The Spatial Distribution of Characterised Fly-Ash Particles and Trace Metals in Lake Sediments and Catchment Mosses: Estonia

The concentrations of fly-ash particles were studied in the surface sediments of 42 lakes in Estonia. Concentrations of both spheroidal carbonaceous particles (SCPs) and inorganic ash spheres (IASs) were determined and the particles chemically characterised to different fuel types. This was accompanied by trace metal analyses from lake surface sediments and catchment mosses in order to determine the distribution of atmospheric pollutants. The obtained spatial distribution data for fly-ash particles varied to a great extent, partly due to differences in sedimentation rates but mainly due to higher deposition in industrial areas. The distribution patterns of the different particle types in lake sediments, as well as the trace metals in mosses, show that the deposition of airborne particulates is of local origin around pollution sources and that the share of long-range transported atmospheric impurities is high along the main cyclonic routes in Estonia.     

Ozone Sensitivity Differences in Five Tomato Cultivars: Visible Injury and Effects on Biomass and Fruits

A complete record derived from the core from the Daihai Lake in a remote area provides new insights into the changing atmospheric heavy metal deposition associated with historical industrial activities, the Asian monsoon, long-range transport, and the chemical composition of matter derived from weathering of catchment. The fluctuation of lithogenic element concentration in the lake sediments can readily be explained by a particle sorting effect induced by the Asian monsoon. The variation of atmospheric deposition of Cu and Pb shows a similar profile in the lower part of the core sediments, and coincides with environmental change, with high atmospheric deposition coupled with wet, temperate period; while low deposition with dry, cold period, indicating a transport variation of heavy metal pollutants entrained by the Asian summer monsoon. From the beginning of nineteenth century, the atmospheric deposition of Cu and Pb decreased and then slowly increased. This may be associated with the destroyed industry induced by long-term wars in China and the less heavy metal pollutants relative to the weak Asian summer monsoon in this period. Comparison between atmospheric-derived metal and sediment trap metal using Ga as the reference element shows that atmospheric Cu and Pb budgets do not exceed the fluvially-induced Cu and Pb budgets in the indirectly disturbed area. On average, there have been approximately 5.4 mg m^?2 yr^?1 of Cu and 5.1 mg m^?2 yr^?1 of Pb atmospherically deposited in the region.     

Modeling atmospheric effects — An assessment of the problems

Our ability to simulate atmospheric processes that affect the life cycle of pollution is reviewed. The transport process is considered on three scales: (a) the near-source or single-plume dispersion problem, (b) the multiple-source dispersion problem, and (c) the long-range transport. Modeling the first of these is shown to be well within the capability of generally available techniques, although determining the input parameters is often difficult. The second scale has been well studied within the context of urban diffusion and is a very productive area of current research. Finally, long range transport is treated mainly as a meteorological problem. The state of the art in modeling the various meteorological processes is reviewed. Removal of pollutants is discussed in the form of both dry deposition and precipitation scavenging. It is suggested that dry removal is especially effective in forested areas, and that the forests may enhance accumulation of pollutants. An approximate transport model is developed which is used to calculate the ambient concentration of SO₂ throughout the United States. Associated calculations include dry deposition and the ratio of dry to wet removal for each State of the contiguous United States.     

Contributions of cloud processes to precipitation chemistry in mixed phase clouds

The role clouds play as processors of atmospheric aerosols and trace gases was studied along the slope of Mt. Rigi in central Switzerland. Upon cloud formation many aerosols and trace gases are efficiently scavenged by cloud drops. The cloud drops can enhance removal of pollutants from the atmosphere by transferring them to snow or rain which falls rapidly to the ground. This often occurs through a process known as riming, where falling ice crystals capture cloud drops. When ice crystals are grown primarily via water vapor deposition, without significant capture of cloud drops, however, the cloud drops isolate atmospheric pollutants from the precipitation process, thereby inhibiting their deposition. Increased riming results in increased precipitation ion concentrations. The extent of ice crystal riming at times exhibits spatial inhomogeneities with greater riming apparent near the mountain summit. Variations in cloud chemistry with drop size indicate that bulk cloudwater composition is not an accurate predictor for the composition of cloud drops captured by the ice crystals.     

