Current and future emissions of selected heavy metals to the atmosphere from anthropogenic sources in Europe

Current atmospheric emissions of As, Cd, Cr, Ni, and Pb (reference year 2000) from major anthropogenic sources in Europe are presented in this paper. Combustion of fuels in stationary sources was the main emission source for As, Cd, Cr, and Ni (more than a half of the total anthropogenic emissions), while combustion of gasoline was the main source of for lead. There is a continuous reduction of heavy metal emissions in Europe during the last 40 years. Better knowledge of heavy metal sources, emissions, pathways, and fate in the environment, and progress in developing efficient emission control equipment has resulted in more efficient regulatory efforts to curb heavy metal emissions from anthropogenic sources very substantially. There is a potential for further reduction of these emissions until the year 2010 up to about 40% for As, Cd, Cr, and Ni and about 57% for Pb, as estimated within various emission scenarios presented in the paper.     

Mosses as biomonitors of atmospheric heavy metal deposition: Spatial patterns and temporal trends in Europe

In recent decades, mosses have been used successfully as biomonitors of atmospheric deposition of heavy metals. Since 1990, the European moss survey has been repeated at five-yearly intervals. Although spatial patterns were metal-specific, in 2005 the lowest concentrations of metals in mosses were generally found in Scandinavia, the Baltic States and northern parts of the UK; the highest concentrations were generally found in Belgium and south-eastern Europe. The recent decline in emission and subsequent deposition of heavy metals across Europe has resulted in a decrease in the heavy metal concentration in mosses for the majority of metals. Since 1990, the concentration in mosses has declined the most for arsenic, cadmium, iron, lead and vanadium (52-72%), followed by copper, nickel and zinc (20-30%), with no significant reduction being observed for mercury (12% since 1995) and chromium (2%). However, temporal trends were country-specific with sometimes increases being found.     

Temporal trends (1990-2000) in the concentration of cadmium, lead and mercury in mosses across Europe

The European heavy metals in mosses survey provides data on the concentration of 10 heavy metals in naturally growing mosses. The survey has been repeated at five-yearly intervals and in this paper we report on the temporal trends in the concentration of cadmium, lead and mercury between 1990 and 2000. Metal- and country-specific temporal trends were observed. In general, the concentration of lead and cadmium in mosses decreased between 1990 and 2000; the decline was higher for lead than cadmium. For mercury not enough data were available to establish temporal trends between 1990 and 1995, but between 1995 and 2000 the mercury concentration in mosses did not change across Europe. The observed temporal trends for the concentrations in mosses were similar to the trends reported for the modelled total deposition of cadmium, lead and mercury in Europe.     

Past and future trends in concentrations of sulphur and nitrogen compounds in the Arctic

Recent trends in nitrogen and sulphur compounds in air and precipitation from a range of Arctic monitoring stations are presented, with seasonal data from the late 70s to 2004 or 2005. Earlier findings of declining sulphur concentrations are confirmed for most stations, while the pattern is less clear for reduced and oxidized nitrogen. In fact there are positive trends for nitrogen compounds in air at several stations. Acidity is generally reduced at many stations while the precipitation amount is either increasing or stable. Variability of sulphate concentrations in air for the period 1991–2000 is reasonably well reproduced at most stations using an Eulerian, hemispherical model. Results for nitrogen compounds are weaker. Scenario studies show that even if large sulphur emission reductions take place in important source regions in South-East Asia in the coming decades, only small changes in Arctic deposition can be expected. This is because South-East Asian emissions have small influence north of the Arctic circle.     

Mercury pollution trends in subarctic lakes in the northern Swedish mountains

Despite many years of research about mercury pollution, data concerning high-latitude regions of Europe are limited, particularly studies of long-term temporal trends. It is not clear whether the mercury load at high latitudes follows the recent decreasing trends in European mercury emissions or whether the load is still high because of continuing global emissions. In this study we use sediments from 12 lakes, located above the Arctic Circle in the Swedish mountains, to assess the past and recent mercury pollution situation, especially for the last 200 y. The mercury load increased clearly in sediment deposited from the late 19th or early 20th century to a peak between 1960 and 1990. This peak represents an enrichment of 1.4 to 4.2 times over background concentrations. This enrichment is comparable with enrichments in sediments from lower latitudes as well as other Arctic regions. Since the 1990s mercury concentration has declined in 8 of the 12 lakes, i.e., similar to emission trends in Europe.     

