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Nitrogen (N 2 )-fixing legumes can be used for phytoremediation of toxic heavy metal Mercury (Hg) contaminated soil, but N 2 -fixation highly relies on phosphorus (P) availability for nodule formation and functioning. Here, we characterized the significance of P deficiency for Hg accumulation and toxicity in woody legume plants. Consequences for foliar and root traits of rhizobia inoculation, Hg exposure (+Hg) and low P (-P) supply, individually and in combination were characterized at both the metabolite and transcriptome levels in seedlings of two Robinia pseudoacacia L. provenances originating from contrasting climate and soil backgrounds, i.e., GS in northwest and the DB in northeast China. Our results reveal that depleted P mitigates the toxicity of Hg at the transcriptional level. In leaves of Robinia depleted P reduced oxidative stress and improved the utilization strategy of C, N and P nutrition; in roots depleted P regulated the expression of genes scavenging oxidative stress and promoting cell membrane synthesis. Rhizobia inoculation significantly improved the performance of both Robinia provenances under individual and combined +Hg and -P by promoting photosynthesis, increasing foliar N and P content and reducing H 2 O 2 and MDA accumulation despite enhanced Hg uptake. DB plants developed more nodules, had higher biomass and accumulated higher Hg amounts than GS plants and thus are suggested as the high potential Robinia provenance for future phytoremediation of Hg contaminated soils with P deficiency., Competing Interests: Declaration of Competing Interest The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2024 Elsevier B.V. All rights reserved.)

The tree ring has been regarded as an emerging archive to reconstruct historical atmospheric mercury (Hg) trends, but with the large knowledge gaps in the reliability. In this study, we comprehensively evaluated the Hg source, radial translocation and age effect of Masson pine (Pinus massoniana) tree ring at Mt. Jinyun in Chongqing, to assess the suitability of such tree ring as the archive of atmospheric Hg. Results showed that distinct variabilities among Masson pine tree-ring Hg concentration profiles. The Hg concentration significantly increased along with stem height (P < 0.05), indicating the Hg in tree rings mainly derived from foliage uptake atmospheric Hg. We found a distinct age effect that the tree ring of young trees had the higher Hg concentration. Besides, we used the advection-diffusion model to demonstrate how Hg concentration shifted by the advection or/and diffusion in tree rings. The modeling results showed that the advection induced radial translocation during the young growth period of tree was a plausible mechanism to result in the tree-ring Hg record largely different from the trend of anthropogenic Hg emissions in Chongqing. We finally suggest that in further Hg dendrochemistry, better discarding the tree-ring Hg profile of the young growth period to reduce impacts of the radial translocation and age effect., 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 article., (Copyright © 2022. Published by Elsevier B.V.)

Biodegradation of soil organic matter (SOM), which involves greenhouse gas (GHG) emissions, plays an essential role in the global carbon cycle. Over the past few decades, this has become an important research focus, particularly in natural ecosystems. SOM biodegradation significantly affects contaminants in the environment, such as mercury (Hg) methylation, producing highly toxic methylmercury (MeHg). However, the potential link between GHG production from SOM turnover in contaminated soils and biogeochemical processes involving contaminants remains unclear. In this study, we investigated the dynamics of GHG, MeHg production, and the relationship between biogeochemical processes in soils from two typical Hg mining sites. The two contaminated soils have different pathways, explaining the significant variations in GHG and MeHg production. The divergence of the microbial communities in these two biogeochemical processes is essential. In addition to the microbial role, abiotic factors such as Hg species can significantly affect MeHg production. On the other hand, we found an inverse relationship between CH 4 and MeHg, suggesting that carbon emission reduction policies and management could inadvertently increase the MeHg levels. This highlights the need for an eclectic approach to organic carbon sequestration and contaminant containment. These findings suggest that it is difficult to establish a general pattern to describe and explain the SOM degradation and MeHg production in contaminated soils within the specific scenarios. However, this study provides a case study and helpful insights for further understanding the links between environmental risks and carbon turnover in Hg mining 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.)

Multifunctional lakes are highly susceptible to anthropogenic influences, potentially introducing exogenous pollutants or nutrients into aquatic sediments. This, in turn, affects the mercury (Hg) methylation in the sediments. This study was conducted in the Changshou Lake, a representative multifunctional lake in southwestern China, with a specific focus on investigating the Hg variations, the potential of Hg methylation, and the influential factors affecting the methylation process within sediments across different functional areas. The results revealed significant variations in total Hg concentrations between the ecological culture area (area I), the ecological tourism area (area II), and the wetland protection area (area III), suggesting the possibility of exogenous Hg introduction associated with human activities. Furthermore, sediments from areas I and II displayed a greater potential for Hg methylation. This was ascribed to the enhanced diversity and relative abundance of Hg-methylating microorganisms, especially Geobacteraceae, induced by elevated levels of dissolved organic carbon in these two areas from human activities like historical cage culture. This study provides evidence that anthropogenic activities enhance the process of Hg methylation in the sediments of multifunctional lakes, highlighting the necessity of implementing comprehensive scientific water quality management practices to mitigate the negative impacts of human influences on these unique 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.)

Biochar could reshape microbial communities, thereby altering methylmercury (MeHg) concentrations in rice rhizosphere and seeds. However, it remains unclear whether and how biochar amendment perturbs microbe-mediated MeHg production in mercury (Hg) contaminated paddy soil. Here, we used pinecone-derived biochar and its six modified biochars to reveal the disturbance. Results showed that selenium- and chitosan-modified biochar significantly reduced MeHg concentrations in the rhizosphere by 85.83% and 63.90%, thereby decreasing MeHg contents in seeds by 86.37% and 75.50%. The two modified bicohars increased the abundance of putative Hg-resistant microorganisms Bacillus, the dominant microbe in rhizosphere. These reductions about MeHg could be facilitated by biochar sensitive microbes such as Oxalobacteraceae and Subgroup&#95;7. Pinecone-derived biochar increased MeHg concentration in rhizosphere but unimpacted MeHg content in seeds was observed. This biochar decreased the abundance in Bacillus but enhanced in putative Hg methylator Desulfovibrio. The increasing MeHg concentration in rhizosphere could be improved by biochar sensitive microbes such as Saccharimonadales and Clostridia. Network analysis showed that Saccharimonadales and Clostridia were the most prominent keystone taxa in rhizosphere, and the three biochars manipulated abundances of the microbes related to MeHg production in rhizosphere by those biochar sensitive microbes. Therefore, selenium- and chitosan-modified biochar could reduce soil MeHg production by these microorganisms, and is helpful in controlling MeHg contamination in rice., 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.)

Previous studies have suggested that growth dilution may be an important factor contributing to the low fish Hg levels in China. To evaluate the impact of growth rate to MeHg bioaccumulation in fish in the Three Gorges Reservoir (TGR), this study used two fish species, Aristichthys nobilis (A. nobilis) and Coilia nasus (C. nasus), which differ significantly in their growth rates. A combined bioenergetic-toxicokinetic model was used to simulate methylmercury (MeHg) concentrations in these two species. The model simulations were compared with the field data and showed good fits. It explained 44.0% and 46.5% of the variation in MeHg concentrations in A. nobilis and C. nasus, respectively. Sensitivity analysis revealed that growth rate accounted for 50.9% and 16.0% of MeHg concentrations in A. nobilis and C. nasus, respectively. This indicated that growth rate was the most critical factor affecting MeHg concentrations in fast-growing fish, such as A. nobilis. However, in species with low growth rate, such as C. nasus, the effect of growth rate was not as prominent as that in fast-growing fish. As a result, MeHg elimination rates and diet MeHg levels could offset the effect of growth, and become the decisive factors for MeHg concentrations in slow-growing fish., 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.)

