Physicochemical characteristics of atmospheric aerosol during winter in the São Paulo Metropolitan area in Brazil

In order to characterize atmospheric aerosol in the São Paulo Metropolitan Area, aerosols were sampled during the winter months of August 1999 and August 2000. A micro-orifice uniform deposit impactor (MOUDI) was used. Samples were submitted to gravimetry, as well as to proton-induced X-ray emission (PIXE), carbon (black and organic) and ion-chromatography analysis. These analyses supplied information about mass concentrations and physicochemical properties of the particles. Due to the higher humidity, which can increase soluble particles diameters, and reduced atmospheric stagnation seen in 2000, average PM₁₀ concentrations were higher (105 μg m⁻³) in the winter of 1999 than in the winter of 2000 (60 μg m⁻³). The PIXE analysis revealed metals and metal compounds, soil-derived elements, Si-rich particles, sulfates, carbonates, chlorides and other anthropogenic air-borne particles, supposing molecules in their usual composition. Mass balance for PM_2.5 revealed significant participation of organic and black carbon, probably resulting from diesel burning by the heavy-duty fleet.     

Arctic haze and clouds observed by lidar during four winter seasons of 1993–1997, at Eureka,Canada

A Mie-scattering-polarized Haze Lidar was installed at Eureka, Canada (80°N, 86°W), in February 1993 and has been used to observe the arctic haze during winter seasons from 1993–94 to 1996–97. Although it is difficult to distinguish between the arctic haze and other scattering objects (mainly clouds) under the specific conditions, two methods were used to classify those objects into two groups. First the vertical profiles of the arctic haze and clouds were compared with meteorological data observed by a radiosonde, and the relations between the scattering and depolarization ratios and the meteorological data were investigated. Then, since the arctic haze had very stable layers, the time dependency of the correlation coefficient between the different vertical profiles for the arctic haze and clouds was investigated. After the scattering objects were classified into two groups (the arctic haze and the clouds), the scattering ratio, the depolarization ratio, and the occurrence probabilities of them were investigated statistically. The statistical results, from the observations over the last four winter seasons, indicate that the average values of the scattering and depolarization ratios of the arctic haze were respectively 1.27 and 1.34%. The average humidity over ice of the layer containing the arctic haze was 42±19% (cloud: 92±13%). The arctic haze was observed at altitudes less than 3 km frequently and at altitudes of 3–5 km occasionally.     

Measurements of aerosol particles in the Škocjan Caves,Slovenia

For the first time, continuous aerosol measurements were performed in the ?kocjan Caves, one of the most important cave systems in the world, and listed by UNESCO as a natural and cultural world heritage site since 1986. Measurements of PM₁₀ were performed during three different periods: (1) in December 2011, the average background concentration was found to be about 4 μg m^?3; (2) in June 2012, a higher concentration was measured (8 μg m^?3); and (3) from 8 to 20 August 2012, the highest concentration of 15.3 μg m^?3 was measured. Based on the PM₁₀ measurement results, and as compared to similar measurements outside the cave, it can be hypothesized that the increase in the cave's aerosol concentration during the summer was connected to both the higher number of visitors and the polluted atmospheric air entering the cave upon entering of the cave system. Additional measurement of nanoparticles with scanning mobility particle sizer spectrometer (size between 14.1 and 710.5 nm) confirmed these findings; during the summer period, a severe raise in the total aerosol concentration of 30–50 times was found when groups of visitors entered the cave. Our results on nanoparticles demonstrated that we were able to detect very small changes and variations in aerosol concentration inside the cave. To our knowledge, these are the first results on nanoaerosol measurements in a cave, and we believe that such measurements may lead to the implementation of better protection of delicate cave systems.     

Aerosol characters from the desert region of Northwest China and the Yellow Sea in spring and summer: observations at Minqin,Qingdao, and Qianliyan in 1995–1996

Aerosol samples were collected from Northwest China desert region (Minqin), coastal suburb (Qingdao) and interior of the Yellow Sea (Qianliyan) in spring and summer of 1995 and 1996. Samples were analysed for major components, carbon and sulphur. The results show that concentrations of aerosols change considerably in time and space. The crustal materials carried by cold front system increase notably the aerosol concentration (mass/unit vol.) over the Yellow Sea but reduce the percentage contribution of pollutants and sea-salt. The sea-salt and regional aerosols become dominant fractions in coastal atmosphere in summer when the dust storms are expired in source region and the Southeast monsoon starts in the Pacific Ocean.     

