Horizontal and vertical variability of mercury species in pore water and sediments in small lakes in Ontario

Mary Lake, St. George Lake, and Philips Lake are located in the Greater Toronto Area, Ontario, Canada. These lakes are relatively small and have no direct inflow and outflow channels. Mercury (Hg) input to the lakes comes mainly from atmospheric deposition. Sediment cores from the points of the maximum lake depth and surface sediment samples from the points of maximum lake depth to the bank of each lake were collected in October 2005. Total and methyl mercury concentrations in the pore water and sediments of these samples were determined. In these small lakes with high organic content, there was no correlation between organic content and total mercury (THg) in the samples throughout the entire sediment cores while strong positive correlation between these two parameters was observed in all the surface sediments. Compared with typical methylmercury (MeHg) depth-profiles of sediment cores in other studies, where MeHg concentrations and methylation rates decreased sharply with increasing depth, MeHg distributions in the sediment cores in this study showed that MeHg might have been produced not only in the upper sediment but also in the deeper sediments, which resulted in a larger MeHg reservoir in the sediment. Organic matter, to some extent, affected MeHg distributions in the samples throughout the entire sediment cores. Concentrations of MeHg in all the surface sediments, however, were not controlled by organic matter, whereas they were largely a function of water column depths. Total mercury concentrations in pore water were relatively homogenous in both the sediment cores and surface sediment while MeHg in pore water generally deceased with increasing depth in the sediment cores and increasing distance from the centre of the lakes in surface sediments. Methylmercury contributed 1% to 76% of THg in the pore water samples. Concentrations and distributions of MeHg in overlying water and sediment-surface water in Mary Lake and St. George Lake suggested that both in situ production of MeHg in lake water and the release of MeHg from sediment contributed to high MeHg in deep anoxic water.     

Early diagenetic processes aspects controlling the mobility of dissolved trace metals in three riverine sediment columns

The behaviour of Mn, Fe, Co, Zn, Cd, Pb and Ni has been studied during early diagenesis in three different riverine sediments (Spierre, Lys and Sheldt). For that purpose (1) pore waters were extracted from sediment cores by centrifugation under nitrogen and further analyzed for the determination of total dissolved metal concentrations and (2) DET and DGT probes have been deployed in situ for the determination of high resolution profiles of labile and total dissolved metal concentrations. Furthermore, sulfidization processes have been examined; they revealed a production of pyrite near the water-sediment interface at Helkijn and Wervik sampling sites, probably due to a partial re-oxidation of reduced sulphur species. In Spierre sediments, where Eh values are the most negative, pyrite production should be mainly due to strict anaerobic processes. Concentrations of AVS in Spierre sediments are also very high and result in low TI values and low trace metal concentrations in the pore waters. Otherwise, in Wervik sediments, the low pH values combined to a TI value close to 0 results in the highest observed dissolved trace metal levels. DOS remains low at the three sites, since it does not exceed 0.4. In Wervik and Helkijn, the limitation is probably due to low sedimentary inputs of sulphate. In Spierre, sulphate is never exhausted in the pore water, suggesting a limitation of the DOS by a lack of bio-degradable organic matter. Values of Cd, Cu and Pb DGT concentrations remain low in pore waters whatever the site, due to their strong affinity with the reduced sulphur pool. It has also been demonstrated that the labile fractions of Pb and Cd are the lowest and do not exceed 0.5, while Co and Ni are the most available metals.     

