OSCILLATORY COOL FLAMES IN THE COMBUSTION OF DIETHYL-ETHER
OSCILLATORY COOL FLAMES IN THE COMBUSTION OF DIETHYL-ETHER
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DOI：
10.1039/ft9928803153
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发表时间：
1992-11-07
期刊：
影响因子：
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通讯作者：
INOMATA, T
中科院分区：
文献类型：
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作者：
GRIFFITHS, JF;INOMATA, T
在射流搅拌流动反应器中，对C_2H_5OC_2H_5 + O_2 + N_2混合物的振荡冷火焰进行了实验和数值研究。平均停留时间为4 +/- 2 s。通过容器中的非常精细的热电偶检测反应。主要目的是研究乙醚的低温氧化反应，并建立这种反应的动力学起源。就冷火焰和点火现象而言，二烷基醚似乎是最具反应性的一类有机化合物，在本实验中观察到振荡冷火焰的最低温度为430 K。它们存在的最高温度为590 K。在这些实验中没有检测到点火，但得到复杂的燃烧-冷-火焰模式。绘制了各种反应存在的p-T（a）区域，数值分析基于92反应方案，该方案是从研究乙醛冷火焰和着火现象的方案发展而来的。特别注意的是涉及烷基过氧和烷基二过氧物种的过程。振荡冷火焰中得到的建模容器温度远低于那些对应的乙醛冷火焰。乙醚氧化的低温反应性似乎与初级氢过氧化物CH 3CH（OOH）OC 2 H5有关。二氢过氧化物似乎在与这种氧化有关的链支化中不起任何作用。非周期性的非等温现象也得到了模拟，动力学的起源似乎是与反应的CH 3CO自由基，也发现在乙醛氧化。
An experimental and numerical study of the oscillatory cool flames of a C2H5OC2H5 + O2 + N2 mixture has been performed in a jet-stirred flow reactor at reactant pressures up to 300 mmHg. The mean residence time was 4 +/- 2 s. Reaction was detected by a very fine thermocouple in the vessel. The primary objective was to study the low-temperature oxidation of diethyl ether and to establish the kinetic origins of this reactivity. The dialkyl ethers appear to be the most reactive class of organic compounds as far as cool flame and ignition phenomena are concerned, the lowest temperature at which oscillatory cool flames were observed in the present experiments being 430 K. The highest temperature for their existence was 590 K. No ignitions were detected in these experiments but complex oscillatory-cool-flame modes were obtained. The p-T(a) regions for the existence of the different kinds of reactions were mapped.Numerical analysis was based on a 92 reaction scheme developed from that used to study the cool flame and ignition phenomena of acetaldehyde. Particular attention was paid to the processes involving alkylperoxy and alkyldiperoxy species. Oscillatory cool flames were obtained in the modelling at vessel temperatures considerably below those corresponding to the cool flames of acetaldehyde. The low-temperature reactivity of diethyl ether oxidation appears to be associated with the primary hydroperoxide CH3CH(OOH)OC2H5. Dihydroperoxides seem not to play any part in the chain branching associated with this oxidation. Aperiodic non-isothermal phenomena were also obtained in the simulations, the kinetic origins of which appear to be related to reactions of the CH3CO radical, as also found in acetaldehyde oxidation.