Wang Chen, Zhu Yan, Ling Yihan, Gong Yansheng, Wang Rui, Wang Huanwen, Jin Jun, Zhao Ling, He Beibei
Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.
School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, China.
ACS Appl Mater Interfaces. 2023 Oct 4;15(39):45905-45914. doi: 10.1021/acsami.3c09913. Epub 2023 Sep 25.
Solid oxide electrolysis cells (SOECs) show great promise in converting CO to valuable products. However, their practicality for the CO reduction reaction (CORR) is restricted by sluggish kinetics and limited durability. Herein, we propose a novel medium-entropy perovskite, Sr(FeTiCrMnMo)O (SFTCMM), as a potential electrode material for symmetrical SOEC toward CORR. Experimental and theoretical results unveil that the configuration entropy of SFTCMM perovskites contributes to the strengthened metal 3d-O 2p hybridization and the reduced O 2p bond center. This variation of electronic structure benefits oxygen vacancy creation and diffusion as well as CO adsorption and activation and ultimately accelerates CORR and oxygen electrocatalysis kinetics. Notably, the SFTCMM-based symmetrical SOEC delivers an excellent current density of 1.50 A cm at 800 °C and 1.5 V, surpassing the prototype SrFeMoO (SFM, 1.04 A cm) and most of the state-of-the-art electrodes for symmetrical SOECs. Moreover, the SFTCMM-based symmetrical SOEC demonstrates stable CORR operation for 160 h.
固体氧化物电解槽（SOECs）在将CO转化为有价值的产品方面显示出巨大的潜力。然而，它们在CO还原反应（CORR）中的实用性受到缓慢动力学和有限耐久性的限制。在此，我们提出一种新型的中熵钙钛矿Sr(FeTiCrMnMo)O（SFTCMM），作为用于对称SOECs进行CORR的潜在电极材料。实验和理论结果表明，SFTCMM钙钛矿的组态熵有助于增强金属3d - O 2p杂化并降低O 2p键中心。这种电子结构的变化有利于氧空位的产生和扩散以及CO的吸附和活化，并最终加速CORR和氧电催化动力学。值得注意的是，基于SFTCMM的对称SOEC在800°C和1.5 V时提供了1.50 A cm的优异电流密度，超过了原型SrFeMoO（SFM，1.04 A cm）以及大多数用于对称SOECs的先进电极。此外，基于SFTCMM的对称SOEC在CORR操作中表现出160小时的稳定性。
