The Importance of Selecting Appropriate Criteria for Calculating Acidity Critical Loads for Terrestrial Ecosystems Using the Simple Mass Balance Equation

The Simple Mass Balance (SMB) equationis commonly used throughout Europe for thecalculation of acidity critical loads for forestsoils. Different criteria can be set in themodel depending on whether the receptor (e.g. treeroots) is more sensitive to the toxic effects ofaluminium or to unfavourable pH conditions. Thispaper examines the effects on critical loadscalculations of using different criteria andcritical limits, and demonstrates the importanceof selecting the most appropriate and justifiablecriteria for the chosen receptor, since they caneffect the critical loads values obtained. Abrief review of the range of different criteriaand limits used throughout Europe is included. In addition, the gibbsite equilibrium constant,used in the SMB equation to represent therelationship between dissolved aluminium andhydrogen ions in soil solution, is discussed. This relationship is not generally described inthe literature as a criterion in the equation,but this work highlights the effects differentgibbsite values have on critical loadcalculations and the importance of applying themost appropriate value for the soil in therooting zone of the receptor.     

On the Calculation and Interpretation of Target Load Functions

In this study critical load functions and target load functions of nitrogen and sulphur deposition with respect to acidity and minimum base cation to aluminium ratio were calculated with the SAFE model using three different averaging strategies: (1) averaging based on current forest generation, (2) averaging based on next generation and (3) averaging based on the entire simulation period. From the results it is evident that although target load calculation and indeed critical load calculation is straight forward, there is a problem in translating a predicted recovery according to the target load calculation back to a site-specific condition. We conclude that a policy strategy for emission reductions that ensures recovery, according to calculated target load functions, is likely to be beneficial from an ecosystem point of view. However, such a strategy may not be sufficient to achieve actual non-violation of the chemical criteria throughout the seasonal or rotational variations. To address this issue we propose a method for calculating dynamic critical loads which ensures that the chosen criteria is not violated.     

Aluminium: The Need for a Re-Evaluation of Its Toxicity and Solubility in Mature Forest Stands

Aluminium (Al) is a key element in critical loadcalculations for forest. Here, we argue for re-evaluating theimportance of Al. Effects of two levels of enhanced Alconcentrations and lowered Ca:Al ratios in the soil solutionin a field manipulation experiment in a mature spruce stand(1996–1999) on tree vitality parameters were tested. Inaddition, Al solubility controls were tested. Various loads ofAl were added to forest plots by means of an irrigationsystem. Potentially toxic Al concentrations and criticalratios of Ca to inorganic Al were established. The ratio of Cato total Al was not a suitable indicator for unfavourableconditions for plant growth. No significant effects on crowncondition, tree growth and fine root production were observedafter three years of treatment. In 1999, foliar Mg content inthe highest Al addition treatment had declined significantly.This agreed with the known response to Al stress of seedlingsin nutrient solution experiments. No support was found forusing the chemical criterion Ca:Al ratio in soil solution,foliar and root tissue as an indicator for forest damage dueto acidification. Al solubility was considerably lower thanimplied by the assumption of equilibrium with gibbsite,particularly in the root zone. The gibbsite equilibrium iscommonly used in critical load models. Substitution of thegibbsite equilibrium with an Al-organic matter complexationmodel to describe Al solubility in soil water may have largeconsequences for calculation of critical loads. The resultsindicate that critical load maps for forests should bereconsidered.     

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 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.     

Critical Loads and Dynamic Modelling to Assess European Areas at Risk of Acidification and Eutrophication

European critical loads and novel dynamic modelling data have been compiled under the LRTAP Convention by the Coordination Centre for Effects. In 2000 9.8% of the pan-European and 20.8% of the EU25 ecosystem area were at risk of acidification. For eutrophication (nutrient N) the areas at risk were 30.1 and 71.2%, respectively. Dynamic modelling results reveal that 95% of the area at risk of acidification could recover by 2030 provided acid deposition is reduced according to present legislation. Insight into the timing of effects of exceedances of critical loads for nutrient N necessitates the further development of dynamic models.     

European Critical Loads of Cadmium, Lead and Mercury and their Exceedances

Critical loads of cadmium, lead and mercury were computed by 18 countries of the LRTAP Convention. These national data were collated into a single database for the purpose of identifying sensitive areas in Europe. Computing exceedances, i.e. comparing the critical loads to atmospheric deposition, shows that cadmium was not a widespread risk in 2000, that the risk from lead deposition has decreased since 1990 but was still widespread in 2000, and that the risk from mercury remains high without much change from 1990 to 2000 in most of the countries.     

The Role of Mineral Weathering Rate Determinations in Generating Uncertainties in the Calculation of Critical Loads of Acidity and their Exceedance

Current legislation within Europe aimed at limitingecosystem damage resulting from inputs of atmosphericpollution is based on the critical load concept. Mineralweathering rates are central to the calculation ofcritical loads (acceptable levels) of acid deposition.The authors have undertaken a number of studies whichillustrate the complications and limitations inherent inpredicting mineral weathering rates and the implicationswhich these have for critical loads calculations andmapping. Calculated weathering rates and critical loadsfor two acid-sensitive parent materials (greywackes andgranites) are presented and are used to illustrate theimpact that uncertainty can have on critical loadexceedances. The results have obvious implications forportraying the uncertainties of critical loads to policy makers.     

