Mass spectrometric investigation and computer modeling of the CH/sub 4/-O/sub 2/-O/sub 3/ reaction from 480 to 830 K
Mass spectrometric investigation and computer modeling of the CH/sub 4/-O/sub 2/-O/sub 3/ reaction from 480 to 830 K
复制标题
CH/sub 4/-O/sub 2/-O/sub 3/ 480 至 830 K 反应的质谱研究和计算机建模
DOI：
10.1021/j100276a039
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发表时间：
1986
期刊：
影响因子：
--
通讯作者：
G. Rotzoll
中科院分区：
文献类型：
--
作者：
G. Rotzoll
在分子束源反应器中研究了甲烷与臭氧化氧气的反应，该反应器由配备有 0.2 毫米喷嘴的加热的 1 毫米直径氧化铝流管组成。压力和停留时间的典型值分别为 600 mbar 和 16 ms，覆盖的温度范围为 480 至 830 K。从反应器中膨胀的气体混合物转化为分子束并通过质谱仪进行分析。发现H/sub 2/O、CO、CH/sub 2/O、CH/sub 3/OH、H/sub 2/O/sub 2/、CO/sub 2/和CH/sub 3/OOH为反应产物。实验结果可以通过由 21 个物质的 47 个基元反应组成的反应机制来很好地建模。对反应途径的动力学敏感性分析和研究得出了反应的主要机理特征。该反应由臭氧的热分解引发。该反应中非常重要的是臭氧与甲基自由基和氢原子的二次反应。除此之外，甲基和甲基过氧自由基的自由基-自由基反应在反应过程中起主导作用。 37 篇参考文献、5 张图、2 个表格。
The reaction of methane with ozonized oxygen was investigated in a molecular beam source reactor, consisting of a heated 1-mm-diameter alumina flow tube equipped with a 0.2-mm nozzle. Typical values for pressure and residence time were 600 mbar and 16 ms, respectively, and the temperature range covered was from 480 to 830 K. The gas mixture expanding from the reactor was transformed into a molecular beam and analyzed by a mass spectrometer. H/sub 2/O, CO, CH/sub 2/O, CH/sub 3/OH, H/sub 2/O/sub 2/, CO/sub 2/, and CH/sub 3/OOH were found as reaction products. The experimental results could be fairly well modeled by a reaction mechanisms consisting of 47 elementary reactions with 21 species. A kinetic sensitivity analysis and investigation of the reaction pathways yields the main mechanistic features of the reaction. The reaction is initiated by the thermal decomposition of ozone. Very important in the reaction are secondary reactions of ozone with methyl radicals and hydrogen atoms. Besides that, radical-radical reactions of methyl and methylperoxy radicals play a dominant role in the course of the reaction. 37 references, 5 figures, 2 tables.