Trend,seasonal and multivariate analysis study of total gaseous mercury data from the Canadian atmospheric mercury measurement network (CAMNet)

Long-term monitoring data of total gaseous mercury (TGM) concentrations from the Canadian Atmospheric Mercury Measurement Network (CAMNet) were analysed for temporal trends, seasonality and comparability within the network and compared to other network and model results. Data collected from 11 Canadian measurement sites between 1995 and 2005 were analysed. Sites within CAMNet were characterized by principle component analysis (PCA) into four main categories. For the first time since automated TGM measurements have been made within CAMNet, this paper reveals statistically significant decreasing TGM concentrations from rural locations in Canada during this time period. The largest declines were observed close to the urban areas of Toronto and Montreal, where levels fell by 17% at Point Petre, and 13% at St. Anicet, respectively. Many of the TGM changes are comparable with the overall trends observed in total mercury concentrations in precipitation, for similar time periods, at co-located or nearby National Atmospheric Deposition programme's Mercury Deposition Network (NADP-MDN) sites. The results show that these changes are mostly driven by local or regional changes in mercury emissions. Other sites within CAMNet reflect reported changes in hemispherical global background concentrations of airborne mercury, where slight decreases or no statistically significant trend in TGM concentrations exist over the same time period.     

Indications for changing deposition patterns in central Europe

The German Federal Environmental Agency (Umweltbundesamt) currently runs a network of 17 air pollution monitoring stations in rural areas within the Federal Republic of Germany. Since 1982, daily bulk precipitation samples have been collected and analysed at five of these stations. As no changes in sampling and chemical analysis techniques have been introduced in this time period, an interpretation with respect to trends is possible. An increase in pH is most obvious at Deuselbach in the western part of Germany. It is related to a decrease in sulphate ions. Reduced SO2 emissions in the western part of Europe have resulted in decreasing ambient air concentrations mainly in the western part of Germany, whereas changes in concentrations close to the eastern border of West Germany were not as pronounced. Part of the decrease, however, was a consequence of three mild winters in sequence at the end of the period, with little easterly air flow. Estimated dry deposition fluxes of sulphur at 3 rural stations in West Germany were lower in 1988/1989 compared to 1980-1987 by 44-69%. Wet deposition showed between 8% increase and 25% decrease. The resulting reduction in total sulphur deposition ranged from 17-54%. Deposition via interception of fog droplets was not measured.     

Trends in air concentration and deposition of mercury in the coastal environment of the North Sea Area

An evaluation of mercury observations from North Sea coastal stations during 1995–2002 has been performed. The mercury data originate from EMEP/OSPAR stations in Ireland, Netherlands, Germany, Norway and Sweden where mercury in precipitation and Total Gaseous Mercury (TGM) have been measured. A decreasing trend in mercury wet deposition is observed. The decrease is sufficiently large to be significant considering measurement precision and appears to occur at all the studied sites. The reduction in deposition is 10–30% when comparing the two periods 1995–1998 and 1999–2002. The trend is likely to be due to emission controls in Europe. In contrast, no decreasing trend in TGM could be observed during the same time periods. A plausible explanation is that the TGM concentration measured in the OSPAR area to a larger extent than before is dominated by the hemispherical background concentration of TGM.     

Characteristics of dioxins and metals emission from radwaste plasma arc melter system

This study investigated the emission characteristics of PCDD/Fs and the partitioning of three heavy metals (Cd, Hg and Pb) and two radioactive metal surrogates (Co and Cs) in a radwaste plasma arc melter system. Typical mixtures of low-level radioactive wastes were simulated as the trial burn surrogate wastes. The emission of PCDD/Fs and the partitioning of the metals were strongly influenced by the feed waste stream and melter operating temperature, respectively. The emissions of PCDD/Fs, cadmium and lead were greatly enhanced when the polyvinyl chloride was included in the feed waste stream. Most of the nonvolatile cobalt partitioned into the glass. A significant quantity of cesium, cadmium and lead was vaporized during the highest melter temperature test. A lower melter temperature resulted in more cesium, cadmium and lead species remaining in the glass. The results of this study suggest that wet scrubbing as well as a low-temperature two-step fine filtration, or both of them together could not effectively capture the gas-phase or fine particle phase PCDD/Fs and mercury species. In order to effectively treat low-level radioactive waste streams, the tested high-temperature melter should include an adsorption system, which could collect the gas-phase PCDD/Fs and mercury species.     

