Preliminary Estimations of Insect Mediated Transfers of Mercury and Physiologically Important Fatty Acids from Water to Land.
ABSTRACT: Aquatic insects provide an energy subsidy to riparian food webs. However, most empirical studies have considered the role of subsidies only in terms of magnitude (using biomass measurements) and quality (using physiologically important fatty acids), negating an aspect of subsidies that may affect their impact on recipient food webs: the potential of insects to transport contaminants (e.g., mercury) to terrestrial ecosystems. To this end, I used empirical data to estimate the magnitude of nutrients (using physiologically important fatty acids as a proxy) and contaminants (total mercury (Hg) and methylmercury (MeHg)) exported by insects from rivers and lacustrine systems in each continent. The results reveal that North American rivers may export more physiologically important fatty acids per unit area (93.0 ± 32.6 Kg Km-2 year-1) than other continents. Owing to the amount of variation in Hg and MeHg, there were no significant differences in MeHg and Hg among continents in lakes (Hg: 1.5 × 10-4 to 1.0 × 10-3 Kg Km-2 year-1; MeHg: 7.7 × 10-5 to 1.0 × 10-4 Kg Km-2 year-1) and rivers (Hg: 3.2 × 10-4 to 1.1 × 10-3 Kg Km-2 year-1; MeHg: 3.3 × 10-4 to 8.9 × 10-4 Kg Km-2 year-1), with rivers exporting significantly larger quantities of mercury across all continents than lakes. Globally, insect export of physiologically important fatty acids by insect was estimated to be ~43.9 × 106 Kg year-1 while MeHg was ~649.6 Kg year-1. The calculated estimates add to the growing body of literature, which suggests that emerging aquatic insects are important in supplying essential nutrients to terrestrial consumers; however, with the increase of pollutants in freshwater systems, emergent aquatic insect may also be sentinels of organic contaminants to terrestrial consumers.
Project description:The Korean National Environmental Health Survey (KoNEHS 2009-2011) tracks levels of environmental pollutants in biological samples from the adult Korean population (age 19-88). Recent survey results for blood mercury (Hg) suggest some exceedance above existing blood Hg reference levels. Because total blood Hg represents both organic and inorganic forms, and methylmercury (MeHg) has been specifically linked to several adverse health outcomes, a need exists to quantify MeHg intake for this population. Gender, age, and frequency of fish consumption were first identified as important predictors of KoNEHS blood Hg levels using generalized linear models. Stratified distributions of total blood Hg were then used to estimate distributions of blood MeHg using fractions of MeHg to total Hg from the literature. Next, a published physiologically based pharmacokinetic (PBPK) model was used to predict distributions of blood MeHg as a function of MeHg intake; ratios of MeHg intake to model-predicted blood MeHg were then combined with KoNEHS-based blood MeHg values to produce MeHg intake estimates. These intake estimates were ultimately compared with the Reference Dose (RfD) for MeHg (0.1 µg/kg/day) and reported as margin of exposure (MOE) estimates for specific KoNEHS subgroups. The derived MOEs across all subgroups, based on estimated geometric mean intake, ranged from 1.6 to 4.1. These results suggest MeHg exposures approaching the RfD for several subgroups of the Korean population, and not just for specific subgroups (eg, those who eat fish very frequently).
