Molecular Composition of Boreal Forest Aerosol from Hyytiala, Finland, Using Ultrahigh Resolution Mass Spectrometry
Molecular Composition of Boreal Forest Aerosol from Hyytiala, Finland, Using Ultrahigh Resolution Mass Spectrometry
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DOI：
10.1021/es3051636
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发表时间：
2013-05-07
影响因子：
11.4
通讯作者：
Kalberer, Markus
中科院分区：
文献类型：
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作者：
Kourtchev, Ivan;Fuller, Stephen;Kalberer, Markus
有机化合物是对流层细颗粒物的重要组成部分。在这项研究中，我们采用直接输注纳米电喷雾（nanoESI）高分辨质谱（UHR-MS）和液相色谱LC/ESI-UHR-MS分析的PM 1气溶胶样品的有机部分收集了两个星期的时间在北方森林网站（Hyytiala），芬兰南部。采用负离子化模式下的nanoESI-UHR-MS鉴别了元素式（总计460-730），并将其归因于分子量低于400的有机化合物。Kendrick质量亏损和货车Krevelen方法用于识别化合物类别和检测到的物质的质量分布。气溶胶的分子组成在具有不同空气质量历史的样品之间变化很大。在与大陆气团相关的日子里，观察到氮、硫和高氧化有机化合物的数量增加。然而，与大西洋气团历史的样品的特点是存在同源系列的不饱和和饱和的C-12-C-20脂肪酸，表明其海洋起源。据我们所知，我们第一次表明，从UHR-MS分析获得的高度详细的化学成分可以清楚地联系到气象参数和痕量气体浓度，是相关的大气氧化过程。额外的LC/ESI-UHR-MS分析揭示了29种物质，其主要归因于生物挥发性化合物BVOC的氧化产物（即，α，β-蒎烯、δ（3）-<$烯、柠檬烯和异戊二烯），支持直接灌注分析的结果。
Organic compounds are important constituents of fine particulate matter (PM) in the troposphere. In this study, we applied direct infusion nanoelectrospray (nanoESI) ultrahigh resolution mass spectrometry (UHR-MS) and liquid chromatography LC/ESI-UHR-MS for the analysis of the organic fraction of PM1 aerosol samples Collected over a two week period at a boreal forest site (Hyytiala), southern Finland. Elemental formulas (460-730 in total), were identified With nanoESI-UHR-MS in the negative ionization mode and attributed to organic compounds with a molecular weight below 400. Kendrick Mass Defect, and Van Krevelen approaches were used to identify compound classes and mass distributions of the detected species. The molecular composition of the aerosols strongly varied between samples with different air mass histories. An increased number of nitrogen, sulfur, and highly oxygenated organic compounds was observed during the days associated with continental air masses. However, the samples with Atlantic air mass history were marked by a presence of homologous series of unsaturated and saturated C-12-C-20 fatty acids suggesting their marine origin. To our knowledge, we show for the first time that the highly detailed chemical composition obtained from UHR-MS analyses can be clearly linked to meteorological parameters and trace gases concentrations that are relevant to atmospheric oxidation processes. The additional LC/ESI-UHR-MS analysis revealed 29 species, which were mainly attributed to oxidation products of biogenic volatile compounds BVOCs (i.e., alpha,beta-pinene, Delta(3)-carene, limonene, and isoprene) supporting the results from the direct infusion analysis.