Aerosol Sources Research Articles

Analysis method for aerosol deposition behavior under sodium spray fire

Sodium spray fire is a significant containment-related safety concern in sodium-cooled fast reactors (SFR). In a highly-energetic accident such as a core disruptive accident (CDA), the sodium spray fire not only poses a threat to containment integrity but also causes the generation and release of sodium aerosol source terms with strong radioactivity and chemical hazards. In our method, the sodium aerosol generation model, log-normal size distribution model, agglomeration models, and deposition models were applied. In particular, different turbulent energy dissipation rates were considered in the agglomeration models according to the different thermal-hydraulic states of containment and confinement, and the simplified Crump model and Beresnev models have been selected to describe the gravity-diffusion and the thermophoresis deposition behavior respectively, due to the specific conditions of sodium spray fires. Simulation studies have been divided into two categories based on a potential design concept: HTCA, AB5, and AB6 experiments were introduced to describe the drastic thermodynamic state variations caused by spray fires in the confinement, while ATF and AB7 experiments characterized a relatively stable environment similar to the containment. From the simulation results, the analysis method can be considered reasonable with respect to experimental values. Moreover, calculations have been performed for a hypothetical sodium spray fire caused by a rotator plug failure case in a paper-based European SFR.

Neutral saccharides and hemicellulose over two urban sites in Indo-Gangetic Plain and Central Europe during winter

Saccharides are ubiquitous organic compounds that are omnipresent in nature and are considered tracers of aerosol sources. Saccharides and hemicellulose were analyzed in the aerosols of two polluted regions (Allahabad, India and Sosnowiec, Poland). The chemical compositions of the compounds and their abundances were significantly different at the two sites. Levoglucosan was the most dominant saccharide present at both sites. Galactosan, anhydroglucofuranose, mannosan, glucose, arabitol, D-pinitol, sucrose, and trehalose were found in Allahabad samples in high abundance but were significantly lower than levoglucosan. Mannosan, galactosan, arabinose, glycerol, and sucrose were significant compounds in Sosnowiec after dominating levoglucosan. The major sources of saccharides present in the Allahabad aerosols are hardwood and agricultural waste-burning emissions, whereas those at Sosnowiec are attributed to the burning of softwood (mainly gymnosperm trees), pine needles, or sporadically grass during the winter. Further, the chemical characteristics of hemicellulose remnants present in ambient aerosol at the Indian and European sites were analyzed and discussed. At both locations, hemicellulose was found using methanolysis of the filter samples; however, its state of preservation was poor. We believe that the primary sources of hemicellulose remnants are incomplete wood burning, crop straw, grass burning, or plant debris. Relatively poor preservation is associated with partial hemicellulose degradation when exposed to elevated temperatures or due to the oxidation and microbial degradation of plant fragments.

Sources, variability, long-term trends, and radiative forcing of aerosols in the Arctic: implications for Arctic amplification.

Atmospheric pollution in the Arctic has been an important driver for the ongoing climate change there. Increase in the Arctic aerosols causes the phenomena of Arctic haze and Arctic amplification. Our analysis of aerosol optical depth (AOD), black carbon (BC), and dust using ground-based, satellite, and reanalysis data in the Arctic for the period 2003-2019 shows that the lowest amount of all these is found in Greenland and Central Arctic. There is high AOD, BC, and dust in the northern Eurasia and parts of North America. All aerosols show their highest values in spring. Significant positive trends in AOD (> 0.003year-1) and BC (0.0002-0.0003year-1) are found in the northwestern America and northern Asia. Significant negative trends are observed for dust (- 0.0001year-1) around Central Arctic. Seasonal analysis of AOD, BC, and dust reveals an increasing trend in summer and decreasing trend in spring in the Arctic. The major sources of aerosols are the nearby Europe, Russia, and North America regions, as assessed using the potential source contribution function (PSCF). Anthropogenic emissions from the transport, energy, and household sectors along with natural sources such as wildfires contribute to the positive trends of aerosols in the Arctic. These increasing aerosols in the Arctic influence Arctic amplification through radiative effects. Here, we find that the net aerosol radiative forcing is high in Central Arctic, Greenland, Siberia, and Canadian Arctic, about 2-4 W/m2, which can influence the regional temperature. Therefore, our study can assist policy decisions for the mitigation of Arctic haze and Arctic amplification in this environmental fragile region of the Earth.

