On the basis of a 2‐year comprehensive data set obtained within the CARBOSOL project, seasonal source apportionment of PM2.5 aerosol is attempted for five rural/remote sites in Europe. The approach ...developed combines radiocarbon measurements with bulk measurements of organic carbon (OC), elemental carbon (EC), and two organic tracers (levoglucosan and cellulose). Source types are lumped into primary emissions from fossil fuel combustion and biomass burning, bioaerosol, and secondary organic aerosol from precursors emitted by fossil and nonfossil sources. Bulk concentration ratios reported for these source types in the literature are used to estimate the source contributions which are constrained by measured radiocarbon concentrations. It has been found that while fossil‐related sources predominate EC throughout the year at all sites, the sources of OC are primarily biogenic and markedly different between summer and winter. In winter biomass burning primary emission is the main source, with sizable additional contribution from fossil fuel combustion. In contrast, in summer secondary organic aerosol (SOA) from nonfossil sources becomes predominant (63–76% of TC), with some contribution of SOA from fossil fuel combustion. The results agree well with recent findings of other authors who established the predominance of biogenic SOA for rural sites in summer in Europe. An uncertainty analysis has been conducted, which shows that the main conclusions from this study are robust.
Atmospheric levoglucosan has been determined as a proxy for “biomass smoke” in samples from six background stations on a west–east transect extending from the Atlantic (Azores) to the mid‐European ...background site KPZ (K‐Puszta, Hungary). Concentration levels of levoglucosan (biannual averages) in the west–east transect range from 0.005 μg/m3 at the oceanic background site AZO (Azores) to 0.52 μg/m3 at AVE (Aveiro, Portugal). The atmospheric concentration of “biomass smoke” (biannual averages) was derived from the levoglucosan data with wood‐type‐specific conversion factors. Annual averages of wood smoke levels ranged from 0.05 μg/m3 at AZO to 4.3 μg/m3 at AVE. Winter (DJF) averages at the low‐level sites AVE and KPZ were 10.8 and 6.7 μg/m3, respectively. Relative contributions of biomass smoke to organic matter (OM) range from around 9–11% at the elevated sites SIL, PDD and SBO, as well as for AZO, to 36% at the low‐level site AVE and 28% at KPZ. Surprisingly high relative concentrations of biomass smoke in OM (68 and 47%) were observed for wintry conditions at the continental low‐level CARBOSOL sites AVE and KPZ. Thus biomass smoke is a very important constituent of the organic material in the mid and west European background with summer contributions to organic matter of around 1–6% and winter levels of around 20% at the elevated mountain sites and 47–68% at rural flat terrain sites, not including secondary organic aerosol from biomass combustion sources.
Brown carbon is a ubiquitous and unidentified component of organic aerosol which has recently come into the forefront of atmospheric research. This component is strongly linked to the class of ...humic‐like substances (HULIS) in aerosol whose ultimate origin is still being debated. Using a simplified spectroscopic method the concentrations of brown carbon have been determined in aqueous extracts of fine aerosol collected during the CARBOSOL project. On the basis of the results of 2‐year measurements of several aerosol constituents at six European sites, possible sources of brown carbon are inferred. Biomass burning (possibly domestic wood burning) is shown to be a major source of brown carbon in winter. At elevated sites in spring, smoke from agricultural fires may be an additional source. Direct comparison of measured brown carbon concentrations with HULIS determined by an independent method reveals that the two quantities correlate well at low‐elevation sites throughout the year. At high‐elevation sites the correlation is still high for winter but becomes markedly lower in summer, implying different sources and/or atmospheric sinks of brown carbon and HULIS. The results shed some light on the relationships between atmospheric brown carbon and HULIS, two ill‐defined and overlapping components of organic aerosol.
Measurements of the oxidative potential (OP) of airborne particulate matter may be applied for the assessment of the health-based exposure by integrating various biologically relevant properties of ...particles. This study aimed at the determination of oxidative activity of two size fractions of particulate using the ascorbic acid (AA) and reduced glutathione (GSH) assay. Samples of PM were collected in Krakow, one of the most polluted cities in Poland, in the city centre. Samples were collected during wintertime, when heating sources used in residential areas have significant influence on the concentrations of particulate matter in the air. PM10 and PM2.5 concentrations varied from 8.9 to 92.5 μg m
−3
. Samples were chemically analysed for elemental carbon, organic carbon, ions and metals. PM2.5 was found as a more oxidative active fraction, where OP
AA
and OP
GSH
depletions were up to 81.7 and 132.0 μg m
−3
, respectively. The average values of OP
AA
of PM10 and PM2.5 were similar and equalled 40.8 and 37.2 μg m
−3
, respectively. The average value of OP
GSH
of PM2.5 equalled 56.7 μg m
−3
and was 3.5 times higher than OP
GSH
of PM10. The loss of AA amount in PM10 and PM2.5 and the depletion of GSH in PM2.5 were best described by the pseudo second-order kinetics model. The kinetics of the GSH depletion reaction in PM10 was best described by the pseudo first-order kinetics model. The strong correlations between carbonaceous and metallic constituents of PM and oxidative potential suggest their relevance in participation in oxidative activity of particulate matter.
