Air pollution is commonly disregarded as a source of nutrient loading to impaired surface waters managed under the Clean Water Act per states’ 303(d) list programs. The contribution of air pollution ...to 2017–2018 South Platte River nitrogen (N) loads was estimated from the headwaters to the gage at Weldona, Colorado, USA (100 km downstream of Denver), using data from the National Atmospheric Deposition Program (NADP) and the SPAtially Referenced Regressions On Watershed attributes (SPARROW) model. The NADP offers wet-deposition raster created by spatial interpolation of data collected from regionally representative monitoring sites, excluding the influences from urban site data. For this study, NADP wet-deposition data obtained from sites within the Denver-Boulder, Colorado, urban corridor were included and excluded in new spatial interpolations of wet-deposition raster, which were used as input for SPARROW to model the influence of urban air pollution sources on South Platte River loads. Because urban air pollution is already incorporated into the NADP Total Deposition modeling methodology, dry N deposition was held constant for each SPARROW modeling scenario when dry deposition was included. By including the urban wet-deposition data in the model, estimated N loading to the South Platte River at Denver increased by 9–11 percent. Factoring in dry deposition at a 1:1.8 dry:wet ratio obtained from the results, urban air pollution was estimated to contribute as much as 20 percent of the nitrate Total Maximum Daily Load for Segment 14 of the South Platte River.
•Urban air pollution accounts for 8–13 percent of river N loads at Denver.•SPARROW model uses National Atmospheric Deposition Program data for river loading.•Atmospheric deposition contributes to water-quality impairment in South Platte Basin.
Transit times are hypothesized to influence catchment sensitivity to atmospheric deposition of acidity and nitrogen (N) because they help determine the amount of time available for infiltrating ...precipitation to interact with catchment soil and biota. Transit time metrics, including fraction of young water (Fyw) and mean transit time (MTT), were calculated for 11 headwater catchments in mountains of the western United States based on differences in the amplitude of the seasonal signal of δ18O in streamflow and precipitation. Results were statistically compared with catchment characteristics to elucidate controlling mechanisms. Transit times also were compared with stream solute concentrations to test the hypothesis that transit times are a primary influence on weathering rates and biological assimilation of atmospherically deposited N. Results indicate that transit times in the study catchments are strongly related to soil, vegetation, and topographic characteristics, with barren terrain (bare rock and talus) and steep slopes linked to high Fyw and short MTT, whereas forest soil (hydrogroup B) was linked to low Fyw and greater MTT. Concentrations of silicate weathering products (Na+ and Si) were negatively related to Fyw and barren terrain, and positively related to MTT and forest soil, supporting the concept that weathering fluxes and buffering capacity tend to be low in alpine areas due to short transit times. Nitrate concentrations were positively related to N deposition, catchment slope, and barren terrain, and negatively related to forest, indicating that hydrologic and/or biogeochemical processes associated with steep slopes limit uptake of atmospherically deposited N by biota. Interannual and seasonal variability in transit times and source water contributions in the study catchments was substantial, reflecting the influence of strong temporal variations in snowmelt inputs in high‐elevation catchments of the western United States. Results from this study confirm that short transit times in these areas are a key reason they are highly sensitive to atmospheric pollution and climate change.
National Atmospheric Deposition Program (NADP)/National Trends Network precipitation type, snow-season duration, and annual timing of selected chemical wet-deposition maxima vary with latitude and ...longitude within a 35-year (1979–2013) data record for the contiguous United States and Alaska. From the NADP data collected within the region bounded by 35.6645°–48.782° north latitude and 124°–68° west longitude, similarities in latitudinal and longitudinal patterns of changing snow-season duration, fraction of annual precipitation recorded as snow, and the timing of chemical wet-deposition maxima, suggest that the chemical climate of the atmosphere is linked to physical changes in climate. Total annual precipitation depth has increased 4–6 % while snow season duration has decreased from approximately 7 to 21 days across most of the USA, except in higher elevation regions where it has increased by as much as 21 days. Snow-season precipitation is increasingly comprised of snow, but annually total precipitation is increasingly comprised of liquid precipitation. Meanwhile, maximum ammonium deposition occurs as much as 27 days earlier, and the maximum nitrate: sulfate concentration ratio in wet-deposition occurs approximately 10–21 days earlier in the year. The maximum crustal (calcium + magnesium + potassium) cation deposition occurs 2–35 days earlier in the year. The data suggest that these shifts in the timing of atmospheric wet deposition are linked to a warming climate, but the ecological consequences are uncertain.