Dredging-related mobilisation of trace metals: a case study in The Netherlands

Mobilisation of contaminants is an important issue in environmental risk assessment of dredging projects. This study has aimed at identifying the effects of dredging on mobilisation of trace metals (Zn, Cu, Cd and Pb). The intensities and time scales of trace metal mobilisation were investigated during an experimental dredging project conducted under field conditions. The loss of contaminated dredge spoil is mainly reflected by increasing levels of trace metals in the suspended matter, dissolved trace metal concentrations in the water column are not significantly influenced by the dredging activities. This indicates a strong binding mechanism of trace metals to the solid phase or a fast redistribution over sorptive phases in response to oxidation of e.g. trace metal sulphides. Given the differences in levels of reactive phases (Mn, Fe, sulphides and organic matter) between the riverine suspended matter and the sediments, changes in the levels of these parameters in the suspended matter upon dredging may give information on the processes influencing the behaviour of trace metals and on the potential loss of sediment during dredging operations. Therefore, we recommend to routinely measure these parameters in studies on contaminant behaviour related to dredging activities.     

Importance of organic matter lability for monomethylmercury production in sulfate-rich marine sediments

Sediment cores were collected from two shallow sites in the Venice Lagoon, Italy, in order to study the lability of organic matter and the methylation rate of inorganic Hg(II). Measurements were made of concentrations of total Hg and monomethylmercury (MMHg), Hg(II) methylation rates, concentrations of total organic carbon and total nitrogen in the sediments, and dissolved sulfate, sulfide, and alkalinity in sedimentary pore waters. A positive linear relationship was detected between the specific Hg(II) methylation rate constant and the fraction of total Hg comprised of MMHg (%MMHg/Hg), indicating that short-term Hg(II) methylation rate reflects a long-term accumulation of MMHg in sediment. In addition, the %MMHg/Hg and specific Hg(II) methylation rate constant in sediment increased with decreasing ratios of total organic carbon to total nitrogen (C/N), whereas concentrations of dissolved sulfate, sulfide, and alkalinity in pore water remained constant. This result suggests that the Hg(II) methylation rate was affected by lability of organic matter. In particular, surface sediments, which contained large fractions of fresh algal organic material (C/N = 5.8-7.8), showed higher Hg(II) methylation rates than did deeper sediments (C/N > 10). Our results indicate that the C/N ratio can be used as a proxy for the lability of organic matter that influences Hg(II) methylation rate in sulfate-rich marine sediments.     

Ion concentrations in interstitial water as indicators for phosphorus release processes and reactions

Sediment composition and interstitial water concentrations of soluble reactive phosphorus (SRP), dissolved iron, ammonia nitrogen and dissolved organic carbon and pH were monitored at five sampling stations in the shallow Lake Loosdrecht (The Netherlands). The differences in concentrations between the sediments were much larger than the differences in overall sediment composition. The concentrations of SRP and ammonia were strongly correlated, the ratio between them was close to that predicted from a mineralization model.Possibly, the high concentrations of refractory organic material in the sediments affect the availability of iron. The pore water was calculated to be frequently supersaturated with respect to vivianite. This, however, did not seem to affect the phosphate concentrations in the pore water.     

Photo-induced formation of dissolved gaseous mercury in coastal and offshore seawater of the Mediterranean basin

The first measurements on the daily trend of dissolved gaseous mercury (DGM) concentration determined in coastal and offshore waters of the Mediterranean basin are reported. Marked daily behaviour tracking solar radiation has been observed at the coastal sampling station with DGM values ranging from 11.0 to 38.9 pg/l. Contrary to these observations the DGM values in offshore water samples (11.9-20.0 pg/l) were independent of the sampling time, thus identifying the absence of higher levels during the hours of maximum insolation. The availability of Hg2+ substrate necessary for the photo-reaction processes of DGM formation has been evaluated by measuring the reactive mercury concentration. In offshore waters the lower DGM concentrations are attributable to the substrate as a limiting factor. The highest concentration of DOC measured in coastal seawater with respect to the offshore one could moreover enhance the reaction rates of DGM production through the formation of inorganic mercury complexes and weaker organic associations.     

