An assessment of temporal trends in mercury concentrations in fish.

The importance of fish consumption as the primary pathway of human exposure to mercury and the establishment of fish consumption advisories to protect human health have led to large fish tissue monitoring programs worldwide. Data on fish tissue mercury concentrations collected by state, tribal, and provincial governments via contaminant monitoring programs have been compiled into large data bases by the U.S. Environmental Protection Agency's Great Lakes National Monitoring Program Office (GLNPO), the Ontario Ministry of the Environment's Fish Contaminants Monitoring and Surveillance Program (FMSP), and many others. These data have been used by a wide range of governmental and academic investigators worldwide to examine long-term and recent trends in fish tissue mercury concentrations. The largest component of the trend literature is for North American freshwater species important in recreational fisheries. This review of temporal trends in fish tissue mercury concentrations focused on published results from freshwater fisheries of North America as well as marine fisheries worldwide. Trends in fish tissue mercury concentrations in North American lakes with marked overall decreases were reported over the period 1972-2016. These trends are consistent with reported mercury emission declines as well as trends in wet deposition across the U.S. and Canada. More recently, a leveling-off in the rate of decreases or increases in fish tissue mercury concentrations has been reported. Increased emissions of mercury from global sources beginning between 1990 and 1995, despite a decrease in North American emissions, have been advanced as an explanation for the observed changes in fish tissue trends. In addition to increased atmospheric deposition, the other factors identified to explain the observed mercury increases in the affected fish species include a systematic shift in the food-web structure with the introduction of non-native species, creating a new or expanding role for sediments as a net source for mercury. The influences of climate change have also been identified as contributing factors, including considerations such as increases in temperature (resulting in metabolic changes and higher uptake rates of methylmercury), increased rainfall intensity and runoff (hydrologic export of organic matter carrying HgII from watersheds to surface water), and water level fluctuations that alter either the methylation of mercury or the mobilization of monomethylmercury. The primary source of mercury exposure in the human diet in North America is from the commercial fish and seafood market which is dominated (>90%) by marine species. However, very little information is available on mercury trends in marine fisheries. Most of the data used in the published marine trend studies are assembled from earlier reports. The data collection efforts are generally intermittent, and the spatial and fish-size distribution of the target species vary widely. As a result, convincing evidence for the existence of fish tissue mercury trends in marine fish is generally lacking. However, there is some evidence from sampling of large, long-lived commercially-important fish showing both lower mercury concentrations in the North Atlantic in response to reduced anthropogenic mercury emission rates in North America and increases in fish tissue mercury concentrations over time in the North Pacific in response to increased mercury loading.

Mercury, omega-3 fatty acids, and seafood intake are not associated with heart rate variability or QT interval.

Mercury (Hg), eicosapentaenoic acid (EPA), and docosahexaenoic acid (DHA) concentrations differ across seafood types. Our aim was to investigate the association of Hg, EPA, and DHA, as well as avid consumption of diverse seafood types, with cardiovascular variables heart rate variability (HRV) and QT interval duration (QTc) in a contemporary population. We measured HRV and QTc by Holter monitor, EPA and DHA in plasma, total Hg in whole blood, and possible confounders in 94 avid seafood consumers from Long Island, NY. Participants had mean Hg of 8.4 mcg/L, mean EPA of 1.2%, and mean DHA of 3.7% of total fatty acids. Adjusted for possible confounders, EPA+DHA, Hg, and total seafood consumption were not associated with HRV or QTc. Associations with consumption of specific seafood types were suggested (eg, tuna steak with QTc and anchovies with HRV) but require verification.

Low levels of lead and glutathione markers of redox status in human blood.

Exposure to lead (Pb) is implicated in a plethora of health threats in both adults and children. Increased exposure levels are associated with oxidative stress in the blood of workers exposed at occupational levels. However, it is not known whether lower Pb exposure levels are related to a shift toward a more oxidized state. To assess the association between blood lead level (BLL) and glutathione (GSH) redox biomarkers in a population of healthy adults, BLL and four GSH markers (GSH, GSSG, GSH/GSSG ratio and redox potential E h ) were measured in the blood of a cross-sectional cohort of 282 avid seafood-eating healthy adults living on Long Island (NY). Additionally, blood levels of two other metals known to affect GSH redox status, selenium (Se) and mercury (Hg), and omega-3 index were tested for effect modification. Regression models were further adjusted for demographic and smoking status. Increasing exposure to Pb, measured in blood, was not associated with GSSG, but was associated with lower levels of GSH/GSSG ratio and more positive GSH redox potential E h , driven by its association with GSH. No effect modification was observed in analyses stratified by Hg, Se, omega-3 index, sex, age, or smoking. Blood Pb is associated with lower levels of GSH and the GSH/GSSG ratio in this cross-sectional study of healthy adults.

