MeHg Bioavailability Research Articles

Biochar amendment to further reduce methylmercury accumulation in rice grown in selenium-amended paddy soil.

Methylmercury (MeHg) accumulation in rice is an emerging food safety issue in China and other countries; however, mitigation methods are scarce. Here, the effects of selenium (Se) and multiple applications of Se and biochar on rice MeHg bioaccumulation were investigated using pot and microcosm experiments. We report that Se amendment was still effective in reducing MeHg levels in paddy soil and rice grain after three years of aging. Biochar amendment (0.5% w/w) further decreased grain (brown rice) MeHg levels by 82-87%. The grain MeHg level decrease following the combination of Se and biochar amendment could be partly attributed to inhibition of net MeHg production in soil by Se. In addition, biochar decreased not only net MeHg production but also MeHg bioavailability in the soil, which could be due to organosulfur compounds in the biochar. Our findings suggest that multiple applications of Se and biochar could be a novel remediation strategy to mitigate MeHg accumulation in rice.

Effects of geography and species variation on selenium and mercury molar ratios in Northeast Atlantic marine fish communities

Methylmercury (MeHg) is a potent neurotoxin that bioaccumulates in seafood. Co-occurrence of selenium (Se) may affect the bioavailability and toxicity of MeHg in organisms. Here we report the concentrations of total mercury (Hg) and Se in 17 teleost fish species (n = 8459) sampled during 2006–2015 from the North East Atlantic Ocean (NEAO) and evaluate species variation and effects of geography. Mean Hg concentration ranged from 0.04 mg kg−1 ww in Atlantic mackerel (Scomber scombrus) and blue whiting (Micromesistius poutassou) to 0.72 mg kg−1 ww in blue ling (Molva dypterygia). Se concentrations were less variable and ranged from 0.27 mg kg−1 ww in Atlantic cod (Gadus morhua) to 0.56 mg kg−1 ww in redfish (Sebastes spp.). The mean Se:Hg molar ratio ranged from 1.9 in blue ling to 43.3 in mackerel. Pelagic species had the lowest Hg concentrations and the highest Se:Hg ratios, whereas demersal species had the highest Hg concentrations and the lowest Se:Hg ratios. Se and Hg concentrations were positively correlated in 13 of the 17 species. Hg concentrations increased from the North to South in contrast to the Se:Hg molar ratio which exhibited the opposite trend. Fish from fjord and coastal areas had higher concentrations of Hg and lower Se:Hg molar ratios compared to fish sampled offshore. All species had average Se:Hg molar ratios >1 and Hg concentrations were largely below the EU maximum level of 0.5 mg kg−1 ww with few exceptions including the deep water species tusk (Brosme brosme) and blue ling sampled from fjord and coastal habitats. Our results show that two fillet servings of tusk, blue ling or Atlantic halibut (Hippoglossus hippoglossus) exceeded the tolerable weekly intake of MeHg although the surplus Se may possibly ameliorate the toxic effects of MeHg. However, some individuals with selenium deficiencies may exhibit greater sensitivity to MeHg.

Spatial and taxonomic variation of mercury concentration in low trophic level fauna from the Mediterranean Sea.

Studies of mercury (Hg) in the Mediterranean Sea have focused on pollution sources, air-sea mercury exchange, abiotic mercury cycling, and seafood. Much less is known about methylmercury (MeHg) concentrations in the lower food web. Zooplankton and small fish were sampled from the neuston layer at both coastal and open sea stations in the Mediterranean Sea during three cruise campaigns undertaken in the fall of 2011 and the summers of 2012 and 2013. Zooplankton and small fish were sorted by morphospecies, and the most abundant taxa (e.g. euphausiids, isopods, hyperiid amphipods) analyzed for methylmercury (MeHg) concentration. Unfiltered water samples were taken during the 2011 and 2012 cruises and analyzed for MeHg concentration. Multiple taxa suggested elevated MeHg concentrations in the Tyrrhenian and Balearic Seas in comparison with more eastern and western stations in the Mediterranean Sea. Spatial variation in zooplankton MeHg concentration is positively correlated with single time point whole water MeHg concentration for euphausiids and mysids and negatively correlated with maximum chlorophyll a concentration for euphausiids, mysids, and "smelt" fish. Taxonomic variation in MeHg concentration appears driven by taxonomic grouping and feeding mode. Euphausiids, due to their abundance, relative larger size, importance as a food source for other fauna, and observed relationship with surface water MeHg are a good candidate biotic group to evaluate for use in monitoring the bioavailability of MeHg for trophic transfer in the Mediterranean and potentially globally.

