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首页> 外文期刊>Environmental Science & Technology >Primary Formation of Highly Oxidized Multifunctional Products in the OH-Initiated Oxidation of Isoprene: A Combined Theoretical and Experimental Study
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Primary Formation of Highly Oxidized Multifunctional Products in the OH-Initiated Oxidation of Isoprene: A Combined Theoretical and Experimental Study

机译：OH引发的异戊二烯氧化中高氧化多功能产物的初步形成：理论和实验研究相结合

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摘要

It is generally assumed that isoprene-derived secondary organic aerosol (SOA) precursors are mainly formed from the secondary reactions of intermediate products with OH radicals in the gas phase and multiphase oxidation in particles. In this paper, we predicted a theoretical mechanism for the primary formation of highly oxygenated molecules (HOM) in the gas phase through successive intramolecular H-shifts and O-2 addition in the specific Z-delta isomer of hydroxyl-peroxy radicals and alkoxy radicals. The position of O-2 addition is different from that in forming hydroperoxy aldehydes. The prediction was further supported experimentally by successfully identifying a few highly oxidized peroxy radicals and closed-shell products such as C5H9O7,9, C5H10O6,7,8, and C4H8O5 in a flow reactor by chemical ionization mass spectrometry at air pressure. These HOM products could serve as important precursors to isoprene-derived SOA. Further modeling studies on the effect of NO concentration suggested that HOM formation could account for up to, similar to 11% of the branching ratio (similar to 9% from the 4-OH channel and similar to 2% from the 1-OH channel) in the reaction of isoprene with OH when the lifetimes of peroxy radicals due to bimolecular reactions are similar to 100 s, which is typical in forest regions.
机译：通常认为，异戊二烯衍生的次级有机气溶胶（SOA）前体主要由中间产物与气相中的OH自由基和颗粒中的多相氧化形成的二次反应形成。在本文中，我们预测了通过连续的分子内H位移和在羟基-过氧自由基和烷氧基的特定Z-δ异构体中添加O-2来在气相中初步形成高氧分子（HOM）的理论机制。 O-2加成的位置与形成氢过氧醛的位置不同。通过在空气压力下通过化学电离质谱法在流动反应器中成功鉴定出一些高度氧化的过氧自由基和闭壳产物（如C5H9O7,9，C5H10O6、7,8和C4H8O5），进一步为该预测提供了实验依据。这些HOM产品可以用作异戊二烯衍生的SOA的重要前体。关于NO浓度影响的进一步模型研究表明，HOM的形成最多可占支化比率的11％（类似于4-OH通道的9％和1-OH通道的2％）。当异戊二烯与OH反应时，双分子反应引起的过氧自由基的寿命接近100 s，这在森林地区是典型的。

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  • 来源
    《Environmental Science & Technology》 |2018年第21期|12255-12264|共10页
  • 作者

    Wang Sainan; Riva Matthieu; Yan Chao; Ehn Mikael; Wang Liming;

  • 作者单位

    South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China;

    Univ Helsinki, Fac Sci, Inst Atmospher & Earth Syst Res Phys, POB 64, FIN-00014 Helsinki, Finland;

    Univ Claude Bernard Lyon 1, Univ Lyon, IRCELYON, CNRS, F-69626 Villeurbanne, France;

    South China Univ Technol, Guangdong Prov Key Lab Atmospher Environm & Pollu, Guangzhou 510006, Guangdong, Peoples R China;

  • 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);美国《化学文摘》(CA);
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