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Changes of emissions and atmospheric deposition of mercury, lead, and cadmium
Atmospheric Environment 43 (2009) 117–127
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Atmospheric Environment journal homepage: www.elsevier.com/locate/atmosenv
Changes of emissions and atmospheric deposition of mercury, lead, and cadmium Jozef M. Pacyna a, b, *, Elisabeth G. Pacyna a, Wenche Aas a a b
Center for Ecological Economics, NILU, Kjeller, Norway Gdansk University of Technology, Chemical Faculty, Gdansk, Poland
a b s t r a c t Keywords: Heavy metals Atmospheric emission Anthropogenic sources Emission trends Emission scenarios Air concentrations Precipitation Europe
This paper reviews the information on trends of past emissions of mercury, lead, and cadmium in Europe, as well as examines current levels and future scenarios of these emissions. The impact of various factors on emission changes is discussed including the implementation of various strategies of emission controls in Europe. Future emissions are forecasted on the basis of various scenarios of economy growth in Europe, implementation of European and global legislation (e.g. the Kyoto agreement), population changes, etc. Changes of emissions of mercury, lead, and cadmium are then related to the changes of concentrations of these contaminants in air and precipitation samples at selected stations in Europe. It can be concluded that the reduction trends of anthropogenic emissions of cadmium and lead in Europe are similar to the reduction trends of air concentrations of these metals during the last 2 decades. Somewhat different relationship has been noted for changes in emissions and precipitation. In general for Europe, 60% reduction of Cd emissions was met by about 45% reductions of Cd concentrations in precipitation at the studied stations during the last 2 decades. There is a potential for further reduction of these emissions until the year 2010 up to about 37% for Cd, 51% for Pb, and 49% for Hg as estimated within various emission scenarios presented in the paper. Ó 2008 Published by Elsevier Ltd.
1. Introduction Heavy metals can create adverse effects on the environment and human health due to their bioavailability and toxicity in various environmental compartments (e.g. a review by Chang, 1996). During the last three decades a number of studies have been carried out to assess the fate and behavior of various heavy metals in the environment, as well as their environmental effects. Mercury, lead, and cadmium have been given a particular attention in these studies and these metals became priority contaminants within various international conventions and programs aiming at the reduction of environmental and human exposure to air pollution. These conventions include the UN Economic Commission for Europe (ECE) Long-Range Transboundary Transport of Air Pollutants (LRTAP) Convention (www.unece.org) (EMEP, 2006), and the OSPAR (www.ospar.org) (OSPAR, 2006), and HELCOM (www. helcom.fi) (HELCOM, 2006) conventions on the reduction of Hg inputs to the North Sea/North-east Atlantic and the Baltic Sea, respectively. Although the research so far has been quite conclusive with regard to the impacts of lead, mercury, and cadmium on environment and human health, much less conclusive is the information on sources and fluxes of these contaminants. Major
* Corresponding author. Center for Ecological Economics, NILU, Kjeller, Norway. E-mail addresses: [email protected], [email protected] (J.M. Pacyna). 1352-2310/$ – see front matter Ó 2008 Published by Elsevier Ltd. doi:10.1016/j.atmosenv.2008.09.066
questions still need to be answered on the origin of these contaminants from anthropogenic sources as compared to emissions from natural sources and to what extent atmospheric deposition is their main pathway to aquatic and terrestrial ecosystems, and finally the main input to the food chain. This paper reviews the information on historical trend of emissions of mercury, lead, and cadmium in Europe, as well as examines current levels and future projects of these emissions. The impact of various factors on emission changes is discussed including the implementation of various strategies of emission controls in Europe. Future emissions are forecasted on the basis of various scenarios of economy growth in Europe, implementation of European and global legislation (e.g. the Kyoto agreement), population changes, etc. Changes of emissions of mercury, lead, and cadmium are then related to the changes of air concentrations and atmospheric deposition of these contaminants in Europe in the past and at present, reported within the UN ECE LRTAP European Monitoring and Evaluation Programme (EMEP) (www.emep.int and EMEP, 2006).
2. Sources of emissions Mercury, lead, and cadmium are emitted to the atmosphere from anthropogenic and natural sources. Major anthropogenic sources include:
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- production of energy and various industrial goods, - incineration of wastes, and - various uses of metals. Information on emissions of mercury, lead, and cadmium from these sources to the atmosphere has been collected within the above mentioned conventions, particularly within the UN ECE LRTAP EMEP (www.emep.int and EMEP, 2006). However, the data reported by national emission experts in the European countries are often incomplete and inaccurate, as concluded at various emission expert and modeler meetings within the UN ECE LRTAP Convention (e.g. EMEP, 2006). Therefore a number of research projects were carried out to help improving the quality of mercury, lead, and cadmium emission data in Europe, including the 5th and 6th EU Framework Programs, such as MAMCS (ENV4CT97-0593 www.eloisegroup.org), MERCYMS (EVK3-CT200200070 www.iia-cnr.unical.it/MERCYMS/project.htm), MOE (www. eloisegroup.org), EMECAP (QLK4-2000-00489 www.emecap.com) and ESPREME (SSPI-CT2003-502527 http://espreme.ier.unistuttgart.de). Major emphasis in these projects was to estimate the past, current and even future emissions of mercury, lead, and cadmium in Europe from the following main emission source categories: combustion of coal in utility boilers (power plants), combustion of oil in utility boilers, combustion of coal in industrial, residential, and commercial boilers, combustion of oil in industrial, residential, and commercial boilers, iron and steel production, cement production, non-ferrous metal manufacturing, waste incineration, gasoline combustion (only for Pb), and other sources (various uses of metals). These estimates were carried out primarily on the basis of information on emission factors and statistical data. The emission factors for most of the above mentioned categories can be obtained from the EMEP/CORINAIR Atmospheric Emission Inventory Guidebook (UN ECE, 2000; see, http://reports.eea.eu.int/EMEPCORINAIR3/ en/). This Guidebook has been developed in the late 1990s and the information presented in this document is under continuous revision and update. The Guidebook is regarded as the main document reporting the state-of-the-art information on emission factors of air pollutants from variety of emission sources. There are four major groups of parameters affecting the emission factors of trace metals to the atmosphere: contamination of raw materials by trace metals, physico-chemical properties of trace metals affecting its behavior during the industrial processes, the technology of industrial processes, and the type and efficiency of control equipment. Detailed description of the impact of these parameters on the quantity and quality of emission factors is presented in other works of the authors (e.g. Pacyna and Pacyna, 2002; Pacyna et al., 2003). One conclusion that is obvious from the analysis of various parameters affecting the trace metal emissions is that processing of mineral resources at high temperatures, such as combustion of fossil fuels, roasting and smelting of ores, kiln operations in cement industry, as well as incineration of wastes results in the release of the largest amounts of trace metals to the environment, particularly to the atmosphere.
