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Exposure of native bees foraging in an agricultural landscape to current-use pesticides

The awareness of insects as pollinators and indicators of environmental quality has grown in recent years, partially in response to declines in honey bee (Apis mellifera) populations. While most pesticide research has focused on honey bees, there has been less work on native bee populations. To determine the exposure of native bees to pesticides, bees were collected from an existing research area in northeastern Colorado from two land cover types: grasslands (2013-2014) and wheat fields (2014). Traps were deployed bi-monthly during the summer at each land cover type and all bees, regardless of species, were composited as whole samples and analyzed for 136 current-use pesticides and degradates. This reconnaissance approach provides a sampling of all species and represents overall pesticide exposure (internal and external). Nineteen pesticides and degradates were detected in 54 composite samples collected. Compounds detected in >10% of the samples included the insecticides thiamethoxam (46%), bifenthrin (28%), clothianidin (24%), chlorpyrifos (17%), and imidacloprid (13%), the fungicides azoxystrobin (17%), and pyraclostrobin (11%), and the herbicide atrazine (19%). Concentrations ranged from 1.1 to 312 ng/g for individual pesticides. Pesticides were detected in samples collected from both grasslands and wheat fields; the location of the sample and the surrounding land cover at the 1000 m buffer influenced the pesticides detected but because of a small number of temporally comparable samples, correlations between pesticide concentration and land cover were not significant. The results show native bees collected in both grasslands and wheat fields are exposed to multiple pesticides, these results can direct future research on routes/timing of pesticide exposure and the design of future conservation efforts for pollinators.

Colorado↗

A synthesis of terrestrial mercury in the western United States: Spatial distribution defined by land cover and plant productivity

A synthesis of published vegetation mercury (Hg) data across 11 contiguous states in the western United States showed that aboveground biomass concentrations followed the order: leaves (26 μg kg − 1 ) ~ branches (26 μg kg − 1 ) > bark (16 μg kg − 1 ) > bole wood (1 μg kg − 1 ). No spatial trends of Hg in aboveground biomass distribution were detected, which likely is due to very sparse data coverage and different sampling protocols. Vegetation data are largely lacking for important functional vegetation types such as shrubs, herbaceous species, and grasses. Soil concentrations collected from the published literature were high in the western United States, with 12% of observations exceeding 100 μg kg − 1 , reflecting a bias toward investigations in Hg-enriched sites. In contrast, soil Hg concentrations from a randomly distributed data set (1911 sampling points; Smith et al., 2013a) averaged 24 μg kg − 1 (A-horizon) and 22 μg kg − 1 (C-horizon), and only 2.6% of data exceeded 100 μg kg − 1 . Soil Hg concentrations significantly differed among land covers, following the order: forested upland > planted/cultivated > herbaceous upland/shrubland > barren soils. Concentrations in forests were on average 2.5 times higher than in barren locations. Principal component analyses showed that soil Hg concentrations were not or weakly related to modeled dry and wet Hg deposition and proximity to mining, geothermal areas, and coal-fired power plants. Soil Hg distribution also was not closely related to other trace metals, but strongly associated with organic carbon, precipitation, canopy greenness, and foliar Hg pools of overlying vegetation. These patterns indicate that soil Hg concentrations are related to atmospheric deposition and reflect an overwhelming influence of plant productivity — driven by water availability — with productive landscapes showing high soil Hg accumulation and unproductive barren soils and shrublands showing low soil Hg values. Large expanses of low-productivity, arid ecosystems across the western U.S. result in some of the lowest soil Hg concentrations observed worldwide.

