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At least 253 records · Page 14Linked to original sources

Changing regional emissions of airborne pollutants reflected in the chemistry of snowpacks and wetfall in the Rocky Mountain region, USA, 1993–2012

Wintertime precipitation sample data from 55 Snowpack sites and 17 National Atmospheric Deposition Program (NADP)/National Trends Network Wetfall sites in the Rocky Mountain region were examined to identify long-term trends in chemical concentration, deposition, and precipitation using Regional and Seasonal Kendall tests. The Natural Resources Conservation Service snow-telemetry (SNOTEL) network provided snow-water-equivalent data from 33 sites located near Snowpack- and NADP Wetfall-sampling sites for further comparisons. Concentration and deposition of ammonium, calcium, nitrate, and sulfate were tested for trends for the period 1993–2012. Precipitation trends were compared between the three monitoring networks for the winter seasons and downward trends were observed for both Snowpack and SNOTEL networks, but not for the NADP Wetfall network. The dry-deposition fraction of total atmospheric deposition, relative to wet deposition, was shown to be considerable in the region. Potential sources of regional airborne pollutant emissions were identified from the U.S. Environmental Protection Agency 2011 National Emissions Inventory, and from long-term emissions data for the period 1996–2013. Changes in the emissions of ammonia, nitrogen oxides, and sulfur dioxide were reflected in significant trends in snowpack and wetfall chemistry. In general, ammonia emissions in the western USA showed a gradual increase over the past decade, while ammonium concentrations and deposition in snowpacks and wetfall showed upward trends. Emissions of nitrogen oxides and sulfur dioxide declined while regional trends in snowpack and wetfall concentrations and deposition of nitrate and sulfate were downward.

Colorado, Idaho, Montana, New Mexico, Utah, Wyomin↗

Response of water chemistry and young-of-year brook trout to channel and watershed liming in streams showing lagging recovery from acidic deposition

Reductions in sulfur emissions have initiated chemical recovery of surface waters impacted by acidic deposition in the Adirondack region of New York State. However, acidified streams remain common in the region, which limits recovery of brook trout ( Salvelinus fontinalis ) populations. To investigate liming as a method to accelerate recovery of brook trout, the channels of two acidified streams were limed annually from 2012 to 2015, and an entire watershed of a third acidified tributary was limed by helicopter in 2013. Stream flow, water chemistry, and density of young-of-year (YOY) brook trout were measured in limed streams, an untreated acidified stream, and a buffered reference stream. Lime additions increased pH and acid-neutralizing capacity and decreased inorganic monomeric aluminum concentrations to less than 2.0 μmol/L, the minimum concentration at which in situ brook trout mortality has been documented. However, of the two channel-limed streams, only stream T8 showed a significant response (P < 0.01) in YOY density, increasing from a mean of 0.4 fish/m2 before liming to 2.7 fish/m2 after liming. No YOY brook trout response was observed in the stream within the limed watershed. Groundwater inputs to streams were identified by relative differences in temperature and concentrations of silica and sodium. YOY brook trout densities increased only in the channel-limed stream (T8) with suitable groundwater inputs for fall spawning and a summer nursery. Results suggest that targeted liming of acidified streams with the necessary groundwater habitat could be beneficial in accelerating recovery of brook trout populations.

New York↗

Variation of wet deposition chemistry in Sequoia National Park, California

Sequoia National Park has monitored wet deposition chemistry in conjunction with the National Atmospheric Deposition Program and National Trends Network (NADP/NTN), on a weekly basis since July, 1980. Annual deposition of H, NO 3 and SO 4 (0.045, 3.6, and 3.9 kg ha −1 a −1 , respectively) is relatively low compared to that measured in the eastern United States, or in the urban Los Angeles and San Francisco areas. Weekly ion concentrations are highly variable. Maximum concentrations of 324,162, and 156 μeq ol −1 of H, NO 3 and SO 4 have been recorded for one low volume summer storm (1.4 mm). Summer concentrations of NO 3 and SO 4 average two and five times higher, respectively, than concentrations reported for remote areas in the world. There is considerable variability in the ionic concentration of low volume samples, and much less variability in moderate and high volume samples.

