MeHg Risk Research Articles

A Meta-Analysis of Mercury Biomagnification in Freshwater Predatory Invertebrates: Community Diversity and Dietary Exposure Drive Variability.

Accurate estimates of methylmercury (MeHg) exposure are valuable to actionably assess risk and protect wildlife and human health. MeHg trophic transfer is a critical driver of risk: MeHg is generally biomagnified by a factor of 8.3 ± 7.5 from one trophic level to the next, averaged across freshwater communities (mean ± standard deviation). This variability can produce disparate risks even where basal MeHg concentrations are similar. Taxonomy may be one driver of this variability: physiologically diverse groups, like vertebrates and invertebrates, may assimilate MeHg differently. To determine whether taxonomy affects trophic transfer efficiency, we conducted a meta-analysis characterizing predatory invertebrate MeHg biomagnification. Our analyses estimated that freshwater predatory invertebrates biomagnify MeHg by factors of 2.1 ± 0.2 to 4.3 ± 0.3, with a 98.9 ± 0.4% posterior probability that factors are below 5 (mean ± standard error). When vertebrates or primary producers were included, a site's trophic magnification factor was 18.6 ± 6.2 to 54.1 ± 7.7% higher than estimates for invertebrates alone. Biomagnification was inversely correlated to prey MeHg concentration and varied among systematic and functional groups. These data suggest that predatory invertebrates biomagnify MeHg less efficiently than vertebrates and that a community's diversity and structure determine its biomagnification efficiency. Incorporating organismal variation in trophic transfer estimates may improve the assessment, communication, and management of MeHg risk.

Impacts of River Damming on Sediment Methylmercury Dynamics

Reservoirs are reported to stimulate mercury (Hg) methylation and thereby affect methylmercury (MeHg) dynamics in rivers by trapping sediment and increasing the hydraulic residence time (HRT). However, whether there are similarities in sediment %MeHg (MeHg/Hg) in relation to reservoir properties for different rivers and their associated mechanisms remain unknown. Here, we investigated the sediment MeHg in two heavily dammed rivers and one naturally flowing river in the same region. We found that river damming results in the accumulation of sediment Hg and OC and a higher abundance of hgcAB, thus elevating the sediment %MeHg. Sediment %MeHg showed a positive correlation with reservoir HRT, and the methylation time of Hg acts as the threshold value to determine the impact of river damming on sediment %MeHg. However, sediment %MeHg had either a positive or a negative correlation with reservoir age in different rivers, and the effect of reservoir age on sediment %MeHg depends on whether the stock of substances in the reservoir has a dominance of internal consumption or is one of external supply. These findings provide an important reference for further research on Hg biogeochemical cycling and MeHg risk management in dammed rivers.

Understanding the risks of mercury sulfide nanoparticles in the environment: Formation, presence, and environmental behaviors

Mercury (Hg) could be microbially methylated to the bioaccumulative neurotoxin methylmercury (MeHg), raising health concerns. Understanding the methylation of various Hg species is thus critical in predicting the MeHg risk. Among the known Hg species, mercury sulfide (HgS) is the largest Hg reservoir in the lithosphere and has long been considered to be highly inert. However, with advances in the analytical methods of nanoparticles, HgS nanoparticles (HgS NPs) have recently been detected in various environmental matrices or organisms. Furthermore, pioneering laboratory studies have reported the high bioavailability of HgS NPs. The formation, presence, and transformation (e.g., methylation) of HgS NPs are intricately related to several environmental factors, especially dissolved organic matter (DOM). The complexity of the behavior of HgS NPs and the heterogeneity of DOM prevent us from comprehensively understanding and predicting the risk of HgS NPs. To reveal the role of HgS NPs in Hg biogeochemical cycling, research needs should focus on the following aspects: the formation pathways, the presence, and the environmental behaviors of HgS NPs impacted by the dominant influential factor of DOM. We thus summarized the latest progress in these aspects and proposed future research priorities, e.g., developing the detection techniques of HgS NPs and probing HgS NPs in various matrices, further exploring the interactions between DOM and HgS NPs. Besides, as most of the previous studies were conducted in laboratories, our current knowledge should be further refreshed through field observations, which would help to gain better insights into predicting the Hg risks in natural environment.

