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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

Effect of variable annual precipitation and nutrient input on nitrogen and phosphorus transport from two Midwestern agricultural watersheds

Precipitation patterns and nutrient inputs affect transport of nitrate (NO 3 -N) and phosphorus (TP) from Midwest watersheds. Nutrient concentrations and yields from two subsurface-drained watersheds, the Little Cobb River (LCR) in southern Minnesota and the South Fork Iowa River (SFIR) in northern Iowa, were evaluated during 1996&ndash;2007 to document relative differences in timings and amounts of nutrients transported. Both watersheds are located in the prairie pothole region, but the SFIR exhibits a longer growing season and more livestock production. The SFIR yielded significantly more NO 3 -N than the LCR watershed (31.2 versus 21.3 kg NO 3 -N ha &minus; 1 y &minus; 1 ). The SFIR watershed also yielded more TP than the LCR watershed (1.13 versus 0.51 kg TP ha &minus; 1 yr &minus; 1 ), despite greater TP concentrations in the LCR. About 65% of NO 3 -N and 50% of TP loads were transported during April&ndash;June, and < 20% of the annual loads were transported later in the growing season from July&ndash;September. Monthly NO 3 -N and TP loads peaked in April from the LCR but peaked in June from the SFIR; this difference was attributed to greater snowmelt runoff in the LCR. The annual NO 3 -N yield increased with increasing annual runoff at a similar rate in both watersheds, but the LCR watershed yielded less annual NO 3 -N than the SFIR for a similar annual runoff. These two watersheds are within 150 km of one another and have similar dominant agricultural systems, but differences in climate and cropping inputs affected amounts and timing of nutrient transport.

Science of the Total Environment

Nationwide reconnaissance of contaminants of emerging concern in source and treated drinking waters of the United States: Pharmaceuticals

Mobile and persistent chemicals that are present in urban wastewater, such as pharmaceuticals, may survive on-site ormunicipal wastewater treatment and post-discharge environmental processes. These pharmaceuticals have the potential to reach surface and groundwaters, essential drinking-water sources. A joint, two-phase U.S. Geological Survey-U.S. Environmental Protection Agency study examined source and treated waters from 25 drinking-water treatment plants from across the United States. Treatment plants that had probable wastewater inputs to their source waters were selected to assess the prevalence of pharmaceuticals in such source waters, and to identify which pharmaceuticals persist through drinking-water treatment. All samples were analyzed for 24 pharmaceuticals in Phase I and for 118 in Phase II. In Phase I, 11 pharmaceuticals were detected in all source-water samples, with amaximumof nine pharmaceuticals detected in any one sample. The median number of pharmaceuticals for all 25 samples was five. Quantifiable pharmaceutical detections were fewer, with a maximum of five pharmaceuticals in any one sample and a median for all samples of two. In Phase II, 47 different pharmaceuticals were detected in all source-water samples, with a maximum of 41 pharmaceuticals detected in any one sample. The median number of pharmaceuticals for all 25 samples was eight. For 37 quantifiable pharmaceuticals in Phase II, median concentrations in source water were below 113 ng/L.

Science of the Total Environment

Spatiotemporal patterns of mercury accumulation in lake sediments of western North America

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 0.2 μg/m 2 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.

Alaska, Alberta, Arizona, British Columbia, Califo

Microbial pathogens in source and treated waters from drinking water treatment plants in the United States and implications for human health

An occurrence survey was conducted on selected pathogens in source and treated drinking water collected from 25 drinking water treatment plants (DWTPs) in the United States. Water samples were analyzed for the protozoa Giardia and Cryptosporidium (EPA Method 1623); the fungi Aspergillus fumigatus , Aspergillus niger and Aspergillus terreus (quantitative PCR [qPCR]); and the bacteria Legionella pneumophila (qPCR), Mycobacterium avium , M. avium subspecies paratuberculosis , and Mycobacterium intracellulare (qPCR and culture). Cryptosporidium and Giardia were detected in 25% and in 46% of the source water samples, respectively (treated waters were not tested). Aspergillus fumigatus was the most commonly detected fungus in source waters (48%) but none of the three fungi were detected in treated water. Legionella pneumophila was detected in 25% of the source water samples but in only 4% of treated water samples. M. avium and M. intracellulare were both detected in 25% of source water, while all three mycobacteria were detected in 36% of treated water samples. Five species of mycobacteria, Mycobacterium mucogenicum , Mycobacterium phocaicum , Mycobacterium triplex , Mycobacterium fortuitum , and Mycobacterium lentiflavum were cultured from treated water samples. Although these DWTPs represent a fraction of those in the U.S., the results suggest that many of these pathogens are widespread in source waters but that treatment is generally effective in reducing them to below detection limits. The one exception is the mycobacteria, which were commonly detected in treated water, even when not detected in source waters.

