Zhang Nan, Zhang Wenyu, Wu Mengyu, Wang Rui, Gong Yansheng, Wang Huanwen, Jin Jun, Zhao Ling, He Beibei
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, 430074, China.
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, 430074, China; Shenzhen Research Institute, China University of Geosciences, Shenzhen, 518057, China.
J Colloid Interface Sci. 2025 Mar 15;682:70-79. doi: 10.1016/j.jcis.2024.11.161. Epub 2024 Nov 23.
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.
固体氧化物电解槽（SOEC）在高温CO还原反应（CORR）中的应用受到阴极材料电化学活性和稳定性的限制。在本研究中，通过系统改变A位构型熵设计了一系列铁基钙钛矿氧化物，作为CORR的阴极材料进行研究。实验结果表明，这些源自LaSrFeO（LSF）的高熵材料表现出高电催化活性和耐久性。值得注意的是，具有LaSrPrBaCaFeO（LSPBCF）阴极的SOEC在800℃和1.5V时实现了2.14A cm的显著电流密度，在120小时的运行中保持了优异的稳定性，波动可忽略不计。密度泛函理论（DFT）计算进一步揭示了高熵材料的电子结构调制机制，表明A位熵工程可以通过降低氧空位形成能来增强CO的吸附和活化。本研究强调了熵工程在改善其他能量转换系统的电催化性能和稳定性方面的潜力。