California↗

Chemistry and petrography of calcite in the KTB pilot borehole, Bavarian Oberpfalz, Germany

The KTB pilot borehole in northeast Bavaria, Germany, penetrates 4000 m of gneiss, amphibolite, and subordinate calc-silicate, lamprophyre and metagabbro. There are three types of calcite in the drilled section: 1) metamorphic calcite in calc-silicate and marble; 2) crack-filling calcite in all lithologies; and 3) replacement calcite in altered minerals. Crack-filling and replacement calcite postdate metamorphic calcite. Multiple calcite generations in individual cracks suggest that different generations of water repeatedly flowed through the same cracks. Crack-filling mineral assemblages that include calcite originally formed at temperatures of 150-350??C. Presently, crack-filling calcite is in chemical and isotopic equilibrium with saline to brackish water in the borehole at temperatures of ???120??C. The saline to brackish water contains a significant proportion of meteoric water. Re-equilibration of crack-filling calcite to lower temperatures means that calcite chemistry tells us little about water-rock interactions in the crystal section of temperatures higher than ~120??C. -from Author

Chemical Geology↗

Inorganic ground-water chemistry at an experimental New Albany Shale (Devonian-Mississippian) in situ gasification site

Experimental in situ gasification of New Albany Shale (Devonian-Mississippian) has been conducted in Clark County. Analyses of ground water sampled from a production well and nine nearby monitoring wells 3 months after a brief in situ gasification period revealed changes in water chemistry associated with the gasification procedure. Dissolved iron, calcium and sulphate in ground water from the production well and wells as much as 2 m away were significantly higher than in ground water from wells over 9 m away. Dissolved components in the more distant wells are in the range of those in regional ground water. Thermal decomposition of pyrite during the gasification process generated the elevated levels of iron and sulphate in solution. High concentrations of calcium indicate buffering by dissolution of carbonate minerals. While iron quickly precipitates, calcium and sulphate remain in the ground water. Trends in the concentration of sulphate show that altered ground water migrated mostly in a south-westerly direction from the production well along natural joints in the New Albany Shale.

Indiana↗

Chemistry and isotope ratios of sulfur in basalts and volcanic gases at Kilauea volcano, Hawaii

Eighteen basalts and some volcanic gases from the submarine and subaerial parts of Kilauea volcano were analyzed for the concentration and isotope ratios of sulfur. By means of a newly developed technique, sulfide and sulfate sulfur in the basalts were separately but simultaneously determined. The submarine basalt has 700 ± 100 ppm total sulfur with δ 34 S Σs of 0.7 &#xB1; 0.1 &#x2030; ">‰ 0.7 ± 0.1 ‰ . The sulfate/sulfide molar ratio ranges from 0.15 to 0.56 and the fractionation factor between sulfate and sulfide is +7.5 &#xB1; 1.5&#x2030; ">‰ +7.5 ± 1.5‰ . On the other hand, the concentration and δ 34 S Σs values of the total sulfur in the subaerial basalt are reduced to 150 ± 50 ppm and &#x2212;0.8 &#xB1; 0.2&#x2030; ">‰ −0.8 ± 0.2‰ , respectively. The sulfate to sulfide ratio and the fractionation factor between them are also smaller, 0.01 to 0.25 and +3.0‰, respectively. Chemical and isotopic evidence strongly suggests that sulfate and sulfide in the submarine basalt are in chemical and isotopic equilibria with each other at magmatic conditions. Their relative abundance and the isotope fractionation factors may be used to estimate the &#x192;o 2 "> ƒo 2 and temperature of these basalts at the time of their extrusion onto the sea floor. The observed change in sulfur chemistry and isotopic ratios from the submarine to subaerial basalts can be interpreted as degassing of the SO 2 from basalt thereby depleting sulfate and 34 S in basalt. The volcanic sulfur gases, predominantly SO 2 , from the 1971 and 1974 fissures in Kilauea Crater have δ 34 S values of 0.8 to 0.9%., slightly heavier than the total sulfur in the submarine basalts and definitely heavier than the subaerial basalts, in accord with the above model. However, the δ 34 S value of sulfur gases (largely SO 2 ) from Sulfur Bank is 8.0%., implying a secondary origin of the sulfur. The δ 34 S values of native sulfur deposits at various sites of Kilauea and Mauna Loa volcanos, sulfate ions of four deep wells and hydrogen sulfide from a geothermal well along the east rift zone are also reported. The high δ 34 S values (+5 to +6%. o ) found for the hydrogen sulfide might be an indication of hot basalt seawater reaction beneath the east rift zone.