Characterization and sources of carbonaceous aerosols in southwest plateau of China: Effects of biomass burning and low oxygen concentration

Carbonaceous aerosols affect atmospheric radiation and visibility and endanger human health. Administrative border and topography have created significant research interests focused on Yunnan Province. We studied the chemical characteristics and sources of OC and EC in four Yunnan cities using manual sampling and positive definite matrix factorization (PMF). Backward trajectories, cluster analysis, potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) were used to evaluate the transport pathways and potential source of carbonaceous aerosols during spring. The impacts of the transport of Biomass burning (BB) emissions in Southeast Asia and incomplete combustion on carbonaceous aerosols were highlighted in the study. Daily PM2.5 concentration ranged from 12.00 μg/m3 to 91.50 μg/m3, with the average concentration of 34.03 ± 13.49 μg/m3. OC and EC accounted for 19.85–44.94 % and 4.99–13.16 % of PM2.5. Average secondary organic carbon (SOC) concentration ranged from 0.82 μg/m3 ∼ 6.42 μg/m3, exhibiting the highest secondary conversion rate in autumn. BB was identified as the largest single source of carbonaceous aerosols through PMF analysis. The results of backward trajectory showed that more than 63.68 % of air mass originated from Myanmar in spring, and Myanmar, Laos and Vietnam were identified as the major potential source areas by PSCF and CWT. Biomass plumes emitted by some Southeast Asian countries in the spring are likely to be transported to the Yunnan Province under the guidance of southwest winds, thereby affecting local carbonaceous aerosols. The proportions of OC and EC in PM2.5 of the Yunnan Plateau were found higher than those in the four plains of China (Northeast Plain, North China, Middle-Lower Yangtze, and Guanzhong Plain). Incomplete combustion caused by low oxygen concentrations at high altitudes was considered as the cause.

Establishment of a Halophilic Bloom in a Sterile and Isolated Hypersaline Mesocosm.

Extreme environments, including hypersaline pools, often serve as biogeographical islands. Putative colonizers would need to survive transport across potentially vast distances of inhospitable terrain. Hyperhalophiles, in particular, are often highly sensitive to osmotic pressure. Here, we assessed whether hyperhalophiles are capable of rapidly colonizing an isolated and sterile hypersaline pool and the order of succession of the ensuing colonizers. A sterile and isolated 1 m3 hypersaline mesocosm pool was constructed on a rooftop in Charleston, SC. Within months, numerous halophilic lineages successfully navigated the 20 m elevation and the greater than 1 km distance from the ocean shore, and a vibrant halophilic community was established. All told, in a nine-month period, greater than a dozen halophilic genera colonized the pool. The first to arrive were members of the Haloarchaeal genus Haloarcula. Like a weed, the Haloarcula rapidly colonized and dominated the mesocosm community but were later supplanted by other hyperhalophilic genera. As a possible source of long-distance inoculum, both aerosol and water column samples were obtained from the Great Salt Lake and its immediate vicinity. Members of the same genus, Haloarcula, were preferentially enriched in the aerosol sample relative to the water column samples. Therefore, it appears that a diverse array of hyperhalophiles are capable of surviving aeolian long-distance transport and that some lineages, in particular, have possibly adapted to that strategy.

