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DOI	10.1039/c9ee00656g
	Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels
	Suter S.; Haussener S.
发表日期	2019
ISSN	1754-5692
起始页码	1668
结束页码	1678
卷号	12 期号:5
英文摘要	Mesostructured silver catalysts have shown a substantial rise in reaction selectivity for the conversion of CO2 into fuels with increasing thickness of ordered, inverse-opal films. The challenge lies in the optimization of the morphology to maximize the CO selectivity. We developed a 3D mass transport model utilizing the accurate electrode geometry to calculate local concentration distributions of CO2(aq), OH-, HCO3-, and CO32- by considering the buffer reactions in the electrolyte and modeling local catalytic surface reaction rates based on Butler-Volmer correlations. Validated with experimental data from the literature, the model predicted the suppression of the hydrogen evolution reaction with an inverse dependency on the hydroxide concentration and the promotion of the CO evolution reaction with a proportional dependency on the carbonate concentration. In order to increase the CO selectivity, we developed design guidelines that suggest high electrode roughness per film thickness, which translates to smaller pore size in practice. Further, the shallow pores of the electrode strongly reduced the overall CO selectivity as the mass transport to the bulk was non-limiting. We demonstrated that the introduction of an additional diffusion layer on top of the silver electrode can enhance the CO selectivity from as low as 39% to more than 90%. © 2019 The Royal Society of Chemistry.
语种	英语
scopus关键词	Carbon dioxide; Electrodes; Electrolytes; Inverse problems; Morphology; Pore size; Reaction rates; Surface reactions; Carbon dioxide conversions; Carbonate concentrations; Concentration distributions; Electrode geometries; Hydrogen evolution reactions; Hydroxide concentration; Mass transport model; Reaction selectivity; Catalyst selectivity; carbon dioxide; carbonate; concentration (composition); diffusion; electrode; electrolyte; film; fuel; geometry; mass transport; optimization; roughness; silver
来源期刊	Energy and Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/162793
作者单位	Laboratory of Renewable Energy Science and Engineering, EPFL Station 9, Lausanne, 1015, Switzerland
推荐引用方式 GB/T 7714	Suter S.,Haussener S.. Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels[J],2019,12(5).
APA	Suter S.,&Haussener S..(2019).Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels.Energy and Environmental Science,12(5).
MLA	Suter S.,et al."Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels".Energy and Environmental Science 12.5(2019).