Methylmercury Bioaccumulation Research Articles

Species-specific mercury speciation in billfishes and its implications for food safety monitoring and dietary advice.

Humans are exposed to toxic methylmercury mainly by consuming marine fish, in particular top predator species like billfishes or tunas. In seafood risk assessments, mercury is assumed to be mostly present as organic methylmercury in predatory fishes; yet high percentages of inorganic mercury were recently reported in marlins, suggesting markedly different methylmercury metabolism across species. We quantified total mercury and methylmercury concentrations in muscle of four billfish species from the Indian and the Pacific oceans to address this knowledge gap. We found low percentages of methylmercury in blue and black marlins (15±7%) compared to swordfish and striped marlin (89±13%), with no significant differences among ocean regions. This illustrates that billfishes exhibit species-specific methylmercury bioaccumulation patterns, likely related to unique selenium-dependent in vivo methylmercury demethylation capacities in muscle. Blue and black marlins therefore appeared generally safer for human consumption than swordfish and striped marlin regarding MeHg toxicological effects. Yet, no matter the species, the frequency of recommended weekly billfish meals decreased with increasing fish size, given that mercury naturally accumulates over time. When assessing potential risks of billfish consumption, we therefore recommend measuring methylmercury, rather than total mercury, and relying on a large number of samples to cover a broad range of fish sizes. This study calls for additional characterization of mercury speciation and bioavailability in billfishes to better understand the mechanisms driving species-specific differences of methylmercury detoxification, and to refine dietary advices associated to marine top predators consumption.

Construction of a triple-mode sensing platform for effective differentiation, speciation, and monitoring of mercury and methylmercury bioaccumulation in crayfish via cation exchange reaction

Developing rapid and sensitive methods for monitoring inorganic mercury (Hg2+) and methylmercury (CH3Hg+) in crayfish is crucial for understanding the environmental impact of these contaminants. In this work, a novel tri-mode strategy was developed for highly sensitive monitoring of Hg2+ and CH3Hg+ bioaccumulation in crayfish by inductively coupled plasma mass spectrometry (ICP-MS)/ fluorescence /smartphone colorimetric (RGB) analysis without chromatographic separation. Cation exchange reaction (CER) was performed between Hg2+ and luminescent CdTe quantum dots (QDs), while CH3Hg+ unrealizable CER. The CH3Hg+ can be transformed to Hg2+ by simple UV irradiation, speciation analysis can be realized by detecting the fluorescence of CdTe QDs after incubation by Hg2+ and total Hg2+. In addition, the filtration of reacted CdTe QDs was carried out, ICP-MS was performed to detect exchanged Cd2+ by Hg2+ and total Hg2+, as well the smartphone RGB analysis was performed for membrane colorimetry. The limits of detection (LODs) of Hg2+ and CH3Hg+ for ICP-MS, fluorescence, and colorimetric (RGB) modes were 0.03 ng mL−1, 18 ng mL−1, and 0.9 μg mL−1 respectively. Density Functional Theory (DFT) was employed to validate the mechanism of the CER reaction. CdTe QDs array analysis with five different ligands was performed to eliminate potential ion interferences of Ag+ and Cu2+ that could occur during the CER reaction. The well-designed system was successfully utilized for monitoring trace Hg2+ and CH3Hg+ in crayfish fed Hg2+ and CH3Hg+ contaminative food over a two-week “uptake” period and a three-week “depuration” period. The results indicated that the Hg2+ uptake in different tissues was significantly different from that of CH3Hg+ in all tissues. There was evidence of Hg uptake from water via leaching from food, although the principal source of uptake was from food.

Influence of genetic polymorphisms of Hg metabolism and DNA repair on the frequencies of micronuclei, nucleoplasmic bridges, and nuclear buds in communities living in gold mining areas