Project description:Mercury (Hg) concentrations in aquatic environments have increased globally, exposing consumers of aquatic organisms to high Hg levels. For both aquatic and terrestrial consumers, exposure to Hg depends on their food sources as well as environmental factors influencing Hg bioavailability. The majority of the research on the transfer of methylmercury (MeHg), a toxic and bioaccumulating form of Hg, between aquatic and terrestrial food webs has focused on terrestrial piscivores. However, a gap exists in our understanding of the factors regulating MeHg bioaccumulation by non-piscivorous terrestrial predators, specifically consumers of adult aquatic insects. Because dissolved organic carbon (DOC) binds tightly to MeHg, affecting its transport and availability in aquatic food webs, we hypothesized that DOC affects MeHg transfer from stream food webs to terrestrial predators feeding on emerging adult insects. We tested this hypothesis by collecting data over 2 years from 10 low-order streams spanning a broad DOC gradient in the Lake Sunapee watershed in New Hampshire, USA. We found that streamwater MeHg concentration increased linearly with DOC concentration. However, streams with the highest DOC concentrations had emerging stream prey and spiders with lower MeHg concentrations than streams with intermediate DOC concentrations; a pattern that is similar to fish and larval aquatic insects. Furthermore, high MeHg concentrations found in spiders show that MeHg transfer in adult aquatic insects is an overlooked but potentially significant pathway of MeHg bioaccumulation in terrestrial food webs. Our results suggest that although MeHg in water increases with DOC, MeHg concentrations in stream and terrestrial consumers did not consistently increase with increases in streamwater MeHg concentrations. In fact, there was a change from a positive to a negative relationship between aqueous exposure and bioaccumulation at streamwater MeHg concentrations associated with DOC above ~5 mg/L. Thus, our study highlights the importance of stream DOC for MeHg dynamics beyond stream boundaries, and shows that factors modulating MeHg bioavailability in aquatic systems can affect the transfer of MeHg to terrestrial predators via aquatic subsidies.
Project description:Aquatic ecosystems are an essential component of the biogeochemical cycle of mercury (Hg), as inorganic Hg can be converted to toxic methylmercury (MeHg) in these environments and reemissions of elemental Hg rival anthropogenic Hg releases on a global scale. Quantification of effluent Hg releases to aquatic systems globally has focused on discharges to the global oceans, rather than contributions to freshwater systems that affect local exposures and risks associated with MeHg. Here we produce a first-estimate of sector-specific, spatially resolved global aquatic Hg discharges to freshwater systems. We compare our release estimates to atmospheric sources that have been quantified elsewhere. By analyzing available quantitative and qualitative information, we estimate that present-day global Hg releases to freshwater environments (rivers and lakes) associated with anthropogenic activities have a lower bound of ~1000 Mg· a-1. Artisanal and small-scale gold mining (ASGM) represents the single largest source, followed by disposal of mercury-containing products and domestic waste water, metal production, and releases from industrial installations such as chlor-alkali plants and oil refineries. In addition to these direct anthropogenic inputs, diffuse inputs from land management activities and remobilization of Hg previously accumulated in terrestrial ecosystems are likely comparable in magnitude. Aquatic discharges of Hg are greatly understudied and further constraining associated data gaps is crucial for reducing the uncertainties in the global biogeochemical Hg budget.
Project description:The paper's objective was to estimate weekly Hg intake from fish meals based on intervention research. Total Hg (THg) concentrations in blood and hair samples collected from men (n = 67) from an intervention study as well as muscular tissues of fresh and after heat-treating fish were determined using the thermal decomposition amalgamation atomic absorption spectrometry method (TDA-AAS) using direct mercury analyzer (DMA-80). The mean of the estimated weekly intake (EWI) was estimated at 0.62 μg/kg bw/week in the range 0.36-0.96 μg/kg body weight (bw) /week through the consumption of 4 edible marine fish species every day (for 10 days) by the participants from the intervention research in Lodz, Poland. The Hg intake in the volunteers in our intervention study accounted for 38.6% of the provisional tolerable weekly intake (PTWI) (1.6 μg/kg bw, weekly) value. The average Hg concentration in the analyzed fish ranged from 0.018 ± 0.006 mg/kg wet weight (Gadus chalcogrammus) to 0.105 ± 0.015 mg/kg wet weight (Macruronus magellanicus). The results for the average consumers were within PTWI of methylmercury (MeHg). Moreover, the average concentration of Hg in the selected fish after heat treatment did not exceed the maximum permitted concentrations for MeHg (MPCs = 0.5 mg/kg wet weight) in food set by the European Commission Regulation (EC/1881/2006). Hence, the risk of adverse effects of MeHg for the participants is substantially low.
