Forecasting acidification effects using a Bayesian calibration and uncertainty propagation approach

We present a statistical framework for model calibration and uncertainty estimation for complex deterministic models. A Bayesian approach is used to combine data from observations, the deterministic model, and prior parameter distributions to obtain forecast distributions. A case study is presented in which the statistical framework is applied using the hydrogeochemical model (MAGIC) for an assessment of recovery from acidification of soils and surface waters at a long-term study site in Norway under different future acid deposition conditions. The water quality parameters are coupled with a simple dose-response model for trout population health. Uncertainties in model output parameters are estimated and forecast results are presented as probability distributions for future water chemistry and as probability distributions of future healthy trout populations. The forecast results are examined for three different scenarios of future acid deposition corresponding to three different emissions control strategies for Europe. Despite the explicit consideration of uncertainties propagated into the future forecasts, there are clear differences among the scenarios. The case study illustrates how inclusion of uncertainties in model predictions can strengthen the inferences drawn from model results in support of decision making and assessments.     

Retrospective analyses and future predictions of snowmelt-induced acidification: example from a heavily impacted stream in the Czech Republic

We have combined a long-term hydrochemistry model (MAGIC) with a model that predicts short-term transient changes in hydrochemistry (pBDM) during hydrological events in order to improve the temporal resolution of retrospective analyses and future predictions of streamwater acidification. The model has been applied to a heavily impacted catchment in the Czech Republic. Spring flood acid-neutralizing capacity (ANC), pH, and inorganic monomeric aluminum (Ali(n+)) were simulated for the years of 1860, 1900, 1930, 1950, 1965, and 1985, measured in 1999, and predicted for 2030 using two different emission control scenarios. If the emission reduction according to the current legislation scenario is implemented, the model predicts that the spring flood pH, ANC, and Ali(n+) will recover close to the level of the 1950s by 2030. This will occur despite the annual average chemistry being farfrom having recovered to that level. The results suggest that the recovery of spring flood events is faster then the recovery of annual average chemistry and that much of what is won by further emission reduction will not be fully realized on an annual time scale.     

Regional assessment of the response of the acid-base status of lake watersheds in the Adirondack region of New York to changes in atmospheric deposition using PnET-BGC

Understanding the response of soil and surface waters to changes in atmospheric deposition is critical for guiding future legislation on air pollution. The Adirondack region of New York experiences among the most severe ecological impacts from acidic deposition. The region is characterized by considerable variability in atmospheric deposition, surficial and bedrock geology, hydrologic flow paths, and vegetation resulting in variability in effects of acidic deposition. In this study, an integrated biogeochemical model (PnET-BGC) was applied to 37 forest lake watersheds to assess the response of soil and surface waters of the Adirondacks to changes in atmospheric deposition at a regional scale. Model-simulated surface water chemistry was validated against data from two synoptic surveys conducted in 1984 and 2001. Results indicate that the model is able to capture the observed changes in surface water chemistry during this period. The model was further used to forecast the response of soil and surface waters to three future emission control scenarios. Results indicate that under the Clean Air Act, surface water SO4(2-) concentrations will continue to decrease at a median rate of -0.38 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.11 microeq/L-yr. More aggressive emission reductions will accelerate the rate of recovery. Under an aggressive control scenario, which represents an additional 75% reduction in SO2 emissions beyond the implementation of the Clean Air Act, surface water SO4(2-) concentrations are predicted to decrease at a median rate of -0.88 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.43 microeq/L-yr. Model predictions of several biologically relevant chemical indicators are also reported.     

The significance of the North Atlantic Oscillation (NAO) for sea-salt episodes and acidification-related effects in Norwegian rivers

