Dissolved and colloidal transport of Cd, Pb, and Zn in a silt loam soil affected by atmospheric industrial deposition.

As a result of processing of metal ores, trace metals have contaminated large areas of northern France. Metal migration from the soil to groundwater presents an environmental risk that depends on the physico-chemical properties of each contaminated soil. Soil water samples were obtained over the course of 1 year with zero-tension lysimeters from an acidic, loamy, metal contaminated soil. The average trace metal concentrations in the soil water were high (e.g. for Zn 11 mg l-1 under the surface horizon), but they varied during the sampling period. Zn concentrations were not correlated with pH or total organic carbon in the solutions but were correlated with Cd concentrations. On average, 95% of the Zn and Cd but only 50% of Pb was present in a dissolved form. Analytical transmission electron microscopy was used to identify the Zn or Pb carriers. Colloids containing Pb and Zn were biocolloids, whereas colloids containing only Zn were smectites.     

Moss (Bryum radiculosum) as a bioindicator of trace metal deposition around an industrialised area in Sardinia (Italy)

The moss Bryum radiculosum (Brid.), a species typical of dry and coastal environments, was used as a bioindicator for the estimation of atmospheric trace metal deposition around the industrial site of Portoscuso (Sardinia, Italy), which includes a lead-zinc smelter, two power plants, and aluminium production factories. For Cd, Pb, Zn, and V the results showed very similar patterns with extremely high values in the immediate surroundings of the industrial area. Copper and Cr showed somewhat different patterns, but still pointing to local pollution sources. The levels of metals at distance of about 13 km from the industrial site were still higher than in background samples. In order to evaluate the suitability of B. radiculosum for monitoring studies, trace metal concentrations in moss were compared with bulk deposition measurements in the same area. Correlation was significant only for Pb, Cd, and Zn. For Cr, Cu, and V the results showed high variability, mainly to be ascribed to soil factors.     

Degradability of ethylenediaminedisuccinic acid (EDDS) in metal contaminated soils: implications for its use soil remediation

Previous research has identified ethylenediaminedisuccinate (EDDS) as a promising biodegradable alternative for persistent compounds such as EDTA for application in soil washing or enhanced phytoextraction of heavy metals. This study examines heavy metal mobilization in three polluted soils varying in soil composition, with specific attention for competitive behaviour for complexation between the various metals and major elements, such as Al, Fe, Mn, Ca and Mg. In addition, amendment biodegradability was compared between the different soil types. The selected soils included a moderately contaminated calcareous clayey soil, a dredged sediment derived surface soil with similar soil characteristics yet more heavily polluted with Cd, Cr and Zn, and a sandy soil moderately contaminated by historical smelter activity (atmospheric deposition). Biodegradability of EDDS in the three soils varied distinctly. This was mainly expressed in the duration of the lag phase prior to metal complex degradation, and not so much in the half life when degradation effectively did set in. Differences in the lag phase were attributed to differences in soil pollution. However, EDDS was fully degraded within a period of 54 d in all soils regardless of initial delay. Assessment of the cation mobilisation patterns in the three soils under study revealed that mainly Ca, Fe and Al can reduce effectiveness of heavy metal mobilisation by competition for complexation.     

Analysis of tree rings using inductively coupled plasma mass spectrometry to record fluctuations in a metal pollution episode

Analysis of Acer pseudoplatanus L. (sycamore) tree rings using ICP-MS was used to assess the impact of metal deposition on trees growing in the vicinity of a metal refinery at Prescot, north-west England compared to a reference site at Croxteth 6 km distant receiving minimal deposition. No difference in tree growth between sites was recorded. Large reductions in Cu and Cd deposition since the late 1970s was accompanied by a steep decline in Cd concentrations in the outer rings in trees close to the refinery. A similar reduction in Cu concentrations was less apparent due to a tendency for Cu to increase in the outer rings. Zinc and Ni were higher in xylem at Prescot compared to Croxteth. There was no trend in Zn concentrations at either site although Ni concentrations increased in trees close to the refinery after 1982. Manganese concentrations in xylem were much higher at Prescot; Mn levels declined until the late 1970s and then increased slightly in later years interspersed by large concentration peaks within individual years during the 1980s. There was little change in Mn concentrations in trees at Croxteth during this period. Calcium, Mg and Sr concentrations remained steady or declined slightly in rings formed since 1965 in trees at Croxteth. Concentrations of Ca, Mg and Sr were higher in rings formed prior to the mid 1970s in trees at Prescot, but declined steadily after this period, although peaks in concentrations of each element were recorded in individual years during the 1980s. Phosphorous concentrations in rings increased towards the cambium at Croxteth, although P levels decreased in rings formed after 1982 at Prescot. No difference in K concentrations between sites was recorded. Lead concentrations in xylem at both sites declined steadily in rings formed after 1970, although concentrations were higher at the reference site. Analysis of individual sycamore tree rings appears to record short-term changes in pollution episodes, with little lateral movement of elements occurring. It is suggested that changes in element concentrations in trees close to the refinery are a result of reduced metal deposition combined with increased soil acidity due to reduced buffering capacity of metal ions in rainfall.     

