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    Hydroxymethanesulfonic acid in size-segregated aerosol particles at nine sites in Germany
    (München : European Geopyhsical Union, 2014) Scheinhardt, S.; van Pinxteren, D.; Müller, K.; Spindler, G.; Herrmann, H.
    In the course of two field campaigns, size-segregated particle samples were collected at nine sites in Germany, including traffic, urban, rural, marine and mountain sites. During the chemical characterisation of the samples some of them were found to contain an unknown substance that was later identified as hydroxymethanesulfonic acid (HMSA). HMSA is known to be formed during the reaction of S(IV) (HSO3− or SO32−) with formaldehyde in the aqueous phase. Due to its stability, HMSA can act as a reservoir species for S(IV) in the atmosphere and is therefore of interest for the understanding of atmospheric sulfur chemistry. However, no HMSA data are available for atmospheric particles from central Europe, and even on a worldwide scale data are scarce. Thus, the present study now provides a representative data set with detailed information on HMSA concentrations in size-segregated central European aerosol particles. HMSA mass concentrations in this data set were highly variable: HMSA was found in 224 out of 738 samples (30%), sometimes in high mass concentrations exceeding those of oxalic acid. On average over all 154 impactor runs, 31.5 ng m−3 HMSA was found in PM10, contributing 0.21% to the total mass. The results show that the particle diameter, the sampling location, the sampling season and the air mass origin impact the HMSA mass concentration. Highest concentrations were found in the particle fraction 0.42–1.2 μm, at urban sites, in winter and with eastern (continental) air masses, respectively. The results suggest that HMSA is formed during aging of pollution plumes. A positive correlation of HMSA with sulfate, oxalate and PM is found (R2 > 0.4). The results furthermore suggest that the fraction of HMSA in PM slightly decreases with increasing pH.
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    ACTRIS ACSM intercomparison - Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments
    (München : European Geopyhsical Union, 2015) Crenn, V.; Sciare, J.; Croteau, P.L.; Verlhac, S.; Fröhlich, R.; Belis, C.A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artiñano, B.; Baisnée, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M.J.; Esser-Gietl, J.K.; Green, D.C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillón, M.C.; Močnik, G.; O'Dowd, C.D.; Ovadnevaite, J.; Petit, J.-E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Estève, R.; Slowik, J.G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prévôt, A.S.H.; Jayne, J.T.; Favez, O.
    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.
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    Diurnal variations of ambient particulate wood burning emissions and their contribution to the concentration of Polycyclic Aromatic Hydrocarbons (PAHs) in Seiffen, Germany
    (München : European Geopyhsical Union, 2011) Poulain, L.; Iinuma, Y.; Müller, K.; Birmili, W.; Weinhold, K.; Brüggemann, E.; Gnauk, T.; Hausmann, A.; Löschau, G.; Wiedensohler, A.; Herrmann, H.
    Residential wood burning is becoming an increasingly important cause of air quality problems since it has become a popular source of alternative energy to fossil fuel. In order to characterize the contribution of residential wood burning to local particle pollution, a field campaign was organized at the village of Seiffen (Saxony, Germany). During this campaign, an Aerosol Mass Spectrometer (AMS) was deployed in parallel to a PM1 high volume filter sampler. The AMS mass spectra were analyzed using Positive Matrix Factorization (PMF) to obtain detailed information about the organic aerosol (OA). Biomass-burning organic aerosol (BBOA), Hydrocarbon-like organic aerosol (HOA), and Oxygenated Organic Aerosol (OOA) were identified and represented 20%, 17% and 62% of total OA, respectively. Additionally, Polycyclic Aromatic Hydrocarbons (PAH) were measured by the AMS with an average concentration of 10 ng m−3 and short term events of extremely high PAH concentration (up to 500 ng m−3) compared to the mean PAH value were observed during the whole measurement period. A comparison with the results from PM1 filter samples showed that the BBOA factor and the AMS PAH are good indicators of the total concentration of the different monosaccharide anhydrides and PAH measured on the filter samples. Based on its low correlation with CO and the low car traffic, the HOA factor was considered to be related to residential heating using liquid fuel. An influence of the time of the week (week vs. weekend) on the diurnal profiles of the different OA components was observed. The weekdays were characterized by two maxima; a first one early in the morning and a stronger one in the evening. During the weekend days, the different OA components principally reached only one maximum in the afternoon. Finally, the PAH emitted directly from residential wood combustion was estimated to represent 1.5% of the total mass of the BBOA factor and around 62% of the total PAH concentration measured at Seiffen. This result highlights the important contribution of residential wood combustion to air quality and PAH emissions at the sampling place, which might have a significant impact on human health. Moreover, it also emphasizes the need for a better time resolution of the chemical characterization of toxic particulate compounds in order to provide more information on variations of the different sources through the days as well as to better estimate the real human exposure.
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    Aerosol size-resolved trace metal composition in remote northern tropical atlantic marine environment: Case study cape verde islands
    (München : European Geopyhsical Union, 2013) Fomba, K.W.; Müller, K.; van Pinxteren, D.; Herrmann, H.
    Size-resolved trace metal concentrations of 15 elements in aerosol particles at the Cape Verde Atmospheric Observatory (CVAO) under remote background conditions were investigated through analysis of aerosol samples collected during intensive field studies from January 2007 to November 2011 using total reflection x-ray fluorescence (TXRF). The identification of the main air mass origin that influence remote marine aerosol in the northern tropical Atlantic has been investigated. In total, 317 samples were collected. The dataset was analyzed according to the main air mass inflow at the station. We found that remote conditions make up about 45% of the meteorological conditions in a year at CVAO and thus the northern tropical Atlantic. Surprisingly, air masses from North America are often responsible for higher trace metal concentrations in this region. Elements such as Zn, Pb, Cu, Cr, Ni, and V were mostly found in the submicron size fractions, while elements with dominant crustal or oceanic origin such as Fe, Ti, Mn, Sr, and Rb were found in the coarse fractions (>1 μm). The highest metal concentrations, especially for Zn (3.23 ng m−3), Cu (0.81 ng m−3), Sr (2.63 ng m−3), and Cr (0.53 ng m−3), were observed in air masses originating from North America and the concentrations were within the same concentration range to those reported previously in the literature for remote marine aerosols. Fe (12.26 ng m−3), Ti (0.91 ng m−3), and Mn (0.35 ng m−3) showed higher concentrations when air mass came from Europe and the Canary Islands. Pb concentration was low (<0.20 ng m−3) and did not vary significantly with air mass direction. The low Pb concentration is indicative of the complete phase-out of leaded gasoline even in African countries. Crustal enrichment factor values decreased from fine to coarse-mode particles with low values (<4) observed for Fe, Mn, and Rb, and high values (>20) for Zn, Cu, Ni, Cr, Pb, and Se. The observed enrichment of the elements was attributed to crustal, marine, anthropogenic, and biogenic sources, as well as long-range transport and resuspension. Zn, Cu and Pb were indicators of anthropogenic activities, while Ti and Sr were indicators of crustal and marine origin, respectively. Oceanic and biogenic emissions might have contributed to most of the Se observed. This work provides the first long-term size-resolved trace metals study for remote tropical northern Atlantic marine aerosols and the dataset could serve as good initiation of yearly flux estimates.