Interaction of different environmental constrains pose severe threats to plants that cannot be predicted from individual stress exposure. In this context, mercury (Hg), as a typical toxic and hazardous heavy metal, has recently attracted particular attention. Nitrogen (N 2 )-fixing legumes can be used for phytoremediation of Hg accumulation, whereas N availability could greatly affect its N 2 -fixation efficiency. However, information on the physiological responses to combined Hg exposure and excess N supply of woody legume species is still lacking. Here, we investigated the interactive effects of rhizobia inoculation, Hg exposure (+Hg), and high N (+N) supply, individually and in combination (+N*Hg), on photosynthesis and biochemical traits in Robinia pseudoacacia L. seedlings of two provenances, one from Northeast (DB) and one from Northwest (GS) China. Our results showed antagonistic effects of combined + N*Hg exposure compared to the individual treatments that were provenance-specific. Compared to individual Hg exposure, combined + N*Hg stress significantly increased foliar photosynthesis (+50.6%) of inoculated DB seedlings and resulted in more negative (-137.4%) δ 15 N abundance in the roots. Furthermore, combined + N*Hg stress showed 47.7% increase in amino acid N content, 39.4% increase in NR activity, and 14.8% decrease in MDA content in roots of inoculated GS seedlings. Inoculation with rhizobia significantly promoted Hg uptake in both provenances, reduced MDA contents of leaves and roots, enhanced photosynthesis and maintained the nutrient balance of Robinia. Among the two Robinia provenances investigated, DB seedlings formed more nodules, had higher biomass and Hg accumulation than GS seedlings. For example, total Hg concentrations in leaves and roots and total biomass of inoculated DB seedlings were 1.3,1.9 and 3.4 times higher than in inoculated GS seedlings under combined + N*Hg stress, respectively. Therefore, the DB provenance is considered to possess a higher potential for phytoremediation of Hg contamination compared to the GS provenance in environments subjected to N deposition., 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 Ltd. All rights reserved.)

The Three Gorges Reservoir (TGR) holds the distinction of being China's largest reservoir, and the presence of pollutants in the fish from the reservoir have a direct impact on the health of local residents. Thus, 349 fish specimens of 21 species and 1 benthos (Bellamya aeruginosas) were collected from four typical tributaries of the TGR from 2019 to 2020. These specimens were analyzed for the concentrations of total mercury (THg) and methylmercury (MeHg), and some representative samples were tested for δ 13 C and δ 15 N values to reveal the characteristics of bioaccumulation and biomagnification. The maximum safe daily consumption was estimated based on the oral reference dose (0.1 μg kg -1 bw/day according to US-EPA, 2017). The results showed that the mean THg and MeHg concentrations in fish from the TGR tributaries were 73.18 ± 49.21 ng g -1 and 48.42 ± 40.66 ng g -1 , respectively, with the trophic magnification factors (TMFs) of THg and MeHg being 0.066 and 0.060, respectively. Among all the fish species in the tributaries, the highest daily maximum safe consumption amount was 1253.89 g for S. asotus consumed by adults, while the lowest was 62.88 g for C. nasus consumed by children., 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.)

The plant microbiota can affect plant health and fitness by promoting methylmercury (MeHg) production in paddy soil. Although most well-known mercury (Hg) methylators are observed in the soil, it remains unclear how rice rhizosphere assemblages alter MeHg production. Here, we used network analyses of microbial diversity to identify bulk soil (BS), rhizosphere (RS) and root bacterial networks during rice development at Hg gradients. Hg gradients greatly impacted the niche-sharing of taxa significantly relating to MeHg/THg, while plant development had little effect. In RS networks, Hg gradients increased the proportion of MeHg-related nodes in total nodes from 37.88% to 45.76%, but plant development enhanced from 48.59% to 50.41%. The module hub and connector in RS networks included taxa positively (Nitrososphaeracea, Vicinamibacteraceae and Oxalobacteraceae) and negatively (Gracilibacteraceae) correlating with MeHg/THg at the blooming stage. In BS networks, Deinococcaceae and Paludibacteraceae were positively related to MeHg/THg, and constituted the connector at the reviving stage and the module hub at the blooming stage. Soil with an Hg concentration of 30 mg kg -1 increased the complexity and connectivity of root microbial networks, although microbial community structure in roots was less affected by Hg gradients and plant development. As most frequent connector in root microbial networks, Desulfovibrionaceae did not significantly correlate with MeHg/THg, but was likely to play an important role in the response to Hg stress., 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 Author(s). Published by Elsevier Ltd.. All rights reserved.)

Pioneer habitat-adapted bermudagrass is prevalent in the water-level-fluctuating zone of the Three Gorges Reservoir area. This study was performed to explore the response characteristics of dissolved organic matter (DOM) qualities to bermudagrass decomposition and their regulation in the distribution and release of mercury (Hg) and methylmercury (MeHg) in the soil-water system. Compared to the control, the bermudagrass decomposition resulted in a great increase in the protein-like components in the water in the initial stages (p < 0.01), but it also greatly reduced the humification degree of water DOM (p < 0.01). However, it accelerated the consumption of protein-like components, the humification rate, and the synthesis of humic-like DOM in the water over time. This changing pattern of the DOM qualities resulted in an initial elevation and a subsequent great decrease in the dissolved Hg and MeHg concentrations in the pore water, which ultimately reduced their release levels into the overlying water by 26.50% and 54.42%, respectively, compared to the control. Our results indicate the potential inhibitory effects of short-term bermudagrass decomposition caused by flooding and how decomposition affects the release of total Hg and MeHg by shaping the DOM qualities, and they have implications for similar aquatic systems in which herbaceous plants are frequently decomposed after submergence., (© 2023. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

To quantify impacts of vegetation and topographic factors on heavy metal accumulation in montane forests, we assessed the spatial distribution and determined the sources of mercury (Hg), cadmium (Cd), lead (Pb), chromium (Cr), copper (Cu) and zinc (Zn) in timberline forests of Gongga Mountain. Our results show that vegetation type has little impact on the soil Hg, Cd and Pb concentrations. The soil concentrations of Cr, Cu and Zn are controlled by litter return, moss and lichen biomass, and canopy interception, with the highest concentrations in shrub forest. In contrast to other forests, the soil Hg pool in coniferous forest is significantly high due to the elevated Hg concentration and greater biomass production in litter. However, the soil pool sizes of Cd, Cr, Cu and Zn show a distinct increase along the elevation, which are attributed to the elevated heavy metal inputs from litter and moss, as well as the greater cloud water-induced atmospheric heavy metal depositions. The highest Hg concentrations of the aboveground parts of plant are in the foliage and bark, while the concentrations of Cd, Pb, Cr, Cu and Zn in the branch and bark are the highest. The decreased biomass density leads to a downward trend in the total vegetation pool sizes of Hg, Cd, Pb, Cr, Cu and Zn by 0.4-4.4 times with increasing elevation. The statistical analysis finally suggests that Hg, Cd and Pb mainly originate from anthropogenic atmospheric deposition, whereas Cr, Cu and Zn are mainly from natural sources. Our results highlight the importance of vegetation types and terrain conditions on distribution patterns of heavy metal in alpine forests., 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.)

Rice consumption is an essential cause of mercury (Hg) exposure for humans in Asia. However, the mechanism of Hg transport and accumulation in rice plants (Oryza sativa L.) remains unclear. Here, rice genotypes with contrasting Hg uptake and translocation abilities, i.e. H655 (high Hg-accumulator) and H767 (low Hg-accumulator), were selected from 261 genotypes. Through comparative physiological and transcriptome analyses, we investigated the processes responsible for the relationship between Hg accumulation, transport and tolerance. The results showed significant stimulation of antioxidative metabolism, particularly glutathione (GSH) accumulation, and up-regulated expression of regulatory genes of glutathione metabolism for H655, but not for H767. In addition, up-regulated expression of GSH S-transferase (GST) and OsPCS1 in H655 that catalyzes the binding of Hg and GSH, enhances the Hg detoxification capacity, while high-level expression of YSL2 in H655 enhances the transport ability for Hg. Conclusively, Hg accumulation in rice is a consequence of enhanced expression of genes related to Hg binding with GSH and Hg transport. With these results, the present study contributes to the selection of rice genotypes with limited Hg accumulation and to the mitigation of Hg migration in food chains thereby enhancing nutritional safety of Hg-polluted rice fields., 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 Ltd. All rights reserved.)

Long-range transport and atmospheric deposition of gaseous mercury (Hg 0 ) result in significant accumulation of Hg in the Qinghai-Tibetan Plateau (QTP). However, there are significant knowledge gaps in understanding the spatial distribution and source contribution of Hg in the surface soil of the QTP and factors influencing Hg accumulation. In this study, we comprehensively investigated Hg concentrations and isotopic signatures in the QTP to address these knowledge gaps. Results show that the average Hg concentration in the surface soil ranks as follows: forest (53.9 ± 36.9 ng g -1 ) > meadow (30.7 ± 14.3 ng g -1 ) > steppe (24.5 ± 16.1 ng g -1 ) > shrub (21.0 ± 11.6 ng g -1 ). Hg isotopic mass mixing and structural equation models demonstrate that vegetation-mediated atmospheric Hg 0 deposition dominates the Hg source in the surface soil, with an average contribution of 62 ± 12% in forests, followed by 51 ± 10% in shrub, 50 ± 13% in steppe, and 45 ± 11% in meadow. Additionally, geogenic sources contribute 28-37% of surface soil Hg accumulation, and atmospheric Hg 2+ inputs contribute 10-18% among the four types of biomes. The Hg pool in 0-10 cm surface soil over the QTP is estimated as 8200 ± 3292 Mg. Global warming, permafrost degradation, and anthropogenic influences have likely perturbed Hg accumulation in the soil of QTP.