Science of the Total Environment↗

Development and application of freshwater sediment-toxicity benchmarks for currently used pesticides

Sediment-toxicity benchmarks are needed to interpret the biological significance of currently used pesticides detected in whole sediments. Two types of freshwater sediment benchmarks for pesticides were developed using spiked-sediment bioassay (SSB) data from the literature. These benchmarks can be used to interpret sediment-toxicity data or to assess the potential toxicity of pesticides in whole sediment. The Likely Effect Benchmark (LEB) defines a pesticide concentration in whole sediment above which there is a high probability of adverse effects on benthic invertebrates, and the Threshold Effect Benchmark (TEB) defines a concentration below which adverse effects are unlikely. For compounds without available SSBs, benchmarks were estimated using equilibrium partitioning (EqP). When a sediment sample contains a pesticide mixture, benchmark quotients can be summed for all detected pesticides to produce an indicator of potential toxicity for that mixture. Benchmarks were developed for 48 pesticide compounds using SSB data and 81 compounds using the EqP approach. In an example application, data for pesticides measured in sediment from 197 streams across the United States were evaluated using these benchmarks, and compared to measured toxicity from whole-sediment toxicity tests conducted with the amphipod Hyalella azteca (28-d exposures) and the midge Chironomus dilutus (10-d exposures). Amphipod survival, weight, and biomass were significantly and inversely related to summed benchmark quotients, whereas midge survival, weight, and biomass showed no relationship to benchmarks. Samples with LEB exceedances were rare (n = 3), but all were toxic to amphipods (i.e., significantly different from control). Significant toxicity to amphipods was observed for 72% of samples exceeding one or more TEBs, compared to 18% of samples below all TEBs. Factors affecting toxicity below TEBs may include the presence of contaminants other than pesticides, physical/chemical characteristics of sediment, and uncertainty in TEB values. Additional evaluations of benchmarks in relation to sediment chemistry and toxicity are ongoing.

Science of the Total Environment↗

A millennial-scale record of Pb and Hg contamination in peatlands of the Sacramento-San Joaquin Delta of California, USA

In this paper, we provide the first record of millennial patterns of Pb and Hg concentrations on the west coast of the United States. Peat cores were collected from two micro-tidal marshes in the Sacramento-San Joaquin Delta of California. Core samples were analyzed for Pb, Hg, and Ti concentrations and dated using radiocarbon, 210Pb, and 137Cs. Pre-anthropogenic concentrations of Pb and Hg in peat ranged from 0.60 to 13.0 µg g-1and from 6.9 to 71 ng g-1, respectively. For much of the past 6000+ years, the Delta was free from anthropogenic pollution, however, beginning in ~1425 CE, Hg and Pb concentrations, Pb/Ti ratios, Pb enrichment factors (EFs), and HgEFs all increased. Pb isotope compositions of the peat suggest that this uptick was likely caused by smelting activities originating in Asia. The next increases in Pb and Hg contamination occurred during the California Gold Rush (beginning ~1850 CE), when concentrations reached their highest levels (74 µg g-1 Pb, 990 ng g-1 Hg; PbEF = 12 and HgEF = 28). Lead concentrations increased again beginning in the ~1920s with the incorporation of Pb additives in gasoline. The phase-out of lead additives in the late 1980s was reflected in Pb isotope ratios and reductions in Pb concentrations in the surface layers of the peat. The rise and fall of Hg contamination was also tracked by the peat archive, with the highest Hg concentrations occurring just before 1963 CE and then decreasing during the post-1963 period. Overall, the results show that the Delta was a pristine region for most of its ~6700-year existence; however, since ~1425 CE, it has received Pb and Hg contamination from both global and regional sources.

