Elucidating the Role of B-Site Cations toward CO 2 Reduction in Perovskite-Based Solid Oxide Electrolysis Cells
Elucidating the Role of B-Site Cations toward CO 2 Reduction in Perovskite-Based Solid Oxide Electrolysis Cells
复制标题
阐明 B 位阳离子对基于钙钛矿的固体氧化物电解池中 CO 2 还原的作用
DOI：
10.1149/1945-7111/ac5e9b
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发表时间：
2022
影响因子：
3.9
通讯作者：
Nikolla, Eranda
中科院分区：
文献类型：
--
作者：
Tezel, Elif;Guo, Dezhou;Whitten, Ariel;Yarema, Genevieve;Freire, Maikon;Denecke, Reinhard;McEwen, Jean-Sabin;Nikolla, Eranda
固体氧化物电解槽（SOECs）是一种将CO2或CO2和H2O混合流选择性电化学转化为CO和H2等高能产物的新型电解槽。然而，这些系统受到现有技术的Ni基阴极电催化剂的差的氧化还原稳定性的限制。由于其良好的氧化还原性能，混合离子电子导电（MIEC）氧化物已被认为是有前途的替代品。然而，需要改进基于MIEC的SOEC电催化剂的电化学性能，并且需要了解支配其活性的因素。本文研究了B位3d金属阳离子（Cr，Fe，Co，Ni）对LaBO3钙钛矿CO2电化学还原活性的影响。结果表明，它们的电化学性能与B位阳离子的性质密切相关，其变化趋势为LaFeO3> LaCoO3> LaNiO3> LaCrO3.在这些钙钛矿中，LaNiO 3是最不稳定的，并且在电化学条件下分解。原位表征和从头算理论计算表明，B位阳离子的性质和表面氧空位的存在影响了CO2吸附和还原的能量学.这些研究提供了重要的基本见解，对设计方法，以提高性能的MIEC为基础的SOEC阴极CO2电还原。
Solid oxide electrolysis cells (SOECs) are promising for the selective electrochemical conversion of CO 2, or mixed streams of CO 2 and H 2 O, into high energy products such as CO and H 2. However, these systems are limited by the poor redox stability of the state-of-the-art Ni-based cathode electrocatalysts. Due to their favorable redox properties, mixed ionic-electronic conducting (MIEC) oxides have been considered as promising alternatives. However, improvement of the electrochemical performance of MIEC-based SOEC electrocatalysts is needed and requires an understanding of the factors that govern their activity. Herein, we investigate the effect of B-site 3d metal cations (Cr, Fe, Co, Ni) of LaBO 3 perovskites on their CO 2 electrochemical reduction activity in SOECs. We find that their electrochemical performance is highly dependent on the nature of the B-site cation and trends as LaFeO 3> LaCoO 3> LaNiO 3> LaCrO 3. Among these perovskites, LaNiO 3 is the least stable and decomposes under electrochemical conditions. In situ characterization and ab initio theoretical calculations suggest that both the nature of the B-site cation and the presence of oxygen surface vacancies impact the energetics of CO 2 adsorption and reduction. These studies provide fundamental insights critical toward devising ways to improve the performance of MIEC-based SOEC cathodes for CO 2 electroreduction.