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Parameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NO_x Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases

机译:不同NO_x水平下异戊二烯氧化半挥发产物的参数化产率:化学老化和反应气体壁损失的影响

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摘要

We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NOx levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NOx-sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NOx levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box model can be expanded to include more explicit chemical aging processes and help ultimately bridge the gap between the process based understanding of SOA formation from VOC oxidation and the bulk-yield parametrizations used in chemical transport models.
机译:我们开发了一种可参数化的盒模型,以使用腔室测量法经验性地从VOC氧化中得出半挥发性产品的产率,同时明确考虑了在不同NOx下的多代化学老化过程(例如气相裂解和功能化以及气溶胶低聚和光解)。水平以及颗粒和气体向室壁的损失。以异戊二烯的氧化为例,我们表明,有关VOx氧化产物对NOx敏感的多代老化过程的假设对参数化产物的收率和SOA形成有很大影响。我们在不同的NOx水平下从异戊二烯氧化中获得了半挥发性产物的产率。但是,我们强调,这些产品的产量必须与化学运输模型中相应的多代老化方案结合使用。随着更多关于VOC氧化形成SOA的机理的见解,我们的盒模型可以扩展到包括更明确的化学老化过程,并最终帮助弥合基于过程的VOC氧化对SOA形成的理解与用于SOC的大批量参数化之间的差距。化学运输模型。

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  • 来源
    《Environmental Science & Technology》 |2018年第16期|9225-9234|共10页
  • 作者单位

    Peking Univ, Dept Atmospher & Ocean Sci, Sch Phys, Beijing 100871, Peoples R China;

    Pacific Northwest Natl Lab, Washington, DC 99352 USA;

    Peking Univ, Dept Atmospher & Ocean Sci, Sch Phys, Beijing 100871, Peoples R China;

    Lund Univ, Div Nucl Phys, POB 118, S-22100 Lund, Sweden;

    Pacific Northwest Natl Lab, Washington, DC 99352 USA;

    Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA;

    Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA;

    Pacific Northwest Natl Lab, Washington, DC 99352 USA;

    Pacific Northwest Natl Lab, Washington, DC 99352 USA;

    Univ Calif Davis, Dept Civil & Environm Engn, Davis, CA 95616 USA;

  • 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);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

  • 入库时间 2022-08-17 13:56:44

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