Ji Yali, Yang Chao, Qian Linping, Zhang Lijuan, Zheng Gengfeng
Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, China.
Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, China.
J Colloid Interface Sci. 2021 Oct 15;600:847-853. doi: 10.1016/j.jcis.2021.05.057. Epub 2021 May 18.
The renewable energy-powered electroreduction of carbon dioxide or monoxide (CO) has been emerging as an attractive means to decarbonize the emission-intensive chemical manufacturing, which heavily relies on fossil fuels nowadays. One potential approach to promote the activity of electrocatalysts is to construct hybrid interface that can increase the stability of intermediates on electrode surfaces. Herein we developed a copper nanoparticle/polypyrrole (Cu-Ppy) nanowire composite as an efficient electrocatalyst for electrochemical CO reduction reaction. Compared to pure Cu nanoparticles, the Cu-Ppy composite exhibited a dramatically enhanced Faradaic efficiency of converting CO to ethylene (CH) from 34% to 69% at -0.78 V vs. reversible hydrogen electrode (RHE) in KOH electrolyte, and an excellent CH partial current density of 276 mA·cm at -1.18 V vs. RHE. Density functional theory calculations showed that the Cu-Ppy composite could bind CO more strongly as compared to pure Cu. As the Ppy coating allowed to stabilize OCCO*, a key intermediate in the CH formation, both the activity and selectivity of Cu-Ppy for CO-to-CH were increased. Our work suggests that constructing rationally designed hybrid interface can tune the local environment of catalyst surface toward enhanced activity and product selectivity.
利用可再生能源将二氧化碳或一氧化碳（CO）进行电还原，已成为减少碳排放密集型化学制造过程中碳排放的一种有吸引力的方法，目前该过程严重依赖化石燃料。促进电催化剂活性的一种潜在方法是构建能增加电极表面中间体稳定性的混合界面。在此，我们开发了一种铜纳米颗粒/聚吡咯（Cu-Ppy）纳米线复合材料，作为用于电化学CO还原反应的高效电催化剂。与纯铜纳米颗粒相比，在KOH电解液中相对于可逆氢电极（RHE）为-0.78 V时，Cu-Ppy复合材料将CO转化为乙烯（CH）的法拉第效率从34%显著提高到69%，并且在相对于RHE为-1.18 V时，具有276 mA·cm的优异CH分电流密度。密度泛函理论计算表明，与纯铜相比，Cu-Ppy复合材料能更强烈地结合CO。由于聚吡咯涂层能够稳定OCCO*（CH形成过程中的关键中间体），Cu-Ppy对CO到CH的活性和选择性均有所提高。我们的工作表明合理设计混合界面可以调节催化剂表面的局部环境，以提高活性和产物选择性。
