Critical loads and steady-state chemistry for streams in the state of Maryland

The critical loads to streams, steady-state stream chemistry and catchment chemical weathering rate in 73 catchments has been determined in the state of Maryland, USA. It was calculated with the PROFILE model from chemical limits for biological indicators, soil mineralogy, soil texture, annual average temperature, average soil moisture, net long-term uptake of base cations and nitrogen to the vegetation, annual precipitation and runoff and deposition of sulphur and nitrogen precursors of acid deposition. The results show a full range of critical loads from very low values in the sensitive catchments of western Maryland and the Coastal Plain on the Chesapeake Bay, to insensitive catchments in the Fredrick Valley and Ridge and the Piedmont plain. The critical loads will be used as an input to an integrated regional assessment of the quantitative sensitivity of streams to acid rain, and the assessment of regional stream alkalinity response to different abatement strategies. The mapping of steady-state stream chemistry indicates that streams in Maryland are still acidfying under the present deposition load. Land-use seems to play an important role in maintaining neutral pH in many of the streams of Maryland.     

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.     

Modelling and mapping long-term risks due to reactive nitrogen effects: an overview of LRTAP convention activities

Long-range transboundary air pollution has caused severe environmental effects in Europe. European air pollution abatement policy, in the framework of the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP Convention) and the European Union Clean Air for Europe (CAFE) programme, has used critical loads and their exceedances by atmospheric deposition to design emission abatement targets and strategies. The LRTAP Convention International Cooperative Programme on Modelling and Mapping Critical Loads and Levels and Air Pollution Effects, Risks and Trends (ICP M&M) generates European critical loads datasets to enable this work. Developing dynamic nitrogen flux models and using them for a prognosis and assessment of nitrogen effects remains a challenge. Further research is needed on links between nitrogen deposition effects, climate change, and biodiversity.     

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.     

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.     

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.     

Forest ecosystems and the changing patterns of nitrogen input and acid deposition today and in the future based on a scenario

A global assessment of the impact of the anthropogenic perturbation of the nitrogen and sulfur cycles on forest ecosystems is carried out for both the present-day [1980-1990] and for a projection into the future [2040-2050] under a scenario of economic development which represents a medium path of development according to expert guess [IPCC IS92a]. Results show that forest soils will receive considerably increasing loads of nitrogen and acid deposition and that deposition patterns are likely to change. The regions which are most prone to depletion of soils buffering capacity and supercritical nitrogen deposition are identified in the subtropical and tropical regions of South America and Southeast Asia apart from the well known 'hotspots' North-Eastern America and Central Europe. The forest areas likely to meet these two risks are still a minor fraction of the global forest ecosystems, though. But the bias between eutrophication and acidification will become greater and an enhanced growth triggered by the fertilizing effects of increasing nitrogen input cannot be balanced by the forest soils nutrient pools. Results show increasing loads into forest ecosystems which are likely to account for 46% higher acid loads and 36% higher nitrogen loads in relation to the 1980-1990 situation. Global background deposition of up to 5 kg N ha-1 a-1 will be exceeded at more than 25% of global forest ecosystems and at more than 50% of forest ecosystems on acid sensitive soils. More than 33% of forest ecosystems on acid sensitive soils will receive acid loads which exceeds their buffering capacity. About 25% of forest areas with exceeded acid loads will receive critical nitrogen loads.     

Nitrogen critical loads using biodiversity-related critical limits

Critical loads are widely used in the effects-based assessment of emission reduction policies. While the impacts of acidification have diminished, there is increasing concern regarding the effects of nitrogen deposition on terrestrial ecosystems. In this context much attention has been focussed on empirical critical loads as well as simulations with linked geochemistry-vegetation models. Surprisingly little attention has been paid to adapt the widely used simple mass balance approach. This approach has the well-established benefit of easy regional applicability, while incorporating specified critical chemical criteria to protect specified receptors. As plant occurrence/biodiversity is related to both the nutrient and acidity status of an ecosystem, a single abiotic factor (chemical criterion) is not sufficient. Rather than an upper limit for deposition (i.e., critical load), linked nutrient nitrogen and acidity chemical criteria for plant occurrence result in an ‘optimal’ nitrogen and sulphur deposition envelope.     

Acidification in developing countries: ecosystem sensitivity and the critical load approach on a global scale

Acidification represents a growing threat to certain developing country ecosystems in tropical and subtropical climates. A methodology investigating the extent of acidification risks from sulfur emissions on a global scale is presented. Atmospheric transfer models have been used to calculate transfer and deposition of sulfur (using emissions for 1990 and a projection for 2050) and alkaline soil dust. A method to derive the relative sensitivity of terrestrial ecosystems is explained and preliminary critical load values are assigned. A range of values for critical loads and base cation deposition have been used to investigate uncertainty in maps depicting the excess of deposition above critical loads. These show an increasing risk of acidification in 2050 in extended regions of southern and eastern Asia, as well as parts of southern Africa, in comparison to 1990. Certain areas, especially in Asia, are shown at risk even when high values of critical load and base cation deposition are used.     

