Long-term trends in water chemistry of acid-sensitive Swedish lakes show slow recovery from historic acidification

Long-term (1987–2012) water quality monitoring in 36 acid-sensitive Swedish lakes shows slow recovery from historic acidification. Overall, strong acid anion concentrations declined, primarily as a result of declines in sulfate. Chloride is now the dominant anion in many acid-sensitive lakes. Base cation concentrations have declined less rapidly than strong acid anion concentrations, leading to an increase in charge balance acid neutralizing capacity. In many lakes, modeled organic acidity is now approximately equal to inorganic acidity. The observed trends in water chemistry suggest lakes may not return to reference conditions. Despite declines in acid deposition, many of these lakes are still acidified. Base cation concentrations continue to decline and alkalinity shows only small increases. A changing climate may further delay recovery by increasing dissolved organic carbon concentrations and sea-salt episodes. More intensive forest harvesting may also hamper recovery by reducing the supply of soil base cations.     

Modeling recovery of Swedish ecosystems from acidification

Dynamic models complement existing time series of observations and static critical load calculations by simulating past and future development of chemistry in forest and lake ecosystems. They are used for dynamic assessment of the acidification and to produce target load functions, that describe what combinations of nitrogen and sulfur emission reductions are needed to achieve a chemical or biological criterion in a given target year. The Swedish approach has been to apply the dynamic acidification models MAGIC, to 133 lakes unaffected by agriculture and SAFE, to 645 productive forest sites. While the long-term goal is to protect 95% of the area, implementation of the Gothenburg protocol will protect approximately 75% of forest soils in the long term. After 2030, recovery will be very slow and involve only a limited geographical area. If there had been no emission reductions after 1980, 87% of the forest area would have unwanted soil status in the long term. In 1990, approximately 17% of all Swedish lakes unaffected by agriculture received an acidifying deposition above critical load. This fraction will decrease to 10% in 2010 after implementation of the Gothenburg protocol. The acidified lakes of Sweden will recover faster than the soils. According to the MAGIC model the median pre-industrial ANC of 107 microeq L(-1) in acid sensitive lakes decreased to about 60 microeq L(-1) at the peak of the acidification (1975-1990) and increases to 80 microeq L(-1) by 2010. Further increases were small, only 2 microeq L(-1) between 2010 and 2040. Protecting 95% of the lakes will require further emission reductions below the Gothenburg protocol levels. More than 7000 lakes are limed regularly in Sweden and it is unlikely that this practice can be discontinued in the near future without adverse effects on lake chemistry and biology.     

Recovery from acidification in Swedish forest streams

Sulphur deposition in Sweden has decreased to less than half of the levels recorded in 1970 and now signs of recovery from acidification of surface waters are beginning to appear. We investigated time trends of water chemistry between 1985 and 1998 in 13 streams draining small forested catchments with generally shallow acid sensitive soils. At nine of the catchments, bulk deposition was monitored as well. Sulphate concentrations decreased in both stream water and deposition, although with somewhat smaller trends in stream water compared with deposition. The magnitude of the trends in sulphate increased from north to south, following a gradient of increasing industrial influence. Five sites in the southern half of the country showed weak signs of recovery from acidification in terms of increasing concentrations of acid neutralising capacity and decreasing concentrations of hydrogen ions, corresponding to annual increases of 0.01 pH units. Changes in stream discharge and concentrations of marine salts and organic acids could not explain the observed decrease in acidity and the results were interpreted as recovery from anthropogenic acidification. For the northern half of Sweden, any changes in water chemistry could be attributed to natural variation in climate and marine influence, and the effect of anthropogenic acidification was negligible.     

