MeHg Accumulation Research Articles

Application of biochar and selenium together at low dose efficiently reduces mercury and methylmercury accumulation in rice grains

Irrespective of cost and ecological risk, literatures have reported that both biochar and selenium (Se) alone at high application rate exhibited positive effects on decreasing rice mercury (Hg) uptake in high Hg contaminated paddy soil. In this study, we investigated whether biochar and Se together at low dose could efficiently reduce the rice grain Hg and MeHg accumulation in the slight Hg-contaminated soil. Compared with control (CK), the Hg concentration of grains in the BC3, Se0.5, and BC3 + Se0.5 treatments decreased by 5.4 %, 38.3 %, and 48.5 %, respectively. Co-application of biochar and Se also decreased the methylmercury (MeHg) concentration in rice grains by 29.1–91.6 %. The decrease of Hg and MeHg level in rice grains for biochar and Se treatments could be attributed to the following mechanisms: (1) high Hg (primarily inorganic Hg) adsorption on biochar through its high hydroxyl groups and large specific surface area; (2) Increased dissolved organic carbon and cysteine contents in pore water after biochar application, which reduced the availability of soil Hg through complexation; (3) Decreased bioavailability of Hg in soil due to the formation of HgSe precipitation which inhibited Hg uptake and translation by rice plant; (4) Both biochar and Se facilitated the reduction of MeHg in soil. Our results indicate that co-application of biochar and Se at low dose is a promising method to effectively mitigate Hg accumulation in rice grains from the slight Hg-contaminated soil.

Converting flooded rice to dry farming can alleviate MeHg accumulation in grains

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.

Cumulative Effects of Watershed Disturbances and Run-of-river Dams on Mercury Cycling: Case Study and Recommendations for Environmental Managers.

Run-of-river power plants (ROR) represent the majority of hydroelectric plants worldwide. Their environmental impacts are not well documented and are believed to be limited, particularly regarding the contamination of food webs by methylmercury (MeHg), a neurotoxin. RORs are typically installed in small rivers where combined effects of watershed disturbances with dam construction can complicate environmental management. We report a multi-year case study on the Saint-Maurice River (Canada) where an unpredicted temporary increase in MeHg accumulation in predator fish was observed after the construction of two ROR plants. The associated pondages acted as sedimentation basins for mercury (Hg) and organic matter from a watershed disturbed by a forest fire and by logging. This fresh organic carbon likely fueled microbial MeHg production. Hg methylation was more associated with environmental conditions than to the presence of Hg, and main methylating microbial groups were identified. A constructed wetland was a site of significant Hg methylation but was not the main source of the fish Hg increase. Organic carbon degradation was the main driver of MeHg accumulation at the base of the food chain whereas trophic levels explained the variations at the top of the food chain. Overall, carbon cycling was a key driver of Hg dynamics in this system, and ROR plants can cause temporary (ca. 12 years) Hg increase in food webs when developed in disturbed watersheds, although this increase is smaller than for large reservoirs. Recommendations for future ROR construction are to establish a good environmental monitoring plan with initial high temporal resolution and to consider recent and potential watershed disturbances in the plan.

Spatiotemporal variation in methylmercury and related water quality variables in a temperate river under highly dynamic hydrologic conditions

The understanding of the essential environmental factors affecting the spatiotemporal variation in methylmercury (MeHg) in river water is limited to date, despite its importance for predicting the effect of ongoing climate change on MeHg accumulation in freshwater ecosystems. This study aimed to explore the variation in MeHg concentration and related environmental factors in the downstream zone of the Yeongsan River under highly dynamic hydrologic conditions by using water quality and hydrologic data collected from 1997 to 2022, and Hg and MeHg data collected from 2017 to 2022. The mean concentration of unfiltered MeHg was 35.7 ± 13.7 pg L−1 (n = 24) in summer and 26.7 ± 7.43 pg L−1 (n = 24) in fall. Dissolved oxygen (DO), conductivity, nitrate, and dissolved organic carbon (DOC) were determined to be the most influential variables in terms of MeHg variation based on the partial least squares regression model, and their effects on the MeHg concentration were negative, except for DOC. Heatmaps representing the similarity distances between temporal trends of hydrologic and water quality variables were constructed to determine fundamental factors related to the time-based variations in DO, conductivity, nitrate, and DOC using a dynamic time warping algorithm. The heatmap cluster analysis showed that the temporal trends of these variables were closely related to rainfall variation rather than irradiance or water temperature. Overall, biogeochemical factors directly related to in situ methylation rate of Hg(II)—rather than transport of Hg(II) and MeHg from external sources—mainly control the spatiotemporal variation of MeHg in the downstream zone of the Yeongsan River.

