Investigating the effects of helium, argon and hydrogen co-feeding on the non-oxidative coupling of methane in a dielectric barrier discharge reactor
Investigating the effects of helium, argon and hydrogen co-feeding on the non-oxidative coupling of methane in a dielectric barrier discharge reactor
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DOI：
10.1016/j.ces.2022.117731
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发表时间：
2022-05
影响因子：
4.7
通讯作者：
P. Maitre;J. Long;M. Bieniek;M. N. Bannerman;P. Kechagiopoulos
中科院分区：
文献类型：
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作者：
P. Maitre;J. Long;M. Bieniek;M. N. Bannerman;P. Kechagiopoulos
研究了介质阻挡放电中氦气、氩气和氢气共进料对甲烷非氧化偶联反应的影响，考察了反应途径和能量效率。一维流体模拟被用来研究短时间尺度。零维全球建模，使用输入的一维模拟，被用来研究相当于实验反应堆的时间尺度。一个先前开发的详细的非热甲烷等离子体的电子和振动激发物种的反应性和弛豫的动力学计划扩展到描述惰性气体与甲烷等离子体内的物种的相互作用。广泛的组成和施加的电压进行了研究，以确定提高甲烷转化的能量效率和增值产品的选择性的条件。潘宁解离在具有高含量氩气的混合物的情况下具有显著影响，而氢气共进料增加了对乙烷和乙烯相对于乙炔的选择性。
The impact of helium, argon, and hydrogen co-feeding on methane non-oxidative coupling in dielectric barrier discharges is investigated in terms of reaction pathways and energy efficiency. One-dimensional fluid simulations are used to investigate short time-scales. Zero-dimensional global modelling, using inputs from the one-dimensional simulations, is utilised to study time-scales equivalent to those of experimental reactors. A previously developed detailed kinetic scheme for non-thermal methane plasma that accounts for the reactivity and relaxation of electronically and vibrationally excited species is extended to describe the interactions of noble gases with the species within the methane plasma. A wide range of compositions and applied voltages are studied to determine the conditions that improve the energy efficiency of methane conversion and the selectivity to value-added products. Penning dissociation has a significant impact in the case of mixtures with high content of argon, while hydrogen co-feeding increases selectivity towards ethane and ethylene versus acetylene.