气候变化领域集成服务门户(CCPortal): Understanding cation effects in electrochemical CO2 reduction

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DOI	10.1039/c9ee01341e
	Understanding cation effects in electrochemical CO2 reduction
	Ringe S.; Clark E.L.; Resasco J.; Walton A.; Seger B.; Bell A.T.; Chan K.
发表日期	2019
ISSN	17545692
起始页码	3001
结束页码	3014
卷号	12 期号:10
英文摘要	Solid-liquid interface engineering has recently emerged as a promising technique to optimize the activity and product selectivity of the electrochemical reduction of CO2. In particular, the cation identity and the interfacial electric field have been shown to have a particularly significant impact on the activity of desired products. Using a combination of theoretical and experimental investigations, we show the cation size and its resultant impact on the interfacial electric field to be the critical factor behind the ion specificity of electrochemical CO2 reduction. We present a multi-scale modeling approach that combines size-modified Poisson-Boltzmann theory with ab initio simulations of field effects on critical reaction intermediates. The model shows an unprecedented quantitative agreement with experimental trends in cation effects on CO production on Ag, C2 production on Cu, CO vibrational signatures on Pt and Cu as well as Au(111) single crystal experimental double layer capacitances. The insights obtained represent quantitative evidence for the impact of cations on the interfacial electric field. Finally, we present design principles to increase the activity and selectivity of any field-sensitive electrochemical process based on the surface charging properties: the potential of zero charge, the ion size, and the double layer capacitance. © 2019 The Royal Society of Chemistry.
英文关键词	Capacitance; Carbon dioxide; Electric fields; Electrochemical electrodes; Electrolytic reduction; Phase interfaces; Reaction intermediates; Silver compounds; Single crystals; Double-layer capacitance; Electrochemical process; Electrochemical reductions; Experimental investigations; Poisson-Boltzmann theory; Potential of zero charge; Quantitative agreement; Solid-liquid interfaces; Positive ions; carbon dioxide; cation; detection method; electric field; electrical conductivity; experimental study; 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/189816
作者单位	SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, United States; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo ParkCA 94025, United States; Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, United States; Surface Physics and Catalysis (SurfCat), Department of Physics Technical, University of Denmark, Denmark; Department of Chemical Engineering, University of California, Santa Barbara, CA 93117, United States; CatTheory Center, Department of Physics, Technical University of Denmark, Kongens Lyngby, 2800, Denmark
推荐引用方式 GB/T 7714	Ringe S.,Clark E.L.,Resasco J.,et al. Understanding cation effects in electrochemical CO2 reduction[J],2019,12(10).
APA	Ringe S..,Clark E.L..,Resasco J..,Walton A..,Seger B..,...&Chan K..(2019).Understanding cation effects in electrochemical CO2 reduction.Energy & Environmental Science,12(10).
MLA	Ringe S.,et al."Understanding cation effects in electrochemical CO2 reduction".Energy & Environmental Science 12.10(2019).