The Hydrologic Benchmark Network (HBN) is a long-term monitoring program established by the US Geological Survey in the 1960s to track changes in the streamflow and stream chemistry in undeveloped ...watersheds across the USA. Trends in stream chemistry were tested at 15 HBN stations over two periods (1970–2010 and 1990–2010) using the parametric Load Estimator (LOADEST) model and the nonparametric seasonal Kendall test. Trends in annual streamflow and precipitation chemistry also were tested to help identify likely drivers of changes in stream chemistry. At stations in the northeastern USA, there were significant declines in stream sulfate, which were consistent with declines in sulfate deposition resulting from the reductions in SO
2
emissions mandated under the Clean Air Act Amendments. Sulfate declines in stream water were smaller than declines in deposition suggesting sulfate may be accumulating in watershed soils and thereby delaying the stream response to improvements in deposition. Trends in stream chemistry at stations in other part of the country generally were attributed to climate variability or land disturbance. Despite declines in sulfate deposition, increasing stream sulfate was observed at several stations and appeared to be linked to periods of drought or declining streamflow. Falling water tables might have enhanced oxidation of organic matter in wetlands or pyrite in mineralized bedrock thereby increasing sulfate export in surface water. Increasing sulfate and nitrate at a station in the western USA were attributed to release of soluble salts and nutrients from soils following a large wildfire in the watershed.
Elevated selenium (Se) concentrations in surface water and groundwater have become a concern in areas of the Western United States due to the deleterious effects of Se on aquatic ecosystems. Elevated ...Se concentrations are most prevalent in irrigated alluvial valleys underlain by Se-bearing marine shales where Se can be leached from geologic materials into the shallow groundwater and surface water systems. This study presents groundwater chemistry and solid-phase geochemical data from the Uncompahgre River Basin in Western Colorado, an irrigated alluvial landscape underlain by Se-rich Cretaceous marine shale. We analyzed Se species, major and trace elements, and stable nitrogen and oxygen isotopes of nitrate in groundwater and aquifer sediments to examine processes governing selenium release and transport in the shallow groundwater system. Groundwater Se concentrations ranged from below detection limit (<0.5μgL−1) to 4070μgL−1, and primarily are controlled by high groundwater nitrate concentrations that maintain oxidizing conditions in the aquifer despite low dissolved oxygen concentrations. High nitrate concentrations in non-irrigated soils and nitrate isotopes indicate nitrate is largely derived from natural sources in the Mancos Shale and alluvial material. Thus, in contrast to areas that receive substantial NO3 inputs through inorganic fertilizer application, Se mitigation efforts that involve limiting NO3 application might have little impact on groundwater Se concentrations in the study area. Soluble salts are the primary source of Se to the groundwater system in the study area at-present, but they constitute a small percentage of the total Se content of core material. Sequential extraction results indicate insoluble Se is likely composed of reduced Se in recalcitrant organic matter or discrete selenide phases. Oxidation of reduced Se species that constitute the majority of the Se pool in the study area could be a potential source of Se in the future as soluble salts are progressively depleted.
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•Selenium is characterized in groundwater and aquifer sediments in an alluvial valley.•Groundwater nitrate derived from geologic materials controls groundwater Se concentrations.•Oxidized, soluble selenium species are more abundant in alluvial sediments.•Reduced, insoluble selenium species are more abundant in shale sediments.
The small watershed approach is well-suited but underutilized in mercury research. We applied the small watershed approach to investigate total mercury (THg) and methylmercury (MeHg) dynamics in ...streamwater at the five diverse forested headwater catchments of the US Geological Survey Water, Energy, and Biogeochemical Budgets (WEBB) program. At all sites, baseflow THg was generally less than 1
ng L
−1 and MeHg was less than 0.2
ng L
−1. THg and MeHg concentrations increased with streamflow, so export was primarily episodic. At three sites, THg and MeHg concentration and export were dominated by the particulate fraction in association with POC at high flows, with maximum THg (MeHg) concentrations of 94 (2.56)
ng L
−1 at Sleepers River, Vermont; 112 (0.75)
ng L
−1 at Rio Icacos, Puerto Rico; and 55 (0.80)
ng L
−1 at Panola Mt., Georgia. Filtered (<0.7
μm) THg increased more modestly with flow in association with the hydrophobic acid fraction (HPOA) of DOC, with maximum filtered THg concentrations near 5
ng L
−1 at both Sleepers and Icacos. At Andrews Creek, Colorado, THg export was also episodic but was dominated by filtered THg, as POC concentrations were low. MeHg typically tracked THg so that each site had a fairly constant MeHg/THg ratio, which ranged from near zero at Andrews to 15% at the low-relief, groundwater-dominated Allequash Creek, Wisconsin. Allequash was the only site with filtered MeHg consistently above detection, and the filtered fraction dominated both THg and MeHg. Relative to inputs in wet deposition, watershed retention of THg (minus any subsequent volatilization) was 96.6% at Allequash, 60% at Sleepers, and 83% at Andrews. Icacos had a net export of THg, possibly due to historic gold mining or frequent disturbance from landslides. Quantification and interpretation of Hg dynamics was facilitated by the small watershed approach with emphasis on event sampling.
