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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >An optimized semidetailed submechanism of benzene formation from propargyl recombination
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An optimized semidetailed submechanism of benzene formation from propargyl recombination

机译：炔丙基重组形成苯的优化半详细亚机理

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摘要

The self-reaction of propargyl (C3H3) radicals has been widely suggested as one of the key routes forming benzene in a variety of aliphatic flames. Currently, in the majority of aromatic models, the C3H3 + C3H3 submechanism often contains one or two C6H6 isomers and a few global reaction steps, which do not adequately represent the actual recombination chemistry. Recent experimental and theoretical studies on the direct propargyl recombination and subsequent C6H6 isomerization have provided sufficient information to revisit and revise the C3H3 + C3H3 reaction submechanism. In the present work, a semidetailed kinetic model consisting of seven isomeric C6H6 species and 14 reaction steps was constructed based on the most recent potential energy surface for this system. The trial model was subjected to systemic optimization by use of a recently developed physically bounded Gauss-Newton (PGN) method against detailed species profiles of direct propargyl recombination and 1,5-hexadiyne (15HD) isomerization obtained front experiments at high temperatures in a shock tube and at low temperatures in a flow reactor, which were all measured at very high pressure (shock tube) or atmospheric (flow reactor) conditions. Predictions of the optimized model were in excellent agreement with all experimental measurements. The optimized C3H3 + C3H3 reaction subset was also tested for flame modeling. Two different aromatic chemistry models that incorporate benzene formation from propargyl radicals as a single step reaction were modified to include the complete submechanism for propargyl recombination. The updated models predict significant percentages of three isomeric species [2-ethynyl-1,3-butadiene (2E13BD), fulvene, and benzene] in premixed fuel-rich acetylene and ethylene flames, reflecting the observed flame structures.
机译：炔丙基（C3H3）自由基的自反应已被广泛认为是在各种脂族火焰中形成苯的关键途径之一。当前，在大多数芳族模型中，C3H3 + C3H3亚机理通常包含一个或两个C6H6异构体和一些整体反应步骤，这些反应步骤不足以代表实际的重组化学反应。最近有关炔丙基直接重组和随后的C6H6异构化的实验和理论研究为重访和修订C3H3 + C3H3反应亚机理提供了足够的信息。在本工作中，基于该系统的最新势能面，构建了由7个异构C6H6物种和14个反应步骤组成的半详细动力学模型。通过使用最新开发的物理有界高斯-牛顿（PGN）方法对试验模型进行了系统优化，以对抗直接炔丙基重组和1,5-己二炔（15HD）异构化的详细物种分布，并在高温下进行了冲击实验流动反应器中的低温和低温，所有这些条件都是在非常高的压力（冲击管）或大气压（流动反应器）条件下测量的。优化模型的预测与所有实验测量都非常吻合。还对优化的C3H3 + C3H3反应子集进行了火焰建模测试。修改了两个不同的芳香化学模型，这些模型将由炔丙基自由基形成的苯作为一步反应进行了修饰，以包括炔丙基重组的完整子机理。更新的模型预测了预混合的富含燃料的乙炔和乙烯火焰中三种同分异构体[2-乙炔基-1,3-丁二烯（2E13BD），富勒烯和苯]的显着百分比，反映了观察到的火焰结构。

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