Distribution and biogeochemical controls on net methylmercury production in Penobscot River marshes and sediment

The distribution of mercury and methylmercury (MeHg) in sediment, mudflats, and marsh soils of the Hg-contaminated tidal Penobscot River was investigated, along with biogeochemical controls on production. Average total Hg in surface samples (0–3 cm) ranged from 100 to 1200 ng/g; average MeHg ranged from 5 to 50 ng/g. MeHg was usually highest at or near the surface except in highly mobile mudflats. Although total Hg concentrations in the Penobscot are elevated, it is the accumulation of MeHg that stands out in comparison to other ecosystems. Surface soils in the large Mendall Marsh, about 17 km downstream from the contamination source, contained particularly high %MeHg (averaging 8%). In Mendall marsh soil porewaters, MeHg often accounted for more than half of total Hg.Salt marshes are areas of particular concern in the Penobscot River, for they are depositional environments for a Hg-contaminated mobile pool of river sediment, hot spots for net MeHg production, and sources of risk to marsh animals. We hypothesized that exceptionally low mercury partitioning between the solid and aqueous phases (with log Kd averaging ~4.5) drives high MeHg in Penobscot marshes. The co-occurrence of iron and sulfide in filtered soil porewaters, sometimes both above 100 μM, suggests the presence of nanoparticulate and/or colloidal metal sulfides. These colloids may be stabilized by high concentrations of aromatic and potentially sulfurized dissolved organic matter (DOM) in marsh soils. Thus, Hg in Penobscot marsh soils appears to be in a highly available for microbial methylation through the formation of DOM-associated HgS complexes. Additionally, low partitioning of MeHg to marsh soils suggests high MeHg bioavailability to animals. Overall, drivers of high MeHg in Penobscot marshes include elevated Hg in soils, low partitioning of Hg to solids, high Hg bioavailability for methylation, rapidly shifting redox conditions in surface marsh soils, and high rates of microbial activity.

Methylmercury Biogeochemistry in Freshwater Ecosystems: A Review Focusing on DOM and Photodemethylation.

Mercury contamination is a growing concern for freshwater food webs in ecosystems without point sources of mercury. Methylmercury (MeHg) is of particular concern, as this is the form of mercury that crosses the blood-brain barrier and is neurotoxic to organisms. Wetlands and benthic sediments have high organic content and low oxygen availability. Anaerobic bacteria drive the metabolic function in these ecosystems and subsequently can methylate mercury. The bioavailability of MeHg is controlled by physicochemical characteristics such as pH, binding affinities, and dissolved organic matter (DOM). Similarly, photodemethylation is influenced by similar characteristics and thereby the two processes should be studied in tandem. The degradation of MeHg through photochemistry is an effective destruction mechanism in freshwater lakes. This review will highlight the uncertainties and known effects of DOM on subsequent photoreactions that lead to the occurrence of mercury photodemethylation and reduction in mercury bioavailability in freshwater ecosystems.

Cellular toxicity pathways of inorganic and methyl mercury in the green microalga Chlamydomonas reinhardtii

Contamination by mercury (Hg) is a worldwide concern because of Hg toxicity and biomagnification in aquatic food webs. Nevertheless, bioavailability and cellular toxicity pathways of inorganic (IHg) and methyl-Hg (MeHg) remain poorly understood. We analyzed the uptake, transcriptomic, and physiological responses in the microalga Chlamydomonas reinhardtii exposed to IHg or MeHg. Bioavailability of MeHg was up to 27× higher than for IHg. Genes involved in cell processes, energy metabolism and transport were dysregulated by both Hg species. Physiological analysis revealed an impact on photosynthesis and reduction–oxidation reaction metabolism. Nevertheless, MeHg dysregulated a larger number of genes and with a stronger fold-change than IHg at equivalent intracellular concentration. Analysis of the perturbations of the cell’s functions helped to derive a detailed mechanistic understanding of differences in cellular handling of IHg and MeHg resulting in MeHg having a stronger impact. This knowledge is central for the prediction of impact of toxicants on organisms.

