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Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon

Open access
Genovese, Chiara, Schuster, Manfred E., Gibson, Emma K., Gianolio, Diego, Posligua, Victor, Grau-Crespo, Ricardo, Cibin, Giannantonio, Wells, Peter P., Garai, Debi, Solokha, Vladyslav, Krick Calderon, Sandra, Velasco-Velez, Juan J., Ampelli, Claudio, Perathoner, Siglinda, Held, Georg, Centi, Gabriele, Arrigo, Rosa·2018·Nature Communications

Abstract

The carbon–carbon coupling via electrochemical reduction of carbon dioxide represents the biggest challenge for using this route as platform for chemicals synthesis. Here we show that nanostructured iron (III) oxyhydroxide on nitrogen-doped carbon enables high Faraday efficiency (97.4%) and selectivity to acetic acid (61%) at very-low potential (−0.5 V vs silver/silver chloride). Using a combination of electron microscopy, operando X-ray spectroscopy techniques and density functional theory simulations, we correlate the activity to acetic acid at this potential to the formation of nitrogen-coordinated iron (II) sites as single atoms or polyatomic species at the interface between iron oxyhydroxide and the nitrogen-doped carbon. The evolution of hydrogen is correlated to the formation of metallic iron and observed as dominant reaction path over iron oxyhydroxide on oxygen-doped carbon in the overall range of negative potential investigated, whereas over iron oxyhydroxide on nitrogen-doped carbon it becomes important only at more negative potentials.

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Metadata

Authors
Genovese, C., Schuster, M. E., Gibson, E. K., Gianolio, D., Posligua, V., Grau-Crespo, R., Cibin, G., Wells, P. P., Garai, D., Solokha, V., Krick Calderon, S., Velasco-Velez, J. J., Ampelli, C., Perathoner, S., Held, G., Centi, G., & Arrigo, R.
Venue
Nature Communications
Published
2018-03-05
Volume
9
Issue
1
Pages
935-935
ISSN
2041-1723 (ISSN-L)
OpenAlex
W2792126723
Cited by
258
References
3
FWCI
7.07
Type
journal article
Language
en
Open access
gold

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CoChat. (2026). Citation check: Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon. https://app.cochat.ai/papers/10.1038/s41467-018-03138-7
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Genovese, C., Schuster, M. E., Gibson, E. K., Gianolio, D., Posligua, V., Grau-Crespo, R., Cibin, G., Wells, P. P., Garai, D., Solokha, V., Krick Calderon, S., Velasco-Velez, J. J., Ampelli, C., Perathoner, S., Held, G., Centi, G., & Arrigo, R. (2018). Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon. Nature Communications. https://doi.org/10.1038/s41467-018-03138-7

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