Can the study of nitrogen isotopic composition in size-segregated aerosol nitrate and ammonium be used to investigate atmospheric processing mechanisms?

Atmospheric fixed-nitrogen deposition can contribute to eutrophication in coastal and estuarine waters. Stable nitrogen isotope data can provide important information regarding the sources and processing of atmospheric fixed-nitrogen species and is thus important in controlling eutrophication. Size-segregated aerosol samples were collected from two coastal sites: Weybourne, England and Mace Head, Ireland and also aboard the RRS Challenger in the Eastern Atlantic Ocean. Aerosol concentrations of ammonium and nitrate were determined prior to δ¹⁵N isotopic analysis. The isotopic enrichment factor, ε, was calculated for both the species by subtracting the respective δ¹⁵N values of the coarse-mode fraction (>1 μm diameter) from those of the fine-mode fraction (<1 μm diameter). Variations in this parameter were observed as weak functions of the percentage of each species in the coarse mode and of meteorological condition. As a result, the presence of two different size-shift processes (dissociation/gas scavenging and dissolution/coagulation) is proposed, consistent with similar arguments based upon major-ion data obtained from the same suite of samples. Dissolution/coagulation processes appear to exhibit negative isotopic enrichment factors whereas dissociation/gas scavenging processes appear to exhibit positive enrichment factors, suggesting that they may be reversible and thermodynamically driven. In offshore-flowing air masses just entering the marine environment, transferral of nitrate to the coarse mode by initial dissociation of NH₄NO₃ followed by scavenging of the HNO₃ produced appears to be significantly more important than in samples of onshore, marine dominated air. In contrast, ammonium appears to be transferred to the coarse mode during offshore flow largely via the dissolution and coagulation of aerosol ammonium, nitrate and sulphate-containing species. During onshore flow, the uptake of gaseous NH₃, arising from the continued dissociation of NH₄NO₃, seems to become increasingly important.     

The distribution and transport of sulfate “species” in the New York metropolitan area during the 1977 Summer Aerosol Study

The atmospheric distribution of sulfate was analyzed at four sites operated by various cooperating laboratories for the period of 18 July–29 August 1977 in the New York metropolitan subregion. The sulfate concentrations measured in NYC were categorized according to wind trajectory and values ≥ 15 μg m⁻³ were normally associated with a strong westerly component. SO^{2 −}₄ values ≤ 5 μg m⁻³ were associated with other wind trajectories, that had not passed over the Ohio Valley. Comparison of the 1977 study with the New York Summer Aerosol Study (1976) indicated that on the average the SO^{2 −}₄ concentrations were slightly lower in 1977. The highest concentrations (> 20 μgm⁻³) occurred simultaneously with the return flow of ozone-laden high pressure systems.The results of a SO^{2 −}₄ episode which affected the region from 3–9 August 1977 were analyzed using trajectory analyses, satellite imagery and measurements of the chemical species H⁺, NH⁺₄, and SO^{2 −}₄. Transport of SO^{2 −}₄ was observed and the presence of a strong acid distribution in the rural areas was denonstrated. The aerosol in New York City appeared to be more nearly neutral, probably a result of reaction with ammonia.     

Chemical composition of snowfall in the high Arctic: 1990–1994

From 1990 to 1994 at Alert, Nunavut, Canada, weekly snow samples were collected under low wind conditions to avoid contamination by blowing snow. They were analysed for major ions, Br⁻, and the organic ions methylsulphonate, formate, acetate and propionate. In the Arctic, where annual precipitation is low and blowing snow is common, these observations are unique. On an equivalent weight basis, acids and sea salt in snowfall are mixed approximately equally from December to January but from March to May acids dominate. The acidity of snowfall increases progressively throughout the winter to a May peak of ∼16 μeq l⁻¹. SO₄²⁻, Br⁻, and the organic acids acetate, and propionate peak in snowfall after polar sunrise indicate the influence of enhanced photochemical reactions. The greater enrichment of halides relative to sea salt Na⁺ in snow compared to aerosols indicates that gaseous uptake by snowflakes is important in the removal of these substances from the atmosphere and their deposition on to the Earth's surface. There is a marked difference between the seasonal variation of enrichment of Cl⁻ and Br⁻ in snow. The latter show a marked increase after polar sunrise while the former does not. These results provide valuable baseline information on the ionic content of fresh snowfall to be used in understanding the results of snowpack chemistry and post-depositional process studies conducted in the high Arctic.     