Mercury exposure, serum antinuclear antibodies, and serum cytokine levels in the Long Island Study of Seafood Consumption: A cross-sectional study in NY, USA.

Mercury (Hg) is a well-known neurotoxin, and has been more recently studied specifically as an immunotoxin. In experimental and a few epidemiologic studies, Hg has been associated with distinct cytokine profiles and antinuclear antibody (ANA) positivity, though patterns at lower levels of exposure, typical of seafood consumers with a western diet, are not well characterized. Seafood consumers (n=287) recruited on Long Island, NY completed food frequency and health questionnaires and provided blood for analysis of Hg, poly-unsaturated fatty acids (omega-3 and omega-6 fatty acids), selenium (Se), ANA, and several cytokines (IL-1ß, IL-4, IL-10, TNF-α, IL-17, IFN-γ, and IL-1ra). Logistic and linear regression analyses were conducted to evaluate associations between serum Hg and cytokines and ANA. Adjusted models accounted for gender, age, ethnicity, income, education, smoking, BMI, selenium, omega-3 fatty acids, omega-6 fatty acids, omega-6/omega-3 ratio, and fish intake. Sex-stratified models were also generated with the expectation that immune profiles would differ between women and men. Median blood Hg was 4.58µg/L with 90th %ile =19.8µg/L. Nine individuals displayed ANA positivity at serum titers above 1:80; many of the cytokines were below detection limits, and the ability to detect was used in the logistic regression analyses. In linear and logistic regression analyses, Hg was not significantly associated with any of the seven investigated cytokines or with ANA-positivity. Therefore, Hg was not associated with altered immune profiles in this population of seafood consumers.

Mercury, eicosapentanoic acid and docosahexaenoic acid demonstrate limited effect on plasma paraoxonase-1 activity and blood pressure among avid seafood consumers in the Long Island Study of Seafood Consumption, NY, USA.

BACKGROUND AND AIM: Moderate fish consumption is recommended for prevention of coronary heart disease (CHD) as docosahexaenoic acid (DHA) and eicosapentaenoic acid (EPA) have known beneficial effects on risk factors such as reducing blood pressure (BP) and increasing paraoxonase-1 (PON-1) activity. However concomitant methylmercury (MeHg) exposure from fish consumption may mitigate these benefits and the net effect on BP and PON-1 activity has not been extensively studied in western populations consuming diverse seafood types. We studied the correlation between EPA, DHA and Hg levels with BP and PON-1 activity in a population of avid seafood consumers. METHODS: Two hundred and eighty-eight avid seafood consumers from Long Island, NY had blood samples drawn for total blood mercury (THg), plasma EPA and DHA levels, and plasma PON-1 activity. Average systolic blood pressure (SBP), diastolic blood pressure (DBP) and pulse pressure (PP) were measured. RESULTS: Subjects' mean EPA+DHA was 4.9% total fatty acids, mean THg was 7.6mcg/L. Mean SBP was 122.5mmHg, mean DBP 70.3mmHg, mean PP 52.2mmHg and mean PON-1 activity 421.2U/L. THg was not associated with any of the BP measures in adjusted linear regression models; EPA+DHA was significantly inversely associated with PP (p=0.02). THg was associated with a significant increase in PON-1 activity (p=0.04), while EPA+DHA was associated with a significant decrease in PON-1 activity (p=0.007); although the size of the effects was small. CONCLUSIONS: Our findings suggest blood THg and serum DHA+EPA levels have limited relationship to BP and PON-1 activity, and may not be important modulators of these known CHD risk factors in this population of avid seafood consumers.

Comparing nearshore benthic and pelagic prey as mercury sources to lake fish: the importance of prey quality and mercury content.