Developing optimal abatement strategies for the effects of sulphur and nitrogen deposition at European scale

Integrated Assessment Models were successfully used to provide input to the negotiations for the Oslo Protocol on Further Reductions of Sulphur Emissions, finalized within the United Nations Economic Commission for Europe Convention on Long-range Transboundary Air Pollution in Oslo in June 1994. The techniques developed within this framework will be extended now to the simultaneous analysis of sulphur and nitrogen deposition. In addition to acidification, atmospheric deposition of nitrogen contributes to eutrophication of certain ecosystems, through a nutrient effect, and originates from the long-range transport of emissions of both oxidised and reduced nitrogen (NO_x and NH₃). Modelling reductions in nitrogen deposition thus introduces a need to establish multi-pollutant multi-effect modelling techniques. This paper investigates the development of a model set up to examine reductions of these pollutants in an economically and environmentally efficient manner. The control of nitrogen deposition encompasses action across several economic sectors, particularly the power, transport and agricultural sectors. Combining sulphur and nitrogen deposition limits on a European scale will require a flexible modelling approach and the issues governing possible approaches are presented.     

Concentration and deposition of acidifying air pollutants over Sweden: Estimates for 1991 based on the match model and observations

The MATCH (Mesoscale Atmospheric Transport and CHemistry) model has been developed as a tool for air pollution assessment studies on different geographical scales. MATCH is an Eulerian atmospheric dispersion model, including physical and chemical processes governing sources, atmospheric transport and sinks of oxidized sulfur and oxidized and reduced nitrogen. Using a combination of air and precipitation chemistry measurements and the MATCH model, the national and long-range transport contributions to air pollution and deposition can be quantified in the model region. The calculations for the year 1991 show that the Swedish import was about 4.5 times larger than the export for sulfur and about six times larger for reduced nitrogen, while the Swedish import of oxidized nitrogen only exceeded the export by 10%. Using the MATCH system we estimate the long-range transport in an independent way compared to EMEP. Comparison between the EMEP and MATCH calculations for 1991 show that the total deposition of oxidized nitrogen over Sweden is similar, while the EMEP-values for total deposition of oxidized sulfur and reduced nitrogen are 25% respectively 40% smaller than what is obtained from MATCH.     

东亚季风与城市活动影响下南京市大气沉降多元特征研究

Atmospheric deposition, a major pathway of metals entering into soils, plays an important role in soil environment, especially in urban regions where a large amount of pollutants are emitted into atmosphere through various sources. In order to understand the characteristics of atmospheric deposition in urban area and its relation with natural and anthropogenic sources, a three-year study of atmospheric deposition at three typical sites, industrial zone (IN), urban residential area (RZ) and suburban forested scenic area (FA), was carried out in Nanjing, a metropolitan city in eastern China from 2005 to 2007. The bulk deposition rate and element composition of atmospheric deposition varied spatio-temporally in the urban zones of Nanjing. The concentrations of Cu, Zn, Pb and Ca in the atmospheric deposits were strongly enriched in the whole Nanjing region; however, anthropogenic pollutants in atmospheric deposits were diluted by the input of external mineral dust transported from northwestern China. Source apportionment through principal component analysis (PCA) showed that the background atmospheric deposition at the FA site was the combination of external aerosol and local emission sources. The input of long-range transported Asian dust had an important influence on the urban background deposition, especially in spring when the continental dust from the northwestern China prevailed. Marine aerosol source was observed in summer and autumn, the seasons dominated by summer monsoon in Nanjing. In contrast, the contribution of local anthropogenic emission source was constant regardless of seasons. At the RZ and IN sites, the atmospheric deposition was more significantly affected by the nearby human activities than at the FA site. In addition, different urban activities and both the winter and summer Asian monsoons had substantial impacts on the characteristics of dust deposition in urban Nanjing.     

