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Although the use of foliar spraying with organic matter has been extensively studied and applied to reduce heavy metals in plants, research on its application for reducing mercury (Hg) accumulation in plants, particularly the more toxic methylmercury (MeHg), remains scarce. Furthermore, previous researches on the barrier mechanisms of foliar spraying primarily concentrated on the effects of spraying agents on plant physiological and biochemical indicators, with limited focus on their impacts on soil environment. Herein, the dynamic effects and mechanisms of organic foliar spraying materials, including earthworm liquid fertilizer (ELF), Tween 80 (T80), and citric acid (CA), on soil Hg methylation and accumulation in lettuce were investigated using pot experiment. The findings revealed that foliar spraying significantly reduced the total mercury (THg) and MeHg concentrations in mature lettuce stems and leaves, with CA demonstrating the highest efficacy, achieving reduction rates of 24-60% for THg and 64-69% for MeHg. Spraying CA and T80 also simultaneously reduced the dissolved Hg and MeHg in the soil during the lettuce maturity period. The reductions of soil Hg methylation and bioaccumulation in lettuce were related to the increased abundance of Hg-reducing bacteria, decreased tartaric acid content and Hg-methylating bacteria abundance in soils, as well as enhanced nutrient absorption by lettuce. Additionally, foliar spraying lessened Hg toxicity to the plant and facilitated Hg sequestration in cell walls and vacuoles. Thus, foliar organic spraying impacted Hg enrichment in plant through altering plant physiological and biochemical indices, soil environment and Hg methylation processes., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2025 Elsevier Ltd. All rights reserved.)

Mercury is a highly toxic trace metal that readily biomagnifies in food webs where it is inaccessible to current bioremediation methods. Animals could potentially be engineered to detoxify mercury within their food webs to clean up impacted ecosystems. We demonstrate that invertebrate (Drosophila melanogaster) and vertebrate (Danio rerio) animal models can express organomercurial lyase (MerB) and mercuric reductase (MerA) from Escherichia coli to demethylate methylmercury and remove it from their biomass as volatile elemental mercury. The engineered animals accumulated less than half as much mercury relative to their wild-type counterparts, and a higher proportion of mercury in their tissue was in the form of less bioavailable inorganic mercury. Furthermore, the engineered animals could tolerate higher exposures to methylmercury compared to controls. These findings demonstrate the potential of using engineered animals for bioremediation and may be applied to reduce the burden of methylmercury in impacted ecosystems by disrupting its biomagnification or to treat contaminated organic waste streams., Competing Interests: Competing interests: Aspects of this research were filed under patent application WO/2023/183984 by K.T. and M.Maselko. K.T., C.P., and M.Maselko are co-founders of EntoZyme PTY LTD. The remaining authors declare no competing interests., (© 2025. The Author(s).)

Mercury pollution is a kind of heavy metal pollution with great harm and strong toxicity which exists worldwide. Some microorganisms can convert highly toxic methylmercury into inorganic mercury compounds with significantly reduced toxicity. This is an effective means of methylmercury pollution remediation. As a safe microorganism with great potential in the remediation of heavy metal pollution, Rhodotorula mucilaginosa has not been studied in the remediation of methylmercury. Here, a R. mucilaginosa strain Rm4 with high methylmercury resistance was obtained by wild-strain screening. Its minimal inhibitory concentration and minimum lethal concentration reached 3 and 6 mg/L, respectively. At the same time, Rm4 can also degrade methylmercury. Unlike the traditional microbial methylmercury degradation pathways, R. mucilaginosa 's genome does not encode the organomercury lyase gene MerB. However, transcriptomic analysis revealed that the glutathione reductase of R. mucilaginosa responds to the methylmercury degradation process. Structural domain analysis and molecular docking experiments suggest that the glutathione reductase of R. mucilaginosa has the potential to directly or indirectly participate in methylmercury degradation metabolism. Metabolic indicator tests of engineered strains overexpressing the glutathione reductase encoding gene also support this notion., Importance: The remediation of methylmercury pollution is crucial for environmental health. The ability of Rhodotorula mucilaginosa to resist and degrade methylmercury offers a new avenue for bioremediation efforts. Understanding the metabolic pathways involved, particularly the role of glutathione reductase, enhances our knowledge of how Rhodotorula mucilaginosa responds to methylmercury and opens up new possibilities for future research in bioremediation strategies., Competing Interests: The authors declare no conflict of interest.

The rapid melting of the Arctic cryosphere due to climate change will result in significant freshwater input into Arctic marine ecosystems. This might also cause the release of legacy mercury (Hg) stored in the cryosphere, increasing Hg concentration and its subsequent effects on the marine biota. However, there is scarce knowledge on the concentration of Hg in the lower trophic level organisms at the base of the Arctic pelagic food web. This is particularly important since these organisms modulate the transfer of Hg to higher trophic levels, including fish and marine mammals. We quantified the total Hg (THg) concentration in two plankton size classes (>200 and 50-200 μm) in coastal waters along the east Greenland coast and investigated the potential assimilation efficiency of both inorganic Hg (IHg) and methyl Hg (MeHg) in mesozooplankton and their faecal pellets in experimental incubations. The concentration of THg in plankton ranged from 12 to 109 ng (g dw) -1 without clear trends between geographic locations or between fjords and coastal areas. Also, the concentrations did not vary between the different plankton size fractions. MeHg concentrations were lower in the mesozooplankton faecal pellets than IHg, which may be due to the higher assimilation of MeHg than IHg in mesozooplankton tissue. Our results confirm that Arctic zooplankton assimilates MeHg more efficiently than IHg and may contribute significantly to the partitioning and cycling of different Hg types in Arctic marine ecosystems., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Paddy soil is recognized as a hotspot for mercury (Hg) transformation. Soil acid-base property (expressed as pH) plays a crucial role in Hg methylation and accumulation in paddy systems. However, it is challenging to study this process in soils with varying pH values due to the rarity of a single soil type spanning a wide pH range. Purple paddy soil, vital for rice cultivation in southwestern China, occurs naturally in three types based on pH: acidic, neutral, and calcareous. This variation makes purple paddy soil an ideal subject for these studies. Thus, this study investigated Hg transformation and bioaccumulation across these three purple soil types. The results showed that during the rice growing seasons, both methylmercury (MeHg) concentration and methylation potential were higher in acidic purple paddy soil than in neutral and calcareous types. In addition, total mercury (THg) and MeHg concentrations in plant tissues grown in acidic purple paddy soil were significantly higher than in other two purple soil types. These results suggest that acidic purple paddy soil was conducive to Hg methylation and accumulation in rice plants. Given that soil acidification is becoming a serious global issue, the findings could offer fundamental data on the potential risk of Hg exposure due to soil acidification., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Mercury (Hg) is a potent neurotoxicant and poses a risk to human health through the ingestion of Hg-contaminated fish. Mercury, especially in its organic form methylmercury (MeHg), biomagnifies up food chains such that even small aqueous concentrations of Hg can result in significant concentrations of total Hg in fish. Understanding the ecological and human health risks associated with Hg and MeHg exposure requires an understanding of the factors that affect its bioaccumulation in aquatic species. We compiled estimates of three biokinetic parameters: uptake rate (k u ), assimilation efficiency (AE), and efflux rate (k e ). These parameters describe contaminant uptake from aqueous (k u ) and dietary (AE) exposure and the rate of excretion (k e ). We found parameter values for 38 and 34 different species of fish and aquatic invertebrates, respectively, and collected 502 parameter values in total. We used a machine learning technique to establish the relationships between experimental and physiological variables and these parameter values. We found differences in which variables were associated with biokinetic parameter values for fish and aquatic invertebrates. The form of Hg was the most impactful variable, influencing values of all parameters except k u for invertebrates, for which aqueous exposure time was the only significant predicator variable. The parameter k e were the only values significantly influenced by more than one variable, with water type (freshwater, brackish, or marine), organism weight, and form of Hg significantly impacting parameter values for fish and/or invertebrates. To our knowledge, this study represents the most extensive review of biokinetic parameters of Hg and MeHg accumulation in aquatic organisms. Environmental parameters found to significantly impact Hg and MeHg bioaccumulation in past studies were not identified as important in our analyses across aquatic ecosystems and species. Our dataset and analysis reveal novel patterns that may help us better understand and manage Hg bioaccumulation., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Oak Ridge National Laboratory. Published by Elsevier B.V. All rights reserved.)

