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Urban organic aerosols measured by single particle mass spectrometry in the megacity of London

机译:通过单颗粒质谱法测量的城市有机气溶胶在伦敦的特征中测量

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During the month of October 2006, as part of the REPARTEE-I experiment (Regent's Park and Tower Environmental Experiment) an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed at an urban background location in the city of London, UK. Fifteen particle types were classified, some of which were already discussed (Dall'Osto et al., 2009a,b; Harrison et al., 2012). In this manuscript the origins and properties of four unreported particle types postulated to be due to locally generated aerosols, independent of the air mass type advected into London, are examined. One particle type, originating from lubricating oil (referred to as Ca-EC), was associated with morning rush hour traffic emissions. A second particle type, composed of both inorganic and organic species (called Na-EC-OC), was found enhanced in particle number concentration during evening time periods, and is likely to originate from a source operating at this time of day, or more probably from condensation of semi-volatile species. A third class, internally mixed with organic carbon and sulphate (called OC), was found to spike both in the morning and evenings although it could not unambiguously associated with a specific source or atmospheric process. The fourth class (Secondary Organic Aerosols – Polycyclic Aromatic Hydrocarbon; SOA-PAH) exhibited maximum frequency during the warmest part of the day, and a number of factors point towards secondary aerosol production from traffic-related volatile aromatic compounds. Single particle mass spectra of this particle type showed an oxidized polycyclic aromatic compound signature. A comparison of ATOFMS particle class data is then made with factors obtained by Positive Matrix Factorization and PAH signatures obtained from Aerosol Mass Spectrometer (AMS) data (Allan et al., 2010). Both the Ca-EC and OC particle types correlate with primary Hydrocarbon-like Organic Aerosol (HOA, R2 = 0.65 and 0.50 respectively), and Na-EC-OC correlates weakly with the AMS secondary Oxygenated Organic Aerosol (OOA), (R2 = 0.35). Cluster SOA-PAH was found not to correlate with any AMS signal. A detailed analysis was conducted to identify ATOFMS particle type(s) representative of the AMS cooking aerosol factor (COA), but no convincing associations were found. The combined ATOFMS and AMS results of this REPARTEE study do not always provide an entirely coherent interpretation.
机译:2006年10月期间,作为Repartee-I的一部分进行了实验(摄政公园和塔环境实验),在英国伦敦市的城市背景位置部署了飞行飞行时间的烟雾飞行时间(ATOFMS)。十五种粒子类型分类,其中一些已经讨论过(Dall'osto等,2009A,B; Harrison等,2012)。在本手稿中,检查了由局部产生的气溶胶出发的四种未报告的粒子类型的起源和性质,独立于进入伦敦的空气质量型。一种源于润滑油(称为CA-EC)的一种颗粒类型与早上高峰时段交通排放相关。在晚上时间段期间发现由无机和有机物质(称为Na-EC-OC)组成的第二种颗粒类型,并且可能源自在这一天的这个时刻或更多的源可能来自半挥发物种的凝结。在早晨和夜晚发现,与有机碳和硫酸碳(称为OC)内部混合的第三类,尽管它不能明确地与特定的来源或大气过程相关联。第四类(二级有机气溶胶 - 多环芳烃; SOA-PAH)在最热部分的最热部分中表现出最大频率,以及来自与交通相关的挥发性芳族化合物的二次气溶胶产量的许多因素。该颗粒类型的单粒子质谱显示氧化多环芳族化合物签名。然后对AtoFMS颗粒类数据进行比较,通过通过气溶胶质谱仪(AMS)数据获得的正基质分解和PAH签名获得的因子(Allan等,2010)。 Ca-EC和OC颗粒类型与初级烃类有机气溶胶(SOA,R2 = 0.65和0.50分别相关),并且Na-EC-OC与AMS二次含氧有机气溶胶(OOA)弱相关(R2 = 0.35)。发现群集SOA-PAH不与任何AMS信号相关。进行了详细的分析以鉴定烹饪气溶胶因子(COA)的AMS的ATOFMS颗粒类型(S),但没有发现令人信服的关联。该重新研究的合并的atofms和AMS结果并不总是提供完全连贯的解释。

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