Impact of macrozoobenthic bioturbation and wind fluctuation interactions on net methylmercury in freshwater lakes

The methylmercury (MeHg) as the toxic fractions has presented significant threats to biota in freshwater ecosystems. Hg methylation process is demonstrated to be manipulated by biota process (benthic disturbance and algae bloom existence) as well as the abiotic influence (wind fluctuation and illumination intensity) in freshwater ecosystems. However, the mechanisms influencing Hg methylation are still unclear, and the coupled influences of the biotic and abiotic process with the shifts in variation on methylmercury remain unexplored. Accordingly, an annular flume experiment which simulated the freshwater ecosystem, was conducted for 108 days to examine the influences of typical disturbance by chironomid larvae and wind fluctuations on MeHg variation in sediment profiles. The in-situ, passive sampler technique of revealing diffusive gradients in thin films (DGT) encompassed the special resin, based on referenced extraction and coloration-computer imaging densitometry, were employed to obtain labile MeHg, Fe, and S concentrations at high resolution. The results indicate that larval bioturbation during the initial period of the experiment could diminish bioavailable MeHg concentrations and change the diffusion direction of MeHg fluxes. However, this inhibitive effect on MeHg concentrations ceased with larvae eclosion. Compared to bioturbation, wind fluctuation exerted slow but sustained inhibition on MeHg release. Furthermore, the eight parameters (dissolved organic carbon (DOC), DO, labile Fe and S concentrations, pH, sulfate-reducing bacteria (SRB) abundance in sediment, oxidation-reduction potential (ORP) and EC) could explain more of variation in MeHg concentrations which indicated by the canonical correspondence analysis. And these eight parameters manifest higher explanatory power for MeHg distributed in newly formed sediment. More notably, the comparison results of the multiple and simple regression directly demonstrated the DOC was the fundamental and robust factor to control the MeHg variation in the freshwater ecosystem.

Bioaccumulation of mercury in invertebrate food webs of Canadian Rocky Mountain streams

AbstractMethylmercury (MeHg) is a contaminant of concern because of its ability to biomagnify in aquatic food webs, resulting in potentially harmful concentrations in higher consumers. Beaver impoundments in the southern Canadian Rockies release bioavailable MeHg to downstream food webs. We examined the magnitude of uptake and trophic transfer of exported Hg (total Hg [THg] and MeHg) to grazing and predatory invertebrates and controls on these transfers by site-specific (dissolved organic C [DOC], MeHg in water, MeHg in diet) and individual (body size, trophic level) variables. Bioconcentration factors (BCFs) were high (79,756 ± 68,204) relative to values from the literature, declined with increasing MeHg in water, and did not differ above and below beaver ponds. Biomagnification factors (BMFs) for uptake from periphyton to grazers (18.3 ± 11.7) were high and increased with increasing DOC, BMFs from grazers to predators (2.1 ± 1.2) were low, and neither of these BMFs differed above and below ponds. Invert...

Dissolved organic carbon modulates mercury concentrations in insect subsidies from streams to terrestrial consumers.

