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Holistic assessment of occurrence and fate of metolachlor within environmental compartments of agricultural watersheds

Background : Metolachlor [(RS)-2-Chloro- N -(2-ethyl-6-methyl-phenyl)- N -(1-methoxypropan-2-yl)acetamide] and two degradates (metolachlor ethane-sulfonic acid and metolachlor oxanilic acid) are commonly observed in surface and groundwater. The behavior and fate of these compounds were examined over a 12-year period in seven agricultural watersheds in the United States. They were quantified in air, rain, streams, overland flow, groundwater, soil water, subsurface drain water, and water at the stream/groundwater interface. The compounds were frequently detected in surface and groundwater associated with agricultural areas. A mass budget approach, based on all available data from the study and literature, was used to determine a percentage-wise generalized distribution and fate of applied parent metolachlor in typical agricultural environments. Results : In these watersheds, about 90% of applied metolachlor was taken up by plants or degraded, 10% volatilized, and 0.3% returned as rainfall. One percent was transported to surface water, while an equal amount infiltrated into the unsaturated zone soil water. < 0.02% reached the groundwater. Subsurface flow paths resulted in greater degradation of metolachlor because degradation reactions had more time to proceed. Conclusions : An understanding of the residence times of water in the different environmental compartments, and the important processes affecting metolachlor as it is transported along flowpaths among the environmental compartments allows for a degree of predictability of metolachlor's fate. Degradates with long half-lives can be used (in a limited capacity) as tracers of metolachlor, because of their persistence and widespread occurrence in the environment.

Science of the Total Environment↗

New-generation pesticides are prevalent in California's Central Coast streams

Pesticides are widely recognized as important biological stressors in streams, especially in heavily developed urban and agricultural areas like the Central California Coast region. We assessed occurrence and potential toxicity of pesticides in small streams in the region using two analytical methods: a broad-spectrum (223 compounds) method in use since 2012 and a newly developed method for 30 additional new-generation fungicides and insecticides. At least one pesticide compound was identified in 83 of the 85 streams sampled. About one-half (48%) of the 253 pesticides measured were detected at least once and 27 were detected in 10% or more of samples. Three of the top 4, and 6 of the top 10 most frequently detected compounds (chlorantraniliprole, dinotefuran, boscalid, thiamethoxam, clothianidin and the fluopicolide degradate 2,6-dichlorobenzamide) were analyzed by the new method. Pesticide mixtures were common, with two or more pesticide compounds detected in 81% of samples and 10 or more in 32% of samples. The pesticide count at a site was relatively consistent over the 6-week study. Four sites with mixed land-use in the lower basin (<5 km from the sampling site) tended to have the highest pesticide counts and the highest concentrations. Potential toxicity (assessed by comparison to benchmarks) to invertebrates was much more common than potential toxicity to fish or plants and was associated with a wide array of insecticides. The common occurrence of new-generation pesticides highlights the need to continuously update analytical methods to keep pace with changing pesticide use for a fuller assessment of pesticide occurrence and effects on the environment.

California↗

Finding minimal herbicide concentrations in ground water? Try looking for their degradates

Extensive research has been conducted regarding the occurrence of herbicides in the hydrologic system, their fate, and their effects on human health and the environment. Few studies, however, have considered herbicide transformation products (degradates). In this study of Iowa ground water, herbicide degradates were frequently detected. In fact, herbicide degradates were eight of the 10 most frequently detected compounds. Furthermore, a majority of a herbicide's measured concentration was in the form of its degradates &mdash; ranging from 55 to over 99%. The herbicide detection frequencies and concentrations varied significantly among the major aquifer types sampled. These differences, however, were much more pronounced when herbicide degradates were included. Aquifer types presumed to have the most rapid recharge rates (alluvial and bedrock/karst region aquifers) were those most likely to contain detectable concentrations of herbicide compounds. Two indirect estimates of ground-water age (depth of well completion and dissolved-oxygen concentration) were used to separate the sampled wells into general vulnerability classes (low, intermediate, and high). The results show that the herbicide detection frequencies and concentrations varied significantly among the vulnerability classes regardless of whether or not herbicide degradates were considered. Nevertheless, when herbicide degradates were included, the frequency of herbicide compound detection within the highest vulnerability class approached 90%, and the median total herbicide residue concentration increased over an order of magnitude, relative to the parent compounds alone, to 2 &mu;g/l. The results from this study demonstrate that obtaining data on herbicide degradates is critical for understanding the fate of herbicides in the hydrologic system. Furthermore, the prevalence of herbicide degradates documented in this study suggests that to accurately determine the overall effect on human health and the environment of a specific herbicide its degradates should also be considered.

