The Link Between the Exceedance of Acidity Critical Loads for Freshwaters,Current Chemical Status and Biological Damage: A Re-Interpretation

Critical loads have for several years been employed bypolicymakers to aid in the development of strategies for aciddeposition abatement. They provide an effects-based approachwhereby an acid deposition flux greater than the critical load(known as critical load exceedance) implies that long-termharmful effects on a selected target organism will occur.Implicit in this approach are two assumptions: first, theexceedance of a critical load will harm the target organism,and second, the severity of biological impact is related to themagnitude of exceedance. However, static models give noindication of when the predicted damage might occur. One suchmodel, the Steady-State Water Chemistry (SSWC) model, employs aseries of empirical relationships to derive the pre-industrial,baseline leaching rate of base cations from measured waterchemistry using the so-called `F-factor'. The SSWC model setsthe critical load relative to pre-industrial base cationleaching (a permanent buffer of acid deposition) and a selectedacid neutralizing capacity (ANC) value which corresponds with aknown likelihood of damage to a biological target organism.Here we interpret the meaning of critical load exceedance as aprediction of steady-state ANC, and explore the relationshipbetween exceedance of the critical load and current chemistry. We demonstrate that a critical loadexceedance with the SSWC model does not necessarily indicatethat the critical chemical threshold (zero ANC) has alreadybeen crossed, and there may be no correlation betweenexceedance and biological status. A reformulation of the SSWCmodel is proposed which provides a direct link between currentdeposition and current chemical conditions, and is thereforemore likely to indicate current biological damage. Thereformulation illustrates the discrepancy between currentchemical status and that predicted by the SSWC model atsteady-state, which is a function of the `F-factor'.     

Critical Loads of Acidity for Surface Waters in South-Central Ontario, Canada: Regional Application of the First-Order Acidity Balance (FAB) Model

Major sulphur emission control programs have been implemented in North America, resulting in current emissions being ～30% less than those in 1980. However, the level of acidic deposition remaining is still unlikely to promote widespread recovery of aquatic ecosystems. The First-order Acidity Balance (FAB) model has been applied to south-central Ontario (285 lakes in the Muskoka River Catchment) to evaluate the need for further reductions in emissions. As a result of the past decline in deposition, the proportion of lakes with critical loads exceedance has dropped substantially; however, further reductions in sulphur and nitrogen emissions are required to eliminate critical loads exceedance. Based on bulk deposition of sulphate and nitrogen (41.1 mmol_c m^-2 yr^-1 and 62.5 mmol_c m^-2 yr^-1, respectively) for the period 1995–1999, 166 lakes (58.3%) exceedcritical loads. Even with full implementation of SO₂ abatementprograms in Canada (achieved in 1994) and the United States (legislated for 2010), critical loads will be exceeded in a large proportion (46.6%) of the study lakes.     

Comparison of Critical Load Exceedance and Its Uncertainty Based on National and Site-specific Data

Critical loads have been used to develop international agreements on acidifying air pollution abatement, and within the UK and other countries, to develop national policies for pollution abatement. The Environment Agency (England and Wales) has regulatory obligations to protect sites of high conservation value from the threat of acidification, and hence requires a practical methodology for acidification assessments at the site-specific scale. The Environment Agency has therefore posed the question: Are the national critical load exceedance models sufficiently robust to form the basis for methods to assess harm to individual sites or are they only useful for national policy development? In order to provide one measure of the appropriateness of applying the models at the site-specific scale we incorporated estimates of uncertainty in both national and site-specific data into the calculation of critical load exceedance for individual sites. The exceedance calculations use data from a wide range of sources and the accuracy of the exceedance will be influenced by the accuracy of the input data sets. Using Monte Carlo methods to incorporate the uncertainty in the input data sets into the calculation a distribution of critical load exceedance values is generated rather than a single point estimate. This paper compares uncertainty analyses for coniferous forested sites in England and Wales using both national scale and site-specific data sets and uncertainty ranges.     

