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首页> 外文期刊>Combustion and Flame >Computational study of polycyclic aromatic hydrocarbons growth by vinylacetylene addition
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Computational study of polycyclic aromatic hydrocarbons growth by vinylacetylene addition

机译：乙烯基乙炔加成生长多环芳烃的计算研究

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摘要

The growth of polycyclic aromatic hydrocarbons (PAH) can proceed via multiple chemical mechanisms. The mechanism of naphthyl radical and vinylacetylene (C4H4) addition reaction has been systematically investigated in this computational study. A combination of DFT/B3LYP/6-311+G(d,p), CCSD/6-311+G(d,p) and CBS-QB3 methods were performed to calculate the potential energy surfaces. It revealed that the products, including phenanthrene, anthracene, a PAH with a five-membered ring structure, and PAH with a C4H3 radical substitution, can be formed in A(2)-1 (1-naphthyl)+C4H4 and A(2)-2 (2-naphthyl) +C4H4 reaction networks. The reaction rate constants at 0.1-100 atm were evaluated by RRKM theory by solving the master equation in the temperature range of 800-2500 K, which showed that the rate constants of reactions A(2)-1 (A(2)-2)+C4H4 - product+H are highly temperature-dependent but nearly pressure-independent. The distribution of products was investigated in a 0-D batch reactor, wherein the initial reactant concentrations were taken from experimental measurements. The results showed that adduct intermediates were the main products at low temperature (T 1000 K), and the phenanthrene and PAH with C4H3 radical substitution became the dominant products at temperatures where PAHs and soot form in flames (T 1000 K). It was observed that a significant amount of phenanthrene is formed from PAH with a C4H3 radical substitution with the assistance of H atom. Reaction pathway sensitivity analysis for the PAH radical+C4H4 reaction system was performed and showed that the new benzene rings are more likely to be generated near the zig-zag edge surface site instead of the free edge. For the development of a PAH mechanism, the analogous treatment of rate constants for larger PAH radical +C4H4 reaction system are discussed. The formation rate of naphthalene from the reaction of phenyl+C4H4 was found to be very close to that of phenanthrene from the reaction of naphthyl+C4H4, suggesting that the analogous treatment of the rates is reasonable in PAH mechanisms. (C) 2019 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
机译：多环芳烃（PAH）的生长可以通过多种化学机理进行。在此计算研究中，系统地研究了萘基和乙烯基乙炔（C4H4）加成反应的机理。结合使用DFT / B3LYP / 6-311 + G（d，p），CCSD / 6-311 + G（d，p）和CBS-QB3方法来计算势能面。结果表明，可以在A（2）-1（1-萘基）+ C4H4和A（2）中形成包括菲，蒽，具有五元环结构的PAH和具有C4H3自由基取代的PAH在内的产物。 ）-2（2-萘基）+ C4H4反应网络。通过在800-2500 K的温度范围内求解主方程，通过RRKM理论评估了0.1-100 atm的反应速率常数，这表明反应A（2）-1（A（2）-2 ）+ C4H4->产品+ H与温度高度相关，但与压力几乎无关。在0-D间歇反应器中研究产物的分布，其中初始反应物浓度取自实验测量值。结果表明，在低温（T <1000 K）下，加合物中间产物是主要产物，在火焰中多环芳烃和烟灰形成（T> 1000 K）的温度下，菲和具有C4H3自由基取代的PAH成为主要产物。观察到，在H原子的辅助下，由具有C4H3自由基取代的PAH形成了大量的菲。进行了PAH自由基+ C4H4反应体系的反应路径敏感性分析，结果表明，在Z字形边缘表面位置附近（而不是在自由边缘附近）更可能生成新的苯环。为了发展PAH机理，讨论了较大PAH自由基+ C4H4反应体系速率常数的类似处理。发现由苯基+ C4H4反应形成的萘的形成速率与由萘基+ C4H4反应形成的菲的形成速率非常接近，这表明该速率的类似处理在PAH机理中是合理的。 （C）2019燃烧研究所。由Elsevier Inc.出版。保留所有权利。

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  • 来源
    《Combustion and Flame》 |2019年第4期|276-291|共16页
  • 作者

    Liu Peng; Zhang Yiran; Li Zepeng; Bennett Anthony; Lin He; Sarathy S. Mani; Roberts William L.;

  • 作者单位

    King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia;

    Shanghai Jiao Tong Univ, Sch Mech Engn, Key Lab Power Machinery & Engn, Minist Educ, Shanghai 200240, Peoples R China;

    King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia;

    King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia;

    Shanghai Jiao Tong Univ, Sch Mech Engn, Key Lab Power Machinery & Engn, Minist Educ, Shanghai 200240, Peoples R China;

    King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia;

    King Abdullah Univ Sci & Technol, Clean Combust Res Ctr, Thuwal 239556900, Saudi Arabia;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    PAHs; Soot; Nucleation; Mechanism; Kinetics;

    机译：多环芳烃;烟尘;成核;机理;运动学;

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