Geochimica et Cosmochimica Acta↗

A note on the chemistry of seawater in the range 350°-500°C

The chemistry of seawater at conditions of 350&deg; to 500&deg;C, 220 to 1000 bars (22 to 100 MPa) is controlled by reactions involving magnesium hydroxide sulfate (MHSH) and anhydrite. During progressive heating from 350&deg; to 500&deg;C at 1000 bars (100 MPa), MHSH with a ratio of 1.25 is formed via precipitation from solution and via reaction of solution with pre-existing anhydrite. During adiabatic expansion the MHSH extracts additional SO 4 from seawater and converts to a stoichiometry in which . These reactions control and greatly change the concentrations of Ca, Mg, SO 4 in solution and produce significant ionizable hydrogen, attaining 11.7 mmoles kg &minus;1 at maximum conditions.

Geochimica et Cosmochimica Acta↗

Chemistry and transport of soluble humic substances in forested watersheds of the Adirondack Park, New York

Studies were conducted in conjunction with the Integrated Lake-Watershed Acidification Study (ILWAS) to examine the chemistry and leaching patterns of soluble humic substances in forested watersheds of the Adirondack region. During the summer growing season, mean dissolved organic carbon (DOC) concentrations in the ILWAS watersheds ranged from 21–32 mg C l −1 in O/A horizon leachates, from 5–7 mg C l −1 in B horizon leachates, from 2–4 mg C l −1 in groundwater solutions, from 6–8 mg C l −1 in first order streams, from 3–8 mg C l −1 in lake inlets, and from 2–7 mg C l −1 in lake outlets. During the winter, mean DOC concentrations dropped significantly in the upper soil profile. Soil solutions from mixed and coniferous stands contained as much as twice the DOC concentration of lysimeter samples from hardwood stands. Results of DOC fractionation analysis showed that hydrophobia and hydrophilic acids dominate the organic solute composition of natural waters in these watersheds. Charge balance and titration results indicated that the general acid-base characteristics of the dissolved humic mixture in these natural waters can be accounted for by a model organic acid having an average p K a of 3.85, an average charge density of 4–5 μeq mg −1 C at ambient pH, and a total of 6–7 meq COOH per gram carbon.

New York↗

Surface chemistry associated with the cooling and subaerial weathering of recent basalt flows

The surface chemistry of fresh and weathered historical basalt flows was characterized using surface-sensitive X-ray photoelectron spectroscopy (XPS). Surfaces of unweathered 1987–1990 flows from the Kilauea Volcano, Hawaii, exhibited variable enrichment in Al, Mg, Ca, and F due to the formation of refractory fluoride compounds and pronounced depletion in Si and Fe from the volatilization of SiF 4 and FeF 3 during cooling. These reactions, as predicted from shifts in thermodynamic equilibrium with temperature, are induced by diffusion of HF from the flow interiors to the cooling surface. The lack of Si loss and solid fluoride formation for recent basalts from the Krafla Volcano, Iceland, suggest HF degassing at higher temperatures. Subsequent short-term subaerial weathering reactions are strongly influenced by the initial surface composition of the flow and therefore its cooling history. Successive samples collected from the 1987 Kilauea flow demonstrated that the fluoridated flow surfaces leached to a predominantly SiO 2 composition by natural weathering within one year. These chemically depleted surfaces were also observed on Hawaiian basalt flows dating back to 1801 AD. Solubility and kinetic models, based on thermodynamic and kinetic data for crystalline AlF 3 , MgF 2 , and CaF 2 , support observed elemental depletion rates due to chemical weathering. Additional loss of alkalis from the Hawaiian basalt occurs from incongruent dissolution of the basalt glass substrate during weathering.

Geochimica et Cosmochimica Acta↗

On the chemistry of Jupiter's upper atmosphere

We conduct a first investigation into the ion-molecule chemistry of the upper Jovian atmosphere. Experimental results show that intense ultraviolet radiation reacts with the constituents of the Jovian atmosphere to produce C 2 H 4 , C 2 H 6 , C 3 H 8 , and higher polymers. The general procedure for calculating both equilibrium and nonequilibrium abundances of these products is formulated and applied to the case of the surface passage of a satellite shadow. A specific example is made of ethylene, for which an analytical approximation gives 10 10 molecules in an atmospheric column of 1 cm 2 cross section after a very rapid rise to equilibrium. Such a concentration of ethylene does not substantially affect the infrared radiation in the shadow.

