Cobaloximes as functional models for hydrogenases. 2. Proton electroreduction catalyzed by difluoroborylbis(dimethylglyoximato)cobalt(II) complexes in organic media

Inorg Chem. 2007 Mar 5;46(5):1817-24. doi: 10.1021/ic061625m. Epub 2007 Feb 2.

Abstract

Cobaloximes are effective electrocatalysts for hydrogen evolution and thus functional models for hydrogenases. Among them, difluoroboryl-bridged complexes appear both to mediate proton electroreduction with low overpotentials and to be quite stable in acidic conditions. We report here a mechanistic study of [Co(dmgBF2)2L] (dmg2- = dimethylglyoximato dianion; L = CH3CN or N,N-dimethylformamide) catalyzed proton electroreduction in organic solvents. Depending on the applied potential and the strength of the acid used, three different pathways for hydrogen production were identified and a unified mechanistic scheme involving cobalt(II) or cobalt(III) hydride species is proposed. As far as working potential and turnover frequency are concerned, [Co(dmgBF2)2(CH3CN)2], in the presence of p-cyanoanilinium cation in acetonitrile, is one of the best synthetic catalysts of the first-row transition-metal series for hydrogen evolution.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Catalysis
  • Cobalt / chemistry*
  • Electrochemistry
  • Hydrogen / chemistry
  • Hydrogen-Ion Concentration
  • Hydrogenase / chemistry*
  • Ligands
  • Molecular Conformation
  • Organometallic Compounds / chemistry*
  • Oxidation-Reduction
  • Oximes / chemistry*
  • Protons*
  • Solvents / chemistry

Substances

  • Ligands
  • Organometallic Compounds
  • Oximes
  • Protons
  • Solvents
  • Cobalt
  • Hydrogen
  • Hydrogenase