California↗

Negative effects of excessive soil phosphorus on floristic quality in Ohio wetlands

Excessive soil nutrients, often from agricultural runoff, have been shown to negatively impact some aspects of wetland plant communities. We measured plant-available phosphorus (Mehlich-3: MeP) in soil samples, and assessed the vascular plant community and habitat degradation at 27 emergent and 13 forested wetlands in Ohio, USA. We tested two hypotheses: (1) that an index of vegetation biological integrity based on floristic quality was lower in wetlands with higher concentrations of MeP in the soil, and (2) that higher concentrations of MeP occurred in wetlands with more habitat degradation (i.e., lower quality), as estimated by a rapid assessment method. Hypothesis (1) was supported for emergent, but not for forested wetlands. Hypothesis (2) was marginally supported ( P = 0.09) for emergent, but not supported for forested wetlands. The results indicate that the effect of concentration of phosphorus in wetland soils and the quality of plant species assemblages in wetlands is more complex than shown in site-specific studies and may depend in part on degree of disturbance in the surrounding watershed and dominant wetland vegetation type. Woody plants in forested wetlands are typically longer lived than herbaceous species in the understory and emergent wetlands, and may persist despite high inputs of phosphorus. Further, the forested wetlands were typically surrounded by a wide band of forest vegetation, which may provide a barrier against sedimentation and the associated phosphorus inputs to the wetland interior. Our results indicate that inferences about soil nutrient conditions made from rapid assessment methods for assessing wetland habitat condition may not be reliable.

Ohio↗

Comparison of in vitro estrogenic activity and estrogen concentrations insource and treated waters from 25 U.S. drinking water treatment plants

In vitro bioassays have been successfully used to screen for estrogenic activity in wastewater and surface water, however, few have been applied to treated drinking water. Here, extracts of source and treated water samples were assayed for estrogenic activity using T47D-KBluc cells and analyzed by liquid chromatography-Fourier transform mass spectrometry (LC-FTMS) for natural and synthetic estrogens (including estrone, 17β-estradiol, estriol, and ethinyl estradiol). None of the estrogenswere detected above the LC-FTMS quantification limits in treated samples and only 5 source waters had quantifiable concentrations of estrone, whereas 3 treated samples and 16 source samples displayed in vitro estrogenicity. Estrone accounted for themajority of estrogenic activity in respective samples, however the remaining samples that displayed estrogenic activity had no quantitative detections of known estrogenic compounds by chemical analyses. Source water estrogenicity (max, 0.47 ng 17β-estradiol equivalents (E2Eq) L−1) was below levels that have been linked to adverse effects in fish and other aquatic organisms. Treated water estrogenicity (max, 0.078 ng E2Eq L−1) was considerably below levels that are expected to be biologically relevant to human consumers. Overall, the advantage of using in vitro techniques in addition to analytical chemical determinations was displayed by the sensitivity of the T47D-KBluc bioassay, coupled with the ability tomeasure cumulative effects of mixtures, specifically when unknown chemicals may be present.

Science of the Total Environment↗

Comparison of mercury mass loading in streams to atmospheric deposition in watersheds of Western North America: Evidence for non-atmospheric mercury sources

Annual stream loads of mercury (Hg) and inputs of wet and dry atmospheric Hg deposition to the landscape were investigated in watersheds of the Western United States and the Canadian-Alaskan Arctic. Mercury concentration and discharge data from flow gauging stations were used to compute annual mass loads with regression models. Measured wet and modeled dry deposition were compared to annual stream loads to compute ratios of Hg stream load to total Hg atmospheric deposition. Watershed land uses or cover included mining, undeveloped, urbanized, and mixed. Of 27 watersheds that were investigated, 15 had some degree of mining, either of Hg or precious metals (gold or silver), where Hg was used in the amalgamation process. Stream loads in excess of annual Hg atmospheric deposition (ratio > 1) were observed in watersheds containing Hg mines and in relatively small and medium-sized watersheds with gold or silver mines, however, larger watersheds containing gold or silver mines, some of which also contain large dams that trap sediment, were sometimes associated with lower load ratios (< 0.2). In the non-Arctic regions, watersheds with natural vegetation tended to have low ratios of stream load to Hg deposition (< 0.1), whereas urbanized areas had higher ratios (0.34–1.0) because of impervious surfaces. This indicated that, in ecosystems with natural vegetation, Hg is retained in the soil and may be transported subsequently to streams as a result of erosion or in association with dissolved organic carbon. Arctic watersheds (Mackenzie and Yukon Rivers) had a relatively elevated ratio of stream load to atmospheric deposition (0.27 and 0.74), possibly because of melting glaciers or permafrost releasing previously stored Hg to the streams. Overall, our research highlights the important role of watershed characteristics in determining whether a landscape is a net source of Hg or a net sink of atmospheric Hg.