Fishing communities living near gold mining areas are at increased risk of mercury (Hg) exposure via bioaccumulation of methylmercury (MeHg) in fish. This exposure has been linked to health effects that may be triggered by genotoxic events. Genetic polymorphisms play a role in the risk associated with Hg exposure. This study evaluated the effect of single nucleotide polymorphisms (SNPs) in metabolic and DNA repair genes on genetic instability and total hair Hg (T-Hg) levels in 78 individuals from "La Mojana" in northern Colombia and 34 individuals from a reference area. Genetic instability was assessed by the frequency of micronuclei (MNBN), nuclear buds (NBUDS), and nucleoplasmic bridges (NPB). We used a Poisson regression to assess the influence of SNPs on T-Hg levels and genetic instability, and a Bayesian regression to examine the interaction between Hg detoxification and DNA repair. Among exposed individuals, carriers of XRCC1Arg399Gln had a significantly higher frequency of MNBN. Conversely, the XRCC1Arg194Trp and OGG1Ser326Cys polymorphisms were associated with lower frequencies of MNBN. XRCC1Arg399Gln, XRCC1Arg280His, and GSTM1Null carriers showed lower NPB frequencies. Our results also indicated that individuals with the GSTM1Nulland GSTT1null polymorphisms had a 1.6-fold risk for higher T-Hg levels. The Bayesian model showed increased MNBN frequencies in carriers of the GSTM1Null polymorphism in combination with XRCC1Arg399Gln and increased NBUDS frequencies in the GSTM1Null carriers with the XRCC3Thr241Met and OGG1Ser326Cys alleles. The GSTM1+ variant was found to be a protective factor in individuals carrying OGG1Ser326Cys (MNBN) and XRCC1Arg280His (NPB); the GSTT1+ polymorphism combined with XRCCArg194Trp also modulated lower MNBN frequencies, while GSTT1+ carriers with the XRCC1Arg399Gln allele showed lower NPB frequencies. Consistent with GSTM1, GSTT1Null carriers with XRCC3Thr241Met showed increased NBUDS frequency. With the rise of gold mining activities, these approaches are vital to identify and safeguard populations vulnerable to Hg's toxic effects.

Soil Geobacteraceae are the key predictors of neurotoxic methylmercury bioaccumulation in rice.

Contamination of rice by the potent neurotoxin methylmercury (MeHg) originates from microbe-mediated Hg methylation in soils. However, the high diversity of Hg methylating microorganisms in soils hinders the prediction of MeHg formation and challenges the mitigation of MeHg bioaccumulation via regulating soil microbiomes. Here we explored the roles of various cropland microbial communities in MeHg formation in the potentials leading to MeHg accumulation in rice and reveal that Geobacteraceae are the key predictors of MeHg bioaccumulation in paddy soil systems. We characterized Hg methylating microorganisms from 67 cropland ecosystems across 3,600 latitudinal kilometres. The simulations of a rice-paddy biogeochemical model show that MeHg accumulation in rice is 1.3-1.7-fold more sensitive to changes in the relative abundance of Geobacteraceae compared to Hg input, which is recognized as the primary parameter in controlling MeHg exposure. These findings open up a window to predict MeHg formation and accumulation in human food webs, enabling more efficient mitigation of risks to human health through regulations of key soil microbiomes.

Suppression of mercury methylation in soil and methylmercury accumulation in rice by dissolved organic matter derived from sulfur-rich rape straw

Straw amendment significantly enhances mercury (Hg) methylation and subsequent methylmercury (MeHg) bioaccumulation in Hg-contaminated paddy fields by releasing dissolved organic matter (DOM). This study comprehensively investigates the regulatory mechanisms of DOM and its different molecular weights derived from sulfur-rich rape straw (RaDOM) and composted rape straw (CRaDOM) applied in the rice-filling stage on soil MeHg production and subsequent bioaccumulation in rice grains. The results indicated that the amendment of RaDOM and CRaDOM significantly reduced soil MeHg content by 42.40–62.42%. This reduction can be attributed to several factors, including the suppression of Hg-methylating bacteria in soil, the supply of sulfate from RaDOM and CRaDOM, and the increase in the humification, molecular weight, and humic-like fractions of soil DOM. Additionally, adding RaDOM increased the MeHg bioaccumulation factor in roots by 27.55% while inhibiting MeHg transportation by 12.24% and ultimately reducing MeHg content in grains by 21.24% compared to the control group. Similarly, CRaDOM enhanced MeHg accumulation by 25.19%, suppressed MeHg transportation by 39.65%, and reduced MeHg levels in the grains by 27.94%. The assimilation of sulfate derived from RaDOM and CRaDOM into glutathione may be responsible for the increased retention of MeHg in the roots. Over the three days, there was a significant decrease in soil MeHg content as the molecular weight of RaDOM increased; conversely, altering the molecular weight of CRaDOM demonstrated an inverse trend. However, this pattern was not observed after 12 days. Applying sulfur-rich rape DOM can help mitigate MeHg accumulation in paddy fields by regulating the quality of soil DOM, sulfur cycling, and Hg-methylating bacteria.

