxygen