Banerji Liam C, Jang Hansaem, Gardner Adrian M, Cowan Alexander J
Department of Chemistry, Stephenson Institute for Renewable Energy, University of Liverpool Liverpool UK
Early Career Laser Laboratory, University of Liverpool Liverpool UK.
Chem Sci. 2024 Jan 17;15(8):2889-2897. doi: 10.1039/d3sc05295h. eCollection 2024 Feb 22.
The nature of the electrolyte cation is known to have a significant impact on electrochemical reduction of CO at catalyst|electrolyte interfaces. An understanding of the underlying mechanism responsible for catalytic enhancement as the alkali metal cation group is descended is key to guide catalyst development. Here, we use vibrational sum frequency generation (VSFG) spectroscopy to monitor changes in the binding modes of the CO intermediate at the electrochemical interface of a polycrystalline Cu electrode during CO reduction as the electrolyte cation is varied. A CO mode is observed only when using Cs, a cation that is known to facilitate CO reduction on Cu, supporting the proposed involvement of CO sites in CO coupling mechanisms during CO reduction. measurements show that the cation dependent CO modes correlate with morphological changes of the Cu surface.
已知电解质阳离子的性质对催化剂|电解质界面处CO的电化学还原有显著影响。理解随着碱金属阳离子族的下移导致催化增强的潜在机制是指导催化剂开发的关键。在这里，我们使用振动和频光谱（VSFG）来监测在CO还原过程中，随着电解质阳离子的变化，多晶Cu电极电化学界面处CO中间体结合模式的变化。仅在使用Cs（一种已知有助于在Cu上进行CO还原的阳离子）时观察到CO模式，这支持了在CO还原过程中CO位点参与CO偶联机制的提议。测量结果表明，阳离子依赖性CO模式与Cu表面的形态变化相关。
