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Area of Science:

  • Electrochemistry
  • Catalysis
  • Materials Science

Background:

  • Molecular electrocatalysts are crucial for sustainable energy solutions.
  • Cobalt complexes show promise for carbon dioxide reduction.

Purpose of the Study:

  • To investigate the mechanism of CO2 reduction by a tetra-aza-macrocyclic Schiff base cobalt complex.
  • To understand the role of product binding in catalyst performance.

Main Methods:

  • Operando UV-vis spectroelectrochemistry
  • Cyclic voltammetry
  • Rotating disk voltammetry
  • Kinetic modeling

Main Results:

  • The cobalt complex catalyzes CO2 to CO reduction in wet acetonitrile.
  • A self-moderation mechanism was identified where CO reversibly binds to the active cobalt species.
  • Product inhibition by CO was observed but did not lead to irreversible deactivation.

Conclusions:

  • The [Co(N4H)(Cl)2]+ complex is a viable molecular platform for CO2 reduction.
  • Reversible product binding offers a design principle for next-generation cobalt catalysts.
  • Self-moderation influences catalytic efficiency and may facilitate subsequent CO activation.