Acidification of Norwegian surface waters, as indicated by elevated concentrations of sulfate and a corresponding reduction in acid neutralizing capacity and pH, is a result of emission and subsequent deposition of sulfur and nitrogen compounds. Episodic sea-salt deposition during severe weather conditions may increase the effects of acidification by mobilizing more toxic aluminum during such episodes. Changes in climatic conditions may increase the frequency and strength of storms along the coast thus interacting with acidification effects on chemistry and biota. We found that the North Atlantic Oscillation (NAO) is linked to sea-salt deposition and sea-salt induced water chemistry effects in five rivers. Particularly, toxic levels of aluminum in all rivers were significantly correlated with higher NAO index values. Further, temporal trends were studied by comparing tendencies for selected statistical indices (i.e. frequency distributions) with time. The selected indices exhibited strong correlations between the NAO index, sea-salt deposition and river data such as chloride, pH and inorganic monomeric aluminum, pointing at the influence of North Atlantic climate variability on water chemistry and water toxicity. The potentially toxic effects of sea-salt deposition in rivers seem to be reduced as the acidification is reduced. This suggests that sea-salt episodes have to increase in strength in order to give the same potential negative biological effects in the future, if acid deposition is further reduced. More extreme winter precipitation events have been predicted in the northwest of Europe as a result of climate change. If this change will be associated with more severe sea-salt episodes is yet unknown.     

Climate-induced episodic acidification of streams in central ontario

In this study we have analyzed the hydrochemical effect of drought conditions during 311 hydrological episodes in nine headwater streams in central Ontario over the past 20 years. Acid Neutralization Capacity (ANC) was logarithmically correlated (p<0.05) to antecedent discharge in eight of the nine streams, with the largest decline in ANC occurring after low antecedent flow. In eight of the nine streams SO4(2-) was the most important driving mechanism of ANC decline, but dilution as well as organic acidity was important in several streams. No decrease in the SO4(2-) driven ANC decline was observed over the 20 year study period despite a approximately 40% reduction in SO4(2-) deposition. The strong correlation between ANC decline and low antecedent discharge demonstrates that episodic acidification during rain events is strongly associated with preceding drought conditions, especially in wetland-dominated catchments. The results have important implications for recoveryfrom acidification, especially in northern ecosystems where climate scenarios forecast that warmer and drier conditions will be more common.     

Recovery of streams from episodic acidification in northern Sweden

Between 1990 and 1999, SO4(2-) deposition in northern Sweden decreased by over 50%. To determine if a corresponding amelioration of stream acidity has occurred, we analyzed trends in anthropogenically driven episodic acidification in five streams during the same time period, using the Boreal Dilution Model (BDM) (Bishop, K. H.; Laudon, H.; Kohler, S. Water Resour. Res. 2000, 36, 1873-1884). Although there was no significant change in the annual average streamwater chemistry, the anthropogenically driven episodic acidification associated with spring flood runoff decreased by between 40% and 80%. A strong correlation between winter SO4(2-) deposition and the anthropogenic component of episodic acidification in these five streams suggests that future reductions of acid deposition will further improve the spring flood acidification situation in northern Sweden. These results argue that reduced emissions of acid precursors have generated significant improvements in the surface water chemistry during episodes associated with spring runoff in northern Sweden.     

Effect of declining lake base cation concentration on freshwater critical load calculations

Steady-state critical load models have been extensively used as the scientific underpinning for air pollution control policies in Europe and are currently being applied to other parts of the world. An important assumption of steady-state models is that critical load estimates do not change through time (or time scale of interest). The most commonly used model for estimating freshwater critical loads is the steady-state water chemistry (SSWC) model. In this study we examined changes in SSWC critical load estimates for 29 lakes in south-central Ontario using data collected 13 years apart (1985-1998), during which time bulk sulfate (SO4(2-)) deposition decreased by 35%. In lakes with the lowest base cation concentrations (<120 microequiv L(-1) Ca2+), the decrease in SO4(2-) concentration was accompanied by an approximately equivalent decrease in base cation concentration, resulting in only a minimal increase in Acid Neutralizing Capacity (ANC) during the 13-year period (median increase 1.6 microequiv L(-1)), and the median critical load for acidity (CL(A)) estimated by the SSWC model decreased by 14.6%. These changes may have been brought about by declining base cation concentrations owing to continued soil acidification in the region. In contrast, in lakes with higher base cation concentrations (>150 microequiv L(-1) Ca2+), the relative decline in base cation concentration was not as great, resulting in a larger increase in ANC (median increase 13.1 microequiv L(-1)) and an increase in the estimated CL(A) (median 5.1%). Lakes with moderate base cation concentrations (120-150 microequiv L(-1) Ca2+) exhibited an intermediate response; the median ANC increased by 8.8 microequiv L(-1) and the estimated CL-(A) decreased by 2.2%. In central Ontario, SSWC critical load estimates based on data taken only 13 years apart change quite dramatically due to changing lake base cation concentrations, and the response appears to depend on the base status of the lakes. The changing values obtained from the SSWC model have important consequences for policy decisions regarding acceptable levels of acid deposition. The application of dynamic models that take into account changes in lake/soil chemistry appears more appropriate for estimating acceptable levels of acid deposition in the region.     

