Mechanistic Insights into the Electrochemical Reduction of CO2 Catalyzed
by Iron Cyclopentadienone Complexes
Posted on 2018-09-20 - 17:43
In
a previous paper we have demonstrated that the easily-synthesized
class of iron(0) cyclopentadienone complexes constitutes a promising
catalyst platform for the electrochemical conversion of CO2 to CO and H2O. One of the unusual features of these catalysts
is that catalysis proceeds efficiently in aprotic electrolytes in
the absence of acidic additives. Herein we present a detailed study
of the underlying catalytic mechanisms. Using a combination of FTIR
spectroelectrochemistry, DFT calculations, and nonelectrochemical
control experiments, we have identified a number of catalytic intermediates
including the active species and the product of catalyst deactivation.
On the basis of these insights, we have carried out digital simulations
in order to decipher the voltammetric profiles of the iron(0) cyclopentadienones.
Further control experiments revealed that the anodic oxidation of
the electrolyte constitutes the terminal proton source for the formation
of CO and H2O. Taken together, our results suggest a competition
between two coexisting catalytic pathways, one of which proceeds via
a hitherto unknown Fe–Fe dimer as an active species.
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Oberem, Elisabeth; Roesel, Arend F.; Rosas-Hernández, Alonso; Kull, Tobias; Fischer, Steffen; Spannenberg, Anke; et al. (2018). Mechanistic Insights into the Electrochemical Reduction of CO2 Catalyzed
by Iron Cyclopentadienone Complexes. ACS Publications. Collection. https://doi.org/10.1021/acs.organomet.8b00517
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AUTHORS (11)
EO
Elisabeth Oberem
AR
Arend F. Roesel
AR
Alonso Rosas-Hernández
TK
Tobias Kull
SF
Steffen Fischer
AS
Anke Spannenberg
HJ
Henrik Junge
MB
Matthias Beller
RL
Ralf Ludwig
MR
Michael Roemelt
RF
Robert Francke
KEYWORDS
electrochemical conversioncontrol experimentscyclopentadienoneanodic oxidationCO 2Iron Cyclopentadienone ComplexesElectrochemical Reductionacidic additivesMechanistic Insightsterminal proton sourcevoltammetric profilesnonelectrochemical control experimentsH 2 Ocatalyst deactivationcatalysis proceedsFTIR spectroelectrochemistryaprotic electrolyteseasily-synthesized classcatalyst platformspeciesDFT calculationsCO 2 Catalyzed