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Functionally Graded Infiltration Triggering Ultrahigh Electrolytic Current in Robust Reversible Solid Oxide Cells
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DOI：10.1002/sstr.202300447.png)
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The reversible solid oxide cell (ReSOC) offers the dual capability to store electricity as chemical fuels and convert fuels to electricity, thereby enabling carbon neutral cycling. The nickel-cermet fuel electrode exhibits high electrocatalytic activity for redox reactions while being particularly vulnerable to carbon deposition and nickel coarsening, especially at high current densities. Herein, a novel approach involving a graded infiltration onto a dendritic Ni-YSZ (yttria-stabilized zirconia) skeleton with Pr6O11 nanoparticles/films is presented, demonstrating remarkable electrolytic current and coke tolerance in CO-CO2 conversion. At 800 degrees C, the current densities achieve approximately -2.0 and +2.0 A cm(-2) under 1.3 and 0.6 V, respectively, showcasing robust cycling stability switching between two operational modes within 20 cycles. Notably, the attained electrolytic current density reaches an unprecedented -3.06 A cm(-2) under 1.6 V. Furthermore, the button cell runs smoothly at ultrahigh electrolytic current densities ranging from -0.5 to -3.0 A cm(-2) for nearly 270 h. The mechanism of high-performance CO2 reduction is elucidated by in/ex situ experimental characterizations and theoretical calculations. These results indicate the viability of employing Ni-YSZ-supported ReSOC for stable renewable electricity storage at previously unattainable reaction rates, and have implications for fundamental understanding of designing robust ReSOC based on the nickel-cermet fuel electrode.
Keyword:
CO-CO2 conversion
density functional theory calculations
graded infiltration
reversible solid oxide cells
ultrahigh current density
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Enhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures.png)
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