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An experimental and kinetic modeling study of phenylacetylene decomposition and the reactions with acetylene/ethylene under shock tube pyrolysis conditions

机译：苯乙烯分解的实验性和动力学建模研究及止回管热解条件下乙炔/乙烯反应的研究

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Pyrolysis of phenylacetylene with and without the presence of C-2 hydrocarbons (acetylene or ethylene) was studied in a single-pulse shock tube coupled to gas chromatography/gas chromatography-mass spectrometry equipment for speciation diagnostics. Quantitative speciation profiles were probed from each reaction system over the temperature range of 1100-1700 K at a nominal pressure of 20 bar. A kinetic model was proposed to interpret how phenylacetylene is consumed under high-pressure pyrolytic conditions and how the resulting intermediates react to form polycyclic aromatic hydrocarbons (PAHs), and furthermore, how the extra acetylene or ethylene alter the reaction schemes. It was found that the bimolecular reaction between phenylacetylene and hydrogen atom leading to phenyl and acetylene dominates phenylacetylene decomposition throughout the temperature window. The addition/elimination reactions between phenylacetylene and phenyl not only produce hydrogen atoms to maintain the reactivity of the fuel decay, but also directly lead to the formation of several C14H10 PAH isomers including diphenylacetylene, 9-methylene-fluorene and phenanthrene. Intermediates pools, regarding both species categories and abundance, are changed by the two C-2 fuels introduced into the reaction system. The added acetylene enables the Hydrogen-Abstraction-Acetylene-Addition (HACA) mechanism starting from the phenylacetylene radical to occur at relatively low temperatures. But the yielded naphthyl core does not stabilize in naphthalene due to the lack of hydrogen atoms in the reaction system, and instead, it carries on the HACA route by further combining with another acetylene molecule, ending up in acenaphthylene. Differently, the added ethylene intensifies the HACA routes by contributing to the acetylene formation, and more importantly, provides hydrogen atoms participating in the naphthalene formation from naphthyl radical. (C) 2020 The Authors. Published by Elsevier Inc. on behalf of The Combustion Institute.
机译：在耦合到气相色谱/气相色谱 - 质谱设备的单脉冲冲击管中，研究了苯乙烯的苯乙烯与苯乙烯的热解，苯乙烯与C-2烃（乙炔或乙烯）进行了用于物种诊断的气相色谱/气相色谱 - 质谱设备。在20巴的标称压力下，在1100-1700k的温度范围内从每个反应系统探测定量的形状曲线。提出了一种动力学模型来解释苯乙炔如何在高压热解条件下消耗以及所得中间体如何反应形成多环芳烃（PAH），此外，额外的乙炔或乙烯改变反应方案。结果发现，苯乙烯和氢原子之间的双分子反应导致苯基和乙炔的亚乙炔分解在整个温度窗口中。苯乙烯和苯基之间的添加/消除反应不仅产生氢原子以保持燃料衰减的反应性，而且还直接导致几种C14H10PAH异构体的形成，包括二苯基乙炔，9-亚甲基 - 芴和菲苯。关于物种类别和丰度的中间体池由引入反应系统的两个C-2燃料改变。添加的乙炔使得从苯乙烯自由基开始的氢紫外线（HACA）机制能够在相对低的温度下发生。但是由于在反应体系中缺乏氢原子，所以产量的萘基核不会稳定在萘中，并且通过进一步组合与另一种乙炔分子进一步结合在丙烷基亚内，它携带Haca途径。不同，添加的乙烯通过促进乙炔形成，更重要的是，提供参与萘基的萘形成的氢原子。 （c）2020作者。由elsevier公司发布代表燃烧研究所。

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