Factors affecting acid neutralizing capacity in the Adirondack region of New York: a solute mass balance approach

High rates of acidic deposition in the Adirondack region of New York have accelerated acidification of soils and surface waters. Annual input-output budgets for major solutes and acid-neutralizing capacity (ANC) were estimated for 43 drainage lake-watersheds in the Adirondacks from 1998 to 2000. Sulfate was the predominant anion on an equivalent basis in both precipitation and drainage export. Calcium ion had the largest cation drainage export, followed by Mg2+. While these watersheds showed net nitrogen (N) retention, the drainage losses of SO4(2-), Cl-, base cations, and ANC exceeded their respective inputs from precipitation. Land cover (forest type and wetlands) affected the export of SO4(2-), N solutes, and dissolved organic carbon (DOC). The relationships of solute export with elevation (negative for base cations and Cl-, positive for NO3- and H+) suggest the importance of the concomitant changes of biotic and abiotic watershed characteristics associated with elevational gradients. The surface water ANC increased with the sum of base cations and was greatest in the lakes with watersheds characterized by thick deposits of glacial till. The surface water ANC was also higher in the lake-watersheds with lower DOC export. Some variation in lake ANC was associated with variability in acidic deposition. Using a classification system previously developed for Adirondack lakes on the basis primarily of surficial geology, lake-watersheds were grouped into five classes. The calculated ANC fluxes based on the major sinks and sources of ANC were comparable with measured ANC for the thick-till (I) and the medium-till lake-watersheds with low DOC (II). The calculated ANC was overestimated for the medium-till with high DOC (III) and the thin-till with high DOC (V) lake-watersheds, suggesting the importance of naturally occurring organic acids as an ANC sink, which was not included in the calculations. The lower calculated estimates than the measured ANC for the thin-till lake-watersheds with low DOC (IV) were probably due to the mobilization of Al as an ANC source in these watersheds that were highly sensitive to strong acid inputs. Our analysis of various drainage lakes across the Adirondacks on the basis of solute mass balances, coupled with the use of a lake classification system and GIS data, demonstrates that the lake-watersheds characterized by shallow deposits of glacial till are highly sensitive to acidic deposition not only in the southwestern Adirondack region where previous field-based studies were intensively conducted but also across the entire Adirondack region. Moreover, the supply of organic acids and Al mobilization substantially modify the acid-base status of surface waters.     

Are brook trout streams in western Virginia and Shenandoah National Park recovering from acidification?

Streamwater composition data obtained through periodic sampling of streams that support brook trout (Salvelinus fontinalis) in the mountains of western Virginia were examined for evidence of recovery from acidification during the 1988-2001 period. Measurements of sulfate deposition in precipitation indicate that sulfate deposition in the region declined approximately 40% between 1985 and 2000. While no significant regional trends in acid-base constituents were observed for the set (n = 65) of western Virginia study streams, significant regional trends were observed for a subset (n = 14) of streams in Shenandoah National Park (SNP). For the subset of SNP streams, the median increase in acid-neutralizing capacity (ANC) was 0.168 microequiv L(-1) year(-1) and the median decrease in sulfate concentration was -0.229 microequiv L(-1) year(-1). Although these trends are consistent with recovery from acidification, the degree of apparent recovery is small compared to estimates of historic acidification in SNP streams and much less than observed in other, more northern regions in the United States. Correlation between sulfate concentration trends and current sulfate concentrations in streamwater suggests that recovery from stream acidification in the western Virginia region is determined by sulfur retention processes in watershed soils. A transient increase in nitrate concentrations that occurred among some western Virginia streams following forest defoliation by the gypsy moth (Lymantria dispar) complicates interpretation of the observed patterns of change in acid-base status.     