Optimized mercury speciation analysis using LC-ICP-MS and microwave assisted extraction for precise determination of methylmercury in fish, rice and soil

Mercury (Hg) is a toxic element that exists in various forms, each with its characteristics and impacts on the environment. Methylmercury (MeHg) bioaccumulates in the food chain and identifying mercury species is crucial to assessing risks to ecology and health. Therefore, accurate, sensitive, and broad-range analytical methods are essential for the determination of methylmercury. This study optimized and validated a procedure for Hg speciation analysis in rice, fish, and soil using different extractants, followed by liquid chromatography inductively-coupled plasma mass spectrometry (LC ICP-MS) using certified references. Microwave-assisted extraction (MAE) parameters were optimized using 25 % KOH, resulting in improved sensitivity, accuracy and processing time. The validated method achieved a limit of quantitation (LOQ) of 12 µg kg−1 and showed acceptable percentage recoveries (75.3–98.1 %) in all matrices, enabling precise determination of MeHg (%RSDr; 3.76–5.78, %RSDR; 2.34–6.75) and Hg in a large number of samples within a short time frame. The validated method is particularly well-suited for rice, followed by fish and then soil. Therefore, the method utilizing microwave-assisted extraction and LC ICP-MS ensures precise methylmercury determination in rice, fish, and soil, crucial for evaluating environmental and health risks associated with mercury bioaccumulation.

Dissolved organic matter thiol concentrations determine methylmercury bioavailability across the terrestrial-marine aquatic continuum

The most critical step for methylmercury (MeHg) bioaccumulation in aquatic food webs is phytoplankton uptake of dissolved MeHg. Dissolved organic matter (DOM) has been known to influence MeHg uptake, but the mechanisms have remained unclear. Here we show that the concentration of DOM-associated thiol functional groups (DOM-RSH) varies substantially across contrasting aquatic systems and dictates MeHg speciation and bioavailability to phytoplankton. Across our 20 study sites, DOM-RSH concentrations decrease 40-fold from terrestrial to marine environments whereas dissolved organic carbon (DOC), the typical proxy for MeHg binding sites in DOM, only has a 5-fold decrease. MeHg accumulation into phytoplankton is shown to be directly linked to the concentration of specific MeHg binding sites (DOM-RSH), rather than DOC. Therefore, MeHg bioavailability increases systematically across the terrestrial-marine aquatic continuum as the DOM-RSH concentration decreases. Our results strongly suggest that measuring DOM-RSH concentrations will improve empirical models in phytoplankton uptake studies and will form a refined basis for modeling MeHg incorporation in aquatic food webs under various environmental conditions.

Ecology and environmental characteristics influence methylmercury bioaccumulation in coastal invertebrates

Quantifying mercury (Hg) concentrations in invertebrates is fundamental to determining risk for bioaccumulation in higher trophic level organisms in coastal food webs. Bioaccumulation is influenced by local mercury concentrations, site geochemistry, individual feeding ecologies, and trophic position. We sampled seven species of invertebrates from five coastal sites in the Minas Basin, Bay of Fundy, and determined body concentrations of methylmercury (MeHg), total mercury (THg), and stable isotopes of nitrogen (δ15N) and carbon (δ13C). To evaluate the effects of environmental chemistry on Hg production and bioaccumulation, bulk sediments from all sites were analysed for THg, %Loss on ignition (LOI) (carbon), and sulfur isotopes (δ34S), and concentrations of MeHg, Total Organic Carbon (TOC), sulfate, and sulfide were measured in porewaters. The mean concentration of MeHg in tissues for all invertebrates sampled was 10.03 ± 7.04 ng g−1). MeHg in porewater (mean = 0.22–1.59 ng L−1) was the strongest predictor of invertebrate MeHg, but sediment δ34S (−0.80–14.1‰) was also a relatively strong predictor. δ34S in tissues (measured in three species; Corophium volutator, Ilyanassa obsoleta, and Littorina littorea) were positively related to MeHg in invertebrates (r = 0.55, 0.22, and 0.71 respectively), and when used in combination with δ15N and δ13C values improved predictions of Hg concentrations in biota. Hg concentrations in the amphipod Corophium volutator (mean MeHg = 10.60 ± 1.90 ng g−1) were particularly well predicted using porewater and sediment chemistry, highlighting this species as a useful bioindicator of Hg contamination in sediments of the Bay of Fundy.