Mercury (Hg) concentrations in aquatic environments have increased globally, exposing consumers of aquatic organisms to high Hg levels. For both aquatic and terrestrial consumers, exposure to Hg depends on their food sources as well as environmental factors influencing Hg bioavailability. The majority of the research on the transfer of methylmercury (MeHg), a toxic and bioaccumulating form of Hg, between aquatic and terrestrial food webs has focused on terrestrial piscivores. However, a gap exists in our understanding of the factors regulating MeHg bioaccumulation by non-piscivorous terrestrial predators, specifically consumers of adult aquatic insects. Because dissolved organic carbon (DOC) binds tightly to MeHg, affecting its transport and availability in aquatic food webs, we hypothesized that DOC affects MeHg transfer from stream food webs to terrestrial predators feeding on emerging adult insects. We tested this hypothesis by collecting data over 2years from 10 low-order streams spanning a broad DOC gradient in the Lake Sunapee watershed in New Hampshire, USA. We found that streamwater MeHg concentration increased linearly with DOC concentration. However, streams with the highest DOC concentrations had emerging stream prey and spiders with lower MeHg concentrations than streams with intermediate DOC concentrations; a pattern that is similar to fish and larval aquatic insects. Furthermore, high MeHg concentrations found in spiders show that MeHg transfer in adult aquatic insects is an overlooked but potentially significant pathway of MeHg bioaccumulation in terrestrial food webs. Our results suggest that although MeHg in water increases with DOC, MeHg concentrations in stream and terrestrial consumers did not consistently increase with increases in streamwater MeHg concentrations. In fact, there was a change from a positive to a negative relationship between aqueous exposure and bioaccumulation at streamwater MeHg concentrations associated with DOC above ~5mg/L. Thus, our study highlights the importance of stream DOC for MeHg dynamics beyond stream boundaries, and shows that factors modulating MeHg bioavailability in aquatic systems can affect the transfer of MeHg to terrestrial predators via aquatic subsidies.

Bioaccessibility and bioavailability of methylmercury from seafood commonly consumed in North America: In vitro and epidemiological studies

Methylmercury (MeHg) is a global contaminant of concern and human exposures are largely realized via seafood consumption. While it is assumed that 95–100% of the ingested MeHg from seafood reaches systemic circulation, recent in vitro studies have yielded results to suggest otherwise. Of the published studies to have characterized the bioaccessibility or bioavailability of MeHg from seafood, only a handful of seafood species have been characterized, there exists tremendous variability in data within and across species, few species of relevance to North America have been studied, and none of the in vitro studies have adapted results to an epidemiology study. The objective of the current study was two-fold: (a) to characterize in vitro MeHg bioaccessibility and bioavailability from ten commonly consumed types of seafood in North America; and (b) to apply the bioaccessibility and bioavailability data from the in vitro study to an existing human MeHg exposure assessment study. Raw seafood samples (cod, crab, halibut, salmon, scallop, shrimp, tilapia, and three tuna types: canned light, canned white, fresh) were purchased in Montreal and their MeHg concentrations generally overlapped with values reported elsewhere. The bioaccessibility of MeHg from these samples ranged from 50.1±19.2 (canned white tuna) to 100% (shrimp and scallop) of the amount measured in the raw undigested sample. The bioavailability of MeHg from these samples ranged from 29.3±10.4 (crab) to 67.4±9.7% (salmon) of the value measured in the raw undigested sample. There were significant correlations between the initial MeHg concentration in seafood with the percent of that Hg that was bioaccessible (r=−0.476) and bioavailable (r=−0.294). When the in vitro data were applied to an existing MeHg exposure assessment study, the estimated amount of MeHg absorbed into systemic circulation decreased by 25% and 42% when considering bioaccessibility and bioavailability, respectively. When the in vitro data were integrated into a regression model relating dietary MeHg intake from seafood with hair and blood Hg biomarkers, there were no differences in key model parameters when comparing the default model (that assumes 100% bioavailability) with models adjusted for the in vitro bioaccessibility and bioavailability data. In conclusion this work adds to a growing number of studies that together suggest that MeHg bioavailability from seafood may be less than 100%, but also documents the challenges when integrating such in vitro data into human exposure and risk assessments.

Managing Swedish forestry's impact on mercury in fish: Defining the impact and mitigation measures.

Inputs of anthropogenic mercury (Hg) to the environment have led to accumulation of Hg in terrestrial and aquatic ecosystems, contributing to fish Hg concentrations well above the European Union standards in large parts of Fennoscandia. Forestry operations have been reported to increase the concentrations and loads of Hg to surface waters by mobilizing Hg from the soil. This summary of available forestry effect studies reveals considerable variation in treatment effects on total Hg (THg) and methylmercury (MeHg) at different sites, varying from no effect up to manifold concentration increases, especially for the bioavailable MeHg fraction. Since Hg biomagnification depends on trophic structures, forestry impacts on nutrient flows will also influence the Hg in fish. From this, we conclude that recommendations for best management practices in Swedish forestry operations are appropriate from the perspective of mercury contamination. However, the complexity of defining effective policies needs to be recognized.