Airborne bacteria as cloud condensation nuclei Bauer, Heidi; Giebl, Heinrich; Hitzenberger, Regina ...
Journal of Geophysical Research - Atmospheres,
16 November 2003, Volume:
108, Issue:
D21
Journal Article
Peer reviewed
Bacteria cultivated from aerosol and cloud water samples collected at a remote Austrian mountain site under wintry conditions were tested for their ability to act as cloud condensation nuclei (CCN). ...The experiment was carried out with a cloud condensation nuclei counter (CCNC) operating on the principle of a static thermal diffusion chamber. Average concentrations of cultivable airborne bacteria amounted to 8 colony forming units (CFU) m−3 in aerosol samples and to 79 CFU mL−1 in cloud water. The set of tested bacteria comprised Gram positive and Gram negative but no known ice nucleating species. At supersaturations between 0.07 and 0.11% all types of bacteria were activated as CCN. As the sizes of the bacteria were smaller than the Kelvin diameters for the respective supersaturations, the physico‐chemical properties of their outer cell walls must have enhanced their CCN activity.
Long-term monitoring of organic aerosol is important for epidemiological studies, validation of atmospheric models, and air quality management. In this study, we apply a recently developed ...filter-based offline methodology using an aerosol mass spectrometer (AMS) to investigate the regional and seasonal differences of contributing organic aerosol sources. We present offline AMS measurements for particulate matter smaller than 10 µm at nine stations in central Europe with different exposure characteristics for the entire year of 2013 (819 samples). The focus of this study is a detailed source apportionment analysis (using positive matrix factorization, PMF) including in-depth assessment of the related uncertainties. Primary organic aerosol (POA) is separated in three components: hydrocarbon-like OA related to traffic emissions (HOA), cooking OA (COA), and biomass burning OA (BBOA). We observe enhanced production of secondary organic aerosol (SOA) in summer, following the increase in biogenic emissions with temperature (summer oxygenated OA, SOOA). In addition, a SOA component was extracted that correlated with an anthropogenic secondary inorganic species that is dominant in winter (winter oxygenated OA, WOOA). A factor (sulfur-containing organic, SC-OA) explaining sulfur-containing fragments (CH3SO2+), which has an event-driven temporal behaviour, was also identified. The relative yearly average factor contributions range from 4 to 14 % for HOA, from 3 to 11 % for COA, from 11 to 59 % for BBOA, from 5 to 23 % for SC-OA, from 14 to 27 % for WOOA, and from 15 to 38 % for SOOA. The uncertainty of the relative average factor contribution lies between 2 and 12 % of OA. At the sites north of the alpine crest, the sum of HOA, COA, and BBOA (POA) contributes less to OA (POA / OA = 0.3) than at the southern alpine valley sites (0.6). BBOA is the main contributor to POA with 87 % in alpine valleys and 42 % north of the alpine crest. Furthermore, the influence of primary biological particles (PBOAs), not resolved by PMF, is estimated and could contribute significantly to OA in PM10.
Background
Growing up on a cattle farm and consuming raw cow's milk protects against asthma and allergies. We expect a cattle‐specific protein as active component in this farm effect.
Methods
Dust ...was collected from cattle and poultry stables and from mattresses of households. Urine was obtained from cattle, and ambient aerosols were sampled. Samples were analysed for BLG by SDS PAGE/immunoblot and mass spectrometry, and for association with metals by SEC‐ICP‐MS. PBMC of healthy donors were incubated with BLG +/− zinc, and proliferation and cytokines determined. BALB/c mice were pre‐treated intranasally with stable dust extract containing BLG or depleted of BLG, and subsequent allergy response after sensitization was evaluated on antibody and symptom level.
Results
A major protein in dust from cattle farms and ambient air was identified as BLG. Urine from female and male cattle is a major source of BLG. In dust samples, BLG was associated with zinc. In vitro, zinc‐BLG provoked significantly lower proliferation of CD4+ and CD8+ cells while inducing significantly higher levels of IFN‐γ and IL‐6 than the apo‐BLG devoid of zinc. In vivo, pre‐treatment of mice with dust extract containing BLG resulted in lower allergy symptom scores to BLG and unrelated Bet v 1 than pre‐treatment with extract depleted of BLG. These in vitro and in vivo effects were independent of endotoxin.