Project description:The flux of dissolved organic carbon (DOC) from mangrove swamps accounts for 10% of the global terrestrial flux of DOC to coastal oceans. Recent findings of high concentrations of mercury (Hg) and methylmercury (MeHg) in mangroves, in conjunction with the common co-occurrence of DOC and Hg species, have raised concerns that mercury fluxes may also be large. We used a novel approach to estimate export of DOC, Hg, and MeHg to coastal waters from a mangrove-dominated estuary in Everglades National Park (Florida, USA). Using in situ measurements of fluorescent dissolved organic matter as a proxy for DOC, filtered total Hg, and filtered MeHg, we estimated the DOC yield to be 180 (±12.6) g C m(-2) yr(-1), which is in the range of previously reported values. Although Hg and MeHg yields from tidal mangrove swamps have not been previously measured, our estimated yields of Hg species (28 ± 4.5 ?g total Hg m(-2) yr(-1) and 3.1 ± 0.4 ?g methyl Hg m(-2) yr(-1)) were five times greater than is typically reported for terrestrial wetlands. These results indicate that in addition to the well documented contributions of DOC, tidally driven export from mangroves represents a significant potential source of Hg and MeHg to nearby coastal waters.
Project description:Reservoirs typically have elevated fish mercury (Hg) levels compared to natural lakes and rivers. A unique feature of reservoirs is water-level management which can result in sediment exposure to the air. The objective of this study is to identify how reservoir water-level fluctuations impact Hg cycling, particularly the formation of the more toxic and bioaccumulative methylmercury (MeHg). Total-Hg (THg), MeHg, stable isotope methylation rates and several ancillary parameters were measured in reservoir sediments (including some in porewater and overlying water) that are seasonally and permanently inundated. The results showed that sediment and porewater MeHg concentrations were over 3-times higher in areas experiencing water-level fluctuations compared to permanently inundated sediments. Analysis of the data suggest that the enhanced breakdown of organic matter in sediments experiencing water-level fluctuations has a two-fold effect on stimulating Hg methylation: 1) it increases the partitioning of inorganic Hg from the solid phase into the porewater phase (lower log Kd values) where it is more bioavailable for methylation; and 2) it increases dissolved organic carbon (DOC) in the porewater which can stimulate the microbial community that can methylate Hg. Sulfate concentrations and cycling were enhanced in the seasonally inundated sediments and may have also contributed to increased MeHg production. Overall, our results suggest that reservoir management actions can have an impact on the sediment-porewater characteristics that affect MeHg production. Such findings are also relevant to natural water systems that experience wetting and drying cycles, such as floodplains and ombrotrophic wetlands.
Project description:The bioaccumulation of the neurotoxin methylmercury (MeHg) in freshwater ecosystems is thought to be mediated by both water chemistry (e.g., dissolved organic carbon [DOC] and dissolved mercury [Hg]) and diet (e.g., trophic position and diet composition). Hg in small streams is of particular interest given their role as a link between terrestrial and aquatic processes. Terrestrial processes determine the quantity and quality of streamwater DOC, which in turn influence the quantity and bioavailability of dissolved MeHg. To better understand the effects of water chemistry and diet on Hg bioaccumulation in stream biota, we measured DOC and dissolved Hg in stream water and mercury concentration in three benthic invertebrate taxa and three fish species across up to 12 tributary streams in a forested watershed in New Hampshire, USA. As expected, dissolved total mercury (THg) and MeHg concentrations increased linearly with DOC. However, mercury concentrations in fish and invertebrates varied non-linearly, with maximum bioaccumulation at intermediate DOC concentrations, which suggests that MeHg bioavailability may be reduced at high levels of DOC. Further, MeHg and THg concentrations in invertebrates and fish, respectively, increased with ?15N (suggesting trophic position) but were not associated with ?13C. These results show that even though MeHg in water is strongly determined by DOC concentrations, mercury bioaccumulation in stream food webs is the result of both MeHg availability in stream water and trophic position.