Iowa↗

Urban proximity while breeding is not a predictor of perfluoroalkyl substance contamination in the eggs of brown pelicans

Identifying sources of exposure to chemical stressors is difficult when both target organisms and stressors are highly mobile. While previous studies have demonstrated that populations of some organisms proximal to urban centers may display increased burdens of human-created chemicals compared to more distal populations, this relationship may not be universal when applied to organisms and stressors capable of transboundary movements. We examined eggs of brown pelicans ( Pelecanus occidentalis ), a nearshore seabird with daily movements ranging from local to 50 km and annual migrations ranging from year-round residency to 1500 km. Thirty-six eggs from three breeding colonies located at increasing distances to a major urban center (Charleston, South Carolina, USA) were analyzed for concentrations of per - and polyfluoroalkyl substances (PFAS). Areas of high use for each colony during the breeding season were also assessed via the tracking of adult pelicans from each colony using GPS-PTT satellite transmitters and overlapped with measures of relative urbanization via land cover data. We report potentially significant ∑PFAS concentrations in the eggs of pelicans (175.4 ± 120.1 ng/g w wt. SD), driven largely by linear perfluorooctane sulfonate (n-PFOS) (48–546 ng/g w wt.). Residues of the precursor compound perfluorooctane sulfonamide (FOSA) were also present in pelican eggs, suggesting continued exposure of local wildlife beyond implemented phaseouts of some PFAS. For most analytes, egg concentrations did not exhibit a significant spatial structure despite some differentiation in high-use areas unlike similar data for another regional apex predator, the bottlenose dolphin ( Tursiops truncatus ). We suggest that the partially migratory nature of brown pelicans during the non-breeding season, combined with daily ranges that may extend to 50 km from local point sources, may have homogenized exposure across individuals. Charleston likely remains a major source for PFAS in the overall region, however, given the high concentrations observed as well as known releases of PFAS in the nearshore environment.

South Carolina↗

Using SPMDs for monitoring hydrophobic organic compounds in urban river water in Korea compared with using conventional water grab samples

We aimed to verify the effectiveness of semi-permeablemembrane devices (SPMDs) formonitoring hydrophobic organic compounds, such as polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs), that are not easy to detect using conventional grab samples (because of their low concentrations), in water.We used SPMDs and grab samples to monitor PCBs and PBDEs upstream and downstream of a sewage treatment plant (STP) in the Suyeong River in Busan, Korea. Concentrations in three different phases (freely dissolved, apparently dissolved, and particulate) were measured, to investigate the aquatic fate of PCBs and PBDEs. The freely dissolved (SPMD) concentrations were 2–3 times higher than the apparently dissolved and particulate phase (grab sample) concentrations. No meaningful relationships were found between the total PCB and PBDE concentrations of the grab sample and SPMD sample because of the different partitioning behaviors and detection frequencies of the individual chemicals. However, the summed concentrations of specific PCB and PBDE congeners (that were abundant in all samples) in the grab and SPMD samples correlated well (r 2 = 0.7451 for PCBs 28 + 52 + 153, r 2 = 0.9987 for PBDEs 28 + 47 + 99). The PBDE concentrations measured using SPMDs decreased with increasing distance from the STP, but no apparent dilution effect was found in the grab samples. Our results show that SPMDs could be used to support grab sampling for specific chemicals, or to trace chemical sources (such as STPs) to the aquatic environment.

Science of the Total Environment↗

Is there a risk associated with the insect repellent DEET (N,N-diethyl-m-toluamide) commonly found in aquatic environments?