Uncertainties in Large Scale Assessments of Critical Load Exceedances

In the 1999 Gothenburg protocol to the UN/ECE LRTAP Convention andin the negotiations for an EU acidification strategy the area withexceedances of critical loads has been the preferred measure forenvironmental impacts. The aim of this study has been to assessthe influence of the uncertainty and spatial variation of both thecritical loads and deposition values on the calculated area withexceedances of critical loads. This has been done on a nationalscale for Denmark and on the European scale based on the dataincluded in the RAINS model. It is demonstrated that includinguncertainty and spatial variation in exceedance calculations, ingeneral gives larger exceeded area for the critical load ofacidity, CL(A). The picture for the critical load of nutrientnitrogen, CL_nut(N), is more mixed because of the higherproportion of exceeded areas. A further point of interest is thepossibility of validating relationships between critical loadexceedances and observable damage based on large scale monitoringand model data. It is demonstrated that it will probably not bepossible to use exceedance calculations on European scale as basisfor validation exercises, linking exceedances to observable damage.     

Variability in Three Finnish Integrated Acidification Models

Integrated assessment models have been used to support ofnegotiations for further emission reductions of acidifyingcompounds in Europe. More attention is being paid to theuncertainties in integrated models. Data from three Finnishintegrated acidification models were compiled to estimate thevariation and relative importance of different modules. Themodels included site-specific and regional dynamic simulationsand steady-state critical load calculations for forest soilsand lakes. The main emphasis was on the variability ofemissions and the uncertainties in ecosystem effects. Althoughmaximum technically feasible emission reduction measures cantheoretically result in very low deposition, the variabilitybetween realistic scenarios is rather restricted. Thevariability of deposition loading is largely determined byreductions in nearby emission sources. The dynamicsimulations, which are often based on detailed input data,seem to retain larger variability than steady-state criticalload approaches. This study suggests that the uncertainties ineffects seem to be larger generally than other modules ofintegrated acidification models. The results indicate the needfor further work on uncertainty analysis for integrated modelsand the availability of useful model systems for furtherconfirmation of ecosystem effects.     

Modelling Acidification and Recovery of Swedish Lakes

The MAGIC model was calibrated to 143 lakes in Sweden, all of which are monitored in Swedish national monitoring programmes conducted by the University of Agricultural Sciences (SLU). Soil characteristics of the lake catchments were obtained from the National Survey of Forest Soils and Vegetation also carried out by SLU. Deposition data were provided by the Swedish Meteorological and Hydrological Institute (SMHI). The model successfully simulated the observed lake and soil chemistry at 133 lakes and their catchments. The fact that 85% of the lakes calibrated successfully without being treated in an individual way suggests that data gathered by the national monitoring programmes are suitable for modelling of soil and surface water recovery from acidification. The lake and soil chemistry data were then projected into the future under the deposition scenario based on emission reductions agreed in the Gothenburg protocol. Deposition of sulphur (sea salt corrected) was estimated to decrease from 1990 to 2010 by 65–73%; deposition of nitrogen was estimated to decrease by 53%. The model simulated relatively rapid improvements in lake water chemistry in response to the decline in deposition from 1990 to 2010, but the improvements levelled off once deposition stabilised at the lower value. There was a major improvement of simulated lake water charge balance acid neutralising capacity (ANC) from 1990 to 2010 in all lakes. The modelled lakes were divided into acidification sensitive and non-sensitive. The modelled sensitive lakes are representative of 20% of the most sensitive lakes in Sweden. By 2010, the ANC in the sensitive lakes was 10 to 50 μeq L^-1 below estimated pre-industrial levels and did not increase much further from 2010 to 2040. Soils at the majority of the modelled catchments continued to lose base cations even after the simulated decline in acid deposition was complete, i.e. after the year 2010. Based on this model prediction, the acidification of the Swedish soils will in general not be reversed by the deposition reduction experienced over the last 10 years and expected to occur by the year 2010.     