NMOC,ozone, and organic aerosol in the southeastern United States, 1999–2007: 1. Spatial and temporal variations of NMOC concentrations and composition in Atlanta,Georgia

Volatile organic compounds (VOCs) are emitted from anthropogenic and natural (biogenic) sources into the atmosphere. Characterizing their ambient mixing ratios or concentrations is a challenge because VOCs comprise hundreds of species, and accurate measurements are difficult. Long-term hourly and daily-resolution data have been collected in the metropolitan area of Atlanta, Georgia, a major city dominated by motor vehicle emissions. A series of observations of daily, speciated C₂–C₁₀ non-methane organic compounds (NMOC) and oxygenated hydrocarbons (OVOC) in mid-town Atlanta (Jefferson Street, JST) are compared with data from three urban-suburban sites and a nearby non-urban site. Annual-average mixing ratios of NMOC and OVOC at JST declined from 1999 through 2007. Downward trends in NMOC, CO, and NO_y corroborate expected emission changes as reflected in emission inventories for Atlanta’s Fulton County. Comparison of the JST NMOC composition with data from roadside and tunnel sampling reveals similarities to motor vehicle dominated samples. The JST annual average VOC-OH reactivities from 1999 to 2007 were relatively constant compared with the decline in annual-average NMOC mixing ratios. Mean reactivity at JST, in terms of concentration*k_OH, was approximately 40% alkenes, 22% aromatics, 16% isoprene and 6% other biogenics, 13% C₇–C₁₀ alkanes and 3% C₂-C₆ alkanes, indicating that biogenic NMOCs are important but not dominant contributors to the urban reactive NMOC mix. In contrast, isoprene constituted ～50% of the VOC-OH reactivities at two non-urban sites. Ratios of 24-hour average CO/benzene, CO/isopentane, and CO/acetylene concentrations indicate that such species are relatively conserved, consistent with their low reactivity. Ratios of more-reactive to less-reactive species show diurnal variability largely consistent with expected emission patterns, transport and mixing of air, and chemical processing.     

Regional sources of pollution aerosol at Barrow,Alaska during winter 1979–1980 as deduced from elemental tracers

A seven-element tracer system for regional pollution aerosol has been applied to 100 daily samples of aerosol from Barrow, Alaska during winter 1979–1980, using regional signatures from eastern N America, Europe, and the Soviet Union. The results suggest that approximately 70% of most tracer elements came from the U.S.S.R., 25 % came from Europe, and the rest came from N America. The large contribution from the U.S.S.R. is consistent with large-scale atmospheric flow patterns for that winter, in which air came strongly and persistently from central Asia northward to the Arctic. The small contribution from eastern N America agrees with previous circumstantial evidence. Apportionment of sulfate between Europe and the Soviet Union suggested that each contributed roughly 50%, however. The greater contribution of Europe to sulfate than to tracer elements is consistent with other data, including emission inventories for SO₂ and elements in the Soviet Union and Europe.     

Assessment of the temporal and spatial distribution of atmospheric PCNs and their air–soil exchange using passive air samplers in Shanghai,East China

A total of 47 passive air samples and 25 soil samples were collected to study the temporal trend, distribution, and air–soil exchange of polychlorinated naphthalenes (PCNs) in Shanghai, China. Atmospheric PCNs ranged from 3.44 to 44.1 pg/m³ (average of 21.9 pg/m³) in summer and 13.6 to 153 pg/m³ (average of 40.0 pg/m³) in winter. In the soil samples, PCN concentrations were 54.7–1382 pg/g dry weight (average of 319 pg/g). Tri-CNs and tetra-CNs were two dominant homolog groups in air samples, while di-CNs were also found at comparable proportions to tri-CNs and tetra-CNs in soil samples. Most air and soil samples from the industrial and urban areas showed higher PCN concentrations than those from suburban areas. However, some soil samples in urban centers presented higher PCN concentrations than industrial areas. Analysis of PCN sources indicated that both industrial thermal process and historical usage of commercial PCN mixtures contributed to the PCN burden in most areas. The fugacity fraction results indicated a strong tendency of volatilization for lighter PCNs (tri- to hexa-CNs) in both seasons, and air–soil deposition for octa-CNs. Moreover, air–soil exchange fluxes indicate that soil was an important source of atmospheric PCNs in some areas. The results of this study provide information for use in the evaluation of the potential impact and human health risk of PCNs around the study areas.