Sulfidic hot springs harbor unique microbial communities and are important in mercury (Hg) species transformations, although the fine scale drivers of these processes remain poorly understood. Here we studied Hg speciation in water, biofilms, and sediment across three sampling seasons in a French sulfidic hot spring with low Hg concentrations. Microbial Hg species methylation and demethylation potentials were evaluated using incubation experiments with species-specific Hg isotope tracers. Temporal variation in inorganic Hg (iHg) and methylmercury (MeHg) concentrations in water, biofilm, and sediment was observed. The incubation of microbial communities in biofilms and sediment under dark conditions exhibited low iHg methylation potentials, whereas a significant extent of biotic MeHg demethylation to oxidized iHg was found in relation to MeHg concentrations. Results from microbial diversity (16S rDNA) and the metabolic inhibition experiments suggest an important role of sulfur-linked bacterial metabolism dynamics. Specifically, sulfate-reducers and anoxygenic phototrophs were important factors in the regulation of MeHg concentrations in our study site. Overall, the observed dominance of microbial MeHg demethylation demonstrates a strong Hg detoxification capacity in sulfidic aquatic environments., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Returning raw straw to the soil can significantly elevate soil methylmercury (MeHg) and crop mercury (Hg) levels, underscoring the need to investigate safer approaches to straw utilization in mercury-contaminated regions. In this study, rice straw underwent anaerobic fermentation with the addition of sulfate, and the resulting fermentation products were utilized in a pot experiment involving water spinach to assess the impact of anaerobically fermented straw return on soil Hg methylation and its bioaccumulation. Findings revealed that the addition of sulfate during straw fermentation markedly increased the fermentation degree of the products, and sulfate was converted into organic sulfur-containing ligands that can functionalize the fermentation residuals. These changes enhanced adsorption or complexation of the fermentation products with Hg. Consequently, compared with raw straw returning to the soil, adding co-fermentation products of straw and sulfate to the soil can significantly reduce the bioavailable Hg and MeHg in the soil, the total mercury (THg) and MeHg in plants, with the maximum reduction rates being 68%, 92%, 66% and 78%, respectively. Therefore, returning the straw that has been anaerobically co-fermented with sulfate to the soil can effectively mitigate Hg methylation and bioaccumulation, while simultaneously increasing biomass, offering a suitable straw utilization method in Hg-contaminated cultivation areas., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Prey fish are vital in transferring nutrients and contaminants from lower to higher trophic levels. Although the role of selenium (Se) on mercury (Hg) detoxification has been identified in marine mammals and seabirds, the metabolic pathways of Hg-Se interaction in fish remain unknown. We used Hg stable isotopes (δ202Hg, Δ199Hg) to characterize the internal dynamics of methylmercury (MeHg) and inorganic Hg (IHg) in the presence and absence of Se in juvenile olive flounders (Paralichthys olivaceus). The fish were exposed to MeHg- (1,223 ng/g, n = 31) and IHg-amended (1,515 ng/g, n = 31) food pellets for 4 weeks (bioaccumulation phase) and switched to control or Se-amended food pellets for 10 weeks (excretion phase). During the bioaccumulation phase, the Hg isotopic composition of all fish tissues shifted toward their respective food pellets. During the excretion phase, significant negative δ202Hg shifts (0.27-0.59 ‰) were recorded in the liver of fish initially fed MeHg food pellets and then switched to Se food pellets, which is indicative of Se-induced hepatic MeHg demethylation. Fish fed IHg food pellets and then switched to control or Se food pellets exhibited similar isotopic behavior, suggesting that Se plays a minor role in IHg excretion. Both δ202Hg and Δ199Hg of the liver shifted toward IHg food pellets even during the excretion phase, which we attribute to slow intestinal IHg mobilization and redistribution to the liver. We found that the liver is the major site for MeHg demethylation in the presence of Se and that Se plays a relatively minor role in IHg excretion. Tissue-specific Hg isotope dynamics and interaction with Se should be considered in future Hg ecotoxicological assessments in fish., (© The Author(s) 2025. Published by Oxford University Press on behalf of the Society of Environmental Toxicology and Chemistry. All rights reserved. For permissions, please email: journals.permissions@oup.com.)

Methylmercury (MeHg) can cause devastating neurotoxicity in animals and human beings. Gut microbiota dysbiosis has been found in MeHg-poisoned animals. Fecal microbiota transplantation (FMT) has been shown to improve clinical outcomes in a variety of diseases such as epilepsy, amyotrophic lateral sclerosis (ALS) and autism. The aim of this study was to investigate the effects of FMT on MeHg-poisoned rats. FMT treatment was applied to MeHg-poisoned rats for 14 days. The neurobehavior, weight changes, dopamine (DA), the total Hg and MeHg level were evaluated. Besides, the gut microbiota and metabolites change in feces were also checked. It was found that FMT helped weight gain, alleviated the neurological disorders, enhanced fecal mercury excretion and MeHg demethylation, reconstructed gut microbiome and promoted the production of gut-brain axis related-metabolites in MeHg-poisoned rats. This study elaborates on the therapeutic efficacy of FMT in treating of MeHg-poisoned rats, which sheds lights on the treatment of neurological diseases like Minamata Disease and even Parkinson's Disease., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Rice contamination with neurotoxic methylmercury (MeHg) from paddy soils is an escalating global concern. Identifying the microorganisms responsible for mercury (Hg) methylation in these soils is essential for controlling Hg contamination in the food chain and mitigating health impacts. Current research often focuses on total Hg-methylating microorganisms, overlooking the contributions of active ones, which can lead to either overestimating or neglecting the specific roles of microorganisms in Hg methylation within paddy soils. In this study, active Hg-methylating microorganisms in paddy soils were identified using a combination of DNA-SIP, Hg isotope labelling, and Hg methylation gene sequencing techniques. Our findings revealed that Geobacter and Anaerolinea are pivotal active Hg-methylating microorganisms across a contamination gradient in paddy soils. Transcriptomic analysis of soils from major rice-producing provinces in China confirmed the widespread and synergistic involvement of these microorganisms. Microbial incubation further validated their interaction significantly enhances Hg methylation, with Me 198 Hg concentrations increasing 2.8-fold compared to Geobacter alone and 5.2-fold compared to Anaerolinea alone. These findings enhance our understanding of microbial Hg methylation in paddy soils, providing critical insights for accurately predicting soil MeHg load, rice grain MeHg contamination, and human MeHg exposure risks., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Developing rapid and sensitive methods for monitoring inorganic mercury (Hg 2+ ) and methylmercury (CH 3 Hg + ) 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 Hg 2+ and CH 3 Hg + 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 Hg 2+ and luminescent CdTe quantum dots (QDs), while CH 3 Hg + unrealizable CER. The CH 3 Hg + can be transformed to Hg 2+ by simple UV irradiation, speciation analysis can be realized by detecting the fluorescence of CdTe QDs after incubation by Hg 2+ and total Hg 2+ . In addition, the filtration of reacted CdTe QDs was carried out, ICP-MS was performed to detect exchanged Cd 2+ by Hg 2+ and total Hg 2+ , as well the smartphone RGB analysis was performed for membrane colorimetry. The limits of detection (LODs) of Hg 2+ and CH 3 Hg + 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 Cu 2+ that could occur during the CER reaction. The well-designed system was successfully utilized for monitoring trace Hg 2+ and CH 3 Hg + in crayfish fed Hg 2+ and CH 3 Hg + contaminative food over a two-week "uptake" period and a three-week "depuration" period. The results indicated that the Hg 2+ uptake in different tissues was significantly different from that of CH 3 Hg + in all tissues. There was evidence of Hg uptake from water via leaching from food, although the principal source of uptake was from food., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Zn as an essential element has the potential to protect against mercury (Hg) toxicity in rice. However, the antagonistic effects between Zn and Hg in rice and their mechanisms remain unknown. This study proposed a promising strategy for Zn application to mitigate Hg accumulation and toxicity in rice and revealed the underlying molecular mechanisms. The findings revealed that Zn supplementation significantly reduced the uptake and transportation of both IHg and MeHg in rice, thereby alleviating Hg phytotoxicity. In particular, Zn profoundly mitigated Hg-induced oxidative damage to rice, which was attributed to the redistribution of Hg and Zn in the root and Zn competing for binding sites on glutathione. The co-binding of Zn 2+ and HgCH 3 + within the same active sites of Zn transporters can promote the transfer of regions with a high charge density distribution at the highest occupied molecular orbital (HOMO) level. This process facilitates proton attack on the Hg-C bond, thereby enhancing MeHg demethylation in rice. By elucidating the molecular mechanisms of Zn, IHg, and MeHg interactions in rice, this study offers new insights for developing efficient strategies to mitigate Hg risks while boosting the Zn content in crops, thereby fortifying food safety.