Salinity and total suspended solids control mercury speciation in a tidal river: Comparisons with a photochemical mercury model

Daytime volatilization of gaseous elemental mercury (Hg(0)aq) is a significant mechanism for mercury removal from aquatic systems and potentially limits the production and bioaccumulation of methylmercury. Changes in incoming solar radiation (in the ultraviolet range), dissolved organic matter, salinity, and total suspended particles were investigated concurrently with several mercury species (Hg(0)aq, dissolved total mercury (THg), easily reducible mercury (ERM), and mercury associated with total suspended solids (THgTSS)) during daylight hours near the mouth of a hypertidal river. There were no predictable temporal changes observed for Hg(0)aq in unfiltered surface water. Hg(0)aq ranged from 0 to 12 pg L−1, THg ranged from 0 to 492 pg L−1, ERM ranged from 13 to 381 pg L−1, and THgTSS ranged from <1.58 ng g−1 to 261.32 ng g−1. The range of Hg(0)aq predicted by the empirical model was similar to measured ERM concentrations, but it was shown that ERM did not significantly predict in-situ photoreducible Hg(II) (Hg(II)RED). Production of Hg(0)aq appears to largely be suppressed by suspended solids, which limits ultraviolet radiation transmission through surface water. Comparison of these results to an empirical model developed for this site to predict Hg(0)aq indicates that significantly more mercury is available for photoreduction near the mouth of the tidal river, and that Hg(II) will likely photoreduce quickly when TSS levels decrease with ocean mixing.

Impacts of autochthonous dissolved organic matter on the accumulation of methylmercury by phytoplankton and zooplankton in a eutrophic coastal ecosystem

The bioaccumulation of methylmercury (MeHg) within the pelagic food webs is a crucial determinant of the MeHg concentration in the organisms at higher trophic levels. Dissolved organic matter (DOM) is recognized for its influence on mercury (Hg) cycling in the aquatic environment because of its role in providing metabolic substrate for heterotrophic organism and serving as a strong ligand for MeHg. However, the impact of DOM on MeHg bioaccumulation in pelagic food chains remain controversial. Here, we explored MeHg bioaccumulation within a pelagic food web in China, in the eutrophic Bohai Sea and adjacent seas, covering a range of DOM concentrations and compositions. Our findings show that elevated concentrations of dissolved organic carbon (DOC) and phytoplankton biomass may contribute to a reduction in MeHg uptake by phytoplankton. Moreover, we observe that a higher level of autochthonous DOM in the water may result in more significant MeHg biomagnification in zooplankton. This can be explained by alterations in the structure of pelagic food webs and/or an increase in the direct consumption of DOM and particulate organic matter (POM) containing MeHg. Our study offers direct field monitoring evidence of dual roles played by DOM in regulating MeHg transfers from water to phytoplankton and zooplankton in coastal pelagic food webs. A thorough understanding of the intricate interactions is essential for a more comprehensive evaluation of ecological risks associated with MeHg exposure in coastal ecosystems.

An examination of the factors influencing the bioaccumulation of methylmercury at the base of the estuarine food web

Estuarine systems have received ongoing mercury (Hg) inputs from both point sources and regional contamination and have high legacy Hg in sediments. This is an environmental concern given that coastal seafood is an important vector for human exposure to methylmercury (MeHg). The base of the food chain represents the most important trophic steps for MeHg bioaccumulation. The magnitude of the uptake by phytoplankton, and their consumers, is influenced by many factors, in addition to sediment and water MeHg concentrations, that impact MeHg assimilation into phytoplankton and the trophic transfer to higher trophic levels, both benthic and pelagic. For forage fish, such as mummichogs (Fundulus heteroclitus), abiotic and biotic (bioenergetic) factors can influence their MeHg content, and diet is also important as they feed both on benthic and pelagic prey. Given that the importance of sediment MeHg versus pelagic MeHg sources has been debated, we updated a phytoplankton bioaccumulation model, and coupled this with a bioaccumulation model for MeHg concentration in mummichog tissue to examine the controlling factors for sites, from Maine to Maryland, USA, ranging widely in their Hg concentrations and other variables. The study highlighted the importance of DOC in modulating uptake into the pelagic food web, but also demonstrated the importance of diet in controlling mummichog MeHg. Finally, the relative importance of MeHg source - sediment or water column – was correlated with the level of Hg contamination. Sediment-derived MeHg was a more important source for highly Hg contaminated systems. As water column and sediment MeHg are not strongly correlated for the studied ecosystems, their importance as a source of MeHg to mummichogs varies with location. The study highlights the differences across ecosystems in MeHg bioaccumulation pathways, and that uptake into phytoplankton is an important variable controlling forage fish concentration.

