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Functional group composition of organic aerosol from combustion emissions and secondary processes at two contrasted urban environments^

机译：来自两个对比城市环境中燃烧排放和次级过程的有机气溶胶的官能团组成^

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摘要

The quantification of major functional groups in atmospheric organic aerosol (OA) provides a constraint on the types of compounds emitted and formed in atmospheric conditions. This paper presents functional group composition of organic aerosol from two contrasted urban environments: Marseille during summer and Grenoble during winter. Functional groups were determined using a tandem mass spec-trometry approach, enabling the quantification of carboxylic (RCOOH), carbonyl (RCOR'), and nitro (RNO_2) functional groups. Using a multiple regression analysis, absolute concentrations of functional groups were combined with those of organic carbon derived from different sources in order to infer the functional group contents of different organic aerosol fractions. These fractions include fossil fuel combustion emissions, biomass burning emissions and secondary organic aerosol (SOA). Results clearly highlight the differences between functional group fingerprints of primary and secondary OA fractions. OA emitted from primary sources is found to be moderately functionalized, as about 20 carbons per 1000 bear one of the functional groups determined here, whereas SOA is much more functionalized, as in average 94 carbons per 1000 bear a functional group under study. Aging processes appear to increase both RCOOH and RCOR' functional group contents by nearly one order of magnitude. Conversely, RNO_2 content is found to decrease with photochemical processes. Finally, our results also suggest that other functional groups significantly contribute to biomass smoke and SOA. In particular, for SOA, the overall oxygen content, assessed using aerosol mass spectrometer measurements by an O:C ratio of 0.63, is significantly higher than the apparent O:C* ratio of 0.17 estimated based on functional groups measured here. A thorough examination of our data suggests that this remaining unexplained oxygen content can be most probably assigned to alcohol (ROH), organic peroxides (ROOH), organonitrates (RONO_2) and/or organosulfates (ROSO_3H).
机译：大气有机气溶胶（OA）中主要官能团的定量分析对大气条件下释放和形成的化合物类型提供了限制。本文介绍了两种截然不同的城市环境中有机气溶胶的官能团组成：夏季的马赛和冬季的格勒诺布尔。使用串联质谱法确定官能团，从而能够定量羧基（RCOOH），羰基（RCOR'）和硝基（RNO_2）官能团。使用多元回归分析，将官能团的绝对浓度与衍生自不同来源的有机碳的绝对浓度相结合，以推断出不同有机气溶胶级分的官能团含量。这些部分包括化石燃料燃烧排放物，生物质燃烧排放物和二次有机气溶胶（SOA）。结果清楚地突出了主要和次要OA组分的功能组指纹之间的差异。发现从主要来源发出的OA具有中等功能性，因为每千个碳中约有20个碳具有此处确定的官能团之一，而SOA的功能性则高得多，因为每千个碳中平均有94个碳具有所研究的官能团。老化过程似乎使RCOOH和RCOR'官能团的含量均增加了近一个数量级。相反，发现RNO_2的含量随着光化学过程而降低。最后，我们的研究结果还表明，其他官能团也对生物质烟雾和SOA做出了重要贡献。特别是对于SOA，使用气溶胶质谱仪测量的O：C比为0.63评估的总氧含量明显高于根据此处测得的官能团估算的表观O：C *比为0.17。彻底检查我们的数据表明，剩余的无法解释的氧含量很可能归因于酒精（ROH），有机过氧化物（ROOH），有机硝酸盐（RONO_2）和/或有机硫酸盐（ROSO_3H）。

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  • 来源
    《Atmospheric environment》 |2013年第8期|308-320|共13页
  • 作者

    Imad El Haddad; Nicolas Marchand; Barbara DAnna; Jean Luc Jaffrezo; Henri Wortham;

  • 作者单位

    Aix-Marseille Univ, Laboratoire Chimie Environnement, 13331 Marseille Cedex 03, Franc,CNRS, FRE 3416, 13331 Marseille Cedex O3, France,Paul Scherrer lnstitut (PSI), Laboratory of Atmospheric Chemistry, 5232 Villigen PSI, Switzerland;

    Aix-Marseille Univ, Laboratoire Chimie Environnement, 13331 Marseille Cedex 03, Franc,CNRS, FRE 3416, 13331 Marseille Cedex O3, France;

    Universite de Lyon 1/CNRS, UMR5256, IRCELYON, Institut de Recherches sur la Catalyse et l'Environnement de Lyon, Villeurbanne, France;

    University Joseph Fourier-Grenoble 1 -CNRS, UMR 5183, Laboratoire de Claciologie et Geophysique de VEnvironnement, Saint Martin d'Heres 38402, France;

    Aix-Marseille Univ, Laboratoire Chimie Environnement, 13331 Marseille Cedex 03, Franc,CNRS, FRE 3416, 13331 Marseille Cedex O3, France;

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  • 正文语种 eng
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  • 关键词

    Oxygenated functional groups; Primary organic aerosol; Secondary organic aerosol; Photochemical aging; Van Krevelen diagram;

    机译：含氧官能团;初级有机气溶胶;二次有机气溶胶;光化学老化;Van Krevelen图;

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