Natural and anthropogenic influences on heavy metals in airborne particles over the Korean Peninsula

Six monitoring stations were selected to characterize the variations in airborne concentrations of heavy metals in South Korea between 1999 and 2012. Three stations represented higher concentrations, and three represented lower concentrations. The heavy metals monitored at these stations include cadmium, chromium, copper, iron (Fe), lead, manganese (Mn), and nickel. During the study period, concentrations of heavy metals at many stations, including those around the Seoul metropolitan area, showed a decreasing trend. However, concentrations of Mn and Fe that are primarily of crustal origin increased at four of the six stations. Some stations were significantly affected by emissions from the local industrial complex (IC), and heavy metal concentrations at those stations were relatively high even in summer. Many heavy metal concentrations were higher in spring than in winter, but wintertime concentrations of Cr and Pb were higher at the stations representing lower concentrations due to the dominant influence of combustion emissions. At stations less affected by emissions from the IC, concentrations of Fe and Mn that are predominantly crustal in origin were higher in spring, when Asian dust (AD) events are most frequent. Although Mn concentrations were also high at stations within the steelmaking IC during AD periods, they were much higher during non-AD periods due to local emissions. Variations in heavy metal concentrations, which are heavily influenced by emissions from the IC, warrant individual analysis because their emission characteristics differ from those of typical cases.     

Estimation of heavy metal emission fluxes on the territory of the NIS

As the result of our research, the specific procedures to use emission factor methodology were developed and applied for trace metal emission evaluation into the atmosphere over the territory of the former Soviet Union. The existing data on heavy metal emissions were revised as background information from official sources and expert estimations. Source categories and different initial information as well as the concept of spatial emission distribution were defined and observed. The calculated atmospheric emissions of lead, cadmium and mercury were produced among the main source categories of 12 NIS countries for 1990, 1995 and 1997, using modified emission coefficients.Total cadmium emissions into the atmosphere from determined source categories were estimated as 388.4 tonnes in 1990 for the whole domain with reduction by up to 207.0 tonnes per year for 1997. Mercury emissions were estimated as equal to 303.2 tonnes in 1990 and 159.8 tonnes in 1997. Lead emission amounted to 24903.0 tonnes in 1990, and 9652.5 tonnes in 1997.The results of the evaluation demonstrated the general trends of atmospheric heavy metal emissions with a greater decrease during the first half of the 1990s followed later by the rather stable level to be explained by recession in industrial activity and fuel consumption in NIS in that period. The significant spatial variations of atmospheric emissions over vast territories are described based on the results of their distribution according to 1×1 degree grid with remarkably higher values in the location of industrial cities.     

Long-term relationships between mercury wet deposition and meteorology

Daily-event precipitation samples collected in Underhill, VT from 1995 to 2006 were analyzed for total mercury and results suggest that there were no statistically significant changes in annual mercury wet deposition over time, despite significant emissions reductions in the Northeast United States. Meteorological analysis indicates that mercury deposition has not decreased as transport of emissions from major source regions in the Midwest and East Coast have consistently contributed to the largest observed mercury wet deposition amounts over the period. In contrast, annual volume-weighted mean (VWM) mercury concentration declined slightly over the 12-years, and a significant decrease was observed from CY 2001 to 2006. An increase in the total annual precipitation amount corresponded with the decline in annual VWM mercury concentration. Analysis suggests that the increase in precipitation observed was strongly related to changes in the amount and type of precipitation that fell seasonally, and this departure was attributed to a response in meteorological conditions to climate variability and the El Niño-Southern Oscillation (ENSO) cycle. Increased amounts of rainfall and mixed precipitation (mixture of rainfall and snowfall), particularly in the spring and fall seasons, enhanced annual precipitation amounts and resulted in declining VWM mercury concentrations during these periods. Thus, declines in concentration at the more remote Underhill site appear to be more directly linked to local scale meteorological and climatological variability than to a reduction in emissions of mercury to the atmosphere.     