Science of the Total Environment↗

Surface-air mercury fluxes across Western North America: A synthesis of spatial trends and controlling variables

Mercury (Hg) emission and deposition can occur to and from soils, and are an important component of the global atmospheric Hg budget. This paper focuses on synthesizing existing surface-air Hg flux data collected throughout the Western North American region and is part of a series of geographically focused Hg synthesis projects. A database of existing Hg flux data collected using the dynamic flux chamber (DFC) approach from almost a thousand locations was created for the Western North America region. Statistical analysis was performed on the data to identify the important variables controlling Hg fluxes and to allow spatiotemporal scaling. The results indicated that most of the variability in soil-air Hg fluxes could be explained by variations in soil-Hg concentrations, solar radiation, and soil moisture. This analysis also identified that variations in DFC methodological approaches were detectable among the field studies, with the chamber material and sampling flushing flow rate influencing the magnitude of calculated emissions. The spatiotemporal scaling of soil-air Hg fluxes identified that the largest emissions occurred from irrigated agricultural landscapes in California. Vegetation was shown to have a large impact on surface-air Hg fluxes due to both a reduction in solar radiation reaching the soil as well as from direct uptake of Hg in foliage. Despite high soil Hg emissions from some forested and other heavily vegetated regions, the net ecosystem flux (soil flux + vegetation uptake) was low. Conversely, sparsely vegetated regions showed larger net ecosystem emissions, which were similar in magnitude to atmospheric Hg deposition (except for the Mediterranean California region where soil emissions were higher). The net ecosystem flux results highlight the important role of landscape characteristics in effecting the balance between Hg sequestration and (re-)emission to the atmosphere.

Science of the Total Environment↗

The importance of quality control in validating concentrationsof contaminants of emerging concern in source and treateddrinking water samples

A national-scale survey of 247 contaminants of emerging concern (CECs), including organic and inorganic chemical compounds, andmicrobial contaminants, was conducted in source and treated drinkingwater samples from 25 treatment plants across the United States.Multiplemethodswere used to determine these CECs, including six analytical methods tomeasure 174 pharmaceuticals, personal care products, and pesticides. A three-component quality assurance/quality control (QA/QC) programwas designed for the subset of 174 CECswhich allowed us to assess and compare performances of themethods used. The three components included: 1) a common field QA/ QC protocol and sample design, 2) individual investigator-developed method-specific QA/QC protocols, and 3) a suite of 46method comparison analytes thatwere determined in two or more analytical methods. Overallmethod performance for the 174 organic chemical CECs was assessed by comparing spiked recoveries in reagent, source, and treated water over a two-year period. In addition to the 247 CECs reported in the larger drinking water study, another 48 pharmaceutical compoundsmeasured did not consistentlymeet predetermined quality standards. Methodologies that did not seem suitable for these analytes are overviewed. The need to exclude analytes based on method performance demonstrates the importance of additional QA/QC protocols.

Science of the Total Environment↗

Organic contaminants in Great Lakes tributaries: Prevalence and potential aquatic toxicity

