Site-Selective Functionalization of Carboranes at the Electron-Rich Boron Vertex: Photocatalytic B-C Coupling via a Carboranyl Cage Radical

Angew Chem Int Ed Engl. 2022 Sep 12;61(37):e202205672. doi: 10.1002/anie.202205672. Epub 2022 Jul 8.

Abstract

Functionalization of carboranes in a vertex-specific manner is a perennial challenge. Here, we report a photocatalytic B-C coupling for the selective functionalization of carboranes at the boron site which is most distal to carbon. This reaction was achieved by the photo-induced decarboxylation of carborane carboxylic acids to generate boron vertex-centered carboranyl radicals. Theoretical calculations also demonstrate that the reaction more easily occurs at the boron site bearing higher electron density owing to the lower energy barrier for a single-electron transfer to generate a carboranyl radical. By using this strategy, a number of functionalized carboranes could be accessed through alkylation, alkenylation, and heteroarylation under mild conditions. Moreover, both a highly efficient blue emitter with a solid-state luminous efficiency of 42 % and a drug candidate for boron neutron capture therapy (BNCT) containing targeting and fluorine units were obtained.

Keywords: Boron Chemistry; Boron-Cluster Materials; B−C Coupling; Carboranes; Carboranyl Radicals.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Boranes*
  • Boron
  • Boron Compounds / therapeutic use
  • Boron Neutron Capture Therapy*
  • Electrons

Substances

  • Boranes
  • Boron Compounds
  • Boron