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.     

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.     

Investigating the Uncertainties in the Simple Mass Balance Equation for Acidity Critical Loads for Terrestrial Ecosystems in the United Kingdom

The Simple Mass Balance (SMB)equation has been developed and used as one ofthe principal methods for calculating criticalloads of acidity for forest ecosystems. Criticalloads have formed the basis for informing policyrelated to the control and abatement of emissionsof acidifying pollutants. The SMB equationrelies on a variety of assumptions and dataderived from a variety of sources. Each of thesecomponent constituents has a potential source oferror depending on the method(s) used for theirderivation and the value(s) assigned. The resultis the possibility of generating a range ofcritical load values for a single ecosystem. This paper summarises the SMB equation, examinesthe uncertainties in deriving input values andreviews other works on the key assumptions.     

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.     

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.     

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.     

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 UN/ECE International Programme on Mapping Critical Loads and Levels

Critical Loads and levels have played a centralrole in the successful development of effect-based emissionreduction strategies for Europe in the fields of acidification,eutrophication and ground-level ozone. The aim of theInternational Programme on Mapping Critical Loads and Levelsled by Germany, with participation of 24 countries, is todetermine critical loads and levels for forest, crops, naturalvegetation, soils, water and materials. The exceedances ofcritical loads and critical levels are used to quantify the riskfor environmental damage by air pollution and tosupport the development of optimised abatement strategies.     

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.     

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.     

Element Removal in Harvested Tree Biomass: Scenarios for Critical Loads in Wallonia,South Belgium

The critical load concept is nowwidely used as a tool for developing emissioncontrol policies in Europe. As a signatorycountry of the Convention of Long-RangeTransboundary Air Pollution, critical loads foracidity, nutrient nitrogen, nitrogen and sulphurhave been calculated for the Flemish and Walloonregions in Belgium. This paper describes themethodology used for estimating critical loadsfor forest soils in the Walloon region accordingto the Steady-State Mass Balance equations. As anexample the methodology was applied to thecatchment `Waroneu', situated in a sensitive areaof the Haute Ardenne. Main input parameters tothe equations were derived from precipitation andrunoff data of the catchment study. Improvedestimates of nitrogen uptake (Nu) and base cationuptake (BCu) were obtained by intensive samplingof Picea abies and Quercus roburtrees. Nutrient contents (Ca, Mg, K, N) andnutrient to nitrogen ratios of Picea abiesreflected the poor soil quality at a site withhigh N deposition. Quercus robur nutrientcontents increased from stem to higher orderbranches with a high proportion of nutrientslocated in the bark. However the simulation ofstem only harvesting had a minor effect oncritical loads. Measured wood densities werelower than reported literature values with a maineffect on Nu and BCu estimates. The use ofrecommended default values and/or data derivedfrom the experimental site resulted in a widerange of critical loads, some of which werelargely overestimated. Results demonstrated theimportance of site specific data for criticalload calculations.     

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.     

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.     

Critical Loads – Is There A Need For A New Concept?

The concept of critical loads has been an important andsuccessful tool for the development of control strategiesfor transboundary air pollution in Europe. The use of theconcept has led us to a situation where very few areas inEurope will have an exceedance of critical loads foracidification in 2010, indicating that the benefits offurther control acidifying substances will be lessuseful. The critical loads concept does not, however,take into account the large benefits of further controlin damaged systems but where critical loads are nolonger exceeded. In this paper we discuss the importanceof widening the critical loads concept to include thesebenefits and we propose an additional effect-relatedmeasure, Dynamic Impact Analysis, to be included infurther control strategies and assessments. With such aconcept the actual situation and its further developmentwill be included in assessments and control strategies.     

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.     

The Applicability of National Critical Loads Data in Assessing Designated Sites

Critical loads have been successfully used within Europe in the development of effects-based policies for pollution abatement, including the Second Sulphur Protocol and the Protocol to abate acidification, eutrophication and ground-level ozone (CLRTAP, 1979). This success has encouraged the UK Environment Agency and Conservation Agencies to use the national critical load maps as a screening tool in assessing the threats from acidification and eutrophication to designated (Natura 2000) sites. The UK maps of critical loads are based on national-scale data sets appropriate for national-scale assessments, and were never intended for use at the site-specific level. Site-based assessments are often targeted at Special Areas of Conservation, a sub-set of the UK Natura 2000 sites. The spatial data available includes the boundaries of the sites but not the location of the designated features. Ancillary data is variable from one site to another; habitat types may be described in detail with cross-reference to classes of the National Vegetation Classification (NVC: Rodwell, 1991 et seq), but information available on soils and geology is generalised and has not been related to the habitats or species being protected. Hence it can be difficult to relate the individual sites to the national maps, even where appropriate to do so. This paper examines the underlying uncertainties in the national critical load maps showing how the maps could give misleading results if used for site-specific assessments. It also includes advice on how to determine when the national data may be appropriate as a policy-tool at the site-level.     

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.     

Alternatives to incineration in remediation of soil and sediments assessed

Contamination of soil and sediment by pollutants represents a major environmental challenge. Remediation of soil during the original Superfund years consisted primarily of dig and haul, capping, or containment. The 1986 amendments to CERCLA—SARA—provided the incentive for treatment and permanent remedies during site remediation. Thermal treatment, which routinely achieves the low cleanup criteria required by RCRA land-ban regulations, became one of the major technologies used for cleanup under the concept of ARAR. As the remediation industry matured and recognized specific market niches in soil remediation, a number of new technologies emerged. Thermal desorption, bioremediation, soil vapor extraction, soil washing, and soil extraction are being used on sites at which the technology offers advantages over incineration. In addition, a continuing stream of emerging technologies is being presented that requires careful evaluation relative to existing cleanup methods. Each of these technologies offers a range of options for achieving appropriate cleanup criteria, application to different soil matrices, cost, time of remediation, and public acceptability. Balancing cleanup criteria defined by regulation or risk assessment with technology cost and capability affords the opportunity to solve these problems with appropriate balance of cost and protection of human health and the environment.     

Critical Review of Norms and Standards for Biodegradable Agricultural Plastics Part Ι. Biodegradation in Soil

A critical review of norms and standards and corresponding tests to determine the biodegradability in soil for biodegradable plastics, possibly applicable also to biodegradable agricultural plastics, is presented. There are only a few norms available at the international level about biodegradable plastics in soil. The criteria, parameters and testing methodologies for the characterization, labelling and validation of the agricultural plastic waste streams with respect to possible biodegradation in soil according to existing international standards are analysed while the relevant controversies are identified. To derive the best suited for agricultural plastics specs and testing methods, the possible developments or adaptation of available specs, is investigated. Considering the existing types of biodegradable plastic products in agriculture and their effective life management at the agricultural field, only a few norms appear to provide suitable tests that could be adapted, following appropriate research work, for testing biodegradability in soil under real field conditions. It is shown that some major revisions are needed, with the support of systematic research work, before a new universal norm and standard testing methods become available for testing agricultural plastics for biodegradation under real, and highly variable, soil conditions. Based on the analysis of the different norms and their content it appears necessary to incorporate provisions for transferability of results to different soils and climates, validation of tests through a positive reference and also, set prerequisites for soil media. Long term biodegradation in soil prediction is another open issue.     

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.