Algal Organic Matter Drives Methanogen-Mediated Methylmercury Production in Water from Eutrophic Shallow Lakes.

Algal blooms bring massive amounts of algal organic matter (AOM) into eutrophic lakes, which influences microbial methylmercury (MeHg) production. However, because of the complexity of AOM and its dynamic changes during algal decomposition, the relationship between AOM and microbial Hg methylators remains poorly understood, which hinders predicting MeHg production and its bioaccumulation in eutrophic shallow lakes. To address that, we explored the impacts of AOM on microbial Hg methylators and MeHg production by characterizing dissolved organic matter with Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and three-dimensional excitation-emission matrix (3D-EEM) fluorescence spectroscopy and quantifying the microbial Hg methylation gene hgcA. We first reveal that the predominance of methanogens, facilitated by eutrophication-induced carbon input, could drive MeHg production in lake water. Specifically, bioavailable components of AOM (i.e., CHONs such as aromatic proteins and soluble microbial byproduct-like materials) increased the abundances (Archaea-hgcA gene: 438-2240% higher) and activities (net CH4 production: 16.0-44.4% higher) of Archaea (e.g., methanogens). These in turn led to enhanced dissolved MeHg levels (24.3-15,918% higher) for three major eutrophic shallow lakes in China. Nevertheless, our model results indicate that AOM-facilitated MeHg production could be offset by AOM-induced MeHg biodilution under eutrophication. Our study would help reduce uncertainties in predicting MeHg production, providing a basis for mitigating the MeHg risk in eutrophic lakes.

Understanding the effects of sulfur input on mercury methylation in rice paddy soils.

Sulfur could be introduced into paddy soils via dry or wet deposition, irrigation, and fertilization, which subsequently impacts the production of methylmercury (MeHg), a bioaccumulative neurotoxicant. However, effects of sulfur input on MeHg production are variable, possibly due to the multiple effects of sulfur on Hg mobility and/or microbial Hg methylators, leading to uncertainties in predicting MeHg risk. To address that, we explored the effects of different types and amounts of sulfur as well as concentrations of ambient sulfate on Hg methylation in paddy soils, and elucidated the mechanisms by quantifying changes in (1) Hg mobility and (2) microbial Hg methylators (e.g., sulfate-reducing bacteria, SRB). Our results indicated that MeHg levels increased by 40-86% and 30-96% in soils under various types (i.e., 200mgkg-1 elemental sulfur, ammonium sulfate, sulfur-coated urea and potassium sulfate (K2SO4)) and different amounts (i.e., 100, 200 and 400mgkg-1 K2SO4) of sulfur input. The enhanced MeHg production could be explained by increased Hg mobility but not changes in microbial Hg methylators. Besides, sulfate input increased MeHg levels (89-240%) in soils with low ambient sulfate levels (<100mgkg-1) but had no effect on high-sulfate soils (>380mgkg-1). These could be explained by the diverse responses of Hg mobility and microbial Hg methylators to sulfate input at different ambient sulfate levels. Our study opens the "black box" of Hg methylation under sulfur input, which would help reduce uncertainties in predicting MeHg risk in soils.

Ecosystem-Scale Modeling and Field Observations of Sulfate and Methylmercury Distributions in the Florida Everglades: Responses to Reductions in Sulfate Loading

The Florida Everglades has one of the most severe methylmercury (MeHg) contamination issues in the USA, resulting from factors including high rates of atmospheric mercury (Hg) deposition and sulfate inputs from agricultural lands. Sulfate loading stimulates microbial sulfate reduction and production of toxic and bioaccumulative MeHg. Controls on regional Hg emissions have been successful in reducing Hg deposition and MeHg production in wetlands in other areas, but this has not been the case for the Everglades as the Hg deposited here appears to come from unknown global sources of emissions. We posit that reductions in sulfate loading to the Florida Everglades can be an effective alternative approach used to reduce MeHg production. This study tested this hypothesis (1) by evaluating temporal trends in MeHg concentrations in response to a reduction in sulfate loading at a site in central Water Conservation Area (WCA) 3 and (2) using ecosystem-scale models to predict the effects of reductions in sulfate loading on sulfate concentrations in surface water and MeHg Risk. At the WCA site, we report a decline in sulfate concentrations (from about 9 mg/L in the late 1990s to levels of 33% in sulfate loading will significantly benefit the Everglades by reducing MeHg Risk.

