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.     

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.     

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.     

Application of Static Critical Load Models for Acidity to High Mountain Lakes in Europe

Critical load models for acidityprovide a measure of the sensitivity of surfacewaters to acid deposition, and can be used todetermine critical load exceedance and potentiallong-term harmful effects. Three static models,the Steady-State Water Chemistry model, diatommodel and First-order Acidity Balance model, arehere applied to 11 high mountain lakes in Norway,Scotland, the Alps, the Pyrenees and the Tatras.Between five and seven of the lakes show criticalload exceedance, depending on the model used.Nitrogen as well as sulphur deposition isimportant in causing exceedance. Since soil andvegetation cover are generally sparse, geologyand lake retention time appear to be key factorsin the determination of critical load. Retentionof nitrogen is observed, but it is unclearwhether this occurs within the lake or theterrestrial part of the catchment.     

Using Multiple Chemical Criteria for Critical Loads of Acidity in Maritime Regions

Critical loads have become a well-establishedpart of the work programme of the UnitedNations Economic Commission for Europe (UNECE) Conventionon Long-Range Transboundary Air Pollution (CLRTAP). Thelinking of ecosystem response to deposition level is thecentral principal of the critical loads approach. Foreach ecosystem, a biological indicator is chosen, asuitable chemical criterion selected and a criticalchemical limit assigned. The Bc:Al ratio is the mostwidely used chemical criterion for setting criticalloads. However, critical loads based on this criterionare very sensitive to marine deposition. In regions whichreceive high depositions of marine-derived base cations,such as the Republic of Ireland (ROI) and the UnitedKingdom (UK), critical loads based on the Bc:Al criterionwill inevitably be high. Therefore, it is proposed thatcritical loads are estimated using multiple chemicalcriteria with appropriate critical limits to protect thechosen biological indicators. The range of publishedchemical criteria have been applied to the ROI and theUK. The chemical criterion corresponding to the mostsensitive critical load have been mapped and thecontribution of each to the final maps investigated. Thesimulations indicate that the most sensitive criteria forsetting critical loads are based on specifying critical Hor Al concentrations. However, the choice of critical limits andmodel parameters will ultimately effect the criticalloads. Therefore, it is important that appropriate criticallimits are chosen to protect the biological indicator andreceptor ecosystem from long-term damage.     

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.     

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'.     

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.     

Chemistry,Mineralogy and Morphology of Spodosols at Two Swedish Sites Used to Assess Methods of Counteracting Acidification

The chemistry, mineralogy and morphology of two soil profiles developed on till material of granitic and gneissic composition in south-western Sweden were studied in relation to podzolization processes. These soils were used for treatments with lime and wood ash. The profiles do not show characteristic Podzol morphology but qualify as Spodosols under Soil Taxonomy criteria and are probably typical for the coniferous forest soils of south-western Sweden. Podzolization features are clear but less well expressed than in classic Podzols. The distribution of major elements shows podzolization features with accumulation of sesquioxides in the B horizons and depletion in the eluvial horizons. Quartz and feldspars dominate the bulk soils reflecting the clear relationship between the composition of the soil and the underlying bedrock. Low amounts of clay contain an interlayered vermiculitic phase as the main phyllosilicate in which the degree of interlayering, known to be pH dependent, varies with depth and is at a maximum in the Bhs horizon. In the B horizons there are small but significant amounts of imogolite-type material which affect the adsorption of sulphate.     

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.     

Use of the Dynamic Model `MAGIC' to Predict Recovery Following Implementation of the Gothenburg Protocol

Reduction of sulphur deposition causesrecovery of acidified surface waters. Processes in thecatchment delay recovery. The acidification model MAGICwas applied to the Vikedal and Tovdal rivers in southernNorway. Response in water chemsitry is delayed by 10–20 yr. The delay is due to release of old sulphate atVikedal and cation exchange at Tovdal. Assuming that theGothenburg protocol is fully implemented by the year2010, much of the predicted increase of ANC will occur inthe next 10 yr with a levelling off by about 2040. Ifnitrogen leaching increases in the future, however,recovery of ANC will not be as rapid, nor as complete.Critical load for acidity calculated by steady-statemodels is confirmed by the MAGIC predictions. Futurerequirement for mitigation measures such as liming willdecrease in the future as acid deposition decreases. Bythe year 2046 the liming requirement will be reduced byabout 45% at Vikedal and 65% at Tovdal. One of the mainpurposes of the Norwegian national monitoring programmeis to provide documentation of changes in environmentalquality due to long-range transported air pollutants.Modelling applications such as this clearly show that thedata fill this purpose.     

High Immobilization of NH4+ in Danish Heath Soil Related to Succession,Soil and Nutrients: Implications for Critical Loads of N

During recent decades heathlands havechanged into grasslands in regions with high atmosphericnitrogen deposition. In regions with intermediatedeposition level (e.g., Denmark) changes have been lesspronounced which may be due to delay or decrease inresponse of the ecosystem. The mor layer (O horizon) mayplay an important role for this delay due to high sinkstrength for N. In this study, the capacity for netNH₄ ⁺ immobilization and mineralization wasstudied during short- and long-term incubations (2–36 days)of mor samples from Danish dry inland heaths. High short-term capacity for net NH₄ ⁺ immobilization wasfound to be a general characteristic of Danish heath morlayers both under heather (Calluna vulgaris) andcrowberry (Empetrum nigrum ssp nigrum), the latterdominating late stages in heathland succession. The netNH₄ ⁺ immobilization was higher under youngcompared to old or dead vegetation, and higher on lessnutrient poor soils than on extremely nutrient poor soils.The addition of N, P and C stimulated CO₂ productionand net NH₄ ⁺ immobilization, but not net Nmineralization. The immobilization of ¹⁵NH₄ ⁺caused release of dissolved organic N, increased N anddecreased C/N ratio in the microbial biomass, and indicatedgrowth of microorganisms with other metabolic abilitiesthan the indigenous population. No evidence was obtained ofstabilization of immobilized ¹⁵NH₄ ⁺ intosoil organic matter during the experiment. On background ofthe results and current knowledge it was concluded that therecognition of the high capacity for net NH₄ ⁺immobilization in mor layers does not allow for a raiseof critical loads for N for northern dry inland heaths.     

Linking field experiments to long-term simulation of impacts of nitrogen deposition on heathlands and moorlands

The results from three long-term field manipulation studies of the impacts of increased nitrogen deposition (0–120 kg N ha^–1 yr^–1) on lowland and upland heathlands in the UK were compared, to test if common responses are observed. Consistent increases in Calluna foliar N content and decreases in litter C:N ratios were found across all sites, while increases in N leaching were not observed at any site over the range 0–80 kg ha^–1 yr^–1. However, the response of Calluna biomass did vary between sites, possibly reflecting site differences in nutrient status and management histories. Five versions of a simulation model of heathland responses to N were developed, each reflecting different assumptions about the fate and turnover of soil N. Model outputs supported the deduction from mass balance calculations at two of the field sites that N additions have resulted in an increase in immobilisation; the latter was needed to prevent the model overestimating measured N leaching. However, this version of the model significantly underestimated Calluna biomass. Model versions, which included uptake of organic N by Callunaand re-mobilisation of N from the soil organic store provided some improvement in the fit between modelled and field biomass data, but re-mobilisation also led to an overestimation of N leaching. Quantification of these processes and their response to increased N deposition are therefore critical to interpreting experimental data and predicting the long-term impacts of atmospheric deposition on heathlands and moorlands.