Organic compounds used in agriculture, industry, and households make their way into surface waters through runoff, leaking septic-conveyance systems, regulated and unregulated discharges, and combined sewer overflows, among other sources. Concentrations of these organic waste compounds (OWCs) in some Great Lakes tributaries indicate a high potential for adverse impacts on aquatic organisms. During 2010&ndash;13, 709 water samples were collected at 57 tributaries, together representing approximately 41% of the total inflow to the lakes. Samples were collected during runoff and low-flow conditions and analyzed for 69 OWCs, including herbicides, insecticides, polycyclic aromatic hydrocarbons, plasticizers, antioxidants, detergent metabolites, fire retardants, non-prescription human drugs, flavors/fragrances, and dyes. Urban-related land cover characteristics were the most important explanatory variables of concentrations of many OWCs. Compared to samples from nonurban watersheds (< 15% urban land cover) samples from urban watersheds (> 15% urban land cover) had nearly four times the number of detected compounds and four times the total sample concentration, on average. Concentration differences between runoff and low-flow conditions were not observed, but seasonal differences were observed in atrazine, metolachlor, DEET, and HHCB concentrations. Water quality benchmarks for individual OWCs were exceeded at 20 sites, and at 7 sites benchmarks were exceeded by a factor of 10 or more. The compounds with the most frequent water quality benchmark exceedances were the PAHs benzo[ a ]pyrene, pyrene, fluoranthene, and anthracene, the detergent metabolite 4-nonylphenol, and the herbicide atrazine. Computed estradiol equivalency quotients (EEQs) using only nonsteroidal endocrine-active compounds indicated medium to high risk of estrogenic effects (intersex or vitellogenin induction) at 10 sites. EEQs at 3 sites were comparable to values reported in effluent. This multifaceted study is the largest, most comprehensive assessment of the occurrence and potential effects of OWCs in the Great Lakes Basin to date.

Great Lakes↗

Mercury risk to avian piscivores across western United States and Canada

The widespread distribution of mercury (Hg) threatens wildlife health, particularly piscivorous birds. Western North America is a diverse region that provides critical habitat to many piscivorous bird species, and also has a well-documented history of mercury contamination from legacy mining and atmospheric deposition. The diversity of landscapes in the west limits the distribution of avian piscivore species, complicating broad comparisons across the region. Mercury risk to avian piscivores was evaluated across the western United States and Canada using a suite of avian piscivore species representing a variety of foraging strategies that together occur broadly across the region. Prey fish Hg concentrations were size-adjusted to the preferred size class of the diet for each avian piscivore (Bald Eagle = 36 cm, Osprey = 30 cm, Common and Yellow-billed Loon = 15 cm, Western and Clark's Grebe = 6 cm, and Belted Kingfisher = 5 cm) across each species breeding range. Using a combination of field and lab-based studies on Hg effect in a variety of species, wet weight blood estimates were grouped into five relative risk categories including: background (< 0.5 &mu;g/g), low (0.5&ndash;1 &mu;g/g), moderate (1&ndash;2 &mu;g/g), high (2&ndash;3 &mu;g/g), and extra high (> 3 &mu;g/g). These risk categories were used to estimate potential mercury risk to avian piscivores across the west at a 1 degree-by-1 degree grid cell resolution. Avian piscivores foraging on larger-sized fish generally were at a higher relative risk to Hg. Habitats with a relatively high risk included wetland complexes (e.g., prairie pothole in Saskatchewan), river deltas (e.g., San Francisco Bay, Puget Sound, Columbia River), and arid lands (Great Basin and central Arizona). These results indicate that more intensive avian piscivore sampling is needed across Western North America to generate a more robust assessment of exposure risk.

Science of the Total Environment↗

Hydrologic indicators of hot spots and hot moments of mercury methylation potential along river corridors