Critical Loads of Acidity for Forest Soils: Tentative Modifications

We reviewed the current methods for calculatingcritical loads of acidity for forest soils. The consequencesof four sets of assumptions concerning the soil modelstructure, parameter values and the critical loads criterionwere explored by comparing the values of the averageaccumulated exceedance (AAE) calculated for Finland withdeposition values for the year 1995. The AAE index is given inthe unit of deposition and is a measure of how far a region isfrom being protected in terms of fulfilling a certaincriterion, taking into account the size of the ecosystem areas.Using a critical limit for the molar ratio of theconcentrations of base cations to aluminium in soil solutiongave the lowest average accumulated exceedance. Assumingorgano-aluminium complexes and leaching of organic anions gaveAAE = 4 eq ha^-1 a^-1, which was close to the valueobtained with the standard approach used in Finland, assuminggibbsite equilibrium and no leaching of organic anions,yielding AAE = 5 eq ha^-1 a^-1. With a critical basesaturation limit, instead of the concentrations criterion, theAAE index was 17 eq ha^-1 a^-1. The highest averageaccumulated exceedance (AAE = 25 eq ha^-1 a^-1),corresponding to the lowest critical load, was obtained whenthe effects-based criterion (critical concentration or criticalbase saturation) was substituted with one restricting thedeterioration of the neutralizing capacity of the soil, ANC _le(crit) = 0. These tests illustrate the variabilityof the critical load values for acidity that can be introducedby changing the criterion or by varying the calculation method,without, however, representing the extreme values of criticalloads that could be derived.     

Predicting Freshwater Critical Loads from Catchment Characteristics using National Datasets

Maps of freshwater critical loads are used toguide emission strategies for sulphur and nitrogen bothnationally and internationally. Water chemistry data arerequired to calculate critical loads and the production ofnational maps therefore relies on the existence of extensivechemistry datasets. However, the data required to calculatecritical loads are not readily available for all sites. Thisarticle explores how empirical statistical models mightpotentially be used to predict critical loads using nationallyavailable datasets representing a range of catchmentcharacteristics. Initially a global regression model forexplaining freshwater critical load variation across a broadspectrum of catchment types (from lowland agricultural tomountain lakes) throughout mainland Britain is described. Whenattention is focused on more specific catchment types (i.e.upland and non-arable) it is shown that the global model hasless explanatory power. A regionalisation of Great Britain(based on 100 km grid squares) shows that the global modelcannot necessarily be applied successfully within a narrowerregional context. Separate analyses were undertaken on each ofthe regional subsets using backward selection regression. Thevariables emerging as significant predictors variedsubstantially across the regions, as did the explanatory powerof the models. This was also the case when the analysis wasconfined to upland and non-arable catchments. This approachcould be developed so that critical loads assessments can bemade for populations of standing waters rather than simplythose for which water chemistry is available.     

Modeling Acidification Recovery on Threatened Ecosystems: Application to the Evaluation of the Gothenburg Protocol in France

To evaluate the acid deposition reduction negotiated for 2010 within the UNECE LRTAP Gothenburg Protocol, sulphur and nitrogen deposition time-series (1880–2100) were compared to critical loads of acidity on five French ecosystems: Massif Central basalt (site 1) and granite (2); Paris Bassin tertiary sands (3); Vosges mountains sandstone (4) and Landes eolian sands (5). The SAFE model was used to estimate the response of soil solution pH and ratio to the deposition scenario. Among the five sites, critical loads were exceeded in the past at sites 3, 4 and 5. Sites 3 and 4 were still expected to exceed in 2010, the Protocol year. Further reduction of atmospheric deposition, mainly nitrogen, would be needed to achieve recovery on these ecosystems. At sites 3, 4 and 5, the delay between the critical load exceedance and the violation of the critical chemical criterion was estimated to be 10 to 30 years in the top soil and 50 to 90 years in the deeper soil. At site 5, a recovery was expected in the top soil in 2010 with a time lag of 10 years. Unexpectedly, soil pH continued to decrease after 1980 in the deeper soil at sites 2 and 5. This time lag indicated that acidification moved down the soil profile as a consequence of slow base cation depletion by ion exchange. This delayed response of the soil solution was the result of the combination of weathering rates and vegetation uptake but also of the relative ratio between base cation deposition and acid compounds.     

