Plasma-Assisted Partial Methane Oxidation. Part I: One-Dimensional Statistical Modeling of a Dielectric Barrier Discharge Reactor

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Mohamed Saadana, Zeina Al Zayed, Hanen Oueslati, Nicolas Barléon, Vincent Robin, Élodie Fourré, Catherine Batiot-Dupeyrat, Sylvie Rossignol
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Abstract

This paper presents an original one-dimensional statistical model designed to complement experimental data from a practical dielectric barrier discharge (DBD) reactor. The experimental setup consists of a plasma-assisted reactor with gas injection composed solely of CH4 and O2. The numerical procedure uses electrical measurements to provide a realistic description of the power consumption and the current flowing through the gas, in a complex scenario where approximately one hundred current peaks are measured per electrical half-period. A plasma kinetic model is then used to analyze the chemistry and characteristic times of both isolated discharges and a representative train of discharges occurring within the reactor. These times are used to optimize the computational costs and to select the most appropriate kinetic schemes for the gas phase, whether in a plasma or quasi-thermodynamic equilibrium state. This approach also allows the separation of fast transformations (plasma) occurring at constant volume, from slower transformations occurring at constant pressure. The statistical approach, based on a Monte Carlo method, clearly identifies the assumptions required to reduce the real complexity of the DBD reactor to a 1D flow model. The combination of chromatographic measurements at the reactor outlet and numerical simulations provides the heterogeneity factor of the discharges, which is identified as a key parameter in the model. Although the flow can be considered stationary on average, the obtained value reveals a highly heterogeneous spatial distribution of the discharges within the reactor. Thus, the numerical results suggest that the gases passing through the reactor are rarely in a plasma state.

Abstract Image

本文介绍了一种独创的一维统计模型,该模型旨在补充来自实用介质阻挡放电(DBD)反应器的实验数据。实验装置包括一个等离子体辅助反应器,注入的气体完全由 CH4 和 O2 组成。数值计算程序使用电学测量方法,在每个电学半周期测量约一百个电流峰值的复杂情况下,对功耗和流经气体的电流进行真实描述。然后使用等离子体动力学模型分析反应器内发生的孤立放电和一列代表性放电的化学性质和特征时间。这些时间用于优化计算成本,并为处于等离子体或准热力学平衡状态的气相选择最合适的动力学方案。这种方法还可以将恒定体积下发生的快速转化(等离子体)与恒定压力下发生的慢速转化区分开来。基于蒙特卡洛方法的统计方法清楚地确定了将 DBD 反应器的实际复杂性降低到一维流动模型所需的假设条件。反应器出口处的色谱测量与数值模拟相结合,提供了排出物的异质性因子,该因子被确定为模型中的一个关键参数。虽然可以认为流动平均是静止的,但所获得的数值显示出反应器内排放物的空间分布非常不均匀。因此,数值结果表明,通过反应器的气体很少处于等离子状态。
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
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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