Dynamic modelling of recovery from acidification of lakes in Killarney Park,Ontario, Canada

During much of the 1900s, the lakes in Killarney Provincial Park have been exposed to high levels of acid deposition due to sulfur emissions from the nearby metal smelters in Sudbury. The sulfur emissions from this large point source have decreased to about 10% of what they were in the 1960s. Lake water quality in Killarney Park has greatly changed in response to reduced emissions, with noticeable declines in sulfate, aluminum and calcium concentrations. Here we apply the dynamic acidification model MAGIC to 3 lakes in Killarney Park. The lakes, which have different buffering capacities and response times, were selected to represent fast, intermediate and slow recovery from acidification. The model was calibrated to match observed data for the lakes and 4 different forecast scenarios for future sulfur deposition reductions were applied. The results indicate that there is still a large potential for improvement in the water quality in Killarney. The recovery time for the different lakes varies greatly. For the lake having the slowest response time several decades are needed for the chemistry to stabilize after implementation of deposition reductions.     

Evidence of biological recovery in acid-stressed lakes near Sudbury, Canada

Reductions in the emissions of SO2 and trace metals from the Sudbury smelters have resulted in substantial improvements in water quality in many surrounding lakes. Significant biological changes have accompanied the chemical improvements. Evidence of relatively rapid recovery was found for benthic filamentous algae, phytoplankton, zooplankton, mobile species of benthic invertebrates, and some fish populations. Organisms with low dispersal ability (e.g. Hyalella azteca) have not yet recolonized these lakes. The partial recovery observed to date shows movement toward re-establishment of biological communities typical of natural Precambrian Shield lakes in this area. These findings offer strong support for further efforts to reduce industrial emissions of pollutants to the atmosphere.     

Mercury in fish in Swedish lakes

The aim of this work has been to try to obtain a picture of the past, present and future mercury situation in fish in Swedish lakes, to make an estimate of the number of lakes threatened by 'blacklisting', and to see if the data can be used to reveal anything about the impact of liming on the Hg content in pike. The register contains a broad set of data from 1456 lakes. The main results are as follows. Trend analyses indicate that the Hg content in 1-kg pike seems to increase with time. This is interesting since there has been a significant decrease in mercury emissions from Swedish industries during the last two decades. High Hg contents in 1-kg pike appear in a very characteristic pattern, linked to specific sources of Hg emission. The data indicate that old Swedish 'sins' are still causing a lot of problems. The factors governing the leakage of Hg from soils to water ought to be a very important topic for further studies. The Hg content in pike shows the highest correlation with the following parameters: Hg in surficial sediments, pH, distance from point source and water hardness, lake water alkalinity and conductivity, water retention time, size of drainage area and lake surface. A formula which provides the best possible degree of explanation (r2 = 0.78) has been derived. At present there are about 250 lakes 'blacklisted' in Sweden due to high Hg content in fish. Our data show that there are at least 9400 lakes that ought to be 'blacklisted' today. A successful liming operation will alter the chemical conditions in lakes and also decrease the Hg content in fish.     

Tracing recovery from acidification in the western Norwegian Nausta watershed

A novel method, redundancy analysis (RDA), has been used to examine whether chemical recovery from acidification in the western Norwegian Nausta watershed produces detectable recovery within the community structure of the macro-zoobenthos. The RDA results have been compared with measures of recovery based on the changes detected using highly specialized and regionally defined biological acidity indices. We found that the beginning of biological recovery in the Nausta watershed was recognizable during the period 1989-1998. Recovery occurred in the upper reaches and in the tributaries. The multivariate approach proved to complement the acidity indices approach, and much biological information can be gained by their combined use. The RDA method is conservative, i.e. does not overestimate biological recovery, and it is not geographically constrained as are the acidity indices. We also found that seasonal climatic factors strongly influence the benthic community, and may confound the detection of the biological recovery process.     