On the use of the partitioning approach to derive Environmental Quality Standards (EQS) for persistent organic pollutants (POPs) in sediments: a review of existing data

A review of experimental data has been performed to study the relationships between the concentration in water, pore water and sediments for different families of organic contaminants. The objective was to determine whether it is possible to set EQS for sediments from EQS defined for surface waters in the Daughter Directive of the European Parliament (COM (2006) 397). The analysis of experimental data showed that even though in some specific cases there is a coupling between water column and sediments, this coupling is rather the exception. Therefore it is not recommendable to use water column data to assess the chemical quality status of sediments and it is necessary to measure in both media. At the moment EQS have been defined for the water column and will assess only the compliance with good chemical status of surface waters. Since the sediment toxicity depends on the dissolved pore water concentration, the EQS developed for water could be applied to pore water (interstitial water); hence, there would be no need of developing another set of EQS. The partitioning approach has been proposed as a solution to calculate sediment EQS from water EQS, but the partitioning coefficient strongly depends on sediment characteristics and its use introduces an important uncertainty in the definition of sediment EQS. Therefore, the direct measurement of pore water concentration is regarded as a better option.     

Isolation of mercury resistant bacteria and influence of abiotic factors on bioavailability of mercury -- a case study in Pulicat Lake North of Chennai, South East India

Pulicat Lake sediments are often severely polluted with mercury compounds and other toxic heavy metals. Several mercury-resistant bacteria were isolated and identified from the sediments and all the isolates exhibited broad spectrum resistance (both organic and inorganic mercuric compounds). Mercury volatilization showed that four of the isolated Bacillus cereus strains were able to reduce water soluble ionic form of mercury into volatile form via the well known enzymatic reduction. The effect of increasing concentration of mercuric chloride and phenyl mercuric acetate in the growth of this mercury reducing strain was also determined. To study the native physico-chemical parameters, which influence the bioavailability of mercury to bacteria in Pulicat Lake ecosystem, a total of 60 water and 30 sediment samples were collected and analyzed for pH, temperature, dissolved oxygen, salinity, nitrate, nitrite, silicate, phosphate, organic matter and organic carbon. Increased levels of phosphate, nitrite, nitrate, silicate, organic matter and organic carbon during the post monsoon reduce the bioavailability of mercury by forming complexes which may increase the concentration of mercury in the sediments during post monsoon.     

The role of suspended solids in the estuarine geochemistry of mercury

The behaviour of mercury in total water (soluble + particulate fractions) and suspended solids of the surface waters of the Wyre estuary, northwest England, has been studied during a tidal cycle. The estuary is contaminated by mercury derived from chlor-alkali effluents and other sources. The results from eight stations in the estuary show that quantitatively mercury in suspended solids dominates the mercury budget of the estuarine waters. At high chlorinity periods in the tidal cycle the mercury concentrations in suspended solids decreased significantly, and can be related to changes in the specific surface area and organic carbon contents of the suspended matter. A very good correlation between mercury and organic carbon concentrations in the suspended solids exists, and laboratory experiments support the conclusion that mercury is mainly associated with the organic phase of the suspended material and is not easily chemically desorbed during estuarine mixing processes.     

Dissolved gaseous mercury formation under UV irradiation of unamended tropical waters from French Guyana

Filtered and non-filtered natural waters from French Guyana were irradiated with lamps emitting within the wavelength range 300-450 nm for 4 days with and without oxygen. Dissolved gaseous mercury (DGM) evolution was observed and quantified in the course of the irradiation. Measurements of total mercury in waters prior to and after the irradiations were also performed. The mass balance in the various mercury species (Hg(total), Hg(reactive) and DGM) proves the capability of the light to extract the mercury linked to the organic matter. DGM evolvement was greater in N2- than in air-saturated solutions, and the formation of volatile oxidized species can account for the inhibiting effect of oxygen. Filtration did not affect the mercury photoreduction, but reduced the formation of DGM in the dark. Great care has to be taken with regard to the following artifact: it was found that DGM originated not only from the natural waters, but also from the experimental device itself when exposed to the light. These non-expected DGM entries were quantitatively evaluated. This stresses the difficulty in measuring mercury at environmental concentrations.     