Dynamics of (total and methyl) mercury in sediment, fish, and crocodiles in an Amazonian Lake and risk assessment of fish consumption to the local population

Increasing concerns have been raised about the toxicity of mercury (Hg) to humans, especially for those that consume a great amount of fish. High Hg concentrations have previously been measured in Amazonian waterbodies, both resulting from natural and anthropogenic sources. However, few studies have been conducted so far in Amazonian lakes that are fished by local populations. In addition, few of those studies included methylmercury (MeHg), the most toxic and bioaccumulative Hg form, and evaluated the influence of physico-chemical conditions and season on Hg dynamics. In the present study, total Hg (THg) and MeHg concentrations were measured in bottom sediment as well as in two fish and two crocodile species of the Amazonian Cuniã Lake. Bottom sediment MeHg concentrations were higher in the dry season than in the wet season, which is related to differences in physico-chemical (pH and electrical conductivity) conditions. Diet appeared to be related with animal tissue MeHg concentrations, with the herbivorous fish having lower MeHg levels than the predatory fish and crocodiles. Based on the measured tissue concentrations and published data on local person weight and fish consumption, MeHg risk to Cuniã Lake populations was estimated. Although the MeHg fish tissue concentrations did not exceed national and international standards, a significant risk to the local population is anticipated due to their high fish consumption rates. Graphical abstract.

Screening-level risk assessment of methylmercury for non-anadromous Arctic char (Salvelinus alpinus).

Non-anadromous forms of Arctic char (Salvelinus alpinus), those that are restricted to lakes and rivers, typically have higher mercury (Hg) concentrations than anadromous forms, which migrate to and from the sea. Using tissue burden data from the literature and our own analyses, we performed a screening-level risk assessment of methylmercury (MeHg) for non-anadromous Arctic char. Our assessment included 1569 fish distributed across 83 sites. Site-specific mean total Hg concentrations in non-anadromous Arctic char muscle varied considerably from 0.01 to 1.13 µg/g wet weight, with 21% (17 of 83 sites) meeting or exceeding a threshold-effect level in fish of 0.33 µg/g wet weight, and 13% (11 of 83 sites) meeting or exceeding a threshold-effect level in fish of 0.5 µg/g wet weight. Of the sites in exceedance of the 0.33-µg/g threshold, 7 were located in Greenland and 10 in Canada (Labrador, Nunavut, and Yukon). All but one of these sites were located in interfrost or permafrost biomes. Maximum total Hg concentrations exceeded 0.33 µg/g wet weight at 53% of sites (40 of the 75 sites with available maximum Hg values), and exceeded 0.5 µg/g wet weight at 27% (20 of 75 sites). Collectively, these results indicate that certain populations of non-anadromous Arctic char located mainly in interfrost and permafrost regions may be at risk for MeHg toxicity. This approach provides a simple statistical assessment of MeHg risk to non-anadromous Arctic char, and does not indicate actual effects. We highlight the need for studies that evaluate the potential toxic effects of MeHg in non-anadromous Arctic char, as well as those that aid in the development of a MeHg toxic-effect threshold specific to this species of fish. Environ Toxicol Chem 2019;38:489-502. © 2018 SETAC.

The implications of following dietary advice regarding fish consumption frequency and meal size for the benefit (EPA + DHA and Se) versus risk (MeHg) assessment

Fish contain healthy nutrients, such as ω3 polyunsaturated fatty acids, particularly eicosapentaenoic acid (EPA) and docosahexaenoic acid (DHA), which protect against cardiovascular disease, and selenium (Se), which reduces methylmercury (MeHg) toxicity. Fish are also a dietary source of MeHg. This requires an assessment of the benefits versus risks. A risk-benefit evaluation showed that blue shark regardless of the way it is cooked generated high probabilities of surpassing the MeHg tolerable weekly intake (TWI), >22%. In tuna, boiling and grilling led to higher MeHg risks than canning, 6–37% versus <7%. EPA + DHA contributed for the prevention of coronary disease. With exception of blue shark, Se neutralised MeHg toxicity. Higher MeHg risk was associated with blue shark and boiled and grilled tuna consumption. For tuna, however, high Se content after boiling and grilling may mitigate MeHg risk.