Considerations of uncertainty in setting critical loads of acidity of soils: the role of weathering rate determination

The concept of critical loads has been generally accepted throughout Europe, and increasingly in Asian countries and the rest of the world, as providing the data which forms the basis for international negotiations on abatement strategies for emissions of acidifying pollutants. Central to the determination of quantitative critical loads of acidity for forests (and other ecosystems) is the rate at which the minerals in the soil weather or dissolve. Seven methods for determining these rates on a regional basis for the production of critical load maps have been suggested by the official bodies which are responsible for co-ordinating the European critical load mapping efforts. These methods are largely correlations which require a knowledge of the soil parent material and/or the soil mineralogy. The purpose of this paper is to review these weathering rate calculation methods and to assess whether it is currently possible to calculate numerically accurate critical loads for the production of regional critical load maps. A consideration of the data used to generate these methods and comparisons of the weathering rates calculated using various methods leads to the conclusion that at present it is not. Further work is needed to develop and maintain the initial credibility of critical loads both scientifically and as an aid to policy decisions.     

Nitrogen sources to watersheds and estuaries: role of land cover mosaics and losses within watersheds

Across most of the World's coastal zone there has been a geographic transition from naturally vegetated to human-altered land covers, both agricultural and urban. This transition has increased the nitrogen loads to coastal watersheds, and from watersheds to receiving estuaries. We modeled the nitrogen entering the watershed of Waquoit Bay, Massachusetts, and found that as the transition took place, nitrogen loads to watersheds increased from 1938 to 1990. The relative magnitude of the contribution by wastewater, fertilizers, and atmospheric deposition depends on the land cover mosaics of a watershed. Atmospheric deposition was the major input to the watershed surface during this period, but because of different rates of loss within the watershed. wastewater became the major source of nitrogen flowing from the watershed to the receiving estuaries. Atmospheric deposition prevails in watersheds dominated by natural vegetation such as forests, but wastewater may become a dominant source in watersheds where urbanization increases. Increased nitrogen loads resulting from conversion of natural to human-altered watershed surfaces create eutrophication of receiving waters, with attendant changes in water quality, and marked shifts in the flora and food webs of the affected estuaries. Management efforts for restoration of eutrophied estuaries require maintenance of forested land, and control of wastewater and fertilizer inputs, the major terms in most affected places subject to local management. Wastewater and fertilizer nitrogen derive from within the watershed, which means local measures may effectively be used to control eutrophication of receiving waters.     

Reduction of Baltic Sea Nutrient Inputs and Allocation of Abatement Costs Within the Baltic Sea Catchment

The Baltic Sea Action Plan (BSAP) requires tools to simulate effects and costs of various nutrient abatement strategies. Hierarchically connected databases and models of the entire catchment have been created to allow decision makers to view scenarios via the decision support system NEST. Increased intensity in agriculture in transient countries would result in increased nutrient loads to the Baltic Sea, particularly from Poland, the Baltic States, and Russia. Nutrient retentions are high, which means that the nutrient reduction goals of 135 000 tons N and 15 000 tons P, as formulated in the BSAP from 2007, correspond to a reduction in nutrient loadings to watersheds by 675 000 tons N and 158 000 tons P. A cost-minimization model was used to allocate nutrient reductions to measures and countries where the costs for reducing loads are low. The minimum annual cost to meet BSAP basin targets is estimated to 4.7 billion €.     

An empirical map of critical loads of acidity for soils in Great Britain

The method used to produce a critical load map of acidity for soils in Great Britain is described. Critical loads were assigned to the dominant soil in each 1 km grid square of the UK national grid. Mineral soils were assigned a critical load based on mineralogy and chemistry, using approaches appropriate to UK conditions. Critical loads for peat soils are based primarily on a maximum acceptable reduction of peat pH, and results from laboratory equilibration studies. The map shows that soils with small critical loads (<0.5 kmol_c ha⁻¹ year⁻¹) i.e. highly sensitive to acidic deposition, dominate in the north and west of Britain; the south and east are dominated by soils with large critical loads, with small areas of more sensitive soils associated with sandy soil-forming materials. A modified critical load map illustrates the potential impact of agricultural liming on soil critical loads.     