Evaluating three trace metal contaminated sites: a field and laboratory investigation

Selecting guidelines to evaluate elevated metals in urban brownfields is hindered by the lack of information for these sites on ecosystem structure and function. A study was performed to compare three trace metal-contaminated sites in the metropolitan Montreal area. The goal was to obtain an idea of the organisms that may be present on urban brownfields and to measure if elevated metals alter the presence and activity of the indigenous biota. Field and laboratory studies were conducted using simple methodologies to determine the extent to which microbial activity affected by trace metal content, to assess diversity of plant and soil invertebrate communities and to measure phytoaccumulation of trace metals. It was found that microbial activity, as measured by substrate-induced respiration (SIR) and nitrification, was not affected by the levels of soil Cd, Cu, Ni, Pb and Zn recorded on the sites. Seven of the 12 invertebrate groups collected were sampled on soils with similar Cd, Cu, Ni, Pb and Zn concentrations. Diversity of plant species increased as a function of the length of time the sites had been inactive. Levels of metals in plant tissue were influenced by soil characteristics and not by total soil Cd, Cu, Ni, Pb and Zn.     

Accumulation of Mn and Pb in linden (Tilia platyphyllos Scop.) bark and wood

As an indicator of environmental pollution, we collected tree rings and bark of linden (Tilia platyphyllos Scop.) from four sampling locations in Serbia. Mn and Pb were determined with a spectrochemical method that has an argon-stabilized U-shaped DC arc with aerosol supply as excitation source. Increased concentrations of Mn in linden tree rings and bark were found at the Debeli Lug location, where the Mn transfer factors were largest. The availability of Mn in soil and tree rings was greatly influenced by pH. Since 1950, Mn level decreased more noticeably on acidic soils. Higher concentrations of Pb were found in linden tree rings and bark at the locations Fru?ka Gora and Zemun. Proximity of the road to Novi Sad at both sites may be a possible reason for this. The Pb transfer factor was highest at Fru?ka Gora. The ratio of bioavailable elements in soil for Mn and Pb were also calculated. Close correlations between Mn and Pb concentrations in linden tree rings and the ratio of bioavailable elements in soil were seen at all four locations.     

Trace metal speciation and bioavailability in urban soils

Urban soils often contain concentrations of trace metals that exceed regulatory levels. However, the threat posed by trace metals to human health and the environment is thought to be dependent on their speciation in the soil solution rather than the total concentration. Three inactive railway yards in Montréal, Québec, were sampled to investigate the speciation and bioavailability of Cd, Cu, Ni, Pb and Zn. Soil solutions were obtained by centrifuging saturated soil pastes. In the soil solutions, up to 59% of the dissolved Cd was in its free ionic form. For Cu, Pb and Zn, organic complexes were the predominant species. Over 40% of Ni was present as inorganic complexes if the solution pH exceeded 8.1. Multiple regression analyses showed that pH and total metals in soil were significantly correlated with the activities of free metal ions, except for Cd(2+), which only had a weak correlation with soil pH. Free, dissolved and total soil metals were tested for their ability to predict metal uptake by plants in the field. However, none of these metal pools were satisfactory predictors. The results indicated that in these urban soils, trace metals were mainly in stable forms and bioavailability was extremely low.     