Bioaccessibility-corrected risk assessment of urban dietary methylmercury exposure via fish and rice consumption in China

The role of seafood consumption for dietary methylmercury (MeHg) exposure is well established. Recent studies also reveal that rice consumption can be an important pathway for dietary MeHg exposure in some Hg-contaminated areas. However, little is known about the relative importance of rice versus finfish in MeHg exposure for urban residents in uncontaminated areas. Especially, the lack of data on MeHg bioaccessibility in rice hinders accurately assessing MeHg exposure via rice consumption, and its importance compared to fish. By correcting commonly used risk models with quantified MeHg bioaccessibility, we provide the first bioaccessibility-corrected comparison on MeHg risk in rice and fish for consumers in non-contaminated urban areas of China, on both city- and province-scales. Market-available fish and rice samples were cooked and quantified for MeHg bioaccessibility. Methylmercury bioaccessibility in rice (40.5±9.4%) was significantly (p<0.05) lower than in fish (61.4±14.2%). This difference does not result from selenium content but may result from differences in protein or fiber content. Bioaccessibility-corrected hazard quotients (HQs) were calculated to evaluate consumption hazard of MeHg for consumers in Nanjing city, and Monte Carlo Simulations were employed to evaluate uncertainty and variability. Results indicate that MeHg HQs were 0.14 (P50) and 0.54 (P90). Rice consumption comprised 27.2% of the overall dietary exposure to MeHg in Nanjing, while fish comprised 72.8%. Employing our bioaccessibility data combined with literature parameters, calculated relative contribution to MeHg exposure from rice (versus fish) was high in western provinces of China, including Sichuan (95.6%) and Guizhou (81.5%), and low to moderate in eastern and southern provinces (Guangdong: 6.6%, Jiangsu: 17.7%, Shanghai: 15.1%, Guangxi: 20.6%, Jiangxi: 22.8% and Hunan: 25.9%). This bioaccessibility-corrected comparison of rice versus fish indicates that rice consumption can substantively contribute to dietary MeHg exposure risk for urban populations in Asia, and should be regularly included in dietary MeHg exposure assessment.

Benefits and risks associated with consumption of raw, cooked, and canned tuna (Thunnus spp.) based on the bioaccessibility of selenium and methylmercury

The Se, Hg, and methylmercury (MeHg) levels in raw, cooked (boiled and grilled), and canned tuna (Thunnus spp.) were determined before and after an in vitro digestion, thereby enabling the calculation of the respective bioaccessibility percentages. A risk–benefit evaluation of raw and canned tuna on the basis of the Se and MeHg data was performed. Selenium bioaccessibility was high in tuna, though slightly lower in canned than in raw products. Mercury levels were high in raw and cooked tuna. Hg bioaccessibility percentages were low (39–48%) in the cooked tuna and even lower (<20%) in canned tuna. For the bioaccessible fraction, all molar Se:MeHg ratios were higher than one (between 10 and 74). A probabilistic assessment of MeHg risk vs Se benefit showed that while a weekly meal of canned tuna presents very low risk, raw, boiled, and grilled tuna consumption should not exceed a monthly meal, at least, for pregnant and nursing women.

Modeling sulfate transport and distribution and methylmercury production associated with Aquifer Storage and Recovery implementation in the Everglades Protection Area

