Yang Xiaoxia, Sun Wang, Ma Minjian, Xu Chunming, Ren Rongzheng, Qiao Jinshuo, Wang Zhenhua, Li Zesheng, Zhen Shuying, Sun Kening
Beijing Key Laboratory for Chemical Power Source and Green Catalysis, Beijing Institute of Technology, Beijing 100081, People's Republic of China.
Key Laboratory of Cluster Science of Ministry of Education, Beijing Institute of Technology, Beijing 100081, People's Republic of China.
ACS Appl Mater Interfaces. 2021 May 5;13(17):20060-20069. doi: 10.1021/acsami.1c02146. Epub 2021 Apr 22.
The design of active cathode catalysts, with abundant active sites and outstanding catalytic activity for CO electroreduction, is important to promote the development of solid oxide electrolysis cells (SOECs). Herein, A-site-deficient perovskite oxide (LaSr)TiMnCuO (LSTMC) is synthesized and studied as a promising cathode for SOECs. Cu nanoparticles can be rapidly and uniformly -exsolved under reducing conditions. The heterostructure formed by the exsoluted Cu and LSTMC provides abundant active sites for the catalytic conversion of CO to CO. Combined with the remarkable oxygen-ion transport capacity of the LSTMC substrate, the specially designed Cu@LSTMC cathode exhibits a dramatically improved electrochemical performance. Furthermore, first-principles calculations proposed a mechanism for the adsorption and activation of CO by the heterostructure. Electrochemically, the Cu@LSTMC presents a high current density of 2.82 A cm at 1.8 V and 800 °C, which is about 2.5 times higher than that of LSTM (1.09A cm).
设计具有丰富活性位点且对CO电还原具有出色催化活性的活性阴极催化剂,对于推动固体氧化物电解槽(SOEC)的发展至关重要。在此,合成了A位缺陷的钙钛矿氧化物(LaSr)TiMnCuO(LSTMC)并将其作为一种有前景的SOEC阴极进行研究。在还原条件下,Cu纳米颗粒能够快速且均匀地析出。析出的Cu与LSTMC形成的异质结构为CO催化转化为CO提供了丰富的活性位点。结合LSTMC基底卓越的氧离子传输能力,特别设计的Cu@LSTMC阴极展现出显著提升的电化学性能。此外,第一性原理计算提出了异质结构对CO进行吸附和活化的机制。在电化学方面,Cu@LSTMC在1.8 V和800°C时呈现出2.82 A cm²的高电流密度,这大约是LSTM(1.09 A cm²)的2.5倍。