Hydrology and oxygen addition drive nutrients, metals, and methylmercury cycling in a hypereutrophic water supply reservoir

Impaired water quality in Mediterranean climate reservoirs is mainly associated with eutrophication and internal nutrient loading. To improve water quality in hypereutrophic Hodges Reservoir, California, United States, a hypolimnetic oxygenation system (HOS), using pure oxygen gas, was implemented in 2020. This study encompasses 3 years of pre-oxygenation data (2017–2019) and 2 years of post-oxygenation data (2020–2021) to understand the cycling of nutrients, metals, and mercury in the reservoir. During the wet year of 2017, mildly reduced conditions lasted until mid-summer in the enlarged reservoir. Nutrients and metals were seen in the hypolimnion including ammonia (~2 mg-N/L), manganese (~0.5 mg/L), phosphate (~0.5 mg-P/L), and sulfide (~10 mg/L). Production of methylmercury (MeHg), an important bioaccumulative toxin, was favored from April to June with a hypolimnetic accumulation rate of around 200 ng/m2·d. In contrast, the dry year of 2018 exhibited higher hypolimnetic concentrations of ammonia (~4 mg-N/L), manganese (~1 mg/L), phosphate (>0.5 mg-P/L), and sulfide (>15 mg/L). The rapid onset of highly reduced conditions in 2018 corresponded with low MeHg hypolimnetic accumulation (~50 ng/m2·d). It seems that mildly reduced conditions were associated with higher MeHg accumulation, while sulfidic, reduced conditions impaired inorganic mercury bioavailability for MeHg production and/or promoted microbial demethylation. Sulfide also appeared to act as a sink for iron via FeS precipitation, and potentially for manganese via MnS precipitation or manganese coprecipitation with FeS. Mass flux estimates for 2017–2019 indicate that much of the nutrients that accumulated in the hypolimnion moved via turbulent diffusion into the epilimnion at loading rates far exceeding thresholds predicting eutrophic conditions. After oxygenation in 2020–2021, the reservoir water column was highly oxidized but showed a lack of thermal stratification, suggesting reservoir operations in combination with HOS implementation inadvertently mixed the water column in this relatively shallow reservoir. Post-oxygenation, concentrations of ammonia, phosphate, manganese, and mercury in bottom waters all decreased, likely in response to oxidized conditions. Oxygenated bottom waters exhibited elevated nitrate, a byproduct of ammonia nitrification, and iron, a byproduct of FeS oxidation, indicating a lake-wide response to oxygenation.

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.

New Insights into MeHg Accumulation in Rice (Oryza sativa L.): Evidence from Cysteine.

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.

Effects of elevated CO2 on MeHg and IHg in rice

Methylmercury (MeHg) and, to a lesser extent, inorganic mercury (IHg) contamination of rice is a global public health concern, but little is known about how soil and grain Hg concentrations respond to elevated CO2 (ECO2), or how ECO2 alters movement of Hg through the soil-plant-grain system. To advance knowledge of how Hg contamination of rice will change in the future, this study explored the effect of elevated CO2 (ECO2, c. 800 ppm) on soil, iron plaque, root, stem/leaf, and grain concentrations of MeHg and IHg. We observed evidence that ECO2 increased accumulation of MeHg, but not IHg, in rice grain. For IHg, ECO2 did not alter its uptake from the soil, translocation through the plant, or concentration in rice grain. However, ECO2 did reduce uptake of IHg from the air into leaf tissues, likely as a result of the reduced stomatal conductivity and thus more limited direct uptake from the air.Methylmercury concentrations in the grain of plants grown at ECO2 were significantly higher than those of plants grown at ambient CO2. Moreover, MeHg concentrations were also elevated in stem/leaf (82 %) and root tissue (37 %) for ECO2 plants, although the root-tissue results were not statistically significant. In contrast, soil MeHg concentrations were virtually indistinguishable between treatments, indicating that higher rice grain MeHg concentrations were not likely due to higher microbial IHg methylation in soil. Plant uptake of MeHg into stem/leaves and grain from the soil was significantly greater in the ECO2 treatment; however, translocation patterns of MeHg within the plant itself did not differ between treatments. Notably, these patterns existed despite consistently lower transpiration in the ECO2 treatment, and thus less mass flow of solute towards and through the plant. Our results indicate that as CO2 concentrations rise, the human health risks related to MeHg in grain will likely increase.

