Reductions In Atmospheric Deposition Research Articles

Hydroclimatic non-stationarity drives stream hydrochemistry dynamics through controls on catchment connectivity and water ages

We used data from 17 years of routine stream flow sampling to characterise hydrochemical dynamics in the Girnock Burn, an internationally important long-term catchment monitoring site. We combined hydrochemical time series analysis with hydrological modelling to understand short- and long-term dynamics in relation to dominant runoff processes. Isotopic tracer data employed within the model enabled flux tracking of water as it transited the catchment, facilitating water age estimates. The stream drains an upland 31 km2 catchment with complex topography and variable geology, which influences soil distributions; peaty soils dominate valley bottoms which receive drainage from more permeable podzolic soils on steeper slopes. Short-term hydrochemical dynamics largely reflect the relative dominance of hydrological sources: summer low flows are dominated by alkaline groundwater high in weathering products (Ca2+, Mg2+, SiO2) whilst high flows generated by overland flow from peaty soils are more acidic, DOC enriched, and dominated by atmospheric solutes (Na+, Cl-, SO42-). Baseflows are dominated by older groundwater (>∼3years) in contrast to storm runoff dominated by younger (<∼0.5 years), near-surface, waters. Usual seasonal distributions of stream flows, with high flows in winter and summer low flows, result in strong seasonality in most solutes. However, coupled effects of hydroclimatic variability and catchment heterogeneity dictates marked scatter in flow-concentration relationships for most determinands. A long-term decreasing trend was evident for SO42-concentrations, reflecting continuing effects of reductions in atmospheric deposition of pollutants from coal burning. Reductions in large storm event frequency post-2016 and protracted periods of low flows in the droughts of 2018 and 2022 have resulted in the catchment becoming dominated by low flows, derived from older groundwater with more alkaline chemistry for longer periods. Changing climatic conditions and stream flow responses seem likely to continue to cause changes in stream water quality and associated ecosystem services of the Girnock Burn and similar upland catchments.

Changing Water Chemistry in One Thousand Norwegian Lakes During Three Decades of Cleaner Air and Climate Change

AbstractWe present long‐term changes in Norwegian lake water quality across regional gradients in atmospheric pollution, air temperature, hydrology, and vegetation using (a) a national representative lake survey carried out in 1995 and 2019 (ThousandLakes), and (b) an annual lake survey from acid‐sensitive catchments (78 lakes, TrendLakes) from 1990 to 2020. Our analysis encompasses all major chemical constituents, for example, anions and cations, dissolved organic matter (DOM), nutrients, iron (Fe), and silicate (SiO2). During these decades, environmental changes included declines in sulfur (S) and nitrogen (N) deposition, climate warming, and increase in forest biomass. Strong chemical recovery from acidification is found, attributed to large reductions in atmospheric deposition, moderated by catchment processing from land use and climate change. Browning counteracted chemical recovery in some regions, while Ca increased unexpectedly. We suggest that increased weathering, from enhanced terrestrial productivity, is an important driver of increased Ca—substantiated by widespread, substantial increases in SiO2. Light‐ and nutrient‐limitation has become more prevalent, indicated by higher DOM, lower nitrate (NO3), and lower NO3to total phosphorous ratios. Declines in lake NO3 occurred independently of N deposition, suggesting increased catchment N retention, possibly from increased terrestrial productivity. We conclude that decreased air pollution continues to be a dominant driver of long‐term trends in lake chemistry, but climate‐induced increase in terrestrial weathering processes, governed by increased biomass, is likely to have an increasing impact on future lake acidity, nutrient, and light status, that may cascade along the aquatic continuum from rivers to the coast.

Localized Water Quality Improvement in the Choptank Estuary, a Tributary of Chesapeake Bay

