Patterns of Streamwater Acidity in Lye Brook Wilderness,Vermont, USA

Under the United States Clean Air Act Amendments of 1977, a class I designation safeguards wilderness areas from the negative effects of new sources of air pollution. We monitored streamwater chemistry in the class I Lye Brook Wilderness in southwestern Vermont from May 1994 through August 1995. Stream samples were collected biweekly at nine sampling locations throughout the wilderness and were analyzed for major cations and anions, dissolved organic carbon, pH, and acid-neutralizing capacity. Eight of nine sites sampled had mean annual acid neutralizing capacity values below zero. During the study period, decreases in streamwater acid neutralizing capacity values were caused primarily by SO₄ ²⁻. At some sites, however, NO₃ ⁻ and naturally occurring, weak organic acids were seasonally important. During high discharge, the low pH and high concentrations of inorganic monomeric Al were at levels that are toxic to acid-sensitive aquatic species. Watershed mass balances were calculated to determine annual gains or losses for measured ions. These budgets indicate that S inputs and outputs were nearly equal, there was a net loss of base cations, and a net gain in N. How long these watersheds can continue to assimilate additional N inputs is unknown.     

Use of Natural 35S to Trace Sulphate Cycling in Small Lakes,Flattops Wilderness Area,Colorado, U.S.A.

Measurements of the cosmogenically-produced ³⁵S, a radioisotope of sulphur (t_1/2 = 87 days), are reported for the Ned Wilson Lake watershed in Colorado. The watershed contains two small lakes and a flowing spring presumed to be representative of local ground water. The watershed is located in the Flattops Wilderness Area and the waters in the system have low alkalinity, making them sensitive to increases in acid and sulphate deposition. Time series of ³⁵S measurements were made during the summers of 1995 and 1996 (July–September) at all three sites. The system is dominated by melting snow and an initial concentration of 16–20 mBq L^-1 was estimated for snowmelt based on a series of snow samples collected in the Rocky Mountains. The two lakes had large initial ³⁵S concentrations in July, indicating that a large fraction of the lake water and sulphate was introduced by meltwater from that year's snowpack. In 1995 and 1996, ³⁵S concentrations decreased more rapidly than could be accounted for by decay, indicating that other processes were affecting ³⁵S concentrations. The most likely explanation is that exchange with sediments or the biota was removing ³⁵S from the lake and replacing it with older sulphate devoid of ³⁵S. In September of 1995 and 1996, ³⁵S concentrations increased, suggesting that atmospheric deposition is important in the sulphate flux of these lakes in late summer. Sulphur-35 concentrations in the spring water were highly variable but never higher than 3.6 mBq L^-1 and averaged 2 mBq L^-1. Using a simple mixing model, it was estimated that 75% of the spring water was derived from precipitation of previous years.     

Development of Stream Water Chemistry during Spring Melt in a Northern Hardwood Forest

The role of snowmelt and subsurface hydrology in determiningthe chemistry of a small headwater stream in the TurkeyLakes Watershed (TLW) was evaluated for the spring meltperiods 1992 to 1996. Spring runoff is the dominanthydrological event at the TLW each year. Processesoccurring within the snowpack during snowmelt wereprincipally responsible for the above-ground changes inchemical fluxes relative to bulk deposition (the effect ofwinter throughfall was minimal). Large changes in chemicalfluxes occurred below ground. Organic matter decomposition,weathering, nitrification, and element cycling are some ofthe more important below-ground processes that operateduring the snow accumulation and ablation season and controlthe composition of the water ultimately appearing in thestream. Maximum stream discharge was accompanied byelevated concentrations of H⁺, NO₃ ^-, K⁺,NH₄ ⁺, DOC, Al and Mn, but reduced levels ofCa²⁺, Mg²⁺, SO₄ ^2- and SiO₂. Theconcentration-discharge relationships were consistent withwater movement through and above the forest floor duringpeak discharge, a flowpath facilitated by rapid infiltrationof meltwater and the existence of a relatively impermeablelayer in the mineral soil creating a perched water table. Averaged over the five periods of snow accumulation andablation, it was estimated that pre-melt stream flow, andwater routed through the forest floor and through the uppermineral soil contributed 9, 28 and 63%, respectively, ofthe discharge measured at the outlet of the catchment. Theforest floor contribution would be greater at peak dischargeand at higher elevations. An end-member mixing modelestimated concentrations of SO₄ ^2-, NO₃ ^-,Cl^-, Ca²⁺, Mg²⁺, Na⁺ and Al that werecomparable to average values measured in the stream. Othervariables (NH₄ ⁺, H⁺, K⁺ and DOC) wereover-estimated implying retention mechanisms operatingoutside the model assumptions.     