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.

Organic matter, eutrophication, and increased mass accumulation rates in the Anthropocene are the main drivers of mercury concentrations and historical enrichment in Canadian lake sediments

AbstractMercury (Hg) contamination in the environment is a persistent issue as emissions from industry are ongoing and legacy cycling is prolonged. To quantify total mercury (total Hg) and methylmercury (MeHg) concentrations in lake sediments across a wide suite of temperate to subarctic lakes, measurements and modeling were conducted for 320 sites across Canada. Total Hg varied from 7 to 567 ng g−1 dry sediment with a mean (median) value of 148 (128) ng g−1 dry sediment, with lowest concentrations observed in eutrophic lakes of the Prairies and Boreal Plains. Average total Hg concentrations have increased twofold in contemporary sediments relative to their preindustrial pair. MeHg concentrations were generally low, with a mean of 0.8 ng g−1 dry sediment and this form representing on average 0.6% of the total contemporary mercury concentrations. Water column variables related to eutrophication were among the strongest predictors of contemporary total Hg, MeHg, and total Hg enrichment in the sediments. In lakes where sediment radiometric data were collected, contemporary total Hg accumulation rates were strongly related to longitude(+) and Hg atmospheric deposition(+). Latitude(−) and Hg atmospheric deposition(+) were the best predictors of MeHg accumulation rates. Chromophoric dissolved organic matter optical properties were key predictors of both total Hg concentrations and accumulation rates. Our work highlights the paramount importance of lake trophic state and the nature of organic matter as key predictors of lake sediment mercury metrics.

Gut microbiome play a crucial role in geographical and interspecies variations in mercury accumulation by fish

Mercury (Hg) contamination in fish has raised global concerns for decades. The Hg biotransformation can be manipulated by gut microbiome and it is found to have a substantial impact on the speciation and final fate of Hg in fish. However, the contribution of intestinal microbiota in geographical and interspecies variations in fish Hg levels has not been thoroughly understood. The present study compared the Hg levels in wild marine fish captured from two distinct regions in South China sea. We observed a quite “ironic” phenomenon that MeHg levels in carnivorous fish from a region with minimal human impacts (Xisha Islands, 92 ± 7.2 ng g−1 FW) were much higher than those from a region with severe human impacts (Daya Bay, 19 ± 0.41 ng g−1 FW). Furthermore, the results showed that gut microbiome determined Hg biotransformation and played a crucial role in the variances in fish Hg levels across different geographical locations and species. The intestinal methylators, rather than demethylators, were more significant in affecting Hg biotransformation in fish. The carnivorous species in Xisha Islands exhibited a higher abundance of intestinal methylators, leading to higher MeHg accumulation. Besides, the gut microbiome could be shaped in response to the elevated Hg levels in these fish, which may benefit their adaptation to Hg toxicity and overall health preservation. However, anthropogenic activities (particularly overfishing) in Daya Bay have severely affected the fish population, disrupting the reciprocal relationships between fish and intestinal microbiota and rendering them more susceptible to pathogenic microbes. Overall, this study provided a comprehensive understanding of the role of gut microbiome in Hg bioaccumulation in fish and offered valuable insights into the co-evolutionary dynamics between fish and gut microbiome in the presence of Hg exposure.