Chesapeake Bay has a long history of nutrient pollution resulting in degraded water quality. However, we report improvements in chlorophyll a in surface waters and dissolved oxygen in bottom waters at one of three estuarine stations in the Choptank tributary of Chesapeake Bay. We updated a previous nutrient budget for the estuary constructed for reference year 1998 using rates of atmospheric deposition, inputs of watershed diffuse sources (primarily agriculture), and discharges of point sources (primarily human waste) for reference year 2017. Parallel trends suggest that improvements in water quality at the one station were likely due to 20% reductions in direct atmospheric deposition on the estuary’s surface and 78–95% reductions in wastewater N and P due to installation of tertiary treatment. The agricultural sector, the dominant source of N and P, appeared to provide little contribution to improved water quality during this period. Although efforts to reduce nutrient losses from agriculture are common throughout the Choptank basin, widespread reductions from agricultural diffuse sources could make large contributions to improved water quality at all stations in the estuary. The response in the Choptank is similar to those observed elsewhere in the USA, Europe, Australia, and New Zealand due to improved wastewater treatment. Similar to our findings, the upper Potomac River of Chesapeake Bay saw improvements driven by reductions in atmospheric deposition. Unfortunately, few studies elsewhere have shown improvements in water quality due to agricultural management. The data presented here indicate that public and industrial investments in reductions of atmospheric emissions and upgrades to wastewater treatment plants have improved estuarine water quality in the Choptank.

Response of river water chemistry to changing atmospheric environment and sulfur dynamics in a forested catchment in central Japan

Reduction of atmospheric sulfur (S) deposition and recovery of terrestrial ecosystems from acidification are matters of concerns in Asia. The Lake Ijira catchment (IJR) is located in the downwind region of the Chukyo Industrial Area in central Japan and has historically experienced large-scale deposition of S and nitrogen (N) from the atmosphere. Long-term monitoring data on the river water (RW) chemistry since 1988 were assessed with intensive-survey datasets on the input–output material budgets and S isotopic analysis (δ34S). Previous studies have suggested that IJR was acidified and N-saturated, which was triggered by climatic anomalies (cold summer and drought summer) in the mid-1990s. Analysis shows that with a decline in \( {\text{NO}}_{3}^{ - } \) concentrations, RW pH recovered to its original level in the early 2000s. Reductions in atmospheric deposition, diminished effects of climatic anomalies, and forest management practices, have all contributed to RW chemistry recovery. Although the \( {\text{SO}}_{4}^{2 - } \) concentration in the RW has declined continuously after the peak in 1994, the mean \( {\text{SO}}_{4}^{2 - } \) output significantly exceeded the input; the 5-year means from 2010 to 2014 are 2.5 kmolc ha−1 year−1 and 0.86 kmolc ha−1 year−1, respectively. The mean δ34S values of \( {\text{SO}}_{4}^{2 - } \) in rainwater and soil solution at 20 cm depth were 4.3 ‰ and 3.5 ‰, respectively, and that in the RW was −13.2‰. The contributions of groundwater S to the RW S were estimated to range from 75 to 91%. Geological S with significantly low δ34S values largely contributed to the discrepancy of the input–output budget, while atmospheric S appeared to accumulate in soil as organic S. The tree-ring δ34S profile recorded historical changes in the atmospheric inputs in the region. With recovery of the RW, the relative contribution of atmospheric S became smaller. However, most of the atmospheric S is still retained in soil. Over the last few decades, RW chemistry has sensitively responded to changes in the atmospheric environment, including the atmospheric deposition of S and N and climatic anomalies, and as future changes are likely, long-term monitoring is essential.

Contemporary Mobilization of Legacy Pb Stores by DOM in a Boreal Peatland.

We examined how different landscape areas in a catchment containing a northern ombrotrophic peatland and upland mineral soils responded to dramatic decreases in atmospheric deposition of lead (Pb). Pb concentrations in the outflow stream from the peatland measured from 2009-2015 indicated continued mobilization and export of Pb derived from historic inputs to the bog. In contrast, Pb concentrations in surface peat and runoff from upland mineral soils have declined in response to reductions in atmospheric deposition. Relative to the early 1980s, Pb concentrations in the streamflow decreased only ∼50%, while Pb in surface peat and upland subsurface runoff decreased by more than 90%. Water level fluctuations in the slow-accumulating peat have allowed dissolved organic matter (DOM) to continue mobilizing Pb deposited in the peatland decades earlier. Strong correlations between dissolved organic carbon (DOC) and Pb concentrations in outflow from the peatland and in bog porewaters demonstrate Pb mobility related to DOM production. Peat stores of Pb in 2016 were less than or equal to those reported in the early 1980s despite the dry mass inventory increasing by 60-80%. Much of the loss in Pb stored in peat can be accounted for by stream runoff from the peatland.