Metal partitioning and uptake in central Ontario forests

Evaluation of the potential environmental risk posed by metals depends to a great extent on modeling the fate and mobility of metals with soil-solution partitioning coefficients (Kd). However, the effect of biological cycling on metal partitioning is rarely considered in standard risk assessments. We determined soil-solution partitioning coefficients for 5 metals (Cd, Zn, Pb, Co and Ni) at 46 forested sites that border the Precambrian Shield in central Ontario, where soil pHaq varied from 3.9 to 8.1. Foliage from the dominant tree species and forest floor samples were also collected from each site to compare their metal levels with Kd predictions. Analogous to other studies, log Kd values for all metals were predicted by empirical linear regression with soil pH (r2=0.66-0.72), demonstrating that metal partitioning between soil and soil solution can be reliably predicted for relatively unpolluted forest mineral soils by soil pH. In contrast, whereas the so-called bioavailable water-soluble metal fraction could be predicted from soil pH, metal concentrations in foliage and the forest floor at each site were not consistently related to pH. Risk assessment of metals should take into account the role of biota in metal cycling and partitioning in forests, particularly if metal bio-accumulation and chronic toxicity in the food chain, rather than metal mobility in soils, are of primary concern.     

Comparison of EDTA and EDDS as potential soil amendments for enhanced phytoextraction of heavy metals

Phytoextraction has been proposed as an alternative remediation technology for soils polluted with heavy metals or radionuclides, but is generally conceived as too slow working. Enhancing the accumulation of trace pollutants in harvestable plant tissues is a prerequisite for the technology to be practically applicable. The chelating aminopolycarboxylic acid, ethylene diamine tetraacetate (EDTA), has been found to enhance shoot accumulation of heavy metals. However, the use of EDTA in phytoextraction may not be suitable due to its high environmental persistence, which may lead to groundwater contamination. This paper aims to assess whether ethylene diamine disuccinate (EDDS), a biodegradable chelator, can be used for enhanced phytoextraction purposes. A laboratory experiment was conducted to examine mobilisation of Cd, Cu, Cr, Ni, Pb and Zn into the soil solution upon application of EDTA or EDDS. The longevity of the induced mobilisation was monitored for a period of 40 days after application. Estimated effect half lives ranged between 3.8 and 7.5 days for EDDS, depending on the applied dose. The minimum observed effect half life of EDTA was 36 days, while for the highest applied dose no decrease was observed throughout the 40 day period of the mobilisation experiment. Performance of EDTA and EDDS for phytoextraction was evaluated by application to Helianthus annuus. Two other potential chelators, known for their biodegradability in comparison to EDTA, were tested in the plant experiment: nitrilo acetic acid (NTA) and citric acid. Uptake of heavy metals was higher in EDDS-treated pots than in EDTA-treated pots. The effects were still considered insufficiently high to consider efficient remediation. This may be partly due to the choice of timing for application of the soil amendment. Fixing the time of application at an earlier point before harvest may yield better results. NTA and citric acid induced no significant effects on heavy metal uptake.     

The distribution of metals in the forest floor of aged conifer stands at a plantation in Northern England

The distribution of the elements Cd, Cr, Cu, Mn, Ni, Pb, Sr, V and Zn has been examined in the horizons of soils under aged Sitka spruce (Picea sitchensis (Bong.) Carr.) stands at a plantation in Northern England. The stands are under first-generation cultivation and are up to 33 years old. Cadmium, Mn, Pb and Zn concentrations were consistently higher in the organic layers than in the underlying mineral soil. This contrasted with the situation for Sr and V. Cadmium, Pb and Zn all showed an increase in concentration in the L + F horizons with stand age and a corresponding increase in the difference between L + F horizon concentrations. Soil pH declined with increasing stand age. Cadmium, Cr, Pb and Zn were all present at higher concentrations in the F horizon than in any other, while Cu and Ni were relatively constant through all the horizons studied. For all nine elements, the H horizon was the largest store of the three organic layers. Calculated rates of accumulation of Cd, Pb and Zn in the L + F horizons gave good agreement with estimated regional atmospheric deposition rates. In comparison to atmospheric deposition, biological mobilisation and deposition of Cd, Pb and Zn make a relatively minor contribution to the surface soil metal burden. Cadmium appeared to be the most readily leached of these three metals from the forest floor, although some transfer of atmospherically-derived Pb to the H+ soil horizons was indicated.     

