Reaction mechanism of methane activation using non-equilibrium pulsed discharge at room temperature
Reaction mechanism of methane activation using non-equilibrium pulsed discharge at room temperature
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DOI：
10.1016/s0016-2361(03)00163-7
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发表时间：
2003-12-01
期刊：
影响因子：
7.4
通讯作者：
Okazaki, K
中科院分区：
文献类型：
--
作者：
Kado, S;Urasaki, K;Okazaki, K
通过发射光谱的研究以及高级烃和几种同位素的实验，初步阐明了非平衡脉冲放电活化甲烷的反应机理。观察到了原子碳和C-2天鹅带系统的强发射以及H巴耳末系列发射。这表明，通过电子碰撞，甲烷高度解离成C和H，这与当CH 4和D-2的混合物被供给到放电区域时，产生的乙炔中的高C2 D2组成的结果一致。高电子能量有利于甲烷直接脱氢生成原子碳，高电子密度有利于CH 3、CH 2和CH依次脱氢生成原子碳。C_2H_2选择性高的原因是碳原子形成的CH或C_2-的浓度高，以及C、CH、C_2-和C_2H_2之间分解和复合的重复机制。(C)2003 Elsevier Ltd.保留所有权利。
The reaction mechanism of methane activation using non-equilibrium pulsed discharge was largely clarified from the emission spectroscopic study and experiments with higher hydrocarbons and some kinds of isotopes. The strong emission of atomic carbon and C-2 swan band system was observed as well as H Balmer series emission. This indicates that methane was highly dissociated into C and H by electron impact, which is consistent with the result of high C2D2 composition in produced acetylene when the mixture of CH4 and D-2, was fed into discharge region. High electron energy contributed to produce atomic carbon directly from methane, and high electron density promoted the dehydrogenation from CH3, CH2 and CH to produce atomic carbon consecutively. The reason for the high selectivity to C2H2 was the high concentration of CH or C-2 formed from atomic carbon, and the repetition mechanism of decomposition and recombination among C, CH, C-2 and C2H,. (C) 2003 Elsevier Ltd. All rights reserved.