Observational insights into the environmental effect for secondary inorganic aerosol formation in the Northeast China: Influence of biomass burning

Secondary inorganic aerosols (SIA), as one of the main ubiquitous components of PM2.5, still have unclear impacts on their formation in the ambient environment, especially under extremely cold weather conditions. To explore the effects of open biomass burning (OBB) source emissions and meteorological factors on SIA formation, biomass burning tracer, i.e., levoglucosan (LG), was observed along with SIA were analyzed during the heating season at the Longfengshan (LFS) background of Northeast China. Based on the LG/OC ratio and fire hotspots, the entire sampling campaign was divided into OBB and non-open biomass burning (NBB) periods.It was found that OBB emissions had little effect on sulfate formation but a significant impact on nitrate formation. High relative humidity (RH) conditions played a crucial role in SIA formation, with both SO42−/EC and NO3−/EC increasing as RH elevated at temperatures below −10 °C. Furthermore, the temperature dependence of SO42−/EC and NO3−/EC indicated that temperature could enhance the activity of either aqueous-phase production or gas-phase reactions, subsequently promoting the formation of SO42− and NO3− in the ambient environment. Additionally, positive matrix factorization (PMF) analysis was used to scientifically separate the sources of ambient aerosols during OBB and NBB periods.

Contribution of fossil and biomass-derived secondary organic carbon to winter water-soluble organic aerosols in Delhi, India

Delhi, among the world's most polluted megacities, is a hotspot of particulate matter emissions, with high contribution from organic aerosol (OA), affecting health and climate in the entire northern India. While the primary organic aerosol (POA) sources can be effectively identified, an incomplete source apportionment of secondary organic aerosol (SOA) causes significant ambiguity in the management of air quality and the assessment of climate change. Present study uses positive matrix factorization analysis on the water-soluble organic aerosol (WSOA) data from the offline-aerosol mass spectrometry (AMS). It revealed POA as the dominant source of WSOA, with biomass-burning OA (31–34 %) and solid fuel combustion OA (∼21 %) being two major contributors. Here we use water-solubility fingerprints to track the SOA precursors, such as oxalates or organic nitrates, instead of identifying them based on their O:C ratio. Non-fossil precursors dominate in more oxidized oxygenated organic carbon (MO-OOC) (∼90 %), a proxy for aged secondary organic carbon (SOC), by coupling offline-AMS with 14C measurements. On the contrary, the oxidation of fossil fuel emissions produces a large quantity of fresh fossil SOC, which accounts for ∼75 % of less oxidized oxygenated organic carbon (LO-OOC). Our study reveals that apart from major POA contributions, large fractions of fossil (10–14 %) and biomass-derived SOA (23–30 %) contribute significantly to the total WSOA load, having impact on climate and air quality of the Delhi megacity. Our study reveals that large-scale unregulated biomass burning was not only found to dominate in POA but was also observed to be a significant contributor to SOA with implications on human health, highlighting the need for effective control strategies.

Oxidative potential in rural, suburban and city centre atmospheric environments in central Europe

Abstract. Oxidative potential (OP) is an emerging health-related metric which integrates several physicochemical properties of particulate matter (PM) that are involved in the pathogenesis of the diseases resulting from exposure to PM. Daily PM2.5-fraction aerosol samples collected in the rural background of the Carpathian Basin and in the suburban area and centre of its largest city of Budapest in each season over 1 year were utilised to study the OP at the related locations for the first time. The samples were analysed for particulate matter mass, main carbonaceous species, levoglucosan and 20 chemical elements. The resulting data sets were subjected to positive matrix factorisation to derive the main aerosol sources. Biomass burning (BB), suspended dust, road traffic, oil combustion mixed with coal combustion and long-range transport, vehicle metal wear, and mixed industrial sources were identified. The OP of the sample extracts in simulated lung fluid was determined by ascorbic acid (AA) and dithiothreitol (DTT) assays. The comparison of the OP data sets revealed some differences in the sensitivities of the assays. In the heating period, both the OP and PM mass levels were higher than in spring and summer, but there was a clear misalignment between them. In addition, the heating period : non-heating period OP ratios in the urban locations were larger than for the rural background by factors of 2–4. The OP data sets were attributed to the main aerosol sources using multiple linear regression with the weighted least squares approach. The OP was unambiguously dominated by BB at all sampling locations in winter and autumn. The joint effects of motor vehicles involving the road traffic and vehicle metal wear played the most important role in summer and spring, with considerable contributions from oil combustion and resuspended dust. In winter, there is temporal coincidence between the most severe daily PM health limit exceedances in the whole Carpathian Basin and the chemical PM composition causing larger OP. Similarly, in spring and summer, there is a spatial coincidence in Budapest between the urban hotspots of OP-active aerosol constituents from traffic and the high population density in central quarters. These features offer possibilities for more efficient season-specific air quality regulations focusing on well-selected aerosol sources or experimentally determined OP, rather than on PM mass in general.

Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain, Northwest China: The importance of biomass burning

The concentration of PM2.5 has considerably reduced in recent years, but remains relatively high in China. In particular, the increasing contribution of organic compounds to PM2.5 generates popular pressure for further reductions, resulting in an urgent need to study organic aerosol (OA). To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain, Northwest China, PM2.5 samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer compounds. The mean concentration of total measured organic compounds is 662 ± 296 ng/m3 in summer and 3258 ± 1925 ng/m3 in winter. Levoglucosan is the most abundant single compound found throughout the sampling period, which is a crucial tracer for biomass burning emissions, preliminary suggesting that biomass burning is an essential source of OA. In summer, organic compounds such as lipid compounds, sugar compounds, and polycyclic aromatic hydrocarbons (PAHs), more come from higher plants, wood burning, vehicle exhausts, plastic waste, and other direct emission sources. Oxygenated PAHs (OPAHs), nitrophenols, and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors, especially photochemical oxidation. However, in winter, most of the increases in concentrations of organic compounds are attributed to biomass burning. The analysis of a haze event (14–19 January 2017) during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity (49.1% ± 13.5%). The main reason for the growth of OA in this haze event is the accumulation of primary OA (POA). The source apportionment by the positive matrix factorization (PMF) model shows that biomass burning (37.1%) is the primary source of OA in the rural regions of the Guanzhong Plain, especially in winter (40.6%). The contribution of secondary formation decreases from 26.0% in summer to 16.9% in winter, and the contribution of fossil fuel emissions is comparable across both seasons.

Temporal variations, sources, and regional transport of carbonaceous species in PM2.5 in a northern China city: the role of domestic heating

Domestic heating is an important source of carbonaceous aerosols in northern China in winter. The seasonal variations, sources, and regional transport of carbonaceous species in PM2.5 in Yuncheng in the winter and summer of 2020–2021 were investigated in this study, with a particular focus on the role of domestic heating. Meanwhile, the pollution characteristics of carbonaceous aerosols in Beijing in winter were also investigated for comparison. The mass concentrations of organic carbon (OC) and elemental carbon (EC) and their contributions to PM2.5 were significantly enhanced during the heating period compared to other sampling periods in Yuncheng, however, no obvious differences were observed before and during the heating periods in Beijing. Source apportionment results showed that the heating related emission (50.9%) was the dominant source of total carbon in Yuncheng in the heating period, while vehicular emission (49.6%) was dominant in summer. Combing the positive matrix factorization (PMF) and potential source contribution function (PSCF) analysis, it was concluded that both local and regional heating activities contributed highly to carbonaceous aerosols in Yuncheng. It would be therefore of great environmental benefits to promote the clean residential heating transition in Yuncheng and other similar cities.Graphical

Primary and Secondary Organic Aerosol Formation from Asphalt Pavements.

Asphalt is ubiquitous across cities and a source of organic compounds spanning a wide range of volatility and may be an overlooked source of urban organic aerosols. The emission rate and composition depend strongly on temperature, but emissions have been observed at both application temperatures and surface temperatures during warm sunny days. Here we report primary organic aerosol (POA) emissions and secondary organic aerosol (SOA) production from asphalt. We reheated real-world asphalt samples to application-relevant temperatures (∼130 °C) and typical summertime road-surface temperatures (∼55 °C) and then flushed the emitted vapors into an environmental oxidation chamber containing ammonium sulfate seed particles. SOA was then formed following the photo-oxidation of emissions under high-NOx conditions typical of urban atmospheres. We find that POA only forms at application temperature as it does not require further oxidation, whereas SOA forms under both conditions; with the resulting POA and SOA both being semi-volatile. While total OA formation rates were substantially greater under the limited time spent under application conditions, SOA formation from passive asphalt heating presents a potential long-term source, as heating continues for the lifetime of the road surface. This suggests that persistent asphalt solar heating is likely a considerable and continued source of summertime SOA in urban environments.