Bioaccumulation of decamethylcyclopentasiloxane in perch in Swedish lakes

Decamethylcyclopentasiloxane (D5), a high production volume chemical used in personal care products, enters the environment both via air and sewage treatment plant (STP) recipients. It has been found in fish, and there is concern that it may be a bioaccumulative substance. In this work D5 was analyzed in perch from six Swedish lakes that did not receive STP effluent, and in perch and sediment from six lakes that received STP effluent. In the lakes receiving the STP effluent, the D5 concentrations in sediment varied over three orders of magnitude and were correlated with the number of persons connected to the STP normalized to the surface area of the receiving body. In the lakes not receiving effluent, the D5 levels in perch were all below the LOQ, while D5 was above the LOQ in almost all perch from lakes that received effluent. The D5 concentrations in perch and sediment from the lakes receiving STP effluent were correlated. This shows that STP effluent is a much more important source of D5 to aquatic ecosystems than atmospheric deposition, and that the risk of adverse effects of D5 on aquatic life will be greatest in small recipients receiving large amounts of STP effluent. The bioaccumulation of D5 was compared to that of PCB 180 on the basis of multimedia bioaccumulation factors (mmBAFs), which describe the fraction of the contaminant present in the whole aquatic environment (i.e. water and surface sediment) that is transferred to the fish. In four of the six lakes the mmBAF of D5 was >0.3 of the mmBAF of PCB 180. Given that PCB 180 is a known highly bioaccumulative chemical, this indicates that the bioaccumulation of D5 in perch is considerable.     

Reversibility of stemflow-induced soil acidification in Swedish beech forest

Stemwater running down the trunks of beech (Fagus sylvatica L.) has an acidifying effect on soil near the stem. The deposition of acidifying substances may be two to four times higher close to the stem compared to in the stand in general. To study reversibility of soil acidification, 72 stumps of beech trees were chosen from five different year classes of felling (3, 6, 9, 14-15, 25-30), representing the years when stemflow ceased to affect the soil. The H(+) concentration (pH KCl) in the topsoil (0-5 cm) differed between the distances 10-30 cm and 230-250 cm from the stumps, the soil close to the stem being more acid. The longer the time since felling the smaller the differences in H(+) concentration became. This reduction in soil acidity amounted to ca. 50% after 15 years, and only small further changes occurred over the next ten years. This indicates that soil may not recover fully from acidification, or does so at a rather slow rate after the initial 15 years of recovery.     

Developing conceptual frameworks for the recovery of aquatic biota from acidification

Surface water acidity is decreasing in large areas of Europe and North America in response to reductions in atmospheric S deposition, but the ecological responses to these water-quality improvements are uncertain. Biota are recovering in some lakes and rivers, as water quality improves, but they are not yet recovering in others. To make sense of these different responses, and to foster effective management of the acid rain problem, we need to understand 2 things: i) the sequence of ecological steps needed for biotic communities to recover; and ii) where and how to intervene in this process should recovery stall. Here our purpose is to develop conceptual frameworks to serve these 2 needs. In the first framework, the primarily ecological one, a decision tree highlights the sequence of processes necessary for ecological recovery, linking them with management tools and responses to bottlenecks in the process. These bottlenecks are inadequate water quality, an inadequate supply of colonists to permit establishment, and community-level impediments to recovery dynamics. A second, more management-oriented framework identifies where we can intervene to overcome these bottlenecks, and what research is needed to build the models to operationalize the framework. Our ability to assess the benefits of S emission reduction would be simplified if we had models to predict the rate and extent of ecological recovery from acidification. To build such models we must identify the ecological steps in the recovery process. The frameworks we present will advance us towards this goal.     

Effects of experimental acidification on mobilisation of metals from sediments of limed and non-limed lakes

In order to study the influence of pH on the mobilisation of metals from lake sediments, intact sediment cores with overlying water were sampled from one lime treated lake and one acidified lake. The overlying water of two cores from each lake was successively acidified to pH 4.2 over a period of 3 months. In the acid treated samples from the limed lake, the initial concentrations of Al, Cd, Mn, Pb and Zn in the overlying water were generally lower and the final concentrations were higher than in the acid treated samples from the acidified lake. The labile inorganic fraction of Al (Al(i)) was increasingly dominating as pH decreased. Redox potential and pH in the sediment indicated that the upper two centimetres were involved in the exchange reactions. The experiment showed that mobilisation of metals from sediments can occur and the results indicated that mobilisation could contribute to increased concentrations of metals in lake water during reacidification of formerly lime treated lakes.     