The Complex Interactions Between Sediment Geochemistry, Methylmercury Production, and Bioaccumulation in Intertidal Estuarine Ecosystems: A Focused Review.

Due to their natural geochemistry, intertidal estuarine ecosystems are vulnerable to bioaccumulation of methylmercury (MeHg), a neurotoxin that readily bioaccumulates in organisms. Determining MeHg concentrations in intertidal invertebrates at the base of the food web is crucial in determining MeHg exposure in higher trophic level organisms like fish and birds. The processes that govern the production of MeHg in coastal ecosystems are influenced by many geochemical factors including sulfur species, organic matter, and salinity. The interactions of these factors with mercury are complex, and a wide variety of results have been reported in the literature. This paper reviews conceptual models to better clarify the various geochemical and physical factors that impact MeHg production and bioavailability in intertidal ecosystems.

Total mercury and methylmercury concentrations in water hyacinth (Eichhornia crassipes) from a South Carolina coastal plain river

The Waccamaw River is located along the eastern coastline of South Carolina. Large areas of the shoreline contain water hyacinth (Eichhornia crassipes) mats. These plants trap organic matter, inhibit light and oxygen penetration into the water and serve as a substrate for bacterial colonization, which may be conducive to the formation of methylmercury. The purpose of this study was to quantify the amount of total and methylmercury in plants, water under the mats and surface water from an area adjacent to the mats. Concentrations of total and methylmercury and percentages of methylmercury in water samples ranged from 2.9 to 8.9 ng L−1, 0.2–2.5 ng L−1, and 9–31 %, respectively and were not significantly different between sites. Concentrations of total mercury in water hyacinth shoots and roots ranged from 2.2 to 58.7 ng g−1 dw and 29.7–71.9 ng g−1 dw, respectively. Methylmercury ranged from 0.84 to 2.24 ng g−1 dw (shoots) and from 8.95 to 37.1 ng g−1 dw (roots). Concentrations of total and methylmercury in the roots were significantly higher than the shoots. Percentages of methylmercury in the roots and shoots varied from 2 % to 63 % and were not significantly different. Total and methylmercury in one square meter of water hyacinth ranged from 8833–52,459 ng m−2 dw and from 2686–15,786 ng m−2 dw, respectively. These plants may represent another vector of methylmercury to aquatic food webs and contribute to the bioaccumulation of methylmercury in aquatic organisms.

Methylmercury bioaccumulation in water flea Daphnia carinata by AIEgen

Mercury ion (Hg2+) is a toxic heavy metal ion and Hg2+ is convertible to methylmercury (MeHg) by many aquatic microorganisms, leading to bioaccumulation and biomagnification in aquatic organisms, which can interfere with brain development and function in humans. This study employs a newly developed AIEgen (Aggregation-induced emission fluorogen) to quantify and visualise the process of MeHg bioaccumulation in vivo on the species of water flea Daphnia carinata. Two approaches to MeHg absorption were taken, either by direct incubation in a MeHg solution or by indirect consumption of algae contaminated with MeHg. We analysed the relationship between the ratio of photoluminescence (PL) intensities (I585/I480) and MeHg concentration (CMeHg) and generated a master curve for determining MeHg concentration based on the measurement of PL intensities. Fluorescent image analysis showed the occurrence of MeHg in D. carinata to be mainly in the compound eyes, optic nerve and carapace. This study indicates that MeHg absorption can be quantified and visualised in the body of zooplankton, and the MeHg transfer to zooplankton is more likely through direct exposure than via indirect food intake. The accumulation of MeHg in the eye and the nervous system could be the cause of the high mortality of D. carinata exposed to MeHg in water.

