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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 (μg/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 μg/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.

Western North America is a region defined by extreme gradients in geomorphology and climate, which support a diverse array of ecological communities and natural resources. The region also has extreme gradients in mercury (Hg) contamination due to a broad distribution of inorganic Hg sources. These diverse Hg sources and a varied landscape create a unique and complex mosaic of ecological risk from Hg impairment associated with differential methylmercury (MeHg) production and bioaccumulation. Understanding the landscape-scale variation in the magnitude and relative importance of processes associated with Hg transport, methylation, and MeHg bioaccumulation requires a multidisciplinary synthesis that transcends small-scale variability. The Western North America Mercury Synthesis compiled, analyzed, and interpreted spatial and temporal patterns and drivers of Hg and MeHg in air, soil, vegetation, sediments, fish, and wildlife across western North America. This collaboration evaluated the potential risk from Hg to fish, and wildlife health, human exposure, and examined resource management activities that influenced the risk of Hg contamination. This paper integrates the key information presented across the individual papers that comprise the synthesis. The compiled information indicates that Hg contamination is widespread, but heterogeneous, across western North America. The storage and transport of inorganic Hg across landscape gradients are largely regulated by climate and land-cover factors such as plant productivity and precipitation. Importantly, there was a striking lack of concordance between pools and sources of inorganic Hg, and MeHg in aquatic food webs. Additionally, water management had a widespread influence on MeHg bioaccumulation in aquatic ecosystems, whereas mining impacts where relatively localized. These results highlight the decoupling of inorganic Hg sources with MeHg production and bioaccumulation. Together the findings indicate that developing efforts to control MeHg production in the West may be particularly beneficial for reducing food web exposure instead of efforts to simply control inorganic Hg sources.

Most investigations of the environmental effects of mercury (Hg) have focused on aquatic food webs that include piscivorous fish or wildlife. However, recent investigations have shown that other species, including passerine songbirds, may also be at risk from exposure to methylmercury (MeHg). We quantified Hg concentrations in eggs of two species of songbirds, red-winged blackbirds (Agelaius phoeniceus) and tree swallows (Tachycineta bicolor), nesting in Voyageurs National Park, Minnesota, USA. Geometric mean concentrations of total Hg (THg) were lower in red-winged blackbird eggs [218 and 107 ng/g dry weight (dw) for 2012 and 2013, respectively] than in tree swallow eggs (228 and 300 ng/g dw for 2012 and 2013, respectively), presumably reflecting differences in the trophic positions of these two species. Concentrations of MeHg averaged 98.4 % of THg in red-winged blackbird eggs. Levels of THg observed in this study were well below critical toxicological benchmarks commonly applied to eggs of avian species, suggesting these breeding populations were not adversely affected by exposure to MeHg. In red-winged blackbirds, concentrations of THg in eggs collected in 2012 were twice those in eggs collected in 2013. Hg levels in eggs of both species increased with date of clutch initiation. In red-winged blackbirds, for example, temporal patterns showed that a 3-week delay in clutch initiation increased egg THg by 60 %. These observations indicate that in ovo exposure of wetland birds to MeHg can vary significantly within nesting season as well as between years.

We present a case study comparing metrics of methylmercury (MeHg) contamination for four undeveloped lakes in Voyageurs National Park to wet atmospheric deposition of mercury (Hg), sulfate (SO4(-2)), and hydrogen ion (H+) in northern Minnesota. Annual wet Hg, SO4(-2), and H+ deposition rates at two nearby precipitation monitoring sites indicate considerable decreases from 1998 to 2012 (mean decreases of 32, 48, and 66%, respectively). Consistent with decreases in the atmospheric pollutants, epilimnetic aqueous methylmercury (MeHgaq) and mercury in small yellow perch (Hgfish) decreased in two of four lakes (mean decreases of 46.5% and 34.5%, respectively, between 2001 and 2012). Counter to decreases in the atmospheric pollutants, MeHgaq increased by 85% in a third lake, whereas Hgfish increased by 80%. The fourth lake had two disturbances in its watershed during the study period (forest fire; changes in shoreline inundation due to beaver activity); this lake lacked overall trends in MeHgaq and Hgfish. The diverging responses among the study lakes exemplify the complexity of ecosystem responses to decreased loads of atmospheric pollutants.

The Laurentian Great Lakes region of North America contains substantial aquatic resources and mercury-contaminated landscapes, fish, and wildlife. This special issue emanated from a bi-national synthesis of data from monitoring programs and case studies of mercury in the region, here defined as including the Great Lakes, the eight U.S. states bordering the Great Lakes, the province of Ontario, and Lake Champlain. We provide a retrospective overview of the regional mercury problem and summarize new findings from the synthesis papers and case studies that follow. Papers in this issue examine the chronology of mercury accumulation in lakes, the importance of wet and dry atmospheric deposition and evasion to regional mercury budgets, the influence of land–water linkages on mercury contamination of surface waters, the bioaccumulation of methylmercury in aquatic foods webs; and ecological and health risks associated with methylmercury in a regionally important prey fish.

We assessed the risks of mercury in yellow perch, a species important in the trophic transfer of methylmercury, in the Great Lakes region. Mean concentrations in whole perch from 45 (6.5%) of 691 waters equaled or exceeded 0.20 μg/g w.w., a threshold for adverse effects in fish. In whole perch within the size range eaten by common loons (

This special issue examines bioaccumulation and risks of methylmercury in food webs, fish and wildlife in the Laurentian Great Lakes region of North America, and explores mercury policy in the region and elsewhere in the United States and Canada. A total of 35 papers emanated from a bi-national synthesis of multi-media data from monitoring programs and research investigations on mercury in aquatic and terrestrial biota, a 3-year effort involving more than 170 scientists and decision-makers from 55 different universities, non-governmental organizations, and governmental agencies. Over 290,000 fish mercury data points were compiled from monitoring programs and research investigations. The findings from this scientific synthesis indicate that (1) mercury remains a pollutant of major concern in the Great Lakes region, (2) that the scope and intensity of the problem is greater than previously recognized and (3) that after decades of declining mercury levels in fish and wildlife concentrations are now increasing in some species and areas. While the reasons behind these shifting trends require further study, they also underscore the need to identify information gaps and expand monitoring efforts to better track progress. This will be particularly important as new pollution prevention measures are implemented, as global sources increase, and as the region faces changing environmental conditions.