The particular condition of the water-level-fluctuation zone (WLFZ) in the Three Gorges Reservoir (TGR), the largest hydroelectric reservoir in China, raises great concerns about mercury (Hg) contamination and ecological risk. In addition, previous research found that soil organic carbon (SOC) plays an essential role in controlling Hg distribution and speciation. However, there is minimal information on the Hg storage distribution and their relationships with SOC in the WLFZ in TGR. This study investigated Hg distribution, storage, and their relationships with SOC in the surface soils in WLFZ. The results showed that the total Hg (THg) content in the surface soils ranged from 18.40 to 218.50 ng g -1 , with an average value of 78.17 ± 41.92 ng g -1 . About 89% of samples had THg content above the background value in Chongqing, showing specific enrichment of Hg in WLFZ due to contamination in the TGR. The surface soils have low SOC, with an average value of 8.10 ± 3.90 g kg -1 . Moreover, THg content showed consistent distribution with the SOC in WLFZ, with a significantly positive correlation ( R = 0.52, p < 0.01, n = 242). THg storage (201.82 ± 103.46 g ha -1 ) in the surface soils was also significantly positively correlated with the SOC storage ( R = 0.47, p < 0.01, n = 242). The reduced SOC sequestration, due to the periodical alternative "flooding-draining" and frequent reclamation and utilization of WLFZ, decreased the Hg adsorption in soil. Those might result in the re-release of Hg into waters when WLFZ is flooded. Therefore, more attention should be directed towards Hg cycling and the consequent environmental risks in the TGR region.

Previous research has found total mercury (THg) and methylmercury (MeHg) levels increase with litterfall decay, thus suggesting litterfall decomposition plays an essential role in the biogeochemical transformation of mercury (Hg). However, it remains unclear how Hg accumulates in the decaying litter, how bacterial taxa networks vary and what roles various microorganisms play during litterfall decomposition, especially nitrogen (N)-fixing, MeHg-degrading and Hg-methylating microbes. Here, we demonstrated as degradation proceeded, a gradually-complex network evolved for litterfall bacteria for the subtropical mixed broadleaf-conifer (MBC) forest, whereas a relatively static network existed for the evergreen broadleaf (EB) forest. N-fixing and MeHg-degrading bacteria dominated throughout litterfall decomposition process, with relative abundances of N-fixing genera and nifH copies maximum and relative abundances of MeHg-degrading bacteria and merAB copies minimum in summer. Hence, N-fixing bacteria likely mediate THg increase in the decomposing litterfall, while MeHg enhancement may be regulated by aerobic MeHg-degrading microbes which can transform MeHg to inorganic divalent Hg (Hg 2+ ) or further to elemental Hg (Hg 0 ). Together, this work elucidates variations of N-fixing and MeHg-degrading microbes in decaying litterfall and their relationships with Hg accumulation, providing novel insights into understanding the biogeochemical cycle of Hg in the forest ecosystem., 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 © 2022 Elsevier B.V. All rights reserved.)

Both inorganic and organic fertilizers are widely used to increase rice yield. However, these fertilizers are also found to aggravate mercury methylation and methylmercury (MeHg) accumulation in paddy fields. The aim of this study was to reveal the mechanisms of inorganic and organic fertilizers on MeHg accumulation in rice grains, which are not yet well understood. Potting cultures were conducted in which different fertilizers were applied to a paddy soil. The results showed that both inorganic and organic fertilizers increased MeHg concentrations rather than biological accumulation factors (BAFs) of MeHg in mature rice grains. Inorganic fertilizers, especially nitrogen fertilizer, enhanced the bioavailability of mercury and the relative amount Hg-methylating microbes and therefore intensified mercury methylation in paddy soil and MeHg accumulation in rice grains. Unlike inorganic fertilizers, organic matter (OM) in organic fertilizers was the main reason for the increase of MeHg concentrations in rice grains, and it also could immobilize Hg in soil when it was deeply degraded. The enhancement of MeHg concentrations in rice grains induced by inorganic fertilizers (5.18-41.69%) was significantly (p < 0.05) lower than that induced by organic fertilizers (80.49-106.86%). Inorganic fertilizers led to a larger increase (50.39-99.28%) in thousand-kernel weight than MeHg concentrations (5.18-41.69%), resulting in a dilution of MeHg concentrations in mature rice grains. Given the improvement of soil properties by organic fertilizer, increasing the proportion of inorganic fertilizer application may be a better option to alleviate MeHg accumulation in rice grains and guarantee the rice yield in the agricultural production., 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 © 2022. Published by Elsevier Ltd.)

To explore the effects of herbaceous plants on mercury (Hg) behaviors after flooding in the water-level fluctuation zone (WLFZ) of Jialing River, three typical local plants (D. pyramidalis, A. philoxeroides and C. dactylon) and their in-situ sediments were collected for flooding experiments to study the Hg dynamics of water and sediment in different treatments. The results showed that flooding increased sediment MeHg concentrations and flooded plants (especially for the D. pyramidalis) promoted this process. Similarly, the highest dissolved MeHg level and proportion of MeHg to total Hg (%MeHg) were observed in plant-water treatments in the presence of D. pyramidalis, indicating the potential for the methylation of Hg in the water body influenced by the decay process of herbaceous plants. These results suggest that the herbaceous plant D. pyramidalis contributes more to Hg methylation and release in the WLFZ of the Jialing River than other plants studied., (© 2022. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Methylmercury (MeHg) is mainly produced by anaerobic δ-proteobacteria such as sulfate-reducing bacteria (SRB). However, mercury bio-methylation has also been found to occur in the aerobic soil of the Three Gorges Reservoir (TGR). Using γ-proteobacterial TGR bacteria (TGRB) and δ-proteobacterial Desulfomicrobium escambiense strains, the efficiency of mercury methylation and demethylation was evaluated using an isotope tracer technique. Kinetics simulation showed that the bacterial Hg methylation rate (k m ) of TGRB3 was 4.36 × 10 -9 pg·cell -1 ·h -1 , which was significantly lower than that of D. escambiense (170.74 ×10 -9 pg·cell -1 ·h -1 ) under anaerobic conditions. Under facultative and/or aerobic conditions, D. escambiense could not survive, while the k m of TGRB3 were 0.35 × 10 -9 and 0.29 × 10 -9 pg·cell -1 ·h -1 , respectively. Furthermore, the bacterial MeHg tolerance threshold of TGRB3 was 3.47 × 10 -9 pg·cell -1 , which was 98.6-fold lower than that of D. escambiense under anaerobic conditions. However, the MeHg tolerance threshold of TGRB3 remained at 0.50-0.52 × 10 -9 pg·cell -1 under facultative and/or aerobic conditions. Notably, bacterial Hg methylation rates (k m ) were higher than the corresponding bacterial MeHg demethylation rates (k d1 ). These results establish the contribution of some aerobic and/or facultative anaerobic bacteria to net environmental MeHg production in terrestrial ecosystems and provide a novel understanding of the biogeochemical cycle of MeHg. SYNOPSIS: Hg methylation of facultative and/or aerobic bacteria may contribute to the net production of environmental methylmercury in terrestrial ecosystems., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Manganese (Mn) ores contain substantial concentrations of mercury (Hg), and mining and smelting of Mn ores can bring Hg into the surrounding aquatic environment through atmospheric deposition, leaching of electrolytic Mn residue and Mn gangue dump. However, limited is known that how these processes influence the environmental behaviors of Hg in waterbody. Therefore, the seasonal distribution and existing form of Hg in water and sediment in one Mn ore area in Xiushan County, Chongqing were investigated. Our results showed that the mean Hg and methylmercury (MeHg) concentrations in water (n=35) were 5.8 ± 4.6 ng/L and 0.22 ± 0.14 ng/L, respectively. The mean Hg concentrations in retained riverbed and fluvial bank sediment (n=35) were 0.74 ± 0.26 mg/kg and 0.63 ± 0.27 mg/kg, respectively (the mean MeHg concentrations were 0.64 ± 0.40 µg/kg and 0.51 ± 0.30 µg/kg, respectively). It indicated that the mining and smelting of Mn ores were the main sources of anthropogenic Hg, and Mn may inhibit Hg methylation in rivers in Mn ore areas. Mercury in the bound to iron/ Mn (Fe/Mn) oxides of low crystallinity fraction (Hg-OX) accounted for 4.01% and 5.25% of the total Hg concentrations in the retained riverbed and fluvial bank sediment, respectively. The amount of Hg bound to Fe/Mn oxides in sediment increased significantly due to the manganese mining activities in the investigated area. Therefore, it could be hypothesized that high Hg concentrations in river sediment in Mn mining areas are closely related to high Mn concentration in sediment., (Copyright © 2021. Published by Elsevier B.V.)