DEET ( N , N -diethyl- m -toluamide) is the active ingredient of most commercial insect repellents. This compound has commonly been detected in aquatic water samples from around the world indicating that DEET is both mobile and persistent, despite earlier assumptions that DEET was unlikely to enter aquatic ecosystems. DEET's registration category does not require an ecological risk assessment, thus information on the ecological toxicity of DEET is sparse. This paper reviews the presence of DEET in aqueous samples from around the world (e.g. drinking water, streams, open seawater, groundwater and treated effluent) with reported DEET concentrations ranging from 40–3000 ng L − 1 . In addition, new DEET data collected from 36 sites in coastal waterways from eastern Australia (detections ranging from 8 to 1500 ng L − 1 ) are examined. A summary of new and existing toxicity data are discussed with an emphasis on preparing a preliminary risk assessment for DEET in the aquatic environment. Collated information on DEET in the aquatic environment suggests risk to aquatic biota at observed environmental concentrations is minimal. However, the information available was not sufficient to conduct a full risk assessment due to data deficiencies in source characterisation, transport mechanisms, fate, and ecotoxicity studies. These risks warrant further investigation due to the high frequency that this organic contaminant is detected in aquatic environments around the world.

Science of the Total Environment↗

Germination potential of baldcypress (Taxodium distichum) swamp soil seed bank along geographical gradients

Changing environments of temperature, precipitation and moisture availability can affect vegetation in ecosystems, by affecting regeneration from the seed bank. Our objective was to explore the responses of soil seed bank germination to climate-related environments along geographic gradients. We collected seed banks in baldcypress ( Taxodium distichum ) swamps along the Mississippi River and the Gulf of Mexico Coast in the United States, which have distinct temperature and/or precipitation gradients, and germinated them in a greenhouse. The frequency, richness and seed density of species germinated from the seed bank were compared between various geographic locations, experimental water regimes (saturated, flooded) and wetland types (tidal, non-tidal and inland swamps). We also analyzed the relationship of seed density to the environment by using a Non-metric Multi-dimensional Scaling (NMDS) model. Sixty-one species germinated from the seed bank, differing in pattern by geographic location, experimental water regime and wetland type. The foundation species (i.e., T. distichum and Cephalanthus occidentalis ) germinated with a niche affinity for the northern part of the latitudinal gradient (Tennessee and Illinois) and these species may shift northward with climate change. Some species had higher seed density in the locations that were subject to more persistent drought conditions (e.g., Texas) including Cyperus rotundus and Gratiola virginiana , indicating that these species may be better adapted to sites with high temperature and low precipitation. In contrast, certain species including Saururus cernuus and Ludwigia palustris were present throughout the range of these gradients, and so may be more resilient to any future climate shifts. We found that the regeneration potential of baldcypress swamps might be altered by changes in local and climate environment because of nuances of responses of seed banks to climates along latitudinal and longitudinal gradients. Our study can help predict vegetation regeneration potential to climate change environments depending on the ability of these species to disperse and maintain seed banks.

Science of the Total Environment↗

Transport and speciation of uranium in groundwater-surface water systems impacted by legacy milling operations

Growing worldwide concern over uranium contamination of groundwater resources has placed an emphasis on understanding uranium transport dynamics and potential toxicity in groundwater-surface water systems. In this study, we utilized novel in-situ sampling methods to establish the location and magnitude of contaminated groundwater entry into a receiving surface water environment, and to investigate the speciation and potential bioavailability of uranium in groundwater and surface water. Streambed temperature mapping successfully identified the location of groundwater entry to the Little Wind River, downgradient from the former Riverton uranium mill site, Wyoming, USA. Diffusive equilibrium in thin-film (DET) samplers further constrained the groundwater plume and established sediment pore water solute concentrations and patterns. In this system, evidence is presented for attenuation of uranium-rich groundwater in the shallow sediments where surface water and groundwater interaction occurs. Surface water grab and DET sampling successfully detected an increase in river uranium concentrations where the groundwater plume enters the Little Wind River; however, concentrations remained below environmental guideline levels. Uranium speciation was investigated using diffusive gradients in thin-film (DGT) samplers and geochemical speciation modelling. Together, these investigations indicate uranium may have limited bioavailability to organisms in the Little Wind River and, possibly, in other similar sites in the western U.S.A. This could be due to ion competition effects or the presence of non- or partially labile uranium complexes. Development of methods to establish the location of contaminated (uranium) groundwater entry to surface water environments, and the potential effects on ecosystems, is crucial to develop both site-specific and general conceptual models of uranium behavior and potential toxicity in affected ground and surface water environments.

