Intramolecular redox-active ligand-to-substrate single-electron transfer: radical reactivity with a palladium(II) complex

J Am Chem Soc. 2014 Aug 20;136(33):11574-7. doi: 10.1021/ja502164f. Epub 2014 Jun 17.

Abstract

Coordination of the redox-active tridentate NNO ligand L(H2) to Pd(II) yields the paramagnetic iminobenzosemiquinonato complex 3. Single-electron reduction of 3 yields diamagnetic amidophenolato complex 4, capable of activating aliphatic azide 5. Experimental and computational studies suggest a redox-noninnocent pathway wherein the redox-active ligand facilitates intramolecular ligand-to-substrate single-electron transfer to generate an open-shell singlet "nitrene-substrate radical, ligand radical", enabling subsequent radical-type C-H amination reactivity with Pd(II).

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Electrons*
  • Free Radicals / chemistry
  • Ligands
  • Molecular Conformation
  • Organometallic Compounds / chemistry*
  • Oxidation-Reduction
  • Palladium / chemistry*
  • Quantum Theory
  • Stereoisomerism

Substances

  • Free Radicals
  • Ligands
  • Organometallic Compounds
  • Palladium