Development and Application of Critical,Target and Monitoring Loads for the Management of Acid Deposition in Alberta,Canada

The Alberta, Canada acid deposition management framework, based upon the application of critical, target and monitoring loads, is described. This framework is the culmination of four years work by stakeholders brought together within Alberta's Clean Air Strategic Alliance (CASA). The elements of the framework include scientific aspects of measurement, model estimation, and monitoring of acid deposition, assessment of receptor sensitivity, and management processes to reduce emissions and deposition (should reductions become necessary). All loads are applied to grid cells measuring 1°latitude × 1° longitude, with each cell being categorized as sensitive, moderately sensitive or of low sensitivity on the basis of the sensitivities of the soil and water systems within the cell. Critical loads have been set at 0.25, 0.50 and 1.00 keq H⁺ ha^-1 yr^-1 for grid cells that are categorized as sensitive, moderately sensitive, and of low sensitivity, respectively. Target loads, the environmental management objectives, have been set at 0.22, 0.45, and 0.90 keq H⁺ ha^-1 yr^-1, and monitoring loads, a new concept in acid deposition management, have been set at 0.17, 0.35 and 0.70 keq H⁺ ha^-1 yr^-1 for the three sensitivity classes. When model prediction indicates that deposition may be exceeding the monitoring load, deposition monitoring and receptor sensitivity studies are to be initiated to confirm the deposition model prediction, and to ensure that the sensitivity of the recipient systems is understood. In this manner, management actions that occur in the event of a target load exceedance will be based upon receptor sensitivity and deposition data rather than upon model prediction alone. A process for stakeholder involvement in the evaluation of the framework and its application in long-term, long-range management of emissions and deposition is also included within the framework.     

The Use of a GIS-based Inventory to Provide a Regional Risk Assessment of Standing Waters in Great Britain Sensitive to Acidification from Atmospheric Deposition

Previous attempts to identify regions of Britain vulnerable to acidification have used sensitivity maps based on the distributionof soils, geology, and land cover across Great Britain. Additionally, a systematic survey of freshwaters undertaken as partof the U.K. critical loads mapping programme provides a regional assessment of both sensitivity (critical loads) and, in tandem withdeposition data, potential impact (critical load exceedance). Both approaches, while useful for identifying regional patterns, do not enable estimates of the number of affected water bodies to be made. Recent EU legislation (e.g., The Water Framework Directive) requires member states to set water quality objectives for all water bodies. We developed a GIS-based inventory of standing water bodies in response to the need for legislation-driven assessments of the status of the U.K. lake population. This paper describes how the inventory can be used to assess the number of standing water bodies in Britain that are vulnerable to acid deposition (at current levels), building on the sensitivity mapping undertaken previously. Using this approach, approximately 31% of all standing waters in Great Britain (excluding the Shetlands and Orkney) larger than 0.02 ha are identified as `at risk' from acidification. Higher proportions are vulnerable in Scotland and Wales. Additionally, large numbers of standing waters in areas designated for environmental protection purposes are also vulnerable.     

How are Results from Critical Load Calculations Reflected in Lake Water Chemistry?

The Steady State Water Chemistry Model (SSWCM) is a common method for determinations of critical loadof acid and subsequently of critical loadexceedance for lakes. One way to verify the modeloutput, is to compare with chemical indicatorssuch as pH-value, alkalinity or ANC. When themedian chemical status (as ANC) is used 65% ofthe lakes responded according to the exceedancevalue. For these the calculated exceedanceresulted in violation of the critical chemicalvalue while non-exceedance gave no violation.Since biota react on extreme conditions a morecorrect evaluation should be based on minimumvalues for the chemical indicator. This raises thefraction of lakes responding to 78%. Non-exceedance is seldom found inlakes with acid conditions. The evaluationindicates that the calculation of critical load ofacidity by means of SSWCM is very reliable.     