Statistical data used in the emission estimates are available from various international and national statistical yearbooks, including the UN Statistical Yearbook (e.g. UN, 2003). The basis for emission estimates can also be data produced by the EU PRIMES (Energy Systems Model of the National University of Athens) model. This model is used to generate information needed within the CAFE´ (Clean Air for Europe) program (http://europa.eu.int/comm/ environment/air/cafe/index.htm). The PRIMES model results are particularly important for the estimates of future scenarios of trace metal emissions. Results of estimates of past and current emissions of mercury, lead, and cadmium from anthropogenic sources in Europe to the atmosphere were published in previous papers by the authors of this article (Pacyna et al., 2006, 2007; van Storch et al., 2003). Summary of these results is presented in Fig. 1 where emissions of Cd and Pb are reported from 1955 until 2005 for major source categories, while emissions of Hg are reported from 1980 until 2005. Emission trends for these three trace metals are somewhat different although they all indicate clearly an emission decrease during the period of analysis. Following the detailed emission trend analysis until 2000 presented by Pacyna et al. (2007) in their recent paper it can be concluded that the highest emissions of Cd in Europe were estimated for the mid 1960s when the production of non-ferrous metals, particularly copper and zinc in high temperature processes employed in various smelters was growing quite rapidly. At the same time efficient emission control devices were still missing. The 1960s emissions of Cd were about 5 times higher than the 2005 emissions of this metal. Clearly, the trend of total anthropogenic emissions of Cd is almost identical with the trend of emissions of Cd from non-ferrous metal industry, the major emission source of Cd in Europe at that time. First major decrease of Cd emissions in Europe has occurred in the mid 1970s when more efficient electrostatic precipitators (ESPs) and fabric filters (FFs) were employed in Europe to reduce dust emissions from major point sources of emissions, such as smelters, power plants, and cement kilns. The second decrease of Cd emissions was observed in the mid 1980s were efficient flue gas desulfurization (FGD) installations were introduced in the European smelters and power plants. Finally, the major decline of Cd emissions in Europe was observed between 1990 and 2000. This decrease was caused mainly by 1) further implementation of the FGD equipment in smelters and power plants in Eastern Europe, and 2) decline of economy in Eastern and Central Europe due to the switch of economies in these countries from centrally planned to market oriented. Trend of past emissions of Pb until the year 2000 has also been discussed by Pacyna et al. (2007). Here the 2005 emission data are added to this analysis. It can be concluded from Fig. 1 that the total Pb emission trend is very much dominated by the Pb emission trend for a single emission category, namely combustion of gasoline. The Pb emissions in Europe picked in the mid 1970s and they were then more than one order of magnitude higher than the 2005 emissions of this element. These changes are quite directly related to the changes of regulation in the use of lead additives to gasoline (van Storch et al., 2003). In the 1970s, the German government was the first in Europe to regulate lead additives in gasoline. A maximum content of 0.4 g Pb l 1 was imposed in Germany in 1972, which was lowered to 0.15 g Pb l 1 (so-called low-leaded gasoline) in 1976. The EU fixed its limit modestly at 0.4 g Pb l 1 beginning only in 1981 and prohibited all countries from stipulating national limits lower than 0.15 g Pb l 1. In 1985 Germany passed a law to reduce total automobile emissions. This law led to the introduction of unleaded gasoline (no lead additives added). In 1985 the EU mandated all member states to offer unleaded gasoline starting October 1989 and recommended a maximum of 0.15 g Pb l 1. The Aarhus Treaty signed in 1998 by nearly all European countries
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Fig. 1. Change of atmospheric emissions of Cd, Pb and Hg in Europe in the period from 1980 through 2005 (in t year
stipulated the exclusive usage of unleaded gasoline by the year 2005. This, however, was not achieved. The last 15 years was the time with very significant decreases of Pb emissions in Europe due to the use of unleaded gasoline and introduction of efficient dedusting installations in industrial plants. Even between 2000 and 2005 there was about 20% decrease of Pb emissions in Europe. Emission trend for Hg in Europe is shorter than for Cd and Pb. Unlike the trends of past emissions of Cd and Pb, the total emission trend for Hg is dependent on the emission trends of two major source categories: 1) combustion of fossil fuels and mainly coal, and 2) industrial processes, such as the production of cement, iron and steel, non-ferrous metals, and chlor-alkali products (Fig. 1). Initial discussion of Hg emission changes between 1980 and 2000 was published by Pacyna et al. (2006). It can be concluded that the
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analysis of information on Hg emissions from 1980 to 2005 in Fig. 1 indicates steady decrease of Hg emissions in Europe during this period. The total emission of Hg has decreased by a factor of more than 4, while the biggest relative reduction in emissions by a factor more than 5 has been estimated for emission from industrial processes. Emissions resulting from combustion of fuels also fell significantly – by a factor almost 4 from 1980 to 2005 – but became the largest source already in the mid 1990s. Major decline of Hg emissions in Europe occurred at the end of the 1980s and the beginning of the 1990s. This decrease was caused mainly by 1) the implementation of the FGD equipment in large power plants and the other emission controls in other industrial sectors, particularly in Western Europe, and 2) decline of economy in Eastern and Central Europe due to the switch in economies in
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these countries from centrally planned to market oriented (Iverfeldt et al., 1995; Munthe et al., 2001). Similar conclusions were drawn earlier in this paper for emission trend for Cd. Emission estimates presented in Fig. 1 differ from ‘‘official’’ emission data reported by national emission experts in Europe to the UN ECE LRTAP Convention (and often presented as EMEP emission data). It is important here to explain these differences once again because the trends of emission data presented in Fig. 1 are compared later in this paper with the trends of air concentrations and atmospheric deposition of cadmium, lead and mercury measured at the EMEP stations. In the year 2000, the official EMEP Cd emissions from fuel combustion in the utility boilers, industrial furnaces and residential and commercial units seem to be underestimated by a factor of more than 3 compared with data in this paper. These emissions from other sources reported in sets of official emission data are lower by a factor of more than 2. The official EMEP emission data for Pb from industrial sources and combustion of fuels in stationary sources are underestimated by almost a factor of 2. However, this underestimation is not that important for the comparison of total emission of Pb because the Pb emissions from gasoline combustion, by far the major source of Pb emissions in Europe are very similar in the EMEP estimates and the estimates in this paper. Following the discussion of comparison of official EMEP emission data and the emission data presented by the authors of this paper (Pacyna et al., 2007) it is concluded that the emission estimates presented in this work are more accurate and complete than the ‘‘official’’ emission data reported to the UN ECE LRTAP Convention. This conclusion has been reached on the basis of discussion of model results obtained within the UN ECE LRTAP EMEP program (http://www.msceast.org). The model estimates of air concentrations and atmospheric deposition of heavy metals, carried out on the basis of ‘‘official’’ emission estimates were lower by a factor of 2 and more than the measured concentrations and deposition. These results, communicated at various consultation meetings within EMEP workshops, have clearly indicated the need for improvement of heavy metal emission data in Europe and thus the development of the emission inventory presented in this work (EMEP, 2006). Thus, it was considered proper and scientifically justified to compare the trends of emission data in Fig. 1 with the EMEP measurements of air concentrations and atmospheric deposition for Cd and Pb. Mercury emission data in Fig. 1 were estimated in close cooperation with EMEP emission experts, as explained in Pacyna et al. (2006). National estimates of anthropogenic emissions of mercury for 2005 were provided by national experts from 29 countries in Europe. The reporting of these data has been done within the UN ECE LRTAP. The emission data received from national authorities have then been checked by the authors for completeness and comparability. The completeness of data regarded mainly the inclusion of all major source categories which may emit mercury to the atmosphere. No major omissions have been detected in the reported data. With regard to the issue of comparability, information from the experts on emissions of mercury from various sources was brought together with statistics on the production of industrial goods and/or the consumption of raw materials, and these two sets of data were used to calculate emission factors. Emission factors calculated in such a way were then compared with emission factors reported in the Joint EMEP/CORINAIR Atmospheric Emission Inventory Guidebook (http://reports.eea.eu.int/EMEPCORINAIR3/ en/, UN ECE, 2000). In a majority of the cases, emission factors estimated on the basis of national emission data reported to the project were within the range of emission factors proposed in the Guidebook. Emission estimates were carried out by Pacyna et al. (2006) for the countries where national emission data were not available. Thus, the comparison of emission trends with the trends
of EMEP data on concentrations and deposition is straightforward for Hg. Concerning the accuracy of emission data presented in Fig. 1, the following accuracy values can be reported for different emission categories:
stationary fossil fuel combustion: 20%, non-ferrous metal production: 20%, iron and steel production: 25%, cement production: 20%, and waste disposal: 100%.
Details on the accuracy estimates are presented in Pacyna et al. (2006) for mercury and in Pacyna et al. (2007) for cadmium and lead. 3. Air concentrations and atmospheric deposition Trace metals were officially included in EMEP’s monitoring program in 1999. Earlier data have been available and collected, and the EMEP database thus also includes older data, even back to 1976 for a few sites. However major trend analysis for Europe is available only from around 1990 where about 40 sites in Europe measured trace metals in either precipitation or air or both. A number of countries have been reporting trace metals within the EMEP area in connection with different national and international programmes such as HELCOM, AMAP and OSPAR. The monitoring programme has developed throughout the last decades. In 1990 there were 42 sites measuring lead, however only two of these stations had co-located air and precipitation at the same site. Co-location is important for better understanding the deposition and transport processes. In 2005 there were 29 sites measuring trace metals in both air and precipitation, and altogether there were 63 measurement sites. There were 18 sites measuring at least one form of mercury (Aas and Breivik, 2007). Nevertheless there are still too few monitoring sites in Europe to have a satisfactory spatial distribution over the whole EMEP domain. The Mediterranean region and the most eastern part of Europe are more or less lacking in measurements of trace metals. The recommended methods for sampling and analysis at the regional monitoring sites in Europe were defined and included in the EMEP manual (EMEP, 2001) in 2000. But trace metals have been included in the annual EMEP laboratory inter-comparison already since 1995. Major improvements in the data quality have been done during the last decades (Uggerud and Hjellbrekke, 2007). Particular progress has been made in development and application of analytical methods. In the first years cadmium and lead were mainly measured using Graphite Furnace Atomic Absorption Spectrometry (GF-AAS) method while at present majorities of the laboratory are using the more sensitive Induced Coupled Plasma Mass Spectrometry (ICP-MS) method. In addition, before a sampling protocol was established, the sampling frequency was often monthly using a bulk collector while weekly collection of wet only collectors is now the recommended reference method (EMEP, 2001). Mercury has mainly been measured with Cold Vapor Atomic Fluorescence Spectroscopy (CV-AFS) during the whole period. For details of which methods used it is referred to the EMEP annual data reports, e.g. Aas and Breivik (2007). Based on the requirements given in the European Council Directive on Ambient Air Quality Assessment and Management (EU, 1996) and its 1st (EU, 1999) and 4th Daughter Directive (EU, 2005), a series of new ISO standards are being developed to improve and harmonize the air and deposition measurements of trace elements in Europe. To monitor the compliance of international protocols of emission reductions, it is essential to have measurements of good and known quality. It is expected that the new ISO standards and
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Fig. 2. Change of air concentrations of Cd and Pb at selected stations in Europe from 1987 through 2005 (in ng m
implementation of the EU air quality daughter directives will further improve the trace element measurements in Europe. Trends of air concentrations of cadmium and lead at selected stations are shown in Fig. 2, while trends of atmospheric deposition for these metals are presented in Fig. 3. It should be noted that the selection of stations is different for the analysis of air concentration and precipitation data. The stations with most reliable data were selected for the analysis. They include stations in the Czech Republic (CZ0001R), Germany (DE0001R), Great Britain (GB0091R), the Netherlands (NL0009R), Slovakia (SK0004R), and Norway (NO0001R). The description of these sites and procedures for collection of samples and analytical methods used is presented in Aas and Breivik (2007). For mercury it is only Sweden that has time series that can be used for proper trend analysis. The Swedish data are shown in Fig. 4. 4. Comparison of emission trends with trends of concentrations and deposition A crucial question for policy making is to what extent the reduction of atmospheric emissions of contaminants would result in the decrease of their concentrations in the air and atmospheric deposition. Usually a comparison is made between changes of emissions in a given region and changes of concentrations modeled in this region. Models used to simulate the concentration and deposition changes use the emission data for which the reduction effect of concentrations and deposition is analyzed. Thus the
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dependence between emissions and concentration/deposition changes is clearly expected and related to the input data for the models. In this paper changes in emission estimates are compared with air concentration and precipitation measurements. The Mann–Kendall test and Sens slope estimator (Gilbert, 1987) have been used to estimate the trends at these sites. At the Norwegian site Birkenes there are precipitation measurements of lead and cadmium since 1976 and the reduction for both elements has been higher than 90%. For the other sites the reduction in precipitation has been around 45% since 1990 for both elements. The corresponding relationships in air concentrations have been more than 70% for both metals. For gaseous elemental mercury the reduction observed at the Swedish sites has been 70% since 1980. No significant trend of Hg in precipitation has been observed, using the Mann–Kendall statistical test for the precipitation measurement data between 1989 and 2005. In other papers, a downward trend is also seen in the deposition measurements. For example, Wangberg et al. (2007) observed a reduction in deposition between 10% and 30% when comparing the periods 1995–1998 and 1999–2002 for various OSPAR sites. However, as can be seen in Fig. 4, there is an increase in the deposition concentration in the last two years. A significant reduction of 29% is observed if calculating the trend from 1989 to 2003 only. The air concentration and atmospheric deposition trends for cadmium and lead for the last 2 decades can be compared with the
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Fig. 3. Change of Cd and Pb concentrations in precipitation at selected stations in Europe from 1979 through 2004 (in mg l
emission changes for these compounds. Total cadmium emissions in Europe were reduced by about 60%, and in Scandinavia about 80%. This corresponds well with the reduction of Cd concentrations in the air (about 70%). With regard to reduction of lead emissions in the same period, more than 85% of this reduction was estimated for the whole Europe, including Scandinavia. This corresponds with the reduction of more than 70% of Pb concentrations in the air. As the combustion of gasoline has been the main source of Pb emissions in Europe, these emissions enter the atmosphere close to the ground and therefore it is expected that any changes of such emissions will be clearly reflected in the changes of air concentrations. Indeed, this is confirmed in our studies. More than 85% reduction of Pb emissions and air concentrations can be noted for the Czech Republic and Slovakia (air concentrations in Fig. 2) for the last 2 decades. Somewhat lower values of Pb air concentration reductions were noted for stations in Great Britain and Germany in comparison with the expectations due to more than 85% Pb emission reduction in these countries. This can be explained by the larger contribution of Pb emissions from major stationary point sources to the air concentrations in these countries compared to the contribution from gasoline combustion. Thus, it can be concluded that the reduction trends of anthropogenic emissions of cadmium and lead in Europe are similar to the reduction trends of air concentrations of these metals during the last 2 decades.