The production and uptake of toxic methylmercury (MeHg) impacts aquatic ecosystems globally. Rivers can be dynamic and difficult systems to study for MeHg production and bioaccumulation, hence identifying sources of MeHg to these systems is both challenging and important for resource management within rivers and main-stem reservoirs. Riparian zones, which are known biogeochemical hotspots for MeHg production, are understudied as potential sources of MeHg to rivers. Here, we present a comprehensive quantification of the hydrologic and biogeochemical processes governing MeHg concentrations, loads, and bioaccumulation at 16 locations along 164 km of the agriculturally intensive Snake River (Idaho, Oregon USA) during summer baseflow conditions, with emphasis on riparian production of MeHg. Approximately one-third of the MeHg load of the Snake River could not be attributed to inflowing waters (upgradient, tributaries, or irrigation drains). Across the study reach, increases in MeHg loads in surface waters were significantly correlated with MeHg concentrations in riparian porewaters, suggesting riparian zones were likely an important source of MeHg to the Snake River. Across all locations, MeHg concentrations in surface waters positively correlated with MeHg concentrations in benthic snails and clams, supporting that riparian produced MeHg was assimilated into local aquatic food webs. This study contributes new insights into riparian MeHg production within rivers which can inform mitigation efforts to reduce MeHg bioaccumulation in fish.

The sulfidogenic process mediated by sulfate-reducing bacteria (SRB) is not ideal for treating mercury (Hg)-bearing wastewater due to the risk of methylmercury (MeHg) production. Addressing this challenge, our study demonstrated that, under S 0 -rich conditions and without organic additives, sulfidogenic communities dominated by sulfur-disproportionating bacteria (SDB) can effectively remove Hg(II) and prevent MeHg production. Using various inocula, we successfully established biological sulfidogenic systems driven separately by SDB and SRB. Batch experiments revealed that SDB cultures completely removed Hg(II) from the solution as HgS. Remarkably, no MeHg production was observed in the SDB cultures, while an average concentration of 0.32 μg/L of MeHg was detected in the SRB cultures. The absence of MeHg production in the SDB cultures could be mainly attributed to the cultivation conditions that reshaped the microbial community, resulting in a rapid decline of SRB-dominated Hg-methylating microorganisms. Consequently, the average abundance of the hgcA gene was 28 times lower than the levels before cultivation. Additionally, we found that the enriched Dissulfurimicrobium sp. bin121 can produce biogenic sulfide through sulfur disproportionation but lacks the hgcA gene, rendering it incapable of methylating Hg. Overall, we propose a novel biotechnology driven by SDB that can safely and sustainably treat Hg-bearing wastewater.

Unraveling the geochemical and microbial controls on methylmercury (MeHg) dynamics in mangrove sediments is important, as MeHg can potentially pose risks to marine biota and people that rely on these ecosystems. While the important role of sulfate-reducing bacteria in MeHg formation has been examined in this ecologically important habitat, the contribution of non-Hg methylating communities on MeHg production remains particularly unclear. Here, we collected sediment samples from 13 mangrove forests in south China and examined the geochemical parameters and microbial communities related to the Hg methylation. MeHg concentrations were significantly correlated to the OM-related parameters such as organic carbon content, total nitrogen, and dissolved organic carbon concentrations, suggesting the importance of OM in the MeHg production. Sulfate-reducing bacteria were the major Hg-methylators in mangrove sediments. Desulfobacteraceae and Desulfobulbaceae dominated the Hg-methylating microbes. Classification random forest analysis detected strong co-occurrence between Hg methylators and putative non-Hg methylators, thus suggesting that both types of microorganisms contribute to the MeHg dynamics in the sediments. Our study provides an overview of MeHg contamination in south China and advances our understanding of Hg methylation in mangrove ecosystems., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

There has been a serious health and environmental concern in conversion of inorganic mercury (Hg) to the neurotoxin, methylmercury (MeHg) by anaerobic microbes, while very little is known about the potential role of vitamin B9 (VB9) regulator in the biochemical generation of MeHg. This study innovatively investigated bacterial Hg methylation by Geobacter sulfurreducens PCA in the presence of VB9 under two existing scenarios. In the low-complexing scenario, the bacterial MeHg yield reached 68 % higher than that without VB9 within 72 h, which was attributed to free VB9-protected PCA cells relieving oxidative stress, as manifested by the increased expression of Hg methylation gene (hgcAB cluster by 19-48 %). The high-complexing scenario emphasized the intracellular Hg accumulation (38-45 %) after 12 h, as indicated by the increased expression of outer membrane protein-related and mercuric reductase-encoding genes, indicating the inefficient bioavailability of Hg due to a gradual shift from Hg reduction toward Hg 0 re-oxidation controlled by competitive ligand exchange. These results suggested that VB9 application significantly raised the potential for bacterial Hg methylation and cellular accumulation, thus proposing insights into the biochemical behaviors of hazardous Hg in farming environments where vulnerable organisms are more possibly co-exposed to higher levels of Hg and VB9., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Methylmercury (MeHg) is a ubiquitous environmental contaminant, well known for its neurotoxic effects. MeHg can interact with several nutrients in the diet and affect nutrient metabolism, however the interaction between MeHg and dietary proteins has not been thoroughly investigated. Male BALB/c mice were fed diets based on either casein, cod or chicken as protein sources, which were or were not spiked with MeHg (3.5 mg Hg kg -1 ). Following 13 weeks of dietary exposure to MeHg, the animals accumulated mercury in a varying degree depending on the diet, where the levels of mercury were highest in the mice fed casein and MeHg, lower in mice fed cod and MeHg, and lowest in mice fed chicken and MeHg in all tissues assessed. Assessment of gut microbiota revealed differences in microbiota composition based on the different protein sources. However, the introduction of MeHg eliminated this difference. Proteomic profiling of liver tissue uncovered the influence of the dietary protein sources on a range of enzymes related to Phase I and Phase II detoxification mechanisms, suggesting an impact of the diet on MeHg metabolism and excretion. Also, enzymes linked to pathways including methionine and glycine betaine cycling, which in turn impact the production of glutathione, an important MeHg conjugation molecule, were up-regulated in mice fed chicken as dietary protein. Our findings indicate that dietary proteins can affect expression of hepatic enzymes that potentially influence MeHg metabolism and excretion, highlighting the relevance of considering the dietary composition in risk assessment of MeHg through dietary exposure., Competing Interests: Declaration of competing interests The authors declare no conflict of interest. The author JD Rasinger declares that he is currently employed with the European Food Safety Authority (EFSA) in the Food Ingredients and Packaging Unit (FIP), which provides scientific and administrative support to the Panel on Food Additives and Flavourings. However, the present article is published under the sole responsibility of the author JD Rasinger and may not be considered as an EFSA scientific output. The positions and opinions presented in this article are those of the author alone and are not intended to represent the views/any official position of EFSA. To know about the views or scientific outputs of EFSA, please consult its website. The author's main contributions to this article were made before joining EFSA when still employed at the Institute of Marine Research., (Copyright © 2024 The Authors. Published by Elsevier Inc. All rights reserved.)