Field evidence for copper mobilization by dissolved organic matter

Fluxes of copper from the sediments to the water column in response to the presence of dissolved organic matter were measured in field enclosures placed on the floor of the Contrary Creek arm of Lake Anna, Virginia. Experimental chambers received a spike input of either sodium humate or phytoplankton; unamended chambers served as controls. Over the subsequent five days, water samples were withdrawn from the chambers and analyzed for total and dissolved copper, total and dissolved organic carbon (DOC) Eh, pH, dissolved oxygen, dissolved sulfides and heterotrophic microbial activity. Chambers amended with phytoplankton did not experience a rise in dissolved copper concentrations. Furthermore, the concentrations of dissolved copper in these chambers were not well-correlated with DOC concentrations (r = 0.1175, P = 0.642). Dissolved copper concentrations in chambers amended with sodium humate rose approximately 500% and remained elevated for the duration of the experimental trial (5 days). In this treatment, dissolved copper concentrations were well-correlated with DOC concentrations (r = 0.798, P < 0.005). The increase in dissolved copper in the chambers amended with sodium humate was observed to persist despite reducing conditions which were confirmed by redox measurements and the occurrence of dissolved sulfides. The addition of sodium humate to the chamber water resulted in a net mobilization of copper to the water column from the sediments. In contrast, dissolved organic carbon generated by the decomposition of phytoplankton did not appear to mobilize copper over the time interval examined. None of the changes in soluble copper concentrations could be related to Eh or pH effects. Supplementary laboratory experiments corroborated the field trials. The results suggest that long term (but not short term) products of decomposition processes may enhance the concentration of dissolved copper in the water column by the formation of soluble organometallic complexes.     

Mineralogical and geochemical controls of arsenic speciation and mobility under different redox conditions in soil, sediment and water at the Mokrsko-West gold deposit, Czech Republic

Naturally contaminated soil, sediment and water at the Mokrsko-West gold deposit, Central Bohemia, have been studied in order to determine the processes that lead to release of As into water and to control its speciation under various redox conditions. In soils, As is bonded mainly to secondary arseniosiderite, pharmacosiderite and Fe oxyhydroxides and, rarely, to scorodite; in sediments, As is bonded mainly to Fe oxyhydroxides and rarely to arsenate minerals.The highest concentrations of dissolved As were found in groundwater (up to 1141 μg L^− 1), which mostly represented a redox transition zone where neither sulphide minerals nor Fe oxyhydroxide are stable. The main processes releasing dissolved As in this zone are attributed to the reductive dissolution of Fe oxyhydroxides and arsenate minerals, resulting in a substantial decrease in their amounts below the groundwater level. Some shallow subsurface environments with high organic matter contents were characterized by reducing conditions that indicated a relatively high amount of S^− 2,0 in the solid phase and a lower dissolved As concentration (70-80 μg L^− 1) in the pore water. These findings are attributed to the formation of Fe(II) sulphides with the sorbed As. Under oxidizing conditions, surface waters were undersaturated with respect to arsenate minerals and this promoted the dissolution of secondary arsenates and increased the As concentrations in the water to characteristic values from 300 to 450 μg L^− 1 in the stream and fishpond waters. The levels of dissolved As(III) often predominate over As(V) levels, both in groundwaters and in surface waters. The As(III)/As(V) ratio is closely related to the DOC concentration and this could support the assumption of a key role of microbial processes in transformations of aqueous As species as well as in the mobility of As.     