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Somewhat different relationship has been noted for changes in emissions and precipitation. In general for Europe, 60% reduction of Cd emissions and 70% reduction of Pb emissions were met by about 45% reductions of Cd and Pb concentrations in precipitation at the studied stations during the last 2 decades. Mercury is a global contaminant with lifetime of some of its chemical forms of about 2 years. This means that the relationship between emissions and air concentrations/atmospheric deposition is less straightforward than the relationships for cadmium and lead. Taking into account the Swedish data from Fig. 4 for the last 2 decades, it can be suggested that the air concentrations of total mercury and concentrations of precipitation have decreased by a factor of 3. The European emissions of mercury have also decreased by a factor of 3 in the same period. The question appears whether this close agreement is coincidental or the impact of European emissions on European concentrations of this contaminant in the air and precipitation is very important and more important than global background in these concentrations related to the global emissions. The data for the period from 1989 through 1995 in Fig. 4 indicating a dramatic change in concentrations seem to support the notion of the high importance of the European emission impacts, much stronger than the global background. This concentration change reflects the emission change caused primarily by the switch of economies in Eastern Europe from centrally planned to market oriented in this period, leaving several industries in this region closing down, specially chemical
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Mercury in air and precip at SE0002/SE0014
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Fig. 4. Change of Hg concentrations in air (total Hg in ng m
industries. On the other hand, clearly visible increases of concentrations during the latest period of measurements from 2003 through 2005 cannot be explained by the changes of European emissions. Thus, the concentrations in that period seem to support the notion that emissions outside Europe, e.g. in Asia may have an important impact on the concentration levels in Europe (Wilson et al., 2006). This would mean that any action to reduce the Hg emissions in Europe should be coordinated with strategies for Hg emission reductions globally. However, one should be careful with taking conclusions on the basis of concentration changes measured and discussed at stations from one region only (Iverfeldt et al., 1995; Munthe et al., 2001, 2003; Slemr et al., 2003).
5. Spatial distribution of emissions and concentrations in Europe in 2005 Information on spatial distribution of emission data is needed for the development of regional policies on emission reduction as well as for modeling purposes. In this paper, the spatial distribution of emissions is used for comparison with spatial distribution of concentrations in the air and precipitation of cadmium and lead at the EMEP stations in 2005. No comparison has been made for mercury due to very low amount of data for this contaminant, available from the EMEP measurement network. Spatial distribution of cadmium and lead emissions in Europe in 2005 within the EMEP grid system of 50 km by 50 km is presented in Fig. 5. Details on the development of emission maps presented in Fig. 5 are available from Pacyna et al. (2007). These maps were prepared within the EU project ESPREME (http://espreme.ier.unistuttgart.de) by experts from the Institute of Energy Economics and the Rational Use of Energy (IER) at the University of Stuttgart, Germany. Cadmium and lead show different patterns of spatial distributions of their emissions. Cadmium is emitted primarily from point sources of emissions, such as non-ferrous metal smelters, power plants, and waste incinerators, while lead emissions come mainly from area sources, such as traffic. These clear points (grids) of emissions are indicated as hot spots on the Cd emission maps in contrast to fairly even distribution over many grids for Pb emissions. Cadmium measurements in air and precipitation follow the emission distribution fairly well with high values in Central Europe and lower concentrations in Northern Europe, as presented in
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Fig. 6. The lowest concentrations are generally observed in northern Scandinavia, Greenland, Iceland, and the westernmost part of Europe. An increasing gradient can in general be seen southeast, but the air concentration and atmospheric deposition levels are not evenly distributed, there are some ‘‘hotspots’’ for some elements. Similar trend is observed for Pb concentrations but the concentration gradient from Central to Northern Europe is less pronounced. Good relationship between spatial distribution of emissions and concentrations in the air and precipitation for cadmium and lead indicates that the impact of emissions on air concentrations and precipitation in the emission areas is very important. Local deposition of these two contaminants seems to be quite important for assessment of the environmental impacts caused by emissions of Cd and Pb. The above conclusions are well supported by the estimates of the atmospheric supply of Cd, Pb and Hg to the Baltic Sea, carried out by EMEP as a contribution to HELCOM (http://www. emep.int/publ/helcom/2007/index.html and Bartnicki et al., 2007). Decreasing emission trends for Cd and Pb can also be confirmed by the analysis of concentration trends in mosses (Harmens et al., 2008). The concentration of lead and cadmium in mosses decreased between 1990 and 2000 by 57% and 42%, respectively. 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 significantly across Europe.
6. Future changes of emissions Information on changes of past emissions and concentrations can be used to discuss their future changes. The past changes of Cd, Pb, and Hg emissions indicate clear decrease of these emissions and suggest that future reduction is possible. Three types of scenarios were elaborated within the EU ESPREME project for the year 2010: the CAFE´ Baseline scenario with climate policies, the CAFE´ Baseline scenario without climate policies, and the CAFE´ Maximum Feasible Technological Reduction (MFTR) scenario. The CAFE´ Baseline scenario without climate policies adopts the baseline energy projection of the ‘‘European energy and transport – Trends to 2030’’ outlook of the Directorate General for Energy and Transport of the European Commission (EC, 2003) as a starting
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Fig. 5. Spatial distribution of Cd and Pb emissions in Europe in the EMEP grid of 50 km 50 km (in t grid
point. This projection does not assume any further climate measures beyond those already adopted in 2002. The implication of further climate measures is included in the CAFE´ Baseline scenario with climate policies. This projection attempts to quantify how the decarbonisation of the energy system would take place due to
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climate policies. The CAFE´ Maximum Feasible Technological Reduction scenario assumes that all measures are in place to maximally reduce or phase-out a given contaminant. The emission scenarios were estimated on the basis of information on emission factors prepared within the ESPREME project
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Pb in precipitation (µg/l)
Cd in precipitation (µg/l)
Pb in aerosols (ng/m3)
Cd in aerosols (ng/m3)
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Fig. 6. Average concentrations of Pb and Cd in the air and precipitation samples in 2005.
on availability and effectiveness of emission control and the CAFE´ statistical data for the year 2000. Both, scenario estimates and emission factors are presented on the ESPREME project website (http://espreme.ier.uni-stuttgart.de). The details are also presented in Pacyna et al. (2007). The statistical data used in the emission scenario estimates were obtained from the CAFE´ Baseline scenario with climate policies and Baseline scenario with no policies, calculated with the use of the PRIMES model version 2 (data available at http://espreme.ier.unistuttgart.de). The results of emission scenario estimates are presented in Fig. 7. The following can be concluded from these estimates: the 2010 CAFE´ Baseline scenario with no climate policies indicates the following emission reductions compared to the emissions in the year 2005: 9% for Cd, 21% for Pb and 22% for Hg, and the 2010 CAFE´ Baseline scenario with climate policies indicates an emission reduction of 15% for Cd, 25% for Pb, and 26% for Hg, compared to the emissions in the year 2005.
