Electrochemical conversion of CO2 plasmas

IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Haytham E. M. Hussein, Panagiotis N. Kechagiopoulos and Angel Cuesta
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Abstract

The integration of non-thermal CO2 plasma (NTP) with a custom-designed electrolyte-gap electrolyser and CuO catalysts represents an innovative strategy to enhance the electrochemical conversion of CO2 into C1–C3 products. Systematic galvanostatic experiments conducted at current densities ranging from 100 to 225 mA cm−2 demonstrated that plasma-on operation significantly reduces cell voltages (by up to ∼1.3 V) and that product selectivity transitions from C1 species (CO and methane) to C2+ products, including ethylene, ethanol, acetate, propylene, and propanol. While CO and H2 predominate under plasma-off conditions, with limited formation of C2 products, the hybrid plasma–electrochemical system increases the faradaic efficiency (FE) for ethylene up to 39.5% and ethanol up to 18.1%. These enhancements are attributed to plasma-generated reactive species (radicals and excited-state molecules) that lower kinetic barriers for C–C coupling and modify the interfacial pH, thereby reducing parasitic carbonate/bicarbonate losses. The plasma-on state resulted in a statistically significant increase in liquid product carbon efficiency, from an average of ∼0.41% during plasma-off experiments to ∼0.91% during plasma-on experiments. Although the system currently exhibits lower overall energy efficiency owing to the power demands of the plasma discharge, this work establishes a robust framework for flexible product tuning and sustainable carbon utilisation via plasma-activated feeds.

Abstract Image

CO2等离子体的电化学转化
非热CO2等离子体(NTP)与定制设计的电解质间隙电解槽和CuO催化剂的集成代表了一种创新策略,可以提高CO2到C1-C3产品的电化学转化。在100 ~ 225 mA cm−2的电流密度下进行的系统恒流实验表明,等离子体操作显著降低了电池电压(高达~ 1.3 V),并且产品选择性从C1物质(CO和甲烷)转变为C2+产物,包括乙烯、乙醇、醋酸盐、丙烯和丙醇。在等离子体分离条件下,CO和H2占主导地位,C2产物的生成有限,混合等离子体-电化学体系将乙烯的法拉第效率(FE)提高到39.5%,乙醇的法拉第效率(FE)提高到18.1%。这些增强归功于等离子体产生的活性物质(自由基和激发态分子),它们降低了C-C耦合的动力学屏障,改变了界面pH,从而减少了寄生碳酸盐/碳酸氢盐的损失。等离子体开启状态导致液体产物碳效率从统计上显著提高,从等离子体关闭实验期间的平均0.41%提高到等离子体开启实验期间的平均0.91%。尽管由于等离子体放电的功率需求,该系统目前表现出较低的整体能源效率,但这项工作建立了一个强大的框架,可以通过等离子体激活馈源实现灵活的产品调整和可持续的碳利用。
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来源期刊
Sustainable Energy & Fuels
Sustainable Energy & Fuels Energy-Energy Engineering and Power Technology
CiteScore
10.00
自引率
3.60%
发文量
394
期刊介绍: Sustainable Energy & Fuels will publish research that contributes to the development of sustainable energy technologies with a particular emphasis on new and next-generation technologies.
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