Mercury emission from a temperate lake during autumn turnover

Lakes in temperate regions stratify during summer and winter months, creating distinct layers of water differentiated by their physical and chemical characteristics. When lakes mix in autumn and spring, mercury cycling may be affected by the chemical changes that occur during mixing. Sampling was conducted in Lake Lacawac, Eastern Pennsylvania, USA, throughout the autumn of 2007 to characterize changes in emission of gaseous elemental mercury (Hg⁰) from the lake surface and dissolved mercury profiles in the water column during mixing. Water chemistry and weather parameters were also measured, including dissolved organic carbon (DOC), iron, and solar radiation which have been shown to interact with mercury species. Results indicate that emission of Hg⁰ from the lake to the atmosphere during turnover was controlled both by solar radiation and by surface water mercury concentration. As autumn turnover progressed through the months of October and November, higher mercury concentration water from the hypolimnion mixed with epilimnetic water, increasing mercury concentration in epilimnetic waters. Dissolved absorbance was significantly correlated with mercury concentrations and with iron, but DOC concentrations were essentially constant throughout the study period and did not exhibit a relationship with either dissolved mercury concentrations or emission rates. Positive correlations between dissolved mercury and iron and manganese also suggest a role for these elements in mercury transport within the lake, but iron and manganese did not demonstrate a relationship with emission rates. This research indicates that consideration of seasonal processes in lakes is important when evaluating mercury cycling in aquatic systems.     

Sediment mercury dynamics and historical trends of mercury deposition in the St. Lawrence River area of concern near Cornwall, Ontario, Canada

The St. Lawrence River near Cornwall, Ontario was designated an Area of Concern by the International Joint Commission in 1985. Sediments from this area have historically been contaminated with mercury (Hg), and although concentrations have decreased since the 1970s, they still remain high. Nine sediment cores were collected from three sites within the Area of Concern in 2004/05 to determine the variability in historical profiles of Hg deposition to the river. Sediment and pore water phases were analyzed for total mercury (THg) and methyl mercury (MeHg) and cores were analyzed for ²¹⁰Pb to determine chronologies of sedimentation at these sites. Mercury diffusion rates in pore waters within the sediment column were determined to be very low (between 0 and 2.15 ng cm^− 2 year^− 1, n = 3) compared to the recent Hg sedimentation rates at these sites (183 ± 30 ng cm^− 2 year^− 1 SE, n = 9) determined by multiplying surface Hg concentrations with ²¹⁰Pb-derived sedimentation rates. These results indicate that Hg profiles in these cores accurately depict historical releases of Hg to the river bed. The influence of federal regulations in the early 1970s to restrict Hg emissions to the river was apparent in these dated sediment cores, as were the closures of several local industries in the mid 1990s. Mercury accumulation rates prior to 1970 were 60 times higher than those occurring after 1995. Methyl mercury showed surface enrichment in most of these sediment cores providing evidence that mercury methylation occurred most rapidly near the sediment surface.     

Behaviour of Hg species in a microtidal deltaic system: the Isonzo River mouth (northern Adriatic Sea)

Mercury species in the highly stratified water column of the Isonzo River mouth (northern Adriatic Sea) were investigated in February, May and August 2002 (low-normal fluvial discharge). Total, dissolved and particulate mercury (Hg) and methylmercury (MeHg) were measured and their concentrations were related to physico-chemical parameters in terms of temperature, salinity, turbidity, O(2) concentrations and total suspended matter (TSM) as well as particulate organic carbon (POC) content. Particulate Hg and MeHg are well correlated to medium-fine silty suspended sediment and organic matter, respectively. Desorption of Hg from particles in the brackish layer was observed. Due to the presence of a saltwedge, the lower river course seems to be a trap for Hg carried by fluvial waters. MeHg normally decreases approaching the sea but the local increase in the inner zone of the saltwedge could be related to methylation processes in the bottom water layer. Hg export is effective only during medium and high riverine flows acting as an important source of Hg into the northern Adriatic and the adjacent lagoon system.     