Abstract Aquifer Storage and Recovery (ASR) technology has been proposed to meet the competing ecological and water-supply needs of south Florida and the Everglades Protection Area (EPA). The water recovered from ASR, however, may have altered water quality. Of particular concern is the enrichment of ASR recovery water in sulfate, which can stimulate microbial sulfate reduction and methylmercury (MeHg) production within the EPA. MeHg is already a serious issue with regard to wildlife and human health, and there is concern that ASR might exacerbate the problem. In order to address these concerns, the Lake Okeechobee Environmental Model (LOEM) and the Everglades Landscape Model (ELM) were adapted with sulfur modules to predict concentrations and distributions of sulfate within Lake Okeechobee and the EPA resulting from the release of ASR water. In addition, equations were developed relating the biogeochemistry of sulfate and MeHg production to produce a MeHg production risk assessment from the modeled ASR sulfate loading. Baseline runs (no ASR discharge water), and three different ASR release scenarios with varying sulfate loading were evaluated. Results show that ASR release will temporarily elevate sulfate concentrations in Lake Okeechobee from the present level of about 30 mg/L to as high as 50 mg/L in a worst case scenario, but that this will have little impact on MeHg production in the lake. The model indicates that ASR release will have minimal impacts on sulfate loading to the EPA, primarily because of the already large sulfate loading from other sources within the Everglades Agricultural Area (EAA). Maps of sulfate distributions show that certain locations in the EPA, especially those near canal or Stormwater Treatment Area (STA) discharges, may experience significantly higher sulfate loading from ASR. Overall impacts with regard to increased MeHg production risk are predicted to be low based on this model, although sites with increased ASR sulfate loading (e.g. canal and STA discharge sites) may experience some change in MeHg risk.

Fish Mercury and Surface Water Sulfate Relationships in the Everglades Protection Area

Few published studies present data on relationships between fish mercury and surface or pore water sulfate concentrations, particularly on an ecosystem-wide basis. Resource managers can use these relationships to identify the sulfate conditions that contain fish with health-concerning total mercury (THg) levels and to evaluate the role of sulfate in methyl-mercury (MeHg) production. In this study, we derived relationships between THg in three fish trophic levels (mosquitofish, sunfish, and age-1 largemouth bass) and surface water sulfate from 1998 to 2009 for multiple stations across the Everglades Protection Area (EPA). Results show the relationship between sulfate and fish THg in each fish type is nonlinear and largely skewed, similar to the relationship between MeHg production and sulfate concentration in peatland sediment pore water identified by other researchers. Peak fish THg levels occurred in ~1 to 12 mg/L sulfate conditions. There was significant variability in the fish THg data, and there were several instances of high-fish THg levels in high-sulfate conditions (>30 mg/L). Health-concerning fish THg levels were present in all surface water sulfate conditions; however, most of these levels occurred in 1–20 mg/L sulfate. The data in this study, including recent studies, show consistent and identifiable areas of high- and low-fish THg across the spectrum of surface water sulfate concentration, therefore, applying an ecosystem-wide sulfur strategy may be an effective management approach as it would significantly reduce MeHg risk in the EPA.

Plausibility of toxicological interaction between lead and methylmercury

Humans are exposed to both lead (Pb) and methylmercury (MeHg), two chemicals known to affect the developing nervous system. It is therefore important to know whether these chemicals interact toxicologically to develop reliable estimates of human health risks. The nature of the potential interaction and how it may change with dose are also critical factors which need to be understood and considered in risk assessment. The available toxicological literature was reviewed and yielded five animal studies which involved combined exposure to both metals. None of these studies examined developmental neurotoxicity, the key endpoint of interest. Doses in these studies were also in the range of 1–100 mg kg−1 day−1, which is far above average exposure levels for Pb and MeHg in the U.S. population. The combined exposure literature is therefore uninformative concerning the potential for Pb–MeHg interaction. A subsequent evaluation of the available mechanistic data was conducted, looking for similarities in proposed modes of action relevant at low doses. Shared biological targets suggesting a potential for low dose interaction include protein kinase C, calcium homeostasis, and apoptosis. Whether interaction actually occurs, and the form the interaction might take, remains to be studied. A phased research program is proposed that may provide data needed to address this significant data gap and permit more robust Pb and MeHg risk assessment.