Conclusion
The lipocalin BLG is found in large amounts in cattle urine, accumulates in bovine dust samples and is aerosolized around farms. Its association with zinc favorably shapes the human cellular immune response towards Th1‐cytokines in vitro. BLG together with zinc in stable dust protects mice from allergic sensitization. BLG with its associated ligands may in an innate manner contribute to the allergy‐protective farm effect.
Air quality is of large concern in the city of Krakow, southern Poland. A comprehensive study was launched by us in which two PM fractions (PM
and PM
) were sampled during 1-year campaign, lasting ...from April 21, 2018 to March 19, 2019. A suite of modern analytical methods was used to characterize the chemical composition of the collected samples. The contents of 14 sugars, sugar alcohols and anhydrosugars, 16 polycyclic aromatic hydrocarbons, selected metals and non-metals and ions were analyzed, in addition to organic and elemental carbon content. The carbon isotope composition in both analysed PM fractions, combined with an isotope-mass balance method, allowed to distinguish three main components of carbonaceous emissions in the city: (1) emissions related to combustion of hard coal, (2) emissions related to road transport, and (3) biogenic emissions. The heating season emissions from coal combustion had the biggest contribution to the reservoir of carbonaceous aerosols in the PM
fraction (44%) and, together with the biogenic emission, they were the biggest contributors to the PM
fraction (41% and 44%, respectively). In the non-heating season, the dominant source of carbon in PM
and PM
fraction were the biogenic emissions (48 and 54%, respectively).
We investigated the interactions of air and snow over one entire winter accumulation period as well as the importance of chemical markers in a pristine free-tropospheric environment to explain ...variation in a microbiological dataset. To overcome the limitations of short term bioaerosol sampling, we sampled the atmosphere continuously onto quartzfiber air filters using a DIGITEL high volume PM10 sampler. The bacterial and fungal communities, sequenced using Illumina MiSeq, as well as the chemical components of the atmosphere were compared to those of a late season snow profile. Results reveal strong dynamics in the composition of bacterial and fungal communities in air and snow. In fall the two compartments were similar, suggesting a strong interaction between them. The overlap diminished as the season progressed due to an evolution within the snowpack throughout winter and spring. Certain bacterial and fungal genera were only detected in air samples, which implies that a distinct air microbiome might exist. These organisms are likely not incorporated in clouds and thus not precipitated or scavenged in snow. Although snow appears to be seeded by the atmosphere, both air and snow showed differing bacterial and fungal communities and chemical composition. Season and alpha diversity were major drivers for microbial variability in snow and air, and only a few chemical markers were identified as important in explaining microbial diversity. Air microbial community variation was more related to chemical markers than snow microbial composition. For air microbial communities Cl−, TC/OC, SO4 2−, Mg2+, and Fe/Al, all compounds related to dust or anthropogenic activities, were identified as related to bacterial variability while dust related Ca2+ was significant in snow. The only common driver for snow and air was SO4 2−, a tracer for anthropogenic sources. The occurrence of chemical compounds was coupled with boundary layer injections in the free troposphere (FT). Boundary layer injections also caused the observed variations in community composition and chemistry between the two compartments. Long-term monitoring is required for a more valid insight in post-depositional selection in snow.
Atmospheric “free cellulose” has been determined as a proxy for “plant debris” in samples from six background stations on a west‐east transect extending from the Atlantic (Azores) to the mid‐European ...background site KPZ (K‐Puszta, Hungary). Concentration levels of cellulose (biannual averages) range from 16.3 ng/m3 at the oceanic background site AZO (Azores) to 181 ng/m3 at KPZ (Hungary). Concentrations decrease with elevation, winter levels at the midtropospheric Sonnblick site (SBO, 3106 m) are comparable to clean Atlantic conditions. The atmospheric concentration of plant debris (biannual averages) was derived from the cellulose data and ranges from 33.4 ng/m3 at AZO to 363 ng/m3 at KPZ. Relative contributions of plant debris to organic matter (OM) range from around 2% at the semirural coastal site Aveiro (AVE) to 10% at SBO. Surprisingly high relative concentrations of plant debris in OM were observed for wintry conditions at the elevated sites. The relative fraction of plant debris in OM ranged as averages from 6.1% at Schauinsland, Germany (1205 m) to 10.1% at Puy de Dome, France (1405 m) and 22.4% at Sonnblick, Austria (3106 m). Thus plant debris is a very important constituent of the organic material at elevated background sites with summer concentrations of around 5% and winter levels from around 6–22% depending on elevation. Since cellulose is considered rather long‐lived with respect to atmospheric oxidation processes, it may become enriched on the way to background regions, which may explain the elevated relative levels at elevated sites.
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