Deposition and Storage of Spheroidal Carbonaceous Fly-Ash Particles in European Mountain Lake Sediments and Catchment Soils

Spheroidal carbonaceous particles(SCPs) are produced only from high temperaturecombustion of fossil-fuels. In mountain lakesystems, they provide an unambiguous indicator ofatmospheric deposition. In order to comparedepositional fluxes of SCPs between mountainareas experiencing various pollutant regimes,intensive bulk deposition sampling was undertakenat five sites across Europe. Catchment soil coresand lake sediment cores were also taken at eachsite to compare SCP storage over the post-industrial period. Atmospheric, sediment and soilSCP data showed similar patterns. Highestcontamination was found in Scotland, Slovakia andSpain with the Austrian site intermediate and themid-Norwegian site least contaminated. A highproportion of accumulated SCPs were found to bestored in catchment soils at each site.Therefore, a significant increase in soilerosion, possibly as a result of future climatechange, could lead to the input of largequantities of catchment stored SCPs and, byimplication, other atmospherically depositedcontaminants to the lake ecosystem.     

Trends in the Water Chemistry of High Altitude Lakes in Europe

Here we present the chemical trends of seven high altitude lakes, analysed within the AL:PE and MOLAR Projects of the EU (1999) and selected on the basis of the availability of complete and reliable data for the period 1984–1999. The lakes are representative of the Scandinavian Alps, the Cairngorm Mountains in Scotland, the Alps and the Pyrenees. Significant trends were identified for some indicators of acidification, for instance pH and alkalinity, but not all lakes reacted similarly to decreasing depositions of sulphate and base cations. Differences in lake response are discussed in relation to recent variations of atmospheric deposition chemistry and associated changes in climatic conditions. Beside individual variations of the studied lakes, depending, among other things, on altitude and morphology, catchment characteristics and climate trends play a major role for the reaction of high altitude lakes on changes in atmospheric depositions.     

Sulfur Metabolism in Polluted Sphagnum Peat Bogs: A Combined 34S–35S–210Pb Study

The size and isotopic behavior of sulfur pools in²¹⁰Pb-dated peat cores were investigated to obtain aninsight into retention mechanisms of pollutant S in twomountain-top peatlands of the Northern Czech Republic, CentralEurope. The bogs were situated 40 km apart in an area whichbetween the years 1985 and 1995 received as much as 130 kg Sha^-1 yr^-1 from the atmosphere. Vertical peataccretion was faster at Pod Jelení horou (JH) than atVelký moál (VM). Organic carbon-bonded S was themost abundant sulfur pool, constituting 77 and 65 wt. % at JHand VM, respectively. At JH both the S concentration maximumand the highest annual S deposition rate were displaceddownward by more than 20 years (from 1987 to the 1960s)indicating that the buried S is vertically mobile. At VM the Sconcentration was the highest in the topmost 2-cm section eventhough atmospheric S deposition peaked in 1987. Differentmechanisms of S isotope redistribution prevailed in thetopmost peat layers at JH, where a negative ³⁴Sshift occurred, and at VM, where a positive ³⁴Sshift occurred. Bacterial sulfate reduction was responsiblefor the negative ³⁴S shift at JH. One possibleexplanation of the positive ³⁴S shift at VM isrelease of ³²S-enriched products of mineralization duringpeat diagenesis. There was a strong positive correlationbetween the abundance of total and pyrite S along the profiles.The presence of pyrite S at VM (526 ± 60 ppm) suggestedthat even at VM bacterial sulfate reduction occurred. Ananaerobic incubation of JH peat indicated sulfate reductionrate of 600 nmol g^-1 day^-1. The turnover times forinorganic S pools were shorter than for the organic S pools.Cumulative S contents in the Czech peat bogs were found to besignificantly lower than in similar sites in the NortheasternU.S., even though the atmospheric S inputs were more thanthree times higher at the Czech sites. Possible causes of suchdiscrepancy are discussed.     

Watershed scale assessment of nitrogen and phosphorus loadings in the Indian River Lagoon basin,Florida

There is a growing evidence that the ecological and biological integrity of the lagoon has declined during the last 50 years, probably due to the decline in water quality. Establishment of a watershed scale seagrass-based nutrient load assessment is the major aim of water quality management in the Indian River Lagoon (IRL). Best estimate loadings incorporate wet and dry deposition, surface water, groundwater, sediment nutrient flux, and point source effluent discharge data. On the average, the IRL is receiving annual external loadings of 832, 645 and 94,476kg of total nitrogen (TN) and total phosphorus (TP), respectively, from stormwater discharges and agricultural runoff. The average internal cycling of TN and TP from sediment deposits in the IRL was about 42,640kg TN and 1050kg TPyr(-1). Indirect evidence suggests that atmospheric deposition has played a role in the ongoing nutrient enrichment in the IRL. The estimated total atmospheric deposition of TN and TP was about 32,940 and 824kgyr(-1), while groundwater contribution was about 84,920 and 24,275kgyr(-1), respectively, to the surface waters of the IRL. The estimated annual contribution of point effluent discharge was about 60,408kg TN and 7248kg TP. In total, the IRL basin is receiving an annual loading of about 1,053,553kg TN and 127,873kg TP. With these results, it is clear that the current rate of nutrient loadings is causing a shift in the primary producers of the IRL from macrophyte to phytoplankton- or algal-based system. The goal is to reverse that shift, to attain and maintain a macrophyte-based estuarine system in the IRL.     

