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Ključne besede: carbonaceous aerosol, organic aerosol
Objavljeno v RUNG: 10.05.2024; Ogledov: 11; Prenosov: 0
Celotno besedilo (8,09 MB)

Opis: 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%).
Ključne besede: carbonaceous aerosols, inorganic species, POC-SOC estimation, biomass burning, MRS method, Greece
Objavljeno v RUNG: 10.05.2024; Ogledov: 11; Prenosov: 0
Celotno besedilo (2,64 MB)
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Opis: Absorption Ångström Exponent (AAE) and Scattering Ångström Exponent (SAE) values, derived from aethalometer and nephelometer measurements during a period of 3 years at an urban background site in Athens, are combined for the first aerosol type classification using in situ measurements in the eastern Mediterranean. In addition, single scattering albedo (SSA) and its wavelength dependence (dSSA), as well as the chemical composition of fine aerosols and precursor gases from collocated measurements, are utilized to provide further insights on the optical-chemical characterization and related sources of seven identified aerosol types. Urban aerosols are mostly characterized as Black Carbon (BC)-dominated (76.3%), representing a background atmosphere where fossil-fuel combustion is dominant throughout the year, while 14.3% of the cases correspond to the mixed Brown Carbon (BrC)-BC type, with a higher frequency in winter. The BrC type is associated with the highest scattering and absorption coefficients during winter nights, representing the impact from residential wood-burning emissions. Dust mixed with urban pollution (1.2%) and large particles mixed with BC (5.3%) have a higher frequency in spring. Furthermore, aging processes and BC coating with organic and inorganic species with weak spectral absorption (AAE<1) account for 2.2%, with a differentiation between small and large particles. dSSA is recognized as a useful parameter for aerosol characterization, since fine aerosols are associated with negative dSSA values. The identified aerosol types are examined on a seasonal, monthly, hourly basis and by potential source areas, as well as in comparison with fine-aerosol chemical composition and apportioned organic aerosol source contributions, in an attempt to explore the linkage between optical, physical and chemical aerosol properties. Chemical analysis indicates high organic fraction (60–68%) for the BrC and BrC/BC, 20–30% larger compared to other types. The results are essential for parametrization in chemical transport models and for reducing the uncertainty in the assessment of aerosol radiative effects.
Ključne besede: aerosol types, classification, AAE, SAE, dSSA, chemical composition, sources, Athens
Objavljeno v RUNG: 10.05.2024; Ogledov: 11; Prenosov: 0
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Opis: Abstract. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well-known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting Earth's radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols are not yet well constrained because these effects depend on the availability of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section (MAC) and absorption enhancement of BC particles (Eabs), at different wavelengths (from 370 to 880 nm for online measurements and at 637 nm for offline measurements) measured at two sites in the western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). The Eabs values ranged between 1.24 and 1.51 at the urban station, depending on the season and wavelength used as well as on the pure BC MAC used as a reference. The largest contribution to Eabs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 % and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 % and 4.6 % of the total enhancement at the short ultraviolet (UV) wavelength (370 nm) was due to externally mixed brown carbon (BrC) particles during the cold and the warm period, respectively. On average, at the MSY station, a higher Eabs value was observed (1.83 at 637 nm) compared to BCN (1.37 at 637 nm), which was associated with the higher fraction of organic aerosols (OA) available for BC coating at the regional station, as denoted by the higher organic carbon to elemental carbon (OC:EC) ratio observed at MSY compared to BCN. At both BCN and MSY, Eabs showed an exponential increase with the amount of non-refractory (NR) material available for coating (RNR-PM). The Eabs at 637 nm at the MSY regional station reached values up to 3 during episodes with high RNR-PM, whereas in BCN, Eabs kept values lower than 2 due to the lower relative amount of coating materials measured at BCN compared to MSY. The main sources of OA influencing Eabs throughout the year were hydrocarbon OA (HOA) and cooking-related OA (COA), i.e. primary OA (POA) from traffic and cooking emissions, respectively, at both 370 and 880 nm. At the short UV wavelength (370 nm), a strong contribution to Eabs from biomass burning OA (BBOA) and less oxidized oxygenated OA (LO-OOA) sources was observed in the colder period. Moreover, we found an increase of Eabs with the ageing state of the particles, especially during the colder period. This increase of Eabs with particle ageing was associated with a larger relative amount of secondary OA (SOA) compared to POA. The availability of a long dataset at both stations from offline measurements enabled a decade-long trend analysis of Eabs at 637 nm, that showed statistically significant (s.s.) positive trends of Eabs during the warmer months at the MSY station. This s.s. positive trend in MSY mirrored the observed increase of the OC:EC ratio over time. Moreover, in BCN during the COVID-19 lockdown period in spring 2020 we observed a sharp increase of Eabs due to the observed sharp increase of the OC:EC ratio. Our results show similar values of Eabs to those found in the literature for similar background stations.
Ključne besede: black carbomn, coating, organic aerosol, light absorption
Objavljeno v RUNG: 10.05.2024; Ogledov: 11; Prenosov: 0
Celotno besedilo (2,74 MB)
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Opis: Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites.
Ključne besede: aerosol, chemical composition, mass spectrometry, phenomenology
Objavljeno v RUNG: 10.05.2024; Ogledov: 11; Prenosov: 0
Celotno besedilo (9,75 MB)
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