Critical loads and their exceedances at intensive forest monitoring sites in Europe

Intensive forest monitoring by means of harmonised methods has been conducted in Europe for more than a decade. Risks of atmospheric nitrogen and sulphur deposition are assessed by means of calculations of critical loads and their exceedances. In the present study throughfall and bulk deposition of nitrate (N-NO(3)), ammonium (N-NH(4)) and sulphate (S-SO(4)) show marked spatial patterns and temporal trends. In the period of observation (1999-2004), sulphate deposition on intensive monitoring plots decreased by about one quarter. This is in line with the reduction of S deposition by 70% since 1981 in Europe as a result of successful air pollution control politics under the Convention on Long-range Transboundary Air Pollution (CLRTAP). However, sulphate and especially nitrate and ammonium deposition were found to still exceed critical loads at many forest sites, indicating a continued need for further implementation of air pollution abatement strategies.     

Regional air pollution at a turning point

The control of transboundary air pollution in Europe has been successful. Emissions of many key pollutants are decreasing and there are signs of improvements in damaged ecosystems. The strategies under development within the CAFE programme under the European Commission and the Convention on Long-range Transboundary Air Pollution (CLRTAP), aim to take regional air pollution control a large step further, in particular with respect to small particles. In this paper we highlight the new strategies but look primarily at socioeconomic trends and climate change feedbacks that may have a significant influence on the outcome of the strategies and which so far have not been considered. In particular, we point out the influence on air quality of increased summer temperatures in Europe and of increasing emissions including international shipping, outside of Europe. Taken together the further emissions reductions in Europe and the increasing background pollution, slowly cause a greying of the Northern Hemisphere troposphere rather than the traditional picture of dominant emissions in Europe and North America ('black') with much lower emission intensities elsewhere ('white'). A hemispheric approach to further combat air pollution will become necessary in Europe and elsewhere.     

Acid rain and air pollution: 50 years of progress in environmental science and policy

Because of its serious large-scale effects on ecosystems and its transboundary nature, acid rain received for a few decades at the end of the last century wide scientific and public interest, leading to coordinated policy actions in Europe and North America. Through these actions, in particular those under the UNECE Convention on Long-range Transboundary Air Pollution, air emissions were substantially reduced, and ecosystem impacts decreased. Widespread scientific research, long-term monitoring, and integrated assessment modelling formed the basis for the policy agreements. In this paper, which is based on an international symposium organised to commemorate 50 years of successful integration of air pollution research and policy, we briefly describe the scientific findings that provided the foundation for the policy development. We also discuss important characteristics of the science–policy interactions, such as the critical loads concept and the large-scale ecosystem field studies. Finally, acid rain and air pollution are set in the context of future societal developments and needs, e.g. the UN’s Sustainable Development Goals. We also highlight the need to maintain and develop supporting scientific infrastructures.

     

First Europe-wide correlation analysis identifying factors best explaining the total nitrogen concentration in mosses

In this study, the indicative value of mosses as biomonitors of atmospheric nitrogen (N) depositions and air concentrations on the one hand and site-specific and regional factors which explain best the total N concentration in mosses on the other hand were investigated for the first time at a European scale using correlation analyses. The analyses included data from mosses collected from 2781 sites across Europe within the framework of the European moss survey 2005/6, which was coordinated by the International Cooperative Programme on Effects of Air Pollution on Natural Vegetation and Crops (ICP Vegetation). Modelled atmospheric N deposition and air concentration data were calculated using the Unified EMEP Model of the European Monitoring and Evaluation Programme (EMEP) of the Convention on Long-range Transboundary Air Pollution (CLRTAP). The modelled deposition and concentration data encompass various N compounds. In order to assess the correlations between moss tissue total N concentrations and the chosen predictors, Spearman rank correlation analysis and Classification and Regression Trees (CART) were applied. The Spearman rank correlation analysis showed that the total N concentration in mosses and modelled N depositions and air concentrations are significantly correlated (0.53 ≤ r_s ≤ 0.68, p < 0.001). Correlations with other predictors were lower than 0.55. The CART analysis indicated that the variation in the total N concentration in mosses was best explained by the variation in NH₄⁺ concentrations in air, followed by NO₂ concentrations in air, sampled moss species and total dry N deposition. The total N concentrations in mosses mirror land use-related atmospheric concentrations and depositions of N across Europe. In addition to already proven associations to measured N deposition on a local scale the study at hand gives a scientific prove on the association of N concentration in mosses and modelled deposition at the European scale.     

