Shen Yuxiang, Liu Tianfu, Li Rongtan, Lv Houfu, Ta Na, Zhang Xiaomin, Song Yuefeng, Liu Qingxue, Feng Weicheng, Wang Guoxiong, Bao Xinhe
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
Natl Sci Rev. 2023 Mar 20;10(9):nwad078. doi: 10.1093/nsr/nwad078. eCollection 2023 Sep.
Solid oxide electrolysis cells provide a practical solution for the direct conversion of CO to other chemicals (i.e. CO), however, an in-depth mechanistic understanding of the dynamic reconstruction of active sites for perovskite cathodes during CO electrolysis remains a great challenge. Herein, we identify that iridium-doped SrFeIrMoO (SFIrM) perovskite displays a dynamic electrochemical reconstruction feature during CO electrolysis with abundant exsolution of highly dispersed IrFe alloy nanoparticles on the SFIrM surface. The reconstructed IrFe@SFIrM interfaces deliver a current density of 1.46 A cm while maintaining over 99% CO Faradaic efficiency, representing a 25.8% improvement compared with the SrFeMoO counterpart. electrochemical spectroscopy measurements and density functional theory calculations suggest that the improved CO electrolysis activity originates from the facilitated formation of carbonate intermediates at the IrFe@SFIrM interfaces. Our work may open the possibility of using an electrochemical poling method for CO electrolysis in practice.
固体氧化物电解池为将一氧化碳直接转化为其他化学品（即一氧化碳）提供了一种切实可行的解决方案，然而，深入理解钙钛矿阴极在一氧化碳电解过程中活性位点的动态重构机理仍然是一个巨大的挑战。在此，我们发现铱掺杂的SrFeIrMoO（SFIrM）钙钛矿在一氧化碳电解过程中表现出动态电化学重构特征，在SFIrM表面有大量高度分散的铱铁合金纳米颗粒析出。重构后的IrFe@SFIrM界面在保持超过99%的一氧化碳法拉第效率的同时，电流密度达到1.46 A cm，与SrFeMoO相比提高了25.8%。电化学光谱测量和密度泛函理论计算表明，一氧化碳电解活性的提高源于IrFe@SFIrM界面处碳酸盐中间体的形成更容易。我们的工作可能为在实际中使用电化学极化方法进行一氧化碳电解开辟可能性。