Mercury pollution trends in subarctic lakes in the northern Swedish mountains

Despite many years of research about mercury pollution, data concerning high-latitude regions of Europe are limited, particularly studies of long-term temporal trends. It is not clear whether the mercury load at high latitudes follows the recent decreasing trends in European mercury emissions or whether the load is still high because of continuing global emissions. In this study we use sediments from 12 lakes, located above the Arctic Circle in the Swedish mountains, to assess the past and recent mercury pollution situation, especially for the last 200 y. The mercury load increased clearly in sediment deposited from the late 19th or early 20th century to a peak between 1960 and 1990. This peak represents an enrichment of 1.4 to 4.2 times over background concentrations. This enrichment is comparable with enrichments in sediments from lower latitudes as well as other Arctic regions. Since the 1990s mercury concentration has declined in 8 of the 12 lakes, i.e., similar to emission trends in Europe.     

Timescales of recovery from acidification: Implications of current knowledge for aquatic organisms

Current understanding of the mechanisms of recovery of surface waters from acidification leads to several conclusions which must be considered when devising emission control strategies. Recovery can be regarded as being in two stages: an initial phase in which the waters respond to the reduced SO4(2-) deposition, and a second phase which depends on recovery of the soil base status. If an acceptable water quality is not produced in the first phase, recovery will be extremely slow, taking centuries. This may be true of very sensitive areas such as S Norway. Faster and deeper emission reductions will not significantly speed recovery in these situations: liming is then the only practicable method. Areas where the weathering rate is higher will recover faster, and here recovery may be delayed (by decades) by two poorly understood processes-release of SO4(2-) and release of organic acids from soils. Research on the control of these processes and on the extent of lake resource in each category is urgently needed.     

Widespread waterborne pollution in central Swedish lakes and the Baltic Sea from pre-industrial mining and metallurgy

Metal pollution is viewed as a modern problem that began in the 19th century and accelerated through the 20th century; however, in many parts of the globe this view is wrong. Here, we studied past waterborne metal pollution in lake sediments from the Bergslagen region in central Sweden, one of many historically important mining regions in Europe. With a focus on lead (including isotopes), we trace mining impacts from a local scale, through a 120-km-long river system draining into Mälaren - Sweden's third largest lake, and finally also the Baltic Sea. Comparison of sediment and peat records shows that pollution from Swedish mining was largely waterborne and that atmospheric deposition was dominated by long-range transport from other regions. Swedish ore lead is detectable from the 10th century, but the greatest impact occurred during the 16th-18th centuries with improvements occurring over recent centuries, i.e., historical pollution > modern industrial pollution.     

Assessing the recovery of lakes in southeastern Canada from the effects of acidic deposition

Reductions in North American sulfur dioxide (SO2) emissions promoted expectations that aquatic ecosystems in southeastern Canada would soon recover from acidification. Only lakes located near smelters that have dramatically reduced emissions approach this expectation. Lakes in the Atlantic provinces, Quebec and Ontario affected only by long-range sources show a general decline in sulfate (SO4(2-)) concentrations, but with a relatively smaller compensating increase in pH or alkalinity. Several factors may contribute to the constrained (or most likely delayed) acidity response: declining base cation concentrations, drought-induced mobilization of SO4(2-), damaged internal alkalinity generation mechanisms, and perhaps increasing nitrate or organic anion levels. Monitoring to detect biological recovery in southeastern Canada is extremely limited, but where it occurs, there is little evidence of recovery outside of the Sudbury/Killarney area. Both the occurrence of Atlantic salmon in Nova Scotia rivers and the breeding success of Common Loons in Ontario lakes are in fact declining although factors beyond acidification also play a role. Chemical and biological models predict that much greater SO2 emission reductions than those presently required by legislation will be needed to promote widespread chemical and latterly, biological recovery. It may be unrealistic to expect that pre-industrial chemical and biological conditions can ever be reestablished in many lakes of southeastern Canada.     