Icarus↗

Organic geochemistry and pore water chemistry of sediments from Mangrove Lake, Bermuda

Mangrove Lake, Bermuda, is a small coastal, brackish-water lake that has accumulated 14 m of banded, gelatinous, sapropelic sediments in less than 10 4 yr. Stratigraphic evidence indicates that Mangrove Lake's sedimentary environment has undergone three major depositional changes (peat, freshwater gel, brackish-water gel) as a result of sea level changes. The deposits were examined geochemically in an effort to delineate sedimentological and diagenetic changes. Gas and pore water studies include measurements of sulfides, ammonia, methane, nitrogen gas, calcium, magnesium, chloride, alkalinity, and pH. Results indicate that sulfate reduction is complete, and some evidence is presented for bacterial denitrification and metal sulfide precipitation. The organic-rich sapropel is predominantly algal in origin, composed mostly of carbohydrates and insoluble macromolecular organic matter called humin with minor amounts of proteins, lipids, and humic acids. Carbohydrates and proteins undergo hydrolysis with depth in the marine sapropel but tend to be preserved in the freshwater sapropel. The humin, which has a predominantly aliphatic structure, increases linearly with depth and composes the greatest fraction of the organic matter. Humic acids are minor components and are more like polysaccharides than typical marine humic acids. Fatty acid distributions reveal that the lipids are of an algal and/or terrestrial plant source. Normal alkanes with a total concentration of 75 ppm exhibit two distribution maxima. One is centered about n -C 22 with no odd/even predominance, suggestive of a degraded algal source. The other is centered at n -C 31 with a distinct odd/even predominance indicative of a vascular plant origin. Stratigraphic changes in the sediment correlate to observed changes in the gas and pore water chemistry and the organic geochemistry.

Mangrove Lake↗

The influence of mountain meteorology on precipitation chemistry at low and high elevations of the Colorado Front Range, USA

We explored the seasonal characteristics in wet deposition chemistry for two sites located at different elevations along the east slope of the Colorado Front Range in Rocky Mountain National Park. Seasonally separated precipitation was stratified into highly concentrated (high salt), dilute (low salt), or acid-dominated precipitation groups. These groups and unstratified precipitation data were related to mean easterly or westerly zonal winds to determine direction of local transport. Strong acid anion associations were also determined for the stratified and unstratified precipitation data sets. We found that strong acid anions, acidity, ammonium, and high salt concentrations originate to the east of Rocky Mountain National Park, and are transported via up-valley funneling winds or convective instability from differential heating of the mountains and the plains to the east. These influence the composition of precipitation at Beaver Meadows, the low elevation site, throughout the year, while their effect on precipitation at Loch Vale, the high elevation site, is felt most strongly during the summer. During the winter, Loch Vale precipitation is very dilute, and occurs in conjunction with westerly winds resulting from the southerly location of the jet stream.

Colorado↗

The springs of Lake Pátzcuaro: chemistry, salt-balance, and implications for the water balance of the lake

Lake Pa??tzcuaro, the center of the ancient Tarascan civilization located in the Mexican altiplano west of the city of Morelia, has neither river input nor outflow. The relatively constant lake-salinity over the past centuries indicates the lake is in chemical steady state. Springs of the south shore constitute the primary visible input to the lake, so influx and discharge must be via sub-lacustrine ground water. The authors report on the chemistry and stable isotope composition of the springs, deeming them representative of ground-water input. The springs are dominated by Ca, Mg and Na, whereas the lake is dominated by Na. Combining these results with previously published precipitation/rainfall measurements on the lake, the authors calculate the chemical evolution from spring water to lake water, and also calculate a salt balance of the ground-water-lake system. Comparing Cl and ??18O compositions in the springs and lake water indicates that 75-80% of the spring water is lost evaporatively during evolution toward lake composition. During evaporation Ca and Mg are lost from the water by carbonate precipitation. Each liter of spring water discharging into the lake precipitates about 18.7 mg of CaCO3. Salt balance calculations indicate that ground water input to the lake is 85.9??106 m3/a and ground water discharge from the lake is 23.0??106 m3/a. Thus, the discharge is about 27% of the input, with the rest balanced by evaporation. A calculation of time to reach steady-state ab initio indicates that the Cl concentration of the present day lake would be reached in about 150 a. ?? 2004 Elsevier Ltd. All rights reserved.

