COMBINED OXIDATION OF GASEOUS AND LIQUID ALKANES IN THE BARRIER DISCHARGE PLASMA

IF 0.4 Q4 CHEMISTRY, MULTIDISCIPLINARY Chemistry for Sustainable Development Pub Date : 2024-06-14 DOI:10.15372/csd2024548
 . RYABOV A,  V. KUDRYASHOV S,  N. OCHEREDKO A
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Abstract

The combined oxidation of gaseous (propane, butane) and liquid (heptane, octane, nonane and decane) alkanes in a barrier discharge plasma in oxygen has been studied. Oxidation process involves simultaneous conversion of gaseous and liquid hydrocarbons. Various C1-C4 hydrocarbon gases and mainly oxygenated compounds corresponding to hydroxyl and carbonyl compounds with the same number of carbon atoms in molecules as in the initial alkanes were detected among reaction products. At the stage of chemical reaction initiation in a barrier discharge, the electrons in the discharge interact with all the molecules of the initial mixture to form atomic oxygen and various hydrocarbon radicals. Their subsequent transformation leads to the formation of peroxide radicals of the corresponding alkanes, and their disproportionation leads to the formation of hydroxyl and carbonyl compounds. The mechanism of gaseous alkane oxidation is generally comparable to the mechanism of liquid hydrocarbon oxidation in a barrier discharge, and the key role in the mechanism of alkane co-oxidation is played by the interaction of atomic oxygen with a gaseous or liquid alkane. A probable mechanism for the combined oxidation of gaseous and liquid alkanes in a barrier discharge is proposed on the basis of experimental and literature data, and a simple equation is deduced, linking the rates of atomic oxygen interaction with alkane molecules to hydrocarbon concentrations in the gas phase of the discharge gas in the reactor. Applying the obtained equation, it is possible to estimate the direction of the oxidation of gaseous and liquid alkane mixtures and to involve the experimental data in calculating yet unknown rate constants of atomic oxygen interaction with alkane molecules. The results obtained make it possible to optimise the experimental conditions for the oxidation of gaseous and liquid alkane mixtures with the predominant oxidation of a gaseous alkane. These data will be useful in developing effective methods for the direct processing of a broad fraction of light hydrocarbons.
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气态和液态烷烃在阻挡放电等离子体中的联合氧化
研究了气态(丙烷、丁烷)和液态(庚烷、辛烷、壬烷和癸烷)烷烃在氧气中的阻挡放电等离子体中的联合氧化。氧化过程涉及气态和液态碳氢化合物的同时转化。在反应产物中检测到了各种 C1-C4 碳氢化合物气体和主要的含氧化合物,这些化合物相当于羟基和羰基化合物,其分子中的碳原子数与初始烷烃中的碳原子数相同。在阻挡放电的化学反应起始阶段,放电中的电子与初始混合物的所有分子相互作用,形成原子氧和各种碳氢化合物自由基。它们随后的转化导致形成相应烷烃的过氧化物自由基,它们的歧化导致形成羟基和羰基化合物。气态烷烃氧化的机理一般与阻挡放电中液态碳氢化合物氧化的机理相似,而烷烃联合氧化机理中的关键作用是原子氧与气态或液态烷烃的相互作用。根据实验和文献数据,提出了气态和液态烷烃在阻挡放电中联合氧化的可能机理,并推导出一个简单方程,将原子氧与烷烃分子相互作用的速率与反应器中放电气体气相中的烃浓度联系起来。应用所得到的方程式,可以估计气态和液态烷烃混合物的氧化方向,并将实验数据用于计算原子氧与烷烃分子相互作用的未知速率常数。所获得的结果可以优化气态和液态烷烃混合物氧化的实验条件,使气态烷烃的氧化占主导地位。这些数据将有助于开发直接处理大量轻烃的有效方法。
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来源期刊
Chemistry for Sustainable Development
Chemistry for Sustainable Development CHEMISTRY, MULTIDISCIPLINARY-
自引率
25.00%
发文量
52
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