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Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

机译：串联质谱法测定环境和源有机气溶胶的官能团组成

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摘要

The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCIMS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R0 respectively) and precursor ion (nitro groups, R-NO_2) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also domi- nated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitroand carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional group mass spectra of all aerosols under study are presented, and additional perspectives offered by the mass spectra in terms of OA characterisation are discussed.
机译：使用最近开发的基于大气压化学电离串联质谱（APCIMS / MS）的分析方法，研究了各种有机气溶胶（OA）的官能团组成。通过串联质谱仪的中性损失（分别为羧基和羰基，R-COOH和R-CO-R0）和前驱离子（硝基，R-NO_2）扫描模式定量测定三个官能团的含量。研究了主要的有机气溶胶来源：主要气溶胶来源的车辆排放和木材燃烧;以及通过邻二甲苯的光氧化产生的次级有机气溶胶（SOA）。结果显示这些来源气溶胶的官能团含量存在显着差异。实验室产生的SOA主要由羰基组成，而木材燃烧颗粒中的羧酸占优势。另一方面，车辆排放物的特征是强烈的硝基含量。这三个官能团的总量占有机碳的1.7％（载体）至13.5％（邻二甲苯光氧化）。然后，使用诊断功能组比率初步区分在强烈的冬季污染事件中位于阿尔卑斯山山谷（法国夏蒙尼）的城市背景环境中收集的颗粒来源。所研究的三个官能团占该环境气溶胶中有机碳的总官能化率为2.2％至3.8％，这也是由羧基部分控制的。在冬季深高山山谷的这一特殊案例研究中，我们表明，硝基和羰基与羧基的诊断比可以作为区分来源的有用工具。在这些条件下，木材燃烧OA在总OA浓度中占主导地位。该结果通过有机标记物源分配方法得到了证实，该方法评估木材燃烧有机碳的贡献约为60％。最后，给出了所有正在研究的气溶胶的官能团质谱的例子，并讨论了由质谱在OA表征方面的其他观点。

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