Chemical recovery of surface waters across the northeastern united states from reduced inputs of acidic deposition: 1984-2001

Changes in lake water chemistry between 1984 and 2001 at 130 stratified random sites across the northeastern United States were studied to evaluate the population-level effects of decreases in acidic deposition. Surface-water S04(2-) concentrations decreased across the region at a median rate of -1.53 microequiv L(-1) year(-1). Calcium concentrations also decreased, with a median rate of -1.73 microequiv L(-1) year(-1). This decrease in Ca2+ retarded the recovery of surface water acid neutralizing capacity (Gran ANC), which increased at a median rate of 0.66 microequiv L(-1) year(-1). There were small increases in pH in all subregions except central New England and Maine, where the changes were not statistically significant. Median NO3- trends were not significant except in the Adirondacks, where NO3- concentrations increased at a rate of 0.53 microequiv L(-1) year(-1). A regionwide decrease in the concentration of total Al, especially in ponds with low ANC values (ANC < 25 microequiv L(-1)), was observed in the Adirondack subregion. These changes in Al were consistent with the general pattern of increasing pH and ANC. Despite the general pattern of chemical recovery, many ponds remain chronically acidic or are susceptible to episodic acidification. The continued chemical and biological recovery at sites in the northeastern United States will depend on further controls on S and N emissions.     

Analysis of trends in episodic acidification of streams in western Maryland

In this study we report on changes in the magnitude and mechanisms of episodic acidification of a small acid-sensitive stream in western Maryland (U.S.) during the 1990s, a period in which wet sulfate deposition declined by 10-25% due to implementation of the Clean Air Act Amendments (CAAA) of 1990. We observed a relatively minor trend in the magnitude of episodic acidification over this period, as measured bytransient changes in acid neutralizing capacity (deltaANC) and minimum values of ANC (ANC(min)) during 22 events sampled prior to and following CAAA implementation. Any relationship to changes in atmospheric deposition appears to be confounded by large hydroclimatological variability between the two sampling periods. Nonetheless, results obtained prior to implementation of the CAAA indicated that the mechanism of episodic acidification was mostly attributable to flushing of accumulated sulfate from the watershed, whereas results obtained post-CAAA indicated domination by base cation dilution. This shift in the mechanism of episodic acidification is qualitatively consistent with hydrochemical theory, as well as with empirical results from surface waters in other regions where dramatic declines in sulfate deposition have taken place.     

Carbon isotopes in tree rings of Norway spruce exposed to atmospheric pollution

The Bohemian Forest was exposed to high levels of sulfur and nitrogen deposition during the last century. The change in acid deposition caused a rapid decline in pH and increase in Al concentrations of soil solutions since the 1950s. A possible negative effect of soil chemistry on growth of Norway spruce tree has been studied using the 13C isotopic signal and chemistry of the tree rings. Tree rings were sectioned by decades, and whole wood was analyzed for isotopic composition (delta 13C) and content of Mg, Ca, and Al. Only those rings that formed after the juvenile effect in early rings were used and trends from the beginning of 20th century were evaluated. The mean delta 13C of the spruce tree rings was 17.6%. The delta 13C did not follow climate changes but had an opposite trend to that of acid depositions and Al concentrations in soil solution, but a similar trend as soil acidification (pH decrease), implying a negative effect of acid deposition and soil acidification on tree physiology. The molar ratio of base cations to Al decreased together with delta 13C.     

Chemical response of lakes in the Adirondack Region of New York to declines in acidic deposition

Long-term changes in the chemistry of wet deposition and lake water were investigated in the Adirondack Region of New York. Marked decreases in concentrations of SO4(2-) and H+ in wet deposition have occurred at two sites since the late 1970s. These decreases are consistent with long-term declines in emissions of sulfur dioxide (SO2) in the eastern United States. Changes in wet NO3- deposition and nitrogen oxides (NOx) emissions have been minor over the same interval. Virtually all Adirondack Lakes have shown marked decreases in concentrations of SO4(2-), which coincide with decreases in atmospheric S deposition. Concentrations of NO3- have also decreased in several Adirondack lakes. As atmospheric N deposition has not changed over this period, the mechanism contributing to this apparent increase in lake/watershed N retention is not evident. Decreases in concentrations of SO4(2-) + NO3- have resulted in increases in acid-neutralizing capacity (ANC) and pH and resulted in a shift in the speciation of monomeric Al from toxic inorganic species toward less toxic organic forms in some lakes. Nevertheless, many lakes continue to exhibit pH values and concentrations of inorganic monomeric Al that are critical to aquatic biota. Extrapolation of rates of ANC increase suggests that the time frame of chemical recovery of Adirondack Lakes will be several decades if current decreases in acidic deposition are maintained.     

