7 results
Search Results
Now showing 1 - 7 of 7
- ItemDiurnal 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.
- ItemChemical mass balance of 300 °c non-volatile particles at the tropospheric research site Melpitz, Germany(München : European Geopyhsical Union, 2014) Poulain, L.; Birmili, W.; Canonaco, F.; Crippa, M.; Wu, Z.J.; Nordmann, S.; Wiedensohler, A.; Held, A.; Spindler, G.; Prévôt, A.S.H.; Wiedensohler, A.; Herrmann, H.In the fine-particle mode (aerodynamic diameter < 1 μm) non-volatile material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyzes non-volatile particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle-size spectrometer (3–800 nm), a thermodenuder operating at 300 °C, a multi-angle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May–June 2008 as well as February–March 2009. As a basic result, we detected average non-volatile particle–volume fractions of 11 ± 3% (2008) and 17 ± 8% (2009). In both periods, BC was in close linear correlation with the non-volatile fraction, but not sufficient to quantitatively explain the non-volatile particle mass concentration. Based on the assumption that BC is not altered by the heating process, the non-volatile particle mass fraction could be explained by the sum of black carbon (47% in summer, 59% in winter) and a non-volatile organic contribution estimated as part of the low-volatility oxygenated organic aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that LV-OOA was more volatile in summer (May–June 2008) than in winter (February–March 2009) which was linked to a difference in oxidation levels (lower in summer). Although carbonaceous compounds dominated the sub-μm non-volatile particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however from the carbonaceous particles by a characteristic particle volume–size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements.
- ItemHygroscopic properties of the Paris urban aerosol in relation to its chemical composition(München : European Geopyhsical Union, 2014) Kamilli, K.A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.
- ItemParticle hygroscopicity during atmospheric new particle formation events: Implications for the chemical species contributing to particle growth(Göttingen : Copernicus, 2013) Wu, Z.; Birmili, W.; Poulain, L.; Poulain, L.; Merkel, M.; Fahlbusch, B.; Van Pinxteren, D.; Herrmann, H.; Wiedensohler, A.This study examines the hygroscopicity of newly formed particles (diameters range 25-45 nm) during two atmospheric new particle formation (NPF) events in the German mid-level mountains during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) field experiment. At the end of the NPF event involving clear particle growth, we measured an unusually high soluble particle fraction of 58.5% at 45 nm particle size. The particle growth rate contributed through sulfuric acid condensation only accounts for around 6.5% of the observed growth rate. Estimations showed that sulfuric acid condensation explained, however, only around 10% of that soluble particle fraction. Therefore, the formation of additional water-soluble matter appears imperative to explain the missing soluble fraction. Although direct evidence is missing, we consider water-soluble organics as candidates for this mechanism. For the case with clear growth process, the particle growth rate was determined by two alternative methods based on tracking the mode diameter of the nucleation mode. The mean particle growth rate obtained from the inter-site data comparison using Lagrangian consideration is 3.8 (± 2.6) nm h-1. During the same period, the growth rate calculated based on one site data is 5.0 nm h-1 using log-normal distribution function method. In light of the fact that considerable uncertainties could be involved in both methods, we consider both estimated growth rates consistent.
- ItemSeasonal and diurnal variations of particulate nitrate and organic matter at the IfT research station Melpitz(München : European Geopyhsical Union, 2011) Poulain, L.; Spindler, G.; Birmili, W.; Plass-Dülmer, C.; Weinhold, K.; Wiedensohler, A.; Herrmann, H.Ammonium nitrate and several organic compounds such as dicarboxylic acids (e.g. succinic acid, glutaric acid), some Polycyclic Aromatic Hydrocarbon (PAHs) or some n-alkanes are semi-volatile. The transition of these compounds between the gas and particulate phase may significantly change the aerosol particles radiative properties, the heterogeneous chemical properties, and, naturally, the total particulate mass concentration. To better assess these time-dependent effects, three intensive field experiments were conducted in 2008–2009 at the Central European EMEP research station Melpitz (Germany) using an Aerodyne Aerosol Mass Spectrometer (AMS). Data from all seasons highlight organic matter as being the most important particulate fraction of PM1 in summer (59%) while in winter, the nitrate fraction was more prevalent (34.4%). The diurnal variation of nitrate always showed the lowest concentration during the day while its concentration increased during the night. This night increase of nitrate concentration was higher in winter (ΔNO3− = 3.6 μg m−3) than in summer (ΔNO3− = 0.7 μg m−3). The variation in particulate nitrate was inherently linked to the gas-to-particle-phase equilibrium of ammonium nitrate and the dynamics of the atmosphere during day. The results of this study suggest that during summer nights, the condensation of HNO3 and NH3 on pre-existing particles represents the most prevalent source of nitrate, whereas during winter, nighttime chemistry is the predominant source of nitrate. During the summer 2008's campaign, a clear diurnal evolution in the oxidation state of the organic matter became evident (Organic Mass to Organic Carbon ratio (OM/OC) ranging from 1.65 during night to 1.80 during day and carbon oxidation state (OSc) from −0.66 to −0.4), which could be correlated to hydroxyl radical (OH) and ozone concentrations, indicating a photochemical transformation process. In summer, the organic particulate matter seemed to be heavily influenced by regional secondary formation and transformation processes, facilitated by photochemical production processes as well as a diurnal cycling of the substances between the gas and particulate phase. In winter, these processes were obviously less pronounced (OM/OC ranging from 1.60 to 1.67 and OSc from −0.8 to −0.7), so that organic matter apparently originated mainly from aged particles and long range transport.