A novel calibration method for continuous airborne metal measurements: Implications for aerosol source apportionment

Continuous metal monitors have been widely used in environmental monitoring due to the high temporal resolution, high detection limit, and necessity for near real-time source apportionment. However, the reliability of the conventional calibration method, the deviation caused by uncalibrated monitoring data, and the subsequent impact on source identification results are rarely discussed. In this study, a reliable multi-point calibration approach by Primary Standard Aerosol Mass Concentration Calibration System (PAMAS) for the Xact625i Ambient Metals Monitor was developed and applied. The measured data was almost meaningless in the low-concentration range with bias even exceeding 100 % by using the conventional single-point calibration method based on thin-film standards. PAMAS was utilized to generate aerosols with known concentrations of the 20 metal elements including Al, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Sr, Cd, Sn, Sb, Ba, Tl, Pb, and Bi, in two concentration ranges of 150–1200 ng m−3 and 2.5–30 ng m−3 to validate the Xact625i Monitor. The results showed that the elemental concentrations were underestimated, especially in the low-concentration range, only for Cr, As, and Sr with slopes close to unity (1.00 ± 0.03). After calibration by PAMAS, the slopes of the linear relationships between measured and standard concentrations were all unity for the 19 elements in the high-concentration range, and close to unity for the 15 elements in the low-concentration range, and the accuracy of the remaining elements was also improved. After considering the calibration of aerosol metal data, it was found the number of source factors and their contributions to metals and PM2.5 in Chongming Dongtan, China, based on the PMF model significantly changed. This study highlighted the need of developing reliable calibration methods for online aerosol monitoring instruments and implied that the source apportionment results could be biased without careful data calibration.

Estimation of Spatial Distribution of Potential Sources of Carbonaceous Aerosol from Local Measurements Near St. Petersburg

The results of back-trajectory analysis of nine-year (2013–2021) measurements of organic (OC) and elemental (EC) aerosol carbon concentrations made at the atmospheric monitoring station near St. Petersburg (Peterhof, 59.88° N, 29.83° E) are presented. The spatial location of sources was estimated by the concentration weighted trajectory method (CWT) in the geographic area 16°–44° E × 48°–68° N. The obtained data allow us to identify the territories with the strongest organic and elemental carbon emissions and to estimate the seasonal variability of these emissions. In particular, the obtained estimates show that the most intense sources of organic and elemental aerosol carbon in the studied region are located in the Volga-Oka interfluve and on the adjacent territories. It is demonstrated that linear regression coefficients between CWT function values for organic and elemental carbon differ for different regions and seasons and may indicate the prevailing type of sources of carbon-containing aerosol particles.

Conditionally Background Level of Aerosol Pollution of Near-Surface Air in Moscow and One of Its Suburbs: Seasonal Variations

The data of continuous observations of aerosol composition in the near-surface atmosphere in Moscow (in the city center) and in Moscow region (near Zvenigorod, Moscow region) for three years, from autumn 2019 to the end of 2022, are analyzed. The obtained data were compared with the results of observations on the Moscow network stations “Mosecomonitoring”. The concept of conditionally background aerosol pollution of the atmosphere in Moscow is introduced for those days when the average daily concentration of PM10 is less than the MPC value (60 µg/m3). Previously, the authors found that all episodes of increased aerosol pollution in Moscow with daily average PM10 concentration higher than the MPC value, are associated either with the presence of a close local source in the city itself, or with the long-range transport of fire aerosols and/or dust from other territories to the Moscow region. The average daily PM2.5 concentration in the city and the suburb is lower than the MPC (35 µg/m3) all year round. The days corresponding to the introduced conditional background make up more than 91% over three years in the center of Moscow. Such a conditional background is formed by both natural and anthropogenic sources of aerosols, and not only of local, but also of remote origin. It implicitly takes into account the influence of meteorological conditions on sources and sinks of aerosols, as well as advective air mass transport of aerosol to and from the city. Seasonal variations in mass concentration of PM10, PM2.5 particles and individual chemical elements, as well as in the distribution of chemical elements by the size of aerosol particles in near-surface atmosphere under conditionally background pollution are analyzed. The emphasis is placed on the similarity and difference in the conditionally background near-surface aerosol for the city and the suburb in different seasons.