Simultaneous assessment of deposition effects of base cations, sulfur, and nitrogen using an extended critical load function for acidification

Base cations (BC) play an important role to prevent soil acidification. In certain acid sensitive areas, such as China, BC deposition is high and a considerable fraction is of anthropogenic origin. BC deposition might decrease in the future with the implementation of air pollution control measures. The effect of changes in BC deposition, however, has seldom been considered in critical load calculations based on the steady-state mass balance (SSMB) method. In order to better quantify the importance of the BC deposition for acid deposition mitigation policy, an extension of the SSMB method for critical load calculation for soil acidification is presented. The BC deposition is taken into account as a variable along with sulfur (S) and nitrogen (N) deposition, creating an S-N-BC critical load function. As a case study, critical loads of S and N for the Tie Shan Ping catchment in Chongqing in southwest China under variable BC deposition were calculated. Results indicate that abatement of BC deposition has significant impact on the critical loads of S and N. A 75% reduction in BC of assumed anthropogenic origin decreases the critical loads of acids by 58%. The current deposition does not exceed the critical loads, but if BC deposition from anthropogenic sources was controlled, then the exceedance would be considerable. Uncertainty analysis show that the size of the BC deposition of natural origin is the single parameter contributing the most to the steady-state S and N critical load. The extended critical load function can be used by policy makers to set more reasonable acidity control strategies in the future. The method also highlights for policymakers the "competition" between emission control of particulate matter driven by human health targets and potential increase of net acid load from such measures.     

The global atmospheric environment for the next generation

Air quality, ecosystem exposure to nitrogen deposition, and climate change are intimately coupled problems: we assess changes in the global atmospheric environment between 2000 and 2030 using 26 state-of-the-art global atmospheric chemistry models and three different emissions scenarios. The first (CLE) scenario reflects implementation of current air quality legislation around the world, while the second (MFR) represents a more optimistic case in which all currently feasible technologies are applied to achieve maximum emission reductions. We contrast these scenarios with the more pessimistic IPCC SRES A2 scenario. Ensemble simulations for the year 2000 are consistent among models and show a reasonable agreement with surface ozone, wet deposition, and NO2 satellite observations. Large parts of the world are currently exposed to high ozone concentrations and high deposition of nitrogen to ecosystems. By 2030, global surface ozone is calculated to increase globally by 1.5 +/- 1.2 ppb (CLE) and 4.3 +/- 2.2 ppb (A2), using the ensemble mean model results and associated +/-1 sigma standard deviations. Only the progressive MFR scenario will reduce ozone, by -2.3 +/- 1.1 ppb. Climate change is expected to modify surface ozone by -0.8 +/- 0.6 ppb, with larger decreases over sea than over land. Radiative forcing by ozone increases by 63 +/- 15 and 155 +/- 37 mW m(-2) for CLE and A2, respectively, and decreases by -45 +/- 15 mW m(-2) for MFR. We compute that at present 10.1% of the global natural terrestrial ecosystems are exposed to nitrogen deposition above a critical load of 1 g N m(-2) yr(-1). These percentages increase by 2030 to 15.8% (CLE), 10.5% (MFR), and 25% (A2). This study shows the importance of enforcing current worldwide air quality legislation and the major benefits of going further. Nonattainment of these air quality policy objectives, such as expressed by the SRES-A2 scenario, would further degrade the global atmospheric environment.     

Response of surface water acidification in upper Yangtze River to SO2 emissions abatement in China

Surface waters in Europe and North America are slowly recovering from acidification following major reductions in emissions of sulfur dioxide (SO(2)) since the 1980s. In contrast, regions affected by acid rain have been reported to be growing in China. Here we show that the rapid change in surface water chemistry in the 1990s in large areas in Southwestern China, specifically the tributary rivers of the Upper Yangtze River, caused by increasing SO(2) emissions, has leveled off. During the 1990s the sulfate (SO(4)(2-)) concentrations in river water increased rapidly and, on average, doubled in only eight years. Simultaneously, calcium (Ca(2+)) concentrations increased, while pH values decreased. In the following decade (2000s), SO(2) emissions stabilized, causing a subsequent stop to the increasing SO(4)(2-) concentrations and pH decline in river water. Although a rapid response to future reduction in SO(2) emissions can be expected, a rapid increase of nitrogen (N) emissions could lead to increases in N leaching and delay recovery.     