Nonlinearities in source receptor relationships for sulfur and nitrogen compounds

The relationship between emissions and deposition of air pollutants, both spatially and in time forms an important focus for science and for policy makers. In practice, this relationship may become nonlinear if the underlying processes change with time, or in space. Nonlinearities may also appear due to errors in emission or deposition data, and careful scrutiny of both data sources and their relationship provides a means of picking up such deficiencies. Nonlinearities in source receptor relationships for sulfur and nitrogen compounds in Europe have been identified in measurement data for the UK. In the case of sulfur, the dry deposition process has been shown to be strongly influenced by ambient concentrations of NH3, leading to substantial increases in deposition rate as SO2 concentrations decline and the ratio SO2/NH3 decreases. The field evidence extends to measurements over three different surfaces in three countries across Europe. A mechanistic understanding of the cause of this nonlinearity has been provided. Apparent nonlinearities also exist in the sulfur deposition field through the influence of shipping emissions. The effect is clear at west coast locations, where during a period in which land-based sulfur emissions declined by 50%, no significant decline in concentrations of SO(2-) in precipitation were observed. The sites affected are primarily the coastal regions of southwestern UK, where shipping sources contribute a substantial fraction of the deposited sulfur, but the effect is not detectable elsewhere. Full quantification of the spatially disaggregated emission and their changes in time will eliminate this apparent nonlinearity in the source-receptor data. For oxidized nitrogen emission and deposition in the UK, there is strong evidence of nonlinearity in the source-receptor relationship. The concentrations and deposition of NO(3-) in precipitation have declined little following a reduction in emissions of 45% during the period 1987 to 2001. The data imply a significant decrease in the average transport distance for oxidized nitrogen and most probably an increase in the average oxidation rate. However, the net effect of changes in aerosol chemistry due to changes in sulfur emissions and less competition for the main oxidants as a consequence of reductions in sulfur emission have not been separated. A quantitative explanation of the cause of this nonlinearity is lacking and the effects are therefore identified as an important uncertainty for the development of further protocols to control acidification, eutrophication and photochemical oxidants in Europe.     

Quantifying natural source mercury emissions from the Ivanhoe Mining District,north-central Nevada,USA

In order to assess the importance of mercury emissions from naturally enriched sources relative to anthropogenic point sources, data must be collected that characterizes mercury emissions from representative areas and quantifies the influence of various environmental parameters that control emissions. With this information, we will be able to scale up natural source emissions to regional areas. In this study in situ mercury emission measurements were used, along with data from laboratory studies and statistical analysis, to scale up mercury emissions for the naturally enriched Ivanhoe Mining District, Nevada. Results from stepwise multi-variate regression analysis indicated that lithology, soil mercury concentration, and distance from the nearest fault were the most important factors controlling mercury flux. Field and lab experiments demonstrated that light and precipitation enhanced mercury emissions from alluvium with background mercury concentrations. Diel mercury emissions followed a Gaussian distribution. The Gaussian distribution was used to calculate an average daily emission for each lithologic unit, which were then used to calculate an average flux for the entire area of 17.1 ng Hg m⁻² h⁻¹. An annual emission of ∼8.7×10⁴ g of mercury to the atmosphere was calculated for the 586 km² area. The bulk of the Hg released into the atmosphere from the district (∼89%) is from naturally enriched non-point sources and ∼11% is emitted from areas of anthropogenic disturbance where mercury was mined. Mercury emissions from this area exceed the natural emission factor applied to mercury rich belts of the world (1.5 ng m⁻² h⁻¹) by an order of magnitude.     

