半挥发产物气相分配比的变化影响α-蒎烯光氧化产生的二次有机气溶胶

IF 3.7 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES
Shijie Liu , Xinbei Xu , Si Zhang , Rongjie Li , Zheng Li , Can Wu , Rui Li , Feiyong Chen , Guiqin Zhang , Gehui Wang
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引用次数: 0

摘要

α-蒎烯是二次有机气溶胶(SOA)的重要前体之一。α-蒎烯衍生SOA的形成受到NOx的强烈影响。然而,NOx对α-蒎烯衍生的SOA形成的影响,特别是NOx对SOA产率的增强作用仍未全面了解。本研究通过常压室在不同NOx浓度下进行了α-蒎烯光氧化实验。α-蒎烯SOA的产率最初随着NOx浓度的升高而升高,但随后随着NOx浓度的升高而降低。在115 ppb α-蒎烯和250 ppb α-蒎烯条件下,SOA的最高收率分别为8.0%和26.2%。发现随着NOx的增加,SOA质量浓度(M0)与SOA产率的拟合曲线向下移动,表明氧化产物的挥发性逐渐增加。然而,在每个光氧化过程中,随着M0的增加,SOA产率更高,这归因于增强的气-气溶胶相分配比。不同NOx实验中SOA产率与M0的关系表明,在低NOx条件下,随着NOx浓度的增加,VOC消耗增加导致的M0升高仍然会促进SOA产率的提高,尽管Odum曲线的位置向下移动。也就是说,在促进NOx对SOA产率的影响时,应考虑到M0的变化导致气-气溶胶-相分配比的变化。本研究还定量分析了含氮有机化合物(NOCs)浓度与NOx的关系。低氮氧化物条件下noc形成的快速增加是另一个促进SOA产量增加的因素。这项研究极大地增强了我们对NOx促进SOA产量的机制的理解,并为改进SOA形成的精确模拟提供了关键信息。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Changes in gas-to-aerosol-phase partitioning ratio of semi-volatile products affect secondary organic aerosol formation from α-pinene photooxidation
α-Pinene is one of the most important precursors of secondary organic aerosols (SOA). The formation of α-pinene derived SOA is strongly affected by NOx. However, the effects of NOx on α-pinene derived SOA formation, especially the enhancing effect of NOx on SOA yield, are still not comprehensively understood. A series of α-pinene photooxidation experiments were performed at different NOx concentrations through an atmospheric chamber in this study. The yields of α-pinene SOA initially increased with rising NOx concentrations but subsequently decreased at higher levels. The maximum SOA yields were 8.0 % and 26.2 % in 115 ppb and 250 ppb α-pinene experiments, respectively. It is found that the fitted curves of SOA mass concentration (M0) versus SOA yield shift downward with increasing NOx, which means the volatility of the oxidation products gradually increases. However, the higher SOA yields observed with the increasing M0 during each photooxidation process, which were attributed to the enhanced gas-to-aerosol-phase partitioning ratio. The relationship of SOA yields with M0 for different NOx experiments shows that, under low-NOx conditions, the elevation in M0 which was driven by enhanced VOC consumption would still promote SOA yield with increasing NOx concentrations, despite the position of the Odum curve shift downward. That is to say, the change of M0 leading to the variation gas-to-aerosol-phase partitioning ratio should be taken into account in the facilitation of NOx on SOA yield. The relation of nitrogen-containing organic compound (NOCs) concentrations with NOx was also quantified in this study. The rapid increase in NOCs formation under low NOx conditions is another factor contributing to the increase of SOA yields. This study greatly enhances our understanding of the mechanisms by which NOx promotes SOA yields, and provides crucial information for improving the accurate simulation of SOA formation.
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来源期刊
Atmospheric Environment
Atmospheric Environment 环境科学-环境科学
CiteScore
9.40
自引率
8.00%
发文量
458
审稿时长
53 days
期刊介绍: Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.
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