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Yearlong variability of oxidative potential of particulate matter in an urban Mediterranean environment
D. Paraskevopoulou, Aikaterini Bougiatioti, Iasonas Stavroulas, T. Fang, Maria Lianou, Eleni Liakakou, Evangelos Gerasopoulos, R. Weber, Athanasios Nenes, Nikolaos Mihalopoulos, 2019, original scientific article

Abstract: 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.
Keywords: oxidative potential, reactive oxygen species, DTT assay, particulate matter, urban aerosol
Published in RUNG: 13.05.2024; Views: 269; Downloads: 0
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Summertime particulate matter and its composition in Greece
M. A. Tsiflikiotou, E. Kostenidou, D. K. Papanastasiou, D. Patoulias, Pavlos Zarmpas, D. Paraskevopoulou, E. Diapouli, Christos Kaltsonoudis, Kalliopi Florou, Iasonas Stavroulas, 2019, original scientific article

Abstract: During the summer of 2012 a coordinated field campaign was conducted in multiple locations in Greece in order to characterize the ambient particulate matter (PM) levels, its chemical composition and the contribution of the regional and local sources. PM1, PM2.5 and PM10 samples were collected simultaneously at seven different sites in Greece: an urban and a suburban station in Patras, a suburban station in Thessaloniki, a suburban and an urban background station in Athens, a rural background station at the Navarino Environmental Observatory (NEO) in southwestern Peloponnese and a remote background site at Finokalia in the northeastern part of Crete. The sites were selected to facilitate the estimation of the contribution of the local emission sources and long range transport. Sulfate and organics were the major PM1 components in all sites suggesting that high sulfate levels still remain in parts of Europe. The photochemistry of the Eastern Mediterranean can convert rapidly the emitted sulphur dioxide to sulfate. Our analysis indicated significant sulfate production over the area, with high sulfate levels, especially in the remote site of Finokalia, associated with air masses that had passed over Turkey. There was high regional secondary organic aerosol production dominating organic aerosol levels even in a major city like Athens. High organic aerosol levels were associated with air masses that had crossed the Balkans with a significant biogenic component. The average PM2.5 concentration ranged from 13 to 18 μg m−3 in the different sites. There were unexpected significant gradients in the concentrations of secondary aerosol components in length scales of a few hundred kilometers. The low concentrations of measured PM2.5 nitrate are mostly organic nitrates and supermicrometer nitrate associated with sea-salt and dust. Dust was a significant PM10 constituent in all areas and was quite variable in space showing the importance of the local sources.
Keywords: PM2.5, sulfate aerosol, secondary inorganic aerosol, secondary organic aerosol, Greece
Published in RUNG: 13.05.2024; Views: 295; Downloads: 0
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Sources and processes that control the submicron organic aerosol composition in an urban Mediterranean environment (Athens) : a high temporal-resolution chemical composition measurement study
Iasonas Stavroulas, Aikaterini Bougiatioti, Georgios Grivas, D. Paraskevopoulou, M. Tsagkaraki, Pavlos Zarmpas, Eleni Liakakou, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2019, original scientific article

Abstract: 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.
Keywords: ACSM, organic aerosol, PMF, source apportionment
Published in RUNG: 13.05.2024; Views: 280; Downloads: 2
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Optical properties of near-surface urban aerosols and their chemical tracing in a Mediterranean city (Athens)
Dimitris Katsanos, Aikaterini Bougiatioti, Eleni Liakakou, Dimitris G. Kaskaoutis, Iasonas Stavroulas, D. Paraskevopoulou, Maria Lianou, Basil E. Psiloglou, Evangelos Gerasopoulos, Christodoulos Pilinis, 2019, original scientific article