An introduction to critical loads

The critical loads approach to emission controls of gaseous pollutants is a concept with a short but eventful history. Despite difficulties with definitions and agreed values, its acceptance within the UN-ECE Convention on Long Range Transboundary Air Pollution has provided the impetus for developing methods to put critical loads to a practical use-the revision of the UNECE emission protocols for sulphur and nitrogen. Methodologies first focus upon quantifying a pollutant threshold at which harmful effects occur on particular sensitive receptors (usually biological species). This threshold is known as the critical load for deposited pollutants, and as the critical level for gaseous pollutants acting on receptors. To calculate a critical load, biological effects are usually 'translated' to critical chemical values, e.g. harmful effects on fish 'translate' to alkalinity or aluminium concentrations in water; thus, critical load calculations may be based upon the chemistry of a system. Such calculations may be performed using simple, steady-state models, whilst the use of more complex, dynamic models provides an insight into the past and future trends. Maps of critical loads can be drawn using calculated values, and maps of pollutant deposition data will then show geographical areas where critical loads are exceeded. Spatial emission-deposition models can identify sources contributing to areas of excess loads and quantify necessary emission reductions. Optimization procedures applied to such models can derive abatement strategies related to economic costs and critical load effects. The critical load calculations may also be used to underpin the setting of target loads; these are pollutant loads, determined by political agreement, which take account of social, economic and political considerations.     

Reactive nitrogen and public policies for environmental protection

A core goal of both US and European pollution control policies has been to establish rules and regulations pertaining to the movement of reactive-nitrogen (Nr) through the environment. This is manifest in US federal legislation such as the Clean Air Act Amendments and the Clean Water Act Amendments and in various protocols of the United Nations Economic Commission for Europe (UNECE) and its Convention on Long-Range Transboundary Air Pollution (CLRTAP). In this paper, we begin by reviewing the two US laws and their effectiveness and make some comparisons with the approaches used mainly in Europe by the UNECE and CLRTAP. Next we use the Mississippi drainage/Gulf of Mexico hypoxia case study to highlight the importance of applying a "systems approach" to address the reactive nitrogen problem at the regional scale. After briefly posing a number of unanswered questions related to nitrogen control policies, we conclude by sketching a blueprint for future actions related to the development of improved policies to regulate reactive nitrogen.     

Regional scale evidence for improvements in surface water chemistry 1990-2001

The main aim of the international UNECE monitoring program ICP Waters under the Convention of Long-range Transboundary Air Pollution (CLRTAP) is to assess, on a regional basis, the degree and geographical extent of the impact of atmospheric pollution, in particular acidification, on surface waters. Regional trends are calculated for 12 geographical regions in Europe and North America, comprising 189 surface waters sites. From 1990-2001 sulphate concentrations decreased in all but one of the investigated regions. Nitrate increased in only one region, and decreased in three North American regions. Improvements in alkalinity and pH are widely observed. Results from the ICP Waters programme clearly show widespread improvement in surface water acid-base chemistry, in response to emissions controls programs and decreasing acidic deposition. Limited site-specific biological data suggest that continued improvement in the chemical status of acid-sensitive lakes and streams will lead to biological recovery in the future.     

Soil quality and vulnerability in a Mediterranean natural ecosystem of Central Italy

Wet and dry atmospheric depositions and soil chemical and microbiological properties were determined in a Mediterranean natural ecosystem of Central Italy near Rome (Castelporziano Estate). The monitoring of depositions permitted us to quantify the exceedances of S and N compounds (expressed as eqH(+)ha(-1)year(-1)) over the critical loads of acidity. Critical loads, i.e. the quantity of a substance which a part of the environment can tolerate without adverse effects occurring, were determined adopting the level 0 methodology following the UN/ECE Convention on Long-range Transboundary Air Pollution. Deposition data were available for the period 1992-1997, and acidity exceedances were referred to the main vegetation types present in the area. Results showed that most part of the Estate has a medium degree of vulnerability to acidification, and the corresponding risk of acidification deriving from the exceedances of atmospheric deposition was rather low. The study of soil chemical and microbiological properties included mainly total soil organic carbon (SOC), microbial biomass-C, biomass-C/SOC, soil respiration, and metabolic quotient (qCO2). Soil organic C metabolism has been discussed on the basis of the results from eight sampling sites.     