Meteorologically adjusted trends of daily maximum ozone concentrations in Taipei,Taiwan

The meteorological conditions exert large impacts on ozone concentrations, and may mask the long-term trends in ozone concentrations resulting from precursor emissions. Estimation of long-term trends of ozone concentrations due to the changes in precursor emissions is important for corresponding control strategy. Multiple linear regression (method I), multilayer perceptron (MLP) neural network (method II) and Komogorov-Zurbenko (KZ) filter method plus MLP methodology (method III), are used to estimate the meteorologically adjusted long-term trends of daily maximum ozone concentrations by removing the masking effects of meteorological conditions in this study. The daily maximum ozone concentrations and relative meteorological variables were extracted from six air-monitoring stations in Taipei area from 1994 to 2001. The data collected during 1994–2000 period were used as modeling set and utilized to estimate the meteorologically adjusted trends, and the data of 2001 were used as the validation data. The meteorologically adjusted trends of ozone for these three methods were calculated and compared. The results show that both MLP and KZ filter +MLP models are more suitable than multiple linear regression for estimating the long-term trends of ozone in Taipei, Taiwan. The long-term linear trends of meteorologically adjusted ozone concentrations due to the precursor emissions show an increase trend at all stations, and the percent changes per year range from 1.0% to 2.25% during the modeling period in Taipei area.     

Road traffic impact on urban water quality: a step towards integrated traffic,air and stormwater modelling

Methods for simulating air pollution due to road traffic and the associated effects on stormwater runoff quality in an urban environment are examined with particular emphasis on the integration of the various simulation models into a consistent modelling chain. To that end, the models for traffic, pollutant emissions, atmospheric dispersion and deposition, and stormwater contamination are reviewed. The present study focuses on the implementation of a modelling chain for an actual urban case study, which is the contamination of water runoff by cadmium (Cd), lead (Pb), and zinc (Zn) in the Grigny urban catchment near Paris, France. First, traffic emissions are calculated with traffic inputs using the COPERT4 methodology. Next, the atmospheric dispersion of pollutants is simulated with the Polyphemus line source model and pollutant deposition fluxes in different subcatchment areas are calculated. Finally, the SWMM water quantity and quality model is used to estimate the concentrations of pollutants in stormwater runoff. The simulation results are compared to mass flow rates and concentrations of Cd, Pb and Zn measured at the catchment outlet. The contribution of local traffic to stormwater contamination is estimated to be significant for Pb and, to a lesser extent, for Zn and Cd; however, Pb is most likely overestimated due to outdated emissions factors. The results demonstrate the importance of treating distributed traffic emissions from major roadways explicitly since the impact of these sources on concentrations in the catchment outlet is underestimated when those traffic emissions are spatially averaged over the catchment area.     

Economics of a global strategy for reduction of carbon emissions

The evolution of natural systems that feed and sustain human populations, and indeed the evolution of modern society, has occurred in the context of a moderate and stable climate. Therefore, recent trends in climate change, most likely caused by increasing concentrations of carbon dioxide and other radiative trace gases in the atmosphere, and the expected consequent global warming, are now a major concern. Carbon emissions from energy systems are considered one of the major contributors to climate change and are the focus of all studies on the prevention of climate changes and adaptation strategies. Two global energy scenarios (each with several options) are analysed in this paper: from a dynamic-as-usual concept to a more advanced concept with the goal of stabilising carbon dioxide concentrations in the atmosphere (equivalent to about a 60% reduction of carbon emission compared with today's level). It is shown that the stabilisation approach will require dramatic changes in energy systems: the share of non-carbon fuels will increase to about three quarters of the total primary energy consumption, which will itself grow by a factor of two by the middle of the next century. Surprisingly, the implementation costs turn out to be approximately the same for all scenarios (taking into account possible errors in the cost appraisals for several decades ahead). However, the cost distributions between energy production and use are quite different. Globally, these costs are 3-4% of the GNP, but for developing countries the share of energy investments is, on average, about 7-8% of the GNP, which is cause for concern and will greatly hamper economic and social progress in the Third World. The introduction of energy taxes or carbon taxes in developed countries and the raising of 'global energy funds' could help developing countries to overcome these difficulties. It is supposed that such a policy would stimulate economic growth in developing countries and, as a feedback, overlap the GNP losses in developed countries. The paper attempts to evaluate an optimal strategy for reducing carbon emissions for the next couple of decades, when large uncertainties surround global warming, and to show ways of establishing 'no-regret' policy.     