Abstract: One-year measurements (October 2016–September 2017) of aerosol optical properties in the Athens urban environment were analyzed; for closure purposes, the results were supported by data of chemical composition of the non-refractory submicron aerosol fraction acquired with an Aerosol Chemical Speciation Monitor (ACSM). Both the spectral scattering (bsca) and absorption (babs) coefficients exhibit a pronounced annual variability with higher values (63.6 Mm–1 at 550 nm and 41.0 Mm–1 at 520 nm, respectively) in winter, due to domestic heating releasing increased carbonaceous emissions and the shallow mixing layer trapping aerosols near the surface. Much lower values (33.5 Mm–1 and 22.9 Mm–1 for bsca and babs, respectively) are found during summer, indicating rather aged aerosols from regional sources. The estimations of the dry spectral single scattering albedo (SSA), scattering (SAE) and absorption (AAE) Ångström exponents focus on the seasonality of the urban aerosols. The high SAE (~2.0) and low SSA (0.62 ± 0.11) values throughout the year indicate the dominance of fine-absorbing aerosols from fossil-fuel combustion, while the high AAE (~1.5) in winter suggests enhanced presence of biomass-burning aerosols. Pronounced morning and late evening/night peaks are found in both bsca and babs during winter, coinciding with the morning traffic rush hour and increased residential wood burning in the evening, while in the other seasons, the diurnal patterns flatten out. The wind speed strongly affects the aerosol loading and properties in winter, since for winds below 3 m s–1, a high increase in bsca and babs is observed, consistent with low dilution processes and hazy/smoggy conditions. Our closure experiments indicate a good agreement (R2 = 0.91, slope = 1.08) between the reconstructed and measured bsca values and reveal that organic matter contributes about half of the sub-micron mass in winter, followed by sulfate (~40%) and nitrate (10%, only in winter) aerosols.
Keywords: urban aerosols, light scattering, absorption, chemical species, wood burning, Athens
Published in RUNG: 10.05.2024; Views: 308; Downloads: 2
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Measuring the spatial variability of black carbon in Athens during wintertime
Georgios Grivas, Iasonas Stavroulas, Eleni Liakakou, Dimitris G. Kaskaoutis, Aikaterini Bougiatioti, D. Paraskevopoulou, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2019, original scientific article

Abstract: A first assessment of the spatial variability of ambient black carbon (BC) concentrations in the Greater Area of Athens (GAA) was carried out during an intensive wintertime campaign, when ambient levels are exacerbated by increased biomass burning for residential heating. Short-term daytime BC measurements were conducted at 50 sites (traffic and urban/suburban/regional background) and on-road along 12 routes. Daytime measurements were adjusted based on BC concentrations continuously monitored at a reference site. Indicative nighttime BC ambient concentrations were also measured at several residences across the area. Daytime BC concentrations recorded an average of 2.3 μg m-3 with considerable between-site variability. Concentrations at traffic sites were significantly higher (43% on average), compared with the rest of the sites. Varying levels were observed between background site subtypes, with concentrations at urban background sites (located near the center of Athens and the port of Piraeus) being 34% and 114% higher, on average, than at suburban and regional background sites, respectively. The traffic intensity at the nearest road and the population and built density in the surrounding area of sites were recognized as important factors controlling BC levels. On-road concentration measurements (5.4 μg m-3 on average) enabled the identification of hot-spots in the road network, with peak levels encountered along motorways (13.5 μg m-3 on average). Nighttime measurements demonstrated that wintertime BC pollution, enhanced by residential biomass burning for heating, affects the entire Athens basin. The reference site in central Athens was found to be representative of the temporal variability for daytime and nighttime BC concentrations at background locations.
Keywords: mobile measurements, microaethalometer, Athens, mapping, traffic, biomass burning
Published in RUNG: 10.05.2024; Views: 293; Downloads: 3
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Long-term variability, source apportionment and spectral properties of black carbon at an urban background site in Athens, Greece
Eleni Liakakou, Iasonas Stavroulas, Dimitris G. Kaskaoutis, Georgios Grivas, D. Paraskevopoulou, Umesh Chandra Dumka, M. Tsagkaraki, Aikaterini Bougiatioti, K. Oikonomou, J. Sciare, 2020, original scientific article