Mercury and methylmercury in the Gulf of Trieste (northern Adriatic Sea)

The distribution, sources and fate of mercury (Hg) in the water column of the Gulf of Trieste (northern Adriatic Sea), affected by the Hg polluted river Soca/Isonzo for centuries draining the cinnabar-rich deposits of the Idrija mining district (NW Slovenia), were studied in terms of total and dissolved Hg, reactive Hg, total and dissolved methylmercury (MeHg), mesozooplankton Hg and MeHg, and sedimentation rates of particulate Hg. Higher total Hg concentrations in the surface layer were restricted to the area of the Gulf in front of the river plume expanding in a westerly direction. Higher concentrations in bottom water layers were the consequence of sediment resuspension. Dissolved Hg exhibited higher concentrations in the surface layer in the area in front of the river plume. Higher bottom concentrations of dissolved Hg observed at some stations were probably due to remobilization from sediments, including resuspension and benthic recycling. The relationship between dissolved Hg in the surface layer and salinity showed nonconservative mixing in June 1995 during higher riverine inflow and nearly conservative mixing in September 1995 during lower riverine inflow. Both mixing curves confirm the river Soca/Isonzo to be the most important source of total and dissolved Hg, which are significantly correlated, in the Gulf. Reactive Hg is significantly correlated with dissolved Hg, indicating that the majority of dissolved Hg is reactive and potentially involved in biogeochemical transformations. The higher total MeHg in the bottom layer is the result of remobilization of MeHg from sediments including benthic fluxes. Strong seasonal variation of sedimentation rates of particulate Hg was found during a 2-year study in the central part of the Gulf. These variations followed those of total sedimented matter, indicating that sedimented Hg is mostly associated with inorganic matter. About a 2.5-fold higher fluxes of particulate Hg were observed at the depth of 20 m relative to 10 m which is attributed to bottom sediment resuspension. Temporal variability of mesozooplankton Hg and MeHg is the consequence of biomass and species variations, and grazing behaviour. From the preliminary Hg mass balance it appears that the Gulf is an efficient trap for total Hg and a net source of MeHg.     

An evaluation of freezing as a preservation technique for analyzing dissolved organic C, N and P in surface water samples

Techniques for preserving surface water samples are recently in demand because of the increased interest in quantifying dissolved organic matter (DOM) in surface waters and the frequent collection of samples in remote locations. Freezing is a common technique employed by many researchers for preserving surface water samples; however, there has been little evaluation of the effects of freezing on DOM concentrations. Ten streams were sampled in southeast Alaska with a range of dissolved organic carbon (DOC) concentrations (1.5 to 39 mg C L(-1)) to evaluate the influence of freezing (flash and standard freeze) and filter pore size (0.2 and 0.7 mum nominal pore size) on dissolved organic C, N and P concentrations. We report a significant decrease in DOC (p<0.005) and total dissolved P (p<0.005) concentrations when streamwater samples were frozen, whereas concentrations of dissolved organic N did not significantly decrease after freezing (p=0.06). We further show that when surface water samples were frozen, there was a decrease in the specific ultraviolet absorbance (SUVA) of DOC that is particularly evident with high concentrations of DOC. This finding suggests that spectroscopic properties of DOC have the potential to be used as indicators of whether surface water samples can be frozen. Our results lead us to recommend that surface water samples with high DOC concentrations (>5 mg C L(-1)) and/or samples with high SUVA values (>3.5-4 L mg-C(-1) m(-1)) should be analyzed immediately and not frozen.     

Removal of inorganic mercury and methylmercury from surface waters following coagulation of dissolved organic matter with metal-based salts

The presence of inorganic mercury (IHg) and methylmercury (MeHg) in surface waters is a health concern worldwide. This study assessed the removal potential use of metal-based coagulants as a means to remove both dissolved IHg and MeHg from natural waters and provides information regarding the importance of Hg associations with the dissolved organic matter (DOM) fraction and metal hydroxides. Previous research indicated coagulants were not effective at removing Hg from solution; however these studies used high concentrations of Hg and did not reflect naturally occurring concentrations of Hg. In this study, water collected from an agricultural drain in the Sacramento-San Joaquin Delta was filtered to isolate the dissolved organic matter (DOM) fraction. The DOM was then treated with a range of coagulant doses to determine the efficacy of removing all forms of Hg from solution. Three industrial-grade coagulants were tested: ferric chloride, ferric sulfate, and polyaluminum chloride. Coagulation removed up to 85% of DOM from solution. In the absence of DOM, all three coagulants released IHg into solution, however in the presence of DOM the coagulants removed up to 97% of IHg and 80% of MeHg. Results suggest that the removal of Hg is mediated by DOM-coagulant interactions. There was a preferential association of IHg with the more aromatic, higher molecular weight fraction of DOM but no such relationship was found for MeHg. This study offers new fundamental insights regarding large-scale removal of Hg at environmentally relevant regarding large-scale removal of Hg at environmentally relevant concentrations.     