Project description:Microorganisms are key players in the transformation of mercury into neurotoxic methylmercury (MeHg). Nevertheless, this mechanism and the opposite MeHg demethylation remain poorly understood. Here, we explored the impact of inorganic mercury (IHg) and MeHg concentrations from 0.05 to 50 ?M on the production and degradation of MeHg in two sulfate-reducing bacteria, Pseudodesulfovibrio hydrargyri BerOc1 able to methylate and demethylate mercury and Desulfovibrio desulfuricans G200 only able to demethylate MeHg. MeHg produced by BerOc1 increased with increasing IHg concentration with a maximum attained for 5 ?M, and suggested a saturation of the process. MeHg was mainly found in the supernatant suggesting its export from the cell. Hg L3-edge High- Energy-Resolution-Fluorescence-Detected-X-ray-Absorption-Near-Edge-Structure spectroscopy (HERFD-XANES) identified MeHg produced by BerOc1 as MeHg-cysteine2 form. A dominant tetracoordinated ?HgS form was detected for BerOc1 exposed to the lowest IHg concentrations where methylation was detected. In contrast, at the highest exposure (50 ?M) where Hg methylation was abolished, Hg species drastically changed suggesting a role of Hg speciation in the production of MeHg. The tetracoordinated ?HgS was likely present as nano-particles as suggested by transmission electron microscopy combined to X-ray energy dispersive spectroscopy (TEM-X-EDS) and nano-X ray fluorescence (nano-XRF). When exposed to MeHg, the production of IHg, on the contrary, increased with the increase of MeHg exposure until 50 ?M for both BerOc1 and G200 strains, suggesting that demethylation did not require intact biological activity. The formed IHg species were identified as various tetracoordinated Hg-S forms. These results highlight the important role of thiol ligands and Hg coordination in Hg methylation and demethylation processes.
Project description:Methylmercury (MeHg) affects wildlife and human health mainly through marine fish consumption. In marine systems, MeHg is formed from inorganic mercury (Hg(II)) species primarily in sediments, then accumulates and biomagnifies in the food web. Most of the fish consumed in the United States are from estuarine and marine systems, highlighting the importance of understanding MeHg formation in these productive regions. Sediment organic matter has been shown to limit mercury methylation in estuarine ecosystems, as a result it is often described as the primary control over MeHg production. In this paper, we explore the role of organic matter by looking at the effects of its changing sediment concentrations on the methylation rates across multiple estuaries. We measured sedimentary MeHg production at eleven estuarine sites that were selected for their contrasting biogeochemical characteristics, mercury (Hg) content, and location in the Northeastern U.S. (ME, NH, CT, NY, and NJ). Sedimentary total Hg concentrations ranged across 5 orders of magnitude, increasing in concentration from the pristine, sandy sediments of Wells (ME), to industrially contaminated areas such as Portsmouth (NH) and Hackensack (NJ). We find that methylation rates are the highest at locations with high Hg content (relative to carbon), and that organic matter does not hinder mercury methylation in estuaries.
Project description:Due to global mercury pollution and the adverse health effects of prenatal exposure to methylmercury (MeHg), an assessment of the economic benefits of prevented developmental neurotoxicity is necessary for any cost-benefit analysis.Distributions of hair-Hg concentrations among women of reproductive age were obtained from the DEMOCOPHES project (1,875 subjects in 17 countries) and literature data (6,820 subjects from 8 countries). The exposures were assumed to comply with log-normal distributions. Neurotoxicity effects were estimated from a linear dose-response function with a slope of 0.465 Intelligence Quotient (IQ) point reduction per ?g/g increase in the maternal hair-Hg concentration during pregnancy, assuming no deficits below a hair-Hg limit of 0.58 ?g/g thought to be safe. A logarithmic IQ response was used in sensitivity analyses. The estimated IQ benefit cost was based on lifetime income, adjusted for purchasing power parity.The hair-mercury concentrations were the highest in Southern Europe and lowest in Eastern Europe. The results suggest that, within the EU, more than 1.8 million children are born every year with MeHg exposures above the limit of 0.58 ?g/g, and about 200,000 births exceed a higher limit of 2.5 ?g/g proposed by the World Health Organization (WHO). The total annual benefits of exposure prevention within the EU were estimated at more than 600,000 IQ points per year, corresponding to a total economic benefit between €8,000 million and €9,000 million per year. About four-fold higher values were obtained when using the logarithmic response function, while adjustment for productivity resulted in slightly lower total benefits. These calculations do not include the less tangible advantages of protecting brain development against neurotoxicity or any other adverse effects.These estimates document that efforts to combat mercury pollution and to reduce MeHg exposures will have very substantial economic benefits in Europe, mainly in southern countries. Some data may not be entirely representative, some countries were not covered, and anticipated changes in mercury pollution all suggest a need for extended biomonitoring of human MeHg exposure.