二氧化碳
乙烯
电化学
拉曼光谱
电极
二氧化碳电化学还原
法拉第效率
扩散
电流密度
联轴节(管道)
氢
化学工程
催化作用
材料科学
分析化学(期刊)
化学
物理化学
一氧化碳
热力学
复合材料
有机化学
光学
工程类
物理
量子力学
作者
Dan Ren,Jing Gao,Shaik M. Zakeeruddin,Michaël Grätzel
标识
DOI:10.1021/acs.jpclett.1c02043
摘要
The implementation of an electrochemical flow cell has enabled improved efficiency for CO2 reduction. However, in situ spectroscopic insights into the interface are still lacking. Here, we investigate a series of copper layers with different thicknesses on gas diffusion electrodes as a benchmark, with the best-performing one showing a Faradaic efficiency of 59.5% and a partial current density of −170 mA cm–2 for ethylene formation in 1 M KOH at −0.70 V against a reversible hydrogen electrode. By comparing the geometric as well as specific current density for ethylene on four Cu catalysts with different thicknesses, we illustrate the effects of bulk pH, local pH, and diffusion of CO2 on C–C coupling. We also reveal that the flexible rotation of the Cu–C bond of the *CO intermediate adsorbed on Cu, as shown by in situ Raman spectroscopy, is likely to be the key factor for efficient C–C coupling in a flow cell.
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