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首页> 外文期刊>Environmental Science & Technology >Secondary Organic Aerosol Formation from in-Use Motor Vehicle Emissions Using a Potential Aerosol Mass Reactor
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Secondary Organic Aerosol Formation from in-Use Motor Vehicle Emissions Using a Potential Aerosol Mass Reactor

机译：使用潜在的气溶胶质量反应器，在使用中的机动车排放中形成二次有机气溶胶

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摘要

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ～0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ～2.9 ± 1.6 Tg SOA yr~(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.
机译：使用在宾夕法尼亚州匹兹堡的公路隧道中部署的潜在气溶胶质量（PAM）流动反应器，研究了在用车辆排放中形成的次级有机气溶胶（SOA）。实验包括使废气占主导地位的隧道空气通过PAM反应器，使其在等效大气氧化的〜0.3天至9.3天的综合羟基自由基（OH）中暴露。在交通繁忙时进行了实验，当时该车队的燃油消耗量至少为80％的轻型汽油车。 SOA产量的峰值出现在等效大气氧化2-3天后。额外的OH暴露可能降低了SOA的产生，这是由于从官能化转变为以碎片为主的反应机理。光氧化还产生大量的硝酸铵，通常超过SOA的质量。使用SOA模型进行分析表明，未指定的有机物（即，未解析的复杂混合物）是非常重要的前体类型，并且气体和颗粒的多代处理对更长的时间范围。 PAM反应器内部有机气溶胶的化学演化似乎与在大气中观察到的相似。未氧化的一级有机气溶胶的质谱非常类似于周围的类烃有机气溶胶（HOA）。在将废气老化相当于大气氧化几小时后，有机气溶胶与半挥发性氧化有机气溶胶（SV-OOA）最相似，然后与暴露于较高OH的低挥发性有机气溶胶（LV-OOA）相似。缩放数据表明，在美国，移动源贡献了约2.9±1.6 Tg SOA yr〜（-1），这是国家排放清单报告的所有移动源颗粒物排放量的6倍。这突显了SOA形成的重要因素，从汽车尾气到城市地区周围的颗粒物浓度。

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  • 来源
    《Environmental Science & Technology》 |2014年第19期|11235-11242|共8页
  • 作者

    Daniel S. Tkacik; Andrew T. Lambe; Shantanu Jathar; Xiang Li; Albert A. Presto; Yunliang Zhao; Donald Blake; Simone Meinardi; John T. Jayne; Philip L. Croteau; Allen L. Robinson;

  • 作者单位

    Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States, Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States;

    Aerodyne Research, Inc., Billerica, Massachusetts 01821, United States;

    Civil and Environmental Engineering, University of California, Davis, Davis, California 95616, United States;

    Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States, Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States;

    Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States, Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States;

    Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States, Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States;

    Department of Chemistry, University of California, Irvine, Irvine, California 92697-2025, United States;

    Department of Chemistry, University of California, Irvine, Irvine, California 92697-2025, United States;

    Aerodyne Research, Inc., Billerica, Massachusetts 01821, United States;

    Aerodyne Research, Inc., Billerica, Massachusetts 01821, United States;

    Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States, Mechanical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, 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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