- ItemRelating particle hygroscopicity and CCN activity to chemical composition during the HCCT-2010 field campaign(München : European Geopyhsical Union, 2013) Wu, Z.J.; Poulain, L.; Henning, S.; Dieckmann, K.; Birmili, W.; Merkel, M.; van Pinxteren, D.; Spindler, G.; Müller, K.; Stratmann, F.; Herrmann, H.; Wiedensohler, A.Particle hygroscopic growth at 90% RH (relative humidity), cloud condensation nuclei (CCN) activity, and size-resolved chemical composition were concurrently measured in the Thüringer Wald mid-level mountain range in central Germany in the fall of 2010. The median hygroscopicity parameter values, κ, of 50, 75, 100, 150, 200, and 250 nm particles derived from hygroscopicity measurements are respectively 0.14, 0.14, 0.17, 0.21, 0.24, and 0.28 during the sampling period. The closure between HTDMA (Hygroscopicity Tandem Differential Mobility Analyzers)-measured (κHTDMA) and chemical composition-derived (κchem) hygroscopicity parameters was performed based on the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Using size-averaged chemical composition, the κ values are substantially overpredicted (30 and 40% for 150 and 100 nm particles). Introducing size-resolved chemical composition substantially improved closure. We found that the evaporation of NH4NO3, which may happen in a HTDMA system, could lead to a discrepancy in predicted and measured particle hygroscopic growth. The hygroscopic parameter of the organic fraction, κorg, is positively correlated with the O : C ratio (κorg = 0.19 × (O : C) − 0.03). Such correlation is helpful to define the κorg value in the closure study. κ derived from CCN measurement was around 30% (varied with particle diameters) higher than that determined from particle hygroscopic growth measurements (here, hydrophilic mode is considered only). This difference might be explained by the surface tension effects, solution non-ideality, gas-particle partitioning of semivolatile compounds, and the partial solubility of constituents or non-dissolved particle matter. Therefore, extrapolating from HTDMA data to properties at the point of activation should be done with great care. Finally, closure study between CCNc (cloud condensation nucleus counter)-measured (κCCN) and chemical composition (κCCN, chem) was performed using CCNc-derived κ values for individual components. The results show that the κCCN can be well predicted using particle size-resolved chemical composition and the ZSR mixing rule.
- ItemSome insights into the condensing vapors driving new particle growth to CCN sizes on the basis of hygroscopicity measurements(München : European Geopyhsical Union, 2015) Wu, Z.J.; Poulain, L.; Birmili, W.; Größ, J.; Niedermeier, N.; Wang, Z.B.; Herrmann, H.; Wiedensohler, A.New particle formation (NPF) and growth is an important source of cloud condensation nuclei (CCN). In this study, we investigated the chemical species driving new particle growth to the CCN sizes on the basis of particle hygroscopicity measurements carried out at the research station Melpitz, Germany. Three consecutive NPF events occurred during summertime were chosen as examples to perform the study. Hygroscopicity measurements showed that the (NH4)2SO4-equivalent water-soluble fraction accounts for 20 and 16 % of 50 and 75 nm particles, respectively, during the NPF events. Numerical analysis showed that the ratios of H2SO4 condensational growth to the observed particle growth were 20 and 13 % for 50 and 75 nm newly formed particles, respectively. Aerosol mass spectrometer measurements showed that an enhanced mass fraction of sulfate and ammonium in the newly formed particles was observed when new particles grew to the sizes larger than 30 nm shortly after the particle formation period. At a later time, the secondary organic species played a key role in the particle growth. Both hygroscopicity and aerosol mass spectrometer (AMS) measurements and numerical analysis confirmed that organic compounds were major contributors driving particle growth to CCN sizes. The critical diameters at different supersaturations estimated using AMS data and κ-Köhler theory increased significantly during the later course of NPF events. This indicated that the enhanced organic mass fraction caused a reduction in CCN efficiency of newly formed particles. Our results implied that the CCN production associated with atmospheric nucleation may be overestimated if assuming that newly formed particles can serve as CCN once they grow to a fixed particle size, an assumption made in some previous studies, especially for organic-rich environments. In our study, the enhancement in CCN number concentration associated with individual NPF events were 63, 66, and 69 % for 0.1, 0.4, and 0.6 % supersaturation, respectively.