The biogeochemical cycling of metals and other contaminants in river-floodplain corridors is controlled by microbial activity responding to dynamic redox conditions. Riverine flooding thus has the potential to affect speciation of redox-sensitive metals such as mercury (Hg). Therefore, inundation history over a period of decades potentially holds information on past production of bioavailable Hg. We investigate this within a Northern California river system with a legacy of landscape-scale 19th century hydraulic gold mining. We combine hydraulic modeling, Hg measurements in sediment and biota, and first-order calculations of mercury transformation to assess the potential role of river floodplains in producing monomethylmercury (MMHg), a neurotoxin which accumulates in local and migratory food webs. We identify frequently inundated floodplain areas, as well as floodplain areas inundated for long periods. We quantify the probability of MMHg production potential (MPP) associated with hydrology in each sector of the river system as a function of the spatial patterns of overbank inundation and drainage, which affect long-term redox history of contaminated sediments. Our findings identify river floodplains as periodic, temporary, yet potentially important, loci of biogeochemical transformation in which contaminants may undergo change during limited periods of the hydrologic record. We suggest that inundation is an important driver of MPP in river corridors and that the entire flow history must be analyzed retrospectively in terms of inundation magnitude and frequency in order to accurately assess biogeochemical risks, rather than merely highlighting the largest floods or low-flow periods. MMHg bioaccumulation within the aquatic food web in this system may pose a major risk to humans and waterfowl that eat migratory salmonids, which are being encouraged to come up these rivers to spawn. There is a long-term pattern of MPP under the current flow regime that is likely to be accentuated by increasingly common large floods with extended duration.

California↗

Assessing potential health risks to fish and humans using mercury concentrations in inland fish from across western Canada and the United States

Fish represent high quality protein and nutrient sources, but Hg contamination is ubiquitous in aquatic ecosystems and can pose health risks to fish and their consumers. Potential health risks posed to fish and humans by Hg contamination in fish were assessed in western Canada and the United States. A large compilation of inland fish Hg concentrations was evaluated in terms of potential health risk to the fish themselves, health risk to predatory fish that consume Hg contaminated fish, and to humans that consume Hg contaminated fish. The probability that a fish collected from a given location would exceed a Hg concentration benchmark relevant to a health risk was calculated. These exceedance probabilities and their associated uncertainties were characterized for fish of multiple size classes at multiple health-relevant benchmarks. The approach was novel and allowed for the assessment of the potential for deleterious health effects in fish and humans associated with Hg contamination in fish across this broad study area. Exceedance probabilities were relatively common at low Hg concentration benchmarks, particularly for fish in larger size classes. Specifically, median exceedances for the largest size classes of fish evaluated at the lowest Hg concentration benchmarks were 0.73 (potential health risks to fish themselves), 0.90 (potential health risk to predatory fish that consume Hg contaminated fish), and 0.97 (potential for restricted fish consumption by humans), but diminished to essentially zero at the highest benchmarks and smallest fish size classes. Exceedances of benchmarks are likely to have deleterious health effects on fish and limit recommended amounts of fish humans consume in western Canada and the United States. Results presented here are not intended to subvert or replace local fish Hg data or consumption advice, but provide a basis for identifying areas of potential health risk and developing more focused future research and monitoring efforts.

Science of the Total Environment↗

Mercury and methylmercury in aquatic sediment across western North America

Large-scale assessments are valuable in identifying primary factors controlling total mercury (THg) and monomethyl mercury (MeHg) concentrations, and distribution in aquatic ecosystems. Bed sediment THg and MeHg concentrations were compiled for > 16,000 samples collected from aquatic habitats throughout the West between 1965 and 2013. The influence of aquatic feature type (canals, estuaries, lakes, and streams), and environmental setting (agriculture, forest, open-water, range, wetland, and urban) on THg and MeHg concentrations was examined. THg concentrations were highest in lake (29.3 ± 6.5 μg kg − 1 ) and canal (28.6 ± 6.9 μg kg − 1 ) sites, and lowest in stream (20.7 ± 4.6 μg kg − 1 ) and estuarine (23.6 ± 5.6 μg kg − 1 ) sites, which was partially a result of differences in grain size related to hydrologic gradients. By environmental setting, open-water (36.8 ± 2.2 μg kg − 1 ) and forested (32.0 ± 2.7 μg kg − 1 ) sites generally had the highest THg concentrations, followed by wetland sites (28.9 ± 1.7 μg kg − 1 ), rangeland (25.5 ± 1.5 μg kg − 1 ), agriculture (23.4 ± 2.0 μg kg − 1 ), and urban (22.7 ± 2.1 μg kg − 1 ) sites. MeHg concentrations also were highest in lakes (0.55 ± 0.05 μg kg − 1 ) and canals (0.54 ± 0.11 μg kg − 1 ), but, in contrast to THg, MeHg concentrations were lowest in open-water sites (0.22 ± 0.03 μg kg − 1 ). The median percent MeHg (relative to THg) for the western region was 0.7%, indicating an overall low methylation efficiency; however, a significant subset of data (n > 100) had percentages that represent elevated methylation efficiency (> 6%). MeHg concentrations were weakly correlated with THg (r 2 = 0.25) across western North America. Overall, these results highlight the large spatial variability in sediment THg and MeHg concentrations throughout western North America and underscore the important roles that landscape and land-use characteristics have on the MeHg cycle.