After tin and mercury salts were added to estuarine microbial mats increasing amounts of methyltin and methylmercury, respectively, were formed over a 30 to 100 hour time period. Inhibition of the methylation by molybdate, a metabolic inhibitor of sulfate reduction, stimulation by pyruvate addition and lack of methylation by sterilized mats, were evidence that sulfate reducing bacteria within the mats were responsible for the tin and mercury methylation. Methyl mercury was formed from mercuric chloride and mercuric cysteine, but not from mercuric sulfide. We suggest that mercury bound to organic complexes in anoxic sediments is likely methylated by microbial mats. Since estuarine meiofauna and macrofauna fed on microbial mats, the methylmercury and methyltin formed by microbial mats could be an important avenue for the entrance of these compounds into the marine food web., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

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.

Methylmercury (MeHg) in aquatic systems poses a serious public health risk through bioaccumulation in the aquatic food web. In recent years, MeHg has been observed to increase to concerning levels globally in rivers near cities; however, the causes of this increase are not well understood. Here, we demonstrate the significant role of sewage contamination by analyzing over 1,300 publicly available metagenomes in urban rivers worldwide, and conducting experiments with water samples across China. We find that sewage contamination significantly increases the abundance of mercury (Hg)-methylating microorganisms in urban rivers globally. This increase is primarily attributed to the high abundance of active Hg-methylating microorganisms in sewage, which migrate to rivers via direct discharge or combined sewer overflows (CSOs), becoming key contributors to elevated riverine MeHg levels. Our findings underscore the importance of effectively eliminating Hg-methylating microorganisms from sewage to mitigate the public health risks associated with MeHg in urban rivers., (© 2024. The Author(s).)

Methylmercury (MeHg) is a bioaccumulating neurotoxin mainly produced by anaerobic microorganisms, with methanogen being one of the important methylators. A critical aspect for understanding the mechanism for microbial mercury (Hg) methylation is the origin of the methyl group. However, the origin of methyl group in methanogen-mediated Hg methylation remains unclear. This study aims to identify the source of methyl group for MeHg synthesis in methanogens. Our study revealed that Hg methylation in Methanospirillum hungatei JF-1 is closely related to methanogenesis process, according to the results of proteomic study and substrate limitation study. Next, we proved that nearly all methyl group in MeHg derives from the Wolfe cycle in this species, rather than the previously demonstrated acetyl-coenzyme A pathway, based on the results of 13 C labeling study. We then proposed the Wolfe cycle-dependent Hg methylation mechanism in this species. Further genome analyses and 13 C labeling experiments indicated that the involvement of the Wolfe cycle in Hg methylation is probably a universal feature among Hg-methylating methanogens. These findings reveal a unique Hg methylation mechanism in methanogens. Our study broadens the carbon substrates and controlling factors for MeHg synthesis in the environment, which can inform the prediction of MeHg production potential and remediation strategies for MeHg contamination., Competing Interests: Competing interests statement:The authors declare no competing interest.

The study explored the impact of water management on rice cultivation in mercury-contaminated paddy soil. The objective was to analyze the characteristics of mercury translocation by converting flooded soils to dry farming (non-flooded) to alleviate mercury accumulation in rice grains. The experiment was conducted over three consecutive rice-growing seasons, employing two distinct water management models: a continuously flooded rice cultivation mode and a flooded rice planting mode in the first season, followed by a non-flooded rice farming mode in the second and third seasons. The results showed that the change from flooded to non-flooded rice cultivation patterns presented extremely excellent environmental potential for inhibiting the uptake of both methylmercury and total mercury in rice. When transitioning from flooded cultivation to dry farming, the concentration of methylmercury and total mercury in the grains of non-flooded rice decreased by 87.15 % and 9.57 %, respectively, compared to that in the grains of flooded rice. In the third season, the methylmercury and total mercury in the grains of non-flooded rice decreased further by 95.03 % and 69.45 %, respectively. This study verified that the conversion of rice cultivation from flooded to non-flooded is an efficient strategy for suppressing the accumulation of methylmercury in rice grains, and it might offer a promising solution for managing soil mercury risks and ensuring the safety of rice for human consumption., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Inc. All rights reserved.)

Dominant microorganisms and functional genes, including hgcA, hgcB, merA, and merB, have been identified to be responsible for mercury (Hg) methylation or methylmercury (MeHg) demethylation. However, their in situ correlation with MeHg levels and the processes of Hg methylation and MeHg demethylation in coastal areas remains poorly understood. In this study, four functional genes related to Hg methylation and MeHg demethylation (hgcA, hgcB, merA, and merB) were all detected in the sediments of the Eastern China Coastal Seas (ECCSs) (representative coastal seas highly affected by human activities) using metagenomic approaches. HgcA was identified to be the key gene controlling the in situ net production of MeHg in the ECCSs. Based on metagenomic analysis and incubation experiments, sulfate-reducing bacteria were identified as the dominant microorganisms controlling Hg methylation in the ECCSs. In addition, hgcA gene was positively correlated with the MeHg content and Hg methylation rates, highlighting the potential roles of Hg methylation genes and microorganisms influenced by sediment physicochemical properties in MeHg cycling in the ECCSs. These findings highlighted the necessity of conducting similar studies in other natural systems for elucidating the molecular mechanisms underlying MeHg production in aquatic environments., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Sulfate-reducing bacteria (SRB) are known to alter methylmercury (MeHg) production in paddy soil, but the effect of SRB on MeHg dynamics in rhizosphere and rice plants remains to be fully elucidated. The present study investigated the impact of SRB on MeHg levels in unsterilized and γ-sterilized mercury-polluted paddy soils, with the aim to close this knowledge gap. Results showed that the presence of SRB reduced MeHg production by ∼22 % and ∼17 % in the two soils, but elevated MeHg contents by approximately 55 % and 99 % in rice grains, respectively. Similar trend at smaller scales were seen in roots and shoots. SRB inoculation exerted the most profound impact on amino acid metabolism in roots, with the relative response of L-arginine positively linking to MeHg concentrations in rhizosphere. The SRB-induced enrichment of MeHg in rice plants may be interpreted by the stronger presence of endophytic nitrogen-related microbes (e.g. Methylocaldum, Hyphomicrobium and Methylocystis) and TGA transcription factors interacting with glutathione metabolism and calmodulin. Our study provides valuable insights into the complex effects of SRB inoculation on MeHg dynamics in rice ecosystems, and may help to develop strategies to effectively control MeHg accumulation in rice grains., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