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.     

An Analysis of the Structure of the Simple Mass Balance Equation: Implications for Testing National Critical Loads Maps

The critical loads concept is used by the UN-ECEConvention on Long Range Transboundary Air Pollution(CLRTAP) for setting pollution reduction targets.Increasing numbers of countries are adopting the SimpleMass Balance equation (SMB) to calculate critical loads ofacidifying S and N for forest soils. The equation is madeup of a series of mass balances each of which is used tocalculate a leaching flux. The assumptions in the SMBequation were investigated by testing its ability topredict current sulphur load and by comparing each of thecalculated leaching fluxes to measured rates. It was notpossible to predict current sulphur load at our sites usingthe SMB equation. The leaching tests demonstrated that,primarily due to its steady state assumptions, the SMBequation generates critical loads that are theoretical longterm estimates of risk, and are untestable. Thesimplifying assumptions sometimes lead to illogicalresults. Some of these can be improved by adding a final,simple but dynamic, calculation step to determine theexpected time until effects are observed. Theacceptability of combining annual average data, which bestapproximates steady state, with a biological indicator isquestionable. It is not possible to test critical loadscalculated using the SMB equation when applied with all ofits assumptions but it is possible to test its fundamentalapproach using non steady state data.     

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.     

A Novel Method for Mapping Critical Loads Across a River Network: Application to the River Dart,Southwest England

To date, estimates of freshwater critical loads have beenbased on a single sample site within a given area, in theUK the `most sensitive' surface water in each 10 km gridsquare. The critical loads obtained are thus highlydependent on the sites chosen, and at a relatively coarsespatial resolution. To produce a higher resolutioncritical load assessment, the PEARLS (Prediction ofAcidification and Recovery on a Landscape Scale)procedure has been used to estimate critical loads acrossa large (248 km²), partially acid-sensitivecatchment in Southwest England. PEARLS utilises availablesoils and land-use databases, and sampled streamchemistry data, to derive characteristic runoffcompositions for a set of landscape types. Mixingequations are then used to calculate runoff chemistry,and subsequently critical loads, throughout the streamnetwork. Results show major spatial variability, withcritical loads lowest in streams draining peat-moorlandheadwaters, and generally increasing downstream asagricultural land contributes an increasing proportion ofrunoff. The 5th percentile freshwater critical loadfor the catchment is estimated at 0.29 keq H⁺ ha^-1yr^-1,and critical loads are exceeded for around 40% of totalstream length. The PEARLS methodology provides a novelopportunity to assess the spatial variability infreshwater critical loads, and to provide estimates ofexceedance at whole catchment scale. It has potentialapplication in the assessment of surface watersensitivity to acidification across wider areas in the UKand elsewhere.     

Why Critical Loads of Acidity and N for Soils Should be Based on Pollutant Effective Concentrations Rather Than Deposition Fluxes

Numerous assumptions have been made over the past 17 years when calculating critical loads for soils, both for acidity (based upon base cation steady state mass balances (SMB)) and for N (eutrophication, based upon N mass balances), often without all the assumptions being explicitly stated. The tacit assumptions that the author believes to be implicit in the SMB approach are critically reviewed, with particular reference to upland regions where slope processes are highly significant. It is concluded that many of them cannot be justified, especially those that involve ignoring many key processes known to be important to biogeochemical cycling and soil evolution in upland catchments. The evidence presented suggests that critical loads of acidity and of N for soils should be based upon effective pollutant and, for acidity, also effective base cation deposition concentrations, rather than upon pollutant deposition fluxes. This is because of the dominant role of cation exchange equilibria, rather than weathering rate, in regulation of the pH and base status of the more acidification-sensitive soils, and because of the importance of transport down slope of base cations, alkalinity and N species.     

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.     

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.     

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.     

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.     

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.     

Freshwater Critical Loads in Wales

The Steady State Water Chemistry (SSWC) modeland the Diatom model have been used to calculate criticalloads for acidity using annual mean chemistry for 102 acidupland streams in Wales sampled as part of the Welsh AcidWaters Survey (WAWS) in 1995. Diatom critical loads werelower than SSWC values reflecting the higher effective[ANC]_limit of the Diatom model compared to the[ANC]_limit of zero used in the SSWC model. The WAWSstream sites were all located within 41 10 × 10 km squares andeach square was assigned the lowest critical load value fromamongst the sites located within it. Comparison with valuesassigned under the UK national critical loads mappingprogramme (UKCLMAP) showed that WAWS critical loads were lowerthan UKCLMAP values in approximately 40% of squares.Differences in critical load class were variable, but exceeded2 keq ha^-1 yr^-1 in up to a maximum of seven squares.It cannot be assumed, therefore, that reducing acid depositionto the currently mapped UKCLMAP critical load will protect allstreams occurring within a given 10 × 10 km grid square inWales. The limited number of sample sites means that even inthose squares where all WAWS sites will be protected, theremay be other, more acid sensitive freshwaters with lowercritical loads. This has important implications for theinterpretation and use of critical loads data for regional andlocal environmental planning.