The effect of aqueous speciation and cellular ligand binding on the biotransformation and bioavailability of methylmercury in mercury-resistant bacteria

Mercury resistant bacteria play a critical role in mercury biogeochemical cycling in that they convert methylmercury (MeHg) and inorganic mercury to elemental mercury, Hg(0). To date there are very few studies on the effects of speciation and bioavailability of MeHg in these organisms, and even fewer studies on the role that binding to cellular ligands plays on MeHg uptake. The objective of this study was to investigate the effects of thiol complexation on the uptake of MeHg by measuring the intracellular demethylation-reduction (transformation) of MeHg to Hg(0) in Hg-resistant bacteria. Short-term intracellular transformation of MeHg was quantified by monitoring the loss of volatile Hg(0) generated during incubations of bacteria containing the complete mer operon (including genes from putative mercury transporters) exposed to MeHg in minimal media compared to negative controls with non-mer or heat-killed cells. The results indicate that the complexes MeHgOH, MeHg-cysteine, and MeHg-glutathione are all bioavailable in these bacteria, and without the mer operon there is very little biological degradation of MeHg. In both Pseudomonas stutzeri and Escherichia coli, there was a pool of MeHg that was not transformed to elemental Hg(0), which was likely rendered unavailable to Mer enzymes by non-specific binding to cellular ligands. Since the rates of MeHg accumulation and transformation varied more between the two species of bacteria examined than among MeHg complexes, microbial bioavailability, and therefore microbial demethylation, of MeHg in aquatic systems likely depends more on the species of microorganism than on the types and relative concentrations of thiols or other MeHg ligands present.

Diffusive gradients in thin films for predicting methylmercury bioavailability in freshwaters after photodegradation

Determination of the dissolved-bioavailable fraction of methylmercury (MeHg) and its degradation pathways in freshwaters deserve attention, to further our understanding of the potential risk and toxicity of MeHg. Since the photodegradation of MeHg is the most important known abiotic process able to demethylate MeHg, this study investigated the role of sunlight on MeHg bioavailability in freshwater environments. Experiments to calculate photodegradation rate constants of MeHg in different types of freshwater in combination with experiments to distinguish the labile fraction of MeHg after being exposed to sunlight were performed. The ability of diffusive gradients in thin films based on polyacrylamide (P-DGT) to assess DGT-labile MeHg during photodegradation was successfully tested. First order photodegradation rate constants (kpd) of bioavailable MeHg determined in five different types of waters with different amount of dissolved organic matter (DOM), were in the range 0.073–0.254h−1, confirming previous findings that once there is DOM in solution, which would favour the photodegradation process, the kpd is mainly affected by light attenuation. Simulated sunlight seems not to alter the lability of MeHg, although photodegradation processes may decrease the concentrations of MeHg, contributing to reduce the amount of bioavailable MeHg (i.e. MeHg uptake by DGT). However, the quality of DOM, rather than the quantity, plays an important role in the bioavailability of MeHg in freshwater.

Influence of soil mercury concentration and fraction on bioaccumulation process of inorganic mercury and methylmercury in rice (Oryza sativa L.).

Recent studies showed that rice is the major pathway for methylmercury (MeHg) exposure to inhabitants in mercury (Hg) mining areas in China. There is, therefore, a concern regarding accumulation of Hg in rice grown in soils with high Hg concentrations. A soil pot experimental study was conducted to investigate the effects of Hg-contaminated soil on the growth of rice and uptake and speciation of Hg in the rice. Our results imply that the growth of rice promotes residual fraction of Hg transforming to organic-bound fraction in soil and increased the potential risks of MeHg production. Bioaccumulation factors deceased for IHg but relatively stabilized for MeHg with soil total mercury (THg) increasing. IHg in soil was the major source of Hg in the root and stalk, but leaf was contributed by Hg from both atmosphere and soil. Soluble and exchangeable Hg fraction can predict the bioavailability of IHg and MeHg in soils, and that can provide quantitative description of the rate of uptake of the bioavailable Hg. Soluble and exchangeable Hg fraction in paddy soil exceeding 0.0087 mg kg(-1) may cause THg concentration in rice grain above the permissible limit standard, and MeHg concentration in paddy soil more than 0.0091 mg kg(-1) may have the health risks to humans.