Cost-effectiveness Analysis of Reducing the Emission of Nitrogen Oxides in Asia

The purpose of this study is to evaluate cost-effective reduction strategies for nitrogen oxides (NO _x ) in the Asian region. The source-receptor relationships of the Lagrangian “puff” model of long-range transportation, ATMOS-N, were used to calculate the wet/dry deposition of the nitrogen (N) in Asia. Critical loads of N deposition in Asia were calculated from the relationships between the critical load of sulfur (S) and balance of N in and out using the data of S critical load of RAINS-ASIA. The cost functions of N reduction of Asian countries were derived by the regression analysis with the data of cost functions of European countries used in RAINS. In order to assess the environmental impact, the gaps between N deposition and critical load of N were calculated. The emission of NO _x was reduced in some cases of this model, and the changes of gaps between N deposition and critical load were observed as well as the changes of the reduction cost. It is shown that a uniform reduction of NO _x emissions by countries in Asia is not cost-effective strategy.     

Critical Loads Exceedances in Germany and their Dependence on the Scale of Input Data

Critical load exceedances have been used as an effects-related parameter for guiding international air emission control negotiations. High-resolution critical load data are combined with low-resolution deposition data.This article shows that doing so systematicallyunderestimates `true' critical load exceedances as obtainedfrom combining critical load and deposition data of identicalhigh spatial resolution. 95th percentile critical loadexceedances in EMEP grids based on high resolution depositiondata are 60 and 150% higher (mean values for nutrientnitrogen and acidity, respectively) than critical loadexceedances based on the low resolution EMEP depositionmodel. The latter are used in international negotiations. Differences in individual EMEP grid squares vary betweeninsignificantly different from zero and 340%, depending onregional deposition and critical load characteristics andcritical load types (nutrient nitrogen versus acidity).Exceedances based on high-resolution deposition values arealso compared to EMEP grid averages of these values forforests only. This comparison excludes the effect ofsystematically higher depositions to forests. Still, thescale difference of (averaged, low-resolution) deposition and(high-resolution) critical loads data yields underestimatesof the 95th percentiles by on average ca. 20%.These systematic errors due to the scale dependence should beborne in mind when interpreting effects of internationalemission control measures.     

Temporal Trends in Mercury Accumulation in Lake Sediments in Sweden

Lake sediment cores were analyzedto study the history of mercury (Hg) pollution andparticularly to determine whether recent sedimentconcentrations have declined in response todeclining atmospheric deposition of Hg. Sedimentcores from 6 forest lakes distributed fromsouthern to northern Sweden and 3 northernmountain lakes were analyzed for Hg using CVAAS. A400 cm sediment profile from Måkevatten insouthwest Sweden indicates that the onset of Hgpollution occurred in the 18th century. Anindisputable increase in Hg concentrationsoccurred concurrent with the appearance ofspheroidal carbonaceous flyash particles (SCP)derived from fossil-fuel combustion, in themid-19th century. There is a strong correlationbetween Hg and SCP concentrations in the sedimentcores (r=0.67 to 0.91), which suggests a strongrelationship between historical Hg pollution andfossil fuel burning. In contrast to sediment corestaken in 1979, maximum Hg concentrations are nowobserved below the sediment surface and declinetowards the sediment surface. This study confirmsthat reductions in atmospheric deposition of Hgover Sweden have resulted in a decreased transferof total Hg to aquatic environments as reflectedby lake sediments, and that lake sediment profilesof Hg concentrations reflect relative trends inthe atmospheric deposition of Hg rather thanpost-depositional diagenetic processes.     

Restoration of a Small High Mountain Lake after Recent Tourist Impact: The Importance of Limnological Monitoring and Palaeolimnology

The natural Park of Peñalara consists of a small mountainousarea near Madrid and includes a series of water bodies (fromsmall mountain lakes to temporary ponds and peat bogs), the mostknown of them being the so-called `Laguna Grande dePeñalara'. Due to growing numbers of visitors theenvironmental conditions of this lake started to decline in theearly 1970s because of: (1) the start of severe soil erosionprocesses; (2) the increase of nutrient load; and (3) theintroduction of a non-native fish species. Since the area wasprotected in 1990, several conservation and restoration projectsincluded in an integrated management plan have been developed. Here we summarise some of the results of these efforts: (1) controlled access of livestock and visitors to the area; (2) palaeolimnology studies aimed at inferring recent changes in thewatershed; and (3) monitoring of the limnological features of thesystem. Restoration of this lake and its watershed is intendedto serve as a model for the management of other severely alteredhigh mountain lakes.     

