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Tracer-based source apportioning of atmospheric organic carbon and the influence of anthropogenic emissions on secondary organic aerosol formation in Hong Kong

机译:基于Tracer的大气有机碳源分配以及香港二次有机气溶胶形成对型辐射排放的影响

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Here we conducted comprehensive chemical characterization and source apportionment of 49 PM 2.5 samples collected in Hong Kong. Besides the major aerosol constituents, 39 polar organic species, including 14 secondary organic aerosol (SOA) tracers of isoprene, monoterpenes, β -caryophyllene, and naphthalene, were quantified using gas chromatography–mass spectrometry (GC–MS). Six factors, i.e., SOA, secondary sulfate (SS), biomass burning (BB)/SOA, sea salt, marine vessels, and vehicle emissions, were apportioned by positive matrix factorization (PMF) as the major sources of ambient organic carbon (OC) in Hong Kong. The secondary formation, including OC from SOA, SS, and aging of BB plume, was the leading contributor to OC (51.4?%, 2.15? ± ?1.37? μg?C?m ?3 ) throughout the year. We then applied a tracer-based method (TBM) to estimate the SOA formation from the photo-oxidation of four selected precursors, and monoterpene SOA was the most abundant. A Kintecus kinetic model was used to examine the formation channels of isoprene SOA, and the aerosol-phase ring-opening reaction of isoprene epoxydiols (IEPOXs) was found to be the dominant formation pathway. Consistently, IEPOX tracers contributed 94?% to total GC–MS-quantified isoprene SOA tracers. The TBM-estimated secondary organic carbon (SOC TBM ) and PMF-apportioned SOC (SOC PMF ) showed similar temporal trends; however, SOC TBM only accounted for 26.5?% of SOC PMF , indicating a large fraction of ambient SOA was from other reaction pathways or precursors. Results of Pearson's R and multivariate linear regression analysis showed that NO x processing played a key role in both daytime and nighttime SOA production in the region. Moreover, sulfate had a significant positive linear relationship with SOC PMF and SS-related SOC, and particle acidity was significantly correlated with SOC from the aging of BB.
机译:在这里,我们在香港收集了全面的化学表征和49例2.5样本的源分摊。除了主要的气溶胶成分,39个极性有机物种,包括异戊二烯,单萜,β-丙基和萘的14个二次有机气溶胶(SOA)示踪剂,使用气相色谱 - 质谱(GC-MS)定量。六个因素,即SOA,仲硫酸盐(SS),生物质燃烧(BB)/ SOA,海盐,海洋血管和载体排放,通过阳性基质分解(PMF)作为环境有机碳的主要来源分配(OC ) 在香港。其中包括SOA,SS和老化的二级形成,包括BB羽流的老化,是OC的主要贡献者(51.4?%,2.15?±1.1.37?μg?c?m?3)全年。然后,我们应用了一种基于示踪剂的方法(TBM)来估计来自四种选定前体的光氧化的SOA形成,并且单萜SOA是最丰富的。用于检查异戊二烯SOA的形成通道,异戊二烯环氧二醇(IePoxs)的气溶胶相开关反应是主要的形成途径。始终如一地,Iepox示踪剂贡献了94%的总GC-MS定量异戊二烯SOA示踪剂。 TBM估计的二次有机碳(SoC TBM)和PMF分配的SoC(SoC PMF)显示出类似的时间趋势;然而,SOC TBM仅占SOC PMF的26.5?%,表明大部分环境SOA来自其他反应途径或前体。 Pearson的R和多变量线性回归分析结果表明,在该地区的日间和夜间SOA生产中,没有X处理在该地区的生产中发挥了关键作用。此外,硫酸盐与SOC PMF和SS相关的SoC具有显着的阳性线性关系,并且颗粒酸度与来自BB的老化的SOC显着相关。

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