Comparison among model estimates of critical loads of acidic deposition using different sources and scales of input data

The critical load (CL) of acidic atmospheric deposition represents the load of acidity deposited from the atmosphere to the earth’s surface at which harmful acidification effects on sensitive biological receptors are thought to occur. In this study, the CL for forest soils was estimated for 27 watersheds throughout the United States using a steady-state mass balance approach based on both national and site-specific data and using different approaches for estimating base cation weathering. Results suggested that the scale and source of input data can have large effects on the calculated CL and that the most important parameter in the steady-state model used to estimate CL is base cation weathering. These results suggest that the data and approach used to estimate weathering must be robust if the calculated CL is to be useful for its intended purpose.     

From critical levels to critical loads for ozone: a discussion of a new experimental and modelling approach for establishing flux-response relationships for agricultural crops and native plant species

Present critical levels for ozone (O3) for protecting vegetation against adverse effects are based on exposure-response relationships mainly derived from open-top chamber experiments and are expressed as an Accumulated exposure Over a Threshold of 40 ppb (AOT40). In that context with a revision of the UN (United Nations)-ECE (Economic Commission for Europe) Gothenburg protocol, AOT40 values should be replaced by flux-oriented quantities, i.e. in the end by critical loads. At present, the database for the derivation of critical loads for O3 is extremely inadequate. Furthermore, the currently available flux-response relationships are also derived from open-top chamber experiments. The use of a relationship for spring wheat in a risk assessment for an agricultural site in Hesse, Germany, demonstrates in principle, the applicability of the critical load concept for O3. Comparisons of diurnal variation of stomatal uptake and AOT40 showed that a major part of toxicologically effective stomatal uptake occurred before noon whereas the AOT40 values were dominated by the O3 concentrations during afternoon. In other words, the AOT40 exposure index do not adequately address the O3 burden during hours when plants are sensitive to O3 uptake. However, due to the differences in radiation, air temperature and humidity between the chamber and the ambient microclimates, a derivation of flux-response relationships from chamber experiments is likely to be questionable, especially for species rich ecosystems: Here, without any changes in the pollution climate, significant modifications of species composition as well as an earlier beginning of the growing season has been previously observed. To overcome the problems associated with chamber-derived flux-response relationships, a new experimental and modelling concept, was developed. The approach, briefly described in this paper, combines methods in air pollution toxicology and micrometeorology. As an analogy to the free-air fumigation concept, O3 is released into the air by an injection system above the plant canopy. The assessment of dispersion and surface deposition of O3 released is based on Lagrangian trajectory modelling. Depending on wind direction and velocity, atmospheric stratification and surface roughness, without any disturbance of the microclimate and micrometeorology, several sub-areas can be identified around the source position with differing deposition rates above the ambient level. Taking into account the actual O3 background deposition, deposition rates and vegetation responses observed in these sub-areas can easily be used to derive flux-effect relationships under ambient conditions and more realistic limiting values to protect our environment.     

Soil sensitivity to acidification in Asia: status and prospects

Exceedance of steady-state critical loads for soil acidification is consistently found in southern China and parts of SE Asia, but there is no evidence of impacts outside of China. This study describes a methodology for calculating the time to effects for soils sensitive to acidic deposition in Asia under potential future sulfur (S), nitrogen (N), and calcium (Ca) emission scenarios. The calculations are matched to data availability in Asia to produce regional-scale maps that provide estimates of the time (y) it will take for soil base saturation to reach a critical limit of 20% in response to acidic inputs. The results show that sensitive soil types in areas of South, Southeast, and East Asia, including parts of southern China, Burma, Hainan, Laos, Thailand, Vietnam, and the Western Ghats of India, may acidify to a significant degree on a 0-50 y timescale, depending on individual site management and abiotic and biotic characteristics. To make a clearer assessment of risk, site-specific data are required for soil chemistry and deposition (especially base cation deposition); S and N retention in soils and ecosystems; and biomass harvesting and weathering rates from sites across Asia representative of different soil and vegetation types and management regimes. National and regional assessments of soils using the simple methods described in this paper can provide an appreciation of the time dimension of soil acidification-related impacts and should be useful in planning further studies and, possibly, implementing measures to reduce risks of acidification.     

Estimates of critical acid loads and exceedances for forest soils across the conterminous United States

Concern regarding the impacts of continued nitrogen and sulfur deposition on ecosystem health has prompted the development of critical acid load assessments for forest soils. A critical acid load is a quantitative estimate of exposure to one or more pollutants at or above which harmful acidification-related effects on sensitive elements of the environment occur. A pollutant load in excess of a critical acid load is termed exceedance. This study combined a simple mass balance equation with national-scale databases to estimate critical acid load and exceedance for forest soils at a 1-km(2) spatial resolution across the conterminous US. This study estimated that about 15% of US forest soils are in exceedance of their critical acid load by more than 250eqha(-1)yr(-1), including much of New England and West Virginia. Very few areas of exceedance were predicted in the western US.     