Insights into the reduction of methylmercury accumulation in rice grains through biochar application: Hg transformation, isotope fractionation, and transcriptomic analysis

Methylmercury (MeHg), a potent neurotoxin, easily moves from the soil into rice plants and subsequently accumulates within the grains. Although biochar can reduce MeHg accumulation in rice grains, the precise mechanism underlying biochar-mediated responses to mercury (Hg) stress, specifically regarding MeHg accumulation in rice, remains poorly understood. In the current study, we employed a 4% biochar amendment to remediate Hg-contaminated paddy soil, elucidate the impacts of biochar on MeHg accumulation through a comprehensive analysis involving Hg isotopic fractionation and transcriptomic analyses. The results demonstrated that biochar effectively lowered the levels of MeHg in paddy soils by decreasing bioavailable Hg and microbial Hg methylation. Furthermore, biochar reduced the uptake and translocation of MeHg in rice plants, ultimately leading to a reduction MeHg accumulation in rice grains. During the process of total mercury (THg) uptake, biochar induced a more pronounced negative isotope fractionation magnitude, whereas the effect was less pronounced during the upward transport of THg. Conversely, biochar caused a more pronounced positive isotope fractionation magnitude during the upward transport of MeHg. Transcriptomics analyses revealed that biochar altered the expression levels of genes associated with the metabolism of cysteine, glutathione, and metallothionein, cell wall biogenesis, and transport, which possibly enhance the sequestration of MeHg in rice roots. These findings provide novel insights into the effects of biochar application on Hg transformation and transport, highlighting its role in mitigating MeHg accumulation in rice.

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.

Variability in methylmercury exposure across migratory terrestrial bird species: Influencing factors, biomagnification and potential risks

Despite China's considerable mercury (Hg) emissions, monitoring of methylmercury (MeHg) levels in its terrestrial environments remains limited. This study examined the occurrence and accumulation of MeHg in body feathers of 12 migratory terrestrial bird species originating from Siberia and northeastern China. Considerable variations in foraging habits and MeHg levels were observed among these species. Accipiters, including Eurasian and Japanese sparrowhawks (A. gularis and A. nisus) and northern goshawk (A. gentilis), along with insectivorous songbirds including grey-backed thrush (T. hortulorum) and orange-flanked bluetail (T. cyanurus), showed notable levels of MeHg (0.62–1.20 mg/kg). Up to 25 % of the individuals within these species were classified as low-risk based on feather Hg toxicity thresholds, while the remaining species fell into the no-risk category. Despite showing enriched δ15N, MeHg concentrations in short-eared and long-eared owls (A. flammeus and A. otus) were lower than in sparrowhawks. The herbivorous oriental turtle dove (S. orientalis) exhibited significantly lower MeHg levels compared to all other species. There was a significant positive correlation between MeHg concentrations and δ15N across species, highlighting the substantial biomagnification potential of MeHg within the terrestrial food web. Additionally, we found significantly higher MeHg levels in adults than juveniles in both sparrowhawk species. Our results demonstrate the effectiveness of utilizing migratory bird feathers for monitoring terrestrial Hg contamination, and underscore the importance of further assessment.

Effects of temperature oscillations on the accumulation of mercury and other trace metals in freshwater zooplankton (Daphnia magna)

Whereas many aquatic species experience daily temperature changes, it is unclear whether temperature fluctuations can affect the accumulation of trace metal independently from changes in mean temperature. Here, the impact of oscillating temperature (MTosc: 7/23 °C, 24 h/cycle) on the accumulation of both inorganic Hg (IHg) and monomethylmercury (MeHg) in Daphnia magna was investigated, by comparing it to a constant temperature treatment with the same average temperature (MTconst: 15 °C). The effects of mean temperature were tested by comparing this latter to a similar treatment with higher temperature (HTconst: 23 °C). Trophic pathway accumulation was estimated by using Chlorella vulgaris labeled with stable Hg isotopes, whereas the water pathway accumulation was estimated by directly spiking Hg isotope solutions into the D. magna incubators. The concentrations of IHg decreased in D. magna under oscillating temperature conditions for both trophic and water pathways by at least 42 % and 25 %, respectively, compared to the MTconst treatment. In contrast, the accumulation of MeHg was reduced only in the trophic pathway in these conditions, whereas it was enhanced in the water pathway. Patterns similar to IHg were observed for Fe, Zn, and Cu in the trophic pathway, but only for Cu in the water pathway. In contrast, no difference on the accumulation of rare earth elements was observed among temperature treatments. These results shed a new light on trace metal accumulation under near-realistic temperature conditions.

