Exploring chemical kinetics of plasma assisted oxidation of dimethyl ether (DME)
Exploring chemical kinetics of plasma assisted oxidation of dimethyl ether (DME)
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探索等离子体辅助氧化二甲醚 (DME) 的化学动力学
DOI：
10.1016/j.combustflame.2020.11.010
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发表时间：
2021-03
影响因子：
4.4
通讯作者：
Bin Yang
中科院分区：
文献类型：
--
作者：
Ruzheng Zhang;H;ong Liao;Jiuzhong Yang;Bin Yang
采用光电离分子束质谱（PI - MBMS）和动力学模拟研究了等离子体辅助氧化二甲醚的化学动力学。通过测量的质谱和光电离效率（PIE）曲线，鉴定出了一系列碳氢化合物和含氧化合物中间体，特别是一些特定于燃料的含氧化合物中间体，包括甲酸甲酯、甲乙醚和二甲氧基甲烷。定量结果显示，随着氧气含量的增加，物质摩尔分数呈现两种主要变化模式，这表明了不同的主要生成途径。除了含氧化合物外，在二甲醚/氧气/氩气和二甲醚/氩气等离子体系统中，在低温下观察到了C1和C2碳氢化合物中间体，而在二甲醚的热氧化中，这些中间体的形成通常发生在高于800 K的温度下。建立了一个包含气相反应和等离子体反应的动力学模型。模型分析表明，氢提取以及涉及电子/氩激发态/氧（1D）/氩离子的等离子体反应都对燃料消耗有贡献。生成的CH3OCH2、CH3O和CH3的后续反应导致了所观察到的碳氢化合物和含氧化合物的生成。实验结果以及动力学模拟表明，燃料和燃料自由基可能直接分解为甲基自由基、氧原子和甲醛，这解释了在二甲醚/氩气等离子体中甲醛预测值偏低以及观察到中等浓度含氧化合物的现象。
Chemical kinetics of plasma assisted oxidation of dimethyl ether was investigated by photoionization molecular beam mass spectrometry (PI-MBMS) and kinetic modeling. A series of hydrocarbon and oxygenated intermediates, especially some fuel-specific oxygenated intermediates including methyl formate, ethyl methyl ether and dimethoxymethane, were identified by the measured mass spectra and photoionization efficiency (PIE) curves. The quantification results displayed two main change patterns of species mole fractions with increasing oxygen, indicating the different dominating formation pathways. In addition to the oxygenates, C1 and C2 hydrocarbon intermediates were observed at low temperatures in the DME/O2/Ar and DME/Ar plasma systems, while the formation of these intermediates usually occurs at temperatures higher than 800 K in the thermal oxidation of DME. A kinetic model containing gas-phase reactions and plasma reactions was developed. The model analysis suggests that both hydrogen abstractions and plasma reactions involving electron/Ar*/O(1D)/Ar+ contribute to the fuel consumption. The subsequent reactions of the resulting CH3OCH2, CH3O and CH3 lead to the yield of the observed hydrocarbons and oxygenates. The experimental results together with kinetic modeling indicate that the fuel and fuel radical may decompose into methyl radical, oxygen atom and formaldehyde directly, which account for the under prediction of formaldehyde and the observation of oxygenates with moderate concentrations in the DME/Ar plasma.
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影响因子：
4.4
作者：
P. Dehmer;D. Holland
通讯作者：
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DOI：
10.1016/j.proci.2016.06.010
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期刊：
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DOI：
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影响因子：
3.4
作者：
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