Online monitoring of carbonaceous aerosols in a northern Chinese city: Temporal variations, main drivers, and health risks

This study examined the variability and source of carbonaceous aerosols, encompassing total carbon (TC), organic carbon (OC), and secondary organic carbon (SOC) for the years 2019–2020, as well as equivalent black carbon (eBC) and equivalent ultraviolet BC (eUVBC) data spanning 2019–2022, in the context of a typical northern Chinese city: Yanzhou. Averaged concentrations of TC, OC, SOC, eBC, eUVBC, and the ratio (OC/elemental carbon (EC)) reached 11.1 ± 6.7, 8.9 ± 5.1, 3.9 ± 2.0, 3.1 ± 1.3, and 4.3 ± 2.4 μg/m3, and 5.0 ± 2.2, respectively. The concentrations of TC, OC, eBC, and eUVBC were higher in winter, followed by spring and autumn, and summer, while SOC presented the opposite seasonal patterns. The diurnal variations of TC, OC, eBC, and eUVBC exhibited a bimodal pattern with peaks in the early morning (08:00–09:00 LT) and late evening (00:00–01:00 LT) and a trough in the afternoon (14:00–16:00 LT), pointing to vehicular emission and meteorological dispersion as major drivers of the hourly variability. The results obtained from the EC tracer method and minimum R squared (MRS) revealed that r(SOC/OC) were highest in summer (60%) and lowest in winter (26%), showing a fast summer photochemical oxidation of volatile organic compounds (VOCs) that generate SOC. In this study, the influence of meteorological conditions on the weighting of diverse carbonaceous aerosols was quantified using a machine learning method. Results showed that the main drivers of carbonaceous aerosols were height of the planetary boundary layer (HPBL), ambient temperature (AT), relative humidity (RH), and atmospheric pressure (AP) in all seasons. Additionally, the potential health risks of eBC based on the equivalent passive smoking of cigarettes (PSC) suggested that there was a certain level of human health risk in this city. The obtained results will provide more in-depth and comprehensive understanding of carbonaceous aerosol pollution and management strategies.

Assessing the role of atmospheric dispersion vs. emission strength in the southern Po Valley (Italy) using dispersion-normalised multi-time receptor modelling

In this paper, we applied the Dispersion Normalised Positive Matrix Factorisation (DN-PMF) approach recently proposed in the literature to provide a more realistic picture of the relative importance of emission strength vs. atmospheric dispersion conditions. The disentanglement of such effects is of great concern in pollution hot spots like the Po Valley (Italy), where particulate matter limit values are exceeded despite the existing abatement measures. To explore the potentiality of the DN-PMF approach – still scarcely applied in the literature – a well-chemically characterised PM1 (atmospheric particles with aerodynamic diameter <1 μm) dataset comprising samples collected at different time resolutions at an urban background site (Bologna) in the southern Po Valley was used. Indeed, it is well known that shallow mixing layers promote pollutant accumulation but this observation is not enough to exclude an enhancement of emission strength which could be tackled by appropriate abatement strategies.The source apportionment of sub-micron sized aerosols having a quite long atmospheric residence time in a complex environment like the Po Valley - which is also strongly impacted by secondary aerosol formation on a basin-scale - is generally quite challenging when using receptor models. Due to the availability of a huge dataset with variables having multiple time resolutions, in this work the DN-PMF was implemented in a multi-time resolution approach (MT) to achieve a better source identification and to gain knowledge about the relative importance of atmospheric dilution vs. emissions. A comparison between results obtained by the application of the regular multi time resolution (REG-MT) vs. the DN-MT approach is presented here for the five factors identified (nitrate-dominated, sulphate-dominated, biomass burning, mineral dust, and urban aerosol). The first interesting outcome is that REG-MT and DN-MT results do not point at significant differences in temporal patterns for aerosol components and sources impacting at the basin-scale (i.e. sulphate- and nitrate-dominated aerosol, biomass burning) thus suggesting that the diel modulation of these PM1 emissions is somehow masked by the stronger variability of the mixing layer. Conversely, contributions from local sources with more pronounced diel variation like traffic are quite well reproduced by DN-MT and the ambient concentrations are enhanced compared to REG-MT. This is an important piece of information highlighting that PM1 concentrations from local sources have been likely underestimated by REG-MT assessments.To our knowledge, this is one of the very few applications of DN-MT and the first one at a European site where the huge effort made to implement air pollution containment measures is still not very much effective in reducing PM levels; moreover, in this paper a detailed discussion about the possible interpretation of the output of DN-MT in terms of temporal patterns is reported.