A partnership of federal and state agencies, tribes, industry, and scientists from academic research and environmental organizations is establishing a national, policy-relevant mercury monitoring network, called MercNet, to address key questions concerning changes in anthropogenic mercury emissions and deposition, associated linkages to ecosystem effects, and recovery from mercury contamination. This network would quantify mercury in the atmosphere, land, water, and biota in terrestrial, freshwater, and coastal ecosystems to provide a national scientific capability for evaluating the benefits and effectiveness of emission controls. Program development began with two workshops, convened to establish network goals, to select key indicators for monitoring, to propose a geographic network of monitoring sites, and to design a monitoring plan. MercNet relies strongly on multi-institutional partnerships to secure the capabilities and comprehensive data that are needed to develop, calibrate, and refine predictive mercury models and to guide effective management. Ongoing collaborative efforts include the: (1) development of regional multi-media databases on mercury in the Laurentian Great Lakes, northeastern United States, and eastern Canada; (2) syntheses and reporting of these data for the scientific and policy communities; and (3) evaluation of potential monitoring sites. The MercNet approach could be applied to the development of other monitoring programs, such as emerging efforts to monitor and assess global mercury emission controls.

We synthesized information on selected contaminants in the Upper Mississippi River, summarized regulatory measures enacted to reduce pollution, and described biotic and ecosystem responses to regulatory actions. Contamination of the river with mercury and lead rapidly followed settlement of the basin by European immigrants in the mid-1800s. Metal contamination peaked in the 1960s and has since decreased substantially. DDT, its degradation product DDE, and PCBs biomagnified to concentrations that adversely affected wildlife in upper trophic levels. National (U.S.A.) environmental regulations enacted from 1972 to 1991 reduced discharges of wastes from point sources, improved wastewater treatment, and reduced or banned the production or usage of certain chemicals, such as DDT, PCBs, and lead. Responses to these regulatory measures include reductions in ecosystem contamination, reductions in biotic exposure, and recovery of affected wildlife populations. Recovery from pollution has been slow, however, and we conclude that proactive approaches focusing on prevention are highly preferable to reactive approaches in management of toxic substances. Past successes in reducing point-source pollution, which is greatest near urban areas, do not extend to nonpoint-source pollution, given that the existing regulatory framework does not adequately address nonpoint sources. The river continues to receive hundreds of recently synthesized chemicals, and the behavior and effects of most of these compounds in aquatic ecosystems are largely unknown. Emerging contaminants and recently discovered mechanisms of adverse biological effects, such as endocrine disruption, pose continuing challenges to scientists and environmental managers concerned with the ecological health of this riverine ecosystem.

The Coast Range of California is one of five global regions that dominated historical production of mercury (Hg) until declining demand led to the economic collapse of the Hg-mining industry in the United States. Calcines, waste rock, and contaminated alluvium from inactive mine sites can release Hg (including methylmercury, MeHg) to the environment for decades to centuries after mining has ceased. Soils, water, and sediment near mines often contain high concentrations of total Hg (TotHg), and an understanding of the biogeochemical transformations, transport, and bioaccumulation of this toxic metal is needed to assess effects of these contaminated environments on humans and wildlife. We briefly review the environmental behavior and effects of Hg, providing a prelude to the subsequent papers in this Special Issue. Clear Lake is a northern California lake contaminated by wastes from the abandoned Sulphur Bank Mercury Mine, a U.S. Environmental Protection Agency Superfund Site. The primary toxicological problem with Hg in aquatic ecosystems is biotic exposure to MeHg, a highly toxic compound that readily bioaccumulates. Processes that affect the abundance of MeHg (including methylation and demethylation) strongly affect its concentration in all trophic levels of aquatic food webs. MeHg can biomagnify to high concentrations in aquatic food webs, and consumption of fish is the primary pathway for human exposure. Fish consumption advisories have been issued for many North American waters, including Clear Lake and other mine-impacted waters in California, as a means of decreasing MeHg exposure. Concerns about MeHg exposure in humans focus largely on developmental neurotoxicity to the fetus and children. Aquatic food webs are also an important pathway for MeHg exposure of wildlife, which can accumulate high, sometimes harmful, concentrations. In birds, wild mammals, and humans, MeHg readily passes to the developing egg, embryo, or fetus, life stages that are much more sensitive than the adult. The papers in this issue examine the origin, transport, transformations, bioaccumulation, and trophic transfer of Hg in Clear Lake, assess its potential effects on biota and humans, and provide information relevant to remediation of mine-impacted aquatic ecosystems.

Monitoring of mercury in fish typically involves removal of individuals from the sampled population and subsequent analysis of fillets. This study assessed whether the analysis of fins, structures routinely clipped to mark released fish in population studies, could provide a nonlethal approach for estimating mercury concentrations in axial muscle (fillets). We analyzed fillets and selected fins from 401 northern pike (Esox lucius) and 79 walleye (Sander vitreus) from 21 lakes in Minnesota and Wisconsin, 19 Arctic grayling (Thymallus arcticus) from Toolik Lake, Alaska, and 14 winter flounder (Pseudopleuronectes americanus) from Long Island Sound, New York. On average, 83% of mercury in fins was methylmercury, and concentrations in the proximal portion were about half-those in the distal portion in pelvic fins. Mean concentrations of mercury in fins, averaged by species and fin type, ranged from 2.7 to 8.9% of those in fillets. Coefficients of determination (r2) for linear regressions of mercury concentrati...

