Sulphur and nitrogen fluxes and budgets in the Bohemian Forest and Tatra Mountains during the Industrial Revolution (1850-2000)

International audienceMajor fluxes of sulphur and dissolved inorganic nitrogen were estimated in Central European mountain ecosystems of the Bohemian Forest (forest lakes) and Tatra Mountains (alpine lakes) over the industrial period. Sulphur outputs from these ecosystems were comparable to inputs during a period of relatively stable atmospheric deposition (10-35 mmol m-2 yr-1) around the 1930s. Atmospheric inputs of sulphur increased by three- to four-fold between the 1950s and 1980s to ~140 and ~60 mmol mm-2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively. Sulphur outputs were lower than inputs due to accumulation in soils, which was higher in forest soils than in the sparser alpine soils and represented 0.8-1.6 and 0.2-0.3 mol m-2, respectively, for the whole 1930-2000 period. In the 1990s, atmospheric inputs of sulphur decreased 80% and 50% in the Bohemian Forest and Tatra Mountains, respectively, and sulphur outputs exceeded inputs. Catchment soils became pronounced sources of sulphur with output fluxes averaging between 15 and 31 mmol m-2 yr-1. Higher sulphur accumulation in the forest soils has delayed (by several decades) recovery of forest lakes from acidification compared to alpine lakes. Estimated deposition of dissolved inorganic nitrogen was 53-75 mmol m-2 yr-1 in the Bohemian Forest and 35-45 mmol m-2 yr-1 in the Tatra Mountains in the 1880- 1950 period, i.e. below the empirically derived threshold of ~70 mmol m-2 yr-1, above which nitrogen leaching often occurs. Dissolved inorganic nitrogen was efficiently retained in the ecosystems and nitrate export was negligible (0-7 mmol m-2 yr-1). By the 1980s, nitrogen deposition increased to ~160 and ~80 mmol m-2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively, and nitrogen output increased to 120 and 60 mmol m-2 yr-1. Moreover, assimilation of nitrogen in soils declined from ~40 to 10-20 mmol m-2 yr-1 in the alpine soils and even more in the Bohemian Forest, where one of the catchments has even become a net source of nitrogen. In the 1990s, nitrogen deposition decreased by ~30% and DIN output decreased to -2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively. New steady-state conditions, with negligible nitrogen export, could be reached in future but at lower nitrogen depositions than in the 1930s. Keywords: emission, deposition, acidification, nitrogen-saturation, recovery, sulphate, nitrate, ammonium, mountain lake

Modelling reversibility of Central European mountain lakes from acidification: Part I - the Bohemian forest

International audienceA dynamic, process-based acidification model, MAGIC7, has been applied to three small, strongly acidified lakes in the Bohemian Forest, the Czech Republic. The model was calibrated for a set of experimental records on lake water composition over the 1984?2000 period, and produced hindcast concentrations that compared well, even with older (40-year) irregular determinations of nitrate, chloride and pH. Water and soil chemistry forecasts up to 2050 were based on reductions in S and N emissions presupposed by the Gothenburg Protocol. Modelled sulphate and chloride concentrations were predicted to decrease to the levels at the beginning of the 20th century by 2050. The lake water carbonate buffering system is predicted to be re-established in only two lakes (Cerné and Ple?né), with current soil base saturations of 12-15%. Concentrations of ionic aluminium species decreased sharply, from 110 ?eq l-1 in the mid-1980s to the current ~40 ?eq l-1, and were predicted to decrease below 10 ?eq l-1 in the 2020s. Diatom-inferred pH in pre-industrial times was substantially lower than modelled pH. It is suggested that the diatom pH, based almost entirely on non-planktonic species, is biased by inwash of diatoms from more acidic tributaries into the sediment of these small lakes. Generally significant results can be summarised as follows: (1) Simulated sulphate levels agree well with observations during acidification progress and retreat only for values of soil SO42- adsorption capacity three to six times (20 to 40 ?eq kg-1) higher than those found experimentally. This implies a further mechanism of S retention and release in addition to physical sulphate adsorption to Fe and Al oxides of soils. (2) The catchments' ability to retain deposited N appeared to decline after ~1950 but this was not connected with a sufficient change in the C:N ratio of the soils. Agreement between modelled and observed concentrations of nitrate was therefore achieved by empirical restriction of N retention in the soils. Based on their current ability to retain N, the catchments will remain N-saturated and could, temporarily, produce more inorganic N than they receive due to additional nitrate production from soil N-organic pools. This situation has occurred already in the Cerné Lake catchment. (3) Differences in responses of individual lakes can be attributed to different land usages over the past several centuries as well as to differences in geology and primary production. Keywords: MAGIC, atmospheric deposition, N retention, diatom-inferred pH, sulphate, nitrate, base cations, aluminium, Czech Republi