Analysis of long-range transported acid aerosol in rime found at kyushu mountainous regions,Japan

Rime-ice and snow samples were collected at mountain sites in Kyushu, Japan during the winter of 1994, and both soluble and insoluble substances in the melted rime-ice were analyzed by ion chromatography, inductively coupled plasma-mass spectrometry (ICP/MS) and analytical electron microscopy, in order to find the evidences of long-range transport of air pollutants from the cities of the East Asian region. The relationships between Al, which is most often used as an index of soil components, and other elements were examined. The positive correlation was found between Al and three elements (Ti, Mn, Ba). Therefore, behaviors of these elements in rime-ice may be similar to that of soil particles. Furthermore, it was possible to classify the elements into three groups with the relation between a lead isotope ratio and concentration ratio of lead and zinc (Pb/Zn). In addition, numbers of particles were found in the rime-ice. The particles around 1 m in diameter were considered to be the combustion products of coal, whose Pb/Zn were similar to that of previous survey report in Korea. The existent forms of chemical species in rime-ice will become an important factor, when we consider the origin of air pollutants transported over long distances in the East Asian region.     

Transport of Atmospheric Pollutants from East Asia

Air-borne measurements of air pollutants transported from northeast Asia to Japan and the Pacific Ocean were carried out three times from 1996 to 1999 over the seas between Japan and Asian Continent. Those campaigns were named PEACAMPOT II under auspices of the IGAC/APARE program. A transport pattern of a highly polluted air mass from central China was found. Such air mass was driven by the quick movement of low pressure traveling from Taiwan area to the northeast of Japan. This finding supported well the results of modeling studies for long-range transport of atmospheric pollutants from East Asia.     

Characteristic Fly-ash Particles from Oil-shale Combustion Found in Lake Sediments

Fly-ash particles accumulate in sediments and can be used to assess spatial distribution and temporal trends of atmospheric deposition of pollutants derived from high temperature combustion of fossil fuels. Previous work has concerned fly-ash derived from oil and coal. Oil-shale is the main fossil fuel used in Estonia and a major source of atmospheric pollution in the Baltic states. To assess if oil-shale power plants produce specific fly-ash particles, we used scanning electron microscopy (SEM) and energy dispersive X-ray analysis (EDX) to compare fly-ash particles from oil-shale combustion with particles from oil and coal combustion. Two types were analysed, large black (10–30 μm) and small glassy (<5 μm) spheroidal particles. Although particle morphology to some extent is indicative of the fuel burnt, morphological characters are not sufficient to differentiate between particles of different origin. However, our results indicate that with EDX analysis the fly-ash from oil-shale can be distinguished from oil and coal derived particles in environmental samples. Concentrations of large black and small glassy spheroidal fly-ash particles in a sediment core from an Estonian lake showed similar trends to oil-shale combustion statistics from Estonian power plants.     

Deposition around a coal-fired power station during a wintertime precipitation event

The contribution to local wet deposition of emissions from a coal-fired power station at Inkoo on the south coast of Finland has been investigated during a wintertime precipitation event. Making use of intensive radiosonde and weather radar observations of meteorological factors, concentrations of sulphur in deposition due to plume washout were predicted by a short-range deposition model. The model used the scavenging coefficient to parametrize the wet removal of pollutants, and it took into account the wind drift of falling precipitation particles within the plume. The model predictions were then compared with the chemical analysis results from snowfall samples collected within 10 km of the power station during the experiment.The experiment was performed ahead of a deeply-occluded front during a period with strong advection of long-range transported pollutants. No reliable sign of the influence of the power station on the sulphate deposition could be identified. On the other hand, the deviations of acidity from the mean pH-value of 4.1 were concentrated in one sector near the expected area of deposited plume pollutants. If local emissions were responsible for these deviations, the explanation may lie in a slightly incorrectly estimated plume direction or the effects of alkaline fly ash. Nevertheless, definite conclusions cannot be drawn, because only a few collectors happened to be sited in the modelled sector of plume washout and none in its maximum area.     

Atmospheric models and acidification: Summary and conclusions of the Warsaw II meeting on atmospheric computations to assess acidification in Europe

Three topics are discussed in this report: sensitivity/uncertainty analysis of long range transport models, the interface between atmospheric models of different scales, and linkage between atmospheric and ecological models. In separate analyses of long range transport models, it was found that uncertainty of annual S deposition was mostly affected by uncertainty of wind velocity, mixing height and wet deposition parameterization. Uncertain parameters collectively caused S deposition errors of around 10–25% (coefficient of variation) in the models examined. The effect of interannual meteorological variability on computed annual S deposition was relatively small. Different methods were presented for combining models of regional and interregional scale. It was found to be more important to include interregional information in regional-scale models for annual computations compared to episodic computations. A variety of linkage problems were noted between atmospheric and ecological models. The vertical distribution of pollutants and ‘forest fittering’ of pollutant deposition were found to be important in ecological impact calculations but lacking in the output of most interregional atmospheric models.     

