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1.
Emission of volatile organic compounds from residential biomass burning and their rapid chemical transformations
Maximillien Desservettaz, Michael Pikridas, Iasonas Stavroulas, Aikaterini Bougiatioti, Eleni Liakakou, Nikolaos Hatzianastassiou, Jean Sciare, Nikolaos Mihalopoulos, Efstratios Bourtsoukidis, 2023, izvirni znanstveni članek

Opis: Biomass combustion releases a complex array of Volatile Organic Compounds (VOCs) that pose significant challenges to air quality and human health. Although biomass burning has been extensively studied at ecosystem levels, understanding the atmospheric transformation and impact on air quality of emissions in urban environments remains challenging due to complex sources and burning materials. In this study, we investigate the VOC emission rates and atmospheric chemical processing of predominantly wood burning emissions in a small urban centre in Greece. Ioannina is situated in a valley within the Dinaric Alps and experiences intense atmospheric pollution accumulation during winter due to its topography and high wood burning activity. During pollution event days, the ambient mixing ratios of key VOC species were found to be similar to those reported for major urban centres worldwide. Positive matrix factorisation (PMF) analysis revealed that biomass burning was the dominant emission source (>50 %), representing two thirds of OH reactivity, which indicates a highly reactive atmospheric mixture. Calculated OH reactivity ranges from 5 s−1 to an unprecedented 278 s−1, and averages at 93 ± 66 s−1 at 9 PM, indicating the presence of exceptionally reactive VOCs. The highly pronounced photochemical formation of organic acids coincided with the formation of ozone, highlighting the significance of secondary formation of pollutants in poorly ventilated urban areas. Our findings underscore the pressing need to transition from wood burning to environmentally friendly sources of energy in poorly ventilated urban areas, in order to improve air quality and safeguard public health.
Ključne besede: biomass burning, urban air quality, VOCs, emission factors, source apportionment
Objavljeno v RUNG: 13.05.2024; Ogledov: 314; Prenosov: 1
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2.
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, izvirni znanstveni članek

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: 267; Prenosov: 0
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3.
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, izvirni znanstveni članek

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: 275; Prenosov: 2
.pdf Celotno besedilo (4,65 MB)
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4.
Regional new particle formation as modulators of cloud condensation nuclei and cloud droplet number in the eastern Mediterranean
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, Nikolaos Mihalopoulos, 2019, izvirni znanstveni članek

Opis: A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN) are thought to originate from the condensational growth of new particle formation (NPF) from the gas phase. Here, 7 years of continuous aerosol and meteorological measurements (June 2008 to May 2015) at a remote background site of the eastern Mediterranean were recorded and analyzed to assess the impact of NPF (of 162 episodes identified) on CCN and cloud droplet number concentration (CDNC) formation in the region. A new metric is introduced to quantitatively determine the initiation and duration of the influence of NPF on the CCN spectrum. NPF days were found to increase CCN concentrations (from 0.10 % to 1.00 % supersaturation) between 29 % and 77 %. Enhanced CCN concentrations from NPF are mostly observed, as expected, under low preexisting particle concentrations and occur in the afternoon, relatively later in the winter and autumn than in the summer. Potential impacts of NPF on cloud formation were quantified by introducing the observed aerosol size distributions and chemical composition into an established cloud droplet parameterization. We find that the supersaturations that develop are very low (ranging between 0.03 % and 0.27 %) for typical boundary layer dynamics (σw ∼0.3 m s−1) and NPF is found to enhance CDNC by a modest 13 %. This considerable contrast between CCN and CDNC response is in part from the different supersaturation levels considered, but also because supersaturation drops from increasing CCN because of water vapor competition effects during the process of droplet formation. The low cloud supersaturation further delays the appearance of NPF impacts on CDNC to clouds formed in the late evening and nighttime – which has important implications for the extent and types of indirect effects induced by NPF events. An analysis based on CCN concentrations using prescribed supersaturation can provide very different, even misleading, conclusions and should therefore be avoided. The proposed approach here offers a simple, yet highly effective way for a more realistic impact assessment of NPF events on cloud formation.
Ključne besede: regional NPF, CCN, cloud droplets, Eastern Mediterranean, regional background
Objavljeno v RUNG: 13.05.2024; Ogledov: 315; Prenosov: 2
.pdf Celotno besedilo (3,07 MB)
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5.
Particle number size distribution statistics at City-Centre Urban Background, urban background, and remote stations in Greece during summer
S. Vratolis, Maria I. Gini, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, E. Kostenidou, E. Louvaris, D. Siakavaras, George Biskos, Nikolaos Mihalopoulos, 2019, izvirni znanstveni članek

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: 255; Prenosov: 0
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6.
Measurement of atmospheric black carbon in some South Mediterranean cities : seasonal variations and source apportionment
Hamza Merabet, Rabah Kerbachi, Nikolaos Mihalopoulos, Iasonas Stavroulas, Maria Kanakidou, Noureddine Yassaa, 2019, izvirni znanstveni članek