Increasing silicon concentrations in Bohemian Forest lakes

International audienceLong-term trends of dissolved silicon (Si) concentrations in five glacial lakes in the Bohemian Forest, Czech Republic, recovering from acidification show higher mobility of Si from the soil to surface waters despite lower atmospheric deposition of acids. Si increased by 0.95 to 1.95 µmol yr-1 (36 to 51%) from 1986-2004 and with increasing pH. A change in soil solution conditions because of a sharp decrease in acidic deposition has led to marked decline in Al mobility and to considerable decreases in dissolved Al, especially Al3+. The increase in Si may be related to: (1) unblocking of the inhibitory effect of dissolved Al on weathering of aluminosilicates, (2) biogenic opal (phytoliths) dissolving faster, and/or (3) lower Si precipitation as secondary aluminosilicates in soil. The change in Al speciation on the dissolution rate of biogenic silica is critical. A lack of change in Si at sites outside central Europe may be explained by small or no decline in mobility of dissolved Al. The effect of a long-term increase in temperature was probably minor

A modelling assessment of acidification and recovery of European surface waters

The increase in emission of sulphur oxides and nitrogen (both oxidised and reduced forms) since the mid-1800s caused a severe decline in pH and ANC in acid-sensitive surface waters across Europe. Since c.1980, these emissions have declined and trends towards recovery from acidification have been widely observed in time-series of water chemistry data. In this paper, the MAGIC model was applied to 10 regions (the SMART model to one) in Europe to address the question of future recovery under the most recently agreed emission protocols (the 1999 Gothenburg Protocol). The models were calibrated using best available data and driven using S and N deposition sequences for Europe derived from EMEP data. The wide extent and the severity of water acidification in 1980 in many regions were illustrated by model simulations which showed significant deterioration in ANC away from the pre-acidification conditions. The simulations also captured the recovery to 2000 in response to the existing emission reductions. Predictions to 2016 indicated further significant recovery towards pre-acidification chemistry in all regions except Central England (S Pennines), S Alps, S Norway and S Sweden. In these areas it is clear that further emission reductions will be required and that the recovery of surface waters will take several decades as soils slowly replenish their depleted base cation pools. Chemical recovery may not, however, ensure biological recovery and further reductions may also be required to enable these waters to achieve the "good ecological status" as required by the EU Water Framework Directive

Sulphur and nitrogen fluxes and budgets in the Bohemian Forest and Tatra Mountains during the Industrial Revolution (1850-2000)