Biochar has been used increasingly as a soil additive to control mercury (Hg) pollution in paddy rice fields. As the most active component of soil organic matter, soil dissolved organic matter (DOM) plays a vital role in the environmental fate of contaminants. However, there are very few studies to determine the impact of biochar on the Hg cycle in rice paddies using insights from DOM. This study used original and modified biochar to investigate their effect on DOM dynamics and their potential impact on methylmercury (MeHg) production and bioaccumulation in rice plants. Porewater DOM was collected to analyze the variations in soil-derived DOM in paddy soils. The results showed that the addition of biochar, whether in original or modified form, significantly reduced the bioaccumulation of MeHg in rice plants, especially in hulls and grains (p<0.05). However, MeHg production in soils was only inhibited by the modified biochar. Biochar addition induced a significant increase in DOM's aromaticity and molecular weight (p<0.05), which decreased Hg bioavailability. Furthermore, enhanced microbial activity was also observed in DOM (p<0.05), further increasing MeHg production in the soil. Thus, the effect of biochar on the fate of Hg cycle involves competition between the two different roles of DOM. This study identified a specific mechanism by which biochar affects Hg behavior in rice paddy soil and contributes to understanding the more general influence of biochar in agriculture and contaminant remediation., (Copyright © 2022. Published by Elsevier B.V.)

The water-level fluctuation zone (WLFZ) has been considered as a hotspot for mercury (Hg) methylation. Flooding-tolerant herbs are gradually acclimated to this water-land ecotone, tending to form substantial root systems for improving erosion resistance. Accompanying rhizosphere microzone plays crucial but unclear roles in methylmercury (MeHg) formation in the WLFZ. Thus, we conducted this study in the WLFZ of the Three Gorges Reservoir, to explore effects of the rhizosphere of a dominant flooding-tolerant herb (bermudagrass) on MeHg production. The elevated Hg and MeHg in rhizosphere soils suggest that the rhizosphere environment provides favorable conditions for Hg accumulation and methylation. The increased bioavailable Hg and microbial activity in the rhizosphere probably serve as important factors driving MeHg formation in the presence of bermudagrass. Simultaneously, the rhizosphere environments changed the richness, diversity, and distribution of hgcA-containing microorganisms. Here, a typical iron-reducing bacterium (Geobacteraceae) has been screened, however, the majority of hgcA genes detected in rhizosphere, near-, and non-rhizosphere soils of the WLFZ were unclassified. Collectively, these results provide new insights into the elevated MeHg production as related to microbial processes in the rhizosphere of perennial herbs in the WLFZ, with general implications for Hg cycling in other ecosystems with water-level fluctuations., (Copyright © 2022. Published by Elsevier B.V.)

Understanding atmospheric mercury (Hg) accumulation in remote montane forests is critical to assess the Hg ecological risk to wildlife and human health. To quantify impacts of vegetation, climatic and topographic factors on Hg accumulation in montane forests, we assessed the Hg distribution and stoichiometric relations among Hg, carbon (C), and nitrogen (N) in four forest types along the elevation of Mt. Gongga. Our results show that Hg concentration in plant tissues follows the descending order of litter > leaf, bark > root > branch > bole wood, indicating the importance of atmospheric Hg uptake by foliage for Hg accumulation in plants. The foliar Hg/C (from 237.0 ± 171.4 to 56.8 ± 27.7 µg/kg) and Hg/N (from 7.5 ± 3.9 to 2.5 ± 1.2 mg/kg) both decrease along the elevation. These elevation gradients are caused by the heterogeneity of vegetation uptake of atmospheric Hg and the variation of atmospheric Hg° concentrations at different altitudes. Organic soil Hg accumulation is controlled by forest types, topographic and climatic factors, with the highest concentration in the mixed forest (244.9 ± 55.7 µg/kg) and the lowest value in the alpine forest (151.9 ± 44.5 µg/kg). Further analysis suggests that soil Hg is positively correlated to C (r 2  = 0.66) and N (r 2  = 0.57), and Hg/C and Hg/N both increase with the soil depth. These stoichiometric relations highlight the combined effects from environmental and climatic factors which mediating legacy Hg accumulation and selective Hg absorption during processes of organic soil mineralization., (Copyright © 2021. Published by Elsevier B.V.)

Manganese (Mn)-related activities would affect the mercury (Hg) cycling in farmlands, whereas this was not well understood. Here, one of the largest Mn ores in China was selected to study the effects of Mn-related activities on the accumulation and distribution of total Hg (THg) and methylmercury (MeHg) in farmland soils. The soil THg concentrations in the mining area were 0.56 ± 0.45, 0.56 ± 0.45, 0.53 ± 0.44, and 0.50 ± 0.46 mg kg−1 in the 0−10, 10−20, 20−30, and 30−40 cm layers, respectively, while they were increased to 0.75 ± 0.75, 0.72 ± 0.60, 0.62 ± 0.46, and 0.52 ± 0.38 mg kg−1 in the smelting area. Similarly, the soil MeHg concentrations in the smelting area were also elevated by 1.04−1.34 times as compared to those in the mining area. Concentrations of THg (0.59 ± 0.50 mg kg−1) and MeHg (0.64 ± 0.82 μg kg−1) in soils were higher than the regional background value but lower than in vicinal Hg-mining areas, while they were largely elevated at the intersection of two rivers in the smelting area. Significant positive Mn-THg relationship (p < 0.01) and negative Mn-MeHg relationship (p < 0.01) favored the conclusion that soil Mn could promote Hg accumulation while inhibiting MeHg production. Approximately 70% of soil Hg was distributed in the residual phase, and the environmental hazard was not elevated according to a geochemical model. Overall, mining and smelting activities of Mn ores have resulted in obvious and distinct effects on the accumulation and methylation of Hg in farmland soils, but the environmental hazards are currently manageable.

Tropical forest contributes to > 50% of global litterfall mercury (Hg) inputs and surface soil Hg storage, while with limited understanding of Hg biogeochemical processes. In this study, we displayed the 5-m resolution of Hg spatial distribution in three 1-ha tropical forest plots across the latitudinal gradient in Southwest China, and determined Hg isotopic signatures to understand factors driving Hg spatial distribution and sequestration processes. Our results show that tropical forest at the lowest latitude has the highest litterfall Hg input (74.95 versus 34.14-56.59 μg m -2 yr -1 at higher latitude plots), but the smallest surface soil Hg concentration (2-3 times smaller than at higher latitude sites). Hg isotopic evidence indicates that the decreasing climate mediated microbial Hg reduction in forest floor leads to the increasing Hg accumulation along the latitudinal gradient in three tropical forests. The terrain induced indirect effects by influencing litterfall Hg inputs, soil organic matters distribution and interplays between surface and deep soils drive the heterogeneity of surface soil Hg distribution within each sampling plot. Our results highlight though the elevated litterfall Hg inputs, the distinct post-depositional reductions induced Hg loss would remarkedly decrease atmospheric Hg net sink in tropical forest., (Copyright © 2022 Elsevier B.V. All rights reserved.)