Uncertainty in Estimation of Wet Deposition of Sulphur

A model is described for predicting wet deposition ofsulphur in Britain from rainfall and site measurementsof ion concentration in precipitation. This modelincludes orographic enhancement of both rainfall andion concentration. The model output is comparedagainst available measurement data. Sensitivity anduncertainty analyses are used to predict the outputuncertainty. If the stated assumptions can be shown tobe correct, the wet deposition for Britain at the 5 kmscale is accurate to ±35% across the country. Theanalyses show a larger uncertainty in central Englandand a possible bias towards underestimation of wetdeposition, the latter being of importance incalculating critical load exceedances in remote areas.     

Critical Loads and Exceedances of Acid Deposition and Associated Forest Growth in the Northern Hardwood and BorealConiferous Forests in Québec,Canada

We used the Québec forest monitoring network (`Réseaud'Étude et de Surveillance des Écosystèmes Forestiers' or RESEF)along with its atmospheric monitoring stations to assess criticalS and N loads and their combined soil acidification exceedancesfor natural ecosystems of the northern hardwood and borealconiferous forests in Québec, Canada. Critical loads (CL) forforest soil acidification were calculated using the simple mass-balance (SMB) approach and with the steady-state PROFILE model.Atmospheric deposition rates for water, S, N, Ca, Mg, Na, and K,for the years 1989–1993, and detailed, plot-specific forest andsoil characteristics were used as input. The SMB model alsorequired information regarding nutrient uptake and storage in theaboveground woody biomass. The CL calculations indicated that,from the 31 RESEF plots, 18 received atmospheric acidic inputs inexcess of their CL (55 and 61% of the hardwood and coniferousplots, respectively). The range of CL exceedance varied from 60to 470 eq ha^-1 yr^-1 for the hardwood stands, and from 10to 590 eq ha^-1 yr^-1 for the coniferous stands. The standswith CL exceedance were mainly located in the western and centralpart of the province. Stand growth associated with exceedanceclass of acidity was determined using the RESEF plots along withselected permanent forest survey plots having similar sitecharacteristics, but for which longer growth records wereavailable. We found a significant negative correlation betweenforest growth rates and critical soil acidification exceedancefor both the northern hardwood and the boreal conifer sites.Specifically, plots with critical load exceedances were found tohave a growth reduction of about 30% during the 1974–1982 andthe 1972–1990 measurement (plots with no soil acidificationexceedance served as a control). While this correlation is notnecessarily causal, it is nevertheless consistent with theexpectation that increased losses of soil base cations on accountof increased soil acidification should and could lead todeteriorating forest health conditions.     

Deposition Loads of Sulphur and Nitrogen in Germany

High spatial resolution maps of deposition loads in Germanyare produced as an input for abatement strategy research andfor critical loads exceedance calculations on a nationalscale. In this paper methods ofmapping total deposition loads in Germany and preliminarymaps of nitrogen and sulphur deposition loads for the year1993 are presented. A comparison of these mapping resultswith EMEP deposition mapping results has been carried out.The differences in the results of the German national and theEuropean EMEP mapping, due to different databases anddifferent methods, are quantified and discussed. Highresolution maps of deposition loads are compared to Europeanlow resolution maps on the same temporal and spatial scale,assuming that on average both should lead to similar results.However, the average differencescalculated for 23 EMEP 150 × 150 km² grid cells over Germanywere found to be 33% higher for sulphur (S) total depositionby the German method 65% higher for S dry deposition and1% lower for S wet deposition. The German results fornitrogen (N) total deposition are 2% higher than the EMEPresult 22% higher for N dry deposition and 10% lower for Nwet deposition.