Forest health status in the Carpathian Mountains over the period 1997-2001

The results of forest health status assessments in the Carpathian Mountains from the monitoring networks developed by the European Union Scheme on the Protection of Forest Against Atmospheric Pollution (EU Scheme) and International Co-operative Programme on Assessment and Monitoring of Air Pollution Effects on Forests (ICP-Forests), have led to a better understanding of the impact of air pollution and other stressors on forests at the regional scale. During the period 1997-2001, forests in the Carpathian Mountains were severely affected by air pollution and natural stresses with 29.7-34.9% of the trees included in defoliation classes 2-4. The broadleaves were slightly healthier than the conifers, and European beech (Fagus sylvatica) was the least affected species. Norway spruce (Picea abies) has poor health status, with 42.9-46.6% of the trees damaged (2-4% defoliation classes). Silver fir (Abies alba) damage was also high, with 46.0-50.9% in defoliation classes 2-4. Pines (primarily Pinus sylvestris) were the least affected of the conifers, with 24.9-33.8% in defoliation classes 2-4. The results from the transnational networks (16 x 16 km) show that the Carpathian forests are slightly more damaged than the average for the entire Europe. The correlative studies performed in individual European countries show the relationships between air pollution stressors with trends in defoliation and a possible effect of natural stresses at each site. More specific, effects of tree age, drought, ozone and acid deposition critical level exceedances were demonstrated to affect crown condition.     

European abatement of surface ozone in a global perspective

EU's programme Clean Air for Europe (CAFE) is presently revising the policy on air quality which will lead to the adoption of a thematic strategy on air pollution under the Sixth Environmental Action Programme by mid-2005. For the abatement of surface ozone it is becoming evident that processes outside European control will be crucial for meeting long-term aims and air quality guidelines in Europe in the future. Measurements and modelling results indicate that there is a strong link between climate change and surface ozone. A warmer and dryer European climate is very likely to lead to increased ozone concentrations. Furthermore, increased anthropogenic emissions in developing economies in Asia are likely to raise the hemispheric background level of ozone. A significant increase in the background concentration of ozone has been observed at several sites in Northern Europe although the underlying causes are not settled. The photochemical formation of tropospheric ozone from increased concentrations of methane and CO may also lead to a higher ozone level on a global scale. Gradually, these effects may outweigh the effect of the reduced European ozone precursor emissions. This calls for a global or hemispheric perspective in the revision of the European air quality policy for ozone.     

Man-made chemicals found in remote areas of the world: the experimental definition for POPs

Members of the United Nations Economic Commission for Europe (UN-ECE) signed a legally binding protocol on persistent organic pollutants (POPs) in February 1998 under the Convention on Long-Range Transboundary Air Pollution. A treaty that intends to control the production, import, export, disposal and use of toxic chemicals that persist for decades in the environment has been formally signed at a conference in May 2001 in Stockholm. The 2001 POP treaty, like the 1998 LRTAP POP protocol, contains a provision on adding further chemicals to the initial group of twelve or fifteen. The occurrence of a compound or a group of compounds in so called remote and pristine areas, e.g. in the Artic or in the Southern Hemisphere, proves its stability under the chemical and biological conditions of the environment. Compounds identified in this way, in samples taken primarily in very remote regions of the planet, are classified by their environmental fate and global distribution as persistent organic pollutants (POPs), regardless of any political assessments.     

Evidence of ozone-induced adverse effects on crops in the Mediterranean region

The impacts of ambient ozone pollution on crops in the Mediterranean countries have been recorded regularly in the so-called “grey literature” of UN/ECE Workshop Reports for the Convention on Long-range Transboundary Air Pollution, and less frequently in the peer-reviewed literature. This short communication reviews such records and shows that ambient ozone episodes have been reported to cause visible injury on 24 agricultural and horticultural crops grown in commercial fields including three of the most important crops in the region (wheat, maize, and grapevine). On one occasion, the damage was so extensive that complete crop loss occurred in commercial glasshouses of Butterhead lettuce in one area of Greece. Experiments with open-top chambers have indicated that ambient ozone caused 17–39% yield loss in crops such as wheat, bean, watermelon and tomato. The applicability of the long-term critical level of ozone described by Fuhrer et al. (Environ. Pollut. 97 (1997) 91) for the Mediterranean areas is also considered.     

