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Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon.
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.
Afiliación
  • Genovese C; Department of Chemical, Biological Pharmaceutical and Environmental Sciences, University of Messina, ERIC aisbl and CASPE/INSTM, V.le F. Stagno d'Alcontres, 31, 98166, Messina, Italy.
  • Schuster ME; Johnson Matthey Technology Centre, Reading, RG4 9NH, UK.
  • Gibson EK; UK Catalysis Hub, Research Complex at Harwell (RCaH), Harwell, Oxforshire, OX11 0FA, UK.
  • Gianolio D; Department of Chemistry, UCL, 20 Gordon Street, London, WC1 0AJ, UK.
  • Posligua V; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
  • Grau-Crespo R; Department of Chemistry, University of Reading, Whiteknights, Reading, RG6 6AD, UK.
  • Cibin G; Department of Chemistry, University of Reading, Whiteknights, Reading, RG6 6AD, UK.
  • Wells PP; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
  • Garai D; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
  • Solokha V; School of Chemistry, University of Southampton, Southampton, SO17 1BJ, UK.
  • Krick Calderon S; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
  • Velasco-Velez JJ; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
  • Ampelli C; FAU Erlangen-Nürnberg, Egerland Str. 3, 91058, Erlangen, Germany.
  • Perathoner S; Max-Planck Institut für Chemische Energiekonversion, Stiftstr. 34 - 36, 45470, Mülheim an der Ruhr, Germany.
  • Held G; Department of Chemical, Biological Pharmaceutical and Environmental Sciences, University of Messina, ERIC aisbl and CASPE/INSTM, V.le F. Stagno d'Alcontres, 31, 98166, Messina, Italy.
  • Centi G; Department of Chemical, Biological Pharmaceutical and Environmental Sciences, University of Messina, ERIC aisbl and CASPE/INSTM, V.le F. Stagno d'Alcontres, 31, 98166, Messina, Italy.
  • Arrigo R; Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, OX11 0DE, UK.
Nat Commun ; 9(1): 935, 2018 03 05.
Article en En | MEDLINE | ID: mdl-29507285
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.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2018 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2018 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Reino Unido