Selective high-temperature CO2 electrolysis enabled by oxidized carbon intermediates

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, Michal Bajdich (), William C. Chueh () and Christopher Graves ()
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Theis L. Skafte: Technical University of Denmark
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

Nature Energy, 2019, vol. 4, issue 10, 846-855

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41560-019-0457-4

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