An Approach for Quantitatively Balancing Methylmercury Risk and Omega-3 Benefit in Fish Consumption Advisories

Background: Nearly all fish consumption advisories for methylmercury (MeHg) are based only on risk. There is a need to also address benefits, especially those from polyunsaturated fatty acids (PUFAs), in neurodevelopmental function and cardiovascular health. However, because MeHg and PUFA generally act on these same end points, disentangling risk and benefit is challenging.Objectives: We propose an approach for balancing risk and benefit that is based on the use of statistically dissociated measures of risk and benefit.Discussion: Because of mutual coexposure of MeHg and PUFAs in population-based studies and their opposite effect on many of the same end points, MeHg risk and PUFA benefit are tightly linked statistically, which results in mutual (negative) confounding. Thus, neither MeHg risk nor PUFA benefit can be accurately quantified without taking the other into account. A statistical approach that generates unconfounded risk and benefit coefficients for each end point can permit their subsequent recombination to describe the overall risk–benefit profile of each species of fish or fish diet. However, it appears that some end points may be adversely affected by MeHg without experiencing counterbalancing benefit from PUFAs. Such end points may drive consumption advisories and may preclude balancing of risk and benefit on the basis of other end points.Conclusions: Our thinking about fish consumption advisories now recognizes the need to balance risk and benefit. However, although statistical analysis of the appropriate data can eliminate mutual confounding, care is required to address the most sensitive end points that may be sensitive to risk and not benefit.

Sulfur in the South Florida Ecosystem: Distribution, Sources, Biogeochemistry, Impacts, and Management for Restoration

Sulfur is broadly recognized as a water quality issue of significance for the freshwater Florida Everglades. Roughly 60% of the remnant Everglades has surface water sulfate concentrations above 1 mg l−1, a restoration performance measure based on present sulfate levels in unenriched areas. Highly enriched marshes in the northern Everglades have average sulfate levels of 60 mg l−1. Sulfate loading to the Everglades is principally a result of land and water management in South Florida. The highest concentrations of sulfate (average 60–70 mg l−1) in the ecosystem are in canal water in the Everglades Agricultural Area (EAA). Potential sulfur sources in the watershed are many, but geochemical data and a preliminary sulfur mass balance for the EAA are consistent with sulfur presently used in agricultural, and sulfur released by oxidation of organic EAA soils (including legacy agricultural applications and natural sulfur) as the primary sources of sulfate enrichment in the EAA canals. Sulfate loading to the Everglades increases microbial sulfate reduction in soils, leading to more reducing conditions, greater cycling of nutrients in soils, production of toxic sulfide, and enhanced methylmercury (MeHg) production and bioaccumulation. Wetlands are zones of naturally high MeHg production, but the combination of high atmospheric mercury deposition rates in South Florida and elevated sulfate loading leads to increased MeHg production and MeHg risk to Everglades wildlife and human consumers. Sulfate from the EAA drainage canals penetrates deep into the Everglades Water Conservation Areas, and may extend into Everglades National Park. Present plans to restore sheet flow and to deliver more water to the Everglades may increase overall sulfur loads to the ecosystem, and move sulfate-enriched water further south. However, water management practices that minimize soil drying and rewetting cycles can mitigate sulfate release during soil oxidation. A comprehensive Everglades restoration strategy should include reduction of sulfur loads as a goal because of the many detrimental impacts of sulfate on the ecosystem. Monitoring data show that the ecosystem response to changes in sulfate levels is rapid, and strategies for reducing sulfate loading may be effective in the near term. A multifaceted approach employing best management practices for sulfur in agriculture, agricultural practices that minimize soil oxidation, and changes to stormwater treatment areas that increase sulfate retention could help achieve reduced sulfate loads to the Everglades, with resulting benefits.

Marine fish food in the United States and methylmercury risk

This paper takes a market-oriented approach to study potential exposure of methylmercury (MeHg) risk to human health from US domestic commercial ocean fish landings (consumption). Information is assembled on MeHg concentration levels of marine species. Landings were examined for 1995–2005. Confined to this seafood source, trends of landings indicating high concentration species (above 0.7 ppm, tilefish, shark, king mackerel and swordfish) were significantly decreased. People bought stable amount of medium MeHg level species (0.3–0.7 ppm, grouper, Spanish mackerel) but less amount of low concentration level species (below 0.3 ppm, catfish, tuna and southern flounder). Based on estimated prices of species and quantities taken it is found that consumers, one crucial link of the entire MeHg risk assessment process, had exhibited awareness of potential MeHg risk in fish and demonstrated in household fish consumption. Information assembled in this paper is insufficient to draw further inference on specific population cohorts more susceptible to potential exposure of MeHg risk. This inquiry may be extended to imported fish in the US for comparison.