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Has files: Yes × Type: Text × Subject: chemical composition × Subject: concentration (composition) × Subject: particle size × Subject: particulate matter ×

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    Identification and source attribution of organic compounds in ultrafine particles near Frankfurt International Airport
    (Katlenburg-Lindau : European Geosciences Union, 2021) Ungeheuer, Florian; van Pinxteren, Dominik; Vogel, Alexander L.
    Analysing the composition of ambient ultrafine particles (UFPs) is a challenging task due to the low mass and chemical complexity of small particles, yet it is a prerequisite for the identification of particle sources and the assessment of potential health risks. Here, we show the molecular characterization of UFPs, based on cascade impactor (Nano-MOUDI) samples that were collected at an air quality monitoring station near one of Europe's largest airports, in Frankfurt, Germany. At this station, particle-size-distribution measurements show an enhanced number concentration of particles smaller than 50 nm during airport operating hours. We sampled the lower UFP fraction (0.010-0.018, 0.018-0.032, 0.032-0.056 classCombining double low lineinline-formula/m) when the air masses arrived from the airport. We developed an optimized filter extraction procedure using ultra-high-performance liquid chromatography (UHPLC) for compound separation and a heated electrospray ionization (HESI) source with an Orbitrap high-resolution mass spectrometer (HRMS) as a detector for organic compounds. A non-Target screening detected classCombining double low lineinline-formulag1/4200/ organic compounds in the UFP fraction with sample-To-blank ratios larger than 5. We identified the largest signals as homologous series of pentaerythritol esters (PEEs) and trimethylolpropane esters (TMPEs), which are base stocks of aircraft lubrication oils. We unambiguously attribute the majority of detected compounds to jet engine lubrication oils by matching retention times, high-resolution and accurate mass measurements, and comparing tandem mass spectrometry (MS classCombining double low lineinline-formula2/) fragmentation patterns between both ambient samples and commercially available jet oils. For each UFP stage, we created molecular fingerprints to visualize the complex chemical composition of the organic fraction and their average carbon oxidation state. These graphs underline the presence of the homologous series of PEEs and TMPEs and the appearance of jet oil additives (e.g.Tricresyl phosphate, TCP). Targeted screening of TCP confirmed the absence of the harmful tri-iortho/i isomer, while we identified a thermal transformation product of TMPE-based lubrication oil (trimethylolpropane phosphate, TMP-P). Even though a quantitative determination of the identified compounds is limited, the presented method enables the qualitative detection of molecular markers for jet engine lubricants in UFPs and thus strongly improves the source apportionment of UFPs near airports./p. © 2021 BMJ Publishing Group. All rights reserved.
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    Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime
    (München : European Geopyhsical Union, 2016) Wu, Z.J.; Zheng, J.; Shang, D.J.; Du, Z.F.; Wu, Y.S.; Zeng, L.M.; Wiedensohler, A.; Hu, M.
    Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16  ±  0.07, 0.19  ±  0.06, 0.22  ±  0.06, 0.26  ±  0.07, and 0.28  ±  0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF  >  1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m−3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.