Major fluxes of sulphur and dissolved inorganic nitrogen were estimated in Central European mountain ecosystems of the Bohemian Forest (forest lakes) and Tatra Mountains (alpine lakes) over the industrial period. Sulphur outputs from these ecosystems were comparable to inputs during a period of relatively stable atmospheric deposition (10-35 mmol m-2 yr-1) around the 1930s. Atmospheric inputs of sulphur increased by three- to four-fold between the 1950s and 1980s to ~140 and ~60 mmol mm-2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively. Sulphur outputs were lower than inputs due to accumulation in soils, which was higher in forest soils than in the sparser alpine soils and represented 0.8-1.6 and 0.2-0.3 mol m-2, respectively, for the whole 1930-2000 period. In the 1990s, atmospheric inputs of sulphur decreased 80% and 50% in the Bohemian Forest and Tatra Mountains, respectively, and sulphur outputs exceeded inputs. Catchment soils became pronounced sources of sulphur with output fluxes averaging between 15 and 31 mmol m-2 yr-1. Higher sulphur accumulation in the forest soils has delayed (by several decades) recovery of forest lakes from acidification compared to alpine lakes. Estimated deposition of dissolved inorganic nitrogen was 53-75 mmol m-2 yr-1 in the Bohemian Forest and 35-45 mmol m-2 yr-1 in the Tatra Mountains in the 1880- 1950 period, i.e. below the empirically derived threshold of ~70 mmol m-2 yr-1, above which nitrogen leaching often occurs. Dissolved inorganic nitrogen was efficiently retained in the ecosystems and nitrate export was negligible (0-7 mmol m-2 yr-1). By the 1980s, nitrogen deposition increased to ~160 and ~80 mmol m-2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively, and nitrogen output increased to 120 and 60 mmol m-2 yr-1. Moreover, assimilation of nitrogen in soils declined from ~40 to 10-20 mmol m-2 yr-1 in the alpine soils and even more in the Bohemian Forest, where one of the catchments has even become a net source of nitrogen. In the 1990s, nitrogen deposition decreased by ~30% and DIN output decreased to -2 yr-1 in the Bohemian Forest and Tatra Mountains, respectively. New steady-state conditions, with negligible nitrogen export, could be reached in future but at lower nitrogen depositions than in the 1930s. Keywords: emission, deposition, acidification, nitrogen-saturation, recovery, sulphate, nitrate, ammonium, mountain lake

Modelling reversibility of central European mountain lakes from acidification: Part II – the Tatra Mountains

A dynamic, process-based model of surface water acidification, MAGIC7, has been applied to four representative alpine lakes in the Tatra Mountains (Slovakia and Poland). The model was calibrated for a set of 12 to 22-year experimental records of lake water composition. Surface water and soil chemistry were reconstructed from 1860 to 2002 and forecast to 2050 based on the reduction in sulphur and nitrogen emissions presupposed by the Gothenburg Protocol. Relatively small changes in the soil C:N ratios were not sufficient to simulate observed changes in NO₃&#8254; concentrations, so an alternative empirical approach of changes in terrestrial N uptake was applied. Measured sulphate sorption isotherms did not allow calibration of the pattern of sulphate response in the lakes, indicating that other mechanisms of S release were also important. The lake water chemistry exhibited significant changes during both the acidification advance (1860 to 1980s) and retreat (1980s to 2010). An increase in lake water concentrations of strong acid anions (SAA; 104–149 &#956;eq l^–1) was balanced by a decline in HCO₃&#8254; (13–62 &#956;eq l^–1) and an increase in base cations (BC; 42–72 &#956;eq l^–1), H⁺ (0-18 &#956;eq l^–1), and Al_iⁿ⁺ (0–26 &#956;eq l^–1). The carbonate buffering system was depleted in three lakes. In contrast, lake water concentrations of SAA, BC, H⁺, and Al_iⁿ⁺ decreased by 57–82, 28–42, 0–11, and 0–22 &#956;eq l^–1, respectively, the carbonate buffering system was re-established, and HCO₃&#8254; increased by 1–21 &#956;eq l^–1 during the chemical reversal from atmospheric acidification (by 2000). The MAGIC7 model forecasts a slight continuation in this reversal for the next decade and new steady-state conditions thereafter. Gran alkalinity should come back to 1950s levels (0–71 &#956;eq l^–1) in all lakes after 2010. Partial recovery of the soil pool of exchangeable base cations can be expected in one catchment, while only conservation of the current conditions is predicted for three lakes. Even though the pre-industrial alkalinity values of 16–80 &#956;eq l^–1 will not be reached due to the insufficient recovery of soil quality, the ongoing chemical improvement of water should be sufficient for biological recovery of most alpine lakes in the Tatra Mountains.</p> <p style='line-height: 20px;'><b>Keywords: </b>MAGIC, atmospheric deposition, sulphate, nitrate, base cations, aluminium, alkalinity, p