Long-term temporal trends and spatial patterns in the acid-base chemistry of lakes in the Adirondack region of New York in response to decreases in acidic deposition

We examined the response of lake water chemistry in the Adirondack Mountains of New York State, USA to decreases in acid deposition. Striking declines in the concentrations and fluxes of sulfate and hydrogen ion in wet deposition have been observed since the late 1970s, while significant decreases in nitrate have been evident since the early 2000s. Decreases in estimated dry sulfur and nitrate deposition have also occurred in the Adirondacks, but with no change in dry to wet deposition ratios. These patterns follow long-term decreases in anthropogenic emissions of sulfur dioxide and nitrogen oxides in the U.S. over the same interval. All of the 48 lakes monitored through the Adirondack Long-Term Monitoring program since 1992 have exhibited significant declines in sulfate concentrations, consistent with reductions in atmospheric deposition of sulfur. Nitrate concentrations have also significantly diminished at variable rates in many (33 of 48) lakes. Decreases in concentrations of sulfate plus nitrate (48 of 48) in lakes have driven widespread increases in acid neutralizing capacity (ANC; 42 of 48) and lab pH (33 of 48), and decreases in the toxic fraction, inorganic monomeric Al (45 of 48). Coincident with decreases in acid deposition, concentrations of dissolved organic carbon (DOC) have also increased in some (29 of 48) lakes. While recovery from elevated acid deposition is evident across Adirondack lakes, highly sensitive and impacted mounded seepages lakes and thin till drainage lakes are recovering most rapidly. Future research might focus on how much additional recovery could be achieved given the current deposition relative to future deposition anticipated under the Clean Power Plan, ecosystem effects of increased mobilization of dissolved organic matter, and the influence of changing climate on recovery from acidification.

Temporal Trends of PCDD/Fs in Baltic Sea Sediment Cores Covering the 20th Century

The pollution trend of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) in the Baltic Sea region was studied based on depth profiles of PCDD/Fs in sediment cores collected from six offshore areas, eight coastal sites impacted by industrial/urban emissions, and one coastal reference site. A general trend was observed for the offshore and coastal reference sites with substantial increase in PCDD/F concentrations in the mid-late 1970s and peak levels during 1985-2002. The overall peak year for PCDD/Fs in Baltic Sea offshore areas was estimated (using spline-fit modeling) to 1994 ± 5 years, and a half-life in sediments was estimated at 29 ± 11 years. For the industrial/urban impacted coastal sites, the temporal trend was more variable with peak years occurring 1-2 decades earlier compared to offshore areas. The substantial reductions from peak levels (38 ± 11% and 81 ± 12% in offshore and coastal areas, respectively) reflect domestic and international actions taken for reduction of the release of PCDD/Fs to the environment. The modeled overall half-life and reductions of PCDD/Fs in offshore Baltic Sea sediment correspond well to both PCDD/F trends in European lakes without any known direct PCDD/F sources (half-lives 30 and 32 years), and previously modeled reduction in atmospheric deposition of PCDD/Fs to the Baltic Sea since 1990. These observations support previous findings of a common diffuse source, such as long-range air transport of atmospheric emissions, as the prime source of PCDD/Fs to the Baltic Sea region. The half-life of PCDD/Fs in Baltic Sea offshore sediments was estimated to be approximately 2 and 4-6 times longer than in semirural and urban European air, respectively. This study highlights the need for further international actions to reduce the levels of PCDD/Fs in Baltic Sea air specifically and in European air in general.

Changes in the chemistry of acidified Adirondack streams from the early 1980s to 2008

Lakes in the Adirondack region of New York have partially recovered in response to declining deposition, but information on stream recovery is limited. Here we report results of Adirondack stream monitoring from the early 1980s to 2008. Despite a 50% reduction in atmospheric deposition of sulfur, overall increases in pH of only 0.28 and ANC of 13 μeq L−1 were observed in 12 streams over 23 years, although greater changes did occur in streams with lower initial ANC, as expected. In the North Tributary of Buck Creek with high dissolved organic carbon (DOC) concentrations, SO42− concentrations decreased from 1999 to 2008 at a rate of 2.0 μmol L−1 y−1, whereas in the neighboring South Tributary with low DOC concentrations, the decrease was only 0.73 μmol L−1 y−1. Ca2+ leaching decreased in the North Tributary due to the SO42− decrease, but this was partially offset by an increase in Ca2+ leaching from increased DOC concentrations.

