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We investigated total mercury (THg) and methylmercury (MeHg) concentrations in coastal mussels (Mytilus spp.) sampled from the Minas Basin, Bay of Fundy and evaluated the relationship with condition index (CI). THg concentrations were low in sediment (mean THg = 5.15 ± 2.11 ng/g dw; n = 6) and soft tissues (mean THg = 62.3 ± 13.7 ng/g; mean MeHg = 13.2 ± 6.3 ng/g; n = 57). The THg in tissues had no significant relationship with CI (R s = -0.205, p = 0.126). MeHg in tissues were significantly and negatively correlated with condition index (R s = -0.361, p = 0.006) indicating that healthier mussels (higher CI) have lower mercury content possibly due to elimination strategies or growth dilution., (© 2024. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Quantifying mercury (Hg) concentrations in invertebrates is fundamental to determining risk for bioaccumulation in higher trophic level organisms in coastal food webs. Bioaccumulation is influenced by local mercury concentrations, site geochemistry, individual feeding ecologies, and trophic position. We sampled seven species of invertebrates from five coastal sites in the Minas Basin, Bay of Fundy, and determined body concentrations of methylmercury (MeHg), total mercury (THg), and stable isotopes of nitrogen (δ 15 N) and carbon (δ 13 C). To evaluate the effects of environmental chemistry on Hg production and bioaccumulation, bulk sediments from all sites were analysed for THg, %Loss on ignition (LOI) (carbon), and sulfur isotopes (δ 34 S), and concentrations of MeHg, Total Organic Carbon (TOC), sulfate, and sulfide were measured in porewaters. The mean concentration of MeHg in tissues for all invertebrates sampled was 10.03 ± 7.04 ng g -1 ). MeHg in porewater (mean = 0.22-1.59 ng L -1 ) was the strongest predictor of invertebrate MeHg, but sediment δ 34 S (-0.80-14.1‰) was also a relatively strong predictor. δ 34 S in tissues (measured in three species; Corophium volutator, Ilyanassa obsoleta, and Littorina littorea) were positively related to MeHg in invertebrates (r = 0.55, 0.22, and 0.71 respectively), and when used in combination with δ 15 N and δ 13 C values improved predictions of Hg concentrations in biota. Hg concentrations in the amphipod Corophium volutator (mean MeHg = 10.60 ± 1.90 ng g -1 ) were particularly well predicted using porewater and sediment chemistry, highlighting this species as a useful bioindicator of Hg contamination in sediments of the Bay of Fundy., 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 © 2023 Elsevier Ltd. All rights reserved.)

Daytime volatilization of gaseous elemental mercury (Hg(0) aq ) is a significant mechanism for mercury removal from aquatic systems and potentially limits the production and bioaccumulation of methylmercury. Changes in incoming solar radiation (in the ultraviolet range), dissolved organic matter, salinity, and total suspended particles were investigated concurrently with several mercury species (Hg(0) aq , dissolved total mercury (THg), easily reducible mercury (ERM), and mercury associated with total suspended solids (THg TSS )) during daylight hours near the mouth of a hypertidal river. There were no predictable temporal changes observed for Hg(0) aq in unfiltered surface water. Hg(0) aq ranged from 0 to 12 pg L -1 , THg ranged from 0 to 492 pg L -1 , ERM ranged from 13 to 381 pg L -1 , and THg TSS ranged from <1.58 ng g -1 to 261.32 ng g -1 . The range of Hg(0) aq predicted by the empirical model was similar to measured ERM concentrations, but it was shown that ERM did not significantly predict in-situ photoreducible Hg(II) (Hg(II) RED ). Production of Hg(0) aq appears to largely be suppressed by suspended solids, which limits ultraviolet radiation transmission through surface water. Comparison of these results to an empirical model developed for this site to predict Hg(0) aq indicates that significantly more mercury is available for photoreduction near the mouth of the tidal river, and that Hg(II) will likely photoreduce quickly when TSS levels decrease with ocean mixing., 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 © 2023 Elsevier Ltd. All rights reserved.)

Studies on mercury bioaccumulation and biomagnification in coastal invertebrates in eastern Canada are limited, but these data are necessary to determine risk of mercury exposure effects in upper trophic level organisms. We quantified methylmercury (MeHg), total mercury (THg), and stable isotopes of δ 13 C and δ 15 N in 14 species of invertebrates in the Minas Basin. The overall mean concentration of MeHg (12.78 ± 11.23 ng/g dw) was approximately 10 times below the Canadian guideline for the protection of wildlife consumers like fish and birds of 157.20 ng/g dry weight (dw). Invertebrates at higher trophic positions (δ 15 N) had greater THg and particularly MeHg. The Trophic Magnification Factors (TMF) for MeHg and THg (1.59 and 1.21 respectively) were similar to others reported in studies of food webs containing higher trophic level organisms., 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 © 2023 Elsevier Ltd. All rights reserved.)