Abstract: This study aims to delineate the characteristics of Black Carbon (BC) in the atmosphere over Athens, Greece, using 4-year (May 2015–April 2019) Aethalometer (AE-33) measurements. The average BC concentration is 1.9 ± 2.5 μg m−3 (ranging from 0.1 to 32.7 μg m−3; hourly values), with a well-defined seasonality from 1.3 ± 1.1 μg m−3 in summer to 3.0 ± 4.0 μg m−3 in winter. Pronounced morning and evening/night peaks are found in the BC concentrations in winter, while during the rest of the seasons, this diurnal cycle appears to flatten out, with the exception of the morning traffic peak. On an annual basis, the biomass-burning fraction (BB%) of BC accounts for 22 ± 12%, while the fossil-fuel combustion (BCff) component (traffic emissions and domestic heating) dominates during summer (83%) and in the morning hours. BCwb exhibits higher contribution in winter (32%), especially during the night hours (39%). BC levels are effectively reduced by precipitation, while they significantly build-up for wind speeds <3 m s−1 and mixing-layer height (MLH) < 500 m. Normalizing the BC diurnal course by the MLH variations on a seasonal basis reveals that the residential wood-burning emissions are mostly responsible for the large BC increase during winter nights, whereas the low BC levels during daytime in the warm season are mainly attributed to dilution into a deeper MLH. BCwb is highly correlated with other BB tracers during winter nights (e.g. levoglucosan, non-sea-salt-K+, m/z 60 fragment), as well as with the fine fraction (PM2.5) OC and EC. The Delta-C, which represents the spectral dependence of BC as the absorption difference between 370 and 880 nm, is analyzed for the first time in Athens. It exhibits a pronounced seasonality with maximum values in winter night-time, and it appears as a valid qualitative marker for wood combustion.
Keywords: black carbon, wood burning, source apportionment, mixing layer, biomass burning tracers, Athens
Published in RUNG: 10.05.2024; Views: 286; Downloads: 1
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Long-term brown carbon spectral characteristics in a Mediterranean city (Athens)
Eleni Liakakou, Dimitris G. Kaskaoutis, Georgios Grivas, Iasonas Stavroulas, M. Tsagkaraki, D. Paraskevopoulou, Aikaterini Bougiatioti, Umesh Chandra Dumka, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2020, original scientific article

Abstract: This study analyses 4-years of continuous 7-λ Aethalometer (AE-33) measurements in an urban-background environment of Athens, to resolve the spectral absorption coefficients (babs) for black carbon (BC) and brown carbon (BrC). An important BrC contribution (23.7 ± 11.6%) to the total babs at 370 nm is estimated for the period May 2015–April 2019, characterized by a remarkable seasonality with winter maximum (33.5 ± 13.6%) and summer minimum (18.5 ± 8.1%), while at longer wavelengths the BrC contribution is significantly reduced (6.8 ± 3.6% at 660 nm). The wavelength dependence of the total babs gives an annual-mean AAE370-880 of 1.31, with higher values in winter night-time. The BrC absorption and its contribution to babs presents a large increase reaching up to 39.1 ± 13.6% during winter nights (370 nm), suggesting residential wood burning (RWB) emissions as a dominant source for BrC. This is supported by strong correlations of the BrC absorption with OC, EC, the fragment ion m/z 60 derived from ACSM and PMF-analyzed organic fractions related to biomass burning (e.g. BBOA). In contrast, BrC absorption decreases significantly during daytime as well as in the warm period, reaching to a minimum during the early-afternoon hours in all seasons due to photo-chemical degradation. Estimated secondary BrC absorption is practically evident only during winter night-time, implying the fast oxidation of BrC species from RWB emissions. Changes in mixing-layer height do not significantly affect the BrC absorption in winter, while they play a major role in summer.
Keywords: spectral aerosol absorption, brown carbon, wood burning, organic aerosols, chemical composition, Athens
Published in RUNG: 10.05.2024; Views: 298; Downloads: 1
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Carbonaceous aerosols in contrasting atmospheric environments in Greek cities : evaluation of the EC-tracer methods for secondary organic carbon estimation
Dimitris G. Kaskaoutis, Georgios Grivas, Christina Theodosi, M. Tsagkaraki, D. Paraskevopoulou, Iasonas Stavroulas, Eleni Liakakou, Antonis Gkikas, Nikolaos Hatzianastassiou, Cheng Wu, 2020, original scientific article