The increasing use of alternative feeds for sustainable aquaculture leads to a reduced selenium content requiring the use of supplements to maintain the antioxidant status of farmed fish. The introduction of tuna by-products in fish feed is attractive for their selenium content, but the presence of mercury limits their use as it may negatively impact fish health. Indeed, selenium and mercury metabolism, in relation to their interaction and biological effects in fish, is far from being fully understood. This study aims to assess the impact of parental and dietary supplementation with selenomethionine and methylmercury on selenium and mercury localisation and concentrations in tissues of 3-week rainbow trout fry. Six diets were used. Broodstock were fed a plant-based diet Bpc (with 0.2 μg g -1 selenium and 0 μg g -1 mercury) or a tuna by-product-based diet Bt (with 4 μg g -1 selenium and basal mercury at 0.2 μg g -1 ) during 6 months, supplemented or not with 4 μg g -1 of selenomethionine for the plant-based diet Bpo and/or with 2 μg g -1 of methylmercury for diets Bph, Bpho and Bth. Their offspring were fed the plant-based diet Fpc, supplemented or not with the same levels of selenomethionine and methylmercury, until their third week. Mercury and selenium concentrations were determined in fry whole-body by ICP MS and quantitative images of selenium and mercury were produced by LA-ICP MS from fry whole-body thin sections. Dietary supplementation of fry with selenium and/or mercury increased their concentration in all tissues, especially in liver, kidney, muscle and intestine. Parental selenomethionine supplementation had a more pronounced effect on fry selenium levels than tuna by-products diet. Mercury transfer from broodstock to their offspring was weak. Mercury concentrations decreased in the kidney of fry supplemented with both selenium and mercury, which could be related to the presence of selenium., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Mercury (Hg) is a naturally occurring heavy metal, but human activities and natural processes have led to increased pollution with Hg in the environment. Organic mercury, such as methyl mercury (MeHg), is considered more toxic than most inorganic mercury compounds. MeHg is rapidly taken up by aquatic organisms and bioaccumulates through the aquatic food web. The bioaccumulation causes high levels of MeHg in apex predators, such as pilot whales. Pilot whale meat is a traditional food source on the Faroe Islands; thus the consumption of pilot whale meat can lead to high Hg exposures in humans. The majority of the total Hg in pilot whale and fish is generally assumed to be MeHg. However, the relative amount of MeHg to total Hg can be highly variable. For risk assessment, it is relevant to know both the MeHg and the total Hg content. This study summarizes the knowledge of muscle MeHg concentrations relative to total Hg concentrations in pilot whales in the Faroe Islands. The pilot whale tissue was sampled during 1977-78, 1986-87, 2009-2010, and 2015. The 2015 samples included two pairs of fetuses/mothers. The results showed that the 1977-78 pilot whale muscle samples had lower relative concentrations of MeHg to total Hg compared to samples from the subsequent years. This discrepancy between early and later years could not solely be explained by increased demethylation related to concentration differences. Instead, the difference is more likely explained by variations in relative amounts of MeHg in prey of the pilot whales. In the fetuses the total Hg concentration was 20% of the Hg concentration in the mother. The relative MeHg concentrations in the fetuses were also lower (∼20%-30%) than in the mother. However, the MeHg to total Hg fraction in the fetus was similar or higher than in the mother., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The increasing frequency and severity of wildfires are among the most visible impacts of climate change. However, the effects of wildfires on mercury (Hg) transformations and bioaccumulation in stream ecosystems are poorly understood. We sampled soils, water, sediment, in-stream leaf litter, periphyton, and aquatic invertebrates in 36 burned (one-year post fire) and 21 reference headwater streams across the northwestern U.S. to evaluate the effects of wildfire occurrence and severity on total Hg (THg) and methylmercury (MeHg) transport and bioaccumulation. Suspended particulate THg and MeHg concentrations were 89 and 178% greater in burned watersheds compared to unburned watersheds and increased with burn severity, likely associated with increased soil erosion. Concentrations of filter-passing THg were similar in burned and unburned watersheds, but filter-passing MeHg was 51% greater in burned watersheds, and suspended particles in burned watersheds were enriched in MeHg but not THg, suggesting higher MeHg production in burned watersheds. Among invertebrates, MeHg in grazers, filter-feeders, and collectors was 33, 48, and 251% greater in burned watersheds, respectively, but did not differ in shredders or predators. Thus, increasing wildfire frequency and severity may yield increased MeHg production, mobilization, and bioaccumulation in headwaters and increased transport of particulate THg and MeHg to downstream environments.

Complexes with low-molecular-weight thiols are crucial species of methylmercury (MeHg) excreted by anaerobic Hg-methylating microbes, notably, MeHg-cysteine (MeHg-Cys). As MeHg-Cys diffuses into surface water, it would undergo a ligand exchange process with dissolved organic matter (DOM) under nonsulfidic conditions, inevitably altering MeHg speciation and bioavailability to phytoplankton. In this study, we investigated the competitive binding kinetics between MeHg-Cys and Suwannee River natural organic matter, and their influence on the adsorption and uptake of MeHg by the cyanobacterium, Synechocystis sp. PCC6803. Liquid chromatography-inductively coupled plasma mass spectrometry was employed to monitor the kinetics processes involving competition of DOM with Cys for MeHg binding, which revealed that competitive binding kinetics were dictated by the abundance of thiol moieties in DOM. Thiol concentrations of 0.97 and 49.34 μmol of thiol (g C) -1 resulted in competitive binding rate constant ( k values) of 0.30 and 3.47 h -1 , respectively. Furthermore, the time-dependent competitive binding of DOM toward MeHg-Cys significantly inhibited MeHg adsorption and uptake by cyanobacteria, an effect that was amplified by an increased thiol abundance in DOM. These findings offer valuable insights into the kinetic characteristics of MeHg's fate and transport, as well as their impact on bioconcentration in aquatic organisms within natural aquatic ecosystems.

The ocean's mercury (Hg) content has tripled due to anthropogenic activities, and although the dark ocean (>200 m) has become an important Hg reservoir, concentrations of the toxic and bioaccumulative methylmercury (MeHg) are low and therefore very difficult to measure. As a consequence, the current understanding of the Hg cycle in the deep ocean is severely data-limited, and the factors controlling MeHg, as well as its transformation rates, remain largely unknown. By analyzing 52 globally distributed bathypelagic deep-ocean metagenomes and 26 new metatranscriptomes from the Malaspina Expedition, our study reveals the widespread distribution and expression of bacterial-coding genes merA and merB in the global bathypelagic ocean (∼4000 m depth). These genes, associated with Hg II reduction and MeHg demethylation, respectively, are particularly prevalent within the particle-attached fraction. Moreover, our results indicate that water mass age and the organic matter composition shaped the structure of the communities harboring merA and merB genes living in different particle size fractions, their abundance, and their expression levels. Members of the orders Corynebacteriales , Rhodobacterales , Alteromonadales , Oceanospirillales , Moraxellales , and Flavobacteriales were the main taxonomic players containing merA and merB genes in the deep ocean. These findings, together with our previous results of pure culture isolates of the deep bathypelagic ocean possessing the metabolic capacity to degrade MeHg, indicated that both methylmercury demethylation and Hg II reduction likely occur in the global dark ocean, the largest biome in the biosphere.