Sulfate sources, biologic cycling, and mobility in Atacama Desert soils revealed by isotope signatures

A set of 55 surface samples from Atacama Desert gypsisols was collected along four altitude transects and analyzed for ∆17OSO4, δ18OSO4, δ34SSO4, and 87Sr/86Sr in order to identify the main depositional mechanisms and quantify the proportional contribution of sulfate sources across the desert's main topographic units – the Coastal Cordillera, the Central Depression, and the Precordillera. Sulfate deposited at any location in the Atacama Desert may derive from up to five different source and process endmembers that can principally be identified by their isotopic composition. Three aerosol sources dominate sulfate deposition and accumulation in gypsisols throughout the Atacama. These are secondary atmospheric Ca- and Na-sulfate derived from global volcanic SO2 oxidized by ozone and its derivates, and a marine sulfate aerosol that is roughly a 9:1 mixture of sea salt (primary) sulfate from evaporated sea spray, and secondary non-sea salt sulfate, i.e., dimethyl sulfide (DMS) mainly oxidized by ozone. These marine sources dominate sulfate deposition in the Coastal Cordillera. Unlike in most places on Earth, the positive mass-independent ∆17OSO4 signature of secondary atmospheric sulfate is ubiquitous in Atacama Desert soils and is never completely erased by biologic cycling. Hence, biologic cycling of the sulfate inventory – i.e., the reduction of sulfate, subsequent oxygen isotope exchange with water, and re-oxidation – is apparently not quantitative in any of the Atacama Desert environments sampled here, including the most biologically active permanent salt lakes. The preservation of highest ∆17OSO4 values (∼ 1.0‰) at altitudes of the Coastal Cordillera above the 1200 m altitude cut-off level of fog advection suggest that episodic rainfall events are insufficient for significant in situ biologic sulfate turnover. At lower altitudes and regular fog advection, moisture supply appears to be sufficient for limited in situ biologic sulfate turnover. Overall, biologically recycled sulfate constitutes a fourth major contributor to the desert's gypsisol sulfate inventory. This may comprise fluvially redeposited sulfate from older sediments, particularly on the debris fans protruding from the Precordillera into the Central Depression. In the Central Depression, Sr-isotopes may allow for a further distinction between redeposition-dominated and aerosol-dominated sedimentation environments. On the Precordillera, rainfall and run-off provide sufficient moisture for significant but still incomplete in situ biologic sulfate cycling. Hydrothermal non-evaporitic Na-sulfate – the fifth potential source – likely originates from larger outflow events or mobilization from rock veins over the course of the Atacama's geologic history may contribute locally to the sulfate inventory. The degree of bio-cycling and mobility of sulfate likely reflects a balance between overall water availability and the mixing proportion of very soluble (mobile) Na-sulfate and less soluble Ca-sulfate inherent in the various sulfate sources.