Abstract: This study examines the carbonaceous-aerosol characteristics at three contrasting urban environments in Greece (Ioannina, Athens, and Heraklion), on the basis of 12 h sampling during winter (January to February 2013), aiming to explore the inter-site differences in atmospheric composition and carbonaceous-aerosol characteristics and sources. The winter-average organic carbon (OC) and elemental carbon (EC) concentrations in Ioannina were found to be 28.50 and 4.33 µg m−3, respectively, much higher than those in Heraklion (3.86 µg m−3 for OC and 2.29 µg m−3 for EC) and Athens (7.63 µg m−3 for OC and 2.44 µg m−3 for EC). The winter OC/EC ratio in Ioannina (6.53) was found to be almost three times that in Heraklion (2.03), indicating a larger impact of wood combustion, especially during the night, whereas in Heraklion, emissions from biomass burning were found to be less intense. Estimations of primary and secondary organic carbon (POC and SOC) using the EC-tracer method, and specifically its minimum R-squared (MRS) variant, revealed large differences between the sites, with a prevalence of POC (67–80%) in Ioannina and Athens and with a larger SOC fraction (53%) in Heraklion. SOC estimates were also obtained using the 5% and 25% percentiles of the OC/EC data to determine the (OC/EC)pri, leading to results contrasting to the MRS approach in Ioannina (70–74% for SOC). Although the MRS method provides generally more robust results, it may significantly underestimate SOC levels in environments highly burdened by biomass burning, as the fast-oxidized semi-volatile OC associated with combustion sources is classified in POC. Further analysis in Athens revealed that the difference in SOC estimates between the 5% percentile and MRS methods coincided with the semi-volatile oxygenated organic aerosol as quantified by aerosol mass spectrometry. Finally, the OC/Kbb+ ratio was used as tracer for decomposition of the POC into fossil-fuel and biomass-burning components, indicating the prevalence of biomass-burning POC, especially in Ioannina (77%).
Keywords: carbonaceous aerosols, inorganic species, POC-SOC estimation, biomass burning, MRS method, Greece
Published in RUNG: 10.05.2024; Views: 257; Downloads: 3
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Impacts of severe residential wood burning on atmospheric processing, water-soluble organic aerosol and light absorption, in an inland city of Southeastern Europe
Dimitris G. Kaskaoutis, Georgios Grivas, K. Oikonomou, P. Tavernaraki, Kyriaki Papoutsidaki, M. Tsagkaraki, Iasonas Stavroulas, Pavlos Zarmpas, D. Paraskevopoulou, Aikaterini Bougiatioti, 2022, original scientific article

Abstract: This study examines the concentrations and characteristics of carbonaceous aerosols (including saccharides) and inorganic species measured by PM2.5 filter sampling and a multi-wavelength Aethalometer during two campaigns in a mountainous, medium-sized, Greek city (Ioannina). The first campaign was conducted in summer and used as a baseline of low concentrations, while the second took place in winter under intensive residential wood burning (RWB) emissions. Very high winter-mean OC concentrations (26.0 μg m−3) were observed, associated with an OC/EC ratio of 9.9, and mean BCwb and PM2.5 levels of 4.5 μg m−3 and 57.5 μg m−3, respectively. Simultaneously, record-high levoglucosan (Lev) concentrations (mean: 6.0 μg m−3; max: 15.9 μg m−3) were measured, revealing a severely biomass burning (BB)-laden environment. The water-soluble OC component (WSOC) accounted for 56 ± 9% of OC in winter, exhibiting high correlations (R2 = 0.93–0.97) with BB tracers (nss-K+, BCwb, Lev), nitrate and light absorption, potentially indicating the formation of water-soluble brown carbon (BrC) from fast oxidation processes. The examination of diagnostic ratios involving BB tracers indicated the prevalence of hardwood burning, while the mean Lev/OC ratio (22%) was remarkably higher than literature values. Applying a mono-tracer method based on levoglucosan, we estimated very high BB contributions to OC (∼92%), EC (∼64%) and WSOC (∼87%) during winter. On the contrary, low levels were registered during summer for all carbonaceous components, with winter/summer ratios of 4–5 for PM2.5 and BC, 10 for OC, 30 for BCwb and ∼1100 for levoglucosan. The absence of local BB sources in summer, combined with the photochemical processing and aging of regional organic aerosols, resulted in higher WSOC/OC fractions (64 ± 13%). The results indicate highly soluble fine carbonaceous aerosol fraction year-round, which when considered alongside the extreme concentration levels in winter can have important implications for short- and long-term health effects.
Keywords: carbonaceous aerosols, biomass burning, levoglucosan, WSOC, heterogeneous chemistry, Greece
Published in RUNG: 10.05.2024; Views: 277; Downloads: 2
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