Implementation of the MFTR scenario will result in further emission reduction of studied trace metals compared to the emissions estimated for the two CAFE´ Baseline scenarios (with and without climate measures). The largest reductions of emissions between the years 2005 and 2010 (the MFTR scenario) are as follows: 37% for Cd, 51% for Pb, and 49% for Hg. It is difficult to assess to what extent the emission reductions mentioned above would affect the reduction of air concentrations and atmospheric deposition of cadmium, lead, and mercury in Europe in the future. This assessment can be carried out with the help of dispersion models on continental and global scale (the latter for Hg). 7. Final remarks and future research Analysis of the information on emissions of cadmium, lead, and mercury from anthropogenic sources in Europe over the last 5 decades indicates that these emissions picked in the late 1960s and the early 1970s. Later on these emissions have been in a continuous decrease until now. This decreasing trend over the last 3 decades is
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aspects of environmental contamination by cadmium, lead, and mercury. Some of these questions could be defined as follows: - to what extent do we need to reduce emissions of these contaminants? - do we have technological and non-technological measures to obtain this reduction and what will be the cost of implementation of these measures? - to what extent future emission reduction will contribute to the decrease of concentrations of these contaminants in the air and precipitation samples and what are the required concentration levels that would guarantee no harmful effects of contaminants on environment and human health?
Fig. 7. Scenarios of future emissions of Cd, Pb, and Hg in Europe (in t year Description of scenarios is given in the main text of the paper.
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partly due to the implementation of emission control equipment, such as high efficiency of de-dusting installations and flue gas desulfurization installations that remove not only sulfur dioxide but also other gaseous contaminants, such as mercury. These emission control devices were employed in various utility and industrial plants, such as power plans, smelters, cement kilns, and incinerators as a way of implementation of various environmental protection policies at local and regional level. Gradual removal of leaded additives to gasoline over the last 3 decades has been the major factor contributing to very high decrease of lead emission in Europe. Introduction and use of gasoline without lead additives have been a major policy success in Europe in combating lead contamination of environment. Another factor contributing to the emission decreases in the late 1980s and the beginning of the 1990s in Central and Eastern Europe was the economic decline in this part of Europe caused by economy transfers from centrally planned to market oriented. Past trends of Cd, Pb, and Hg concentrations in air and precipitation samples have followed closely the decrease of emissions of these metals for the last 3 decades, particularly the air concentration trend. However, it should be cautioned that only limited amount of information is available from the EMEP program on these concentrations. Therefore the results presented here can be regarded as a first step in analyzing the relationships between the emission changes and changes of concentration in the air and precipitation for cadmium, lead, and mercury. The amount of EMEP stations measuring these concentrations is increasing and therefore it is expected that more complete analysis of emissions and concentrations will be possible in the near future. An interesting feature has appeared for Hg concentrations measured in the latest years indicating some small increases in selected regions. This fact may indicate how important it is to consider mercury as a global contaminant, because emissions in other regions may and probably do affect the concentrations in the air and precipitation of this pollutant in Europe. Again, it is too early to develop any major conclusions on the basis of data presented here, but in the near future one should focus more on the impact of global emission of mercury on the contamination of the environment in Europe. So far, major conclusions were drawn in this direction on the basis of information on mercury depletion in the air over the Arctic. It is very interesting to further develop future emission scenarios and discuss to what extent these emissions would affect future concentrations of contaminants in the air and precipitation. There are a number of questions that would need to be addressed in future research that are related to environmental and economic
Major development of procedures for valuation of environmental benefits from the emission reduction of cadmium, lead, and mercury and procedures for various costs of this reduction would need to be made in order to address these questions. This means that multidisciplinary analysis of cost–benefits in relation to the reduction of cadmium, lead, and mercury emissions is going to be a very important tool for integrated assessment of drivers, pressures, and the state of the environment in Europe with regard to the contamination by these pollutants. Concentration measurements would need to be improved with regard to the coverage of station network in Europe and completeness of measurement programs at these stations. Efforts to achieve this improvement within EMEP are very important and they hold a promise of more complete knowledge of the state of the European environment with regard to contamination by trace metals (and other pollutants). A larger number of so-called ‘‘EMEP super-stations’’ measuring extended sets of parameters and chemicals (e.g. EMEP, 2006) will also contribute to this improvement of our knowledge. Improved monitoring networks are the key element in developing new policies on reduction of air contaminants. Emission estimates presented in this paper should be improved through more complete and accurate emission estimates in individual countries in Europe. There is a clear need for such improvement for both policy makers and modelers. Complete and accurate emission data are the basis for new policies on regional (e.g. EU territory) and global scale. It is understood that the estimates prepared by international experts are valuable for having the information on national emissions in the European countries as long as no better data are available from national emission experts. National emission experts are more familiar with various technical and other specificities affecting the amount of emissions from a given source or even source category in a given country. Major projections of future use of energy, transportation patterns, and industrial development are largely in place in connection with the progress of work within Intergovernmental Panel on Climate Change (IPCC), CAFE´, EU Directives and national development plans and strategies. These projects form a good basis for development of emission scenarios for various contaminants, including cadmium, lead, and mercury. One may expect lower emissions of these contaminants in the future through the implementation of various policies aiming at more efficient use of renewable energy sources for the production of electricity and heat. A number of European countries plan to have up to 20% of their energy budgets met by the use of renewable energy until the year 2020. Acknowledgements The paper was financially supported by the EU project DROPS (Contract No. FP6-2004-SSP-4-022788) and the UN ECE European Monitoring and Assessment Programme (EMEP). The authors are
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grateful to the European Commission and the UN Economic Commission for Europe for this support. The authors would like to thank Dr. Steffen Nitter of University of Stuttgart, Germany for his help in presenting emission data on maps. The authors would also like to thank Mrs. Ewa Jastrzab – Strzelecka of the Institute for Ecology of Industrial Areas (IETU) in Katowice, Poland for her support in preparing the emission scenarios. References Aas, W., Breivik, K., 2007. Heavy Metals and POP Measurements, 2004. The Norwegian Institute for Air Research Report EMEP/CCC-Report 6/2007, Kjeller, Norway. Bartnicki, J., Gusev, A., Aas, W., Fagerli, H. 2007. Atmospheric Supply of Nitrogen, Lead, Cadmium, Mercury and Dioxines/Furanes to the Baltic Sea in 2005. The Norwegian Meterological Institute, EMEP/MSC-W Technical Report 3/2007, Oslo, Norway. Chang, L.W., 1996. Toxicology of Metals. CRC Lewis Publishers, Boca Raton, FL. EC, 2003. European Energy and Transport. Trends to 2030. KO-AC-02-001-EN-C Report, European Commission, Directorate General for Energy and Transport, Luxemburg. EMEP, 2001. Manual for Sampling and Chemical Analysis. Norwegian Institute for Air Research, Report EMEP/CCC-Report 1/1995, revision 1/2001, Kjeller, Norway. Available from:. EMEP, 2006. Inventory Review 2006. Emission Data Reported to the LRTAP Convention and NEC Directive. Evaluation of Inventories of Heavy metals and POPs. Convention on Long-range Transboundary Air Pollution, the European Monitoring and Evaluation Programme. Technical Report MSC-W 1/2006, Oslo, Norway. EU, 1996. Council Directive 96/62/EC of 27 September 1996 on ambient air quality assessment and management. Official Journal L 296, 0055–0063. 21/11/1996. EU, 1999. Council Directive 1999/30/EC of 22 April 1999 relating to limit values for sulphur dioxide, nitrogen dioxide and oxides of nitrogen, particulate matter and lead in ambient air. Official Journal L 163, 0041–0060. 29/06/1999. EU, 2005. Council Directive 2004/107/EC of 15 December 2004 relating to arsenic, cadmium, mercury, nickel and polycyclic aromatic hydrocarbons in ambient air. Official Journal L 23. 26/1/2005. Gilbert, R.O., 1987. Statistical Methods for Environmental Pollution Monitoring. Van Nostrand Reinhold, New York, NY. Harmens, H., Norris, D.A., Koerber, G.R., Buse, A., Steinnes, E., Ru¨hling, A., 2008. Temporal trends (1990–2000) in the concentration of cadmium, lead and mercury in mosses across Europe. Environmental Pollution 151, 368–376. HELCOM, 2006. Atmospheric supply of nitrogen, lead, cadmium, mercury and lindane to the Baltic Sea over the period 1996–2000. Helsinki Commission,
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Baltic Marine Environment Protection Commission. In: Baltic Sea Environment Proceedings No. 101, Helsinki, Finland. Iverfeldt, A., Munthe, J., Brosset, C., Pacyna, J., 1995. Long term changes in concentration and deposition of atmospheric mercury over Scandinavia. Water, Air, and Soil Pollution 80, 227–233. Munthe, J., Kindborn, K., Kruger, O., Petersen, G., Pacyna, J., Iverfeldt, A., 2001. Examining source–receptor relationships for mercury in Scandinavia – modelled and empirical evidence. Water, Air, and Soil Pollution: Focus 1 (80), 299–310. Munthe, J., Wangberg, I., Iverfeldt, A., Lindqvist, O., Stromberg, D., Sommar, J., Gardfeldt, K., Petersen, G., Ebinghaus, R., Prestbo, E., Larjava, K., Siemens, V., 2003. Distribution of atmospheric mercury species in Northern Europe: final results from the MOE project. Atmospheric Environment 37, 9–20. OSPAR, 2006. Review of actions on priority substances identified in background documents adopted by OSPAR (2006 update). In: Hazardous Substances Series. OSPAR Commission, London, UK. Pacyna, E.G., Pacyna, J.M., 2002. Global emission of mercury from anthropogenic sources in 1995. Water, Air, and Soil Pollution 137, 149–165. Pacyna, J.M., Pacyna, E.G., Steenhuisen, F., Wilson, S., 2003. Mapping 1995 global anthropogenic emissions of mercury. Atmospheric Environment 37 (Suppl. 1), 109–117. Pacyna, E.G., Pacyna, J.M., Fudala, J., Strzelecka-Jastrzab, E., Hlawiczka, S., Panasiuk, D., 2006. Mercury emissions from anthropogenic sources in Europe and their scenarios until 2020. The Science of the Total Environment 370, 147– 156. Pacyna, E.G., Pacyna, J.M., Fudala, J., Strzelecka-Jastrzab, E., Hlawiczka, S., Panasiuk, D., Nitter, S., Pregger, T., Pfeiffer, H., Friedrich, R., 2007. Current and future emissions of selected heavy metals to the atmosphere from anthropogenic sources in Europe. Atmospheric Environment 41, 8557–8566. Slemr, F., Brunke, E.-G., Ebinghaus, R., Temme, C., Munthe, J., Wangberg, I., Schroeder, W., Steffen, A., Berg, T., 2003. Worldwide trend of atmospheric mercury since 1977. Geophysical Research Letters 30, 1516. van Storch, H., Costa-Cabral, M., Hagner, C., Feser, F., Pacyna, J.M., Pacyna, E.G., Kolb, S., 2003. Four decades of gasoline lead emissions and control policies in Europe: a retrospective assessment. The Science of the Total Environment 311, 151–176. Uggerud, H., Hjellbrekke, A.-G., 2007. Analytical Intercomparison of Heavy Metals in Precipitation 2005 and 2006. Norwegian Institute for Air Research, Report EMEP/CCC-Report 4/2007, Kjeller, Norway. UN, 2003. Statistical Yearbook. United Nations, New York, NY. UN ECE, 2000. Joint EMEP/CORINAIR Atmospheric Emission Inventory Guidebook. The United Nations Economic Commission for Europe, Geneva, Switzerland. Wangberg, I., Munthe, J., Berg, T., Ebinghaus, R., Kock, H.H., Temme, C., Bieber, E., Spain, T.G., Stolk, A., 2007. Trends in air concentration and deposition of mercury in the coastal environment of the North Sea. Atmospheric Environment 41, 2612–2619. Wilson, S.J., Steenhuisen, F., Pacyna, J.M., Pacyna, E.G., 2006. Mapping the spatial distribution of global anthropogenic mercury atmospheric emission inventories. Atmospheric Environment 40, 4621–4632.