Trace element pollution records in some UK lake sediments, their history, influence factors and regional differences

Sediment cores were taken from six sites across the UK. Apart from Banbury Reservoir in London, all the other sites are relatively remote lakes. Trace elements Pb, Zn, Cu, Cd, Cr, Ni, Sn, As and V, major elements such as Fe, Mn, Ti and Al were analysed, and organic content measured as loss-on-ignition was determined in all of these cores. The result shows that these relatively remote sites have experienced enhanced atmospheric deposition of anthropogenically derived trace elements for over 100 years, and the contamination might start before industrialisation. Trace metal contamination remains the highest level at Banbury Reservoir showing “pollution source” influence. Despite the considerable reduction in atmospheric deposition in recent years, although some of the element concentrations in the surface sediments have declined, they are still much higher than their natural background values. In these sites, trace element pollution records have been influenced by many different factors. Redox condition could affect As distribution in the sediments. Sediment matrix could also affect trace element pollution signal. Apart from direct atmospheric deposition, the distributions of trace elements in the sediments have been affected by forestry activities and catchment erosion, and more contaminated soil in-wash could increase sediment pollution whilst less contaminated soil could dilute sediment pollution. In some sites, data suggest that catchment in-wash is an important source of elements for the lakes.

Response of acid lakes in the UK to reductions in atmospheric deposition of sulfur

United Kingdom emissions of sulfur dioxide declined by 82% between 1970 and 2000. This decline has been accompanied by reductions in the atmospheric deposition of anthropogenic sulfur. A further expected response, possibly delayed, is a reduction in sulfur concentrations, as sulphate, in upland surface waters. Associated water quality changes, including an increase in alkalinity and reduction in acidity are also anticipated. We examine annual data from 1988 to the present from 10 lakes in the UK acid waters monitoring network for evidence of changes in water chemistry as a response to reductions in the atmospheric deposition of sulfur. We show that there is a close association between reduction in sulfur deposition and reduction in lake water concentrations of sulphate and this provides some supporting evidence for the efficacy of the international agreements to reduce S emissions. However, only 3 of the 10 lakes show an upward trend in alkalinity, and this is not related in a simple fashion to reductions in sulphate concentrations. This suggests that recovery from acidification, measured as an increase in pH and alkalinity, while requiring a reduction in sulphate concentration, may not occur over the same time scale.

Changes in large-scale patterns of plant biodiversity predicted from environmental economic scenarios

In the industrialized world large sums of money are spent on measures to preserve biodiversity by improving environmental quality. This creates a need to evaluate the effectiveness of such measures. In response we devel oped a model, NTM, that links plant biodiversity to abiotic variables that are under human control. These vari ables are: vegetation management, and the soil variables groundwater level, and nitrogen availability. We used species richness and the criteria of the Red Lists, i.e., the rarity and decline per species as measure for potential changes in biodiversity. NTM uses a statistical approach, and models potential plant biodiversity based on the above criteria as a non-linear function of the three soil variables. The regression model is calibrated on a data set consisting of 33,706 vegetation releves. Because field data of vegetation combined with measurements of soil variables are insufficiently available, we used the average of Ellenberg’s indicator values of the species in each releve as a proxy. NTM was subjected to both validation and uncertainty analysis. The validation was car ried out by comparison with an independent data set. The uncertainty analysis showed that uncertainty in abso lute biodiversity values is large, but that comparative scenario studies can be carried out with an acceptable uncertainty. As an example we show the evaluation of the impact of three European economic scenarios on po tential plant biodiversity in the Netherlands. Although there were differences per vegetation type and per region, potential plant biodiversity had a tendency to increase, with the highest increase for the scenario with the highest reduction in atmospheric deposition of nitrogen and acidity.

