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Plasma-Activated Copper Nanocube Catalysts for Efficient Carbon Dioxide Electroreduction to Hydrocarbons and Alcohols

作者:Dunfeng Gao, Ioannis Zegkinoglou, Núria J. Divins, Fabian Scholten, Ilya Sinev, Philipp Grosse, Beatriz Roldán Cuenya · 发表于:ACS Nano · 年份:2017 · DOI:10.1021/acsnano.7b01257 · 被引用次数:455 · 研究领域:CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Electrocatalysts for Energy Conversion

Carbon dioxide electroreduction to chemicals and fuels powered by renewable energy sources is considered a promising path to address climate change and energy storage needs. We have developed highly active and selective copper (Cu) nanocube catalysts with tunable Cu(100) facet and oxygen/chlorine ion content by low-pressure plasma pretreatments. These catalysts display lower overpotentials and higher ethylene, ethanol, and n -propanol selectivity, resulting in a maximum Faradaic efficiency (FE) of ∼73% for C 2 and C 3 products. Scanning electron microscopy and energy-dispersive X-ray spectroscopy in combination with quasi- in situ X-ray photoelectron spectroscopy revealed that the catalyst shape, ion content, and ion stability under electrochemical reaction conditions can be systematically tuned through plasma treatments. Our results demonstrate that the presence of oxygen species in surface and subsurface regions of the nanocube catalysts is key for achieving high activity and hydrocarbon/alcohol selectivity, even more important than the presence of Cu(100) facets.