Mercury (Hg) bioaccumulation in fish poses well-known health risks to wildlife and humans through fish consumption. Yet fish Hg concentrations are highly variable, and key factors driving this variability remain unclear. One little studied source of variation is the influence of habitat-specific feeding on Hg accumulation in lake fish. However, this is likely important because most lake fish feed in multiple habitats during their lives, and the Hg and caloric content of prey from different habitats can differ. This study used a three-pronged approach to investigate the extent to which habitat-specific prey determine differences in Hg bioaccumulation in fish. This study first compared Hg concentrations in common nearshore benthic invertebrates and pelagic zooplankton across five lakes and over the summer season in one lake, and found that pelagic zooplankton generally had higher Hg concentrations than most benthic taxa across lakes, and over a season in one lake. Second, using a bioenergetics model, the effects of prey caloric content from habitat-specific diets on fish growth and Hg accumulation were calculated. This model predicted that the consumption of benthic prey results in lower fish Hg concentrations due to higher prey caloric content and growth dilution (high weight gain relative to Hg from food), in addition to lower prey Hg levels. Third, using data from the literature, links between fish Hg content and the degree of benthivory, were examined, and showed that benthivory was associated with reduced Hg concentrations in lake fish. Taken together, these findings support the hypothesis that higher Hg content and lower caloric content make pelagic zooplankton prey greater sources of Hg for fish than nearshore benthic prey in lakes. Hence, habitat-specific foraging is likely to be a strong driver of variation in Hg levels within and between fish species.

Mercury, selenium and fish oils in marine food webs and implications for human health.

Humans who eat fish are exposed to mixtures of healthful nutrients and harmful contaminants that are influenced by environmental and ecological factors. Marine fisheries are composed of a multitude of species with varying life histories, and harvested in oceans, coastal waters and estuaries where environmental and ecological conditions determine fish exposure to both nutrients and contaminants. Many of these nutrients and contaminants are thought to influence similar health outcomes (i.e., neurological, cardiovascular, immunological systems). Therefore, our understanding of the risks and benefits of consuming seafood require balanced assessments of contaminants and nutrients found in fish and shellfish. In this paper, we review some of the reported benefits of fish consumption with a focus on the potential hazards of mercury exposure, and compare the environmental variability of fish oils, selenium and mercury in fish. A major scientific gap identified is that fish tissue concentrations are rarely measured for both contaminants and nutrients across a range of species and geographic regions. Interpreting the implications of seafood for human health will require a better understanding of these multiple exposures, particularly as environmental conditions in the oceans change.

Mercury exposure and a shift toward oxidative stress in avid seafood consumers.

Mechanisms of mercury (Hg) toxicity at low doses from seafood consumption, the most common exposure route, are not well understood. We tested the hypothesis that seafood Hg exposure is related to a shift in redox status, indicated by a decrease in the ratio of reduced to oxidized glutathione (GSH:GSSG) in blood, or increase in redox potential (Eh). We also examined whether key seafood nutrients (selenium (Se), omega-3 fatty acids) confound or modify this shift. We measured blood concentrations of total Hg, Se, GSH, GSSG, and the Omega-3 Index (% omega-3s of total fatty acids in red blood cell membranes) in seafood consumers in Long Island, NY. We examined relationships between Hg, GSH:GSSG ratio and Eh. Elevated blood Hg (>5.8µgL(-1)) was associated with lower GSH:GSSG (ß=-116.73, p=0.01), with no evidence of confounding by Se or Omega-3 Index. However, in models stratified by Omega-3 Index levels, Hg-GSH:GSSG associations were weakened among those with high Omega-3 Index levels (>6% of fatty acids, ß=-63.46, p=0.28), and heightened among those with low Omega-3 Index (ß=-182.53, p<0.01). We observed comparable patterns for Eh in relation to Hg. These results support the hypothesis that Hg exposure from seafood is linked to a shift in redox status toward oxidative stress, modified by omega-3 fatty acids in this population. Further work should examine the role of different seafood nutrients and Hg-induced shifts in redox status in the diverse health effects associated with elevated Hg exposure.

Low-level mercury, omega-3 index and neurobehavioral outcomes in an adult US coastal population.