Identifying metabolism and detoxification mechanisms of Hg in biota has important implications for biomonitoring, ecotoxicology, and food safety. Compared to marine mammals and waterbirds, detoxification of MeHg in fish is understudied. Here, we investigated Hg detoxification in Atlantic bluefin tuna Thunnus thynnus using organ-specific Hg and Se speciation data, stable Hg isotope signatures, and Hg and Se particle measurements in multiple tissues. Our results provide evidence for in vivo demethylation and biomineralization of HgSe particles, particularly in spleen and kidney. We observed a maximum range of 1.83‰ for δ 202 Hg between spleen and lean muscle, whereas Δ 199 Hg values were similar across all tissues. Mean percent methylmercury ranged from 8% in spleen to 90% in lean muscle. The particulate masses of Hg and Se were higher in spleen and kidney (Hg: 61% and 59%, Se: 12% and 6%, respectively) compared to muscle (Hg: 2%, Se: 0.05%). Our data supports the hypothesis of an organ-specific, two-step detoxification of methylmercury in wild marine fish, consisting of demethylation and biomineralization, like reported for waterbirds. While mass dependent fractionation signatures were highly organ specific, stable mass independent fractionation signatures across all tissues make them potential candidates for source apportionment studies of Hg using ABFT., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Mercury (Hg) contaminated paddy soils are hot spots for methylmercury (MeHg) which can enter the food chain via rice plants causing high risks for human health. Biochar can immobilize Hg and reduce plant uptake of MeHg. However, the effects of biochar on the microbial community and Hg (de)methylation under dynamic redox conditions in paddy soils are unclear. Therefore, we determined the microbial community in an Hg contaminated paddy soil non-treated and treated with rice hull biochar under controlled redox conditions (< 0 mV to 600 mV) using a biogeochemical microcosm system. Hg methylation exceeded demethylation in the biochar-treated soil. The aromatic hydrocarbon degraders Phenylobacterium and Novosphingobium provided electron donors stimulating Hg methylation. MeHg demethylation exceeded methylation in the non-treated soil and was associated with lower available organic matter. Actinobacteria were involved in MeHg demethylation and interlinked with nitrifying bacteria and nitrogen-fixing genus Hyphomicrobium. Microbial assemblages seem more important than single species in Hg transformation. For future directions, the demethylation potential of Hyphomicrobium assemblages and other nitrogen-fixing bacteria should be elucidated. Additionally, different organic matter inputs on paddy soils under constant and dynamic redox conditions could unravel the relationship between Hg (de)methylation, microbial carbon utilization and nitrogen cycling., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Mercury (Hg) methylation is a microbially mediated process that produces methylmercury (MeHg), a bioaccumulative neurotoxin. A highly conserved gene pair, hgcAB, is required for Hg methylation, which provides a basis for identifying Hg methylators and evaluating their genomic composition. In this study, we conducted a large-scale omics analysis in which 281 metagenomic freshwater and marine sediment samples from 46 geographic locations across the globe were queried. Specific objectives were to examine the prevalence of Hg methylators, to identify horizontal gene transfer (HGT) events involving hgcAB within Hg methylator communities, and to identify associations between hgcAB and microbial biochemical functions/genes. Hg methylators from the phyla Desulfobacterota and Bacteroidota were dominant in both freshwater and marine sediments while Firmicutes and methanogens belonging to Euryarchaeota were identified only in freshwater sediments. Novel Hg methylators were found in the Phycisphaerae and Planctomycetia classes within the phylum Planctomycetota, including potential hgcA-carrying anammox metagenome-assembled genomes (MAGs) from Candidatus Brocadiia. HGT of hgcA and hgcB were identified in both freshwater and marine methylator communities. Spearman's correlation analysis of methylator genomes suggested that in addition to sulfide, thiosulfate, sulfite, and ammonia may be important parameters for Hg methylation processes in sediments. Overall, our results indicated that the biochemical drivers of Hg methylation vary between marine and freshwater sites, lending insight into the influence of environmental perturbances, such as a changing climate, on Hg methylation processes., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Methylmercury (MeHg) remains a global public health issue because of its frequent presence in human food sources obtained from the water. The excretion of MeHg in humans occurs slowly with a biological half-time of 32-47 days. Short-term MeHg exposure may cause long-lasting neurotoxicity. The excretion through feces is a major route in the demethylation of MeHg. Accumulating evidence suggests that the intestinal microbiota plays an important role in the demethylation of MeHg, thereby protecting the host from neurotoxic effects. Here, we discuss recent developments on the role of intestinal microbiota in MeHg metabolism, based on in vitro cell culture experiments, experimental animal studies and human investigations. Demethylation by intestinal bacteria is the rate-limiting step in MeHg metabolism and elimination. The identity of bacteria strains responsible for this biotransformation is currently unknown; however, the non-homogenous distribution of intestinal microbiota may lead to different demethylation rates in the intestinal tract. The maintenance of intestinal barrier function by intestinal microbiota may afford protection against MeHg-induced neurotoxicity, which warrant future investigations. We also discuss studies investigating the effects of MeHg exposure on the population structural stability of intestinal microbiota in several host species. Although this is an emerging area in metal toxicity, current research suggests that a change in certain phyla in the intestinal microbiota may indicate MeHg overexposure., (© 2023. The Author(s), under exclusive licence to Springer Nature B.V.)

Methyl mercury, a toxic compound, is produced by anaerobic microbes and magnifies in aquatic food webs, affecting the health of animals and humans. The exploration of mercury methylators based on genomes is still limited, especially in the context of river ecosystems. To address this knowledge gap, we developed a genome catalogue of potential mercury-methylating microorganisms. This was based on the presence of hgcAB from the sediments of a river affected by two run-of-river hydroelectric dams, logging activities and a wildfire. Through the use of genome-resolved metagenomics, we discovered a unique and diverse group of mercury methylators. These were dominated by members of the metabolically versatile Bacteroidota and were particularly rich in microbes that ferment butyrate. By comparing the diversity and abundance of mercury methylators between sites subjected to different disturbances, we found that ongoing disturbances, such as the input of organic matter related to logging activities, were particularly conducive to the establishment of a mercury-methylating niche. Finally, to gain a deeper understanding of the environmental factors that shape the diversity of mercury methylators, we compared the mercury-methylating genome catalogue with the broader microbial community. The results suggest that mercury methylators respond to environmental conditions in a manner similar to the overall microbial community. Therefore, it is crucial to interpret the diversity and abundance of mercury methylators within their specific ecological context., (© 2024 The Author(s). Environmental Microbiology published by John Wiley & Sons Ltd.)

