Organic tracer-based source analysis of PM2.5 organic and elemental carbon: A case study at Dongguan in the Pearl River Delta, China

Organic tracer-based source analysis of PM2.5 organic and elemental carbon: A case study at Dongguan in the Pearl River Delta, China
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基于有机示踪的 PM2.5 有机碳和元素碳来源分析:以中国珠江三角洲东莞市为例

DOI:
10.1016/j.atmosenv.2015.07.033
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发表时间:
2015-10
影响因子:
5
通讯作者:
Jian Zhen Yu(*)
Jian Zhen Yu(*)
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Zibing Yuan;Dui Wu;Alexis K. H. Lau;Jian Zhen Yu(*)

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有机碳(OC)和元素碳(EC)是PM2.5的主要成分,由于其来源的多样性和缺乏特定来源的示踪数据,其来源解析仍然是一个具有挑战性的任务。在这项工作中,对2010年至2012年在珠江三角洲东莞采集的156个过滤样品的PM2.5化学成分数据(包括主要离子、OC、EC、元素和有机分子源标志物)进行了正矩阵因式分解(PMF)分析。关键的有机示踪剂包括左旋葡聚糖、甘露糖、霍烷、C27-C33n-烷烃和多环芳烃(PAHs)。利用这些物种作为PMF模型的输入,解决了9个因素。其中,生物质燃烧和燃煤对有机碳的贡献率分别为15-17%和24-30%,对总有机碳的贡献率为34-35%。工业排放和船舶排放分别占有机碳的16-24%和7-8%,对碳排放的贡献分别为8-11%和16-17%。汽车尾气是一个不太重要的来源,占OC的3-4%和EC的5-8%。次生有机碳是次生硫酸盐和硝酸盐形成源因素中有机碳的总和,占有机碳的27-36%。塑料燃烧,通过1,3,5-三苯基苯作为示踪剂,是OC(≤4%)和EC(5-10%)的次要来源,但是该地点多环芳烃的重要来源。通过比较PMF和从输入物种列表中移除的不同有机示踪剂组合,证明了有机来源示踪剂的有效性。左旋葡聚糖和甘露聚糖是区分生物质燃烧和煤燃烧的重要添加剂,它们减少了来源特征之间的共线性。研究发现,在解决汽车尾气和塑料燃烧等不太重要的来源时,有必要包括霍烷和1,3,5-三苯基苯。C27-C33n-烷烃和多环芳烃的包裹体会影响PMF解析的源剖面,从而影响源对OC和EC的贡献。当只考虑主要成分时,与使用全套有机示踪剂的PMF分析相比,更多的有机碳(占有机碳的44%比27%)被分配到次要因素中,主要是以煤炭燃烧和工业排放为代价。EC对少数几个主要燃烧源的分配对有机示踪剂的包含比对OC的分配更敏感,其中多环芳烃起着突出的作用。这项工作证明了在识别和量化有机碳和有机碳来源时,拥有不同的有机示踪剂的重要性。
Organic carbon (OC) and elemental carbon (EC) are major constituents of PM2.5and their source apportionment remains a challenging task due to the great diversity of their sources and lack of source-specific tracer data. In this work, sources of OC and EC are investigated using positive matrix factorization (PMF) analysis of PM2.5chemical composition data, including major ions, OC, EC, elements, and organic molecular source markers, for a set of 156 filter samples collected over three years from 2010 to 2012 at Dongguan in the Pearl River Delta, China. The key organic tracers include levoglucosan, mannosan, hopanes, C27–C33n-alkanes, and polycyclic aromatic hydrocarbons (PAHs). Using these species as input for the PMF model, nine factors were resolved. Among them, biomass burning and coal combustion were significant sources contributing 15–17% of OC and 24–30% and 34–35% of EC, respectively. Industrial emissions and ship emissions, identified through their characteristic metal signatures, contributed 16–24% and 7–8% of OC and 8–11% and 16–17% of EC, respectively. Vehicle exhaust was a less significant source, accounting for 3–4% of OC and 5–8% of EC. Secondary OC, taken to be the sum of OC present in secondary sulfate and nitrate formation source factors, made up 27–36% of OC. Plastic burning, identified through 1,3,5-triphenylbenzene as a tracer, was a less important source for OC(≤4%) and EC (5–10%), but a significant source for PAHs at this site.The utility of organic source tracers was demonstrated by comparing PMF runs with different combinations of organic tracers removed from the input species list. Levoglucosan and mannosan were important additions to distinguish biomass burning from coal combustion by reducing collinearity among source profiles. Inclusion of hopanes and 1,3,5-triphenylbenzene was found to be necessary in resolving the less significant sources vehicle exhaust and plastic burning. Inclusion of C27–C33n-alkanes and PAHs can influence the source profiles resolved by PMF and thereby affect the source contributions to OC and EC. Considerably more OC (44% vs. 27% of OC) was apportioned to the secondary factors when only major components were considered in comparison with the PMF analysis with the full suite of organic tracers, mainly at the expense of coal combustion and industrial emissions. EC apportionment to the few major combustion sources was found more sensitive to inclusion of organic tracers than OC apportionment, with PAHs playing a prominent role. This work demonstrates the importance of having distinct organic tracers in identifying and quantifying OC and EC sources.
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