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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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The functional group composition of various organic aerosols (OA) isinvestigated using a recently developed analytical approach based onatmospheric pressure chemical ionisation-tandem mass spectrometry(APCI-MS/MS). The determinations of three functional groups contents areperformed quantitatively by neutral loss (carboxylic and carbonyl groups,R-COOH and R-CO-R′ respectively) and precursor ion (nitro groups,R-NO2) scanning modes of a tandem mass spectrometer. Major organicaerosol sources are studied: vehicular emission and wood combustion forprimary aerosol sources; and a secondary organic aerosol (SOA) producedthrough photooxidation of o-xylene. The results reveal significant differencesin the functional group contents of these source aerosols. The laboratorygenerated SOA is dominated by carbonyls while carboxylics are preponderatein the wood combustion particles. On the other hand, vehicular emissions arecharacterised by a strong nitro content. The total amount of the threefunctional groups accounts for 1.7% (vehicular) to 13.5% (o-xylenephotooxidation) of the organic carbon. Diagnostic functional group ratiosare then used to tentatively discriminate sources of particles collected inan urban background environment located in an Alpine valley (Chamonix,France) during a strong winter pollution event. The three functional groupsunder study account for a total functionalisation rate of 2.2 to 3.8% ofthe organic carbon in this ambient aerosol, which is also dominated bycarboxylic moieties. In this particular case study of a deep alpine valleyduring winter, we show that the nitro- and carbonyl-to-carboxylic diagnosticratios can be a useful tool to discriminate sources. In these conditions,the total OA concentrations are highly dominated by wood combustion OA. Thisresult is confirmed by an organic markers source apportionment approachwhich assess a wood burning organic carbon contribution of about 60%.Finally, examples of functional group mass spectra of all aerosols understudy are presented, and additional perspectives offered by the mass spectrain 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(APCI-MS / MS)的分析方法,研究了各种有机气溶胶(OA)的官能团组成。通过中性丢失(分别为羧基和羰基,R-COOH和R-CO-R')和前体离子(硝基,R-NO 2 )扫描定量测定三个官能团含量串联质谱仪的模式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;和通过 o -二甲苯的光氧化产生的次级有机气溶胶(SOA)。结果表明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以羰基为主,而木材燃烧颗粒中以羧酸为主。另一方面,车辆排放物的特征在于强的硝基含量。三个官能团的总量占有机碳的1.7%(媒介)至13.5%(邻二甲苯光氧化)。然后,使用诊断性官能团比率来初步区分在强烈的冬季污染事件中位于阿尔卑斯山谷(法国夏蒙尼)的城市背景环境中收集的颗粒物来源。所研究的三个官能团占该环境气溶胶中有机碳的总功能化率为2.2%至3.8%,这也是以羧基部分为主。在冬季深高山峡谷的这一特殊案例研究中,我们表明硝基和羰基至羧基的诊断比值可以作为区分来源的有用工具。在这些条件下,总的OA浓度在很大程度上由木材燃烧OA决定。通过有机标记物源分摊方法评估了这一结果,该方法评估了木材燃烧的有机碳贡献率约为60%。最后,给出了所有正在研究的气溶胶的官能团质谱的示例,并从OA表征的角度提供了质谱的其他观点。讨论过。

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