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Electrolysis03:00

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In a galvanic cell, the electrical work is done by a redox system on its surroundings as electrons produced by the spontaneous redox reactions are transferred through an external circuit. Alternatively, an external circuit does work on a redox system by imposing a voltage sufficient to drive an otherwise nonspontaneous reaction in a process known as electrolysis. For instance, recharging a battery involves the use of an external power source to drive the spontaneous (discharge) cell reaction in...
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Local Proton Source in Electrocatalytic CO2 Reduction with [Mn(bpy-R)(CO)3 Br] Complexes.

Federico Franco1, Claudio Cometto1,2, Luca Nencini1

  • 1Department of Chemistry and NIS, University of Turin, Via P. Giuria 7, 10125, Turin, Italy.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|January 21, 2017
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Summary
This summary is machine-generated.

This study explores manganese catalysts for electrochemical CO2 reduction. Catalyst selectivity is highly sensitive to acid strength, influencing product formation and revealing unique reaction pathways.

Keywords:
carbon dioxidedensity functional calculationselectrocatalysiselectrochemistrymanganese

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Area of Science:

  • Inorganic Chemistry
  • Electrochemistry
  • Catalysis

Background:

  • Manganese complexes are investigated for CO2 electroreduction.
  • Understanding the influence of proton sources on catalytic mechanisms is crucial.

Purpose of the Study:

  • To detail the electrochemical behavior and catalytic performance of fac-[Mn(pdbpy)(CO)3 Br] for CO2 reduction.
  • To explore the impact of varying proton sources (water, TFE, phenol) on CO2 electroreduction selectivity.
  • To compare the catalytic activity with a newly synthesized manganese complex, fac-[Mn(ptbpy)(CO)3 Br].

Main Methods:

  • Preparative-scale electrolysis at -1.5 V vs SCE in CO2-saturated acetonitrile.
  • Detailed spectroelectrochemical analysis (IR and UV/Vis) under inert and CO2 atmospheres.
  • Comparative investigation of two related manganese catalysts with different ligand structures.

Main Results:

  • Electrocatalytic CO2 reduction selectivity is highly sensitive to acid strength, affecting CO and formate yields.
  • The manganese complex (1) exhibits suppressed dimer formation and an atypical reduction mechanism.
  • Spectroscopic evidence confirms manganese hydride formation, indicating diverse electrocatalytic pathways.
  • A second manganese complex (2) provides insights into the role of local proton sources.

Conclusions:

  • The study elucidates the complex electrocatalytic CO2 reduction mechanism of manganese complexes.
  • Acid strength and ligand design significantly influence catalyst performance and reaction pathways.
  • The findings contribute to the development of efficient catalysts for CO2 conversion.