Sulfur deposition simulations over China, Japan, and Korea: a model intercomparison study for abating sulfur emission

In response to increasing trends in sulfur deposition in Northeast Asia, three countries in the region (China, Japan, and Korea) agreed to devise abatement strategies. The concepts of critical loads and source?Creceptor (S?CR) relationships provide guidance for formulating such strategies. Based on the Long-range Transboundary Air Pollutants in Northeast Asia (LTP) project, this study analyzes sulfur deposition data in order to optimize acidic loads over the three countries. The three groups involved in this study carried out a full year (2002) of sulfur deposition modeling over the geographic region spanning the three countries, using three air quality models: MM5-CMAQ, MM5-RAQM, and RAMS-CADM, employed by Chinese, Japanese, and Korean modeling groups, respectively. Each model employed its own meteorological numerical model and model parameters. Only the emission rates for SO₂ and NO_x obtained from the LTP project were the common parameter used in the three models. Three models revealed some bias from dry to wet deposition, particularly the latter because of the bias in annual precipitation. This finding points to the need for further sensitivity tests of the wet removal rates in association with underlying cloud?Cprecipitation physics and parameterizations. Despite this bias, the annual total (dry plus wet) sulfur deposition predicted by the models were surprisingly very similar. The ensemble average annual total deposition was 7,203.6?±?370 kt S with a minimal mean fractional error (MFE) of 8.95?±?5.24?% and a pattern correlation (PC) of 0.89?C0.93 between the models. This exercise revealed that despite rather poor error scores in comparison with observations, these consistent total deposition values across the three models, based on LTP group's input data assumptions, suggest a plausible S?CR relationship that can be applied to the next task of designing cost-effective emission abatement strategies.     

Air quality management in Portugal: example of needs and available tools

The Framework Directive (FWD) and the proposed Daughter Directives are the newest legislative instruments concerning a new political strategy and air quality management approach for Europe. Additionally, the member countries of the United Nations Economic Commission for Europe have included the concepts of critical load and level for planning air pollution abatement strategies and as a base of international agreements concerning limitation of the emissions of air pollutants. These concepts imply an accurate knowledge about pollutants deposition fluxes. The paper describes the main needs and the tools available to define a strategy of air quality management in Portugal. Two study cases are presented: (1) extensive monitoring plan to assess the impact of an urban incinerator plant; and (2) contribution to a methodology to estimate critical levels for a coastal region in Portugal. These different approaches allowed illustrating the complexity of the implementation of an air pollution management strategy.     

An application and review of the critical load concept to the soils of northern England

In common with other member states of UN-ECE, maps of critical loads of transboundary air pollutants are to be produced in the UK for different receptor (waters, soils and vegetation) types. These maps will be used as a tool for assessing different deposition scenarios with proposed pollution abatement strategies. This paper presents the methodology, results and a discussion of the principles used in applying critical loads of sulphur as a pilot study for soils in northern England. For the study area, critical load classes for soils vary with geology, drift cover and slope/elevation. The area of soils in which the critical load is exceeded varies significantly according to the type of deposition data utilised.     

Reduced European emissions of S and N--effects on air concentrations, deposition and soil water chemistry in Swedish forests

Changes in sulphur and nitrogen pollution in Swedish forests have been assessed in relation to European emission reductions, based on measurements in the Swedish Throughfall Monitoring Network. Measurements were analysed over 20 years with a focus on the 12-year period 1996 to 2008. Air concentrations of SO₂ and NO₂, have decreased. The SO₄-deposition has decreased in parallel with the European emission reductions. Soil water SO₄-concentrations have decreased at most sites but the pH, ANC and inorganic Al-concentrations indicated acidification recovery only at some of the sites. No changes in the bulk deposition of inorganic nitrogen could be demonstrated. Elevated NO₃-concentrations in the soil water occurred at irregular occasions at some southern sites. Despite considerable air pollution emission reductions in Europe, acidification recovery in Swedish forests soils is slow. Nitrogen deposition to Swedish forests continues at elevated levels that may lead to leaching of nitrate to surface waters.     