Plankton population dynamics and methylmercury bioaccumulation in the pelagic food web of mine-impacted surface water reservoirs

Thermal stratification of reservoirs can lead to anaerobic conditions that facilitate the microbial conversion of mercury (Hg) to neurotoxic and bioaccumulative methylmercury (MeHg). But MeHg production is just the first step in a complex set of processes that affect MeHg in fish. Of particular relevance is uptake into suspended particulate matter (SPM) and zooplankton at the base of the pelagic food web. We assessed plankton dynamics and Hg uptake into the pelagic food web of four Hg-impaired California water reservoirs. Combining water chemistry, plankton taxonomy, and stable carbon (C) and nitrogen (N) isotope values of SPM and zooplankton samples, we investigated differences among the reservoirs that may contribute to differing patterns in MeHg bioaccumulation. Methylmercury accumulated in SPM during the spring and summer seasons. Percent MeHg (MeHg/Hg*100%) in SPM was negatively associated with δ15N values, suggesting that “fresh” algal biomass could support the production and bioaccumulation of MeHg. Zooplankton δ13C values were correlated with SPM δ13C values in the epilimnion, suggesting that zooplankton primarily feed in surface waters. However, zooplankton MeHg was poorly associated with MeHg in SPM. Our results demonstrate seasonal patterns in biological MeHg uptake and how multiple data sources can help constrain the drivers of MeHg bioaccumulation.

Health risk assessment of mercury in Nile tilapia (Oreochromis niloticus) fed housefly maggots

The bioaccumulation of total mercury (THg) and methylmercury (MeHg) by housefly maggots (HM) during the conversion of food waste (vegetables and meat (VM) and rice waste) under various waste feed ratios were investigated. Subsequently, Nile tilapia (Oreochromis niloticus) were fed with the commercial feed, commercial dried HM, dried HM, and fresh HM, followed by a human health risk assessment of Hg via fish consumption. The THg concentrations of HM fed with food waste ranged from 39.5 to 100 μg kg−1 ww. Concentrations of MeHg in the maggots fed with 100 % vegetables and meat (VM) waste (13.7 ± 1.12 μg kg−1 ww) was significantly higher than that fed with other mixed ratios of rice waste and VM waste (p<0.05). Concentrations of MeHg were positively correlated with the weight and lipid content of houseflies (p<0.05). THg and MeHg concentrations in tilapia fed with the converted HM (dried and fresh HM) were 22.5 ± 6.50 μg kg−1 ww and 2.43 ± 0.36 μg kg−1 ww, respectively. There was no significant difference in MeHg between tilapia fed the four experiment diets (p>0.05). Health risk assessment results indicated that mercury in tilapia fed the food waste-grown HM did not pose potential health risks to humans (target hazard quotient < 1). In conclusion, HM could convert food waste into high-quality and safe fish feeds for cultivating tilapia.

Export and bioaccumulation of methylmercury in streams draining distinct soils in the Central Brazilian Amazon, 2012-2013

BackgroundUpland forest streams of the Central Amazon are unique aquatic systems.These small streams have short, unpredictable and multimodal flood-pulses that are influenced by local rainfall. The biogeochemical cycles in these systems are almost unknown. This study investigated the role of soil type on the export and bioaccumulation of methylmercury (MeHg) in upland forest streams of the Central Amazon during a complete annual cycle. Basic ProceduresLimnological measurements and water samples for MeHg analyses were collected monthly from October 2012 to October 2013 in two headwater streams drained by different soil types, spodzol (Campina Stream) and oxisol (Barro Branco Stream), in natural forest reserves. Shrimp and fish were collected for total mercury (THg) in April 2013 in both streams. Main findingsMeHg in water varied from 0.04 to 0.50 ng/L in the Campina Stream and between <detection limit and 0.04 ng/L in Barro Branco Stream. Physical characteristics of soils and the interaction between mercury and organic matter influenced the methylation of mercury and its export to the streams. In both streams, MeHg export was highest during the rainy season, probably due to soil leaching, lateral flooding and soil hydromorphism during this period, processes conducive to mercury methylation and export. THg in shrimps (omnivores) and carnivorous fish, which fed on aquatic food items, reflected the MeHg differences between streams while those in insectivorous fish, feeding on allochthonous food items, did not. Principal ConclusionsMeHg dynamics in streams were influenced by the physical characteristics of basin soils and by local seasonal rainfall.