Trace metal distribution in sediments of the Pearl River Estuary and the surrounding coastal area, South China

Surface sediments and sediment cores collected at the Pearl River Estuary (PRE) and its surrounding coastal area were analysed for total metal concentrations, chemical partitioning, and Pb isotopic compositions. The distribution of Cu, Cr, Pb, and Zn demonstrated a typical diffusion pattern from the land to the direction of the sea. Two hotspots of trace metal contamination were located at the mixed zone between freshwater and marine waters. The enrichment of metals in the sediments could be attributed to the deposition of the dissolved and particulate trace metals in the water column at the estuarine area. The similar Pb isotopic signatures of the sediments at the PRE and its surrounding coastal area offered strong evidence that the PRE was a major source of trace metals to the adjacent coastal area. Slightly lower (206)Pb/(207)Pb ratios in the coastal sediments may indicate other inputs of Pb in addition to the PRE sources, including the inputs from Hong Kong and other parts of the region.     

Storage and distribution of trace metals and spheroidal carbonaceous particles (SCPs) from atmospheric deposition in the catchment peats of Lochnagar, Scotland.

Lochnagar is a remote mountain lake to the south-east of the Cairngorm region in Scotland. Its catchment receives anthropogenic trace metals solely from atmospheric deposition. Ten peat cores were taken from the catchment and analysis confirmed that they have been contaminated by trace metals. The peats have an high affinity for trace metals and this results in metal accumulation in the surface peat layers. The formation of trace metal sulphides may also reduce remobilisation. In this way, trace metals derived from atmospheric deposition have been scavenged and accumulated. In contaminated peat layers, 77.4% Hg, 89.6% Pb, 93.4% Cu, 72.4% Zn and 86.5% Cd of the total stored are from anthropogenic sources. The accumulated trace metals in the peats can potentially influence the lake system through erosion. Spheroidal carbonaceous particle (SCP) profiles were used to date the peat cores. By referring to the SCP profiles in the peats and comparing these with the trace metal profiles in the lake sediments, the mobility of trace metals in the catchment peats is confirmed.     

Leaching of heavy metals from contaminated soils using EDTA

Ethylenediaminetetraacetic acid (EDTA) extraction of Zn, Cd, Cu and Pb from four contaminated soils was studied using batch and column leaching experiments. In the batch experiment, the heavy metals extracted were virtually all as 1:1 metal-EDTA complexes. The ratios of Zn, Cd, Cu and Pb of the extracted were similar to those in the soils, suggesting that EDTA extracted the four heavy metals with similar efficiency. In contrast, different elution patterns were obtained for Zn, Cd, Cu and Pb in the column leaching experiment using 0.01 M EDTA. Cu was either the most mobile or among the most mobile of the four heavy metals, and its peak concentration corresponded with the arrival of full strength EDTA in the leachate. The mobility of Zn and Cd was usually slightly lower than that of Cu. Pb was the least mobile, and its elution increased after the peaks of Cu and Zn. Sequential fractionations of leached and un-leached soils showed that heavy metals in various operationally defined fractions contributed to the removal by EDTA. Considerable mobilisation of Fe occurred in two of the four soils during EDTA leaching. Decreases in the Fe and Mn oxide fraction of heavy metals after EDTA leaching occurred in both soils, as well as in a third soil that showed little Fe mobilisation. The results suggest that the lability of metals in soil, the kinetics of metal desorption/dissolution and the mode of EDTA addition were the main factors controlling the behaviour of metal leaching with EDTA.     

Trace metal contents in Parmelia caperata (L.) Ach. compared to bulk deposition,throughfall and leaf-wash fluxes in two holm oak forests in Montseny (NE Spain)

The metal concentrations of V, Cr, Co, Ni, Cu, Zn, Cd, Hg and Pb were analysed in distilled water extracts of Parmelia caperata and in bulk deposition, throughfall and an experimental in situ washing of leaves at two forests at Montseny (NE Spain) submitted to differential exposure to the industrial and traffic activities around Barcelona. Lichen concentrations of Zn, Cu, V, and Cd were higher at the site of greater exposure to pollutants. Consistently, there was higher dry deposition of these metals at the more exposed site. The order of abundance of trace metals in the lichen was similar to that in the deposition variables, although Pb and Cu had intermediate concentrations in the lichen but were very low in the deposition measurements. This indicated the higher affinity of Pb and Cu for the exchange sites in the lichen cell wall and the fact that lichens accumulated Pb for the last 12–18 y when emissions were much higher than today. The ability of Parmelia caperata to indicate the deposition of heavy metals, together with its easy sampling and handling, its broad distribution and its easy identification suggest that the lichen extract procedure described here could be used to establish gradients of atmospheric deposition of heavy metals at a general geographic level.     