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.

Mercury (Hg) in water, sediment, soils, seston, and biota were quantified for three streams in the Grand Portage National Monument (GRPO) in far northeastern Minnesota to assess ecosystem contamination and the potential for harmful exposure of piscivorous fish, wildlife, and humans to methylmercury (MeHg). Concentrations of total Hg in water, sediment, and soil were typical of those in forest ecosystems within the region, whereas MeHg concentrations and percent MeHg in these ecosystem components were markedly higher than values reported elsewhere in the western Great Lakes Region. Soils and sediment were Hg-enriched, containing approximately 4-fold more total Hg per unit of organic matter. We hypothesized that localized Hg enrichment was due in part to anthropogenic pollution associated with historic fur-trading activity. Bottom-up forcing of bioaccumulation was evidenced by MeHg concentrations in larval dragonflies, which were near the maxima for dragonflies sampled concurrently from five other national park units in the region. Despite its semi-remote location, GRPO is a Hg-sensitive landscape in which MeHg is produced and bioaccumulated in aquatic food webs to concentrations that pose ecological risks to MeHg-sensitive piscivores, including predatory fish, belted kingfisher, and mink.

Cadmium was quantified in the surface sediments of six seepage lakes ranging from 8 to 70 ha in surface area, 6 to 20 m in maximum depth, 5.2 to 7.0 in mean epilimnetic pH, and 1.7 to 6.8 mg·L−1 in dissolved organic carbon. Within each lake, dry-weight concentrations of cadmium (range, 0.02–7.17 μg·g−1) were positively correlated with volatile matter content of the sediments, which increased with water depth. Volumetric concentrations (i.e., mass per volume of wet sediment) were correlated with water depth in only one lake, and they more accurately represented the spatial distribution of sedimentary cadmium within the lakes. Analysis of sediment cores from two of the lakes indicated that surface sediments were enriched with cadmium. The source of cadmium and the within-lake processes controlling deposition to the sediments were presumably similar among the lakes, as demonstrated by the strong correlation between lake area and whole-lake burdens of cadmium in the surface sediments (range, 625–5785 g/lake). Hence, cadmium in these lakes appears to be derived largely from atmospheric deposition. When normalized for lake area, cadmium burdens in the surface sediments ranged from 62 to 92 g·ha−1 and were strongly correlated with dissolved organic carbon, but not with lake pH, which suggests a link between the transport of cadmium and organic matter to the sediments.

We examined the bioavailability of mercury in sediments from the contaminated Sudbury River (Massachusetts, U.S.A.). Mayfly nymphs (Hexagenia) were exposed in four 21-day bioaccumulation tests to contaminated and reference sediments (treatments) from reservoirs, flowing reaches, palustrine wetlands, and a riverine lake. Mean total mercury (ΣHg) ranged from 880 to 22 059 ng·g dry weight-1in contaminated sediments and from 90 to 272 ng·g-1in reference sediments. Mean final concentrations of methyl mercury (MeHg) in test water were greatest (8-47 ng Hg·L-1) in treatments with contaminated wetland sediments, which had mean ΣHg ranging from 1200 to 2562 ng·g-1. In mayflies, final mean concentrations of MeHg were highest in treatments with contaminated wetland sediments (122-183 ng Hg·g-1), intermediate in treatments with contaminated sediments from reservoirs, flowing reaches, and a riverine lake (75-127 ng Hg·g-1), and lowest in treatments with reference sediments (32-41 ng Hg·g-1). We conclude that the potential entry of MeHg into the benthic food chain was greater in contaminated palustrine wetlands than in the contaminated reservoirs, which had the most contaminated sediments.

The distribution and deposition of sedimentary mercury in the Sudbury River were linked to an industrial complex (Nyanza site) that operated from 1917 through 1978. In two reservoirs just downstream from the Nyanza site, estimated rates of mercury accumulation increased markedly in the 1920s and 1930s, were greatest during 1976-1982, decreased within 5 years after industrial operations ceased, and have decreased further since capping of contaminated soil at the Nyanza site was completed in 1991. The most contaminated sediments were typically buried, yet the 0- to 1-cm stratum remained substantially contaminated in all cores. Mercury accumulating in the surficial, reservoir sediments was probably from continuing, albeit much lesser, inputs from the Nyanza site, whereas recent inputs to downstream wetland areas were attributed to recycling of sedimentary mercury or to mercury from unidentified local sources. In the reservoirs, burial of highly contaminated sediments is gradually decreasing the amount of sedimentary mercury available for methylation. In downstream wetlands, however, sedimentary mercury seemed to be more available than that in the reservoirs for physical transport and biogeochemical cycling.

A single stress, acidification with sulfuric acid, was applied to Little Rock Lake in a whole-ecosystem manipulation. We documented a wide range of responses to the acidification, including increases in the concentrations of various chemicals, shifts in microbial processes and a major increase in water clarity to UV-B radiation. Each of these changes could in itself be considered as a separate ecosystem stress that is distinct from the intended manipulation. Acidification in Little Rock Lake was accompanied by a number of substantial changes in the occurrence of organisms. A series of detailed investigations indicates that the mechanisms underlying these organismal changes are varied but cannot usually be tied to the direct effects of acidification. Overall, our results demonstrate how multiple stresses can arise from a single agent operating on an ecosystem and suggest that singly operating stresses may actually be quite rare.

