Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge
Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge
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DOI：
10.1016/j.ces.2020.116399
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发表时间：
2021-04
影响因子：
4.7
通讯作者：
P. Maitre;M. Bieniek;P. Kechagiopoulos
中科院分区：
文献类型：
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作者：
P. Maitre;M. Bieniek;P. Kechagiopoulos
非热甲烷等离子体的详细动力学计划的开发，认为电子和振动激发物种的反应性和弛豫。建立了大气压介质阻挡放电甲烷无氧化偶联反应器的模型。通过1D流体建模研究短时间段，而对于较长时间段，按照反应器停留时间的顺序，遵循组合的1D-0 D方法。模拟结果与文献实验定性一致。大约86%的能量输入被发现用于激发物种的产生。甲烷的振动激发态表现出非常瞬态的响应，由于它们的快速形成过程中的电子流和快速猝灭VV和VT过程。更高能量的电子激发态被迅速转换，其中许多基本上立即解离。超过70%的甲烷转化是通过电子激发进行的，而振动激发态的贡献有限。
A detailed kinetic scheme for non-thermal methane plasma is developed that considers the reactivity and relaxation of electronically and vibrationally excited species. An atmospheric pressure dielectric barrier discharge reactor for methane non-oxidative coupling is modelled. Via 1D fluid modelling short periods of time are investigated, while for longer periods of time, in the order of the reactor residence time, a combined 1D-0D approach is followed. Modelling results are in good qualitative agreement with literature experiments. Around 86% of the energy input is found to channel into the creation of excited species. The vibrationally excited states of methane exhibit very transient responses due to their rapid formation during electron streamers and fast quenching by VV and VT processes. The, higher energy, electronically excited states are rapidly converted, many of which essentially instantly dissociate. Over 70% of methane’s conversion proceeds via electronical excitation, while the contribution of vibrationally excited states is limited.