To develop high-performance biochar adsorbents, the adsorption ability and rate of untreated (BC-CK) and six modified biochars with amino (BC-NH), epoxy (BC-C 2 H 2 O), ethoxy (BC-C 2 H 5 O), hydrosulfuryl (BC-SH), selenium (BC-Se), and chitosan (BC-Chitosan) on Hg(II) and MeHg were investigated by simulated experiment. The results indicated that the some modified biochars (BC-NH, BC-C 2 H 2 O, BC-C 2 H 5 O and BC-Chitosan) showed lower adsorption capacity than the untreated, possibly due to the decreased specific surface area and pore volume. Whereas, BC-SH and BC-Se was improved immensely by forming stable -SH-Hg and Hg-Se with the adsorption capacity 1.26 and 1.51 times as much as BC-CK, respectively. In spite of that, Hg desorption capacities and rates of all biochars were extremely low, exhibiting great adsorption stability of biochars on Hg in another way. In addition, BC-Chitosan performed the highest adsorption speed. These provided insights on the adsorption effectiveness for Hg in the aqueous solution that was critical for evaluating the application of modified biochars., (© 2021. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Dissolved organic matter (DOM) influences the environmental fate and toxic effects of trace metals such as mercury (Hg). However, because of limits in DOM analytical techniques and lack of sample diversity in past studies, it remains unclear whether the binding strength of DOM complexed with Hg(II) is related to the DOM properties. In this study, different DOM isolates (n = 26) from various sources were used to determine the conditional stability constant (logK) of DOM-Hg complexes using the equilibrium dialysis ligand exchange (EDLE) method. UV-Vis and fluorescence spectrometry were used to evaluate the correlation between logK values and DOM properties, such as chromophoric moieties, aromaticity, and molecular weight. Results demonstrated that the DOM from different sources presented an extensive range of binding strengths to Hg(II), because of their heterogeneous properties. Moreover, DOM chromophores, including aromaticity and molecular weight, are critical indicators of the DOM-Hg affinity in ambient-relevant circumstances. Significantly, higher terrestrial DOM led to greater DOM-Hg affinity. Additionally, this study supports that UV-Vis and fluorescence spectroscopy can be used to estimate DOM composition and its binding strength with Hg(II). Furthermore, the observed relationship between logK and DOM properties provided a possible pathway of explanation for the spatial co-variations between Hg(II) concentrations and DOM characters observed in previous field investigations., 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 © 2021 Elsevier B.V. All rights reserved.)

Straw sizes were found to affect the methylmercury (MeHg) accumulation in rice grains induced by straw incorporation. The mechanism behind, however, still remains unclear. Here, we incorporated rice straw in different sizes (powder, 2 cm and 5 cm) into a Hg-contaminated paddy soil. Our results showed that straw sizes regulated the release of different fractions of organic matter (OM) in straw residues and further Hg methylation in paddy soil. The easily degradable OM (EDOM) was a key driving factor that facilitated net Hg methylation, though it only occupied a small fraction (1.12-3.12%) of the soil OM. Powdered straw reduced the duration of net Hg methylation by 74.39% compared to 5 cm straw, resulting in a strong and rapid net Hg methylation in paddy soil before the rice flowering. After the release of EDOM, the humified OM dominated in paddy soil and bound to MeHg, leading to less MeHg being transported to rice grains during the grain filling. Powdered straw decreased MeHg accumulation by 25.32% in the mature rice grains compared with 5 cm straw. Our study suggests that straw powdering before incorporation provides a feasible pathway for reducing MeHg accumulation in rice grains induced by straw incorporation., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Litterfall mercury (Hg) input has been regarded as the dominant Hg source in montane forest floor. To depict combining effects of vegetation, climate and topography on accumulation of Hg in montane forests, we comprehensively quantified litterfall Hg deposition and decomposition in a serial of subtropical forests along an elevation gradient on both leeward and windward slopes of Mt. Ailao, Southwest China. Results showed that the average litterfall Hg deposition increased from 12.0 ± 4.2 μg m -2 yr -1 in dry-hot valley shrub at 850-1000 m, 14.9 ± 6.8 μg m -2 yr -1 in mixed conifer-broadleaf forest at 1250-2400 m, to 23.1 ± 8.3 μg m -2 yr -1 in evergreen broadleaf forest at 2500-2650 m. Additionally, the windward slope forests had a significantly higher litterfall Hg depositions at the same altitude because the larger precipitation promoted the greater litterfall biomass production. The one-year litter Hg decomposition showed that the Hg mass of litter in dry-hot valley shrub decreased by 29%, while in mixed conifer-broadleaf and evergreen broadleaf forests increased by 22-48%. The dynamics of Hg in decomposing litter was controlled by the temperature mediated litter decomposition rate and the additional adsorption of environmental Hg during decomposition. Overall, our study highlights the litterfall mediated atmospheric mercury inputs and sequestration increase with the montane elevation, thus driving a Hg enhanced accumulation in the high montane forest., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Three Gorges Dam (TGD) is the largest hydroelectric construction in the world, and its potential impacts on the ecological environment and human health risks have invoked considerable global concern. However, as a mercury (Hg) sensitive system, limited work was conducted on the Hg exposure level of local residents around the Three Gorges Reservoir (TGR). Thus, 540 human hair samples and 22 species of local food samples were collected to assess the Hg exposure and human health risk to the residents located in the Three Gorges Reservoir Region (TGRR) and to investigate their dietary exposure to Hg. The results showed that the geometric mean concentrations of total mercury (THg) and methylmercury (MeHg) in hair were 0.42 ± 0.43 μg g -1 and 0.23 ± 0.32 μg g -1 , respectively, lower than the reference level (1.0 μg g -1 ) recommended by the United States Environmental Protection Agency (US EPA), indicating a low level Hg exposure for residents around the TGR. No significant difference in the accumulation of Hg in hair between the gender subgroups was observed, whereas age difference, smoking and alcohol drinking behavior, and fish consumption frequency were significant predictors of hair Hg level. Besides, THg and MeHg of all the investigated food samples did not exceed the corresponding Chinese national standard. The average probable daily intakes (PDIs) of THg and MeHg were 0.032 μg kg -1 day -1 and 0.007 μg kg -1 day -1 , which were obviously below the recommended values of 0.57 μg kg -1 day -1 and 0.1 μg kg -1 day -1 , respectively. The cereal (mainly rice) contribution of THg (76.0%) and MeHg (74.4%) intakes to the local residents around the TGR was much higher than that of fish (10.7% and 22.9%, respectively) due to the considerable rice consumption. Overall, residents around the TGR were at a low Hg exposure and rice consumption was the major pathway for Hg exposure., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

The identification of dominant microbes in anaerobic mercury (Hg) methylation, methylmercury (MeHg) demethylation, and methane oxidation as sulfate-reducing bacteria, methanogens or, probably, anaerobic methanotrophic archaea (ANMEs) is of great interest. To date, however, the interrelationship of bacteria and archaea involved in these processes remains unclear. Here, we demonstrated the dynamics of microorganisms participating in these processes. Anaerobic fixed-bed reactors were operated with swine manure and sludge to produce methane stably, and then, sulfate (reactor C), sulfate and Hg(II) (reactor H), and sulfate and MeHg (reactor M) were added, and the reactors were operated for 120 d, divided equally into four periods, P1-P4. The bacterial compositions changed nonsignificantly, whereas Methanosaeta in reactors H and M decreased significantly, revealing that it was irrelevant for Hg transformation. The abundances of Syntrophomonadaceae, Methanoculleus, Candidatus Methanogranum and Candidatus Methanoplasma increased continuously with time; these species probably functioned in these processes, but further evidence is needed. Desulfocella and Desulfobacterium dominated first but eventually almost vanished, while the dominant archaeal genera Methanogenium, Methanoculleus and Methanocorpusculum were closely related to ANME-1 and ANME-2. PLS-DA results indicated that both bacteria and archaea in different periods in the three reactors were clustered separately, implying that the microbial compositions in the same periods were similar and changed markedly with time., 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 © 2021 Elsevier Ltd. All rights reserved.)