We examined the influence of maternal mercury and selected lacustrine variables on the mercury content of eggs from yellow perch (Perca flavescens). Total mercury, methylmercury, and inorganic mercury were determined in eggs and carcasses (less eggs) from three seepage lakes with a pH range of 6.1−7.0 and a fourth lake in which pH was experimentally increased from 5.5 to 6.8 by addition of alkaline groundwater. The concentration of total mercury in eggs was strongly correlated with that in the maternal carcass. Concentrations and burdens of mercury in eggs and carcasses were inversely correlated with lake water pH, acid-neutralizing capacity, calcium, and dissolved organic carbon. In eggs containing more than 30 ng/g dry weight (4.5 ng/g wet weight) of total mercury, methylmercury averaged 91% of total mercury and ranged from 85% to 96%. Mean burdens of total mercury in individual eggs varied greatly among lakes (range, 2.3−63 pg), and the egg mass averaged 1.9% of the whole-body burden. We conclude that ...

Burrowing mayfly nymphs (Ephemeroptera) inhabit and ingest fine-grained sediments and detritus that may be enriched with metals and persistent organic compounds. The burrowing nymphs can externally adsorb and internally assimilate these contaminants, providing a link for the food chain transfer of potentially toxic substances from sediments to organisms in higher trophic levels. The emergent adults are short-lived and do not feed, thus their gut contents do not contribute greatly to their total contaminant burden. These characteristics make Hexagenia spp. and certain other burrowing mayflies useful for assessing ecosystem contamination. General protocols are presented for the collection, processing and analysis of emergent mayflies to assess the spatial distribution and bioaccumulation of sediment-associated contaminants in aquatic ecosystems. Two essential components of this bioassessment approach are a network of on-site volunteers with the materials and instructions needed to correctly collect and store samples and quality assurance procedures to estimate the accuracy of chemical analyses. The utility of this approach is demonstrated with an example of its application to the Upper Mississippi River (USA). Determination of cadmium, mercury and polychlorinated biphenyl congeners in emergent Hexagenia bilineata from a 1250km reach of this river revealed (1) several source areas of contaminants and (2) distinct patterns in the bioaccumulation (and apparent sediment-associated transport) of each residue on both small and large spatial scales.

We examined recent temporal trends in the abundance of fingernail clams Musculium transversum (formerly Sphaerium transversum) in the upper Mississippi River. Historical data on densities of fingernail clams were obtained from regional scientists and published literature. We also sampled benthos in six navigation pools in summer 1991, finding very few fingernail clams. The combined data set, including historical data and sampling results, extended from 1973 to 1992 and was sufficient to statistically evaluate trends in densities of fingernail clams in eight pools. Populations of fingernail clams declined significantly in five of the eight pools examined (Pools 2, 5, 7, 9, and 19), which spanned a 700-km reach of river from St. Paul, Minnesota, to Keokuk, Iowa. Densities in Pool 19, which had the longest historical record on fingernail clam abundance, averaged 30000 m -2 in 1985 and progressively declined to zero in 1990. Combined data from all eight pools showed a significant decline in abundance of fingernail clams. An evaluation of potential causal factors led us to hypothesize that the population declines in Pools 2 to 9 were linked to point-source pollution rather than to dredging activity or commercial navigation traffic. In Pool 19, the declines of fingernail clams may have resulted from low-flow conditions during drought periods, but the causal mechanisms by which low flow influences fingernail clam abundance are unclear. The decrease in fingernail clam populations may adversely affect certain fish and wildlife, such as migrating lesser scaup Aythya affinis, which feed heavily on the small mollusk. Moreover, the decreases in populations of this pollution-sensitive mollusk may signal a large-scale deterioration in the health of this riverine ecosystem.

We exposed juvenile bluegill (Lepomis macrochirus) to ~1000 mg∙L−1 of continuously suspended river sediment in a 28-d test with six treatments (randomized block with one sediment-free control and five sediments ranging from 1.3 to 21.4 μg Cd∙g dry weight−1). Each treatment had three replicates, each with 25 fish. Growth was reduced by exposure to suspended sediment, probably due to physical effects of sediment on feeding and to toxicity in the treatment with the greatest concentrations of metals. Mean whole-body concentrations of cadmium (0.04–0.14 μg∙g wet weight−1) were correlated with cadmium concentration in filtered water (8–72 ng∙L−1), suspended sediment (0.61–16.8 μg∙L−1), and bulk sediment. The concentration of hepatic nonthionein cytosolic cadmium (cadmium not bound by metal-binding proteins, MBP) in fish exposed to the two most contaminated sediments exceeded that in controls. The mean concentration of hepatic MBP was correlated with cadmium concentration in filtered water, suspended sediment, bulk sediment, and whole fish. Whole-body cadmium concentration was the most sensitive indicator of cadmium exposure, with lowest observed effect concentrations of 1.9 μg Cd∙L−1 for suspended sediment and 13 ng Cd∙L−1 for filtered water. Sediment-associated cadmium was less available than waterborne cadmium for uptake by fish.

We examined sublethal responses of juvenile bluegills Lepomis macrochirus to aqueous cadmium in two 28-d tests (test I, 0.0-8.4 μg Cd per liter; test II, 0.0-32.3 μg Cd per liter) in an intermittent-flow diluter. The experimental design was completely randomized, with two replicates in each of eight treatments (seven Cd exposures and one water control with 25 fish per replicate). Cadmium did not affect the growth of test fish. The mean whole-body concentrations of Cd in exposed fish were 1.8- to 44-fold those in controls in the two tests. Mean concentrations of hepatic nonthionein cytosolic Cd (not bound by metal-binding proteins, MBP) in all Cd treatments greatly exceeded those in controls, and mean concentrations of hepatic MBP in all treatments except one (0.8 μg Cd per liter in test I) exceeded those in controls. Nonthionein cytosolic Cd, hepatic MBP, and whole-body Cd in bluegills were linearly related to exposure concentrations within the range 0 to 20 μg Cd per liter. Much of the total Cd-binding capacity of hepatic MBP per fish was occupied by Cd after the 28-d exposures, although additional Cd-binding capacity remained unoccupied by Cd in fish in all treatments. The mean total Cd-binding capacity of hepatic MBP per fish, which ranged from 1.7 to 14 nmol Cd in test I and from 0.8 to 24 nmol Cd in test II, increased in a concentration-response manner at exposure concentrations below 13 μg/L. Nonthionein cytosolic Cd was the most sensitive indicator of Cd exposure, based on an LOEC of 0.8 μg Cd per liter.

