$$\hbox {CO}_2$$ / $$\hbox {CH}_4$$辉光放电等离子体:第一部分-反应途径的实验和数值研究

IF 2.6 3区 物理与天体物理 Q3 ENGINEERING, CHEMICAL
Edmond Baratte, Carolina A. Garcia-Soto, Tiago Silva, Vasco Guerra, Vasile I. Parvulescu, Olivier Guaitella
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引用次数: 0

摘要

在几托的辉光放电中对\(\hbox {CO}_2\) / \(\hbox {CH}_4\)等离子体进行了基础研究。对实验结果和数值结果进行了比较,确定了主要的反应途径。基于oes的技术和FTIR(傅里叶变换红外)光谱用于确定分子密度和气体温度。测量了压力、初始混合物和停留时间等条件。主要解离产物为CO和\(\hbox {H}_2\)。利用LoKI模拟工具建立了一个简化的动力学方案,以限制速率系数的不确定性,但足以再现实验数据。为此,根据实验观察,只考虑最多含有一个碳原子的分子。在实验数据和模拟之间获得良好的匹配需要包含涉及激发态的反应\(\hbox {O}(^{1}\hbox {D})\)。强调了\(\hbox {CH}_3\)自由基的关键作用。实验结果与模拟结果吻合较好,可以绘制出低压\(\hbox {CO}_2\) - \(\hbox {CH}_4\)等离子体的主要反应路径,特别是确定了\(\hbox {CO}_2\)的主要反反应机制。\(\hbox {CH}_2\) O和\(\hbox {H}_2\) O在气相中的作用也进行了深入的讨论,因为它们在本研究的第二部分所研究的催化表面上似乎起着重要的作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

$$\hbox {CO}_2$$ / $$\hbox {CH}_4$$ Glow Discharge Plasma: Part I—Experimental and Numerical Study of the Reaction Pathways

$$\hbox {CO}_2$$ / $$\hbox {CH}_4$$ Glow Discharge Plasma: Part I—Experimental and Numerical Study of the Reaction Pathways

A fundamental study of \(\hbox {CO}_2\)/\(\hbox {CH}_4\) plasma is performed in a glow discharge at a few Torr. Experimental and numerical results are compared to identify the main reaction pathways. OES-based techniques and FTIR (Fourier Transform Infrared) spectroscopy are used to determine molecules densities and gas temperature. Several conditions of pressure, initial mixture and residence time are measured. The main dissociation products are found to be CO and \(\hbox {H}_2\). The LoKI simulation tool was used to build a simplified kinetic scheme to limit the uncertainties on rate coefficients, but sufficient to reproduce the experimental data. To this aim, only molecules containing at most one carbon atom are considered based on the experimental observations. Obtaining a good match between the experimental data and the simulation requires the inclusion of reactions involving the excited state \(\hbox {O}(^{1}\hbox {D})\). The key role of \(\hbox {CH}_3\) radical is also emphasized. The good match obtained between the experiment and the simulation allows to draw the main reaction pathways of the low-pressure \(\hbox {CO}_2\)-\(\hbox {CH}_4\) plasmas, in particular to identify the main back reaction mechanisms for \(\hbox {CO}_2\). The role of \(\hbox {CH}_2\)O and \(\hbox {H}_2\)O in the gas phase is also discussed in depth as they appear to play an important role on catalytic surface studied in the part II of this study.

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来源期刊
Plasma Chemistry and Plasma Processing
Plasma Chemistry and Plasma Processing 工程技术-工程:化工
CiteScore
5.90
自引率
8.30%
发文量
73
审稿时长
6-12 weeks
期刊介绍: Publishing original papers on fundamental and applied research in plasma chemistry and plasma processing, the scope of this journal includes processing plasmas ranging from non-thermal plasmas to thermal plasmas, and fundamental plasma studies as well as studies of specific plasma applications. Such applications include but are not limited to plasma catalysis, environmental processing including treatment of liquids and gases, biological applications of plasmas including plasma medicine and agriculture, surface modification and deposition, powder and nanostructure synthesis, energy applications including plasma combustion and reforming, resource recovery, coupling of plasmas and electrochemistry, and plasma etching. Studies of chemical kinetics in plasmas, and the interactions of plasmas with surfaces are also solicited. It is essential that submissions include substantial consideration of the role of the plasma, for example, the relevant plasma chemistry, plasma physics or plasma–surface interactions; manuscripts that consider solely the properties of materials or substances processed using a plasma are not within the journal’s scope.
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