Methylmercury (MeHg) in rice is presumed to be derived from MeHg formed in the soil, although it is still controversial. Moderate soil mercury (Hg) concentration can affect the diversity of soil microorganisms and may also impact the physiological changes and MeHg absorption of rice. In this study, the pot experiment was conducted to explore the effects of Hg concentration gradients (0, 0.3, 3, and 30 mg kg -1 ) stress on Hg transformation in the rhizosphere, Hg translocation in rice, and physiological changes in rice leaves during the whole rice growing season. Moderate soil Hg concentration (3 mg kg -1 ) greatly increased the MeHg/THg (1.69%) of rhizosphere, while 30 mg kg -1 soil Hg concentration sharply reduced the MeHg/THg (0.29%) of rhizosphere. Highest MeHg/THg of the four groups all appeared at the blooming or filling stage. There was a significant positive correlation between Fe 2+ in rhizosphere and MeHg/THg, but no significant correlation between SO 4 2- and MeHg/THg was observed. Although the 3 mg kg -1 soil Hg concentration significantly enhanced MeHg concentrations in seeds, it considerably reduced the bioaccumulation factors of MeHg in roots, stalks, old leaves and young leaves. Soil Hg concentration of 30 mg kg -1 , to a certain extent, curtailed MeHg concentrations in seeds, while MeHg concentrations in the husk were significantly increased. Consistent with the result that there was no significant difference for THg concentrations in old and young leaves among the four Hg treatment groups, the content of chlorophyll, H 2 , malondialdehyde and antioxidant substances, and the activities of antioxidant enzyme in old and young leaves varied indistinctly among groups. MAIN FINDING: Moderate soil mercury concentration (3 mg kg 2 , malondialdehyde and antioxidant substances, and the activities of antioxidant enzyme in old and young leaves varied indistinctly among groups. MAIN FINDING: Moderate soil mercury concentration (3 mg kg -1 ) could extremely enhance MeHg production in the rhizosphere soil and its accumulation in rice; MeHg production in the rhizosphere soil increased greatly at the blooming or filling stage, whereas little effect on antioxidant systems in leaves was observed., 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 © 2020 Elsevier B.V. All rights reserved.)

Recently, there has been increasing interest in reducing methylmercury (MeHg) phytoavailability using biochar, although the underlying mechanisms are not fully understood. By combining lab-scale batch incubation with pot and field validations, we demonstrate that biochar-impacted sulfur cycling in soils and MeHg-soil binding play key roles in controlling MeHg phytoavailability. (1) Under anoxic conditions, biochar-associated sulfate and biochar-facilitated microbial sulfate reduction enhanced the production of reduced inorganic sulfur species as acid-volatile sulfide (AVS) in soils by 122%, facilitating MeHg binding with soils and thus reducing MeHg phytoavailability. (2) In contrast, under oxic conditions, the reduced inorganic sulfur was oxidized (resulting in a 68-91% decrease in AVS), which released soil-bound MeHg and increased MeHg phytoavailability. The proposed mechanisms could explain the distinct effects of biochar amendment on MeHg bioaccumulation observed under anoxic (10-88% lower in rice grains) and oxic conditions (48-84% higher in wheat grains). Our results dispute the commonly held assumption that reduced MeHg phytoavailability under biochar amendment can be primarily attributed to MeHg-biochar binding. Therefore, the potential increased risk of MeHg in oxic soils following biochar amendment should be evaluated in more detail., (Copyright © 2020 Elsevier B.V. All rights reserved.)

It is of great importance to elucidate the mechanism of mercury (Hg) migration in the forest litterfall so as to clearly understand global Hg deposition. However, it is still unclear for the migration and transformation of Hg in different forest litters during long-term decomposition. Therefore, the dynamics of total Hg (THg), methylmercury (MeHg), carbon, nitrogen, microbial biomass carbon and nitrogen in the litterfall of the evergreen broadleaf (EB) and mixed broadleaf-conifer (MBC) forests, southwest China were investigated, aiming to understand the migration characteristics of Hg in the two-year decomposing litterfall. Results showed that carbon decreased, while nitrogen accumulated slightly in the process of litterfall decomposition. THg levels in the second year of the EB and MBC forests decreased by 16.9% and 11.3%, while MeHg levels reduced by 141.4% and 210.7% respectively comparing with those in the first year. The total percentage of hydrochloric acid-soluble mercury (Hg-h) and water-soluble mercury (Hg-w) had a significant impact on the migration of THg and MeHg in the two forest stands. The C/N ratio in the EB forest bore a positive correlation with THg and MeHg levels, whereas that in the MBC forest was adverse. Besides, microbial biomass C and N were positively related with THg and MeHg levels in both the EB and MBC forests. It is proposed that THg and MeHg accumulation in the second year drastically decreased probably due to finite nutritional conditions, which implies that Hg accumulation risks alleviate with degradation time., (Copyright © 2020 Elsevier Inc. All rights reserved.)

Limited information is available about the bio-methylation of inorganic mercury (iHg) under aerobic conditions. In this study, two γ-proteobacteria strains (P. fluorescens TGR-B2 and P. putida TGR-B4) were obtained from the soil of The Three Gorges Reservoir (TGR), demonstrating effective aerobic transformation capacities of iHg into methylmercury (MeHg). Based on periodical changes in soil oxygen content of the TGR, a culture system was established, in which 300 ng Hg (II) L -1 and O 2 were set at 7%, 14%, and 21%, respectively. Results indicated that the two strains differed significantly in bacterial growth rate and MeHg production. The kinetic model of MeHg showed typical characteristics of a "two-staged" process: The first stage was dominated by bio-methylation, which was shown by increasing of net MeHg content. Moreover, the second stage was dominated by bio-demethylation, which decreased net MeHg content. Thus, we hypothesized that the mechanism of aerobic bacterial iHg bio-methylation: (1) should inefficiency compared to anaerobic bacteria i.e.SRB, which were regulated by hgcA/B gene clusters, (2) might be regarded as a passive stress response and depended on the bacterial iHg intoxication threshold and MeHg tolerance threshold., (Copyright © 2020 The Authors. Published by Elsevier Inc. All rights reserved.)

Total mercury (THg) and methylmercury (MeHg) concentrations were measured in hair of 98 Chinese university students to study their levels of Hg exposure and influencing factors. The results showed that Hg exposure for university students was at a low level with concentrations lower than the USEPA recommended reference level (1 µg/g) across all hair samples. The percentage of MeHg to THg (%MeHg) in hair was about 50%, lower than the previously reported value of 70-100%, probably associated with the low %MeHg in the diet of university students. Fish and rice consumption were not a primary factor affecting hair Hg levels of university students, while smoking could be one main pathway of Hg exposure. In addition, the similarly dietary structure in the studied university narrowed the difference of Hg exposure levels among students.

Human exposure to methylmercury (MeHg) through rice consumption is raising health concerns. It has long been recognized that MeHg found in rice grain predominately originated from paddy soil. Anaerobic conditions in paddy fields promote Hg methylation, potentially leading to high MeHg concentrations in rice grain. Understanding the transformation and migration of Hg in the rice paddy system, as well as the effects of farming activities, are keys to assessing risks and developing potential mitigation strategies. Therefore, this review examines the current state of knowledge on: 1) sources of Hg in paddy fields; 2) how MeHg and inorganic Hg (IHg) are transformed (including abiotic and biotic processes); 3) how IHg and MeHg enter and translocate in rice plants; and 4) how regular farming activities (including the application of fertilizer, cultivation methods, choice of cultivar), affect Hg cycling in the paddy field system. Current issues and controversies on Hg transformation and migration in the paddy field system are also discussed., (Copyright © 2020 Elsevier Inc. All rights reserved.)

In the recent decade, the hydroelectric reservoir is identified as a methylmercury (MeHg) hotspot and gained much attention. The artificial water level management in the Three Gorges Reservoir (TGR) in China formed a water-level-fluctuation zone (WLFZ) undergoing flooding drying rotations annually. However, the mercury (Hg) methylation and major geochemical driving factors at different elevations in the WLFZ remain unclear. Here we use total Hg (Hg T ) normalized MeHg (MeHg/Hg T ratio) to evaluate Hg methylation degree in a one-year field study at 155, 165 m elevations in the WLFZ and with >175 m elevation as the reference. Results demonstrate that MeHg/Hg T ratio at the WLFZ could reach 4.1% in soils, and both 155 and 165 m elevations have a higher Hg methylation degree than the >175 m elevation. However, the differences in MeHg/Hg T ratios both in soils and waters between 155 and 165 m elevations are not significant. This indicates the influence of different submerging periods on the MeHg/Hg T at the WLFZ elevations is not observed. The significant correlation between the MeHg/Hg T ratio and soil organic carbon (SOC) content implies a MeHg retention in re-exposed soils after flooding. Decoupling of MeHg/Hg T ratios between submerged soil and overlying water are found at both elevations and therefore make MeHg/Hg T in waters alone cannot be used to evaluate Hg methylation degree in this study. The calculation of Hg T and MeHg partitioning coefficient (K d ) found an immobilization of MeHg by submerged soils at the WLFZ during the flooding period. Major geochemical factors, determined through principal component analysis (PCA), in affecting Hg methylation are the redox cycling of sulfur and the distribution of organic matters in the WLFZ., 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 © 2020 Elsevier Inc. All rights reserved.)

