材料科学
原位
选择性
化学
分析化学(期刊)
色谱法
催化作用
有机化学
作者
Rosa M. Arán‐Ais,Fabian Scholten,Sebastian Kunze,Rubén Rizo,Beatriz Roldán Cuenya
出处
期刊:Nature Energy
[Springer Nature]
日期:2020-03-30
卷期号:5 (4): 317-325
被引量:505
标识
DOI:10.1038/s41560-020-0594-9
摘要
The efficient electrochemical conversion of CO2 provides a route to fuels and feedstocks. Copper catalysts are well-known to be selective to multicarbon products, although the role played by the surface architecture and the presence of oxides is not fully understood. Here we report improved efficiency towards ethanol by tuning the morphology and oxidation state of the copper catalysts through pulsed CO2 electrolysis. We establish a correlation between the enhanced production of C2+ products (76% ethylene, ethanol and n-propanol at −1.0 V versus the reversible hydrogen electrode) and the presence of (100) terraces, Cu2O and defects on Cu(100). We monitored the evolution of the catalyst morphology by analysis of cyclic voltammetry curves and ex situ atomic force microscopy data, whereas the chemical state of the surface was examined via quasi in situ X-ray photoelectron spectroscopy. We show that the continuous regeneration of defects and Cu(i) species synergistically favours C–C coupling pathways. Carbon dioxide can be reduced electrocatalytically to fuels using copper catalysts, but the key features that determine the selectivity of these materials to specific products remains uncertain. Here Aran–Ais et al. use in situ methods to explore the influence of morphology and oxidation state on the performance of copper catalysts.
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