Robust Cathode for Efficient CO<sub>2</sub> Electrolysis Driven by Entropy Engineering in Solid Oxide Electrolysis Cells
Meiting Yang, Shuai Liu, Xinran Shen, Ruijia Xu, Jiangyuan Feng, Zhixin Luo, Guangming Yang, Yu Liu, Ran Ran, Wei Zhou, Zongping Shao
Abstract
Herein, we introduce an innovative approach of entropy engineering to design high-performance and durable electrodes. A series of perovskite oxides with varying configurational entropy ( S config ) based on Pr 1/2 Ba 1/2 FeO 3−δ (PBF) matrix are synthesized, and their physicochemical properties and electrochemical performances in CO 2 reduction reaction process are explored via manipulating S config . Notably, a high-entropy perovskite, Pr 1/6 La 1/6 Sm 1/6 Ba 1/6 Sr 1/6 Ca 1/6 FeO 3−δ (PLSBSCF), with an S config of 1.79 R, exhibits significant lattice distortion due to homogeneous distributed A-site elements. It demonstrates a high concentration of oxygen vacancies, good CO 2 adsorption capability, and rapid O 2– /e – conductions. Compared to bare PBF perovskite, PLSBSCF offers a greater number of active sites for CO 2 RR, and the corresponding cell achieves remarkably high current densities of 2.86 A cm –2 at 850 °C (1.5 V) during direct CO 2 electrolysis, while maintaining good thermal stability and operational durability. Density Functional Theory calculations also confirm the good CO 2 reduction activity of PLSBSCF perovskite.