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Opis: The oxidative potential (OP) of fine and coarse fractions of ambient aerosols was studied in the urban environment of Athens, Greece. OP was quantified using a dithiothreitol (DTT) assay, applied to the water soluble fraction of aerosol that was extracted from 361 fine and 84 coarse mode of 24-h and 12-h filter samples over a one-year period. During the cold period, samples were collected on a 12-h basis, to assess the impact of night-time biomass burning emissions from domestic heating on OP. The chemical characteristics of aerosols were measured in parallel using an Aerosol Chemical Speciation Monitoring (ACSM) and a 7-wavelength Aethalometer. A source apportionment analysis on the ACSM data resulted in the identification of organic aerosol (OA) factors on a seasonal basis. A good correlation of OP with NO3−, NH4+, BC (Black Carbon), Organics and LV-OOA (low volatility oxygenated OA) was found during winter, revealing the importance of combustion and aging processes for OP. During the summertime, a good correlation between OP and SO4−2 and NH4+indicates its association with regional aerosol – thus the importance of oxidative aging that reduces its association with any characteristic source. Multiple regression analysis during winter revealed that highly oxygenated secondary aerosol (LV-OOA) and, to a lesser extent, fresh biomass burning (BBOA) and fossil fuel (HOA) organic aerosol, are the prime contributors to the OP of fine aerosol, with extrinsic toxicities of 54 ± 22 pmol min−1 μg−1, 28 ± 7 and 17 ± 4 pmol min−1μg−1, respectively. In summer, OP cannot be attributed to any of the identified components and corresponds to a background aerosol value. In winter however, the regression model can reproduce satisfactorily the water soluble DTT activity of fine aerosol, providing a unique equation for the estimation of aerosol OP in an urban Mediterranean environment.
Ključne besede: oxidative potential, reactive oxygen species, DTT assay, particulate matter, urban aerosol
Objavljeno v RUNG: 13.05.2024; Ogledov: 135; Prenosov: 0
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Opis: Submicron aerosol chemical composition was studied during a year-long period (26 July 2016–31 July 2017) and two wintertime intensive campaigns (18 December 2013–21 February 2014 and 23 December 2015–17 February 2016), at a central site in Athens, Greece, using an Aerosol Chemical Speciation Monitor (ACSM). Concurrent measurements included a particle-into-liquid sampler (PILS-IC), a scanning mobility particle sizer (SMPS), an AE-33 Aethalometer, and ion chromatography analysis on 24 or 12 h filter samples. The aim of the study was to characterize the seasonal variability of the main submicron aerosol constituents and decipher the sources of organic aerosol (OA). Organics were found to contribute almost half of the submicron mass, with 30 min resolution concentrations during wintertime reaching up to 200 µg m−3. During winter (all three campaigns combined), primary sources contributed about 33 % of the organic fraction, and comprised biomass burning (10 %), fossil fuel combustion (13 %), and cooking (10 %), while the remaining 67 % was attributed to secondary aerosol. The semi-volatile component of the oxidized organic aerosol (SV-OOA; 22 %) was found to be clearly linked to combustion sources, in particular biomass burning; part of the very oxidized, low-volatility component (LV-OOA; 44 %) could also be attributed to the oxidation of emissions from these primary combustion sources. These results, based on the combined contribution of biomass burning organic aerosol (BBOA) and SV-OOA, indicate the importance of increased biomass burning in the urban environment of Athens as a result of the economic recession. During summer, when concentrations of fine aerosols are considerably lower, more than 80 % of the organic fraction is attributed to secondary aerosol (SV-OOA 31 % and LV-OOA 53 %). In contrast to winter, SV-OOA appears to result from a well-mixed type of aerosol that is linked to fast photochemical processes and the oxidation of primary traffic and biogenic emissions. Finally, LV-OOA presents a more regional character in summer, owing to the oxidation of OA over the period of a few days.
