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Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway

机译:通过非IEPOX途径高效异戊二烯二次有机气溶胶形成

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摘要

With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are subjects of intense research because particles affect Earth's climate and local air quality. In the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2 or more higher than those typically used in coupled chemistry climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 50 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO_2 radicals is key to understanding the efficient SOA formation and the NO_x-dependent yields described here and in the literature. These insights allow for improved quantitative estimates of SOA formation in the preindustrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest that a more-complex representation of NO_x-dependent SOA yields may be important in models.
机译:异戊二烯具有大的全球排放率和高反应活性,对大气化学和组成具有深远的影响。异戊二烯转化为次级有机气溶胶(SOA)的大气途径以及诸如氧化氮和硫等人为污染物如何影响该过程的过程一直是研究的热点,因为颗粒会影响地球的气候和当地空气质量。在没有氮氧化物和反应性含水种子粒子的情况下,我们测量的异戊二烯光化学氧化的SOA质量产率高达15%,这是偶合化学气候模型中通常使用的那些因子的2倍或更多。随着添加一氧化氮(NO)的增加,SOA产量最初是恒定的,但随后在输入浓度高于50 ppbv时急剧下降。气溶胶分子组成的在线测量结果表明,第二代RO_2自由基的命运对于理解此处和文献中描述的有效SOA形成和依赖NO_x的产率至关重要。这些见解允许改进工业界前大气和人为影响有限的生物富集区域中SOA形成的定量估计,并表明在模型中更复杂地表示依赖NO_x的SOA产量可能很重要。

著录项

  • 来源
    《Environmental Science & Technology》 |2016年第18期|9872-9880|共9页
  • 作者单位

    Atmospheric Sdences and Global Change Division, Pacific Northwest National Laboratory Richland, Washington 99352 United States;

    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States;

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195, United States;

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195, United States;

    Atmospheric Sdences and Global Change Division, Pacific Northwest National Laboratory Richland, Washington 99352 United States;

    Paulson School of Engineering and Applied Sciences and Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States;

    Paulson School of Engineering and Applied Sciences and Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States;

    Department of Chemistry, University of Helsinki, Helsinki FI-00014, Finland;

    Department of Chemistry, University of Helsinki, Helsinki FI-00014, Finland;

    Department of Environmental Sciences and Engineering, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, University of North Carolina, Chapel Hill, North Carolina 27599 United States;

    Atmospheric Sdences and Global Change Division, Pacific Northwest National Laboratory Richland, Washington 99352 United States;

    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States,Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195, 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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  • 正文语种 eng
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  • 入库时间 2022-08-17 13:58:55

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