     

Atmospheric concentrations,gaseous–particulate distribution,and carcinogenic potential of polycyclic aromatic hydrocarbons in Assiut,Egypt

The concentrations of 15 priority PAHs were determined in the atmospheric gaseous and particulate phases from nine sites across Assiut City, Egypt. While naphthalene, acenaphthene, and fluorene were the most abundant in the gaseous phase with average concentrations of 377, 184, and 181 ng/m³, benzo[b]fluoranthene, chrysene, and benzo[g,h,i]perylene showed the highest levels in the particulate phase with average concentrations of 76, 6, and 52 ng/m³. The average total atmospheric concentration of target PAHs (1,590 ng/m³) indicates that Assiut is one of the highest PAH-contaminated areas in the world. Statistical analysis revealed a significant difference between the levels of PAHs in the atmosphere of urban and suburban sites (P?=?0.029 and 0.043 for gaseous and particulate phases, respectively). Investigation of diagnostic PAH concentration ratios revealed vehicular combustion and traffic exhaust emissions as the major sources of PAHs with a higher contribution of gasoline rather than diesel vehicles in the sampled areas. Benzo[a]pyrene has the highest contribution (average?=?32, 4 % for gaseous and particulate phases) to the total carcinogenic activity (TCA) of atmospheric PAHs. While particulate phase PAHs have higher contribution to the TCA, gaseous phase PAHs present at higher concentrations in the atmosphere are more capable of undergoing atmospheric reactions to form more toxic derivatives.     

Abundance,characteristics, and spatial–temporal distribution of microplastics in sea salts along the Cox’s Bazar coastal area,Bangladesh

Environmental Science and Pollution Research - Microplastics (MPs), together with microfibers, have emerged as a contaminant of concern all around the globe. MPs have been detected in freshwater,...     

An evaluation of sulfate in European precipitation 1955–1982

More than 25 years of data on sulfate in precipitation from the European Air Chemistry Network (EACN) are analysed for seasonal and long-term trends and their spatial variability. The number of stations has varied between about 50 and 100, all of them located in the central and northern parts of western Europe. Despite considerable shortcomings of the data (indicated among other things by poor ionic balance during several years, particularly in the late 1950s and the early 1960s) the following conclusions are drawn.In Norway, Sweden, Denmark and Finland, the sulfate concentration increased by roughly 50 per cent between the late 1950s and the late 1960s. A further increase during the 1970s is indicated at the Danish stations but most stations in Sweden and Norway show a decline by on the average about 20 per cent since the early 1970s. Sulfate data from the U.K. and the European continent seem to exhibit less systematic variations.A comparison between the long-term changes in the Scandinavian data on sulfate in precipitation and the corresponding changes in anthropogenic SO₂ emission in Europe indicates a fair agreement with regard both to the increase in emission during the 1950s and 1960s and, except for the Danish stations, also the subsequent decrease in emission in several of the West European countries.In most parts of the network the annual cycle of concentration of sulfate exhibits a maximum in February through May and a minimum in July to October, whereas the wet deposition normally has its maximum in May to August and minimum in December to March. A comparison with the annual cycle of anthropogenic emission, which has a clear maximum in December to March, indicates that the fraction of sulfur exported out of the region is larger in winter than in summer.     

Characteristics and distribution of microplastics in shoreline sediments of the Yangtze River,main tributaries and lakes in China—From upper reaches to the estuary

Environmental Science and Pollution Research - Microplastics (MPs) pervade the environment and increasingly threaten both natural ecosystems and human health. In this study, we investigated MP...     

