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Influence of the NO/NO_2 Ratio on Oxidation Product Distributions under High-NO Conditions

机译：NO / NO_2比率对高无条件下氧化产品分布的影响

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摘要

Organic oxidation reactions in the atmosphere can be challenging to parse due to the large number of branching points within each molecule's reaction mechanism. This complexity can complicate the attribution of observed effects to a particular chemical pathway. In this study, we simplify the chemistry of atmospherically relevant systems, and particularly the role of NO_x, by generating individual alkoxy radicals via alkyl nitrite photolysis (to limit the number of accessible reaction pathways) and measuring their product distributions under different NO/NO_2 ratios. Known concentrations of NO in the classically "high-NO" range are maintained in the chamber, thereby constraining first-generation RO_2 (peroxy radicals) to react nearly exclusively with NO. Products are measured in both the gas phase (with a proton-transfer reaction mass spectrometer) and the particle phase (with an aerosol mass spectrometer). We observe substantial differences in measured products under varying NO/NO_2 ratios (from ～0.1 to >1); along with modeling simulations using the Master Chemical Mechanism (MCM), these results suggest indirect effects of NO_x chemistry beyond the commonly cited RO_2 + NO reaction. Specifically, lower-NO/NO_2 ratios foster higher concentrations of secondary OH, higher concentrations of peroxyacyl nitrates (PAN, an atmospheric reservoir species), and a more highly oxidized product distribution that results in more secondary organic aerosol (SOA). The impact of NO_x concentration beyond simple RO_2 branching must be considered when planning laboratory oxidation experiments and applying their results to atmospheric conditions.
机译：由于每种分子内的反应机制内的大量分支点，大气中的有机氧化反应可能是挑战的。这种复杂性可以使观察到的效果的归因复杂化对特定化学途径。在这项研究中，我们通过通过烷基亚硝酸盐光解（限制可接近的反应途径）和测量不同NO / NO_2比率的烷基氧基自由基来简化大气相关系统的化学，尤其是NO_X的作用。 。在经典的“高”范围内的已知浓度保持在腔室中，从而限制了第一代RO_2（过氧基团）以几乎完全反应。在气相（具有质子转移反应质谱仪）和颗粒相（用气溶胶质谱仪）中测量产品。我们在不同的NO / NO_2比率下观察测量产品的大量差异（从〜0.1至> 1）;除了使用母材化学机制（MCM）的建模模拟，这些结果表明NO_X化学超出常识的RO_2 + NO反应的间接影响。具体地，低/ NO_2比率促进较高浓度的仲珠，较高浓度的过氧羰基硝酸盐（锅，大气储层物种），以及更高度氧化的产物分布，导致更多的二次有机气溶胶（SOA）。在规划实验室氧化实验并将其结果应用于大气条件时，必须考虑NO_X浓度超出简单RO_2分支的影响。

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  • 来源
    《Environmental Science & Technology》 |2021年第10期|6594-6601|共8页
  • 作者

    Kevin J. Nihill; Qing Ye; Francesca Majluf; Jordan E. Krechmer; Manjula R. Canagaratna; Jesse H. Kroll;

  • 作者单位

    Department of Civil and Environmental Engineering Massachusetts Institute of Technology Cambridge Massachusetts 02139 United States;

    Department of Civil and Environmental Engineering Massachusetts Institute of Technology Cambridge Massachusetts 02139 United States;

    Aerodyne Research Inc. Billerica Massachusetts 01821 United States;

    Aerodyne Research Inc. Billerica Massachusetts 01821 United States;

    Aerodyne Research Inc. Billerica Massachusetts 01821 United States;

    Department of Civil and Environmental Engineering Massachusetts Institute of Technology Cambridge Massachusetts 02139 United States;

  • 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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