We determined polychlorinated biphenyls (PCBs) in emergent mayflies (Hexagenia bilineata) from a 1250-km reach of the upper Mississippi River (UMR). Total PCB concentrations (sum of 125 congeners) ranged from 0.21 to 4.1 μg/g of dry weight (1.2-29 μg/g of lipid weight). Concentrations were highest in pools near the Twin Cities and the Quad Cities metropolitan areas. Longitudinal movement of PCBs was extensive downstream from the Twin Cities (175-320 K) but was not apparent downstream from the Quad Cities. The PCB composition of mayflies was relatively homogeneous throughout most of the river. However, the congener composition in mayflies from two distant locations differed markedly from the other samples and contained a greater abundance of lower molecular weight congeners

Threshold concentrations associated with adverse effects of dietary exposure to methylmercury (MeHg) were derived from published results of laboratory studies on a variety of fish species. Adverse effects related to mortality were uncommon, whereas adverse effects related to growth occurred only at dietary MeHg concentrations exceeding 2.5 m gg � 1 wet weight. Adverse effects on behavior of fish had a wide range of effective dietary concentrations, but generally occurred above 0.5 m gg � 1 wet weight. In contrast, effects on reproduction and other subclinical endpoints occurred at dietary concentrations that were much lower (

Sublethal and reproductive effects of methylmercury in freshwater fish have been observed at environmentally relevant exposure levels in a number of recent field and laboratory studies. The consequences of methylmercury exposure may be more severe for wild fish than for fish in laboratory tests in which fish are provided ample food. WA Paul Drevnick et al. proposed that methylmercury induces apoptosis in steroidogenic cells in the gonads of fish. They observed an increase in the number of apoptotic follicular cells in the gonads of female fathead minnows that had impaired reproduction due to chronic methylmercury exposure. Laboratory and field studies have shown that methylmercury exposure causes oxidative stress in fish tissues through the formation of radical oxygen species and lipid peroxidation. Species differences in sensitivity to methylmercury exposure in fishes have not been assessed, but may be considerable given the variation in avian sensitivity reported by Germany Gary H. Heinz et al.

We quantified total mercury in surficial sediments (uppermost 5 cm) of six small seepage lakes. Fifty cores were taken from each lake, based on a random sampling design stratified by water depth. Volumetric concentrations (mass per volume of wet sediment) more accurately portrayed the depth distribution of mercury in the lakes than did dry-weight concentrations, which underrepresented the significance of the shallow-water sediments as a reservoir of potentially available mercury. Estimates of whole-lake burdens (masses) of mercury in the surficial sediment, which represent the maximum amount of sedimentary mercury available for methylation, ranged from 45 to 149 g. These sedimentary pools of mercury greatly exceeded the inventories of the metal in water, seston, and fish, and the release of mercury from the sediments could significantly increase its bioaccumulation. Areal burdens of mercury (mass per unit of lake area) varied fivefold among lakes (1.65–7.84 g/ha) and were strongly correlated with lake pH, but were not correlated with dissolved organic carbon, conductance, or chlorophyll a of lakes. We hypothesize that the observed variation in areal burdens of mercury was partly due to variation among lakes in the pH-related efflux of gaseous mercury (Hg0) from the lakes to the atmosphere.

Monitoring of mercury in fish typically involves removal of individuals from the sampled population and subsequent analysis of fillets. This study assessed whether the analysis of fins, structures routinely clipped to mark released fish in population studies, could provide a nonlethal approach for estimating mercury concentrations in axial muscle (fillets). We analyzed fillets and selected fins from 401 northern pike (Esox lucius) and 79 walleye (Sander vitreus) from 21 lakes in Minnesota and Wisconsin, 19 Arctic grayling (Thymallus arcticus) from Toolik Lake, Alaska, and 14 winter flounder (Pseudopleuronectes americanus) from Long Island Sound, New York. On average, 83% of mercury in fins was methylmercury, and concentrations in the proximal portion were about half-those in the distal portion in pelvic fins. Mean concentrations of mercury in fins, averaged by species and fin type, ranged from 2.7 to 8.9% of those in fillets. Coefficients of determination (r2) for linear regressions of mercury concentrations in fillets against those in fins of individual fish ranged from 0.04 to 0.96 among species and water bodies (median r2 = 0.52). The concentration in fin clips was a better predictor of mercury in fillets for individual Arctic grayling (r2 = 0.65, n = 12 and r2 = 0.84, n = 8) and winter flounder (r2 = 0.94, n = 14) than for individual northern pike (median r2 = 0.56) or walleye (median r2 = 0.22) from a given lake. In northern pike in the 400-500 mm total-length interval, the mean concentrations of total mercury in caudal fins and fillets, averaged by lake (n = 12), were strongly correlated (r2 = 0.95). The analysis of composited samples of fin clips from fish within a restricted length interval could, therefore, be a useful screening tool for assessing the relative mercury contamination of fish among different water bodies.

We studied relations between lacustrine characteristics and the total mercury (Hg) content of calendar age-2 yellow perch (Perca flavescens) in 10 seepage lakes in north-central Wisconsin. Mean concentrations and burdens (masses) of Hg in whole perch varied widely among lakes, were negatively correlated with lake pH and were positively correlated with total Hg concentration in surficial profundal sediment. Approximately 80 to 90% of the variation in Hg concentration and burden in whole perch was explained with multiple regressions containing two independent variables: either lake pH or alkalinity, and Hg concentration in surficial sediment. Variation among lakes in the Hg concentration in yellow perch was unrelated to their relative rates of growth. The mean concentration of Hg in axial muscle tissue of age-5 walleyes (Stizostedion vitreum vitreum) from five of the study lakes was highly correlated with the mean concentration in whole age-2 perch in the same lakes. We hypothesized that the high Hg concentrations often seen in piscivorous fish in low-alkalinity lakes (relative to high-alkalinity lakes) is at least partly due to a greater dietary intake of Hg in such waters. Furthermore, the analysis of small yellow perch—the preferred prey of adult walleyes and an important forage species for many predatory fishes in the north-central United States—may be an effective approach to assessing Hg bioavailability in the region's lakes.