Applied Geochemistry↗

Responses of soil and water chemistry to mountain pine beetle induced tree mortality in Grand County, Colorado, USA

Pine forest in northern Colorado and southern Wyoming, USA, are experiencing the most severe mountain pine beetle epidemic in recorded history, and possible degradation of drinking-water quality is a major concern. The objective of this study was to investigate possible changes in soil and water chemistry in Grand County, Colorado in response to the epidemic, and to identify major controlling influences on stream-water nutrients and C in areas affected by the mountain pine beetle. Soil moisture and soil N increased in soils beneath trees killed by the mountain pine beetle, reflecting reduced evapotranspiration and litter accumulation and decay. No significant changes in stream-water NO 3 - "> NO 3 - or dissolved organic C were observed; however, total N and total P increased, possibly due to litter breakdown or increased productivity related to warming air temperatures. Multiple-regression analyses indicated that % of basin affected by mountain pine beetles had minimal influence on stream-water NO 3 - "> NO 3 - and dissolved organic C; instead, other basin characteristics, such as percent of the basin classified as forest, were much more important.

Colorado↗

Evolution of the chemistry of Fe bearing waters during CO 2 degassing

The rates of Fe(II) oxidation and precipitation from groundwater are highly pH dependent. Elevated levels of dissolved CO 2 can depress pH and cause difficulty in removing dissolved Fe and associated metals during treatment of ferruginous water. This paper demonstrates interdependent changes in pH, dissolved inorganic C species, and Fe(II) oxidation rates that occur as a result of the removal (degassing) of CO 2 during aeration of waters discharged from abandoned coal mines. The results of field monitoring of aeration cascades at a treatment facility as well as batchwise aeration experiments conducted using net alkaline and net acidic waters in the UK are combined with geochemical modelling to demonstrate the spatial and temporal evolution of the discharge water chemistry. The aeration cascades removed approximately 67% of the dissolved CO 2 initially present but varying the design did not affect the concentration of Fe(II) leaving the treatment ponds. Continued removal of the residual CO 2 by mechanical aeration increased pH by as much as 2 units and resulted in large increases in the rates of Fe(II) oxidation and precipitation. Effective exsolution of CO 2 led to a reduction in the required lime dose for removal of remaining Fe(II), a very important factor with regard to increasing the sustainability of treatment practices. An important ancillary finding for passive treatment is that varying the design of the cascades had little impact on the rate of CO 2 removal at the flow rates measured.

Applied Geochemistry↗

Modeling and management of pit lake water chemistry 1: Theory

Pit lakes are permanent hydrologic/landscape features that can result from open pit mining for metals, coal, uranium, diamonds, oil sands, and aggregates. Risks associated with pit lakes include local and regional impacts to water quality and related impacts to aquatic and terrestrial ecosystems. Stakeholders rely on predictive models of water chemistry to prepare for and manage these risks. This paper is the first of a two part series on the modeling and management of pit lakes. Herein, we review approaches that have been used to quantify wall-rock runoff geochemistry, wall-rock leachate geochemistry, pit lake water balance, pit lake limnology (i.e. extent of vertical mixing), and pit lake water quality, and conclude with guidance on the application of models within the mine life cycle. The purpose of this paper is to better prepare stakeholders, including future modelers, mine managers, consultants, permitting agencies, land management agencies, regulators, research scientists, academics, and other interested parties, for the challenges of predicting and managing future pit lakes in un-mined areas.

Applied Geochemistry↗

Trends in snowpack chemistry and comparison to National Atmospheric Deposition Program results for the Rocky Mountains, US, 1993-2004

Seasonal snowpack chemistry data from the Rocky Mountain region of the US was examined to identify long-term trends in concentration and chemical deposition in snow and in snow-water equivalent. For the period 1993-2004, comparisons of trends were made between 54 Rocky Mountain Snowpack sites and 16 National Atmospheric Deposition Program wetfall sites located nearby in the region. The region was divided into three subregions: Northern, Central, and Southern. A non-parametric correlation method known as the Regional Kendall Test was used. This technique collectively computed the slope, direction, and probability of trend for several sites at once in each of the Northern, Central, and Southern Rockies subregions. Seasonal Kendall tests were used to evaluate trends at individual sites. Significant trends occurred during the period in wetfall and snowpack concentrations and deposition, and in precipitation. For the comparison, trends in concentrations of ammonium, nitrate, and sulfate for the two networks were in fair agreement. In several cases, increases in ammonium and nitrate concentrations, and decreases in sulfate concentrations for both wetfall and snowpack were consistent in the three subregions. However, deposition patterns between wetfall and snowpack more often were opposite, particularly for ammonium and nitrate. Decreases in ammonium and nitrate deposition in wetfall in the central and southern rockies subregions mostly were moderately significant (p<0.11) in constrast to highly significant increases in snowpack (p<0.02). These opposite trends likely are explained by different rates of declining precipitation during the recent drought (1999-2004) and increasing concentration. Furthermore, dry deposition was an important factor in total deposition of nitrogen in the region. Sulfate deposition decreased with moderate to high significance in all three subregions in both wetfall and snowpack. Precipitation trends consistently were downward and significant for wetfall, snowpack, and snow-telemetry data for the central and southern rockies subregions (p<0.03), while no trends were noted for the Northern Rockies subregion.