Geochemical and Dietary Drivers of Mercury Bioaccumulation in Estuarine Benthic Invertebrates

Sediments represent the main reservoir of mercury (Hg) in aquatic environments and may act as a source of Hg to aquatic food webs. Yet, accumulation routes of Hg from the sediment to benthic organisms are poorly constrained. We studied the bioaccumulation of inorganic and methylmercury (HgII and MeHg, respectively) from different geochemical pools of Hg into four groups of benthic invertebrates (amphipods, polychaetes, chironomids, and bivalves). The study was conducted using mesocosm experiments entailing the use of multiple isotopically enriched Hg tracers and simulation of estuarine systems with brackish water and sediment. We applied different loading regimes of nutrients and terrestrial organic matter and showed that the vertical localization and the chemical speciation of HgII and MeHg in the sediment, in combination with the diet composition of the invertebrates, consistently controlled the bioaccumulation of HgII and MeHg into the benthic organisms. Our results suggest a direct link between the concentration of MeHg in the pelagic planktonic food web and the concentration of MeHg in benthic amphipods and, to some extent, in bivalves. In contrast, the quantity of MeHg in benthic chironomids and polychaetes seems to be driven by MeHg accumulation via the benthic food web. Accounting for these geochemical and dietary drivers of Hg bioaccumulation in benthic invertebrates will be important to understand and predict Hg transfer between the benthic and the pelagic food web, under current and future environmental scenarios.

Effects of physical disturbance of sediment on the cycling of mercury in coastal regions

Mercury (Hg) is a global pollutant of health concern due to formation and bioaccumulation of methylmercury (MeHg) during its biogeochemical cycle. Coastal areas are important regions in the biogeochemical cycling of Hg (Liu et al., 2017), where often-occurring natural and anthropogenic perturbations affect Hg transport and transformation and the associated health risk from Hg. The rapidly growing mariculture associated with the rising global demand for food may have a profound effect on coastal Hg cycling, due to the environmental alterations (e.g., resuspension and sedimentation) caused by maricultural activities (e.g., bottom sowing and harvesting). Through simulating the effect of water scouring, a common harvesting method, this study investigated Hg migration and distribution in particulate and dissolved phases in Laizhou Bay of Bohai Sea, China, where mariculture exists extensively. Particulate total and methyl Hg (PTHg and PMeHg) in water (expressed as ng/L) increased sharply due to the resuspension of sediment, but decreased rapidly after a one-off scouring event. When normalized by particle mass, PTHg and PMeHg (ng/g) in suspended sediment particles were significantly higher than that in the initial sediment, suggesting a higher distribution coefficient and higher affinity to bind Hg in the suspended particles. This may be due to the smaller particle sizes, and higher contents of organic matter and Fe/Mn of suspended sediments compared to the initial sediment. While the concentrations of dissolved THg (DTHg) in water column showed minimum changes or decreased, dissolved MeHg (DMeHg) concentrations increased sharply after the perturbation, due to the possible release of MeHg from porewater and potential Hg methylation during the event. These results provide fundamental information needed for ecological and health risk assessment of Hg in mariculture, and highlights the increased mobility and bioaccumulation of MeHg during anthropogenic perturbations in these areas.

Are There Longitudinal Effects of Forest Harvesting on Carbon Quality and Flow and Methylmercury Bioaccumulation in Primary Consumers of Temperate Stream Networks?

Forest harvesting affects dissolved organic matter (DOM) and aqueous mercury inputs as well as the food web structure in small-headwater streams, but how these upstream changes manifest downstream is unclear. To address this uncertainty, we examined DOM quality, autochthony in the caddisfly Hydropsychidae (using δ2 H), and methylmercury (MeHg) concentrations in stream water and the caddisfly along a longitudinal gradient (first- to fourth-order streams, subcatchments of 50-1900 ha) in paired partially harvested and reference catchments in central Ontario, Canada. Although measures of DOM quality (specific ultraviolet absorbance at 254 nm 2.20-11.62) and autochthony in caddisflies (4.9%-34.0%) varied among sites, no upstream-to-downstream differences in these measures were observed between the paired harvested and reference catchments. In contrast, MeHg levels in stream water (0.06-0.35 ng/L) and caddisflies(29.7-192 µg/kg dry wt) were significantly higher in the upstream sites but not the farthest downstream sites in the harvested catchments compared to the reference catchments. This suggests that while current mitigation measures used by forestry companies did not prevent elevated MeHg in water and invertebrates at smaller spatial scales (subcatchments of 50-400 ha), these upstream impacts did not manifest at larger spatial scales (subcatchments of 800-1900 ha). The present study advances our understanding of spatially cumulative impacts within harvested catchments, which is critical to help forest managers maintain healthy forest streams and their provisioning of aquatic ecosystem services. Environ Toxicol Chem 2022;41:1490-1507. © 2022 SETAC.