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Current knowledge about the transformation of total mercury and methylmercury (MeHg) in aerobic composting process is limited. In this study, the composition and transformation of mercury and dissovled organic matter (DOM) in aerobic composting process of municipal sewage sludge were were comprehensively characterized, and the differences among the three C/N ratio (20, 26 and 30) were investigated. The main form of mercury in C/N 20 and 26 was organo-chelated Hg (F3, 46%-60%); while the main form of mercury in C/N 30 was mercuric sulfide (F5, 64%-70%). The main component of DOM in C/N 20 and 26 were tyrosine-like substance (C1, 53%-76%) while the main fractions in C/N 30 were tyrosine-like substance (C1, 28%-37%) and fulvic-like substance (C2, 17%-39%). The mercury and DOM varied significantly during the 9 days composting process. Compared to C/N 20 and 26, C/N 30 produced the less MeHg after aerobic composting process, with values of 658% (C/N 20), 1400% (C/N 26) and 139% (C/N 30) of the initial, respectively. Meanwhile, C/N 30 produced the best compost showed greater degree of DOM molecular condensation and humification. Hg fraction had been altered by DOM, as indicated by a significant correlation between mercury species and DOM components. Notably, C/N 30 should be used as an appropriate C/N ratio to control the methylation processes of mercury and degration of DOM., 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 B.V.)

Sewage sludge (SS) production in China has increased rapidly, accompanying the fast expansion of its sewage treatment capacity. Heavy metals (HMs) in SS have been a great concern, hampering the utilization and disposal of SS. In this study, heavy metal (HM) contents in SS from throughout China were determined. The median values of HMs in SS decreased in the order Zn > Cu > Cr > Pb > Ni > As > Hg > Cd. The general attainment rates of HMs in SS are satisfying (> 90%). Combining the present data with those obtained from references, spatial distributions and temporal trends of HMs in SS were analyzed. Depending on the specific HM element, the spatial variation trend might be decreasing trends from south to north and from east to west of China. The element-specific hot spots of SS with relatively high HM contents were identified. Analysis of the historical data in different time intervals reviewed obvious decreasing trends in HM contents of SS in China, indicating the well implementation of more and more stringent environmental regulations.

Mercury (Hg) that leaches from municipal sewage sludge (MSS) landfill under natural rain is of increasing concern. The column leaching experiments were conducted to investigate the leaching characteristics of total mercury (THg) and methylmercury (MeHg) as well as pH, total organic carbon (TOC), and total suspended solids (TSS) in the raw sludge (RS) and lime-conditioned sludge (LCS) under simulated rain with different acidities (pH 6.5 and 2.9). Results showed the release of MeHg in the leachates presented different patterns from THg. And the final amounts of MeHg in the MSS columns were 1.49 (RS at pH = 6.5), 1.88 (RS at 2.9), 1.97 (LCS at pH = 6.5), and 2.06 times (LCS at pH = 2.9) higher than the initial amounts, suggesting methylation of inorganic Hg (IHg) occurred in the leaching process. The leaching efficiencies of THg and MeHg in RS was lower than that in LCS, indicating lime was more favorable for the release of THg and MeHg. And lower values of pH of the simulated rain promoted the release of THg and MeHg from RS while the opposite was true for LCS. This study provides a better understanding of the release and biogeochemical transformations of Hg in MSS., 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 Ltd. All rights reserved.)

Municipal sewage has been identified to be an important source of mercury (Hg) to the environment. However, as the major sink of sewage-borne Hg, sewage sludge (SS) remains unresolved in terms of the occurrence status of Hg species. We presented here, a nation-wide survey on the speciation of Hg in SS of China. Total Hg (THg) and methylmercury (MeHg) were detected in all SS samples, within ranges of 0.4-12.4 mg/kg and 0.1-27.0 μg/kg, respectively. Sludge-borne Hg mainly occurred in the mercury sulfide and organo-chelated phases, with only tiny portions occurring as soluble Hg. The mass loadings of sludge-borne THg and MeHg in China for year 2016 were estimated to be 12.2 metric tons and 19.9 kg, respectively. Landfill was the most important sink of sludge-borne Hg, followed by incineration, land application, and building materials., (Copyright © 2019 Elsevier Inc. All rights reserved.)