Science of the Total Environment↗

Reservoirs and water management influence fish mercury concentrations in the western United States and Canada

Anthropogenic manipulation of aquatic habitats can profoundly alter mercury (Hg) cycling and bioaccumulation. The impoundment of fluvial systems is among the most common habitat manipulations and is known to increase fish Hg concentrations immediately following impoundment. However, it is not well understood how Hg concentrations differ between reservoirs and lakes at large spatial and temporal scales or how reservoir management influences fish Hg concentrations. This study evaluated total Hg (THg) concentrations in 64,386 fish from 883 reservoirs and 1387 lakes, across the western United States and Canada, to assess differences between reservoirs and lakes, as well as the influence of reservoir management on fish THg concentrations. Fish THg concentrations were 1.4-fold higher in reservoirs (0.13 &plusmn; 0.011 &mu;g/g wet weight &plusmn; standard error) than lakes (0.09 &plusmn; 0.006), though this difference varied among ecoregions. Fish THg concentrations were 1.5- to 2.6-fold higher in reservoirs than lakes of the North American Deserts, Northern Forests, and Mediterranean California ecoregions, but did not differ between reservoirs and lakes in four other ecoregions. Fish THg concentrations peaked in three-year-old reservoirs then rapidly declined in 4&ndash;12 year old reservoirs. Water management was particularly important in influencing fish THg concentrations, which were up to 11-times higher in reservoirs with minimum water storage occurring in May, June, or July compared to reservoirs with minimum storage occurring in other months. Between-year changes in maximum water storage strongly influenced fish THg concentrations, but within-year fluctuations in water levels did not influence fish THg concentrations. Specifically, fish THg concentrations increased up to 3.2-fold over the range of between-year changes in maximum water storage in all ecoregions except Mediterranean California. These data highlight the role of reservoir creation and management in influencing fish THg concentrations and suggest that water management may provide an effective means of mitigating Hg bioaccumulation in some reservoirs.

Science of the Total Environment↗

Hg concentrations in fish from coastal waters of California and Western North America

The State of California conducted an extensive and systematic survey of mercury (Hg) in fish from the California coast in 2009 and 2010. The California survey sampled 3483 fish representing 46 species at 68 locations, and demonstrated that methylHg in fish presents a widespread exposure risk to fish consumers. Most of the locations sampled (37 of 68) had a species with an average concentration above 0.3 &mu;g/g wet weight (ww), and 10 locations an average above 1.0 &mu;g/g ww. The recent and robust dataset from California provided a basis for a broader examination of spatial and temporal patterns in fish Hg in coastal waters of Western North America. There is a striking lack of data in publicly accessible databases on Hg and other contaminants in coastal fish. An assessment of the raw data from these databases suggested the presence of relatively high concentrations along the California coast and in Puget Sound, and relatively low concentrations along the coasts of Alaska and Oregon, and the outer coast of Washington. The dataset suggests that Hg concentrations of public health concern can be observed at any location on the coast of Western North America where long-lived predator species are sampled. Output from a linear mixed-effects model resembled the spatial pattern observed for the raw data and suggested, based on the limited dataset, a lack of trend in fish Hg over the nearly 30-year period covered by the dataset. Expanded and continued monitoring, accompanied by rigorous data management procedures, would be of great value in characterizing methylHg exposure, and tracking changes in contamination of coastal fish in response to possible increases in atmospheric Hg emissions in Asia, climate change, and terrestrial Hg control efforts in coastal watersheds.

