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Formation mechanisms of soot from high-molecular-weight polycyclic aromatic hydrocarbons

机译:高分子量多环芳烃形成烟灰的机理

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摘要

The feedstocks, including benzene, acetylene, and benzene with acetylene or 2-7 ring PAH, were pyrolyzed in an isothermal laminar flow at 1400-1650 K. The particle size distributions (PSDs) of soot and nascent soot were analyzed using a scanning mobility particle sizer (SMPS). The morphology of particles with the same mobility particle diameter was examined using a scanning electron microscope (SEM), where the grid was sampled via thermophoretic sampling assisted by a differential mobility analyzer (DMA). The soot produced by the pyrolysis of acetylene at 1400 K exhibited the highest number concentration and a log-normal distribution compared with those of the soot produced by the pyrolysis of benzene and the PAH additives. At 1500 K, the pyrolysis of PAHs with three or more rings with zigzag sites significantly increased the number concentration, although the added carbon concentration was smaller than that of acetylene. The addition of dibenzo[a,e]pyrene, which possesses three armchair sites, inhibited soot formation, suggesting that the bay site is easily formed and that the formation of anisotropic PAHs inhibits dimerization. The morphology of the soot formed by the addition of dibenzo[a,e]pyrene exhibited a primary particle diameter of 10 nm and similar primary particles, whereas the morphology of the soot formed by the addition of PAHs with zigzag sites clearly indicated a structure with a primary particle diameter of 20-40 nm. These observations indicate that the incipient soot is formed by the formation of dimers or small clusters of large PAHs via the mechanisms of aromatic molecule addition to aromatic radicals referred to as the PAH-addition cyclization (PAR-AC) mechanism at high temperatures, whereas moderate-sized PAHs developed via the hydrogen-abstraction-carbon-addition (HACA) mechanism form clusters and incipient soot at relatively low temperatures. (C) 2015 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
机译:在等温层流中以1400-1650 K的温度将原料(包括苯,乙炔和带有乙炔或2-7环PAH的苯)热解。使用扫描迁移率分析了烟灰和新生烟灰的粒度分布(PSD)粒度仪(SMPS)。使用扫描电子显微镜(SEM)检查了具有相同迁移率粒径的颗粒的形态,其中通过差动迁移率分析仪(DMA)辅助的热泳采样对网格进行了采样。与通过苯和PAH添加剂的热解产生的烟灰相比,在1400 K的乙炔热解产生的烟灰表现出最高的浓度和对数正态分布。在1500 K下,具有三个或三个以上带有锯齿形位点的环的PAH的热解显着增加了数字浓度,尽管添加的碳浓度小于乙炔。具有三个扶手椅位的二苯并[a,e] py的添加抑制了烟灰的形成,表明海湾位置易于形成,且各向异性PAHs的形成抑制了二聚化。通过添加二苯并[a,e] formed形成的烟灰的形态显示出10 nm的初级粒径和相似的初级粒子,而通过添加带有锯齿形位点的PAH形成的烟尘的形态清楚地表明其结构为初级粒径为20-40 nm。这些观察结果表明,初生烟灰是通过在高温下通过芳族分子向芳族自由基中添加芳族分子的机理(称为PAH加成环化(PAR-AC)机理)形成大PAH的二聚体或小簇而形成的通过吸氢加碳(HACA)机理开发的大尺寸PAH在相对较低的温度下会形成团簇和初期烟ot。 (C)2015年燃烧研究所。由Elsevier Inc.出版。保留所有权利。

著录项

  • 来源
    《Combustion and Flame》 |2015年第6期|2670-2678|共9页
  • 作者单位

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan;

    Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan|ASAHI CARBON CO LTD, Higashi Ku, Niigata 9500883, Japan;

    ASAHI CARBON CO LTD, Higashi Ku, Niigata 9500883, Japan;

    ASAHI CARBON CO LTD, Higashi Ku, Niigata 9500883, Japan;

  • 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

    Soot; PAH; Nascent soot; Particle mobility and sizing; Particle size distribution;

    机译:烟灰;PAH;新生烟灰;颗粒迁移率和施胶;颗粒尺寸分布;

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