Metabolic pathways of methylmercury in rotifer Brachionus plicatilis

Methylmercury (MeHg) readily accumulates in aquatic organisms while transferring and amplifying in the aquatic food chains. This study firstly explores the in vivo accumulation sites and metabolic regulation of MeHg in the rotifer Brachionus plicatilis by aggregation-induced emission fluorogen (AIEgen) and metabolomics. Fluorescent image analysis by AIEgen showed that MeHg in B. plicatilis mainly occured in the ciliary corona, esophagus, mastax, stomach and intestine in the direct absorption group. In the other group, where B. plicatilis were indirectly supplied with MeHg via food intake, the accumulation of MeHg in the rotifer occurred in the ciliary corona, various digestive organs, and the pedal gland. However, the MeHg accumulated in the rotifer is difficult to metabolize outside the body. Metabolomics analysis showed that the significant enrichment of ABC transporters was induced by the direct exposure of rotifers to dissolved MeHg. In contrast, exposure of rotifers to MeHg via food intake appeared to influence carbon, galactose, alanine, aspartate and glutamate metabolisms. Besides, the disturbed biological pathways such as histidine metabolism, beta-alanine metabolism and pantothenate and CoA biosynthesis in rotifers may be associated with L-aspartic acid upregulation in the feeding group. The significant enrichment of ABC transporters and carbon metabolism in rotifers may be related to the accumulation of MeHg in the intestine of rotifers. In both pathways of MeHg exposure, the arginine biosynthesis and metabolism of rotifers were disturbed, which may support the hypothesis that rotifers produce more energy to resist MeHg toxicity. This study provides new insight into the accumulation and toxicity mechanisms of MeHg on marine invertebrates from the macro and micro perspectives.

Sulfate-reduction and methanogenesis are coupled to Hg(II) and MeHg reduction in rice paddies

Methylmercury (MeHg) produced in rice paddies is the main source of MeHg accumulation in rice, resulting in high risk of MeHg exposure to humans and wildlife. Net MeHg production is affected by Hg(II) reduction and MeHg demethylation, but it remains unclear to what extent these processes influence net MeHg production, as well as the role of the microbial guilds involved. We used isotopically labeled Hg species and specific microbial inhibitors in microcosm experiments to simultaneously investigate the rates of Hg(II) and MeHg transformations, as well as the key microbial guilds controlling these processes. Results showed that Hg(II) and MeHg reduction rate constants significantly decreased with addition of molybdate or BES, which inhibit sulfate-reduction and methanogenesis, respectively. This suggests that both sulfate-reduction and methanogenesis are important processes controlling Hg(II) and MeHg reduction in rice paddies. Meanwhile, up to 99% of MeHg demethylation was oxidative demethylation (OD) under the incubation conditions, suggesting that OD was the main MeHg degradative pathway in rice paddies. In addition, [202Hg(0)/Me202Hg] from the added 202Hg(NO3)2 was up to 13.9%, suggesting that Hg(II) reduction may constrain Hg(II) methylation in rice paddies at the abandoned Hg mining site. This study improves our understanding of Hg cycling pathways in rice paddies, and more specifically how reduction processes affect net MeHg production and related microbial metabolisms.

The divergent effects of nitrate and ammonium application on mercury methylation, demethylation, and reduction in flooded paddy slurries