Chemistry of Selected High-Elevation Lakes in Seven National Parks in the Western United States

A chemical survey of 69 high-altitude lakes in seven national parks in the western United States was conducted during the fallof 1999; the lakes were previously sampled during the fall of 1985, as part of the Western Lake Survey. Lakes in parks in the Sierra/southern Cascades (Lassen Volcanic, Yosemite, Sequoia/Kings Canyon National Parks) and in the southern RockyMountains (Rocky Mountain National Park) were very dilute; medianspecific conductance ranged from 4.4 to 12.2 S cm^-1 andmedian alkalinity concentrations ranged from 32.2 to 72.9 eqL^-1. Specific conductances and alkalinity concentrations were substantially higher in lakes in the central and northernRocky Mountains parks (Grand Teton, Yellowstone, and GlacierNational Parks), probably due to the prevalence of more reactivebedrock types. Regional patterns in lake concentrations of NO₃ and SO₄ were similar to regional patterns in NO₃ and SO₄ concentrations in precipitation, suggestingthat the lakes are showing a response to atmospheric deposition.Concentrations of NO₃ were particularly high in Rocky Mountain National Park, where some ecosystems appear to be undergoing nitrogen saturation.     

Long Term Trends in Sulphur and Nitrogen Deposition in Europe and the Cause of Non-linearities

Emissions of sulphur and oxidized nitrogen compounds in Europe have been reduced following a series of control measures during the last two decades. These changes have taken place during a period in which the primary gases and the wet deposition throughout Europe were extensively monitored. Since the end of the 1970s, for example land based sulphur emissions declined by between 90 and 70% depending on the region. Over the same period the total deposition of sulphur and its partitioning into wet and dry deposition have declined, but the spatial pattern in the reduction in deposition differs from that of emission and has changed with time. Such non-linearities in the emission-deposition relationship are important to understand as they complicate the process of assessing the effects of emission reduction strategies. Observed non-linearities in terrestrial sulphur emission-deposition patterns have been identified in north west Europe due to increases in marine emissions, and are currently slowing the recovery of freshwater ecosystems. Changes in the relative amounts of SO₂ and NH₃ in air over the last two decades have also changed the affinity of terrestrial surfaces for SO₂ and have therefore changed the deposition velocity of SO₂ over substantial areas. The consequence of this effect has been the very rapid reduction in ambient SO₂ concentration in some of the major source areas of Europe, where NH₃ did not change much. Interactions between the different pollutants, generating non-linearities are now being incorporated in long-range transport models to simulate the effects of historical emission trends and to provide projections into the future. This paper identifies non-linearities in emission deposition relationships for sulphur and nitrogen compounds in Europe using data from the EMEP long-rang transport model and measured concentration fields of the major ions in precipitation and of SO₂ and NO₂ in surface air.     

Effects of Nitrogen Deposition on Bryophyte Species Composition of Calcareous Grasslands

Regular additions of NH₄NO₃ (35–140 kg N ha⁻¹ yr⁻¹) and (NH₄)₂SO₄ (140 kg N ha⁻¹ yr⁻¹) to a calcareous grassland in northern England over a period of 12 years have resulted in a decline in the frequency of the indigenous bryophyte species and the establishment of non-indigenous calcifuge species, with implications for the structure and composition of this calcareous bryophyte community. The lowest NH₄NO₃ additions of 35 kg N ha⁻¹ yr⁻¹ produced significant declines in frequency of Hypnum cupressiforme, Campylium chrysophyllum, and Calliergon cuspidatum. Significant reductions in frequency at higher NH₄NO₃ application rates were recorded for Pseudoscleropodium purum, Ctenidum molluscum, and Dicranum scoparium. The highest NH₄NO₃ and (NH₄)₂SO₄ additions provided conditions conducive for the establishment of two typical calcifuges – Polytrichum spp. and Campylopus introflexus, respectively. Substrate-surface pH measurements showed a dose-related reduction in pH with increasing NH₄NO₃ deposition rates of 1.6 pH units between the control and highest deposition rate, and a further significant fall in pH, of >1 pH unit, between the NH₄NO₃ and (NH₄)₂SO₄ treatments. These results suggest that indigenous bryophyte composition may be at risk from nitrogen deposition rates of 35 kg N ha⁻¹ yr⁻¹ or less. These effects are of particular concern for rare or endangered species of low frequency.