Numerical Simulation of Thermal Conversion of Aromatic Hydrocarbons in the Presence of Hydrogen and Steam using a Detailed Chemical Kinetic Model
Numerical Simulation of Thermal Conversion of Aromatic Hydrocarbons in the Presence of Hydrogen and Steam using a Detailed Chemical Kinetic Model
复制标题
使用详细的化学动力学模型对氢气和蒸汽存在下芳香烃的热转化进行数值模拟
DOI：
10.1016/j.cej.2011.10.003
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发表时间：
2011
影响因子：
15.1
通讯作者：
and Jun-ichiro Hayashi
中科院分区：
文献类型：
--
作者：
Koyo Norinaga;Ryota Sato;and Jun-ichiro Hayashi
一个详细的化学动力学模型被成功地用于预测碳氢燃料的燃烧和裂解特性，该模型的反应机理包括数千个基本的阶跃反应。然而，这种方法很少用于预测芳香烃的水蒸气重整反应。在这项研究中，一个现有的详细的化学动力学模型对芳香烃在氢气和水蒸气存在下的热转化率的预测能力进行了严格的评估。已发表的关于模拟焦炉煤气(氢、蒸汽和苯、甲苯或萘等芳香烃的混合物)在管式流动反应器(总压为160kPa，温度为1073-1673K，停留时间长达1s)中水蒸气重整的实验数据被用于评估。基于包含200多个化学物种和2000多个基本阶跃反应的动力学模型和推流反应器模型的模拟很好地再现了CO、CO2和CH4等主要产物的实验结果以及源芳烃的转化趋势。在假设计算得到的多环芳烃和乙炔的总产率与实验确定的焦产率相对应的情况下，焦炭产率也得到了很好的预测。此外，对于萘的转化，氢分压和停留时间对产物分布的影响也得到了很好的预测。
A detailed chemical kinetic model with a reaction mechanism consisting of thousands of elementary step-like reactions has been successfully applied to predict the combustion and pyrolysis characteristics of hydrocarbon fuels. This approach, however, has seldom been used for predicting steam reforming of aromatic hydrocarbons. In this study, the predictive capability of an existing detailed chemical kinetic model was critically evaluated for the thermal conversion rates of aromatic hydrocarbons in the presence of hydrogen and steam. Published experimental data on steam reforming of simulated coke oven gas (a mixture of hydrogen, steam, and an aromatic hydrocarbon such as benzene, toluene, or naphthalene) in a tubular flow reactor (total pressure of 160kPa, temperature of 1073–1673K, and residence time of up to 1s) were used for the evaluations. Simulations based on a kinetic model that consists of more than 200 chemical species, more than 2000 elementary step-like reactions, and a plug flow reactor model well reproduced experimental results for major products such as CO, CO2, and CH4as well as the conversion trends of source aromatic hydrocarbons. The coke yield was also fairly well predicted under the assumption that the computationally obtained total yields of polycyclic aromatic hydrocarbons and acetylene, both of which are the most likely coke precursors, correspond to the experimentally determined coke yields. In addition, the influences of the hydrogen partial pressure and residence time on the product distributions were also well predicted for the naphthalene conversion.