Nitrous oxide sources and sinks in coastal aquifers and coupled estuarine receiving waters

Sources and sinks of the atmospherically reactive gas nitrous oxide (N(2)O) were determined in the heavily nutrient loaded Childs River in Cape Cod, MA. Surface waters were supersaturated and bottom waters were depleted with N(2)O throughout the system. In apparent septic effluent plumes, N(2)O concentrations reached 3 orders of magnitude above atmospheric equilibrium. Because nitrate and N(2)O concentrations correlated in groundwater entering the estuary, septic tank effluent appeared responsible for the supersaturated concentrations of N(2)O in surface waters. A hyperbolic function fit nitrate and N(2)O concentrations in the water column of the estuary with a maximum supersaturation of approximately 60 nM. From surface water supersaturation we predicted a release of 480 nmol N(2)O m(-2) h(-1) to the atmosphere in the summer. Property plots of salinity vs. bottom-water N(2)O suggested a benthic sink of N(2)O. Consistent with this trend, sediments consumed rather than released N(2)O in most flux measurements. Nutrient loading did not directly alter benthic N(2)O flux, potentially because stratification limited exposure of sediments to nitrate-rich surface waters, but macroalgal cover increased benthic N(2)O consumption. Sediment N(2)O consumption averaged 111 nmol N(2)O m(-2) h(-1) and correlated with oxygen uptake. Losses from the system to the atmosphere and sediments exceeded inputs of N(2)O contaminated groundwater, which suggests missing N(2)O sources.     

Mercury distribution and speciation in Lake Balaton, Hungary

The distribution and speciation of mercury in air, rain, lake water, sediment, and zooplankton in Lake Balaton (Hungary) were investigated between 1999 and 2002. In air, total gaseous mercury (TGM) ranged from 0.4 to 5.9 ng m(-3) and particulate phase mercury (PPM) from 0.01 to 0.39 ng m(-3). Higher concentrations of both TGM and PPM occurred during daytime. Higher concentrations of PPM occurred in winter. In rain and snow, total mercury ranged from 10.8 to 36.7 ng L(-1) in summer but levels up to 191 ng L(-1) in winter. Monomethylmercury (MMHg) concentrations ranged from 0.09 to 1.26 ng L(-1) and showed no seasonal variations. Total Hg in the unfiltered lake water varied spatially, with concentrations ranging from 1.4 to 6.5 ng L(-1). Approximately 70% of the total Hg is dissolved. MMHg levels ranged from 0.08 to 0.44 ng L(-1) as total and from 0.05 to 0.37 ng L(-1) in the dissolved form. Lower Hg concentrations in the water column occurred in winter. In suspended particulate matter and in sediment, total mercury ranged from 9 to 160 ng g(-1) dw, and MMHg ranged from 0.07 to 0.84 ng g(-1) dw. In zooplankton, an average mercury level of 31.0+/-6.8 ng g(-1) dw occurred, with MMHg accounting for approximately 17%. In sediments, suspended-matter- and zooplankton-high Hg and MMHg levels occurred at the mouth of the River Zala, but, in the lake, higher concentrations occurred on the Northern side, and an increasing trend from north-west to north-east was observed. In general, regarding Hg, Lake Balaton can be considered as a relatively uncontaminated site. The high-pH and well-oxygenated water as well as the low organic matter content of the sediment does not favour the methylation of Hg. In addition, bioconcentration and bioaccumulation factors are relatively low compared to other aquatic systems.