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Atmospheric Environment journal homepage: www.elsevier.com/locate/atmosenv
Changes of emissions and atmospheric deposition of mercury, lead, and cadmium Jozef M. Pacyna a, b, *, Elisabeth G. Pacyna a, Wenche Aas a a b
Center for Ecological Economics, NILU, Kjeller, Norway Gdansk University of Technology, Chemical Faculty, Gdansk, Poland
a b s t r a c t Keywords: Heavy metals Atmospheric emission Anthropogenic sources Emission trends Emission scenarios Air concentrations Precipitation Europe
This paper reviews the information on trends of past emissions of mercury, lead, and cadmium in Europe, as well as examines current levels and future scenarios of these emissions. The impact of various factors on emission changes is discussed including the implementation of various strategies of emission controls in Europe. Future emissions are forecasted on the basis of various scenarios of economy growth in Europe, implementation of European and global legislation (e.g. the Kyoto agreement), population changes, etc. Changes of emissions of mercury, lead, and cadmium are then related to the changes of concentrations of these contaminants in air and precipitation samples at selected stations in Europe. It can be concluded that the reduction trends of anthropogenic emissions of cadmium and lead in Europe are similar to the reduction trends of air concentrations of these metals during the last 2 decades. Somewhat different relationship has been noted for changes in emissions and precipitation. In general for Europe, 60% reduction of Cd emissions was met by about 45% reductions of Cd concentrations in precipitation at the studied stations during the last 2 decades. There is a potential for further reduction of these emissions until the year 2010 up to about 37% for Cd, 51% for Pb, and 49% for Hg as estimated within various emission scenarios presented in the paper. Ó 2008 Published by Elsevier Ltd.
1. Introduction Heavy metals can create adverse effects on the environment and human health due to their bioavailability and toxicity in various environmental compartments (e.g. a review by Chang, 1996). During the last three decades a number of studies have been carried out to assess the fate and behavior of various heavy metals in the environment, as well as their environmental effects. Mercury, lead, and cadmium have been given a particular attention in these studies and these metals became priority contaminants within various international conventions and programs aiming at the reduction of environmental and human exposure to air pollution. These conventions include the UN Economic Commission for Europe (ECE) Long-Range Transboundary Transport of Air Pollutants (LRTAP) Convention (www.unece.org) (EMEP, 2006), and the OSPAR (www.ospar.org) (OSPAR, 2006), and HELCOM (www. helcom.fi) (HELCOM, 2006) conventions on the reduction of Hg inputs to the North Sea/North-east Atlantic and the Baltic Sea, respectively. Although the research so far has been quite conclusive with regard to the impacts of lead, mercury, and cadmium on environment and human health, much less conclusive is the information on sources and fluxes of these contaminants. Major
* Corresponding author. Center for Ecological Economics, NILU, Kjeller, Norway. E-mail addresses: [email protected], [email protected] (J.M. Pacyna). 1352-2310/$ – see front matter Ó 2008 Published by Elsevier Ltd. doi:10.1016/j.atmosenv.2008.09.066
questions still need to be answered on the origin of these contaminants from anthropogenic sources as compared to emissions from natural sources and to what extent atmospheric deposition is their main pathway to aquatic and terrestrial ecosystems, and finally the main input to the food chain. This paper reviews the information on historical trend of emissions of mercury, lead, and cadmium in Europe, as well as examines current levels and future projects of these emissions. The impact of various factors on emission changes is discussed including the implementation of various strategies of emission controls in Europe. Future emissions are forecasted on the basis of various scenarios of economy growth in Europe, implementation of European and global legislation (e.g. the Kyoto agreement), population changes, etc. Changes of emissions of mercury, lead, and cadmium are then related to the changes of air concentrations and atmospheric deposition of these contaminants in Europe in the past and at present, reported within the UN ECE LRTAP European Monitoring and Evaluation Programme (EMEP) (www.emep.int and EMEP, 2006).
2. Sources of emissions Mercury, lead, and cadmium are emitted to the atmosphere from anthropogenic and natural sources. Major anthropogenic sources include:
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- production of energy and various industrial goods, - incineration of wastes, and - various uses of metals. Information on emissions of mercury, lead, and cadmium from these sources to the atmosphere has been collected within the above mentioned conventions, particularly within the UN ECE LRTAP EMEP (www.emep.int and EMEP, 2006). However, the data reported by national emission experts in the European countries are often incomplete and inaccurate, as concluded at various emission expert and modeler meetings within the UN ECE LRTAP Convention (e.g. EMEP, 2006). Therefore a number of research projects were carried out to help improving the quality of mercury, lead, and cadmium emission data in Europe, including the 5th and 6th EU Framework Programs, such as MAMCS (ENV4CT97-0593 www.eloisegroup.org), MERCYMS (EVK3-CT200200070 www.iia-cnr.unical.it/MERCYMS/project.htm), MOE (www. eloisegroup.org), EMECAP (QLK4-2000-00489 www.emecap.com) and ESPREME (SSPI-CT2003-502527 http://espreme.ier.unistuttgart.de). Major emphasis in these projects was to estimate the past, current and even future emissions of mercury, lead, and cadmium in Europe from the following main emission source categories: combustion of coal in utility boilers (power plants), combustion of oil in utility boilers, combustion of coal in industrial, residential, and commercial boilers, combustion of oil in industrial, residential, and commercial boilers, iron and steel production, cement production, non-ferrous metal manufacturing, waste incineration, gasoline combustion (only for Pb), and other sources (various uses of metals). These estimates were carried out primarily on the basis of information on emission factors and statistical data. The emission factors for most of the above mentioned categories can be obtained from the EMEP/CORINAIR Atmospheric Emission Inventory Guidebook (UN ECE, 2000; see, http://reports.eea.eu.int/EMEPCORINAIR3/ en/). This Guidebook has been developed in the late 1990s and the information presented in this document is under continuous revision and update. The Guidebook is regarded as the main document reporting the state-of-the-art information on emission factors of air pollutants from variety of emission sources. There are four major groups of parameters affecting the emission factors of trace metals to the atmosphere: contamination of raw materials by trace metals, physico-chemical properties of trace metals affecting its behavior during the industrial processes, the technology of industrial processes, and the type and efficiency of control equipment. Detailed description of the impact of these parameters on the quantity and quality of emission factors is presented in other works of the authors (e.g. Pacyna and Pacyna, 2002; Pacyna et al., 2003). One conclusion that is obvious from the analysis of various parameters affecting the trace metal emissions is that processing of mineral resources at high temperatures, such as combustion of fossil fuels, roasting and smelting of ores, kiln operations in cement industry, as well as incineration of wastes results in the release of the largest amounts of trace metals to the environment, particularly to the atmosphere.