Atmospheric Environment↗

Trends in precipitation chemistry across the U.S. 1985–2017: Quantifying the benefits from 30 years of Clean Air Act amendment regulation

Acid rain was first recognized in the 1970s in North America and Europe as an atmospheric pollutant that was causing harm to ecosystems. In response, the U.S. Congress enacted Title IV of the Clean Air Act Amendments (CAA) in 1990 to reduce sulfur and nitrogen emissions from fossil fuel burning power plants. This study reports trends in wet-precipitation chemistry in response to emissions reductions implemented as part of the CAA. Trends were calculated for sulfate (SO 4 ), nitrate (NO 3 ) and ammonium (NH 4 ) from 1985 to 2017 at 168 stations operated by the National Atmospheric Deposition Program (NADP); stations were divided into 9 regions across the United States. Trend analyses were conducted for three time periods: Period 1 (1985–1999), Period 2 (2000–2017), and the entire study period (1985–2017). Seasonal and regional Kendall trend analyses reveal significant decreasing trends in mean wet-precipitation SO 4 concentrations in all 9 regions during the entire study period. The largest decreasing trends in monthly mean SO 4 precipitation-weighted concentrations were measured in the Mid-Atlantic (−1.29 μeq/l/yr), Midwest (−1.15 μeq/l/yr), and Northeast regions (−1.10 μeq/l/yr). The trends in monthly mean NO 3 concentrations were not as strong as those for SO 4 , but all of the regions had significant decreasing trends in NO 3 and again the Mid-Atlantic (−0.53 μeq/l/yr), Midwest (−0.44 μeq/l/yr), and Northeast regions (−0.50 μeq/l/yr) had the strongest trends. Trends were steepest during Period 2 for SO 4 and NO 3 , in fact for NO 3 86% of the stations had significant decreasing trends during Period 2 while only 8% of the stations had significant decreasing trends during Period 1. The stations with the highest concentrations of SO 4 and NO 3 at the beginning of the study had the strongest decreasing trends and the relations were stronger during Period 2 than Period 1. For NH 4 , 22% of the stations had statistically significant increasing trends in concentration during Period 1. The largest increasing trends in wet-precipitation NH 4 concentration occurred in the North-Central region during Period 1, Period 2 and throughout the entire study. By comparison, NH 4 trends in the Rocky-North and Rocky-South regions were about half as steep and trends in the South-Central and Midwest regions were about one-third as steep. We compared trends in SO 4 and NO 3 concentrations from NADP stations to emissions of sulfur dioxide and nitrogen oxides, respectively to determine whether there was a relation between emissions and wet-precipitation concentration trends within proximity to NADP stations. There was a statistically significant relation (r 2 = 0.62–0.69, p < 0.01) between the trend in SO 4 concentrations at individual NADP stations and total and mean sulfur dioxide (SO 2 ) emissions from power plants within a range of 750 km and 1000 km from each station. There were also significant relations between NO 3 concentration trends at NADP stations and power plant emissions of nitrogen oxides, but they were not nearly as strong (r 2 = 0.18–0.36, p < 0.01) as those for SO 4 and were strongest for emissions within a range of 1000 km and 1500 km from each NADP station. Decreases in wet-precipitation SO 4 concentrations were more consistent across regions and through time than decreases in NO 3 and SO 4 trends were more closely linked to stationary emissions sources than NO 3 trends. There were statistically significant increases in NH 4 wet-precipitation concentrations, as have been reported in previous studies, but this study found that those increases were strongest during Period 1 and were not consistent across the United States. During the first 3 years of the study period, wet-precipitation acidity was dominated by SO 4 in 8 of the 9 regions; by 2017 NO 3 dominated the acidity of wet-precipitation in 7 of the 9 regions. There has also been a downward shift in the NO 3 :NH 4 ratio of wet-precipitation as the emissions of nitrogen oxides have declined while ammonia emissions have remained essentially constant. This shift has resulted in an increase in wet-precipitation total nitrogen concentrations in 7 of the 9 regions and indicate that efforts to control NH 3 emissions will become increasingly important as emissions of nitrogen oxides continue to decline.

Atmospheric Environment↗