First principles calculation and experimental study of Ln0.125Sr0.875Co0.875Ta0.125O3-δ(Ln = La, Sm, and Nd) as potential cathode materials for intermediate-temperature solid oxide fuel cells

Solid oxide fuel cells (SOFCs), as important energy equipment, have excellent characteristics, including low pollution and high catalytic activity. The cathode, which is the key component of an SOFC, plays a vital role in practical applications. Herein, we study the properties of Ln0.125Sr0.875Co0.875Ta0.125O3-δ (Ln = La, Sm, and Nd, abbreviated as LSCT, SSCT, and NSCT, respectively) cathode materials both theoretically and experimentally. The conductivity of LnSCT gradually decreased with decreasing Ln3+ ionic radius. Density of states (DOS) analysis indicated that LSCT has the highest conductivity owing to the band center of Co 3d being closer to O 1s. Density functional theory (DFT) calculations showed that the SSCT sample has the lowest oxygen vacancy formation energy, which facilitated the formation of oxygen vacancies. The binding energy results show that SSCT and NSCT have relatively good structural stability compared to LSCT. The polarization impedance values of LSCT, SSCT, and NSCT at 700 °C are 0.105, 0.069, and 0.304 Ω cm2, respectively. The CO2 sensitivity of LSCT, SSCT, and NSCT was evaluated by calculating the CO2 adsorption energy and performing impedance tests under different CO2 concentrations. These results indicate that LSCT and SSCT have better CO2 tolerance than NSCT. At 700 °C, for Ln = La, Sm, and Nd, the maximum power of NiCu-SDC/SDC/LSGM/LnSCT electrolyte-supported fuel cell reached 430, 462, and 382 mW cm-2, respectively. These findings provide a reference for the future design and development of SOFCs cathode material.