Wide occurrence of mercury species, including the highly toxic and readily bioaccumulative methylmercury (MeHg), in municipal sewage (MS) and sewage sludge (SS) has been evidenced in recent studies. Considering that vast amounts of MS and SS are produced globally each year and the majority of MS is discharged into aqueous environments, i.e., the main sites for MeHg bioaccumulation, special attention should be paid on the source and environmental behaviors of sewage-borne and sludge-borne mercury species. This review aims to summarize the findings on the occurrence of mercury species in MS and SS, their transport and transformation in MS treatment plants, as well as their fate and environmental implications.

Occurrence and fate of sewage- and sludge-borne total mercury (THg) and methylmercury (MeHg) have received little attention, although they might be an important component of the global Hg inventory. To address the knowledge gap, sewage and sewage sludge (SS) samples were collected from a secondary municipal sewage treatment plant (MSTP) located in Jiaozuo, China. Total Hg in the raw sewage varied between 95.3 ng/L and 1.2 × 10 3  ng/L, while MeHg occurred in the sewage within ranges of 2.7-21.3 ng/L. On average, 93.4% of THg and 89.1% of MeHg were removed from the raw sewage by the MSTP. Around 80% of net THg input into the MSTP was transported to the SS, while 80% of net MeHg input was decomposed during the treatment processes. Thus, MSTPs would be regarded as an important sink of sewage-borne THg and MeHg. On the other hand, MeHg widely occurred in the SS, with concentrations between 7.2 and 10.2 ng/g, accounting for 0.2% of the corresponding THg contents in the SS. Occurrence of THg and MeHg in the SS indicated that SS would be a significant source of MeHg and THg to the environment.

Municipal wastewater treatment plants (WWTPs) play an important role in controlling pollutant discharges to surface waters. Previous studies suggested that the removal of mercury (Hg) by WWTPs was strongly correlated with solid removal. However, conclusions regarding possible transformations of Hg species within WWTPs were not consistent across those studies. We characterized total Hg (THg) and methylmercury (MeHg) concentrations and loads in a WWTP located in Jiaozuo, China, to further understand Hg fate and transformations in WWTPs. THg and MeHg were primarily associated with wastewater solids, and removal of both were greater than 90%; concentrations in the sewage were (2.0±2.7)×10(3)ng/L and 7.5±5.8ng/L, respectively. A mass balance calculation revealed that 80% of the THg input to the WWTP ended up in the sewage sludge (SS), while more than 70% of the influent MeHg mass was degraded, indicating WWTPs are an important sink for sewage-borne Hg. THg and MeHg concentrations in SS were (3.9±1.4)×10(3)ng/g and 6.3±2.3ng/g, respectively, suggesting SS could be a significant source of THg and MeHg to the environment if not handled properly. The significance of sewage and SS in the biogeochemical cycling of THg and MeHg in China is discussed., (Copyright © 2015 Elsevier B.V. All rights reserved.)

The role of macrophytes in mercury (Hg) cycling in the Florida Everglades ecosystem has not been fully understood. In this study, a stable isotope ((199)Hg(2+)) addition technique was used to trace the methylation, uptake, and translocation of Hg by sawgrass ( Cladium jamaicense ) and quantitatively evaluate the contribution of atmospheric and soil Hg to Hg in sawgrass leaves and below-ground biomass. The results showed that spiked (199)Hg(2+) could be rapidly methylated to monomethylmercury (Me(199)Hg) in the soil of the sawgrass pots. Only small portions of total Hg (THg) and monomethylmercury (MeHg) in the soil could be taken up by sawgrass, indicated by the ratios of T(199)Hg and Me(199)Hg (tracer) concentrations in the sawgrass below-ground biomass (BGBM) over that in the soil (6.50 ± 1.9% and 12.8 ± 3.6% for THg and MeHg, respectively). Concentrations of T(199)Hg (tracer) and Me(199)Hg (tracer) in sawgrass leaves only accounted for 5.50 ± 2.8% and 15.6 ± 4.0%, respectively, of that in the BGBM, implying that the fractions of mercury species transported upward by sawgrass were also small. Statistical analysis (t test) showed that sawgrass preferred MeHg over THg in both uptake and upward translocation. The majority (>90%) of THg in sawgrass leaves were estimated to be obtained from atmospheric Hg, rather than from soil, suggesting that assimilation of atmospheric Hg could increase the overall Hg stock in the Florida Everglades ecosystem. The finding about foliar uptake of Hg is especially important for a better understanding of mercury cycling in the Everglades, given the large amount of sawgrass biomass in this ecosystem.