Statistical data used in the emission estimates are available from various international and national statistical yearbooks, including the UN Statistical Yearbook (e.g. UN, 2003). The basis for emission estimates can also be data produced by the EU PRIMES (Energy Systems Model of the National University of Athens) model. This model is used to generate information needed within the CAFE´ (Clean Air for Europe) program (http://europa.eu.int/comm/ environment/air/cafe/index.htm). The PRIMES model results are particularly important for the estimates of future scenarios of trace metal emissions. Results of estimates of past and current emissions of mercury, lead, and cadmium from anthropogenic sources in Europe to the atmosphere were published in previous papers by the authors of this article (Pacyna et al., 2006, 2007; van Storch et al., 2003). Summary of these results is presented in Fig. 1 where emissions of Cd and Pb are reported from 1955 until 2005 for major source categories, while emissions of Hg are reported from 1980 until 2005. Emission trends for these three trace metals are somewhat different although they all indicate clearly an emission decrease during the period of analysis. Following the detailed emission trend analysis until 2000 presented by Pacyna et al. (2007) in their recent paper it can be concluded that the highest emissions of Cd in Europe were estimated for the mid 1960s when the production of non-ferrous metals, particularly copper and zinc in high temperature processes employed in various smelters was growing quite rapidly. At the same time efficient emission control devices were still missing. The 1960s emissions of Cd were about 5 times higher than the 2005 emissions of this metal. Clearly, the trend of total anthropogenic emissions of Cd is almost identical with the trend of emissions of Cd from non-ferrous metal industry, the major emission source of Cd in Europe at that time. First major decrease of Cd emissions in Europe has occurred in the mid 1970s when more efficient electrostatic precipitators (ESPs) and fabric filters (FFs) were employed in Europe to reduce dust emissions from major point sources of emissions, such as smelters, power plants, and cement kilns. The second decrease of Cd emissions was observed in the mid 1980s were efficient flue gas desulfurization (FGD) installations were introduced in the European smelters and power plants. Finally, the major decline of Cd emissions in Europe was observed between 1990 and 2000. This decrease was caused mainly by 1) further implementation of the FGD equipment in smelters and power plants in Eastern Europe, and 2) decline of economy in Eastern and Central Europe due to the switch of economies in these countries from centrally planned to market oriented. Trend of past emissions of Pb until the year 2000 has also been discussed by Pacyna et al. (2007). Here the 2005 emission data are added to this analysis. It can be concluded from Fig. 1 that the total Pb emission trend is very much dominated by the Pb emission trend for a single emission category, namely combustion of gasoline. The Pb emissions in Europe picked in the mid 1970s and they were then more than one order of magnitude higher than the 2005 emissions of this element. These changes are quite directly related to the changes of regulation in the use of lead additives to gasoline (van Storch et al., 2003). In the 1970s, the German government was the first in Europe to regulate lead additives in gasoline. A maximum content of 0.4 g Pb l 1 was imposed in Germany in 1972, which was lowered to 0.15 g Pb l 1 (so-called low-leaded gasoline) in 1976. The EU fixed its limit modestly at 0.4 g Pb l 1 beginning only in 1981 and prohibited all countries from stipulating national limits lower than 0.15 g Pb l 1. In 1985 Germany passed a law to reduce total automobile emissions. This law led to the introduction of unleaded gasoline (no lead additives added). In 1985 the EU mandated all member states to offer unleaded gasoline starting October 1989 and recommended a maximum of 0.15 g Pb l 1. The Aarhus Treaty signed in 1998 by nearly all European countries
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Fig. 1. Change of atmospheric emissions of Cd, Pb and Hg in Europe in the period from 1980 through 2005 (in t year
stipulated the exclusive usage of unleaded gasoline by the year 2005. This, however, was not achieved. The last 15 years was the time with very significant decreases of Pb emissions in Europe due to the use of unleaded gasoline and introduction of efficient dedusting installations in industrial plants. Even between 2000 and 2005 there was about 20% decrease of Pb emissions in Europe. Emission trend for Hg in Europe is shorter than for Cd and Pb. Unlike the trends of past emissions of Cd and Pb, the total emission trend for Hg is dependent on the emission trends of two major source categories: 1) combustion of fossil fuels and mainly coal, and 2) industrial processes, such as the production of cement, iron and steel, non-ferrous metals, and chlor-alkali products (Fig. 1). Initial discussion of Hg emission changes between 1980 and 2000 was published by Pacyna et al. (2006). It can be concluded that the
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analysis of information on Hg emissions from 1980 to 2005 in Fig. 1 indicates steady decrease of Hg emissions in Europe during this period. The total emission of Hg has decreased by a factor of more than 4, while the biggest relative reduction in emissions by a factor more than 5 has been estimated for emission from industrial processes. Emissions resulting from combustion of fuels also fell significantly – by a factor almost 4 from 1980 to 2005 – but became the largest source already in the mid 1990s. Major decline of Hg emissions in Europe occurred at the end of the 1980s and the beginning of the 1990s. This decrease was caused mainly by 1) the implementation of the FGD equipment in large power plants and the other emission controls in other industrial sectors, particularly in Western Europe, and 2) decline of economy in Eastern and Central Europe due to the switch in economies in
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these countries from centrally planned to market oriented (Iverfeldt et al., 1995; Munthe et al., 2001). Similar conclusions were drawn earlier in this paper for emission trend for Cd. Emission estimates presented in Fig. 1 differ from ‘‘official’’ emission data reported by national emission experts in Europe to the UN ECE LRTAP Convention (and often presented as EMEP emission data). It is important here to explain these differences once again because the trends of emission data presented in Fig. 1 are compared later in this paper with the trends of air concentrations and atmospheric deposition of cadmium, lead and mercury measured at the EMEP stations. In the year 2000, the official EMEP Cd emissions from fuel combustion in the utility boilers, industrial furnaces and residential and commercial units seem to be underestimated by a factor of more than 3 compared with data in this paper. These emissions from other sources reported in sets of official emission data are lower by a factor of more than 2. The official EMEP emission data for Pb from industrial sources and combustion of fuels in stationary sources are underestimated by almost a factor of 2. However, this underestimation is not that important for the comparison of total emission of Pb because the Pb emissions from gasoline combustion, by far the major source of Pb emissions in Europe are very similar in the EMEP estimates and the estimates in this paper. Following the discussion of comparison of official EMEP emission data and the emission data presented by the authors of this paper (Pacyna et al., 2007) it is concluded that the emission estimates presented in this work are more accurate and complete than the ‘‘official’’ emission data reported to the UN ECE LRTAP Convention. This conclusion has been reached on the basis of discussion of model results obtained within the UN ECE LRTAP EMEP program (http://www.msceast.org). The model estimates of air concentrations and atmospheric deposition of heavy metals, carried out on the basis of ‘‘official’’ emission estimates were lower by a factor of 2 and more than the measured concentrations and deposition. These results, communicated at various consultation meetings within EMEP workshops, have clearly indicated the need for improvement of heavy metal emission data in Europe and thus the development of the emission inventory presented in this work (EMEP, 2006). Thus, it was considered proper and scientifically justified to compare the trends of emission data in Fig. 1 with the EMEP measurements of air concentrations and atmospheric deposition for Cd and Pb. Mercury emission data in Fig. 1 were estimated in close cooperation with EMEP emission experts, as explained in Pacyna et al. (2006). National estimates of anthropogenic emissions of mercury for 2005 were provided by national experts from 29 countries in Europe. The reporting of these data has been done within the UN ECE LRTAP. The emission data received from national authorities have then been checked by the authors for completeness and comparability. The completeness of data regarded mainly the inclusion of all major source categories which may emit mercury to the atmosphere. No major omissions have been detected in the reported data. With regard to the issue of comparability, information from the experts on emissions of mercury from various sources was brought together with statistics on the production of industrial goods and/or the consumption of raw materials, and these two sets of data were used to calculate emission factors. Emission factors calculated in such a way were then compared with emission factors reported in the Joint EMEP/CORINAIR Atmospheric Emission Inventory Guidebook (http://reports.eea.eu.int/EMEPCORINAIR3/ en/, UN ECE, 2000). In a majority of the cases, emission factors estimated on the basis of national emission data reported to the project were within the range of emission factors proposed in the Guidebook. Emission estimates were carried out by Pacyna et al. (2006) for the countries where national emission data were not available. Thus, the comparison of emission trends with the trends
of EMEP data on concentrations and deposition is straightforward for Hg. Concerning the accuracy of emission data presented in Fig. 1, the following accuracy values can be reported for different emission categories:
stationary fossil fuel combustion: 20%, non-ferrous metal production: 20%, iron and steel production: 25%, cement production: 20%, and waste disposal: 100%.