Soil dissolved organic matter (DOM) plays an essential role in the Three Gorges Reservoir (TGR) as a linkage between terrestrial and aquatic systems. In particular, the reducing capacities of soil DOM influence the geochemistry of contaminants such as mercury (Hg). However, few studies have investigated the molecular information of soil DOM and its relationship with relevant geochemical reactivities, including redox properties. We collected samples from eight sites in the TGR areas and studied the link between the molecular characteristics of DOM and their electron donation capacities (EDCs) toward Hg(II). The average kinetic rate and EDC of soil DOM in TGR areas were (0.004 ± 0.001) hr -1 and (2.88 ± 1.39) nmol e - /mg DOM bulk , respectively. Results suggest that higher EDCs and relatively rapid kinetics were related to the greater electron donating components of lignin-derived and perhaps pyrogenic DOM, which are the aromatic constituents that influenced the reducing capacities of DOM in the present study. Molecular details revealed that even the typical autochthonous markers are important for the EDCs of DOM as well, in contrast to what is generally assumed. More studies identifying specific DOM molecular components involved in the abiotic reduction of Hg(II) are required to further understand the relations between DOM sources and their redox roles in the environmental fate of contaminants., (Copyright © 2019. Published by Elsevier B.V.)

Soils in the water-level-fluctuating zone (WLFZ) of Three Gorges Reservoir (TGR) inundated by water for different periods of time are confirmed to have disparate characteristics to mercury (Hg), and thus it is of great significance to further investigate microbial compositions and influencing factors. The objective of this study was to compare bacterial and archaeal richness, α-diversities and compositions, as well as affecting variables, especially Hg concentrations, among soils under different submergence time-SI (inundated soil), SS (semi-inundated soil), SN(non-inundated soil) and SSe (sediment)-based on high throughput sequencing. Results showed that sediment had significantly higher bacterial and archaeal richness and α-diversities than the other soil types. Anaerolinea and Aeromonas, as well as Altiarchaeales, Nitrosoarchaeum, and Methanosarta were dominant in SSe, while sharply decreasing in the other soil types, with significant difference among groups. An unclassified genus in SCG critically predominating in SI, SS and SN, drastically reduced in SSe, with extremely significant difference among groups. Bathyarchaeota and Nitrososphaera, both dominating in SSe, decreased dramatically and almost vanished in SI and SN. All the variables except pH posed a significant positive effect on bacterial and archaeal compositions in SSe, while opposite effect in the other three soil types. MeHg and THg concentrations had relatively weaker effects on microbial compositions comparing to variables like NH 4 + , CEC, OM and SO 4 2+ ., (Copyright © 2020 Elsevier Inc. All rights reserved.)

The reducing capacity (RC) of natural organic matter plays an important role in the carbon cycle and biogeochemical fates of environmental contaminants in the aquatic system. However, the electron donation potentials of dissolved organic matter (DOM) from high-latitude lakes are still uncertain. In this study, we collected DOM samples from high-latitude lakes across the Arctic and boreal regions in Sweden and Norway to investigate the effects of the DOM concentration and characteristics on its ambient reducing capacity (ARC). Mercury (Hg(II)) abiotic reduction in darkness was used to determine the ARC. The results showed that the DOM in Arctic lakes is less terrestrial-dominant than in reference sites (i.e., forest lakes). Between the two categories of Arctic lakes, tundra lakes are more terrestrial-influenced compared to mountain lakes. Additionally, terrestrial-originated DOM is a main controlling factor for enhancing the ambient reducing capacity, whereas the DOM concentration, i.e., dissolved organic carbon (DOC), resulted in variations in the Hg/DOC ratios that also cause the variations of the observed ARC values. Thus, comparisons of the ARC values can be conducted while oxidant/DOC ratios are kept the same and reported through the method using heavy metals as a chemical probe. After correction for Hg/DOC ratio interference, the ambient reducing capacity of DOM followed the order: boreal forest lakes > Arctic tundra lakes > Arctic mountain lakes. This study highlights that the DOM concentration should also be considered when estimating the ARC as compared to the previous that mainly focusing on the properties of DOM such as its origins. As climate change is projected to be severe in high latitudes, this study demonstrates a significant connection between aquatic DOM geochemical reactivity and terrestrial inputs, which is crucial for a better prediction of the role of DOM in high-latitude lakes in the context of climate change., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Water-level-fluctuating zone (WLFZ) is a prevalent water-land ecotone favorable for mercury (Hg) methylation. The succession of flooding tolerance plants in WLFZ gradually changes the landscape, and also brings a new question worth understanding whether these plants would enhance methylmercury (MeHg) production in WLFZ and increase risks to the aquatic environment. Given bermudagrass (Cynodon dactylon (L). Pers) as the dominant perennial herb with high flooding-tolerance in WLFZ of the Three Gorges Reservoir (TGR), we conducted a comprehensive study to investigate its roles in the production and migration of MeHg in WLFZ by field observations and stable isotope tracer experiments. Results showed that both elevated MeHg levels and Hg methylation rates appeared in soil/sediment in bermudagrass growing area, implying that the growth of bermudagrass could significantly enhance MeHg production. However, MeHg migration from sediment to water was restricted during the flooding period of the TGR, as obviously higher partitioning coefficients of MeHg between the sediment and porewater (p <  0.05) and lower MeHg release fluxes were observed in vegetated area, indicating that the presence of bermudagrass instead probably decreased the water MeHg level. Whereas, it is noteworthy that elevated MeHg in soil/sediment induced by the bermudagrass could pose potential risks to the benthos and further to the TGR food chain., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Forest ecosystem has long been suggested as a vital component in the global mercury (Hg) biogeochemical cycling. However, there remains large uncertainties in understanding total Hg (THg) and methylmercury (MeHg) variations and their controlling factors during the whole hydrological processes in forest ecosystems. Here, we quantified Hg mass flow along hydrological processes of wet deposition, throughfall, stemflow, litter leachate, soil leachate, surface runoff, and stream, and litterfall Hg deposition, and air-forest floor elemental Hg (Hg 0 ) exchange flux to set up a Hg mass balance in a subtropical forest of China. Results showed that THg concentration in stream was lower than that in wet deposition, while an opposite characteristic for MeHg concentration, and both THg and MeHg fluxes of stream were lower than those of wet deposition. Variations of THg and MeHg in throughfall and litter leachate had strong direct and indirect effects on controlling variations of THg and MeHg in surface runoff, soil leachate and stream, respectively. Especially, the net Hg methylation was suggested in the forest canopy and forest floor layers, and significant particulate bound Hg (PBM) filtration was observed in soil layers. The Hg mass balance showed that the litterfall Hg deposition was the main Hg input for forest floor Hg, and the elemental Hg vapor (Hg 0 ) re-emission from forest floor was the dominant Hg output. Overall, we estimated the net THg input flux of 13.8 μg m -2 yr -1 and net MeHg input flux of 0.6 μg m -2 yr -1 within the forest ecosystem. Our results highlighted the important roles of forest canopy and forest floor to shape Hg in output flow, and the forest floor is a distinct sink of MeHg., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Moss is usually as an initial colonizer in alpine glacier retreated regions. We hypothesized that moss can significantly facilitate the toxic metals accumulation in alpine ecosystems based on its strong ability of absorption and the role in soil development. Hence, we investigated the trace element pool sizes and enrichment factors, especially for mercury (Hg) by using the Hg isotopic compositions to determine the source contributions in a moss-dominated ecosystem over glacial erratic in Eastern Tibetan Plateau. Results show that Hg, lead (Pb) and cadmium (Cd) are highly enriched in organic soils. Specifically, Cd concentration is 5-20 times higher than the safety limit of the acid soil (pH ≤ 5.5) in China. Atmospheric depositions dominantly contribute to the Pb and Cd sources in organic soils, and followed by the moraine particles influences. The lowering pH in organic soils increasing with glacial retreated time results in the desorption of Cd in organic soils. Atmospheric Hg 0 uptake by moss predominantly contributes to the Hg sources in organic soils. The average Pb accumulation rate over last 125-year is about 5.6 ± 1.0 mg m -2 yr -1 , and for Cd is 0.4 ± 0.1 mg m -2 yr -1 , and for Hg 0 is 27.6 ± 3.2 μg m -2 yr -1 . These elevated accumulation rates are caused by the high moss biomass and elevated atmospheric Hg, Pb and Cd pollution levels in China and neighbouring regions. Our study indicates that the moss not only as the bioindicator, but also plays an important role in the hazardous metal biogeochemical cycling in alpine regions., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Rice (Oryza sativa) paddy is the hotspot of mercury (Hg) methylation. Given distinct influences of rotation systems on the physicochemical properties of paddy soils, we hypothesized different rotation systems in rice paddies inducing a large difference in Hg methylation. Here, we investigated Hg species distribution, dissolved organic matter (DOM) features, and Hg methylation in five rotation systems (Other farmland newly reclaim into paddy field, i.e., NR-R; Drain the water in winter, i.e., DW-R; Flooding in winter, i.e., FW-R; Rape-Rice rotation, i.e., Ra-R; Wheat-Rice rotation, i.e., Wh-R) of paddy fields to identify such hypothesis. Results shown that FW-R had the strongest Hg methylation, followed by Ra-R and Wh-R, then DW-R, and finally NR-R. We further found that much higher soil organic matter (SOM) and organo-chelated Hg (Hg-o) from straw residues and root exudates were the main cause for the greater Hg methylation in FW-R, Ra-R and Wh-R. This was because the protein-like fraction of SOM facilitated the net production of methyl Hg (MeHg), meanwhile the humin-like fraction had a strong affinity to MeHg in paddy soils. Therefore, it can be concluded that paddy soil under DW-R was the optimum pattern in order to reduce the occurrence of Hg methylation. However, paddy soils under Ra-R and Wh-R were the recommendable patterns if the productivity of paddy fields was considered., (Copyright © 2019 Elsevier Inc. All rights reserved.)