The methylation of inorganic Hg by anaerobic bacteria in aquatic environments is considered to be the major pathway for methylmercury (MeHg) production. However, recent research has suggested that abiotic or chemical methylation by humic substances and other low-molecular-weight organic compounds in natural environments is also possible. Here, the aqueous photo-transformation of Hg(2+) to organomercurials was investigated in the presence of ketones, aldehydes and low molecular weight organic acids under UV irradiation. MeHg and/or ethylmercury (EtHg) were identified as the main organomercurial products by multiple analytical techniques, including chromatography-atomic spectrometry and molecular mass spectrometry and further confirmed by stable isotope tracer experiments. The yield of organomercurials was markedly influenced by pH, NaCl concentration, alkylation donor concentration and the presence of chelating ligands in the aqueous solution. Electron paramagnetic resonance spectrometry demonstrated that the radical reaction was not the predominating alkylation pathway, although methyl radicals were detected in the photo-alkylation procedure. A mechanism based on intra-molecular alkyl transfer in the Hg(2+)-low-molecular-weight organic compound complex is proposed. The present work helps us better understand of MeHg and EtHg photo-generation in natural environments., (Copyright © 2012. Published by Elsevier Ltd.)

Methylmercury (MeHg) is recognized as one of the major water quality concerns in the Florida Everglades. Degradation of MeHg in the water is thought to be one of the most important processes to the cycling of MeHg, but there is a lack of quantitative estimations of its effect on the distribution and cycling of MeHg in this ecosystem. Stable isotope (Me201Hg) addition method was implemented to investigate the degradation of MeHg in the Everglades. By combining these results with the field monitoring data, effects of photodegradation on MeHg distribution and its contribution to MeHg cycling were estimated. The results indicate that degradation of MeHg in Everglades water is mediated by sunlight and that UV-A and UV-B radiations are the principal driver. The spatial pattern of MeHg photodegradation potential (PPD) generally illustrated an increasing trend from north to south in the Everglades, which was opposite to the distribution of MeHg in water column. Correlation analysis shows that MeHg concentration in the water had a significant negative relation to PPD, suggesting that photodegradation could play an important role in controlling the distribution of MeHg in Everglades water. Furthermore, about 31.4% of MeHg input into the water body was removed by photodegradation, indicating its importance in the biogeochemical cycling of MeHg in the Everglades. This percent reduction is much lower than that reported for other ecosystems, which could be caused by the higher concentration of DOC in the Everglades. The relatively slower degradation of MeHg could be one of the main reasons for the high ratio of MeHg to total mercury (THg) in this ecosystem.

Spatial patterns in mercury cycling and bioaccumulation at the landscape level in the Everglades were investigated by collecting and analyzing multimedia samples for mercury species and biogeochemical characteristics from 228 randomly located stations. Higher total mercury (THg) in environmental compartments (surface water, soil, flocculent detrital material (floc), and periphyton) generally occurred in the northern and central Everglades, but higher THg in water and periphyton in the Everglades National Park was an exception. Multiple biogeochemical characteristics, such as surface water dissolved organic matter (DOC(sw)), pH, chloride, and compositional properties of solid compartments (soil and floc), were identified to be important factors controlling THg distribution. Methylmercury (MeHg) was also higher in the northern Everglades for water, soil, and floc, but not for periphyton. Higher mosquitofish THg and bioaccumulation factor were observed in the central and southern Everglades, partially in accordance with periphyton MeHg distribution, but not in the "hot spot" areas of water, soil, or floc MeHg. The discrepancy in mercury bioaccumulation and mercury distribution in environmental compartments suggests that in addition to MeHg production, biogeochemical controls that make MeHg available to aquatic organisms, such as DOC(sw) and compositional properties of soil and floc, are important in mercury bioaccumulation.