Details on the accuracy estimates are presented in Pacyna et al. (2006) for mercury and in Pacyna et al. (2007) for cadmium and lead. 3. Air concentrations and atmospheric deposition Trace metals were officially included in EMEP’s monitoring program in 1999. Earlier data have been available and collected, and the EMEP database thus also includes older data, even back to 1976 for a few sites. However major trend analysis for Europe is available only from around 1990 where about 40 sites in Europe measured trace metals in either precipitation or air or both. A number of countries have been reporting trace metals within the EMEP area in connection with different national and international programmes such as HELCOM, AMAP and OSPAR. The monitoring programme has developed throughout the last decades. In 1990 there were 42 sites measuring lead, however only two of these stations had co-located air and precipitation at the same site. Co-location is important for better understanding the deposition and transport processes. In 2005 there were 29 sites measuring trace metals in both air and precipitation, and altogether there were 63 measurement sites. There were 18 sites measuring at least one form of mercury (Aas and Breivik, 2007). Nevertheless there are still too few monitoring sites in Europe to have a satisfactory spatial distribution over the whole EMEP domain. The Mediterranean region and the most eastern part of Europe are more or less lacking in measurements of trace metals. The recommended methods for sampling and analysis at the regional monitoring sites in Europe were defined and included in the EMEP manual (EMEP, 2001) in 2000. But trace metals have been included in the annual EMEP laboratory inter-comparison already since 1995. Major improvements in the data quality have been done during the last decades (Uggerud and Hjellbrekke, 2007). Particular progress has been made in development and application of analytical methods. In the first years cadmium and lead were mainly measured using Graphite Furnace Atomic Absorption Spectrometry (GF-AAS) method while at present majorities of the laboratory are using the more sensitive Induced Coupled Plasma Mass Spectrometry (ICP-MS) method. In addition, before a sampling protocol was established, the sampling frequency was often monthly using a bulk collector while weekly collection of wet only collectors is now the recommended reference method (EMEP, 2001). Mercury has mainly been measured with Cold Vapor Atomic Fluorescence Spectroscopy (CV-AFS) during the whole period. For details of which methods used it is referred to the EMEP annual data reports, e.g. Aas and Breivik (2007). Based on the requirements given in the European Council Directive on Ambient Air Quality Assessment and Management (EU, 1996) and its 1st (EU, 1999) and 4th Daughter Directive (EU, 2005), a series of new ISO standards are being developed to improve and harmonize the air and deposition measurements of trace elements in Europe. To monitor the compliance of international protocols of emission reductions, it is essential to have measurements of good and known quality. It is expected that the new ISO standards and
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Fig. 2. Change of air concentrations of Cd and Pb at selected stations in Europe from 1987 through 2005 (in ng m
implementation of the EU air quality daughter directives will further improve the trace element measurements in Europe. Trends of air concentrations of cadmium and lead at selected stations are shown in Fig. 2, while trends of atmospheric deposition for these metals are presented in Fig. 3. It should be noted that the selection of stations is different for the analysis of air concentration and precipitation data. The stations with most reliable data were selected for the analysis. They include stations in the Czech Republic (CZ0001R), Germany (DE0001R), Great Britain (GB0091R), the Netherlands (NL0009R), Slovakia (SK0004R), and Norway (NO0001R). The description of these sites and procedures for collection of samples and analytical methods used is presented in Aas and Breivik (2007). For mercury it is only Sweden that has time series that can be used for proper trend analysis. The Swedish data are shown in Fig. 4. 4. Comparison of emission trends with trends of concentrations and deposition A crucial question for policy making is to what extent the reduction of atmospheric emissions of contaminants would result in the decrease of their concentrations in the air and atmospheric deposition. Usually a comparison is made between changes of emissions in a given region and changes of concentrations modeled in this region. Models used to simulate the concentration and deposition changes use the emission data for which the reduction effect of concentrations and deposition is analyzed. Thus the
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dependence between emissions and concentration/deposition changes is clearly expected and related to the input data for the models. In this paper changes in emission estimates are compared with air concentration and precipitation measurements. The Mann–Kendall test and Sens slope estimator (Gilbert, 1987) have been used to estimate the trends at these sites. At the Norwegian site Birkenes there are precipitation measurements of lead and cadmium since 1976 and the reduction for both elements has been higher than 90%. For the other sites the reduction in precipitation has been around 45% since 1990 for both elements. The corresponding relationships in air concentrations have been more than 70% for both metals. For gaseous elemental mercury the reduction observed at the Swedish sites has been 70% since 1980. No significant trend of Hg in precipitation has been observed, using the Mann–Kendall statistical test for the precipitation measurement data between 1989 and 2005. In other papers, a downward trend is also seen in the deposition measurements. For example, Wangberg et al. (2007) observed a reduction in deposition between 10% and 30% when comparing the periods 1995–1998 and 1999–2002 for various OSPAR sites. However, as can be seen in Fig. 4, there is an increase in the deposition concentration in the last two years. A significant reduction of 29% is observed if calculating the trend from 1989 to 2003 only. The air concentration and atmospheric deposition trends for cadmium and lead for the last 2 decades can be compared with the
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Fig. 3. Change of Cd and Pb concentrations in precipitation at selected stations in Europe from 1979 through 2004 (in mg l
emission changes for these compounds. Total cadmium emissions in Europe were reduced by about 60%, and in Scandinavia about 80%. This corresponds well with the reduction of Cd concentrations in the air (about 70%). With regard to reduction of lead emissions in the same period, more than 85% of this reduction was estimated for the whole Europe, including Scandinavia. This corresponds with the reduction of more than 70% of Pb concentrations in the air. As the combustion of gasoline has been the main source of Pb emissions in Europe, these emissions enter the atmosphere close to the ground and therefore it is expected that any changes of such emissions will be clearly reflected in the changes of air concentrations. Indeed, this is confirmed in our studies. More than 85% reduction of Pb emissions and air concentrations can be noted for the Czech Republic and Slovakia (air concentrations in Fig. 2) for the last 2 decades. Somewhat lower values of Pb air concentration reductions were noted for stations in Great Britain and Germany in comparison with the expectations due to more than 85% Pb emission reduction in these countries. This can be explained by the larger contribution of Pb emissions from major stationary point sources to the air concentrations in these countries compared to the contribution from gasoline combustion. Thus, it can be concluded that the reduction trends of anthropogenic emissions of cadmium and lead in Europe are similar to the reduction trends of air concentrations of these metals during the last 2 decades.
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Somewhat different relationship has been noted for changes in emissions and precipitation. In general for Europe, 60% reduction of Cd emissions and 70% reduction of Pb emissions were met by about 45% reductions of Cd and Pb concentrations in precipitation at the studied stations during the last 2 decades. Mercury is a global contaminant with lifetime of some of its chemical forms of about 2 years. This means that the relationship between emissions and air concentrations/atmospheric deposition is less straightforward than the relationships for cadmium and lead. Taking into account the Swedish data from Fig. 4 for the last 2 decades, it can be suggested that the air concentrations of total mercury and concentrations of precipitation have decreased by a factor of 3. The European emissions of mercury have also decreased by a factor of 3 in the same period. The question appears whether this close agreement is coincidental or the impact of European emissions on European concentrations of this contaminant in the air and precipitation is very important and more important than global background in these concentrations related to the global emissions. The data for the period from 1989 through 1995 in Fig. 4 indicating a dramatic change in concentrations seem to support the notion of the high importance of the European emission impacts, much stronger than the global background. This concentration change reflects the emission change caused primarily by the switch of economies in Eastern Europe from centrally planned to market oriented in this period, leaving several industries in this region closing down, specially chemical
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Mercury in air and precip at SE0002/SE0014
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Fig. 4. Change of Hg concentrations in air (total Hg in ng m
industries. On the other hand, clearly visible increases of concentrations during the latest period of measurements from 2003 through 2005 cannot be explained by the changes of European emissions. Thus, the concentrations in that period seem to support the notion that emissions outside Europe, e.g. in Asia may have an important impact on the concentration levels in Europe (Wilson et al., 2006). This would mean that any action to reduce the Hg emissions in Europe should be coordinated with strategies for Hg emission reductions globally. However, one should be careful with taking conclusions on the basis of concentration changes measured and discussed at stations from one region only (Iverfeldt et al., 1995; Munthe et al., 2001, 2003; Slemr et al., 2003).
5. Spatial distribution of emissions and concentrations in Europe in 2005 Information on spatial distribution of emission data is needed for the development of regional policies on emission reduction as well as for modeling purposes. In this paper, the spatial distribution of emissions is used for comparison with spatial distribution of concentrations in the air and precipitation of cadmium and lead at the EMEP stations in 2005. No comparison has been made for mercury due to very low amount of data for this contaminant, available from the EMEP measurement network. Spatial distribution of cadmium and lead emissions in Europe in 2005 within the EMEP grid system of 50 km by 50 km is presented in Fig. 5. Details on the development of emission maps presented in Fig. 5 are available from Pacyna et al. (2007). These maps were prepared within the EU project ESPREME (http://espreme.ier.unistuttgart.de) by experts from the Institute of Energy Economics and the Rational Use of Energy (IER) at the University of Stuttgart, Germany. Cadmium and lead show different patterns of spatial distributions of their emissions. Cadmium is emitted primarily from point sources of emissions, such as non-ferrous metal smelters, power plants, and waste incinerators, while lead emissions come mainly from area sources, such as traffic. These clear points (grids) of emissions are indicated as hot spots on the Cd emission maps in contrast to fairly even distribution over many grids for Pb emissions. Cadmium measurements in air and precipitation follow the emission distribution fairly well with high values in Central Europe and lower concentrations in Northern Europe, as presented in
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) and precipitation (in ng l
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Fig. 6. The lowest concentrations are generally observed in northern Scandinavia, Greenland, Iceland, and the westernmost part of Europe. An increasing gradient can in general be seen southeast, but the air concentration and atmospheric deposition levels are not evenly distributed, there are some ‘‘hotspots’’ for some elements. Similar trend is observed for Pb concentrations but the concentration gradient from Central to Northern Europe is less pronounced. Good relationship between spatial distribution of emissions and concentrations in the air and precipitation for cadmium and lead indicates that the impact of emissions on air concentrations and precipitation in the emission areas is very important. Local deposition of these two contaminants seems to be quite important for assessment of the environmental impacts caused by emissions of Cd and Pb. The above conclusions are well supported by the estimates of the atmospheric supply of Cd, Pb and Hg to the Baltic Sea, carried out by EMEP as a contribution to HELCOM (http://www. emep.int/publ/helcom/2007/index.html and Bartnicki et al., 2007). Decreasing emission trends for Cd and Pb can also be confirmed by the analysis of concentration trends in mosses (Harmens et al., 2008). The concentration of lead and cadmium in mosses decreased between 1990 and 2000 by 57% and 42%, respectively. 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 significantly across Europe.
