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Mercury (Hg) contamination in mangrove ecosystems has received increasing attention in recent years. Although many studies have investigated methylmercury (MeHg) contamination and its relationship to a number of environmental factors in mangrove sediments, the production of MeHg in this carbon-rich ecosystem has not been fully evaluated. In this study, we measured the total mercury (THg) and MeHg concentrations in the sediments collected from seven mangrove forests in China. In addition, we examined the origin and quality of sedimentary organic matter (OM), trying to evaluate their influence on the MeHg accumulation in mangrove sediments. We found that litterfall played an important role in regulating THg and MeHg contents in mangrove sediments. THg and MeHg concentrations in the mangrove sediments were positively correlated to OM content and the labile fraction of the OM. Multiple evidence (stable carbon isotopes, monosaccharide compositions, and biogenic silica) suggested that OM in mangrove sediments was dominated by input from litterfall. THg and MeHg concentrations were elevated at the sediments with higher input of mangrove OM. We observed that addition of mangrove litter stimulated the production of MeHg under anaerobic conditions. Overall, our results suggested that litterfall acted as a source of inorganic Hg, labile carbon, and low-molecular-weight OM which greatly favor the Hg methylation. Our study provides new insights into the MeHg production in mangrove sediments. Unlabelled Image • Litterfall played an important role in regulating sedimentary THg and MeHg. • THg and MeHg contents were positively correlated to the labile fraction of OM. • THg and MeHg contents were elevated at the sediments with higher input of mangrove OM. • Mangrove litter stimulated MeHg production in sediments under anaerobic conditions. [ABSTRACT FROM AUTHOR]

Mangrove ecosystems serve as an important carbon sink but also could be a hotspot that produces neurotoxic methylmercury (MeHg). Although many studies have focused on mercury (Hg) contamination in this carbon-rich ecosystem, our understanding of the effects and mechanisms of the organic matter (OM) regulation of MeHg production in mangrove sediments is still limited. Here, we examined the effects of Hg contamination and OM enrichment on MeHg production in anoxic mangrove sediments and identified the major microbial guilds attending this process. The mangrove sediments possessed a high potential for producing MeHg, but this was counterbalanced by its rapid degradation. Sulfate-reducing bacteria (SRB) such as Desulfobacterales , Desulfovibrionales , and Syntrophobacterales were the major methylators. OM diagenesis significantly changed the biogeochemical conditions, accelerating MeHg degradation in the sediments. The enhanced MeHg degradation could be attributed to the abundant sulfide produced during OM decomposition, which could potentially inhibit the Hg methylation by immobilization of inorganic Hg, abiotically degrade MeHg, and favor the non- mer -mediated degradation of MeHg by SRB. Our study provides both geochemical and microbial clues that can partly explain the low MeHg levels widely observed in mangrove sediments. [Display omitted] • Geochemistry and microbial analysis explain the low MeHg in mangrove sediments. • Hg methylation counterbalanced with MeHg degradation in mangrove sediments. • OM enrichment facilitated MeHg degradation in the sediments. • SRB played critical roles in both Hg methylation and MeHg demethylation. [ABSTRACT FROM AUTHOR]

Mangrove sediments act as an important natural sink and a secondary source for trace metals. The main objective of this study was to investigate metal contamination and its relationship to mangrove-derived carbohydrates in mangrove sediments. Sixteen metals (Be, V, Cr, Co, Ni, Cu, Zn, Ga, As, Sr, Cd, Sn, Sb, Ba, Tl, and Pb）were analyzed in the surface sediments from four sites at different latitudes on the southeast coastline of China. The sedimentary organic matter was characterized by Rock-Eval pyrolysis, and the neutral sugars were examined by gas chromatograph mass spectrometry. Our results from the enrichment factors indicated that the mangrove sediments were no enriched by Ga, Sr, and Ba, minor enriched by Be, V, Cr, Co, Ni, Cu, Zn, As, Sn, Sb, Tl, and Pb, and moderate enriched by Cd. Litterfall was a major source of organic matter in the mangrove sediments, and the neutral sugars were mainly derived from this litterfall. Significant correlations were detected between the total organic carbon, pyrolytic parameters, neutral sugars, and enrichment factors of V, Cr, Co, Ni, Zn, and Cd, suggesting the input of neutral carbohydrates played an important role in enhancing the metal accumulation in the mangrove sediments. The mangrove litterfall itself was a major source of metals for the sediments, and the mangrove-derived organic matter enhanced the sediment's metal accumulation. • Metal concentrations in mangrove sediments decreased from low to high latitudes. • Litterfall was the main source of organic matter in the mangrove sediments. • V, Cr, Co, Ni, Zn, Cd were strongly correlated with mangrove-derived carbohydrates. • Litterfall was both a metal source and metal storage pool in the sediments. [ABSTRACT FROM AUTHOR]