Resolving ambient organic aerosol formation and aging pathways with simultaneous molecular composition and volatility observations.
Resolving ambient organic aerosol formation and aging pathways with simultaneous molecular composition and volatility observations.
复制标题
通过同时进行分子组成和挥发性观察，解决环境有机气溶胶的形成和老化途径。
DOI：
10.1021/acsearthspacechem.9b00302
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发表时间：
2020
影响因子：
3.4
通讯作者：
J. Thornton
中科院分区：
文献类型：
--
作者：
B. H. Lee;E. D’Ambro;F. Lopez‐Hilfiker;S. Schobesberger;C. Mohr;M. Zawadowicz;Jiu;J. Shilling;Weiwei Hu;B. Palm;J. Jimenez;L. Hao;A. Virtanen;Haofei Zhang;A. Goldstein;H. Pye;J. Thornton
有机气溶胶(OA)是大气细颗粒物质量的重要组成部分。然而，负责大多数骨性关节炎的前体和化学过程很少被最终确定。我们利用从15个实验室OA形成实验中获得的数百个同时测量的分子组分的在线观察，在其有效饱和蒸汽浓度的限制下，对VOC前体和随后的化学路径进行归属，这些化学路径导致在两个森林地区测量到的绝大多数OA质量。我们发现，调节OA组成和挥发性的前体和化学途径是从几个小时到几天的动态变化，它们的变化是由多种氧化剂之间的耦合作用驱动的。物理和光化学老化的程度，以及NOx对其的调节，是唯一全面描述OA的组成-挥发性的关键。因此，我们的发现为空气质量和地球系统模型中的办公自动化描述的发展提供了一些最完整的机械层面的指导。
Organic aerosol (OA) constitutes a significant fraction of atmospheric fine particle mass. However, the precursors and chemical processes responsible for a majority of OA are rarely conclusively identified. We use online observations of hundreds of simultaneously measured molecular components obtained from 15 laboratory OA formation experiments with constraints on their effective saturation vapor concentrations to attribute the VOC precursors and subsequent chemical pathways giving rise to the vast majority of OA mass measured in two forested regions. We find that precursors and chemical pathways regulating OA composition and volatility are dynamic over hours to days, with their variations driven by coupled interactions between multiple oxidants. The extent of physical and photochemical aging, and its modulation by NOx, were key to a uniquely comprehensive combined composition-volatility description of OA. Our findings thus provide some of the most complete mechanistic-level guidance to the development of OA descriptions in air quality and Earth system models.
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影响因子：
3.4
作者：
Massoli, Paola;Stark, Harald;Worsnop, Douglas R.
通讯作者：
Worsnop, Douglas R.
影响因子：
6.3
作者：
Hu, W. W.;Campuzano-Jost, P.;Jimenez, J. L.
通讯作者：
Jimenez, J. L.
影响因子：
64.8
作者：
McFiggans, Gordon;Mentel, Thomas F.;Kiendler-Scharr, Astrid
通讯作者：
Kiendler-Scharr, Astrid
影响因子：
3.4
作者：
Claflin, Megan S.;Krechmer, Jordan E.;Ziemann, Paul J.
通讯作者：
Ziemann, Paul J.