BACKGROUND: Neurodevelopmental effects of omega-3 fatty acids and mercury from fish consumption have been characterized in children. In contrast, neurobehavioral outcomes associated with fish are not well studied in adults. OBJECTIVE: This study of avid seafood consumers on Long Island (NY, USA) sought to define associations between mercury, seafood consumption, omega-3 fatty acids and neurobehavioral outcomes. METHODS: A computer-based test system was used to assess neurobehavioral function. Blood total Hg (Hg) and omega-3 index were measured in 199 adult avid seafood eaters, who also completed the neurobehavioral assessment and an extensive food and fish frequency and demographic questionnaire. RESULTS: For most of the outcomes considered, neither Hg nor omega-3 index was associated with neurobehavioral outcomes after adjustment for key confounding variables. Fish consumption, however, was associated with decreased odds of both self-reported fatigue (OR 0.85; 95 % CI 0.72, 1.01) and a constellation of neurologic symptoms (OR 0.79; 95 % CI 0.66, 0.96). CONCLUSIONS: Results from our study provide little evidence that omega-3 fatty acids or Hg is associated with cognitive function in adult avid seafood consumers. Larger studies are needed to confirm our finding of associations between fish consumption and decreased self-reported fatigue and neurologic impairment.

Demographic Profiles, Mercury, Selenium, and Omega-3 Fatty Acids in Avid Seafood Consumers on Long Island, NY.

Seafood consumption is known to confer nutritional benefits and risks from contaminant exposure. Avid seafood consumers are neither well-characterized with regard to their demographic profile nor their underlying risk-benefit profile. Contaminants [e.g., mercury (Hg)] and nutrients [e.g., selenium (Se), omega-3 fatty acids] are prevalent in some seafood. Participants (N = 285) recruited on Long Island, NY, completed food frequency and health questionnaires and received blood draws analyzed for Hg, omega-3s, and Se. Participants were categorized based on frequency and type of seafood consumption. Logistic regression analyses evaluated relationships between seafood consumption and demographics, and were age- and sex-adjusted. t tests assessed relationships between seafood consumption patterns and biomarkers Hg, omega-3s, and Se. Consumption of both tuna and salmon was associated with older age: those aged 55-75 and over 75 years old were more likely than participants aged 18-34 to eat tuna and salmon (OR 2.27; 95% CI 1.05, 4.89 and OR 3.67; 95% CI 1.20, 11.20, respectively). Males were less likely than females to eat fish other than tuna or salmon (OR 0.58; 95% CI 0.34, 0.97). Caucasians were more likely to consume tuna (OR 0.31; 95% CI 0.10, 0.96) or salmon and tuna (OR 0.34; 95% CI 0.12, 0.91), while non-Caucasians were more likely to consume other fish types (OR 2.73; 95% CI 1.45, 5.12). Total blood Hg was associated with weekly consumption of any type of fish (p = 0.01) and with salmon and tuna consumption (p = 0.01). Salmon was associated with plasma omega-3s (p = 0.01). Se was not associated with fish intake categories. Risk communicators can use these findings to influence seafood preferences of different demographic groups.

High mercury seafood consumption associated with fatigue at specialty medical clinics on Long Island, NY.

We investigated the association between seafood consumption and symptoms related to potential mercury toxicity in patients presenting to specialty medical clinics at Stony Brook Medical Center on Long Island, New York. We surveyed 118 patients from April-August 2012 about their seafood consumption patterns, specifically how frequently they were eating each type of fish, to assess mercury exposure. We also asked about symptoms associated with mercury toxicity including depression, fatigue, balance difficulties, or tingling around the mouth. Of the 118 adults surveyed, 14 consumed high mercury seafood (tuna steak, marlin, swordfish, or shark) at least weekly. This group was more likely to suffer from fatigue than other patients (p = 0.02). Logistic regression confirmed this association of fatigue with frequent high mercury fish consumption in both unadjusted analysis (OR = 5.53; 95% CI: 1.40-21.90) and analysis adjusted for age, race, sex, income, and clinic type (OR = 7.89; 95% CI: 1.63-38.15). No associations were observed between fish intake and depression, balance difficulties, or tingling around the mouth. Findings suggest that fatigue may be associated with eating high mercury fish but sample size is small. Larger studies are needed to determine whether fish intake patterns or blood mercury tests warrant consideration as part of the clinical work-up in coastal regions.

Elevated blood Hg at recommended seafood consumption rates in adult seafood consumers.