NMOC,ozone, and organic aerosol in the southeastern United States, 1999–2007: 2. Ozone trends and sensitivity to NMOC emissions in Atlanta,Georgia

Non-methane organic carbon (NMOC) measurements made in Atlanta, Georgia from 1999–2007 are used with nitrogen oxide (NO_x or NO_y) and ozone (O₃) data to investigate relationships between O₃ precursors and peak 8-hour O₃ concentrations in the city. Data from a WNW-to-ENE transect of sites illustrate that the mean urban peak 8-hour O₃ excess constitutes about 20% of the peak 8-hour O₃ measured at the area-wide maximum O₃ site when air-mass movement is from the northwest quadrant; local influence is potentially greater on days with more stagnation or recirculation. The peak 8-hour O₃ concentrations in Atlanta increase as (1) surface temperature (T), ambient NMOC and NO_y concentrations, and previous-day peak O₃ concentrations increase, and as (2) relative humidity, surface wind speeds, and ratios of NMOC-to-NO_y decrease. An observation-based statistical model is introduced to relate area-wide peak 8-hour O₃ concentrations to ambient NMOC and NO_y concentrations, while accounting for the non-linear dependences of peak 8-hour O₃ concentrations on meteorological factors. On the majority of days when the area-wide peak 8-hour O₃ exceeds 75 ppbv, meteorologically-adjusted peak 8-hour O₃ concentrations increase as ambient NMOC concentrations increase (NMOC sensitive) and ambient NO_y concentrations decrease. This result contrasts with regional conditions in which O₃ formation appears to be NO_x-sensitive in character. The results offer observationally-based information of relevance to O₃ management strategies in the Atlanta area, potentially contributing to “weight-of-evidence” assessments.     

Characterization of size segregated particles collected over Alaska and the CAnadian high Arctic,AGASP-II flights 204–206

Ten aircraft-collected cascade impactor samples from the North American Arctic were analyzed using analytical electron microscopy. Morphological, mineralogical and elemental information were obtained from individual particles, as well as compositional data and size distribution estimates of the bulk aerosol. Categorization of carbonaceous material into organic-type and combustion-type carbon particles was performed in this study. This was accomplished through the use of a new ultra-thin window X-ray spectrometer, which can directly detect carbon X-rays emitted from particles, and through interpretation of morphological and electron diffraction data. Verification of graphite as a specific carbon mineral phase present in Arctic soot particles was performed in this manner.Several classes of particles were present in most of the aerosol samples and size fractions. These included liquid H₂SO₄ droplets, which were always present in the highest numbers, and crustal-type and composite SO₄⁻² particles. A small fraction (0–30%) of a random sampling of SO²⁻₄particles from all impactor stages were found to contain detectable nitrogen, suggesting that partial neutralization by NH₃ may have occurred in this minority of the SO²⁻₄ droplets. Particles rich in non-combustion carbon and thought to be composed of organic material were also observed in most samples. Haze samples collected off the coast of Alert, NWT, show moderate loadings of H₂SO₄ droplets. Judging from these loadings and those from higher-altitude samples, ambient aerosol particle concentrations must have been considerably higher in the haze. The extent to which local activity at Alert has influenced these haze samples is not known, although a major contribution is not expected. Stratospheric samples did not contain several classes of particles thought to have major anthropogenic source inputs to the Arctic, such as black carbon and coal-fired combustion spheres. The lightest particle loadings in any samples were collected in the upper troposphere near the tropopause, where condensation nuclei counts during sampling fell to as low as 10 cm⁻³.     

Sources and concentrations of gaseous and particulate reduced nitrogen in the city of Münster (Germany)

Atmospheric ammonia mixing ratios and the main inorganic ions NH₄⁺, NO₃⁻ and SO₄²⁻ of size-resolved particles in the range from 0.05 to 10 μm were measured at an urban site in Münster, Germany. High mixing ratios of ammonia with a median of 5.2 ppb and a maximum of 50 ppb were detected. The mass fraction of submicron particles was much higher during the day than at night. At night, a greater particle mass and an increased presence of particulate nitrate was measured. Recurring patterns of particle distribution were distinguished and their characteristics analysed. In half of the measurements, the accumulation mode was clearly dominating, which is an indication of aged aerosol. In some measurements, higher concentrations of fine particles were found indicating particle formation. In these cases, a smaller particle mass and about four times greater ratios of ammonia versus ammonium concentrations were observed. These data show that ammonia contributes considerably to the formation of secondary particulate material.