Wyoming↗

Spatiotemporal variation in occurrence and co-occurrence of pesticides, hormones, and other organic contaminants in rivers in the Chesapeake Bay Watershed, United States

Investigating the spatiotemporal dynamics of contaminants in surface water is crucial to better understand how introduced chemicals are interacting with and potentially influencing aquatic organisms and environments. Within the Chesapeake Bay Watershed, USA, there are concerns about the potential role of contaminant exposure on fish health. Evidence suggests that exposure to contaminants in surface water is causing immunosuppression and intersex in freshwater fish species. Despite these concerns, there is a paucity of information regarding the complex dynamics of contaminant occurrence and co-occurrence in surface water across both space and time. To address these concerns, we applied a Bayesian hierarchical joint-contaminant model to describe the occurrence and co-occurrence patterns of 28 contaminants and total estrogenicity across six river sites and over three years. We found that seasonal occurrence patterns varied by contaminant, with the highest occurrence probabilities during the spring and summer months. Additionally, we found that the proportion of agricultural landcover in the immediate catchment, as well as stream discharge, did not have a significant effect on the occurrence probabilities of most compounds. Four pesticides (atrazine, metolachlor, fipronil and simazine) co-occurred across sites after accounting for environmental covariates. These results provide baseline information on the contaminant occurrence patterns of several classes of compounds within the Chesapeake Bay Watershed. Understanding the spatiotemporal dynamics of contaminants in surface water is the first step in investigating the effects of contaminant exposure on fisheries and aquatic environments.

Delaware, Maryland, New York, Pennsylvania, Virgin↗

Density currents in the Chicago River: Characterization, effects on water quality, and potential sources

Bidirectional flows in a river system can occur under stratified flow conditions and in addition to creating significant errors in discharge estimates, the upstream propagating currents are capable of transporting contaminants and affecting water quality. Detailed field observations of bidirectional flows were made in the Chicago River in Chicago, Illinois in the winter of 2005-06. Using multiple acoustic Doppler current profilers simultaneously with a water-quality profiler, the formation of upstream propagating density currents within the Chicago River both as an underflow and an overflow was observed on three occasions. Density differences driving the flow primarily arise from salinity differences between intersecting branches of the Chicago River, whereas water temperature is secondary in the creation of these currents. Deicing salts appear to be the primary source of salinity in the North Branch of the Chicago River, entering the waterway through direct runoff and effluent from a wastewater-treatment plant in a large metropolitan area primarily served by combined sewers. Water-quality assessments of the Chicago River may underestimate (or overestimate) the impairment of the river because standard water-quality monitoring practices do not account for density-driven underflows (or overflows). Chloride concentrations near the riverbed can significantly exceed concentrations at the river surface during underflows indicating that full-depth parameter profiles are necessary for accurate water-quality assessments in urban environments where application of deicing salt is common.

Science of the Total Environment↗

Pesticides in US Rivers: Regional differences in use, occurrence, and environmental toxicity, 2013 to 2017