Littoral microcrustacean (Cladocera and Copepoda) indicators of acidification in Canadian Shield lakes

We identify littoral microcrustacean indicators of acidification in 2 surveys of Canadian Shield lakes conducted 10 years apart. We found a total of 90 cladoceran and copepod species with richness increasing severalfold from acidic to nonacidic lakes. The fauna of the nonacidic lakes differed between the surveys. The 1987 survey employed activity traps, and caught more littoral taxa than the more recent, net-haul-based survey. Similar faunas were identified in the acidified lakes in both surveys, and several good indicator species were identified. For example, Acanthocycops vernalis was restricted to lakes with pH < 6. Sinobosmina sp. was very common but only in lakes with pH > 4.8. Tropocyclops extensus, Mesocyclops edax, and Sida crystallina were commonly found but only at pH > 5, and Chydorus faviformis only at pH > 5.9. These indicators showed promise in gauging the early stages of recovery from acidification in 3 lakes that were included in both surveys.     

Enhanced biological phosphorus removal and recovery

Activated sludge systems designed for enhanced nutrient removal are based on the principle of altering anaerobic and aerobic conditions for growth of microorganisms with a high capacity of phosphorus accumulation. Most often, filamentous bacteria constitute a component of the activated sludge microflora. The filamentous microorganisms are responsible for foam formation and activated sludge bulking. The results obtained confirm unanimously that the filamentous bacteria have the ability of phosphorus uptake and accumulation as polyphosphates. Hydrodynamic disintegration of the foam microorganisms results in the transfer of phosphorus and metal cations and ammonium-nitrogen into the liquid phase. It was demonstrated that the disintegration of foam permits the removal of a portion of the nutrients in the form of struvite.     

Methane emission from lakes

A physico-chemical model to describe methane and carbon dioxide emission from lakes was developed. The model describes the emission by diffusion, bubbles and plants. The intensity of the fluxes can be calculated either for total or particular emission in dependence on gas bubbles composition. It was found, that diffusional (Q) and bubble (J) fluxes depend on the methane molar ratio (X) in bubbles as follows: [formula: see text]. The model allows to estimate the role of the methane oxidation by atmospheric oxygen in the total methane flux. It was shown, that the methane oxidation does not influence much methane fluxes to the atmosphere for most of the experimentally observed situations.     

The Solling roof revisited--slow recovery from acidification observed and modeled despite a decade of "clean-rain" treatment

Soil chemistry under the Solling clean-rain roof was simulated using the dynamic multi-layer soil chemistry model SAFE, including sulfate adsorption. Soil was sampled in order to parameterize the pH and sulfate concentration dependent sulfate adsorption isotherm used in SAFE. Modeled soil solution chemistry was compared to the 14 year long time-series of monthly measurements of soil solution data at 10 and 100cm depth. The deposition of N and S under the roof has been reduced by 68% and 53%, respectively, compared to the surrounding area. Despite this the soil solution concentrations of sulfate are still high (a median of 420mumol(c)/L at 100cm depth between 2000 and 2002) and the soil base saturation low (approximately 3% in the whole profile in 1998). Sulfate adsorption is an important process in Solling. The soil capacity to adsorb sulfate is large, the modeled adsorbed pool in 2003 down to 100cm was 1030kg S/ha, and the measured sulfate concentration is high, due to release of adsorbed sulfate. The addition of sulfate adsorption improved the modeled sulfate dynamics although the model still slightly underestimated the sulfate concentration at 100cm. Model predictions show no recovery, based on the criteria of Bc/Al ratio above 1 in the rooting zone, before the year 2050, independent of future deposition cuts.     

Temporal change estimation of mercury concentrations in northern pike (Esox lucius L.) in Swedish lakes

Adequate temporal trend analysis of mercury (Hg) in freshwater ecosystems is critical to evaluate if actions from the human society have affected Hg concentrations ([Hg]) in fresh water biota. This study examined temporal change in [Hg] in Northern pike (Esox lucius L.) in Swedish freshwater lakes between 1994 and 2006. To achieve this were lake-specific, multiple-linear-regression models used to estimate pike [Hg], including indicator variables representing time and fish weight and their interactions. This approach permitted estimation of the direction and magnitude of temporal changes in 25 lakes selected from the Swedish national database on Hg in freshwater biota. A significant increase was found in 36% of the studied lakes with an average increase in pike [Hg] of 3.7 ± 6.7% per year that was found to be positively correlated with total organic carbon. For lakes with a significant temporal change the dataset was based on a mean of 30 fish, while for lakes with no temporal change it was based on a mean of 13 fish.