The neurotoxic methylmercury (MeHg) is a product of inorganic mercury (IHg) after microbial transformation. Yet it remains unclear whether microbial activity or IHg supply dominates Hg methylation in paddies, hotspots of MeHg formation. Here, we quantified the response of MeHg production to changes in microbial activity and Hg supply using 63 paddy soils under the common scenario of straw amendment, a globally prevalent agricultural practice. We demonstrate that the IHg supply is the limiting factor for Hg methylation in paddies. This is because IHg supply is generally low in soils and can largely be facilitated (by 336-747 %) by straw amendment. The generally high activities of sulfate-reducing bacteria (SRB) do not limit Hg methylation, even though SRB have been validated as the predominant microbial Hg methylators in paddies in this study. These findings caution against the mobilization of legacy Hg triggered by human activities and climate change, resulting in increased MeHg production and the subsequent flux of this potent neurotoxin to our dining tables., Competing Interests: Declaration of competing interest The authors have no competing interests to declare., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Uptake of methylmercury (MeHg), a potent neurotoxin, by phytoplankton is a major concern due to its role as the primary pathway for MeHg entry into aquatic food webs, thereby posing a significant risk to human health. While it is widely believed that the MeHg uptake by plankton is negatively correlated with the concentrations of dissolved organic matter (DOM) in the water, ongoing debates continue regarding the specific components of DOM that exerts the dominant influence on this process. In this study, we employed a widely-used resin fractionation approach to separate and classify DOM derived from algae (AOM) and natural rivers (NOM) into distinct components: strongly hydrophobic, weakly hydrophobic, and hydrophilic fractions. We conduct a comparative analysis of different DOM components using a combination of spectroscopy and mass spectrometry techniques, aiming to identify their impact on MeHg uptake by Microcystis elabens, a prevalent alga in freshwater environments. We found that the hydrophobic components had exhibited more pronounced spectral characteristics associated with the protein structures while protein-like compounds between hydrophobic and hydrophilic components displayed significant variations in both distributions and the values of m/z (mass-to-charge ratio) of the molecules. Regardless of DOM sources, the low-proportion hydrophobic components usually dominated inhibition of MeHg uptake by Microcystis elabens. Results inferred from the correlation analysis suggest that the uptake of MeHg by the phytoplankton was most strongly and negatively correlated with the presence of protein-like components. Our findings underscore the importance of considering the diverse impacts of different DOM fractions on inhibition of phytoplankton MeHg uptake. This information should be considered in future assessments and modeling endeavors aimed at understanding and predicting risks associated with aquatic Hg contamination., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Mercury (Hg), particularly organic mercury, poses a global concern due to its pronounced toxicity and bioaccumulation. Bioremediation of organic mercury in high-salt wastewater faces challenges due to the growth limitations imposed by elevated Cl - and Na + concentrations on microorganisms. In this study, an isolated marine bacterium Alteromonas macleodii KD01 was demonstrated to degrade methylmercury (MeHg) efficiently in seawater and then was applied to degrade organic mercury (MeHg, ethylmercury, and thimerosal) in simulated high-salt wastewater. Results showed that A. macleodii KD01 can rapidly degrade organic mercury (within 20 min) even at high concentrations (>10 ng/mL), volatilizing a portion of Hg from the wastewater. Further analysis revealed an increased transcription of organomercury lyase (merB) with rising organic mercury concentrations during the exposure process, suggesting the involvement of mer operon (merA and merB). These findings highlight A. macleodii KD01 as a promising candidate for addressing organic mercury pollution in high-salt wastewater., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The role of forest ecosystems in the global mercury (Hg) biogeochemical cycle is widely recognized; however, using litterfall as a surrogate to assess the Hg sink function of forests encounters limitations. We investigated the accumulation characteristics and influencing factors of Hg in mosses from two remote subalpine forests in southwestern China. The results indicated that there was high Hg accumulation in subalpine forest mosses, with average concentrations of 82 ± 49 ng g -1 for total mercury (THg) and 1.3 ± 0.8 ng g -1 for methylmercury (MeHg). We demonstrated that the accumulation capacity of Hg in mosses was significantly dependent on species and substrates (micro-habitats), the mosses on tree trunks exhibited significantly elevated Hg accumulation levels (THg 132 ± 56 ng g -1 , MeHg 1.6 ± 0.2 ng g -1 ) compared to mosses in other substrates. The surface morphologies and biochemical components of leaf (phyllidia), such as cation exchange capacity (CEC), pectin, uronic acid, and metallothionein, play a crucial role in the accumulation of Hg by mosses. These findings provide valuable insights into Hg accumulation in forest mosses. Suggesting that the contribution of mosses Hg accumulation should be considered when assessing atmospheric Hg sinks of forests., Competing Interests: Declaration of Competing Interest The authors declare there is no conflict of interest regarding the publication of this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Algae are an entry point for mercury (Hg) into the food web. Bioconcentration of Hg by algae is crucial for its biogeochemical cycling and environmental risk. Herein, considering the cell heterogeneity, we investigated the bioconcentration of coexisting isotope-labeled inorganic ( 199 IHg) and methyl Hg ( 201 MeHg) by six typical freshwater and marine algae using dual-mass single-cell inductively coupled plasma mass spectrometry (scICP-MS). First, a universal pretreatment procedure for the scICP-MS analysis of algae was developed. Using the proposed method, the intra- and interspecies heterogeneities and the kinetics of Hg bioconcentration by algae were revealed at the single-cell level. The heterogeneity in the cellular Hg contents is largely related to cell size. The bioconcentration process reached a dynamic equilibrium involving influx/adsorption and efflux/desorption within hours. Algal density is a key factor affecting the distribution of Hg between algae and ambient water. Cellular Hg contents were negatively correlated with algal density, whereas the volume concentration factors almost remained constant. Accordingly, we developed a model based on single-cell analysis that well describes the density-driven effects of Hg bioconcentration by algae. From a novel single-cell perspective, the findings improve our understanding of algal bioconcentration governed by various biological and environmental factors.

Methylmercury (MeHg), as a global environmental pollutant, is of concern globally due to its neurodevelopmental toxicity. Mitochondria-associated membranes (MAMs) are highly dynamic sites of endoplasmic reticulum (ER)-haemocyte contact. MAMs are closely associated with the pathophysiology of neurological disorders due to their role in the transfer of calcium ions (Ca 2+ ) between mitochondria and the ER. However, the molecular mechanisms that control these interactions in MeHg-induced neurotoxicity have not yet been characterized. In the current study, MeHg caused increases in the levels of both cytosolic and mitochondrial Ca 2+ in PC12 cells and promoted MAMs formation in both in vivo and in vitro experiments. Of note, MeHg perturbed mitochondrial dynamics, promoting a shift toward a fission phenotype, and this was supported by the dysregulation of fission regulators. Interestingly, the MeHg-induced promotion of MAMs formation and increase in Ca 2+ levels were effectively attenuated by the inhibition of mitochondrial fission using Mdivi-1, a DRP1 inhibitor. Furthermore, MeHg triggered the AMPK pathway, and most of the aforementioned changes were significantly rescued by Compound C. Mechanistic investigations revealed a reciprocal relationship between AMPK- and Ca 2+ -mediated mitochondrial fission. The specific inhibitor of Ca 2+ uniporter, ruthenium-red (RuR), effectively abolished the feedback regulation of mitochondrial dynamics and MAMs formation mediated by AMPK in response to MeHg-induced Ca 2+ overload. This study reveals a novel role of AMPK-DRP1-mediated mitochondrial fragmentation in the coupling of ER-mitochondrial calcium microdomains in MeHg-induced neurotoxicity. The findings provide valuable insights for the development of strategies to regulate mitochondrial imbalances in neurological diseases., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Methylmercury (MeHg) is one of the most worrisome pollutants in marine systems. MeHg detoxification is mediated by merB and merA genes, responsible for the demethylation of MeHg and the reduction of inorganic mercury, respectively. Little is known about the biological capacity to detoxify this compound in marine environments, and even less the bacterial transcriptional changes during MeHg detoxification. This study provides the genomic and transcriptomic characterization of the deep ocean bacteria Alteromonas mediterranea ISS312 with capacity for MeHg degradation. Its genome sequence revealed four mer operons containing three merA gene and two merB gene copies, that could be horizontally transferred among distant related genomes by mobile genetic elements. The transcriptomic profiling in the presence of 5 μM MeHg showed that merA and merB genes are within the most expressed genes, although not all mer genes were equally transcribed. Besides, we aimed to identify functional orthologous genes that displayed expression profiles highly similar or identical to those genes within the mer operons, which could indicate they are under the same regulatory controls. We found contrasting expression profiles for each mer operon that were positively correlated with a wide array of functions mostly related to amino acid metabolism, but also to flagellar assembly or two component systems. Also, this study highlights that all merAB genes of the four operons were globally distributed across oceans layers with higher transcriptional activity in the mesopelagic deeper waters. Our study provides new insights about the transcriptional patterns related to the capacity of marine bacteria to detoxify MeHg, with important implications for the understanding of this process in marine ecosystems., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

The intake of methylmercury (MeHg)-contaminated rice poses immense health risks to rice consumers. However, the mechanisms of MeHg accumulation in rice plants are not entirely understood. The knowledge that the MeHg-Cysteine complex was dominant in polished rice proposed a hypothesis of co-transportation of MeHg and cysteine inside rice plants. This study was therefore designed to explore the MeHg accumulation processes in rice plants by investigating biogeochemical associations between MeHg and amino acids. Rice plants and underlying soils were collected from different Hg-contaminated sites in the Wanshan Hg mining area. The concentrations of both MeHg and cysteine in polished rice were higher than those in other rice tissues. A significant positive correlation between MeHg and cysteine in rice plants was found, especially in polished rice, indicating a close geochemical association between cysteine and MeHg. The translocation factor (TF) of cysteine showed behavior similar to that of the TF of MeHg, demonstrating that these two chemical species might share a similar transportation mechanism in rice plants. The accumulation of MeHg in rice plants may vary due to differences in the molar ratios of MeHg to cysteine and the presence of specific amino acid transporters. Our results suggest that cysteine plays a vital role in MeHg accumulation and transportation inside rice plants.

