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德国奥格斯堡环境准超细颗粒物(PM)的有机形态:季节性变化和来源解析。

Organic speciation of ambient quasi-ultrafine particulate matter (PM) in Augsburg, Germany: Seasonal variability and source apportionment.

机构信息

Joint Mass Spectrometry Center, Cooperation Group Comprehensive Molecular Analytics, Helmholtz Zentrum München, Neuherberg, Germany; Joint Mass Spectrometry Center, Chair of Analytical Chemistry, University of Rostock, Germany.

Joint Mass Spectrometry Center, Cooperation Group Comprehensive Molecular Analytics, Helmholtz Zentrum München, Neuherberg, Germany.

出版信息

Sci Total Environ. 2018 Feb 15;615:828-837. doi: 10.1016/j.scitotenv.2017.09.158. Epub 2017 Oct 7.

DOI:10.1016/j.scitotenv.2017.09.158
PMID:28992506
Abstract

To investigate the organic composition and their sources of very fine atmospheric particulate matter (PM), size-segregated PM was sampled using rotating drum impactor (RDI) in series with a sequential filter sampler in Augsburg, Germany, from April 2014 to February 2015. Organic speciation analysis and organic carbon/elemental carbon (OC/EC) analysis was performed for the smallest size fraction PM (PM<360nm). Different OC fractions were determined by thermal optical EC/OC analyzer, and OC2, OC3 and OC4 refer to OC fractions that were derived at 280, 480 and 580°C, respectively. Positive matrix factorization (PMF) analysis was applied for source apportionment study. PMF resolved 5 sources including biogenic dominated secondary organic aerosol (bioSOA), isoprene dominated SOA (isoSOA), traffic, biomass burning (BB) and biomass burning originated SOA (bbSOA). On annual average, PMF results indicate the largest contribution of biogenic originated SOA (bioSOA plus isoSOA) to OC, followed by traffic and then BB related sources (BB plus bbSOA). Traffic was found to be associated with the smallest particles; whereas bioSOA and BB are associated with larger particles. Secondary organic marker compounds from biogenic precursors, OC2, OC3 and bioSOA, isoSOA source factors show summer maximum. Polycyclic aromatic hydrocarbons (PAHs), biomass burning markers, OC4 and BB, bbSOA source factors show winter maximum. Hopanes and the traffic source factor show little seasonal variation. Summer peaks of OC3 and OC2 are well modeled by PMF and are attributed mainly to biogenic SOA. OC4 was generally poorly modeled due to lack of characteristic low volatile markers. Summer maxima of biogenic SOA related compounds and source factors are positively correlated with temperature, global radiation, O concentration and mixing layer height (MLH). Winter maxima of BB related compounds and source factors are negatively correlated with temperature and MLH; whereas positively correlated with NO level.

摘要

为了研究非常细颗粒大气颗粒物(PM)的有机组成及其来源,我们于 2014 年 4 月至 2015 年 2 月在德国奥格斯堡使用旋转滚筒撞击器(RDI)与顺序过滤器采样器串联对 PM 进行了分段采样。对最小粒径 PM(PM<360nm)进行了有机形态分析和有机碳/元素碳(OC/EC)分析。热光 EC/OC 分析仪测定了不同的 OC 馏分,OC2、OC3 和 OC4 分别指分别在 280、480 和 580°C 下衍生的 OC 馏分。采用正矩阵因子化(PMF)分析进行源分配研究。PMF 解析了 5 个源,包括以生物为主的二次有机气溶胶(bioSOA)、异戊二烯为主的 SOA(isoSOA)、交通、生物质燃烧(BB)和生物质燃烧衍生的 SOA(bbSOA)。在年平均水平上,PMF 结果表明,生物源 SOA(bioSOA 加 isoSOA)对 OC 的贡献最大,其次是交通,然后是 BB 相关源(BB 加 bbSOA)。交通与最小的颗粒有关;而 bioSOA 和 BB 与较大的颗粒有关。生物前体的二次有机标记化合物、OC2、OC3 和 bioSOA、isoSOA 源因子夏季达到最大值。多环芳烃(PAHs)、生物质燃烧标记物、OC4 和 BB、bbSOA 源因子冬季达到最大值。藿烷和交通源因子的季节性变化很小。OC3 和 OC2 的夏季峰值与 PMF 很好地吻合,主要归因于生物 SOA。OC4 通常由于缺乏特征低挥发性标记而建模效果较差。与生物 SOA 相关的化合物和源因子的夏季最大值与温度、总辐射、O 浓度和混合层高度(MLH)呈正相关。与温度和 MLH 呈负相关;而与 NO 水平呈正相关。与 BB 相关的化合物和源因子的冬季最大值。

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