Pesticides pose a threat to the environment, but because of the substantial number of compounds, a comprehensive assessment of pesticides and an evaluation of the risk that they pose to human and aquatic life is challenging. In this study, improved analytical methods were used to quantify 221 pesticide concentrations in surface waters over the time period from 2013 to 2017. Samples were collected from 74 river sites in the conterminous US (CONUS). Potential toxicity was assessed by comparing surface water pesticide concentrations to standard concentrations that are considered to have adverse effects on human health or aquatic organisms. The majority of pesticide use is related to agriculture, and agricultural production varies across the CONUS. Therefore, our results were summarized by region (Northeast, South, Midwest, West and Pacific), with the expectation that crop production differences would drive variability in pesticide use, detection frequency, and benchmark exceedance patterns. Although agricultural pesticide use was at least 2.5 times higher in the Midwest (49 kg km −2 ) than in any of the other four regions (Northeast, South, West, and Pacific, 3 to 21 kg km −2 ) and the average number of pesticides detected in the Midwest was at least 1.5 higher ( n = 25) than the other four regions ( n = 8 to n = 16), the potential toxicity results were more evenly distributed. At least 50% of the sites within each of the 5 regions had at least 1 chronic benchmark exceedance. Imidacloprid posed the greatest potential threat to aquatic life with a total of 245 benchmark exceedances at 60 of the 74 sites. These results show that pesticides persist in the environment beyond the site of application and expected period of use. Continued monitoring and research are needed to improve our understanding of pesticide effects on aquatic and human life.

Science of the Total Environment↗

Methylmercury degradation and exposure pathways in streams and wetlands impacted by historical mining

Monomethyl mercury (MMHg) and total mercury (THg) concentrations and Hg stable isotope ratios (&delta; 202 Hg and &Delta; 199 Hg) were measured in sediment and aquatic organisms from Cache Creek (California Coast Range) and Yolo Bypass (Sacramento Valley). Cache Creek sediment had a large range in THg (87 to 3870 ng/g) and &delta; 202 Hg (&minus;1.69 to &minus;0.20&permil;) reflecting the heterogeneity of Hg mining sources in sediment. The &delta; 202 Hg of Yolo Bypass wetland sediment suggests a mixture of high and low THg sediment sources. Relationships between %MMHg (the percent ratio of MMHg to THg) and Hg isotope values (&delta; 202 Hg and &Delta; 199 Hg) in fish and macroinvertebrates were used to identify and estimate the isotopic composition of MMHg. Deviation from linear relationships was found between %MMHg and Hg isotope values, which is indicative of the bioaccumulation of isotopically distinct pools of MMHg. The isotopic composition of pre-photodegraded MMHg (i.e., subtracting fractionation from photochemical reactions) was estimated and contrasting relationships were observed between the estimated &delta; 202 Hg of pre-photodegraded MMHg and sediment IHg. Cache Creek had mass dependent fractionation (MDF; &delta; 202 Hg) of at least &minus;0.4&permil; whereas Yolo Bypass had MDF of +0.2 to +0.5&permil;. This result supports the hypothesis that Hg isotope fractionation between IHg and MMHg observed in rivers (&minus;MDF) is unique compared to +MDF observed in non-flowing water environments such as wetlands, lakes, and the coastal ocean.

California↗

Patterns of metal composition and biological condition and their association in male common carp across an environmental contaminant gradient in Lake Mead National Recreation Area, Nevada and Arizona, USA

There is a contaminant gradient in Lake Mead National Recreation Area (LMNRA) that is partly driven by municipal and industrial runoff and wastewater inputs via Las Vegas Wash (LVW). Adult male common carp ( Cyprinus carpio ; 10 fish/site) were collected from LVW, Las Vegas Bay (receiving LVW flow), Overton Arm (OA, upstream reference), and Willow Beach (WB, downstream) in March 2008. Discriminant function analysis was used to describe differences in metal concentrations and biological condition of fish collected from the four study sites, and canonical correlation analysis was used to evaluate the association between metal and biological traits. Metal concentrations were determined in whole-body extracts. Of 63 metals screened, those initially used in the statistical analysis were Ag, As, Ba, Cd, Co, Fe, Hg, Pb, Se, Zn. Biological variables analyzed included total length (TL), Fulton's condition factor, gonadosomatic index (GSI), hematocrit (Hct), and plasma estradiol-17β and 11-ketotestosterone (11kt) concentrations. Analysis of metal composition and biological condition both yielded strong discrimination of fish by site (respective canonical model, p < 0.0001). Compared to OA, pairwise Mahalanobis distances between group means were WB < LVB < LVW for metal concentrations and LVB < WB < LVW for biological traits. Respective primary drivers for these separations were Ag, As, Ba, Hg, Pb, Se and Zn; and TL, GSI, 11kt, and Hct. Canonical correlation analysis using the latter variable sets showed they are significantly associated ( p < 0.0003); with As, Ba, Hg, and Zn, and TL, 11kt, and Hct being the primary contributors to the association. In conclusion, male carp collected along a contaminant gradient in LMNRA have distinct, collection site-dependent metal and morpho-physiological profiles that are significantly associated with each other. These associations suggest that fish health and reproductive condition (as measured by the biological variables evaluated in this study) are influenced by levels of certain metals in the Lake Mead environment.