Science of the Total Environment

Spatial and temporal patterns of mercury concentrations in freshwater fish across the Western United States and Canada

Methylmercury contamination of fish is a global threat to environmental health. Mercury (Hg) monitoring programs are valuable for generating data that can be compiled for spatially broad syntheses to identify emergent ecosystem properties that influence fish Hg bioaccumulation. Fish total Hg (THg) concentrations were evaluated across the Western United States (US) and Canada, a region defined by extreme gradients in habitat structure and water management. A database was compiled with THg concentrations in 96,310 fish that comprised 206 species from 4262 locations, and used to evaluate the spatial distribution of fish THg across the region and effects of species, foraging guilds, habitats, and ecoregions. Areas of elevated THg exposure were identified by developing a relativized estimate of fish mercury concentrations at a watershed scale that accounted for the variability associated with fish species, fish size, and site effects. THg concentrations in fish muscle ranged between 0.001 and 28.4 (&mu;g/g wet weight (ww)) with a geometric mean of 0.17. Overall, 30% of individual fish samples and 17% of means by location exceeded the 0.30 &mu;g/g ww US EPA fish tissue criterion. Fish THg concentrations differed among habitat types, with riverine habitats consistently higher than lacustrine habitats. Importantly, fish THg concentrations were not correlated with sediment THg concentrations at a watershed scale, but were weakly correlated with sediment MeHg concentrations, suggesting that factors influencing MeHg production may be more important than inorganic Hg loading for determining fish MeHg exposure. There was large heterogeneity in fish THg concentrations across the landscape; THg concentrations were generally higher in semi-arid and arid regions such as the Great Basin and Desert Southwest, than in temperate forests. Results suggest that fish mercury exposure is widespread throughout Western US and Canada, and that species, habitat type, and region play an important role in influencing ecological risk of mercury in aquatic ecosystems.

Science of the Total Environment

Modeled effects of soil acidification on long-term ecological and economic outcomes for managed forests in the Adirondack region (USA)

Sugar maple ( Acer saccharum ) is among the most ecologically and economically important tree species in North America, and its growth and regeneration is often the focus of silvicultural practices in northern hardwood forests. A key stressor for sugar maple (SM) is acid rain, which depletes base cations from poorly-buffered forest soils and has been associated with much lower SM vigor, growth, and recruitment. However, the potential interactions between forest management and soil acidification &ndash; and their implications for the sustainability of SM and its economic and cultural benefits &ndash; have not been investigated. In this study, we simulated the development of 50 extant SM stands in the western Adirondack region of NY (USA) for 100 years under different soil chemical conditions and silvicultural prescriptions. We found that interactions between management prescription and soil base saturation will strongly shape the ability to maintain SM in managed forests. Below 12% base saturation, SM did not regenerate sufficiently after harvest and was replaced mainly by red maple ( Acer rubrum ) and American beech ( Fagus grandifolia ). Loss of SM on acid-impaired sites was predicted regardless of whether the shelterwood or diameter-limit prescriptions were used. On soils with sufficient base saturation, models predicted that SM will regenerate after harvest and be sustained for future rotations. We then estimated how these different post-harvest outcomes, mediated by acid impairment of forest soils, would affect the potential monetary value of ecosystem services provided by SM forests. Model simulations indicated that a management strategy focused on syrup production &ndash; although not feasible across the vast areas where acid impairment has occurred &ndash; may generate the greatest economic return. Although pollution from acid rain is declining, its long-term legacy in forest soils will shape future options for sustainable forestry and ecosystem stewardship in the northern hardwood forests of North America.

New York