The production of methylmercury (MeHg) in flooded paddy fields determines its accumulation in rice grains; this, in turn, results in MeHg exposure risks for not only rice-eating humans but also wildlife. Nitrogen (N) fertilizers have been widely applied in rice cultivation fields to supply essential nutrients. However, the effects of N fertilizer addition on mercury (Hg) transformations are not unclear. This limits our understanding of MeHg formation in rice paddy ecosystems. In this study, we spiked three Hg tracers (200HgII, Me198Hg, and 202Hg0) in paddy slurries fertilized with urea, ammonium, and nitrate. The influences of N fertilization on Hg methylation, demethylation, and reduction and the underlying mechanisms were elucidated. The results revealed that dissimilatory nitrate reduction was the dominant process in the incubated paddy slurries. Nitrate addition inhibited HgII reduction, HgII methylation, and MeHg demethylation. Competition between nitrates and other electron acceptors (e.g., HgII, sulfate, or carbon dioxide) under dark conditions was the mechanism underlying nitrate-regulated Hg transformation. Ammonium and urea additions promoted HgII reduction, and anaerobic ammonium oxidation coupled with HgII reduction (Hgammox) was likely the reason. This work highlighted that nitrate addition not only inhibited HgII methylation but also reduced the demethylation of MeHg and therefore may generate more accumulation of MeHg in the incubated paddy slurries. Findings from this study link the biogeochemical cycling of N and Hg and provide crucial knowledge for assessing Hg risks in intermittently flooded wetland ecosystems.

Effects of diet composition on gut microbiome and mercury biotransformation in the gobyfish

Mercury (Hg) biotransformation (methylation and demethylation) could play a key role in affecting the final Hg speciation and level in fish. The gut microbiota was identified to be involved in this process. Diet is recognized to greatly influence the gut microbiome, whereas the impact of food composition on Hg biotransformation in fish has yet to be addressed. The study investigated the biotransformation and bioaccumulation of Hg in the gobyfish (Mugilogobius chulae) under different food choices (natural prey and artificial food) and evaluated the role of gut microbiome in these processes. The results showed that different diet composition significantly affected the gut microbiome and subsequently resulted in varied phenomenon of Hg biotransformation within fish body. Significant demethylation (0.33 % d−1) was only observed in the natural prey (brine shrimp) treatment, whereas methylation was occurred extremely slowly (0.013 % d−1) only in the artificial food (commercial dry pellets) treatment. Furthermore, the growth of demethylators was also enhanced in the natural prey treatment, which contributed to the demethylation process in fish. Furthermore, the gut microbial structure of gobyfish was greatly altered by different diet composition. This study highlights the significance of food choices in the minimization of Hg contamination in aquaculture. Incorporating natural prey into fish diets could be a better choice to balance the fish production and control MeHg levels. CapsuleDiet composition greatly affects the gut microbial composition, and natural prey could help to reduce the potential of MeHg accumulation by fish.

Mercury and methylmercury in Hg-contaminated paddy soil and their uptake in rice as regulated by DOM from different agricultural sources.

In this study, from the perspectives of structural and compositional variations of soil-dissolved organic matter (DOM), we explored the effects of agricultural DOM inputs on methylmercury (MeHg) accumulation in the soil and mercury (Hg) bioaccumulation in rice grains. Pot experiments with the addition of DOMs from maize straw (MaS), rape straw (RaS), rice straw (RiS), composted rice straw (CRiS), cow dung (CD), and composted cow dung (CCD) were then conducted. Results showed that, relative to the control, the DOM amendment from each agricultural source elevated MeHg concentrations in the soil, with an increase of 18-227%, but only parts of DOMs elevated total dissolved Hg (DHg) and MeHg (DMeHg) concentrations in pore water. Among all DOM species, RiS, CRiS, and CCD significantly increased total Hg (THg) and MeHg contents in rice grains by 34-64% and 32-118%, respectively. Compared with RiS, THg and MeHg contents in rice grains in the CRiS treatment decreased slightly, which was consistent with the distributions of DHg and DMeHg concentrations in pore water and the aromaticity variation of soil DOM. In contrast, the CCD input significantly enhanced the enrichment of THg and MeHg in rice grains relative to CD because it significantly reduced the humification of soil DOM at all rice-growing stages while increasing the low-molecular-weight fractions in soil DOM. The THg and MeHg contents in the rice grains were significantly lower treated by RaS than those by MaS and RiS, which may be related to the higher sulfur-containing compounds such as sulfate and cysteine in rape straw or its DOM solution. Overall, DOM amendment from different agricultural sources resulted in significantly discriminative effects on the MeHg accumulation in soil and Hg enrichment in rice in the Hg-contaminated paddy field by shaping soil DOM properties.