Ključne besede: ACSM, organic aerosol, PMF, source apportionment
Objavljeno v RUNG: 13.05.2024; Ogledov: 140; Prenosov: 2
Celotno besedilo (4,65 MB)
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Opis: Particle number size distribution measurements were conducted during the summer of 2012 at City-Centre Urban Background (Patras-C), Urban Background (ICE-HT in Patras, DEM in Athens, EPT in Thessaloniki), and Regional Background stations (FIN in Crete). At the City-Centre Urban Background station, the average number distribution had a geometric mean diameter peak approximately at 60 nm and the highest number concentration, whereas at the Regional Background station and the Urban Background stations it displayed a major peak approximately at 100 nm, with the Regional Background station exhibiting the lowest number concentration. The particle number size distribution at each site was divided into size fractions and, based on their diurnal variation and previous studies, we concluded that the main sources for the City-Centre Urban Background station are traffic and the regional background concentration, for the Urban Background stations fresh traffic, aged traffic, cooking and the regional background concentration, and for the Regional Background station local activities (tourism, cooking) and regional background concentration. The median number concentration that is attributed to regional background concentration for the City-Centre Urban Background, the Urban Background and the Regional Background stations are respectively 13, 29 and 45% of the total number concentration. Nucleation events were identified at DEM station, where the newly formed particles accounted for 4% of the total particle concentration for the measurement period in the size range 10–20 nm, EPT, where they accounted for 12%, and FIN, where they accounted for 1%, respectively. New Particle Formation events contribution during summer to Condensation Cloud Nuclei were therefore insignificant in the Eastern Mediterranean. Modal analysis was performed on the number distributions and the results were classified in clusters. At the City-Centre Urban Background station, the cluster-source that dominated number concentration and frequency is related to fresh and aged traffic emissions, at the Urban Background stations aged traffic emissions, while at the Regional Background station number and frequency were dominated by the regional background concentration. Based on cluster analysis, 18% of the median number distribution was due to long range transport at the City-Centre Urban Background site, 37% at the Urban Background sites, and 59% at the Regional Background site. The Flexible Particle Dispersion Model (FLEXPART) was used in order to acquire geographic origin clusters and we concluded that the Etesian flow increases the median regional background number concentration in the Mediterranean basin by a factor of 2.5–4.
Ključne besede: Mediterranean aerosol, particle number size distribution clustering, FLEXPART clustering
Objavljeno v RUNG: 13.05.2024; Ogledov: 131; Prenosov: 0
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Ključne besede: carbonaceous aerosol, organic aerosol
Objavljeno v RUNG: 10.05.2024; Ogledov: 148; Prenosov: 1
Celotno besedilo (8,09 MB)

Opis: Port cities are affected by a wide array of emissions, including those from the shipping, road transport, and residential sectors; therefore, the characterization and apportionment of such sources in a high temporal resolution is crucial. This study presents measurements of fine aerosol chemical composition in Piraeus, one of the largest European ports, during two monthly periods (winter vs. summer) in 2018–2019, using online instrumentation (Aerosol Chemical Speciation Monitor—ACSM, 7-λ aethalometer). PMF source apportionment was performed on the ACSM mass spectra to quantify organic aerosol (OA) components, while equivalent black carbon (BC) was decomposed to its fossil fuel combustion and biomass burning (BB) fractions. The combined traffic, shipping and, especially, residential emissions led to considerably elevated submicron aerosol levels (22.8 μg m−3) in winter, which frequently became episodic late at night under stagnant conditions. Carbonaceous compounds comprised the major portion of this submicron aerosol in winter, with mean OA and BC contributions of 61% (13.9 μg m−3) and 16% (3.7 μg m−3), respectively. The contribution of BB to BC concentrations was considerable and spatially uniform. OA related to BB emissions (fresh and processed) and hydrocarbon-like OA (from vehicular traffic and port-related fossil fuel emissions including shipping) accounted for 37% and 30% of OA, respectively. In summer, the average PM1 concentration was significantly lower (14.8 μg m−3) and less variable, especially for the components associated with secondary aerosols (such as OA and sulfate). The effect of the port sector was evident in summer and maintained BC concentrations at high levels (2.8 μg m−3), despite the absence of BB and improved atmospheric dispersion. Oxygenated components yielded over 70% of OA in summer, with the more oxidized secondary component of regional origin being dominant (41%) despite the intensity of local sources, in the Piraeus environment. In general, with respect to local sources that can be the target of mitigation policies, this work highlights the importance of port-related activities but also reveals the extensive wintertime impact of residential wood burning. While a separation of the BB source is feasible, more research is needed on how to disentangle the short-term effects of different fossil-fuel combustion sources.
Ključne besede: Athens, harbor, shipping emissions, PM1, chemical speciation, organic aerosol, black carbon, ACSM, aethalometer, PMF
Objavljeno v RUNG: 10.05.2024; Ogledov: 130; Prenosov: 2
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