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

Author

Listed:
  • Chiara Genovese

    (University of Messina)

  • Manfred E. Schuster

    (Johnson Matthey Technology Centre)

  • Emma K. Gibson

    (UK Catalysis Hub, Research Complex at Harwell (RCaH)
    Department of Chemistry, UCL)

  • Diego Gianolio

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus)

  • Victor Posligua

    (University of Reading)

  • Ricardo Grau-Crespo

    (University of Reading)

  • Giannantonio Cibin

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus)

  • Peter P. Wells

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus
    University of Southampton)

  • Debi Garai

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus)

  • Vladyslav Solokha

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus)

  • Sandra Krick Calderon

    (FAU Erlangen-Nürnberg)

  • Juan J. Velasco-Velez

    (Max-Planck Institut für Chemische Energiekonversion)

  • Claudio Ampelli

    (University of Messina)

  • Siglinda Perathoner

    (University of Messina)

  • Georg Held

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus
    University of Reading)

  • Gabriele Centi

    (Computer, Physical and Earth Sciences - University of Messina, ERIC aisbl and CASPE/INSTM, V.le F. Stagno d’Alcontres 31)

  • Rosa Arrigo

    (Diamond Light Source Ltd., Harwell Science and Innovation Campus
    University of Reading)

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.

Suggested Citation

  • Chiara Genovese & Manfred E. Schuster & Emma K. Gibson & Diego Gianolio & Victor Posligua & Ricardo Grau-Crespo & Giannantonio Cibin & Peter P. Wells & Debi Garai & Vladyslav Solokha & Sandra Krick Ca, 2018. "Operando spectroscopy study of the carbon dioxide electro-reduction by iron species on nitrogen-doped carbon," Nature Communications, Nature, vol. 9(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03138-7
    DOI: 10.1038/s41467-018-03138-7
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    Cited by:

    1. Ruiz-López, Estela & Gandara-Loe, Jesús & Baena-Moreno, Francisco & Reina, Tomas Ramirez & Odriozola, José Antonio, 2022. "Electrocatalytic CO2 conversion to C2 products: Catalysts design, market perspectives and techno-economic aspects," Renewable and Sustainable Energy Reviews, Elsevier, vol. 161(C).

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