Herranz Daniel, Maroto Antonio, Rodriguez Martina, Avilés Moreno Juan Ramón, Ocón Pilar
Departamento de Química Física Aplicada, Universidad Autónoma de Madrid, C/ Francisco Tomás y Valiente 7, 28049 Madrid, Spain.
Materials (Basel). 2025 Aug 30;18(17):4070. doi: 10.3390/ma18174070.
The electrochemical reduction in CO (CO2RR) to syngas and value-added hydrocarbons offers a promising route for sustainable CO utilization. This work develops tuneable Cu-Sn bimetallic catalysts via electrodeposition, optimized for CO2RR in a zero-gap flow cell fed with CO-saturated KHCO solution, a configuration closer to industrial scalability than conventional H-cells. By varying electrodeposition parameters (pH, surfactant DTAB, and metal precursors), we engineered catalysts with distinct selectivity profiles: Cu-Sn(B), modified with DTAB, achieved 50% Faradaic efficiency (FE) to CO at -2.2 V and -50 mA·cm, outperforming Ag-based systems that require higher overpotentials. Meanwhile, Cu-Sn(A) favoured CH (35% FE at -100 mA·cm), and Cu-Sn(C) shifted selectivity to CH (26% FE), demonstrating product tunability. The catalysts' performance stems from synergistic Cu-Sn interactions and DTAB-induced morphological control, as revealed by SEM/EDX and electrochemical analysis. Notably, all systems operated at lower voltages than literature benchmarks while maintaining moderate CO utilization (32-49% outlet). This study highlights the potential of electrodeposited Cu-Sn catalysts for energy-efficient CO2RR, bridging the gap between fundamental research and industrial application in syngas and hydrocarbon production.
将一氧化碳电化学还原为合成气和高附加值碳氢化合物为可持续利用一氧化碳提供了一条有前景的途径。本工作通过电沉积开发了可调节的铜 - 锡双金属催化剂，该催化剂针对在零间隙流动池中以一氧化碳饱和的KHCO溶液为原料的二氧化碳电化学还原进行了优化，这种配置比传统的H型电池更接近工业可扩展性。通过改变电沉积参数（pH值、表面活性剂DTAB和金属前驱体），我们设计出了具有不同选择性的催化剂：用DTAB改性的Cu - Sn(B)在-2.2 V和-50 mA·cm²时对一氧化碳的法拉第效率（FE）达到50%，优于需要更高过电位的银基体系。同时，Cu - Sn(A)有利于生成甲烷（在-100 mA·cm²时FE为35%），而Cu - Sn(C)将选择性转向甲烷（FE为26%），表明产物具有可调节性。扫描电子显微镜/能谱仪（SEM/EDX）和电化学分析表明，催化剂的性能源于铜 - 锡的协同相互作用以及DTAB诱导的形态控制。值得注意的是，所有体系在比文献基准更低的电压下运行时仍保持适度的一氧化碳利用率（出口处为32 - 49%）。这项研究突出了电沉积铜 - 锡催化剂在高效二氧化碳电化学还原方面的潜力，弥合了合成气和碳氢化合物生产中基础研究与工业应用之间的差距。
