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DOI10.1039/c9ee00656g
Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels
Suter S.; Haussener S.
发表日期2019
ISSN17545692
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.
英文关键词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
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/189915
作者单位Laboratory of Renewable Energy Science and Engineering, EPFL Station 9, Lausanne, 1015, Switzerland
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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 & Environmental Science,12(5).
MLA Suter S.,et al."Optimizing mesostructured silver catalysts for selective carbon dioxide conversion into fuels".Energy & Environmental Science 12.5(2019).
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