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Forests play a significant role in the biogeochemical cycling of mercury (Hg). Litterfall represent a dominant pathway for Hg to reach the ground surface under a forest canopy. In order to understand Hg accumulation in the litterfall, the dynamics of Hg, carbon (C), nitrogen (N), microbial C and N, as well as bacterial community in the decaying litterfall of two typical subtropical forest stands in southwest China were investigated for one year. THg levels in the litterfall after one-year increased to 124.64% and 135.90%, and MeHg levels in the litterfall increased up to 295.65% and 209.38% of the initial values in the mixed broadleaf-conifer forest and evergreen broadleaf forest respectively. Differently, the concentrations of THg and MeHg in the organic layer of the underlying soil were quite stable. The concentrations of THg in the decaying litterfall corresponded negatively with C/N ratios. Bacterial community analysis found that the bacteria previously being confirmed as Hg methylators did not occur in the genera of the decomposing litterfall in the two forest stands, which might imply that the increase of MeHg during decomposing did not mainly due to the contribution of confirmed Hg methylators, and other sources of MeHg might exert certain roles. [ABSTRACT FROM AUTHOR]

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 (Hg0) 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 (Hg0) 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. Image 1 • Forest canopy and forest floor shape mercury concentrations in runoff. • Both forest canopy and forest floor induce net Hg methylation. • Mineral soil is a distinct methylmercury sink. • Subtropical forest in south China plays a sink role of atmospheric mercury. [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]