Acid rain and acidification in China: the importance of base cation deposition

Acid deposition has been recognized as a serious environmental problem in China. Most acid deposition studies have focused on sulfur deposition and the pH of precipitation. However, as high concentration of alkaline dust is an important feature of the atmosphere in large parts of China, base cation deposition must be taken into account when discussing possible effects on soils and vegetation from acid deposition. We estimate the deposition of sulfur as well as calcium, i.e. the dominating anion and cation, on a regional scale in China using data both from measurements and modeling. The ratio of sulfur/calcium in deposition is then used as an indicator for identifying areas where deposition acidity exceeds alkalinity, and where soils may be at risk to acidification. The dynamic soil acidification model MAGIC is applied with data from two sites receiving high deposition loads in southwest China. The model predictions indicate that considerable soil acidification has been going on for the last decades due to acid deposition inputs. Effects on the spatial distribution of acidic deposition in China, using different future deposition scenarios, are illustrated. As the size of the anthropogenic fraction of the base cation deposition is unknown, different possible future trends in calcium deposition were used. Soil response, according to the model, using different combinations of sulfur and calcium deposition scenarios is shown. Applying the most strict measures to reduce sulfur emission will almost eliminate the acid deposition problem; however, such a scenario is not economically feasible in the short term. A strict, but possibly realistic, future scenario for sulfur may be enough to keep the situation at the present level, assuming only moderate reductions in calcium deposition. With large decreases in base cation deposition, increased soil acidification can be expected even with considerable sulfur emission reductions.     

Systematic comparison of ILWAS, MAGIC, and ETD watershed acidification models: 3. Mass balance budgets for acid neutralizing capacity

Three watershed acidification models-ILWAS, MAGIC, and ETD-were quantitatively compared to determine model structural differences by using a combination of input mapping and ANC mass balance budgets. Input mapping is a set of rules and algorithms to ensure that consistent input values were simultaneously derived for all three models. ANC budget analysis under current SO4(2-) deposition and a 70% reduction in SO4(2-) deposition allows examination of the relative importance of biogeochemical processes in affecting predictions of ANC or predicted changes in ANC. Model inputs were based on two dissimilar watersheds having characteristics typical of watersheds in the northeastern US. After mapping inputs, the three models predicted values of outflow ANC fluxes that were similar among the models for each watershed and deposition scenario. Within each watershed, the changes in outflow ANC fluxes between the scenarios were similar for the three models. Terrestrial weathering was the major source of ANC for all three models for both watersheds and deposition scenarios. The contributions of other processes to the ANC of the two watersheds were, under certain conditions, model-specific. Cation exchange was responsible for changes in ANC when deposition decreased for the three models. Other processes responsible for changes in ANC between scenarios were SO4(2-) sorption (for MAGIC) and in-lake weathering (for ETD). The processes responsible for the change in ANC from a change in deposition (cation exchange, SO4(2-) sorption, and in-lake weathering) were different from the processes contributing to the absolute ANC for a given deposition scenario (terrestrial weathering). The budget analysis complements an earlier Monte Carlo analysis that showed that the three models are structurally different and that predictions viewed on a relative scale are more similar than absolute scale predictions.     

Use of historical assessment for evaluation of process-based model projections of future environmental change: Lake acidification in the Adirondack mountains, New York, USA

Because of the considerable uncertainties associated with modeling complex ecosystem processes, it is essential that every effort be made to test model performance prior to relying on model projections for assessment of future surface water chemical response to environmental perturbation. Unfortunately, long-term chemical data with which to validate model performance are seldom available. The authors present here an evaluation of historical acidification of lake waters in the northeastern United States, and compare historical changes in a set of lakes to hindcasts from the same watershed model (MAGIC) used to estimate future changes in response to acidic deposition. The historical analyses and comparisons with MAGIC model hindcasts and forecasts of acid-base response demonstrate that the acidic and low-ANC lakes in this region are responsive to strong acid inputs. However, the model estimates suggest lakewater chemistry is more responsive to atmospheric inputs of sulfur than do the estimates based on paleolimnological historical analyses. A 'weight-of-evidence approach' that incorporates all available sources of information regarding acid-base response provides a more reasonable estimate of future change than an approach based on model projections alone. The results of these analyses have important implications for predicting future surface water chemical change in response to acidic deposition, establishing critical loads of atmospheric pollutants, and other environmental assessment activities where natural variation often exceeds the trends under investigation (high noise-to-signal ratio). Under these conditions, it is particularly important to evaluate future model projections in light of historical trends data.