Genovese, C;
Schuster, ME;
Gibson, E;
Gianolio, D;
Posligua, V;
Grau-Crespo, R;
Cibin, G;
... Arrigo, R; + view all
(2018)
Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon.
Nature Communications
, 9
, Article 935. 10.1038/s41467-018-03138-7.
Preview |
Text
s41467-018-03138-7.pdf - Published Version Download (2MB) | Preview |
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
| Type: | Article |
|---|---|
| Title: | Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41467-018-03138-7 |
| Publisher version: | https://doi.org/10.1038/s41467-018-03138-7 |
| Language: | English |
| Additional information: | Open Access: This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
| UCL classification: | UCL > Provost and Vice Provost Offices UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10067810 |
Archive Staff Only
 |
View Item |
