Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.265
Publication date: 7th February 2022
Greenhouse gases have maintained the conditions on Earth habitable. Nonetheless, the
atmospheric level of these gases, in particular carbon dioxide (CO2), has increased considerably in
the latest years. One way to cope with this increase is by electrochemically reduce CO2 into other
building blocks or fuels. However, the kinetic inertness and the thermodynamic stability of this
molecule makes its activation rather difficult, requiring the use of catalysts. Molecular catalysts,
such as iron porphyrins, are among the most efficient, robust, and selective catalysts towards the
reduction of CO2 to CO, by also being optimal catalysts in both organic and aqueous solutions.1,2 In
order to consider the reduction of CO2 by iron porphyrins as an interesting path to re-use and take
advantage of a waste product, fundamental knowledge is a pre-requisite to better understand this
reaction, improve their performance and orient their selectivity.
Even if electrochemical methods have allowed the determination of kinetic parameters,3,4 a
complete picture of the mechanism is still missing due to the lack of spectroscopic evidence. By
coupling electrochemical techniques with X-Ray absorption spectroscopy, we aimed at obtaining
a complete view of the modifications undergone by the catalyst during electroreduction and
catalysis. In this context, we have recently developed a spectroelectrochemical set-up for in situ
CO2RR studies by iron porphyrins in organic media. We present here the spectral changes
observed at the pre-edge and XANES region. This has allowed to give insights on the structural
and electronic changes that occur at the iron center and its interactions with the CO2, proposing
some possible intermediate species which are crucial to describe the CO2 reduction mechanism.
References:
(1) Costentin, C.; Robert, M.; Savéant, J.-M.; Tatin, A. Proc Natl Acad Sci USA 2015, 112 (22), 6882–6886.
(2) Costentin, C.; Drouet, S.; Robert, M.; Savéant, J.-M. Science 2012, 338 (6103), 90–94.
(3) Bhugun, I.; Lexa, D.; Savéant, J.-M. J. Am. Chem. Soc. 1996, 118 (7), 1769–1776.
(4) Costentin, C.; Passard, G.; Robert, M.; Savéant, J.-M. J. Am. Chem. Soc. 2014, 136 (33), 11821–11829.
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