We studied the partitioning of mercury (Hg) among air, water, sediments and fish at Little Rock Lake, a clear water seepage lake in north-central Wisconsin. The lake was divided with a sea curtain into two basins, one acidified with sulfuric acid to pH 5.6 for two years and the other an untreated reference site (mean pH 6.1), to document the effects of acidification. Trace-metal-free protocols were used to measure Hg at the picomolar level in air and water. Total gaseous Hg in air samples averaged 2.0 ng/m3. Total Hg in unfiltered water samples collected in 1986 after the fall overturn averaged about 1 ng/L in the acidified and reference basins. Mercury in surficial sediments was strongly correlated with volatile matter content and ranged from 10 to about 170 ng/g (dry weight) in both basins. Total Hg concentrations in whole, calendar age-1 yellow perch (Perca flavescens), sampled after one year of residence in the lake, averaged 114 ng/g (fresh weight) in the reference basin and 135 ng/g in the acidified basin – a highly significant (p < 0.01) difference. The mean whole-body burden (quantity) of Hg in age-1 perch did not differ between basins after the first year, but was significantly greater in the treatment basin than in the reference basin after the second year of acidification. Differences between the two basins in the bioaccumulation of Hg were attributed to internal (within-lake) processes that influence the bioavailability of the metal. An initial Hg budget for the treatment basin of Little Rock Lake showed that atmospheric deposition and sedimentary remobilization of Hg are potentially important processes influencing its biogeochemical cycling and uptake by fish.

Concentrations of methylmercury in game fish from many interior lakes in Voyageurs National Park (MN, U.S.A.) substantially exceed criteria for the protection of human health. We assessed the importance of atmospheric and geologic sources of mercuryto interior lakes and watersheds within the Park and identified ecosystem factors associated with variation in methylmercury contamination of lacustrine food webs. Geologic sources of mercury were small, based on analyses of underlying bedrock and C-horizon soils, and nearly all mercury in the 0- and A-horizon soils was derived from atmospheric deposition. Analyses of dated sediment cores from five lakes showed that most (63% +/- 13%) of the mercury accumulated in lake sediments during the 1900s was from anthropogenic sources. Contamination of food webs was assessed by analysis of whole, 1-year-old yellow perch (Perca flavescens), a regionally important prey fish. The concentrations of total mercury in yellow perch and of methylmercury in lake water varied substantially among lakes, reflecting the influence of ecosystem processes and variables that affect the microbial production and abundance of methylmercury. Models developed with the information-theoretic approach (Akaike Information Criteria) identified lake water pH, dissolved sulfate, and total organic carbon (an indicator of wetland influence) as factors influencing methylmercury concentrations in lake water and fish. We conclude that nearly all of the mercury in fish in this seemingly pristine

James G. Wiener, David P. Krabbenhoft, Gary H. Heinz, and Anton M. ScheuhammerCONTENTS16.1 Introduction 409 16.2 Evolution of the Environmental Mercury Problem 410 16.3 Global-Scale Environmental Cycling and Fate 413 16.4 Mercury Speciation and Environmental Concentrations 415

We examined effects of dietary methylmercury (MeHg) on reproduction of fathead minnows (Pimephales promelas). Juvenile fish were fed one of four diets until sexual maturity (phase 1): a control diet (0.06 microg Hg g(-1) dry weight) and three diets contaminated with MeHg at 0.88 (low), 4.11 (medium), and 8.46 microg Hg g(-1) dry weight (high). At sexual maturity, male and female fish were paired, again fed one of the four diets, and allowed to reproduce (phase 2). To assess effects of MeHg during gametogenesis, some fish were fed diets during phase 2 that differed from those during phase 1. Spawning success of pairs fed the same diet during phases 1 and 2 was 75% for controls and 46%, 50%, and 36% for the low-, medium-, and high-MeHg treatments, respectively. Spawning success of pairs fed a contaminated diet during phase 1 and a control diet during phase 2 was 63%, 40%, and 14% for the low-, medium-, and high-MeHg treatments, respectively, whereas exposure to dietary MeHg only during phase 2 did not reduce spawning success. Dietary MeHg delayed spawning, and days to spawning was positively correlated with concentration of total mercury in the carcasses of test fish. MeHg reduced the instantaneous rate of reproduction of fish fed the same diets during phases 1 and 2. Both the gonadosomatic index and reproductive effort of female fish were inversely correlated with mercury in carcasses, whereas developmental and hatching success of embryos, 7-d survival, and 7-d growth of larvae were unrelated to mercury concentrations in parental fish or their diets. MeHg decreased reproduction of adult fathead minnows at dietary concentrations encountered by predatory fishes in aquatic systems with MeHg-contaminated food webs, implying that exposed fish populations could be adversely affected by this widespread contaminant.