Application of stable isotope mixing models for defining trophic biomagnification pathways of mercury and selenium

Trophic models based on nitrogen stable isotope ratios (δ15N) have been shown to predict changes in mercury (Hg) concentrations in fish; however, they are usually applied at the ecosystem scale and are rarely directed at known trophic pathways. We discuss a novel approach in which we combined gut contents analysis and stable isotope analyses (δ15N and δ13C) into a Bayesian isotopic mixing model to provide a quantitative estimate of Hg and selenium (Se) biomagnification in an estuarine food web. Estimates of the relationship between total mercury (THg) and methylmercury (MeHg) were significantly improved in mixing model‐adjusted food webs over models that included all known prey sources. Spatial differences in dietary composition and MeHg bioavailability offer strong evidence that local food webs can have a significant effect on the biomagnification of Hg within benthic fish species. While no evidence of Se biomagnification was found, lower Se : Hg ratios at higher trophic levels could be attributed to increasing trophic Hg concentration. Furthermore, stable isotope analysis suggested Hg and Se biotransfer from benthic sources to fish. Overall, the findings highlight that isotope mixing models can be a significant aid in assessments of contaminant biomagnification, particularly when it is important to define food pathways to top predators.

Complex patterns in fish – sediment mercury concentrations in a contaminated estuary: The influence of selenium co-contamination?

Environmental mercury (Hg) loads do not always correspond to Hg concentrations in resident fish and selenium (Se) presence has been reported to play a pivotal role in mitigating Hg bioaccumulation. Total mercury (THg), methylmercury (MeHg) and Se concentrations were measured in sediments and a benthic fish species (Platycephalus bassensis) from a contaminated estuary (Derwent Estuary, Tasmania). Elevated sediment concentrations of Se did not result in increased Se concentrations in fish, but low concentrations of Se were associated with increased MeHg bioavailability (% MeHg) from sediments to fish. Where MeHg (≈99% of total Hg) concentration in fish was high Se uptake also increased, indicating that maintaining positive Se:Hg ratios may reduce the toxicity of MeHg. MeHg was detectable in sediments throughout the estuary, and a molar excess of THg over Se suggested that there was insufficient Se to prevent methylation from the sediments. Se:Hg ratios of less than 1.0 in sediments, coupled with high %MeHg fraction and high biotic sediment accumulation factors for MeHg (BSAFMeHg), indicated that the lower region of the Derwent Estuary could be a hotspot for Hg methylation, despite having significantly lower THg concentrations. In contrast, Hg bioavailability to fish from sediments close to the source may be reduced by both inorganic Hg species complexation and lower methylation rates. There was a strong association between THg and Se in estuarine sediments, suggesting that Se plays an important role in sediment Hg cycling and should be a key consideration in any future assessments of Hg methylation, bioavailability and bioaccumulation.

Methylmercury Accumulation in Rice Grain (Oryza sativaL.): Environment and Genotype Controls

In 2010, 50 indica rice varieties were cultivated in three sites in southwestern China along a contamination gradient (background, moderately-contaminated and highly-contaminated sites) to determine environment and genotype controls on MeHg accumulation in polished white rice and bran. Rice grain MeHg concentrations were significantly higher in the moderately-contaminated site compared to the other two sites (ANOVA, p<0.0001). Lower rice grain MeHg concentrations in the highly-contaminated site possibly reflected differences in surface water pH (highly-contaminated site: pH 11, other two sites: pH 7.6-8.0). More alkaline conditions at the highly-contaminated site possibly decreased the bioavailability of MeHg and/or other trace elements, thus lowering the uptake of MeHg from paddy soil to rice grain. Polished white rice MeHg concentrations were significantly associated with rice genotype (p<0001), indicating there may be genetic markers associated with the translocation of MeHg from the maternal tissue to the filial tissue (i.e., from the bran to the polished grain). Additionally, low MeHg-accumulating rice varieties were identified, which decreased MeHg exposure up to 69%, and may be recommended to farmers to mitigate MeHg accumulation in rice grain.