Nevada↗

Pharmaceutical manufacturing facility discharges can substantially increase the pharmaceutical load to U.S. wastewaters

Discharges from pharmaceutical manufacturing facilities (PMFs) previously have been identified as important sources of pharmaceuticals to the environment. Yet few studies are available to establish the influence of PMFs on the pharmaceutical source contribution to wastewater treatment plants (WWTPs) and waterways at the national scale. Consequently, a national network of 13 WWTPs receiving PMF discharges, six WWTPs with no PMF input, and one WWTP that transitioned through a PMF closure were selected from across the United States to assess the influence of PMF inputs on pharmaceutical loading to WWTPs. Effluent samples were analyzed for 120 pharmaceuticals and pharmaceutical degradates. Of these, 33 pharmaceuticals had concentrations substantially higher in PMF-influenced effluent (maximum 555,000 ng/L) compared to effluent from control sites (maximum 175 ng/L). Concentrations in WWTP receiving PMF input are variable, as discharges from PMFs are episodic, indicating that production activities can vary substantially over relatively short (several months) periods and have the potential to rapidly transition to other pharmaceutical products. Results show that PMFs are an important, national-scale source of pharmaceuticals to the environment.

Science of the Total Environment↗

Density currents in the Chicago River: Characterization, effects on water quality, and potential sources

Bidirectional flows in a river system can occur under stratified flow conditions and in addition to creating significant errors in discharge estimates, the upstream propagating currents are capable of transporting contaminants and affecting water quality. Detailed field observations of bidirectional flows were made in the Chicago River in Chicago, Illinois in the winter of 2005-06. Using multiple acoustic Doppler current profilers simultaneously with a water-quality profiler, the formation of upstream propagating density currents within the Chicago River both as an underflow and an overflow was observed on three occasions. Density differences driving the flow primarily arise from salinity differences between intersecting branches of the Chicago River, whereas water temperature is secondary in the creation of these currents. Deicing salts appear to be the primary source of salinity in the North Branch of the Chicago River, entering the waterway through direct runoff and effluent from a wastewater-treatment plant in a large metropolitan area primarily served by combined sewers. Water-quality assessments of the Chicago River may underestimate (or overestimate) the impairment of the river because standard water-quality monitoring practices do not account for density-driven underflows (or overflows). Chloride concentrations near the riverbed can significantly exceed concentrations at the river surface during underflows indicating that full-depth parameter profiles are necessary for accurate water-quality assessments in urban environments where application of deicing salt is common.

Illinois↗

Toxicity and accumulation of silver nanoparticles during development of the marine polychaete Platynereis dumerilii

Pollutants affecting species at the population level generate ecological instability in natural systems. The success of early life stages, such as those of aquatic invertebrates, is highly affected by adverse environmental conditions. Silver released into the environment from emerging nanotechnology represents such a threat. Sediments are sinks for numerous pollutants, which aggregate and/or associate with depositing suspended particles. Deposit feeder such as the annelid Platynereis dumerilii, which has a large associated literature on its development, is an excellent model organism for exposure studies in coastal environments. We exposed eggs, larvae, juveniles and adults of P. dumerilii to various concentrations of citrate (cit-Ag NPs) or humic acid (HA-Ag NPs) capped silver nanoparticles (Ag NPs) as well to dissolved Ag (added as AgNO3). We showed that mortality and abnormal development rate increased with younger life stages. While adults and juvenile were the most tolerant life stages, fertilized eggs were highly sensitive to AgNO3, cit-Ag NPs and HA-Ag NPs. Exposures to HA-Ag NPs triggered the highest cute toxicity responses in P. dumerilii and in most cases both Ag NPs were more toxic than AgNO3. Uptake rate of HA-Ag NPs in adult worms was also higher than from other Ag forms, consistent with toxicity to other life stages. The early stages of the life cycle of marine coastal organisms are more affected by Ag NPs than the juvenile or adult life stages, indicating that exposure experiments at the larval level contribute to realistic eco-toxicological studies in aquatic environments.