Mercury (Hg) exposure from seafood continues to be a public health concern due to health effects from elevated exposure, increasing worldwide seafood consumption, and continued Hg inputs into the environment. Elevated Hg exposure can occur in populations with specialized diets of sport-caught freshwater fish. However, we need a better understanding of Hg exposure from seafood, the most common exposure source, and from specific seafood types. We examined Hg exposure in avid seafood consumers, and the seafood items and consumption frequency that confer the largest Hg exposure. Adult, avid seafood consumers, in Long Island, NY, USA, with blood total Hg concentrations predicted to exceed the USEPA reference concentration that is considered safe (5.8 µg L(-1)), were eligible for the study; 75% of self-reported avid seafood consumers were eligible to participate. We measured blood total Hg concentrations and seafood consumption in 285 participants. We examined relationships between Hg and seafood consumption using multiple linear regression. Seafood consumption rate for our population (14.4 kg yr(-1)) was >2 times that estimated for the U.S. (6.8 kg yr(-1)), and lower than the worldwide estimate (18.4 kg yr(-1)). Mean blood Hg concentration was 4.4 times the national average, and 42% of participants had Hg concentrations exceeding 5.8 µg L(-1). Elevated Hg exposures occurred at all seafood consumption frequencies, including the recommended frequency of 2 meals per week. Blood Hg concentrations were positively associated with weekly tuna steak or sushi intake (ß=6.30 change in blood Hg, µg L(-1)) and monthly (ß=2.54) or weekly (ß=9.47) swordfish, shark or marlin intake. Our findings show that seafood consumers in this population have elevated Hg exposures even at relatively low seafood consumption rates that are at or below current dietary recommendations. Further study should examine health risks and benefits of avid seafood consumption, and consider modifying guidelines to include recommendations for specific seafood types.

Mercury-nutrient signatures in seafood and in the blood of avid seafood consumers.

Dietary recommendations for seafood are confusing due to the desire to balance both benefits from nutrients and risks from contaminants. The overall health value of different fish and shellfish items depends on concentrations of multiple nutrients (e.g., selenium (Se), omega-3 fatty acids) and contaminants (e.g., mercury (Hg)). However, few studies have examined the connections between human exposure to multiple nutrients and contaminants and the consumption of specific types of seafood. Our goals were to compare 1) Hg, Se and omega-3 fatty acid concentrations (Hg-nutrient signatures) among common fish and shellfish items and 2) Hg-nutrient signatures in the blood of avid seafood consumers, based on seafood consumption habits. We compiled nutrient and Hg concentration data for common fish and shellfish items from the literature. We also measured blood concentrations of Hg and seafood nutrients collected from adult, avid seafood consumers on Long Island, NY. Canonical discriminant analyses revealed distinct Hg-nutrient signatures among seafood items, and these signatures were reflected in the blood of consumers based on different consumption habits. For example, consumers with a salmon-dominated seafood diet had relatively high percentage of omega-3 fatty acids in blood, and consumers who tend to eat top predator seafood have higher Hg, but similar blood nutrient concentrations compared to consumers who tend to eat low trophic level seafood. These results provide direct evidence of links between the ecological characteristics of the type of seafood consumed and Hg-nutrient exposure. This approach helps assess the overall human health value of specific seafood types, leads to specific diet recommendations, and can be used to characterize risk:benefit status among seafood consumers.

Diet and toenail arsenic concentrations in a New Hampshire population with arsenic-containing water.

BACKGROUND: Limited data exist on the contribution of dietary sources of arsenic to an individual's total exposure, particularly in populations with exposure via drinking water. Here, the association between diet and toenail arsenic concentrations (a long-term biomarker of exposure) was evaluated for individuals with measured household tap water arsenic. Foods known to be high in arsenic, including rice and seafood, were of particular interest. METHODS: Associations between toenail arsenic and consumption of 120 individual diet items were quantified using general linear models that also accounted for household tap water arsenic and potentially confounding factors (e.g., age, caloric intake, sex, smoking) (n = 852). As part of the analysis, we assessed whether associations between log-transformed toenail arsenic and each diet item differed between subjects with household drinking water arsenic concentrations <1 µg/L versus ≥1 µg/L. RESULTS: As expected, toenail arsenic concentrations increased with household water arsenic concentrations. Among the foods known to be high in arsenic, no clear relationship between toenail arsenic and rice consumption was detected, but there was a positive association with consumption of dark meat fish, a category that includes tuna steaks, mackerel, salmon, sardines, bluefish, and swordfish. Positive associations between toenail arsenic and consumption of white wine, beer, and Brussels sprouts were also observed; these and most other associations were not modified by exposure via water. However, consumption of two foods cooked in water, beans/lentils and cooked oatmeal, was more strongly related to toenail arsenic among those with arsenic-containing drinking water (≥1 µg/L). CONCLUSIONS: This study suggests that diet can be an important contributor to total arsenic exposure in U.S. populations regardless of arsenic concentrations in drinking water. Thus, dietary exposure to arsenic in the US warrants consideration as a potential health risk.