We assessed the utility of larval burrowing dragonflies (Odonata: Anisoptera: Gomphidae) as biosentinels of methylmercury (MeHg) contamination. Gomphids were the most abundant family of dragonflies sampled during 2008-2010 from 17 lakes in four national parks of the northwestern Laurentian Great Lakes region. Ten species of burrowing gomphids were sampled; 13 lakes contained 3 or more species, and 2 species of Gomphus co-occurred in 12 lakes. Most of the total Hg (THg) in whole, late-instar larvae was MeHg, with mean percent MeHg exceeding 60% in 16 lakes. Mean MeHg in larvae of a given species varied greatly among lakes, ranging from 4 to 109 ng g(-1) dry weight. Methylmercury levels in larvae, however, were much less variable within a given lake and species. The mean concentration of MeHg in burrowing gomphids was positively correlated with mean MeHg concentration in unfiltered lake water. Mean concentrations of THg and MeHg in multispecies assemblages of Gomphus were also positively correlated with mean THg in coexisting prey fish and game fishes. We recommend-and provide guidance on-the application of burrowing gomphids as biosentinels of MeHg contamination, which can extend the bioassessment of MeHg to fishless fresh waters.

We describe a new test system for exposing fish to resuspended sediments and associated contaminants. Test sediments were resuspended by revolving test chambers on rotating shafts driven by an electric motor. The timing, speed, and duration of test-chamber revolution were controlled by a rheostat and electronic timer. Each chamber held 45 litres of water and accommodated about 49 g of test fish. The system described had three water baths, each holding six test chambers. We illustrate the performance of this system with results from a 28-day test in which juvenile bluegills Lepomis macrochirus were exposed to resuspended, riverine sediments differing in texture and cadmium content. The test had one sediment-free control and five sediment treatments, with three replicates (chambers) per treatment and 25 fish per replicate. Two-thirds (30 litres) of the test water and sediment in each chamber was renewed weekly. The mean concentration of total suspended solids (TSS) did not vary among treatments; the grand-mean TSS in the five sediment treatments was 975 mg litre −1 , similar to the target TSS of 1000 mg litre −1 . At the end of the test, an average of 50% of the introduced cadmium was associated with the suspended sediment compartment, whereas the filtered (0.45 μm) water contained 0.4% and bluegills 1.8% of the cadmium.

Burrowing mayflies (Hexagenia bilineata) were analyzed to assess longitudinal patterns in their cadmium and mercury content along the upper Mississippi River. Emergent mayflies (subimagoes and imagoes) were collected in 1988 at 34 sites (25 navigation pools), extending 1260 km from Little Falls, Minnesota, downstream to St. Louis, Missouri. Cadmium concentrations in composite samples of whole mayflies ranged from 7 to 219 ng/g dry weight in females and from

Fish in low-alkalinity lakes having pH of 6.0-6.5 or less often have higher body or tissue burdens of mercury, cadmium, and lead than do fish in nearby lakes with higher pH. The greater bioaccumulation of these metals in such waters seems to result partly from the greater aqueous abundances of biologically available forms (CH(3) Hg(+), Cd(2+), and Pb(2+)) at low pH. In addition, the low concentrations of aqueous calcium in low-alkalinity lakes increase the permeability of biological membranes to these metals, which in fish may cause greater uptake from both water and food. Fish exposed to aqueous inorganic aluminum in the laboratory and field accumulate the metal in and on the epithelial cells of the gills; however, there is little accumulation of aluminum in the blood or internal organs. In low-pH water, both sublethal and lethal toxicity of aluminum has been clearly demonstrated in both laboratory and field studies at environmental concentrations. In contrast, recently measured aqueous concentrations of total mercury, methylmercury, cadmium, and lead in low-alkalinity lakes are much lower than the aqueous concentrations known to cause acute or chronic toxicity in fish, although the vast majority of toxicological research has involved waters with much higher ionic strength than that in low-alkalinity lakes. Additional work with fish is needed to better assess (1) the toxicity of aqueous metals in low-alkalinity waters, and (2) the toxicological significance of dietary methylmercury and cadmium.

Survivorship data can be effectively summarized using the shape and scale parameters of the Weibull frequency distribution. The shape parameter controls the rate of change of the age- specific mortality rate and, therefore, the general form of the survivorship curve. Estimates of shape and scale parameters and their confidence intervals can be easily calculated and used to compare survivorship curves of different populations.

Inputs of trace elements derived from coal ash to terrestrial and aquatic environments were investigated near an 83 MW coal-burning power plant. Comparisons were made between terrestrial inputs of trace elements through aerial deposition during 23 years before installation of electrostatic precipitators and aquatic inputs from ash disposal basins after installation. A gaussian plume model was used to predict deposition patterns of 29 trace elements in coal ash about the power plant. Detectable increases of only Sr, As, Sb, and Be in surface soils within 3 km of the power plant were predicted. Concentrations measured in surface soils were largely consistent with these predictions. Measurements of aerial deposition of Cd, Pb, Cu, and Mn at a site 5.5 km distant were similar to those in other rural areas and indicated that little of the measured Cd, Cu, Mn, or Pb was derived from fly ash. Concentrations of 12 heavy metals in effluents from the basin receiving ash were comparable to those predicted in rainfal...

Cadmium, Cu, Mn, and Pb were analyzed in bulk precipitation for 21 mo at a 2 ha pond, located 5.5 km northwest of an 83 MW coal-fired power plant in South Carolina. No significant changes in mean concentrations of the four metals in bulk precipitation were observed after installation of modern electrostatic precipitators on the stacks of the power plant, which had previously been equipped with mechanical cyclone collectors for removal of fly ash. Hence, fly ash from stack emissions was apparently not a major source of aerially deposited trace metals at the pond site. Annual inputs of the four metals in bulk precipitation at the pond were similar to values reported for other rural areas in North America. Enrichment factors, with Mn as a reference element, indicated that Cd, Cu, and Pb in bulk precipitation were not derived from soil or crustal material. Cadmium, Cu, and Pb were enriched in all samples of bulk precipitation relative to their abundances in local soils, and were most enriched during autumn and winter. A multiple regression procedure suggested that wetfall was the primary mode of aerial deposition of Cd and Cu, whereas both wetfall and dryfall were important modes of aerial deposition of Pb.