Acidification and buffering mechanisms in acid sulfate soil wetlands of the Murray-Darling Basin, Australia

The acid generation mechanisms and neutralizing capacities of sulfidic sediments from two inland wetlands have been studied in order to understand the response of these types of systems to drying events. The two systems show vastly different responses to oxidation, with one (Bottle Bend (BB) lagoon) having virtually no acid neutralizing capacity (ANC) and the other (Psyche Bend (PB) lagoon) an ANC that is an order of magnitude greater than the acid generation potential. While BB strongly acidifies during oxidation the free acid generation is less than that expected from the measured proton production and consumption processes, with additional proton consumption attributed to the formation of an acid-anion (chloride) FeIII (oxyhydr)oxide product, similar to akagane?ite (Fe(OH)2.7Cl0.3). While such products can partially attenuate the acidification of these systems, resilience to acidification is primarily imparted by sediment ANC.     

Past, present, and future exceedance of critical loads of acidity for surface waters in Finland

A critical load is a deposition limit below which harmful effects for a given ecosystem do not occur; the approach has underpinned European sulfur (S) and nitrogen (N) effects-based emission reduction policies during the last two decades. Surface waters are an important resource in Finland, as such the development of models and determination of critical loads has played a central role in supporting their recovery from acidification or preservation of ecosystem health. Critical loads of acidity for Finnish lakes were determined using the steady-state First-order Acidity Balance (FAB) model in conjunction with comprehensive national surveys of surface waters (headwater lakes; n = 1066) and soils. In the 1980s almost 60% of the study lakes were exceeded, impacting brown trout and perch populations. The steep decline in emissions and acidic (S and N) deposition during the last two decades has reduced exceedance to <10%, and by 2020 exceedance is predicted to reach preindustrial (1880) levels. In concert with these reductions, chemical and biological recovery has been observed. The critical load approach has been instrumental in assessing impacts to surface waters in Finland and directing effects-based emission reduction policies.     

Predicting acidification recovery at the Hubbard Brook Experimental Forest, New Hampshire: evaluation of four models

The performance and prediction uncertainty (owing to parameter and structural uncertainties) of four dynamic watershed acidification models (MAGIC, PnET-BGC, SAFE, and VSD) were assessed by systematically applying them to data from the Hubbard Brook Experimental Forest (HBEF), New Hampshire, where long-term records of precipitation and stream chemistry were available. In order to facilitate systematic evaluation, Monte Carlo simulation was used to randomly generate common model input data sets (n = 10,000) from parameter distributions; input data were subsequently translated among models to retain consistency. The model simulations were objectively calibrated against observed data (streamwater: 1963-2004, soil: 1983). The ensemble of calibrated models was used to assess future response of soil and stream chemistry to reduced sulfur deposition at the HBEF. Although both hindcast (1850-1962) and forecast (2005-2100) predictions were qualitatively similar across the four models, the temporal pattern of key indicators of acidification recovery (stream acid neutralizing capacity and soil base saturation) differed substantially. The range in predictions resulted from differences in model structure and their associated posterior parameter distributions. These differences can be accommodated by employing multiple models (ensemble analysis) but have implications for individual model applications.     

Hydrochloric acid: an overlooked driver of environmental change

Research on the ecosystem impacts of acidifying pollutants, and measures to control them, has focused almost exclusively on sulfur (S) and nitrogen (N) compounds. Hydrochloric acid (HCl), although emitted by coal burning, has been overlooked as a driver of ecosystem change because most of it was considered to redeposit close to emission sources rather than in remote natural ecosystems. Despite receiving little regulatory attention, measures to reduce S emissions, and changes in energy supply, have led to a 95% reduction in United Kingdom HCl emissions within 20 years. Long-term precipitation, surface water, and soil solution data suggest that the near-disappearance of HCl from deposition could account for 30-40% of chemical recovery from acidification during this time, affecting both near-source and remote areas. Because HCl is highly mobile in reducing environments, it is a more potent acidifier of wetlands than S or N, and HCl may have been the major driver of past peatland acidification. Reduced HCl loadings could therefore have affected the peatland carbon cycle, contributing to increases in dissolved organic carbon leaching to surface waters. With many regions increasingly reliant on coal for power generation, HCl should be recognized as a potentially significant constituent of resulting emissions, with distinctive ecosystem impacts.