Opis: This study aims to investigate, for the first time in Algeria, the atmospheric black carbon (BC) concentrations over one year measured at the Scientific Observatory of Algiers and to compare their concentration levels with other Mediterranean cities (i.e., Athens and Crete). The diurnal cycles as well as seasonal variations of BC concentrations were evaluated and attributed to their emission sources (fossil fuel: BCff and wood burning: BCwb). The annual mean concentrations of BC, BCff and BCwb were 1.113±2.030, 1.064±2.002 and 0.049±0.262 µgm-3, respectively. The highest seasonal mean concentrations were recorded in summer and autumn with 1.283±1.346 and 1.209±1.149 µgm-3 for BC and 1.217±1.431 and 1.177±1.151 µgm-3 for BCff, respectively. However, the lowest mean concentrations were recorded in winter and spring with 1.023±1.189 and 0.966±0.964 µgm-3 for BC and 0.933±1.177 and 0.956±0.874 µgm-3 for BCff, respectively. For BCwb, the highest mean concentrations were reached in winter and summer with 0.090±0.055 and 0.066±0.050 µgm-3, respectively, very likely due to the forest fires and long-range transport of air pollution from Europe. The lowest mean concentrations of BCwb were recorded in autumn and spring with 0.032±0.033 and 0.010±0.021 µgm-3, respectively. Seggregating BC levels into eight wind sectors, showed that the prevailing BC pollution with concentrations reaching up to 5.000 µgm-3 originated from the North-West wind sector. A source apportionment of BC for the wet and dry period was also perfomed followed by a back trajectory cluster analysis for long-range transport.
Ključne besede: aerosol, black carbon, atmospheric pollution, source apportionment, seasonal variation, year modulation
Objavljeno v RUNG: 10.05.2024; Ogledov: 291; Prenosov: 3
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7.
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, izvirni znanstveni članek

Opis: 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.
Ključne besede: mobile measurements, microaethalometer, Athens, mapping, traffic, biomass burning
Objavljeno v RUNG: 10.05.2024; Ogledov: 290; Prenosov: 3
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8.
Yearlong measurements of monoterpenes and isoprene in a Mediterranean city (Athens) : natural vs anthropogenic origin
Anastasia Panopoulou, Eleni Liakakou, Stéphane Sauvage, Valérie Gros, Nadine Locoge, Iasonas Stavroulas, Bernard Bonsang, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2020, izvirni znanstveni članek

Opis: Monoterpenes and isoprene are important constituents of the volatile organic compounds (VOCs) due to their high reactivity and participation in ozone and secondary aerosol formation. The current work focuses on the results of a 13-month intensive campaign of high resolution time-resolved measurements of these compounds, at an urban background site in Athens, Greece. On an annual basis, monoterpenes (α-pinene and limonene) surpass the isoprene levels presenting mean values of 0.70 ± 0.83 μg m−3, 0.33 ± 0.78 μg m−3 and 0.19 ± 0.36 μg m−3, respectively. The large standard deviation highlights the significant diurnal and day-to-day variability. Isoprene presents a typical seasonal cycle, with a photochemically induced summer-time maximum. Enhanced noon levels are observed during summer, whereas a morning peak in the autumn and winter profiles occurs, despite the generally low levels encountered during these seasons. The monoterpenes deviate from the expected biogenic pattern, presenting higher mean levels during the cold period and a night-to-early morning enhancement strongly related to local anthropogenic tracers such as BC, CO, NO or toluene, as well as increased levels under wind speeds lower than 3 m s−1. Estimations of the anthropogenic and biogenic fractions based on the enhancement ratios of α-pinene versus a variety of anthropogenic tracers, demonstrate a clear dominance of the anthropogenic sources in all studied seasons. Simultaneously, the biogenic fraction increased during summer relative to winter by more than 10 times. Both α-pinene and limonene significantly contribute to locally formed secondary organic aerosol (SOA), determined by means of an ACSM, accounting for at least 22% and 13% of their levels in summer and winter respectively. Additionally, monoterpenes and isoprene contribute 6% to the observed oxidants levels (O3 + NOx) during summer.
Ključne besede: volatile organic compounds, biogenic compounds, monoterpenes, isoprene, Athens
Objavljeno v RUNG: 10.05.2024; Ogledov: 300; Prenosov: 2
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9.
On the regional aspects of new particle formation in the Eastern Mediterranean : a comparative study between a background and an urban site based on long term observations
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Georgios Grivas, Iasonas Stavroulas, Nikos Kalivitis, Eleni Liakakou, Evangelos Gerasopoulos, Christodoulos Pilinis, Nikolaos Mihalopoulos, 2020, izvirni znanstveni članek

Opis: Atmospheric new particle formation (NPF) is an important source of submicron particles. In remote background environments where local sources are scarce such processes may impact significantly on climate-relevant parameters. On the other hand, in urban environments, newly-formed particles are adding up to submicron particles emitted from primary sources. As the exact mechanism which triggers NPF still remains elusive, so are the circumstances for simultaneous occurrence of such events in two different environments (urban vs. regional background). In this study, concurrent number size distribution measurements were conducted in the urban environment of Athens and at the regional background site of Finokalia, Crete, located 340 km away and spanning a 2-year period. It occurred that the relative frequency of NPF was similar at both sites (around 20%), with a higher frequency during spring and autumn at the urban site, while at the background site most events took place in August and December, during the studied period. There were 35 event days when NPF took place at both sites simultaneously, all associated with air masses originating from the Northern sector, indicating the presence of regional events in the extended geographical area and characterized by low condensation sink (CS). By comparing the common with the non-common class I NPF episodes, we conclude that the conditions applying when regional NPF events with growth are observed in the same day at the surface level of both areas, are: (i) lower CS, (ii) higher SO2 concentrations, (iii) lower RH, and finally (iv) lower formation and growth rates than those observed during the site-specific and more rapidly evolving NPF events.
Ključne besede: NPF, Athens, Eastern Mediterranean, particle number concentrations, size distributions, concurrent regional events
Objavljeno v RUNG: 10.05.2024; Ogledov: 290; Prenosov: 0
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10.
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, izvirni znanstveni članek

Opis: 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.
Ključne besede: spectral aerosol absorption, brown carbon, wood burning, organic aerosols, chemical composition, Athens
Objavljeno v RUNG: 10.05.2024; Ogledov: 294; Prenosov: 1
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