The Impact of Atmospheric Deposition of Non-Acidifying Substances on the Quality of European Forest Soils and the North Sea

In the pilot study ESQUAD the impact of atmospheric deposition of three heavy metals (cadmium, copper and lead) and two persistent organic pollutants (benzo(a)-pyrene and lindane) on the quality of European soils and seawater has been calculated. Calculations have been made of atmospheric transport and deposition using a detailed emissions database for Europe. This enabled deposition maps to be produced to a resolution of approximately 50 km. The distribution of pollutant concentrations in forest soils was calculated for each grid cell using a database of soil property parameters in Europe. For the North Sea, a model was used to map long-term concentrations in water and sediment, which are due to atmospheric deposition and other, non-atmospheric sources. The model calculations allowed detailed comparisons of deposition fluxes and concentrations of the substances studied with critical loads and environmental quality threshold values, including critical loads. Although significant uncertainties were identified, the study gives insight in how threshold exceedance rates in Europe relate to pollutant type, threshold type, environmental compartment and chemophysical phase (adsorbed, dissolved). For all pollutants and for all compartments exceedances were calculated for at least some of the quality thresholds that were chosen.     

Environmental biogeochemistry of mercury in Antarctic ecosystems

Polar regions are recognized as important sinks for long-range transport and deposition of Hg derived from natural and anthropogenic sources at lower latitudes. In previous studies we found enhanced Hg accumulation in soils, mosses and lichens from ice-free areas of Victoria Land facing the Terra Nova Bay coastal polynya. This study extends research to the distribution of organic C, total N, S, Hg, Al and Fe in surface soils, cyanobacterial mats and short sediment cores from four lacustrine ecosystems, each with different environmental characteristics and varying distances from the polynya. Results show that planktonic and benthic mats from lakes, along with mosses in the watershed, are the main sinks for Hg in summer meltwater. The C-normalized Hg concentrations in short sediment cores were higher in samples from lakes more exposed to marine aerosols from the coastal polynya. Reactive halogens in the aerosol promote the oxidation and deposition of atmospheric Hg in coastal ecosystems. The analysis of sediment cores did not reveal increasing Hg concentrations in recent sediments, except in the Lake 14 at Edmonson Point. The latter ice-free area is unaffected by the polynya and the increase in Hg concentrations in surface sediments could be due to local changes in lake water level and S biogeochemistry. Although change in sea ice coverage may enhance the role of Antarctic coastal ecosystems as sink in the global Hg cycle, our results seem to exclude possible risks for Antarctic terrestrial and freshwater organisms.     

Input of pesticides by atmospheric deposition

Sampling and analytical methods were developed to examine the input of various pesticides on noncultivated areas of the FAM (Research Network on Agroecosystems) Research Station Scheyern. Off-target drift from pesticide application on nearby cultivated land, as well as input due to long-range atmospheric transport, were measured. The wet deposition was determined by a cooled wet-only sampler. Bulk samplers and specially designed samplers with glass-fiber surface were used for total deposition measurements. Analysis of pesticides was carried out using liquid/liquid or solid-phase extraction and high performance liquid chromatography-UV (HPLC-UV) or gas chromatography-nitrogen/phosphorus-sensitive detector/MS (GC-NPD/MS) detection. Obtained results demonstrated that for several compounds, total deposition, i.e. the sum of wet and dry deposition, was marginally higher than wet deposition alone. In contrast, total deposition data of pesticides having been applied near the sampling site exceeded wet deposition values by orders of magnitude. In addition to direct drift, determined as droplets depositing near pesticide application areas, an indirect drift represented by particle-associated or gaseous transport was observed, both of which contributed considerably to total deposition. Therefore, to determine the input of pesticides to nontarget areas in the close vicinity of pesticide application, direct and indirect drift, and background deposition must be considered.     