Cooking as an organic aerosol source leading to urban air quality degradation

Air quality degradation events in the urban environment are often attributed to anthropogenic aerosol sources related to combustion of liquid or solid fuels in various activities. The effects of massive cooking emissions during Greek nationwide traditional festivities were investigated by a combined characterization of particulate matter (PM) levels and organic aerosol (OA) sources. Focus was centered on periods around two major festivities, namely “Fat Thursday” and Easter Sunday along six different years. OA sources were apportioned through Positive Matrix Factorization (PMF) on Aerosol Chemical Speciation Monitor (ACSM) mass spectra, while the spatial characteristics of the episodes were assessed through a low-cost, sensor-based PM2.5 monitoring network operating in Athens and other Greek cities. Contrasts were examined by considering a 15-day period around each event, while the effect of the 2020–2021 mobility restrictions, related to COVID-19, was also assessed. An episode-specific cooking organic aerosol (COA) spectral profile was delineated, and can be considered as a reference for ambient COA from meat grilling. Severe pollution episodes that affected the entire Athens basin were recorded, with PM2.5 concentrations exceeding 300 μg m−3 on occasions. COA contributions dominated primary organic aerosol (POA) and made up almost half of OA concentrations. During “Fat Thursday” COA concentrations and contributions peaked during night-time (23.2 μg m−3 and 46 %, respectively) while for Easter Sunday COA maxima were recorded in the early afternoon (27.4 μg m−3 and 39 %). Analyzing a full-year OA source dataset, revealed a pronounced recreational cooking pattern in central Athens, with COA concentrations rising towards the weekend, reflecting the impact of the food service sector. In view of the upcoming review of the EU air quality directive, foreseeing stricter annual PM2.5 limits as well as 24-h limit values and related alerts, the mitigation of cooking emissions appears as a potent instrument for achieving tangible air quality benefits.

Analysis of the Vertical Distribution and Driving Factors of Aerosol and Ozone Precursors in Huaniao Island, China, Based on Ground-Based MAX-DOAS

Urban air pollution has become a regional environmental problem. In order to explore whether island areas were affected by the urban development of surrounding areas, in this paper, we systematically study the vertical distribution characteristics of atmospheric components, meteorological drivers, potential pollution sources, and the population health risks of fine particulate matter in island cities in China. The vertical profiles of three atmospheric pollutants (aerosols, NO2, and HCHO) in the lower troposphere of Huaniao Island in the East China Sea (ECS) were obtained using ground-based multi-axial differential optical absorption spectroscopy (MAX-DOAS). The results show that the aerosol extinction coefficients, NO2, and HCHO were primarily distributed at altitudes below 1 km, and the atmospheric pollutants in Zhoushan were obviously affected by high-altitude transfer. The main meteorological driving factors of aerosols, NO2, and HCHO were different at different altitudes. The key factor contributing to the high column concentrations of NO2 and HCHO in the upper air (greater than 400 m) was the transport of pollutants brought about by changes in wind speed. By exploring the main potential sources of atmospheric pollutants, it was found that the main sources of aerosols, NO2, and HCHO are coastal cities in the Yangtze River Delta, including southeast Zhejiang Province, southeast Fujian Province, Shanghai, ECS, and the Yellow Sea. Compared with aerosols and HCHO, local primary emissions are an important source of NO2, which are mainly related to industrial activities in Zhoushan Port. In addition, using the expose-response function model, the number of attributable cases of PM2.5 air pollution in Zhoushan City in 2019 accounted for 6.58% of the total population. This study enriches our understanding of the vertical distribution characteristics of atmospheric composition and health risk assessment on Chinese islands.

High enrichment of heavy metals in fine particulate matter through dust aerosol generation

Abstract. Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Here, we generated dust aerosols from soils to determine if there is particle-size-dependent selectivity of heavy metals in the dust generation. Mn, Cd, Pb and other heavy metals were found to be highly enriched in fine-dust (PM2.5) aerosols, which can be up to ∼ 6.5-fold. To calculate the contributions of dust to atmospheric heavy metals, regional air quality models usually use the dust chemical profiles from the U.S. Environmental Protection Agency's (EPA) SPECIATE database, which does not capture the correct size-dependent selectivity of heavy metals in dust aerosols. Our air quality modeling for China demonstrates that the calculated contribution of fine-dust aerosols to atmospheric heavy metals, as well as their cancer risks, could have significant errors without using proper dust profiles.