The objective of this study was to investigate the transport dynamics of total mercury (THg) and methylmercury (MeHg) in the first rainfall-runoff event after summer drought, to understand flushing effects (FFEs) and to quantificationally estimate contributions to the annual outputs of Hg. The results showed that both THg and MeHg in rainfall-runoff predominated by particulate fraction peaked at the beginning of the monitoring period. On average, more than 80% of THg and MeHg loadings were transported during the initial runoff (≤ 6 h). Simultaneously, significant FFEs were observed for both THg and MeHg, with a larger effect for MeHg. More importantly, the estimated output fluxes of THg and MeHg in runoff produced by this rainfall event contributed 3.0% (THg) and 7.8% (MeHg) to the annual output fluxes, respectively, suggesting the importance of the first-rainfall on the Hg loss (especially for MeHg).

The Three Gorges Reservoir (TGR) is a relatively large reservoir, and its water level management actions produce a widespread water level fluctuation zone (WLFZ), which has characteristics of both terrestrial and aquatic ecosystems. Here, an integrated overview of current knowledge on Hg behaviors in the TGR, especially the WLFZ, as well as exposure risk to local residents was presented. Hg levels in the TGR were comparable with other natural aquatic systems. WLFZ in the TGR was confirmed to be an environment favorable for Hg methylation by enhancing microbial activity, promoting sulfur cycling and increasing the level of low-molecular-weight organic matters. However, elevated fish Hg concentrations did not follow the impoundment of TGR, indicating no obvious reservoir effect, while it is still noteworthy that frequently consuming fish is likely to be a methylmercury (MeHg) exposure pathway for specific populations e.g. fishermen around the TGR.

Mercury (Hg) is one of the most toxic heavy metal pollutants, which can be easily transmitted and enriched through the food chain, posing severe threat to human beings. Forest ecosystems are one of the most active environments for biogeochemical cycles of Hg. It is essential to research on Hg cycling in the forest ecosystem, which contributes to a comprehensive understanding of global biogeochemical cycle of Hg. However, there is still a lack of consensus on whether the forest ecosystem is a "source" or "sink" of Hg in the global Hg cycle so far. Therefore, it is necessary to elucidate the current state of knowledge on Hg deposition, transformation and fate in the forest ecosystem, especially the existing puzzles or issues encountered by scientists worldwide. This review highlights the complexity and uncertainties of Hg cycling in forest ecosystems. It is proposed that a new perspective is required to further understand the role of forest ecosystems in global Hg cycle based on a sufficient understanding of Hg exchange fluxes at the interface of air-soil and air-plant, Hg deposition flux through litterfall, and accurate construction of Hg mass balance system.

As a global toxic pollutant, mercury (Hg) bioaccumulation within food chain could be influenced by human disturbance. Ten typical fish species were collected from Changshou Lake, an artificial lake used to carry out cage fish culture, to investigate the C/N isotopic compositions and Hg bioaccumulation in fish. The results showed that the total Hg (THg) and methylmercury (MeHg) levels in fish muscles ((56.03 ± 43.96) and (32.35 ± 29.57) ng/g, wet weight), comparable with those in most studies in China, were significantly lower than the international marketing limit (0.5 mg/kg). Past human input for cage culture in this lake led to abnormal 15 N enrichment in food chain, as the quantitative trophic levels based on δ 15 N were different with that classified by feeding behaviors. This phenomenon subsequently demonstrated that it should be considered thoughtfully with respect to the application of the traditional method for understanding Hg bioaccumulation power by the slope of log 10 [Hg] with δ 15 N regression in specific water body (i.e., Changshou Lake). In addition, no significant linear correlation between Hg and body weight or length of some fish species was observed, suggesting that the fish growth in the eutrophic environment was disproportionate with Hg bioaccumulation, and fish length or weight was not the main factor affecting Hg transfer with food web. The occurrence of human disturbance in aquatic system presents a challenge to a better understanding of the Hg bioaccumulation and biomagnification within the food chain., (Copyright © 2018. Published by Elsevier B.V.)

Several strains of archaea have the ability to methylate or resist mercury (Hg), and the paddy field is regarded to be conducive to Hg methylation. However, our knowledge of Hg-methylating or Hg-resistant archaea in paddy soils is very limited so far. Therefore, the distribution of archaea and bacteria in the rhizosphere (RS) and bulk soil (BS) of the rice growing in Xiushan Hg-mining area of southwest China was investigated. Bacterial and archaeal 16S rRNA gene amplicon sequencing of the rice rhizosphere along the Hg gradient was conducted. THg concentrations in RS were significantly higher than that in BS at site S1 and S2, while MeHg concentrations in RS was always higher than that in BS, except S6. Bacterial species richness estimates were much higher than that in archaea. The bacterial α-diversity in high-Hg sites was significant higher than that in low-Hg sites based on ACE and Shannon indices. At the genus level, Thiobacillus, Xanthomonas, Defluviicoccus and Candidatus Nitrosoarchaeum were significantly more abundant in the rhizosphere of high-Hg sites, which meant that strains in these genera might play important roles in response to Hg stress. Hg-methylating archaea in the paddy field could potentially be affiliated to strains in Methanosarcina, but further evidence need to be found. The results provide reference to understand archaeal rhizosphere community along an Hg gradient paddy soils., (Copyright © 2018 Elsevier B.V. All rights reserved.)

The origin and composition of dissolved organic matter (DOM) in porewater of lake sediments is intricate and decisive for fate of pollutants including mercury (Hg). While there are many reports on the relationship between dissolved organic carbon concentration (DOC) and mercury (Hg) concentrations in aquatic systems, there are few in which DOM compositional properties, that may better explain the fate of Hg, have been the focus. In this study, porewaters from sediments of three lakes, Caihai Lake (CH), Hongfeng Lake (HF) and Wujiangdu Lake (WJD), all located in southwest China, were selected to test the hypothesis that DOM optical properties control the fate of Hg in aquatic ecosystems. Porewater DOM was extracted and characterized by UV-Vis absorption and fluorescence spectroscopy. A two end-member (autochthonous and allochthonous DOM) mixing model was used to unveil the origin of DOM in porewaters of the three lakes. Our results show a higher input of terrestrial DOM in the pristine lake CH, as compared to lakes HF and WJD lakes, which were both influenced by urban environments and enriched in autochthonous DOM. While the relationships between the concentrations of DOC and the different chemical forms of Hg forms were quite inconsistent, we found important links between specific DOM components and the fate of Hg in the three lakes. In particular, our results suggest that allochthonous, terrestrial DOM inhibits Hg(II) availability for Hg methylating micro-organisms. In contrast, autochthonous DOM seems to have been stimulated MeHg formation, likely by enhancing the activity of microbial communities. Indeed, DOM biodegradation experiments revealed that differences in the microbial activity could explain the variation in the concentration of MeHg. While relationships between concentrations of DOC and Hg vary among different sites and provide little information about Hg cycling, we conclude that the transport and transformation of Hg (e.g. the methylation process) are more strongly linked to DOM chemical composition and reactivity., (Copyright © 2018 Elsevier Ltd. All rights reserved.)