Temporal Trends in Mercury Accumulation in Lake Sediments in Sweden

Lake sediment cores were analyzedto study the history of mercury (Hg) pollution andparticularly to determine whether recent sedimentconcentrations have declined in response todeclining atmospheric deposition of Hg. Sedimentcores from 6 forest lakes distributed fromsouthern to northern Sweden and 3 northernmountain lakes were analyzed for Hg using CVAAS. A400 cm sediment profile from Makevatten insouthwest Sweden indicates that the onset of Hgpollution occurred in the 18th century. Anindisputable increase in Hg concentrationsoccurred concurrent with the appearance ofspheroidal carbonaceous flyash particles (SCP)derived from fossil-fuel combustion, in themid-19th century. There is a strong correlationbetween Hg and SCP concentrations in the sedimentcores (r=0.67 to 0.91), which suggests a strongrelationship between historical Hg pollution andfossil fuel burning. In contrast to sediment corestaken in 1979, maximum Hg concentrations are nowobserved below the sediment surface and declinetowards the sediment surface. This study confirmsthat reductions in atmospheric deposition of Hgover Sweden have resulted in a decreased transferof total Hg to aquatic environments as reflectedby lake sediments, and that lake sediment profilesof Hg concentrations reflect relative trends inthe atmospheric deposition of Hg rather thanpost-depositional diagenetic processes.

Simulated Responses of Red Spruce Forest Soils to Reduced Sulfur and Nitrogen Deposition

Implications of reducing S and N deposition on red spruce forests of the southern Appalachians are explored using the Nutrient Cycling Model (NuCM). We hypothesized that reducing deposition would cause (i) large reductions in soil solution NO{sub 3}{sup {minus}}, SO{sub 4}{sup 2{minus}}, Al and Ca/Al ratios, but (II) small changes in exchangeable base cation reserves. Hypothesis (I) was supported in part: simulated reductions in atmospheric deposition had substantial and nearly immediate effects upon soil solution mineral acid anions, Ca{sup 2+}, and Al{sup 3+} concentrations. Ca/Al molar ratios were much less sensitive to changes in deposition and soil solution ionic strength than either Ca{sup 2+} or Al{sup 3+} separately. Hypothesis (II) was not supported: although the increases in base saturation and exchangeable cation pools were small relative to cation exchange, they were large relative to initial exchangeable base cation pools. These changes in base cation pools and base saturation were of sufficient magnitude to affect simulated soil solution composition during a very short time. 29 refs., 11 figs., 2 tabs.

Sulphur mineralisation in five Danish soils as measured by plant uptake in a pot experiment

Reductions in atmospheric S deposition have created S deficiency in some agricultural soils. In such soils the release of S from organic matter may be important for the supply of S to plants. In this study net mineralisation of S was measured during two successive growth seasons as S removed by plant material and leachates. Pots were subjected to natural conditions and cropped with either Italian rye grass ( Lolium multiflorum Lam.) both years or spring oilseed rape ( Brassica napus L.) followed by spring barley ( Hordeum vulgare L.) Sulphur was the limiting factor for dry matter yield in the pots. Sulphur concentrations in Italian rye grass, rape and barley varied from 0.055 to 0.21, 0.06 to 0.078 to 0.17%, respectively. Net mineralisation was 3.3–6.7 μg S per g soil year −1 (1.7 to 3.1% of total organic S), and could not prevent S deficiency in the crops; differences among soils developed early in the experiment. Net mineralisation of S was not significantly correlated with total organic S, C-bonded S or sulphate-ester S content of the soils but with microbial activity in the soils ( r = 0.90). Net mineralisation was significantly affected by the type of cropping system but differences between systems were small compared to differences in net mineralisation among soils. It may be concluded that reductions in atmospheric deposition of S must, at least partly, be replaced by S fertilisation to maintain crop yield and quality.

Trends in stream quality in the continental United States, 1978–1987

The nonparametric seasonal Kendall's test, and a related multivariate test were used to analyze 403 National Stream Quality Accounting Network (NASQAN) stations for trend for the period 1978–1987. Nominal sampling frequencies were quarterly or bimonthly. For all groups and individual constituents, trends were detected for only a minority of stations at the relatively liberal 10% significance level. The groups with the greatest percentage of trends were common ions (mostly upward) and nutrients and suspended sediment (mostly upward for total nitrogen and mostly downward for total phosphorus). In the pH and alkalinity group, the trends were dominantly upward; while this might be the result of reductions in atmospheric deposition, this hypothesis is clouded by the existence of uptrends in sulfate at many of the same stations. The trace metal analyses showed that the constituents with the greatest number of trends (dominantly downward) were arsenic and cadmium; most of the stations with downtrends were in the major population areas of the east and midwest. Additional exploratory analyses of possible relationships between trends and land use and population did not give strong evidence of possible causation.