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Elucidating the Role of B-Site Cations toward CO2 Activation in Perovskite-Based Solid Oxide Electrolysis Cells


 Solid oxide electrolysis cells (SOECs) are promising systems for the selective electrochemical conversion of CO2, or mixed streams of CO2 and H2O, into high energy products, such as CO and H2. These products can be converted to fuels and chemicals using existing technologies. Although promising, state-of-the-art SOEC Ni-based cathode electrocatalysts are affected by poor redox stability leading to limited long-term performance. Due to their favorable redox properties, mixed ionic-electronic conducting (MIEC) oxides are promising alternatives to minimize these adverse effects. However, the electrochemical activities of MIECs are inferior to the Ni-based cathode electrocatalysts. Thus, improvement of the electrochemical performance of MIEC-based SOEC electrocatalysts is needed and requires an understanding of the factors that govern their activity. Herein, we investigate the effect of the B-site cations of LaBO3 perovskites on their electrochemical activity toward the reduction of CO2 in SOECs. We correlate changes in the B-site composition to the nature of adsorbed species and active sites on the oxide surfaces by integrating in situ CO2 Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFT) studies with density functional theory (DFT)-based calculations. These studies provide insights critical toward devising ways to improve the performance of MIEC-based SOEC cathodes for the electroreduction of CO2.