气候变化领域集成服务门户(CCPortal): Sequential catalysis controls selectivity in electrochemical CO2 reduction on Cu

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DOI	10.1039/c8ee01501e
	Sequential catalysis controls selectivity in electrochemical CO2 reduction on Cu
	Lum Y.; Ager J.W.
发表日期	2018
ISSN	17545692
起始页码	2935
结束页码	2944
卷号	11 期号:10
英文摘要	Electrochemical reduction of CO2 in aqueous media is a strategy for sustainable production of fuels and commodity chemicals. Cu is the only catalyst which converts CO2 to significant quantities of hydrocarbons and oxygenates. Here we demonstrate that oxygenate products can be favored over hydrocarbons by positioning a local source of CO generated by a CO producing catalyst (Au or Ag) in close proximity to a Cu catalyst. Use of a bimetallic device comprising interdigitated and independently controllable lines of Au and Cu allows the local CO concentration to be modulated. Notably, diffusional simulations show that the saturation concentration of CO can be exceeded locally. Actuating both the Au and Cu lines increases the oxygenate to ethylene ratio compared to actuating Cu only. Increasing the relative area of CO-producing Au relative to Cu also increases this ratio. These insights are translated into a second bimetallic system comprising Cu dots/lines patterned directly onto a Ag substrate, allowing for the distance between Cu and the CO generating metal to be precisely controlled. Controlling the relative areas of Ag and Cu allows for tuning of the oxygenate to ethylene ratio from 0.59 to 2.39 and an increase in oxygenate faradaic efficiency from 21.4% to 41.4%, while maintaining the selectivity to C2/C3 products in the 50-65% range. We attribute this change in selectivity to be due to an increased ∗CO coverage on Cu. By utilizing diffusional transport of CO to the Cu, a sequential catalysis pathway is created which allows for the control of oxygenate selectivity in aqueous CO2 reduction. © 2018 The Royal Society of Chemistry.
英文关键词	Carbon dioxide; Catalysis; Catalysts; Electrolytic reduction; Ethylene; Gold; Silver; Silver compounds; Bimetallic systems; CO concentrations; Commodity chemicals; Diffusional transport; Electrochemical reductions; Faradaic efficiencies; Saturation concentration; Sustainable production; Copper; aqueous solution; carbon dioxide; catalysis; catalyst; concentration (composition); copper; electrochemical method; energy efficiency; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190114
作者单位	Joint Center for Artificial Photosynthesis, Materials Science Division, Lawrence Berkeley National LaboratoryCA 94720, United States; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720, United States
推荐引用方式 GB/T 7714	Lum Y.,Ager J.W.. Sequential catalysis controls selectivity in electrochemical CO2 reduction on Cu[J],2018,11(10).
APA	Lum Y.,&Ager J.W..(2018).Sequential catalysis controls selectivity in electrochemical CO2 reduction on Cu.Energy & Environmental Science,11(10).
MLA	Lum Y.,et al."Sequential catalysis controls selectivity in electrochemical CO2 reduction on Cu".Energy & Environmental Science 11.10(2018).