Science of the Total Environment↗

Levels of mercury in alligators (Alligator mississippiensis) collected along a transect through the Florida Everglades

As part of a multi-agency study of alligator health, 28 American alligators (Alligator mississippiensis) were captured along a transect through the Florida Everglades in 1999. Liver and tail muscle tissues were sampled and analyzed on a wet weight basis for total mercury (THg) using cold-vapor atomic absorption spectrophotometry. All tissues had detectable concentrations of THg that ranged from 0.6 to 17 mg/kg in liver and from 0.1 to 1.8 mg/kg in tail muscle. THg was more concentrated in liver tissue than tail muscle, but levels were highly correlated between tissues. THg concentrations in tissue differed significantly among locations, with animals from Everglades National Park (ENP) having mean concentrations of THg in liver (10.4 mg/kg) and tail muscle (1.2 mg/kg) that were two-fold higher than basin-wide averages (4.9 and 0.64 mg/kg, respectively). The reasons for higher contamination of ENP alligators were unclear and could not be explained by differences in sex, length, weight or animal age. While ??15N values were positively correlated with THg concentrations in tail muscle, spatial patterns in isotopic composition did not explain the elevated THg levels in ENP alligators. Therefore, it appears that ENP alligators were more highly exposed to mercury in their environment than individuals in other areas. Comparisons to a previous survey by Yanochko et al. [Arch Environ Contam Toxicol 32 (1997) 323] suggest that mercury levels have declined in some Everglades alligators since 1994. ?? 2002 Elsevier Science B.V. All rights reserved.

Science of the Total Environment↗

Mercury sources and budget for the Snake River above a hydroelectric reservoir complex

Understanding sources of mercury (Hg) and methylmercury (MeHg) to a water body is critical for management but is often complicated by poorly characterized Hg inputs and in situ processes, such as inorganic Hg methylation. In this study, we determined inorganic Hg and MeHg concentrations and loads (filter-passing and particulate fractions) for a semi-arid 164-kilometer stretch of the Snake River above the Hells Canyon Complex, a Hg-impaired hydroelectric reservoir complex on the Idaho-Oregon border, and used water quality measurements and Hg stable isotope ratios to create a comprehensive Hg source budget for the river. Results show that whereas most of the streamflow to the study reach comes from the main branch of the Snake River (i.e., the upstream watershed), major tributaries within the study reach contribute a greater proportion of inorganic Hg and MeHg loads. Mercury stable-isotope analyses highlight that Hg within the tributaries is predominantly associated with geologic deposits and snowmelt sources, the latter reflecting wet deposition. Surprisingly, irrigation return drains contribute 40–50 % of particulate inorganic Hg loads despite being ≤4.3 % of the overall water budget. Together, tributaries and irrigation return drains account for 97–100 % of the inorganic Hg and streamflow to the study reach, but ~65 % of the MeHg, indicating in-stream and riparian methylation may be an important and previously unrecognized source of MeHg. Streamflow, total suspended solids, dissolved organic carbon, and agricultural land cover were found to be important controls on the mobilization and transport of different Hg species and fractions. This study represents the first fluvial budget for Hg in the Snake River that accounts for particulate and filter-passing Hg species from both major tributaries and irrigation return drains, and expands our understanding of Hg sources and methylation processes within semi-arid environments. This information is critical to inform management decisions related to elevated Hg burdens in biota.

Idaho, Nevada, Oregon↗