Contrasting food web factor and body size relationships with Hg and Se concentrations in marine biota.

Marine fish and shellfish are primary sources of human exposure to mercury, a potentially toxic metal, and selenium, an essential element that may protect against mercury bioaccumulation and toxicity. Yet we lack a thorough understanding of Hg and Se patterns in common marine taxa, particularly those that are commercially important, and how food web and body size factors differ in their influence on Hg and Se patterns. We compared Hg and Se content among marine fish and invertebrate taxa collected from Long Island, NY, and examined associations between Hg, Se, body length, trophic level (measured by δ(15)N) and degree of pelagic feeding (measured by δ(13)C). Finfish, particularly shark, had high Hg content whereas bivalves generally had high Se content. Both taxonomic differences and variability were larger for Hg than Se, and Hg content explained most of the variation in Hg:Se molar ratios among taxa. Finally, Hg was more strongly associated with length and trophic level across taxa than Se, consistent with a greater degree of Hg bioaccumulation in the body over time, and biomagnification through the food web, respectively. Overall, our findings indicate distinct taxonomic and ecological Hg and Se patterns in commercially important marine biota, and these patterns have nutritional and toxicological implications for seafood-consuming wildlife and humans.

A quantitative synthesis of mercury in commercial seafood and implications for exposure in the United States.

BACKGROUND: Mercury (Hg) is a toxic metal that presents public health risks through fish consumption. A major source of uncertainty in evaluating harmful exposure is inadequate knowledge of Hg concentrations in commercially important seafood. OBJECTIVES: We examined patterns, variability, and knowledge gaps of Hg in common commercial seafood items in the United States and compared seafood Hg concentrations from our database to those used for exposure estimates and consumption advice. METHODS: We developed a database of Hg concentrations in fish and shellfish common to the U.S. market by aggregating available data from government monitoring programs and the scientific literature. We calculated a grand mean for individual seafood items, based on reported means from individual studies, weighted by sample size. We also compared database results to those of federal programs and human health criteria [U.S. Food and Drug Administration Hg Monitoring Program (FDA-MP), U.S. Environmental Protection Agency (EPA)]. RESULTS: Mean Hg concentrations for each seafood item were highly variable among studies, spanning 0.3-2.4 orders of magnitude. Farmed fish generally had lower grand mean Hg concentrations than their wild counterparts, with wild seafood having 2- to 12-fold higher concentrations, depending on the seafood item. However, farmed fish are relatively understudied, as are specific seafood items and seafood imports from Asia and South America. Finally, we found large discrepancies between mean Hg concentrations estimated from our database and FDA-MP estimates for most seafood items examined. CONCLUSIONS: The high variability in Hg in common seafood items has considerable ramifications for public health and the formulation of consumption guidelines. Exposure and risk analyses derived from smaller data sets do not reflect our collective, available information on seafood Hg concentrations.

Multielement stoichiometry in aquatic invertebrates: when growth dilution matters.

