Experimental Study and Kinetic Modeling for Ethanol Treatment by Air Dielectric Barrier Discharges
Experimental Study and Kinetic Modeling for Ethanol Treatment by Air Dielectric Barrier Discharges
复制标题
空气介电势垒放电处理乙醇的实验研究和动力学模型
DOI：
10.1007/s11090-014-9601-x
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发表时间：
2015
影响因子：
3.6
通讯作者：
S. Pasquiers
中科院分区：
文献类型：
--
作者：
S. Lovascio;N. Blin;L. Magne;F. Jorand;S. Pasquiers
本文研究了干空气和湿空气介质阻挡放电中乙醇的去除。的实验结果进行了比较的零维动力学模型的预测，以阐明发生在等离子体相的主要化学路线。这一比较表明，氮氧化物的解离猝灭和由氧原子或羟基自由基的氧化反应应考虑到解释在这些种类的放电中的EtOH减排。CH 3CHOH自由基似乎是氮解离碰撞的主要产物，而由α-和β-H原子裂解产生的自由基是主要的乙醇氧化副产物。这些自由基占乙醛的生产，这里调查的乙醇/空气进料放电的主要副产品。除了完全氧化产物，即碳氧化物和水，含有多达6个碳原子的醛，酮，羧酸，臭氧，氮氧化物，硝酸和有机硝酸盐被发现在废气中。提出了一种动力学途径来解释检测到的副产物的形成。向进料气体中加入水蒸气略微改善了EtOH的去除，并促进了主要副产物的进一步氧化，从而提高了CO2的选择性。这种行为可以归因于较高量的羟基自由基，这可以促进CO2直接前体的产生。
This paper deals with the ethanol (EtOH) removal in both dry and humid air fed dielectric barrier discharges. The experimental results were compared to the predictions of a zero dimension kinetic model to elucidate the main chemical routes occurring in the plasma phase. This comparison shows that both the dissociative quenching of the nitrogen metastables and the oxidation reactions by the oxygen atom or the hydroxyl radical should be taken into account to explain the EtOH abatement in these kinds of discharges. The CH3CHOH radical seems to be the main product of the nitrogen dissociative collisions, whereas radicals issued from the α- and β-H atom cleavage are the dominant ethanol oxidation by-products. These radicals account for the production of acetaldehyde, the main by-product of the ethanol/air fed discharges investigated here. Apart the complete oxidation products, i.e. carbon oxides and water, aldehydes containing up to six carbon atoms, ketones, carboxylic acids, ozone, nitrogen oxides, nitric acid and organic nitrates were found in the exhaust gas. A kinetic pathway is proposed to explain the formation of the detected by-products. Water vapour addition to the feeding gas slightly improves the EtOH removal and promotes further oxidation of the main by-products, thus enhancing the CO2 selectivity. This behaviour could be ascribed to the higher amount of hydroxyl radicals, which could boost the production of the direct precursors of CO2.