Bioaccumulation of elements in bryophytes from Serra da Estrela, Portugal, and Veluwezoom, the Netherlands

Background, Aims and Scope Pollution by heavy metals over large areas and long periods of time may cause chronic damage to living organisms and must be carefully controlled. One way to determine the extent of environmental contamination is by measuring the levels of contaminants in plants. The use of mosses as biomonitors is a convenient method to determine levels of (atmospheric) deposition, as terrestrial mosses obtain most of their supply of mineral elements from precipitation and dry deposition of airborne particles. Mosses have therefore received increasing attention as a suitable tool for monitoring regional patterns of elemental deposition from the atmosphere in large-scale studies in various countries, in areas close to industrial installations as well as in areas not expected to be contaminated. Although this technique is widely known, ecological studies of this type have rarely been done in Portugal. The aim of this paper is to evaluate and compare the spatial distribution of heavy metals in Hypnum cupressiforme, Pleurozium schreberi, Dicranum scoparium and Polytrichum piliferum collected from the Serra da Estrela natural park in Portugal and in the Veluwezoom natural park in the Netherlands. The selected species are the most widely used bryophytes for biomonitoring in the boreal region. The popularity of these species for this purpose is due to their wide ecological amplitude and distribution.Methods At 54 sampling sites in both nature parks, samples of Hypnum cupressiforme, Pleurozium schreberi, Dicranum scoparium and Polytrichum piliferum were collected. Plant digests were analysed for Al, Ba, Ca, Cr, Fe, K, Mg, Mn, Ni, Sr, V, Zn, Pb, Cu, Cd, N and P. Differentiations between sampling sites in terms of concentrations of elements in mosses were evaluated by ANOVA and the least significant difference was calculated. The normality of the analysed features was checked with the chi square test. After standardization, the matrix of 54 samples and 10 heavy metals was subjected to numerical classification to detect groups of samples with similar patterns of metal concentrations. The clustering algorithm was prepared with Ward’s method, and the City Block Manhattan method was used for the similarity measure. Metals and samples were also subjected to ordination to reveal possible gradients of heavy metal levels, using PCA. Correlations were calculated between concentrations of metals and factors 1 and 2, allowing the dependence between the concentration of metals and factors (factor loading) to be estimated.Results and Discussion All species examined in both areas contained elevated levels of Mn and Pb. For each particular species, concentrations of N, P and Pb were significantly higher at Serra da Estrela, while concentrations of Cu were significantly higher at the Veluwezoom. Mosses from Portugal and the Netherlands differed significantly mainly in the concentrations of Al, Ba, Cr, Fe, Mn, Ni, Pb and V. This differentiation did not exceed that within the mosses from Portugal.Conclusions Mosses from Portugal and the Netherlands differ significantly mainly in the concentrations of Al, Ba, Cr, Fe, Mn, Ni, Pb and V. This differentiation does not exceed the differentiation within the mosses from Portugal.Recommendation and Outlook Further research is required into the origin and deposition of the polluting elements in other environmental compartments.     

The organic carbon derived from sewage sludge as a key parameter determining the fate of trace metals

In a sandy agricultural soil of south-west of France, continuously cultivated with maize and amended with sewage-sludge over 20 years, the behavior of three trace metals (Cu, Pb, and Zn) was studied during the sludge applications (1974-1993) and after its cessation (1993-1998). Using the delta13C analysis, the dynamics of different sources of organic matter were followed in order to elucidate the influence of the sludge-derived organic matter on the fate of trace metals in the soil and its particle size fractions. This study revealed that sludge-derived organic matter contributed to the formation of macroaggregates through the binding of preexisting microaggregates. These macroagreggates were thus responsible for the accumulation of trace metals in the coarsest fraction as well as for the protection of maize-derived organic matter against biodegradation. After sludge application ceased, the disaggregation of macroaggregates occurred simultaneously with high losses in Cu and Pb. On the contrary, Zn appeared less affected by the cessation of sludge application, with only a location change from coarse to fine fractions.     