6. Future changes of emissions Information on changes of past emissions and concentrations can be used to discuss their future changes. The past changes of Cd, Pb, and Hg emissions indicate clear decrease of these emissions and suggest that future reduction is possible. Three types of scenarios were elaborated within the EU ESPREME project for the year 2010: the CAFE´ Baseline scenario with climate policies, the CAFE´ Baseline scenario without climate policies, and the CAFE´ Maximum Feasible Technological Reduction (MFTR) scenario. The CAFE´ Baseline scenario without climate policies adopts the baseline energy projection of the ‘‘European energy and transport – Trends to 2030’’ outlook of the Directorate General for Energy and Transport of the European Commission (EC, 2003) as a starting
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Fig. 5. Spatial distribution of Cd and Pb emissions in Europe in the EMEP grid of 50 km 50 km (in t grid
point. This projection does not assume any further climate measures beyond those already adopted in 2002. The implication of further climate measures is included in the CAFE´ Baseline scenario with climate policies. This projection attempts to quantify how the decarbonisation of the energy system would take place due to
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climate policies. The CAFE´ Maximum Feasible Technological Reduction scenario assumes that all measures are in place to maximally reduce or phase-out a given contaminant. The emission scenarios were estimated on the basis of information on emission factors prepared within the ESPREME project
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Pb in precipitation (µg/l)
Cd in precipitation (µg/l)
Pb in aerosols (ng/m3)
Cd in aerosols (ng/m3)
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Fig. 6. Average concentrations of Pb and Cd in the air and precipitation samples in 2005.
on availability and effectiveness of emission control and the CAFE´ statistical data for the year 2000. Both, scenario estimates and emission factors are presented on the ESPREME project website (http://espreme.ier.uni-stuttgart.de). The details are also presented in Pacyna et al. (2007). The statistical data used in the emission scenario estimates were obtained from the CAFE´ Baseline scenario with climate policies and Baseline scenario with no policies, calculated with the use of the PRIMES model version 2 (data available at http://espreme.ier.unistuttgart.de). The results of emission scenario estimates are presented in Fig. 7. The following can be concluded from these estimates: the 2010 CAFE´ Baseline scenario with no climate policies indicates the following emission reductions compared to the emissions in the year 2005: 9% for Cd, 21% for Pb and 22% for Hg, and the 2010 CAFE´ Baseline scenario with climate policies indicates an emission reduction of 15% for Cd, 25% for Pb, and 26% for Hg, compared to the emissions in the year 2005.
Implementation of the MFTR scenario will result in further emission reduction of studied trace metals compared to the emissions estimated for the two CAFE´ Baseline scenarios (with and without climate measures). The largest reductions of emissions between the years 2005 and 2010 (the MFTR scenario) are as follows: 37% for Cd, 51% for Pb, and 49% for Hg. It is difficult to assess to what extent the emission reductions mentioned above would affect the reduction of air concentrations and atmospheric deposition of cadmium, lead, and mercury in Europe in the future. This assessment can be carried out with the help of dispersion models on continental and global scale (the latter for Hg). 7. Final remarks and future research Analysis of the information on emissions of cadmium, lead, and mercury from anthropogenic sources in Europe over the last 5 decades indicates that these emissions picked in the late 1960s and the early 1970s. Later on these emissions have been in a continuous decrease until now. This decreasing trend over the last 3 decades is
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aspects of environmental contamination by cadmium, lead, and mercury. Some of these questions could be defined as follows: - to what extent do we need to reduce emissions of these contaminants? - do we have technological and non-technological measures to obtain this reduction and what will be the cost of implementation of these measures? - to what extent future emission reduction will contribute to the decrease of concentrations of these contaminants in the air and precipitation samples and what are the required concentration levels that would guarantee no harmful effects of contaminants on environment and human health?
Fig. 7. Scenarios of future emissions of Cd, Pb, and Hg in Europe (in t year Description of scenarios is given in the main text of the paper.
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partly due to the implementation of emission control equipment, such as high efficiency of de-dusting installations and flue gas desulfurization installations that remove not only sulfur dioxide but also other gaseous contaminants, such as mercury. These emission control devices were employed in various utility and industrial plants, such as power plans, smelters, cement kilns, and incinerators as a way of implementation of various environmental protection policies at local and regional level. Gradual removal of leaded additives to gasoline over the last 3 decades has been the major factor contributing to very high decrease of lead emission in Europe. Introduction and use of gasoline without lead additives have been a major policy success in Europe in combating lead contamination of environment. Another factor contributing to the emission decreases in the late 1980s and the beginning of the 1990s in Central and Eastern Europe was the economic decline in this part of Europe caused by economy transfers from centrally planned to market oriented. Past trends of Cd, Pb, and Hg concentrations in air and precipitation samples have followed closely the decrease of emissions of these metals for the last 3 decades, particularly the air concentration trend. However, it should be cautioned that only limited amount of information is available from the EMEP program on these concentrations. Therefore the results presented here can be regarded as a first step in analyzing the relationships between the emission changes and changes of concentration in the air and precipitation for cadmium, lead, and mercury. The amount of EMEP stations measuring these concentrations is increasing and therefore it is expected that more complete analysis of emissions and concentrations will be possible in the near future. An interesting feature has appeared for Hg concentrations measured in the latest years indicating some small increases in selected regions. This fact may indicate how important it is to consider mercury as a global contaminant, because emissions in other regions may and probably do affect the concentrations in the air and precipitation of this pollutant in Europe. Again, it is too early to develop any major conclusions on the basis of data presented here, but in the near future one should focus more on the impact of global emission of mercury on the contamination of the environment in Europe. So far, major conclusions were drawn in this direction on the basis of information on mercury depletion in the air over the Arctic. It is very interesting to further develop future emission scenarios and discuss to what extent these emissions would affect future concentrations of contaminants in the air and precipitation. There are a number of questions that would need to be addressed in future research that are related to environmental and economic
Major development of procedures for valuation of environmental benefits from the emission reduction of cadmium, lead, and mercury and procedures for various costs of this reduction would need to be made in order to address these questions. This means that multidisciplinary analysis of cost–benefits in relation to the reduction of cadmium, lead, and mercury emissions is going to be a very important tool for integrated assessment of drivers, pressures, and the state of the environment in Europe with regard to the contamination by these pollutants. Concentration measurements would need to be improved with regard to the coverage of station network in Europe and completeness of measurement programs at these stations. Efforts to achieve this improvement within EMEP are very important and they hold a promise of more complete knowledge of the state of the European environment with regard to contamination by trace metals (and other pollutants). A larger number of so-called ‘‘EMEP super-stations’’ measuring extended sets of parameters and chemicals (e.g. EMEP, 2006) will also contribute to this improvement of our knowledge. Improved monitoring networks are the key element in developing new policies on reduction of air contaminants. Emission estimates presented in this paper should be improved through more complete and accurate emission estimates in individual countries in Europe. There is a clear need for such improvement for both policy makers and modelers. Complete and accurate emission data are the basis for new policies on regional (e.g. EU territory) and global scale. It is understood that the estimates prepared by international experts are valuable for having the information on national emissions in the European countries as long as no better data are available from national emission experts. National emission experts are more familiar with various technical and other specificities affecting the amount of emissions from a given source or even source category in a given country. Major projections of future use of energy, transportation patterns, and industrial development are largely in place in connection with the progress of work within Intergovernmental Panel on Climate Change (IPCC), CAFE´, EU Directives and national development plans and strategies. These projects form a good basis for development of emission scenarios for various contaminants, including cadmium, lead, and mercury. One may expect lower emissions of these contaminants in the future through the implementation of various policies aiming at more efficient use of renewable energy sources for the production of electricity and heat. A number of European countries plan to have up to 20% of their energy budgets met by the use of renewable energy until the year 2020. Acknowledgements The paper was financially supported by the EU project DROPS (Contract No. FP6-2004-SSP-4-022788) and the UN ECE European Monitoring and Assessment Programme (EMEP). The authors are
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grateful to the European Commission and the UN Economic Commission for Europe for this support. The authors would like to thank Dr. Steffen Nitter of University of Stuttgart, Germany for his help in presenting emission data on maps. The authors would also like to thank Mrs. Ewa Jastrzab – Strzelecka of the Institute for Ecology of Industrial Areas (IETU) in Katowice, Poland for her support in preparing the emission scenarios. References Aas, W., Breivik, K., 2007. Heavy Metals and POP Measurements, 2004. The Norwegian Institute for Air Research Report EMEP/CCC-Report 6/2007, Kjeller, Norway. Bartnicki, J., Gusev, A., Aas, W., Fagerli, H. 2007. Atmospheric Supply of Nitrogen, Lead, Cadmium, Mercury and Dioxines/Furanes to the Baltic Sea in 2005. The Norwegian Meterological Institute, EMEP/MSC-W Technical Report 3/2007, Oslo, Norway. Chang, L.W., 1996. Toxicology of Metals. CRC Lewis Publishers, Boca Raton, FL. EC, 2003. European Energy and Transport. Trends to 2030. KO-AC-02-001-EN-C Report, European Commission, Directorate General for Energy and Transport, Luxemburg. EMEP, 2001. Manual for Sampling and Chemical Analysis. Norwegian Institute for Air Research, Report EMEP/CCC-Report 1/1995, revision 1/2001, Kjeller, Norway. Available from:
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