Element concentrations in organisms can be variable, often causing deviations from otherwise consistent, taxon-specific multielement stoichiometries. Such variation can have considerable ecological consequences, yet physiological mechanisms remain unclear. We tested the influence of somatic growth dilution (SGD) on multiple element concentrations under different bioenergetic conditions. SGD occurs when rapid individual growth causes a disproportional gain in biomass relative to gain of a specific element. SGD can strongly affect elements in various organisms, but we lack a general framework to unify results across studies and assess its overall importance. We derived the general conditions that trigger SGD from an element accumulation model. We parameterized the model with bioenergetic and element-specific rates summarized from the literature to compare SGD effects on 15 elements (nonessential metals, essential trace elements, macronutrients) in three aquatic invertebrate taxa. For all taxa, we found that SGD (1) occurs to some degree for all 15 elements over realistic ranges of growth and ingestion rates and (2) has the greatest effect on elements with low efflux (excretion) rates, including certain nonessential metals (e.g., MeHg, Po), essential trace elements, and macronutrients (e.g., N, Fe). Thus, SGD can strongly affect concentrations of a spectrum of elements under natural conditions. These results provide a framework for predicting variation in the elemental composition of animals.

Stoichiometric controls of mercury dilution by growth.

Rapid growth could significantly reduce methylmercury (MeHg) concentrations in aquatic organisms by causing a greater than proportional gain in biomass relative to MeHg (somatic growth dilution). We hypothesized that rapid growth from the consumption of high-quality algae, defined by algal nutrient stoichiometry, reduces MeHg concentrations in zooplankton, a major source of MeHg for lake fish. Using a MeHg radiotracer, we measured changes in MeHg concentrations, growth and ingestion rates in juvenile Daphnia pulex fed either high (C:P = 139) or low-quality (C:P = 1317) algae (Ankistrodesmus falcatus) for 5 d. We estimated Daphnia steady-state MeHg concentrations, using a biokinetic model parameterized with experimental rates. Daphnia MeHg assimilation efficiencies (approximately 95%) and release rates (0.04 d(-1)) were unaffected by algal nutrient quality. However, Daphnia growth rate was 3.5 times greater when fed high-quality algae, resulting in pronounced somatic growth dilution. Steady-state MeHg concentrations in Daphnia that consumed high-quality algae were one-third those of Daphnia that consumed low-quality algae due to higher growth and slightly lower ingestion rates. Our findings show that rapid growth from high-quality food consumption can significantly reduce the accumulation and trophic transfer of MeHg in freshwater food webs.

Beyond macronutrients: element variability and multielement stoichiometry in freshwater invertebrates.

We contrasted concentrations of macronutrients (C, N and P), essential (As, Cu, Zn and Se) and non-essential metals (Pb, Hg and Cd) in invertebrates across five lakes and June to October in one lake. We predicted that somatic concentrations of tightly regulated elements would be less variable than weakly and unregulated elements. Within each taxon, variation was lowest in macronutrients, intermediate in essential micronutrients, and highest in non-essential metals, which corresponded in rank to homeostatic regulation strength for the same elements calculated from the literature. Hence, homeostatic regulation may strongly influence variation in element concentrations of biota in situ. Of the individual elements, only taxonomic differences in C and N were consistent across lakes and over a season. Nevertheless, canonical discriminant analyses successfully discriminated among taxa based on taxonomic multielement composition. Thus, relative taxonomic differences in multielement composition appear more informative than absolute stoichiometric formulae when considering the role of inherently variable trace elements in ecological investigations.

Impact of land disturbance on the fate of arsenical pesticides.

Increasing development of historic farmlands raises questions regarding the fate of pesticides applied when these land were in cultivation. We quantified As and Pb budgets in field soils in two orchards where arsenical pesticides were applied in the early 20th century and a third uncontaminated control field. Sequential extractions and X-ray analyses also were used to determine mineral phases. In addition, we measured metal loads in drainages adjacent to the fields and in two common macroinvertebrate taxa within the wetland at the outlet of the drainages. We find that the applied As and Pb have undergone little vertical redistribution; concentrations of As and Pb in the top 25 cm of contaminated orchard soils are higher than in the uncontaminated control field. However, none of the applied lead arsenate (PbHAsO4) remains in its original mineral phase. Instead, the metals are now primarily adsorbed onto fine silt and clay-sized amorphous oxides and organic matter. Further, physical erosion associated with tilling and replanting appears to have mobilized the fine-particulate-bound As and Pb in one orchard. The remobilized metals are found in sediments in the stream channel draining the tilled orchard. It is unclear if the As and Pb transported sediments are biologically active; average macroinvertebrate metal burdens in the wetland are not elevated above those observed elsewhere in the region. However, little of the mobilized metals may have reached the wetland. These results demonstrate that land use change can significantly impact the retention of arsenical pesticides.