High-flow sampling reveals strong contrasts in total mercury and methylmercury cycling in five diverse USA watersheds.
Long-term patterns of stream nitrate export and atmospheric N deposition were evaluated over three decades in Loch Vale, a high-elevation watershed in the Colorado Front Range. Stream nitrate ...concentrations increased in the early 1990s, peaked in the mid-2000s, and have since declined by over 40%, coincident with trends in nitrogen oxide emissions over the past decade. Similarities in the timing and magnitude of N deposition provide evidence that stream chemistry is responding to changes in atmospheric deposition. The response to deposition was complicated by a drought in the early 2000s that enhanced N export for several years. Other possible explanations, including forest disturbance, snow depth, or permafrost melting, could not explain patterns in N export. Our results show that stream chemistry responds rapidly to changes in N deposition in high-elevation watersheds, similar to the response observed to changes in sulfur deposition.
For the Western North America Mercury Synthesis, we compiled mercury records from 165 dated sediment cores from 138 natural lakes across western North America. Lake sediments are accepted as faithful ...recorders of historical mercury accumulation rates, and regional and sub-regional temporal and spatial trends were analyzed with descriptive and inferential statistics. Mercury accumulation rates in sediments have increased, on average, four times (4×) from 1850 to 2000 and continue to increase by approximately 0.2μg/m2 per year. Lakes with the greatest increases were influenced by the Flin Flon smelter, followed by lakes directly affected by mining and wastewater discharges. Of lakes not directly affected by point sources, there is a clear separation in mercury accumulation rates between lakes with no/little watershed development and lakes with extensive watershed development for agricultural and/or residential purposes. Lakes in the latter group exhibited a sharp increase in mercury accumulation rates with human settlement, stabilizing after 1950 at five times (5×) 1850 rates. Mercury accumulation rates in lakes with no/little watershed development were controlled primarily by relative watershed size prior to 1850, and since have exhibited modest increases (in absolute terms and compared to that described above) associated with (regional and global) industrialization. A sub-regional analysis highlighted that in the ecoregion Northwestern Forest Mountains, <1% of mercury deposited to watersheds is delivered to lakes. Research is warranted to understand whether mountainous watersheds act as permanent sinks for mercury or if export of “legacy” mercury (deposited in years past) will delay recovery when/if emissions reductions are achieved.
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•We compiled Hg records from lakes across western North America.•Hg accumulation rates increased, on average, four times from 1850 to 2000.•Regional and global emissions of Hg to the atmosphere result in enhanced Hg deposition.•Watershed disturbance exacerbates the problem, by reducing the retention of Hg in soils.•Hg deposition rates are highest near urban areas, where watershed disturbance is greatest.
Changes in stream chemistry were studied for 4 years following large wildfires that burned in Glacier National Park during the summer of 2003. Burned and unburned drainages were monitored from ...December 2003 through August 2007 for streamflow, major constituents, nutrients, and suspended sediment following the fires. Stream-water nitrate concentrations showed the greatest response to fire, increasing up to tenfold above those in the unburned drainage just prior to the first post-fire snowmelt season. Concentrations in winter base flow remained elevated during the entire study period, whereas concentrations during the growing season returned to background levels after two snowmelt seasons. Annual export of total nitrogen from the burned drainage ranged from 1·53 to 3·23 kg ha⁻¹ yr⁻¹ compared with 1·01 to 1·39 kg ha⁻¹ yr⁻¹ from the unburned drainage and exceeded atmospheric inputs for the first two post-fire water years. Fire appeared to have minimal long-term effects on other nutrients, dissolved organic carbon, and major constituents with the exception of sulfate and chloride, which showed increased concentrations for 2 years following the fire. There was little evidence that fire affected suspended-sediment concentrations in the burned drainage. Sediment yields in subalpine streams may be less affected by fire than in lower elevation streams because of the slow release rate of water during spring snowmelt. Published in 2008 by John Wiley & Sons, Ltd.
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