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Selective high-temperature CO2 electrolysis enabled by oxidized carbon intermediates

Author

Listed:
  • Theis L. Skafte

    (Technical University of Denmark
    Stanford University
    SLAC National Accelerator Laboratory
    Haldor Topsoe A/S)

  • Zixuan Guan

    (Stanford University)

  • Michael L. Machala

    (Stanford University)

  • Chirranjeevi B. Gopal

    (Stanford University)

  • Matteo Monti

    (Stanford University)

  • Lev Martinez

    (Technical University of Denmark)

  • Eugen Stamate

    (Technical University of Denmark)

  • Simone Sanna

    (Technical University of Denmark)

  • Jose A. Garrido Torres

    (SLAC National Accelerator Laboratory)

  • Ethan J. Crumlin

    (Lawrence Berkeley National Laboratory)

  • Max García-Melchor

    (Trinity College)

  • Michal Bajdich

    (SLAC National Accelerator Laboratory)

  • William C. Chueh

    (Stanford University)

  • Christopher Graves

    (Technical University of Denmark
    Stanford University
    SLAC National Accelerator Laboratory)

Abstract

High-temperature CO2 electrolysers offer exceptionally efficient storage of renewable electricity in the form of CO and other chemical fuels, but conventional electrodes catalyse destructive carbon deposition. Ceria catalysts are known carbon inhibitors for fuel cell (oxidation) reactions; however, for more severe electrolysis (reduction) conditions, catalyst design strategies remain unclear. Here we establish the inhibition mechanism on ceria and show selective CO2 to CO conversion well beyond the thermodynamic carbon deposition threshold. Operando X-ray photoelectron spectroscopy during CO2 electrolysis—using thin-film model electrodes consisting of samarium-doped ceria, nickel and/or yttria-stabilized zirconia—together with density functional theory modelling, reveal the crucial role of oxidized carbon intermediates in preventing carbon build-up. Using these insights, we demonstrate stable electrochemical CO2 reduction with a scaled-up 16 cm2 ceria-based solid-oxide cell under conditions that rapidly destroy a nickel-based cell, leading to substantially improved device lifetime.

Suggested Citation

  • Theis L. Skafte & Zixuan Guan & Michael L. Machala & Chirranjeevi B. Gopal & Matteo Monti & Lev Martinez & Eugen Stamate & Simone Sanna & Jose A. Garrido Torres & Ethan J. Crumlin & Max García-Melchor, 2019. "Selective high-temperature CO2 electrolysis enabled by oxidized carbon intermediates," Nature Energy, Nature, vol. 4(10), pages 846-855, October.
    • Handle: RePEc:nat:natene:v:4:y:2019:i:10:d:10.1038_s41560-019-0457-4
    DOI: 10.1038/s41560-019-0457-4
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    Cited by:

    1. Castle, Jennifer L. & Hendry, David F., 2024. "Five sensitive intervention points to achieve climate neutrality by 2050, illustrated by the UK," Renewable Energy, Elsevier, vol. 226(C).

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