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., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Specimens of the Mediterranean sea anemone Anemonia viridis were exposed to methylmercury (MeHg) and bacterial infection to study their immune responses to a well-known toxic pollutant. Anemones were housed in laboratory conditions and divided into five experimental groups: 1. control (no microinjection); 2. filtered seawater + buffer injection; 3. filtered seawater + Escherichia coli injection; 4. MeHg + buffer injection; 5. MeHg + E. coli injection. Data showed an increase in antioxidant enzyme production compared to the constitutive condition, while methylmercury inhibited lysozyme production. The buffer inoculation had no statistically significant effects on the animals. In addition, electrophoretic and protease analyses revealed differences in the type of proteins produced, as well as a modulation of proteases depending on the treatment. The study demonstrated the immunomodulatory effect of the organic pollutant on A. viridis, validating its use as a model organism for marine coastal biomonitoring programmes and multiple stress studies., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Rapid, anthropogenic activity-induced global warming is a severe problem that not only raises water temperatures but also shifts aquatic environments by increasing the bioavailability of heavy metals (HMs), with potentially complicated effects on aquatic organisms, including small aquatic invertebrates. For this paper, we investigated the combined effects of temperature (23 and 28 °C) and methylmercury (MeHg) by measuring physiological changes, bioaccumulation, oxidative stress, antioxidants, and the mitogen-activated protein kinase signaling pathway in the marine rotifer Brachionus plicatilis. High temperature and MeHg adversely affected the survival rate, lifespan, and population of rotifers, and bioaccumulation, oxidative stress, and biochemical reactions depended on the developmental stage, with neonates showing higher susceptibility than adults. These findings demonstrate that increased temperature enhances potentially toxic effects from MeHg, and susceptibility differs with the developmental stage. This study provides a comprehensive understanding of the combined effects of elevated temperature and MeHg on rotifers. ENVIRONMENTAL IMPLICATION: Methylmercury (MeHg) is a widespread and harmful heavy metal that can induce lethal effects on aquatic organisms in even trace amounts. The toxicity of metals can vary depending on various environmental conditions. In particular, rising temperatures are considered a major factor affecting bioavailability and toxicity by changing the sensitivity of organisms. However, there are few studies on the combinational effects of high temperatures and MeHg on aquatic animals, especially invertebrates. Our research would contribute to understanding the actual responses of aquatic organisms to complex aquatic environments., Competing Interests: Declaration of Competing Interest The authors declare no competing financial interest., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Mercury is a hazardous pollutant of global concern. While advances have been made in identifying the detrimental effects caused by Hg species in phytoplankton, knowledge gaps remain regarding the metabolomic perturbations induced by inorganic mercury (Hg(II)) and monomethylmercury (MeHg) in these organisms. Diatoms represent a major phytoplankton group essential in various global biogeochemical cycles. The current study combined targeted metabolomics, bioaccumulation, and physiological response assays to investigate metabolic perturbations in diatom Cyclotella meneghiniana exposed for 2 h to nanomolar concentrations of Hg(II) and MeHg. Our findings highlight that such exposures induce reprogramming of the metabolism of amino acids, nucleotides, fatty acids, carboxylic acids and antioxidants. These alterations were primarily mercury-species dependent. MeHg exposure induced more pronounced reprogramming of the metabolism of diatoms than Hg(II), which led to less pronounced effects on ROS generation, membrane permeability and chlorophyll concentrations. Hg(II) treatments presented distinct physiological responses, with more robust metabolic perturbations at higher exposures. The present study provides first-time insights into the main metabolic alterations in diatom C. meneghiniana during short-term exposure to Hg species, deepening our understanding of the molecular basis of these perturbations., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier B.V. All rights reserved.)

Methylmercury (MeHg) production in aquatic ecosystems is a global concern because of its neurotoxic effect. Dissolved organic matter (DOM) plays a crucial role in biogeochemical cycling of Hg. However, owing to its complex composition, the effects of DOM on net MeHg production have not been fully understood. Here, the Hg isotope tracer technique combined with different DOM treatments was employed to explore the influences of DOM with divergent compositions on Hg methylation/demethylation and its microbial mechanisms in eutrophic lake waters. Our results showed that algae-derived DOM treatments enhanced MeHg concentrations by 1.42-1.53 times compared with terrestrial-derived DOM. Algae-derived DOM had largely increased the methylation rate constants by approximately 1-2 orders of magnitude compared to terrestrial-derived DOM, but its effects on demethylation rate constants were less pronounced, resulting in the enhancement of net MeHg formation. The abundance of hgcA and merB genes suggested that Hg-methylating and MeHg-demethylating microbiomes responded differently to DOM treatments. Specific DOM components (e.g., aromatic proteins and soluble microbial byproducts) were positively correlated with both methylation rate constants and the abundance of Hg-methylating microbiomes. Our results highlight that the DOM composition influences the Hg methylation and MeHg demethylation differently and should be incorporated into future Hg risk assessments in aquatic ecosystems., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Terrestrial soils in forested landscapes represent some of the largest mercury (Hg) reserves globally. Wildfire can alter the storage and distribution of terrestrial-bound Hg via reemission to the atmosphere or mobilization in watersheds where it may become available for methylation and uptake into food webs. Using data associated with the 2007 Moonlight and Antelope Fires in California, we examined the long-term direct effects of wildfire burn severity on the distribution and magnitude of Hg concentrations in riparian food webs. Additionally, we quantified the cross-ecosystem transfer of Hg from aquatic invertebrate to riparian bird communities; and assessed the influence of biogeochemical, landscape variables, and ecological factors on Hg concentrations in aquatic and terrestrial food webs. Benthic macroinvertebrate methylmercury (MeHg) and riparian bird blood total mercury (THg) concentrations varied by 710- and 760-fold, respectively, and Hg concentrations were highest in predators. We found inconsistent relationships between Hg concentrations across and within taxa and guilds in response to stream chemical parameters and burn severity. Macroinvertebrate scraper MeHg concentrations were influenced by dissolved organic carbon (DOC); however, that relationship was moderated by burn severity (as burn severity increased the effect of DOC declined). Omnivorous bird Hg concentrations declined with increasing burn severity. Overall, taxa more linked to in situ energetic pathways may be more responsive to the biogeochemical processes that influence MeHg cycling. Remarkably, 8 years post-fire, we still observed evidence of burn severity influencing Hg concentrations within riparian food webs, illustrating its overarching role in altering the storage and redistribution of Hg and influencing biogeochemical processes., (© 2024. This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.)

Mercury (Hg), a heavy metal pollutant worldwide, can be transformed into methylmercury (MeHg) by various aquatic microorganisms in water, thus accumulating along the aquatic food chain and posing a particular challenge to human health. Zooplankton plays a crucial role in aquatic ecosystems and serves as a major component of the food chain. To evaluate the effects of MeHg on the rotifer Brachionus plicatilis and reveal the underlying mechanism of these effects, we exposed B. plicatilis to MeHg by either direct immersion or by feeding with MeHg-poisoned Chlorella pyrenoidesa, respectively, and conducted a transcriptomic analysis. The results showed that B. plicatilis directly exposed to MeHg by immersion showed significant enrichment of the glutathione metabolism pathway for detoxification of MeHg. In addition, the exposure to MeHg by feeding induced a significant enrichment of lysosome and notch signaling pathways of rotifers, supporting the hypothesis that MeHg can induce autophagy dysfunction in cells and disturb the nervous system of rotifers. In two different routes of MeHg exposure, the pathway of cytochrome P450 in rotifers showed significant enrichment for resisting MeHg toxicity. Our results suggest further studies on the potential mechanism and biological responses of MeHg toxicity in other links of the aquatic food chain., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)