Prediction of Methyl Mercury Uptake by Rice Plants (Oryza sativa L.) Using the Diffusive Gradient in Thin Films Technique

Rice consumption is the primary pathway for methyl mercury (MeHg) exposure at inland mercury (Hg) mining areas of SW China. Mechanistic information on MeHg accumulation in rice is, however, limited. The process of MeHg exchange between paddy soil and rice plants predominantly occurs in pore water. The detection of bioavailable MeHg in pore water is therefore important to predict MeHg uptake by rice plants ( Oryza sativa L.). This study investigated MeHg dynamics and spatial MeHg trends in pore water during the rice growing season using the diffusive gradient in thin films (DGT) technique and tested the ability of DGT to predict MeHg uptake by rice. The MeHg uptake flux from soil to rice plants via roots was significantly correlated with the DGT-measured MeHg flux (R = 0.853, p < 0.01). Our study implies that DGT can predict the bioavailability of MeHg in rice paddy soil and that the DGT method can provide quantitative description of the rate of uptake of this bioavailable MeHg. The DGT technique is demonstrated as a useful indicator of the likely ecotoxicological risk that might be apparent where paddy rice is grown in MeHg contaminated soil.

Factors regulating the bioavailability of methylmercury to breeding rusty blackbirds in northeastern wetlands

Rusty blackbirds are undergoing rapid population decline and have elevated Hg concentrations while breeding in the Acadian ecoregion of North America. Factors regulating the bioavailability of methyl-Hg (MeHg) within this population's habitat were determined using water, invertebrates, and blood from adult rusty blackbirds collected for Hg-speciation, along with additional water column parameters: MeHg and THg, dissolved organic carbon, pH, dissolved oxygen, conductivity, redox potential, and temperature. Both DO2 and pH were negatively related to biota MeHg, while water MeHg concentrations were positively related. Both invertebrate MeHg concentration and %MeHg increased with trophic level. Invertebrate MeHg concentrations were among the greatest reported when compared with those reported elsewhere for wetlands and waterbodies—often several times greater for similar taxa—while percent MeHg of THg were similar. An environment with high bioavailability of MeHg in combination with a high trophic position best explains elevated Hg concentrations for this species regional population.

Influence of Dissolved Organic Carbon on Methylmercury Bioavailability across Minnesota Stream Ecosystems

Stream ecosystems are widely contaminated by mercury (Hg) via atmospheric transport and deposition in watersheds. Dissolved organic carbon (DOC) is well-known to be the dominant ligand for aqueous methylmercury (MeHg), the bioaccumulative form of Hg in aquatic food webs. However, it is less clear if and how the concentration and character (e.g., aromaticity) of DOC influences the availability of dissolved MeHg to stream food webs. In this work, we analyzed total-Hg and/or MeHg concentrations in water, seston, and macroinvertebrates (filter-feeding hydropsychid caddisflies), and other physiochemical properties in 30 streams along a south-north geographic gradient in eastern Minnesota that corresponds to substantial changes in dominant land cover (i.e., agriculture, urban, wetland, and forest). In general, MeHg concentrations in seston and hydropsychids were higher in watersheds with more forest and wetland coverage, and increased with dissolved MeHg concentration. However, we found that the efficiency of MeHg incorporation into the stream food webs (i.e., bioconcentration factors of MeHg in both seston and hydropsychids, BCF(MeHg) = solid MeHg ÷ dissolved MeHg) decreased significantly with DOC concentration and aromaticity, suggesting that MeHg bioavailability to the base of food webs was attenuated at higher levels of terrestrial DOC. Therefore, our findings suggest that there is a dual role of DOC on MeHg cycling in streams: terrestrial DOC acts as the primary carrier ligand of dissolved MeHg for transport into surface waters, yet this aromatic DOC also attenuates dissolved MeHg uptake by aquatic food webs. Thus, consideration of MeHg bioavailability and its environmental regulation could help improve predictive models of MeHg bioaccumulation in stream ecosystems.