Contaminant trends in soils and crops

The evidence for long-term changes in the contaminant content of soils and crops is reviewed. Heavy metals, acidification and trace organic contaminants are each considered separately, with the emphasis placed on changes brought about by inputs from long-term atmospheric deposition. It is argued that effectively all soils in industrialised countries have become contaminated with selected trace substances (notably Pb, Cd, polynuclear aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and polychlorinated dibenzo-p-dioxins and -furans) above their true (historical) background level by aerial inputs. In the case of Pb, for example, cumulative deposition inputs over several centuries have probably roughly doubled the Pb burden of contemporary UK surface soils. Despite this, there is little evidence for a concomitant rise in the contaminant content of UK crops through the twentieth century. In fact, the burden of many contaminants in vegetation may well be somewhat lower than in earlier decades of this century because (1) crop composition is strongly influenced by direct deposition onto the above-ground portion of the plant, (2) root uptake and translocation of soil-borne heavy metals and recalcitrant organic contaminants are inefficient processes, and (3) UK air quality has generally improved over the last 10-20 years. Acidification of soils is of considerable regional significance. The evidence for changes in soil pH over this century is reviewed, and it is concluded that atmospheric inputs have enhanced the rate of soil acidification over large areas of Scandinavia and elsewhere.     

Distribution of metals in grassland soils following surface applications of sewage sludge

In order to decide on a suitable sampling depth for grassland soil treated with sewage sludge and to assess implications for grazing animals, a field trial on two soils was designed to estimate the distribution of metals in grassland soil profiles following surface applications of sludge. Thus the sites represented permanent grassland where no form of cultivation had taken place. Soil cores were taken using specialised equipment to 30 cm depth and divided into seven sections. Movement from the soil surface to a depth of 10 cm was observed for all of the seven metals, Cd, Cr, Cu, Mo, Ni, Pb and Zn, but most of the metal (60%-100%, mean 87%) remained in the upper 5 cm of soil. It was concluded that sampling to a depth of 5 or 7.5 cm would be most suitable for monitoring long-term grassland treated with surface applications of sludge.     

Influence of organic acids on the transport of heavy metals in soil

Vegetation historically has been an important part of reclamation of sites contaminated with metals, whether the objective was to stabilize the metals or remove them through phytoremediation. Understanding the impact of organic acids typically found in the rhizosphere would contribute to our knowledge of the impact of plants in contaminated environments. Heavy metal transport in soils in the presence of simple organic acids was assessed in two laboratory studies. In the first study, thin layer chromatography (TLC) was used to investigate Zn, Cd, and Pb movement in a sandy loam soil as affected by soluble organic acids in the rhizosphere. Many of these organic acids enhanced heavy metal movement. For organic acid concentrations of 10mM, citric acid had the highest R(f) values (frontal distance moved by metal divided by frontal distance moved by the solution) for Zn, followed by malic, tartaric, fumaric, and glutaric acids. Citric acid also has the highest R(f) value for Cd movement followed by fumaric acid. Citric acid and tartaric acid enhanced Pb transport to the greatest degree. For most organic acids studied, R(f) values followed the trend Zn>Cd>Pb. Citric acid (10mM) increased R(f) values of Zn and Cd by approximately three times relative to water. In the second study, small soil columns were used to test the impact of simple organic acids on Zn, Cd, and Pb leaching in soils. Citric acid greatly enhanced Zn and Cd movement in soils but had little influence on Pb movement. The Zn and Cd in the effluents from columns treated with 10mM citric acid attained influent metal concentrations by the end of the experiment, but effluent metal concentrations were much less than influent concentrations for citrate <10mM. Exchangeable Zn in the soil columns was about 40% of total Zn, and approximately 80% total Cd was in exchangeable form. Nearly all of the Pb retained by the soil columns was exchangeable.     

Simulating the long-term chemistry of an upland UK catchment: heavy metals

CHUM-AM was used to investigate the behaviours of atmospherically-deposited heavy metals (Ni, Cu, Zn, Cd and Pb) in three moorland sub-catchments in Cumbria UK. The principal processes controlling cationic metals are competitive partitioning to soil organic matter, chemical interactions in solution, and chemical weathering. Metal deposition histories were generated by combining measured data for the last 30 years with local lake sediment records. For Ni, Cu, Zn and Cd, default parameters for the interactions with organic matter provided reasonable agreement between simulated and observed present-day soil metal pools and average streamwater concentrations. However, for Pb, the soil binding affinity in the model had to be increased to match the observations. Simulations suggest that weakly-sorbing metals (Ni, Zn, Cd) will respond on timescales of decades to centuries to changes in metal inputs or acidification status. More strongly-sorbing metals (Cu, Pb) will respond over centuries to millennia.