Growth and condition of bluegills Lepomis macrochirus from five acidic lakes (pH 5.1–6.0) and six circumueutral lakes (pH 6.7–7.5) in northern Wisconsin were compared. Although mean condition factors and mean back-calculated total lengths at ages 1 to 4 varied significantly among lakes, the differences were not related to lake pH. Rather, the ranks of mean condition factors and back-calculated lengths at ages 2, 3, and 4 were negatively correlated with relative density of bluegills among the lakes. Because of the dominating effect of density, growth rates and condition factors are not useful as indicators of chronic, pH-related stress on bluegill populations.

Many lakes in three areas in the Upper Midwest – northeastern Minnesota, northern Wisconsin, and the Upper Peninsula of Michigan – have low acid neutralizing capacity (ANC) and may be susceptible to change by acidic deposition. Northcentral Wisconsin and the Upper Peninsula of Michigan together contain about 150–300 acidic lakes (ANC ≤ 0), whereas none have been found in Minnesota. These acidic lakes are precipitation-dominated, Clearwater seepage lakes having small surface area, shallow depth, and low concentrations of dissolved organic carbon. The spatial distribution of these acidic lakes parallels a west to east gradient of increasing sulfate and hydrogen ion deposition. Several of these acidic lakes exhibit chemical characteristics and biological changes consistent with those observed elsewhere in waters reported to be acidified by acidic deposition. However, an hypothesis of recent lake acidification is not supported by analyses of either historical chemical data or diatom remains in lake s...

Numerous surveys have shown that fish species richness (number of species) is positively correlated with lake pH. However, species richness of fish communities is also correlated with lake size, and low-pH lakes are often small. Thus, conclusions drawn from examination of fish community structure relative to spatial (among-lake) variation in pH have been limited by uncertainties regarding the confounded effects of lake area. We used two statistical methods, analysis of covariance and a nonparametric blocked comparison test, to remove effects of lake area and compare fish species richness in low-pH and high-pH lakes. Data from six previous surveys of water chemistry and fish communities in lakes of Ontario and northern Wisconsin were examined. Lakes with low pH (≤6.0) contained significantly fewer fish species than lakes with high pH (>6.0) when the effect of lake area was considered. A simple probabilistic model showed that the ability to detect differences in species richness is low when lake ar...

Profiles of total mercury (Hg) concentrations in sediments were examined in 11 lakes in north-central Wisconsin having a broad range of pH (5.1 to 7.8) and alkalinity (−12 to 769 μeq/L). The sediments, which were hydrous and flocculent, were collected at or near the area of maximum depth in each lake with a diver-operated sampler that permittedin situ sectioning of a 1-m core. Mercury concentrations were greatest in the top 15 cm of the cores and were much lower in the deeper strata. The Hg content in the most enriched stratum of individual cores ranged from 0.09 to 0.24 μg/g dry weight, whereas concentrations in deep, precolonial strata ranged from 0.04 to 0.07 μg/g. Sediment enrichment factors varied from 0.8 to 2.8 and were not correlated with lake pH. The increase in the Hg content of recent sediments was attributed to increased atmospheric deposition of the metal. Eight of the 11 systems studied were low-alkalinity lakes that presumably received most (≥90%) of their hydrologic input from precipitation falling directly onto the lake surface. Thus, the sedimentary Hg in these lakes seems more likely linked to direct atmospheric deposition onto the lake surfaces than to influxes from the watershed. The data imply that a potentially significant fraction of the high Hg burdens measured in game fish in certain lakes in north-central Wisconsin originated from atmospheric sources.

Kaufman D. W., Gentry J. B., Kaufman G. A., Smith M. H. & Wiener J. G., 1978: Density estimation of small mammals: comparison of techniques utilizing removal trapping. Acta theriol., 23, 7: 147—171 [With 10 Tables]. Removal trapping was conducted on 12X12 grids with assessment lines to test the relative effectiveness of the Standard Minimum, Inner Square and Assessment Line methods for small mammal density estimation. Twelve study sites were trapped in desert, chaparral and woodland habitats in California and Nevada to provide a wide array of species and densities for the comparison of estimation techniques. The procedure used was to trap each grid for 10 days followed by 4 days of trapping on the associated assessment lines. Field sites were quite variable with a range of 12—167 rodents per grid representing 2—10 species. Density estimates ranged from 3.7—51.5 animals/ha for the Standard Minimum method, 4.0—36.9 animals/ha for the Inner Square method and 0.7—114.4 animals/ha for the Assessment Line method. All methods provide restive density estimates for within method comparisons but their usefulness for estimating absolute density is limited. The Assessment Line technique probably yields the best absolute density estimates (DAL) when sufficient numbers of assessment lines are trapped; however, under most conditions a single 12X12 grid with 8 assessment lines is not sufficient. To obtain reliable Dal values, captures on assessment lines need to be combined for two or more grids from the same habitat to delineate the area of effect around a grid. Problems associated with each of the methods are discussed in detail. Savannah River Ecol. Lab., SROO, Bldg. 772-G, Aiken, South Ca

Concentrations of Cd, Pb, and three essential metals (Cu, Mn, and Zn) in stocked bluegill (Lepomis macrochirus) and eight resident species of fish were studied in an acidic, highly organic pond on the southeastern U.S. coastal plain. Concentrations of Cu, Mn, and Zn in stocked and resident fish were apparently homeostatically controlled in liver tissue, axial musculature, and whole body. Concentrations of all metals studied in axial muscle tissue and whole body of stocked bluegill remained relatively constant after 200 d of residence in the pond. Analysis of concentration factors from pond water to whole stocked bluegill indicated that Pb in this system was less available to fish than in hardwater lakes. In contrast, Cd in the pond was as available to fish as in harder waters. Differences in relative availabilities of Cd and Pb were explained by the tendency of Pb to form complexes with naturally occurring organics. The need for metal-specific analysis of biological availability of metals in highly organic softwater systems is stressed. Key words: trace metal, availability, fish, soft water, concentration factor, organic water