Science of the Total Environment↗

Decadal-scale export of nitrogen, phosphorus, and sediment from the Susquehanna River basin, USA: Analysis and synthesis of temporal and spatial patterns

The export of nitrogen (N), phosphorus (P), and suspended sediment (SS) is a long-standing management concern for the Chesapeake Bay watershed, USA. Here we present a comprehensive evaluation of nutrient and sediment loads over the last three decades at multiple locations in the Susquehanna River basin (SRB), Chesapeake's largest tributary watershed. Sediment and nutrient riverine loadings, including both dissolved and particulate fractions, have generally declined at all sites upstream of Conowingo Dam (non-tidal SRB outlet). Period-of-record declines in riverine yield are generally smaller than those in source input, suggesting the possibility of legacy contributions. Consistent with other watershed studies, these results reinforce the importance of considering lag time between the implementation of management actions and achievement of river quality improvement. Whereas flow-normalized loadings for particulate species have increased recently below Conowingo Reservoir, those for upstream sites have declined, thus substantiating conclusions from prior studies about decreased reservoir trapping efficiency. In regard to streamflow effects, statistically significant log-linear relationships between annual streamflow and annual constituent load suggest the dominance of hydrological control on the inter-annual variability of constituent export. Concentration-discharge relationships revealed general chemostasis and mobilization effects for dissolved and particulate species, respectively, both suggesting transport-limitation conditions. In addition to affecting annual export rates, streamflow has also modulated the relative importance of dissolved and particulate fractions, as reflected by its negative correlations with dissolved P/total P, dissolved N/total N, particulate P/SS, and total N/total P ratios. For land-use effects, period-of-record median annual yields of N, P, and SS all correlate positively with the area fraction of non-forested land but negatively with that of forested land under all hydrological conditions. Overall, this work has informed understanding with respect to four major factors affecting constituent export ( i.e. , source input, reservoir modulation, streamflow, and land use) and demonstrated the value of long-term river monitoring.

Maryland, New York, Pennsylvania↗

Endocrine disrupting activities of surface water associated with a West Virginia oil and gas industry wastewater disposal site

Currently, >95% of end disposal of hydraulic fracturing wastewater from unconventional oil and gas operations in the US occurs via injection wells. Key data gaps exist in understanding the potential impact of underground injection on surface water quality and environmental health. The goal of this study was to assess endocrine disrupting activity in surface water at a West Virginia injection well disposal site. Water samples were collected from a background site in the area and upstream, on, and downstream of the disposal facility. Samples were solid-phase extracted, and extracts assessed for agonist and antagonist hormonal activities for five hormone receptors in mammalian and yeast reporter gene assays. Compared to reference water extracts upstream and distal to the disposal well, samples collected adjacent and downstream exhibited considerably higher antagonist activity for the estrogen, androgen, progesterone, glucocorticoid and thyroid hormone receptors. In contrast, low levels of agonist activity were measured in upstream/distal sites, and were inhibited or absent at downstream sites with significant antagonism. Concurrent analyses by partner laboratories (published separately) describe the analytical and geochemical profiling of the water; elevated conductivity as well as high sodium, chloride, strontium, and barium concentrations indicate impacts due to handling of unconventional oil and gas wastewater. Notably, antagonist activities in downstream samples were at equivalent authentic standard concentrations known to disrupt reproduction and/or development in aquatic animals. Given the widespread use of injection wells for end-disposal of hydraulic fracturing wastewater, these data raise concerns for human and animal health nearby.

Science of the Total Environment↗