Atmospheric deposition of trace elements in Norway: Temporal and spatial trends studied by moss analysis

The atmospheric deposition of sixteen trace elements, as inferred by their concentration in moss samples collected in 1985 from 500 sites in Norway, is compared with data from a similar survey in 1977. The deposition patterns of V, Zn, As, Se, Cd, Sb, and Pb are substantially influenced by long-range transport from other parts of Europe, but a general decline is evident from 1977 to 1985, most strongly for Pb. For Cr, Fe, Co, Ni, and Cu the deposition patterns are largely determined by contributions from point sources within Norway and on the Kola peninsula close to the Russian/ Norwegian border. The moss data for Br, I, and partly Se reflect airborne supply from the marine environment, whereas Al and Sc serve as indicators of contributions from soil dust. Contributions to the trace element concentrations in moss from sources other than atmospheric deposition are identified and discussed.     

Heavy metal concentrations in some non-vascular plants in an Amazonian rainforest

The presence of acid rain in the remote Amazon rainforest of southwestern Venezuela suggests the possibility of long-range transport of industrial pollutants to that region. Heavy metal concentrations were analyzed in samples of bryophytes and epiphyllous organisms growing on leaves and on bark in this forest. Concentrations of Cd, Pb, Ni, and Cr were higher in leaves with epiphylls than in leaves without epiphylls. All heavy metal concentrations in bryophytes from the Amazon basin site were lower than in bryophytes from temperature zones. The results indicate that long-range transport of air pollutants from industrial centers to the remote Amazon basin is occurring at only extremely low rates. Heavy metal concentrations in bryophytes and epiphylls at this site may still be considered close to present day background levels.     

Sources of heavy metal pollution in the rhine basin

The concept of industrial metabolism is introduced as an analytical framework for many diffuse sources of pollution for which ‘end of pipe’ control will not work and pollution prevention at the source is required. the concept is applied to pollution in the Rhine Basin which ends up in the Netherlands Delta and the North Sea, where the character of the pollutants changes over time. Cadmium, lead and zinc pollution from point sources, traffic, corrosion and atmospheric deposition are considered. Calculations cover the period from 1950 to 2010. in this study strongly urbanized paved and unpaved areas are distinguished based on their transport of pollutants to surface waters.     

Atmospheric Impacts due to Anthropogenic Activities in Remote Areas: The Case Study of Admiralty Bay/King George Island/Antarctic Peninsula

The aim of the present work is to characterize the local atmospheric emissions levels and compare them to the component derived from global pollution in a remote site at South Hemisphere (Admiralty Bay located at King George Island in Antarctic Peninsula). Airborne particles, snow and soil/sediments samples were analyzed. Local-produced atmospheric aerosol dispersion was estimated for metals originated by fossil fuel burning from the permanent scientific stations using a simplified Gaussian model. Validation of atmospheric dispersion was established by in situ measurements. Soluble and insoluble particles deposited in freshly snow and airborne particles were analyzed by PIXE (Particle Induced X-Ray Emission) for the determination of the elemental mass concentration and to obtain the Mass Median Aerodynamic Diameter (MMAD). The results showed significant correlation between the concentration of atmospheric aerosol and the freshly deposited particles in the snow, and permitted an estimate of the atmospheric snow deposition factor for K, Cu, Zn, Fe, Pb, and Ti. Results of long-term aerosol data compilation suggest that besides the local aerosol sources, the continental atmospheric transport of airborne particles is not significantly affected by the airborne particles produced by local human impacts at King George Island.     

Long-Range Transport of Sulfur from Northeast Asia to Chengshantu, Shandong Peninsula: Measurement and Simulation

Observations of air pollutants were conducted at Chengshantu in January 1996 to clarify the extent of trans-boundary pollution from the Asian continent. A nested air quality prediction modeling system (NAQPMS), which included parameters on emission, transport, diffusion, deposition and transformation of sulfur oxides, was performed to compile sulfur concentrations over the observation site. The model calculation reproduced the observed variations of sulfur oxides and sulfate well, although the model calculations could not reproduce the extensively low sulfate concentrations. Using nesting improves the ability of the modeling system to capture peak episodes seen in the observations. Calculation of the origins of deposited sulfur in each country with the NAQPMS shows that the long-range transport of sulfur is very serious. For Japan, 49% of sulfur deposition was from other countries during the campaign period.