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Proton electroreduction catalyzed by cobaloximes: functional models for hydrogenases.

Mathieu Razavet1, Vincent Artero, Marc Fontecave

  • 1Laboratoire de Chimie et Biochimie des Centres Rédox Biologiques, UMR 5047 CEA/CNRS/Université Joseph Fourier, CEA-Grenoble, DRDC/CB, Bat K', 17 rue des Martyrs, 38054 Grenoble Cedex 09, France.

Inorganic Chemistry
|June 21, 2005
PubMed
Summary

Cobaloxime catalysts efficiently facilitate proton reduction in nonaqueous solvents. Modified ligands tune catalytic rates, demonstrating potential for hydrogen evolution applications.

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Area of Science:

  • Electrochemistry
  • Catalysis
  • Inorganic Chemistry

Background:

  • Cobaloximes are investigated as electrocatalysts for proton reduction.
  • Proton reduction is crucial for energy conversion technologies.
  • Nonaqueous solvents present unique challenges and opportunities for catalysis.

Purpose of the Study:

  • To evaluate cobaloximes as electrocatalysts for proton reduction in nonaqueous media.
  • To understand the influence of ligand substituents on catalytic activity.
  • To explore the mechanism of electrocatalyzed hydrogen evolution.

Main Methods:

  • Controlled-potential electrolysis was used to assess catalyst performance.
  • Cyclic voltammogram simulations were employed to determine kinetic parameters.

Related Experiment Videos

  • Systematic modification of axial pyridine and equatorial glyoxime ligands was performed.

    • Main Results:

    • The cobaloxime complex [Co(III)(dmgH)2pyCl] demonstrated efficient catalysis at moderate potentials (-0.90 V) in neutral conditions.
    • Over 100 turnovers were achieved without catalyst degradation.
    • Electron-donating substituents on the pyridine ligand increased the catalytic rate, correlating with Hammett coefficients.
    • BF2-bridged species also showed capability for electrocatalyzed hydrogen evolution.

    Conclusions:

    • Cobaloximes are promising electrocatalysts for proton reduction in nonaqueous solvents.
    • Ligand modification offers a route to tune and optimize catalytic efficiency.
    • The study provides insights into the mechanism of cobaloxime-catalyzed hydrogen evolution.