A Dynamic Air Resource Management Program,City of Chicago

A review of air pollution control activities since 1881, and the current needs to change from a smoke abatement to an air resource management program are presented. The rapid and dynamic transition made by the City of Chicago since 1962 in its air pollution control activities are explored in terms of organizational changes, training of professional and nonprofessional personnel, ambient air quality measurements, emission inventory of commercial and industrial operations directed toward issuance of certificates of operation, evaluation of health effects and materials damage, modifications to the municipal code, and the interrelationship of air pollution control activities with urban planning and the regional complex. The multidiscipline Public Health Service, Division of Air Pollution, Technical Assistance program initiated in October 1962, and planned for a period of five years, is discussed. The achievements, particularly since 1962, in the many faceted Chicago air resource management program together with some of its longrange plans are delineated.     

The long range transport of ozone within Europe and its control

It is widely accepted that the ozone concentrations experienced during photochemical episodes over large areas of Europe may exceed levels at which adverse environmental effects could be expected. These peak ozone concentrations can be reduced by controlling atmospheric emissions of the hydrocarbon and nitrogen oxide precursors. For ozone control to be successful over the spatial scale of Europe, long term international cooperation is required in the formulation of emission abatement strategies. A significant barrier to rapid progress has been the complexity of the processes that describe ozone formation. Highly sophisticated computer models of chemistry and transport have, up to now, been the only means to study the impact of abatement strategies. An alternative approach has been adopted here involving the development of a simplified long range transport model for ozone based on the analysis of over 60 experimental runs of a photochemical trajectory model applied to a wide range of hydrocarbon-nitrogen oxide emission combinations. Using the ozone-precursor relationship obtained, it has been possible to examine various policy options in the European context. Although taken together, three illustrative emission control scenarios reduce NO(x) and hydrocarbon emissions substantially through controls on motor vehicle exhaust, large combustion plant and solvent usage, a significant potential for photochemical ozone formation and long range transport may still remain after their implementation. The extents of precursor emission abatement that will be required, if the potential for ozone formation is to be reduced below published air quality criteria guidelines or critical levels, have been determined for each European country. The implied reductions in NO(x) and hydrocarbons relative to current levels amount to between 50 and 90%.     

Changes in the Chemistry of Small Irish lakes

A re-survey of acid-sensitive lakes in Ireland (initial survey 1997) was carried out during spring 2007 (n = 60). Since 1997, atmospheric emissions of sulfur dioxide and deposition of non-marine sulfate (SO₄ ²⁻) in Ireland have decreased by ~63 and 36%, respectively. Comparison of water chemistry between surveys showed significant decreases in the concentration of SO₄ ²⁻, non-marine SO₄ ²⁻, and non-marine base cations. In concert, alkalinity increased significantly; however, no change was observed in surface water pH and total aluminum. High inter-annual variability in sea salt inputs and increasing (albeit non-significant) dissolved organic carbon may have influenced the response of pH and total aluminum (as ~70% is organic aluminum). Despite their location on the western periphery of Europe, and dominant influence from Atlantic air masses, the repeat survey suggests that the chemistry of small Irish lakes has shown a significant response to reductions in air pollution driven primarily by the implementation of the Gothenburg Protocol under the UNECE Convention on Long-Range Transboundary Air Pollution.     

Assessing the Impacts of Long-Range Sulfur and Nitrogen Deposition on Arctic and Sub-Arctic Ecosystems

For more than a decade, anthropogenic sulfur (S) and nitrogen (N) deposition has been identified as a key pollutant in the Arctic. In this study new critical loads of acidity (S and N) were estimated for terrestrial ecosystems north of 60° latitude by applying the Simple Mass Balance (SMB) model using two critical chemical criteria (Al/Bc = 1 and ANC_le = 0). Critical loads were exceeded in large areas of northern Europe and the Norilsk region in western Siberia during the 1990s, with the more stringent criterion (ANC_le = 0) showing the larger area of exceedance. However, modeled deposition estimates indicate that mean concentrations of sulfur oxides and total S deposition within the Arctic almost halved between 1990 and 2000. The modeled exceeded area is much reduced when currently agreed emission reductions are applied, and almost disappears under the implementation of maximum technically feasible reductions by 2020. In northern North America there was no exceedance under any of the deposition scenarios applied. Modeled N deposition was less than 5 kg ha⁻¹ y⁻¹ almost across the entire study area for all scenarios; and therefore empirical critical loads for the eutrophying impact of nitrogen are unlikely to be exceeded. The reduction in critical load exceedances is supported by observed improvements in surface water quality, whereas the observed extensive damage of terrestrial vegetation around the mining and smelter complexes in the area is mainly caused by direct impacts of air pollution and metals.