Motor Vehicle Lead Embssbons Bo the Unfed States: An Analysis of Important Determinants,Geographic Patterns and Future Trends

This paper presents a simple method which utilizes composite emission factors to estimate motor vehicle lead emissions for large areas. Composite emission factors incorporate information on vehicle lead emission rates, sales-weighted average fuel economies, annual vehicle travel fractions, and average gasoline lead concentrations. The lead emissions estimation procedure takes as given estimates of motor vehicle travel and, hence, can be applied to any region or road system for which current or projected travel estimates are available. Estimates of motor vehicle lead emissions for major highway systems in individual states and national forecasts of motor vehicle lead emissions for six potential scenarios regarding the future use of lead additives in gasoline are presented to demonstrate the application of the method.     

Lead,cadmium and mercury contents and bioaccumulation potential of wild edible saprophytic and ectomycorrhizal mushrooms,Croatia

ABSTRACT

Lead (Pb), cadmium (Cd), and mercury (Hg) contents in ten species of edible mushrooms in Trako??an, Croatia were determined. In addition, the similarity between the studied species was determined by cluster analysis. The caps and stipes of the fruiting bodies were analysed separately. The analyses were carried out by inductively coupled plasma - optical emission spectrometry (ICP-OES). The greatest mean lead concentrations of 1.91 and 1.60 mg kg ^?1 were determined in caps and stipes of Macrolepiota procera. The greatest mean concentrations of cadmium (3.23 and 2.24 mg kg^?1) were determined in caps and stipes of Agaricus campestris and of mercury (2.56 and 2.35 mg kg^?1) in Boletus edulis. In terms of the anatomical parts of the fruiting body (cap-stipe), a considerably greater concentration of the analysed elements was found in the cap for all mushroom species. According to calculated bio-concentration factors, all the examined species were found to be bio-accumulators of Cd and Hg. On the basis of the accumulation of the studied metals, great similarity of mushroom species belonging to the same genus and partial similarity of species of the same ecological affiliation was obtained by cluster analysis.     

Resolving the interactions between population density and air pollution emissions controls in the San Joaquin Valley, USA

The effectiveness of emissions control programs designed to reduce concentrations of airborne particulate matter with an aerodynamic diameter < 2.5 microm (PM2.5) in California's San Joaquin Valley was studied in the year 2030 under three growth scenarios: low, medium, and high population density. Base-case inventories for each choice of population density were created using a coupled emissions modeling system that simultaneously considered interactions between land use and transportation, area source, and point source emissions. The ambient PM2.5 response to each combination of population density and emissions control was evaluated using a regional chemical transport model over a 3-week winter stagnation episode. Comparisons between scenarios were based on regional average and population-weighted PM2.5 concentrations. In the absence of any emissions control program, population-weighted concentrations of PM2.5 in the future San Joaquin Valley are lowest undergrowth scenarios that emphasize low population density. A complete ban on wood burning and a 90% reduction in emissions from food cooking operations and diesel engines must occur before medium- to high-density growth scenarios result in lower population-weighted concentrations of PM2.5. These trends partly reflect the fact that existing downtown urban cores that naturally act as anchor points for new high-density growth in the San Joaquin Valley are located close to major transportation corridors for goods movement. Adding growth buffers around transportation corridors had little impact in the current analysis, since the 8-km resolution of the chemical transport model already provided an artificial buffer around major emissions sources. Assuming that future emissions controls will greatly reduce or eliminate emissions from residential wood burning, food cooking, and diesel engines, the 2030 growth scenario using "as-planned" (medium) population density achieves the lowest population-weighted average PM2.5 concentration in the future San Joaquin Valley during a severe winter stagnation event. Implications: The San Joaquin Valley is one of the most heavily polluted air basins in the United States that are projected to experience strong population growth in the coming decades. The best plan to improve air quality in the region combines medium- or high-density population growth with rigorous emissions controls. In the absences of controls, high-density growth leads to increased population exposure to PM2.5 compared with low-density growth scenarios (urban sprawl).