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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_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. [Display omitted] • Effects of six modified biochars on the enrichment of MeHg in rice were compared • Selenium and chitosan modified biochars greatly reduced MeHg contents in rice. • Bacillus altered soil MeHg production by MeHg degradation under biochar amendment. • Saccharimonadales and Clostridia could increase MeHg contents in rhizosphere. [ABSTRACT FROM AUTHOR]

[Display omitted] • Methylators were dominating in rice rhizosphere, rather than the bulk soil. • Hg-promoted methylators are key taxa in the rhizosphere at the flowering stage. • In planta demethylation and methylation in rice roots are possible. • Desulfovibrionaceae may play an important role in Hg detoxification of rice. 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. [ABSTRACT FROM AUTHOR]

Some thiols, such as cysteine (CYS) at moderate concentrations (10–500 µM), can enhance methylmercury (MeHg) formation by Geobacter sulfurreducens PCA, whereas others such as dithiol 2,3-dimercaptopropanesulfonate (DMPS) and 2,3-dimercaptosuccinic acid (DMSA) abolish mercury [Hg(II)] methylation. Little is known, however, about whether Hg(II) methylation could be enhanced or inhibited by the presence of mixed thiol ligands at low concentrations observed in the environment. Surprisingly we found that mixing CYS (1 µM) with DMPS (0.025–0.5 µM) or DMSA (0.025–1 µM) substantially increased MeHg production by 1.5–3.5-fold, compared to the no-thiol control, whereas complexation with a single DMPS, or DMSA, or CYS (1 µM) strongly inhibited Hg(II) methylation. Pre-equilibration between Hg(II) and thiols before the addition of cells was necessary to observe enhanced methylation. Spectroscopic analyses indicated the formation of mixed or heteroleptic coordinated Hg(II)-S 3 /S 4 complexes, which likely facilitated exchange of Hg(II) with cells and its uptake and internal transfer to the HgcAB proteins required for methylation. These results suggest that the effects of thiols on Hg(II) methylation were more complex than previously thought (using a single thiol) and thus underscore the importance of understanding how mixed thiols and their interactions with Hg(II) may ultimately influence MeHg production in the natural environment. [ABSTRACT FROM AUTHOR]

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 (Hg2+) or further to elemental Hg (Hg0). 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. [Display omitted] • A gradually-complex network evolved for the decaying litterfall of MBC forest. • A relatively static network existed for the decomposing EB forest litterfall. • N-fixing bacteria may mediate the increase of THg levels in the decomposing litterfall. • MeHg enhancement is likely regulated by aerobic MeHg-degrading microbes. • Underlying soil is the source of litterfall THg, while MeHg is transported from litterfall to soil. [ABSTRACT FROM AUTHOR]