Quantification of the porosity in template-based ordered porous Ag electrodes and its effect on electrochemical CO2 reduction.

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Maaike E T Vink-van Ittersum, Erik Betz-Güttner, Eric Hellebrand, Claudia J Keijzer, Matt L J Peerlings, Peter Ngene, Petra E de Jongh
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引用次数: 0

Abstract

The electrochemical reduction of CO2 combined with efficient CO2 capture is a promising approach to close the carbon cycle. We studied the effect of pore size on the activity and selectivity of porous Ag electrodes using template-based electrodes as model catalysts. Using polymer spheres with sizes between 115 nm and 372 nm as templates, ordered porous Ag catalysts with different pore diameters were obtained. These well-defined model systems allowed us to understand the effect of pore size on CO and H2 production. At the most cathodic potential, around -1.05 V, up to 4 times more CO than H2 was formed. The intrinsic CO production depends on the pore size, as it increases when changing the pore diameters from ∼100 nm to ∼300 nm. At pore diameters above ∼300 nm, the pore size does not affect the intrinsic CO production anymore. For the first time, FIB-SEM was used to quantitatively analyse the porosity of the electrodes and correlate it with trends in intrinsic activity. The catalyst with a pore diameter of ∼200 nm had the highest tortuosity of 2.41, which led to an increased CO production. The catalysts with a pore diameter of ∼200 nm and smaller have pore networks that are twice as long as the pore network of catalysts with ∼400 nm pores. This leads to an additional potential drop, which lowers the effective driving force for the electrochemical reaction. Disentanglement of these different factors is important for rational design of porous CO2 reduction catalysts.

模板基有序多孔银电极孔隙率的量化及其对电化学CO2还原的影响。
电化学还原二氧化碳并结合有效的二氧化碳捕获是一种很有前途的关闭碳循环的方法。以模板电极为模型催化剂,研究了孔径对多孔银电极活性和选择性的影响。以尺寸为115 ~ 372 nm的聚合物球为模板,制备了不同孔径的有序多孔银催化剂。这些定义良好的模型系统使我们能够了解孔径对CO和H2生成的影响。在阴极电位最高时,约为-1.05 V, CO的生成量是H2的4倍。固有CO产量取决于孔径,当孔径从~ 100 nm改变到~ 300 nm时,它会增加。在孔径大于~ 300 nm时,孔径大小不再影响本征CO的产生。FIB-SEM首次用于定量分析电极的孔隙率,并将其与内在活性趋势相关联。孔径为~ 200 nm的催化剂扭曲度最高,达到2.41,导致CO产量增加。孔径为~ 200nm及以下的催化剂的孔网长度是孔径为~ 400nm催化剂的两倍。这会导致额外的电位下降,从而降低了电化学反应的有效驱动力。研究这些因素对合理设计多孔CO2还原催化剂具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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