The application of solid oxide electrolysis cells (SOECs) for high-temperature CO reduction reaction (CORR) is constrained by the electrochemical activity and stability of the cathode materials. In this study, a series of iron-based perovskite oxides, designed by systematically varying A-site configurational entropy, are investigated as cathode materials for the CORR. Experimental results reveal that these high-entropy materials, derived from LaSrFeO (LSF), exhibit high electrocatalytic activity and durability. Notably, the SOEC with LaSrPrBaCaFeO (LSPBCF) cathode achieves a remarkable current density of 2.14 A cm at 800 °C and 1.5 V, maintaining excellent stability over 120 h of operation with negligible fluctuations. Density functional theory (DFT) calculations further unveil the electronic structure modulation mechanism of the high-entropy material, revealing that A-site entropy engineering could enhance CO adsorption and activation by reducing the oxygen vacancy formation energy. This study underscores the potential of entropy engineering to improve the electrocatalytic performance and stability of other energy conversion systems.
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