Net photoreduction of divalent mercury (Hg(II)) and volatilization of photoreduction products (i.e., elemental mercury (Hg(0))/dissolved gaseous mercury (DGM)) is a mechanism by which mercury burdens in ecosystems are lessened. The effects of salinity on mercury photoreactions were investigated while controlling the concentration of DOM (>1 kDa) using natural surface water from the tidal Jijuktu'kwejk (Cornwallis River) and processed with a tangential ultrafiltration-dilution technique. Pseudo first-order rate constants in estuarine water salinity dilutions ranged between 0.22 h -1 and 0.73 h -1 . The amount of mercury available for photoreduction (Hg(II) RED ) ranged between 67.2 and 265.9 pg. Pseudo first-order rate constants decreased with increasing salinity treatments (0-13.5 g L -1 ), with minimal change in rate constants occurring in higher salinity treatments (e.g. 20.3 or 26.8 g L -1 ), while Hg(II) RED increased with salinity. In lower salinity treatments, DOM was more photoactive. Taken together, results suggest changes in the mercury photoreduction mechanism from DOM-bound electron transfer to photochemically produced secondary reduction products with increasing salinity. Experiments examining photooxidation showed decreases in Hg (0) with longer exposure time, suggesting transformation of Hg(II) RED into a non-reducible form. This research highlights the importance of salinity and DOM interactions in estuarine surface water and their effects on mercury photochemistry., 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 Elsevier Ltd. All rights reserved.)

Due to their natural geochemistry, intertidal estuarine ecosystems are vulnerable to bioaccumulation of methylmercury (MeHg), a neurotoxin that readily bioaccumulates in organisms. Determining MeHg concentrations in intertidal invertebrates at the base of the food web is crucial in determining MeHg exposure in higher trophic level organisms like fish and birds. The processes that govern the production of MeHg in coastal ecosystems are influenced by many geochemical factors including sulfur species, organic matter, and salinity. The interactions of these factors with mercury are complex, and a wide variety of results have been reported in the literature. This paper reviews conceptual models to better clarify the various geochemical and physical factors that impact MeHg production and bioavailability in intertidal ecosystems., (© 2022. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

The biomagnification of toxic methylmercury (MeHg) and selenium (Se) through aquatic food webs using nitrogen stable isotopes (δ 15 N) varies among ecosystems but underlying mechanisms are yet unexplained. Given the strong links between MeHg and thiol-containing amino acids and proteins containing selenocysteine, our hypothesis was that cysteine content is a better predictor of MeHg and Se transfer through lake food webs than δ 15 N. Food web samples were collected from six lakes in Kejimkujik National Park, Nova Scotia, Canada, and the regression slopes of log MeHg or Se versus protein-bound cysteine or bulk δ 15 N were compared. Across all six lakes, MeHg varied by a factor of 10 among taxa and was significantly and positively related to both cysteine (R 2  = 0.65-0.80, p < 0.001) and δ 15 N (R 2  = 0.88-0.94, p < 0.001), with no among-system differences in these slopes. In contrast, total Se concentrations varied by less than a factor of 2 among taxa in four lakes and were significantly related to cysteine in only two food webs (R 2  = 0.20 & 0.37, p = 0.014 & < 0.001); however, δ 15 N was not a predictor of Se in any lake (p = 0.052-0.777). Overall, these novel results indicate that cysteine content predicts MeHg, and sometimes Se, across trophic levels, providing a potential mechanism for among-system differences in their biomagnification., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests. Karen Kidd reports financial support was provided by Natural Sciences and Engineering Research Council of Canada (NSERC) Discovery Program [429389-2012 and 312237-201], the Canada Research Chair program, the Canada Foundation for Innovation, Environment and Climate Change Canada, and the Stephen A. Jarislowsky Chair in Environment & Health. Robin Stewart reports financial support from the U.S. Geological Survey through the Water Mission Area's Water Quality Program. Jennifer Thera reports financial support was provided by the Society of Environmental Toxicology and Chemistry Student Training Exchange., (Copyright © 2022 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Seabirds are important biovectors of contaminants, like mercury, moving them from marine to terrestrial environments around breeding colonies. This transfer of materials can have marked impacts on receiving environments and biota. Less is known about biotransport of contaminants by generalist seabirds that exploit anthropogenic wastes compared to other seabird species. In this study, we measured total mercury (THg) in O-horizon soils at four herring gull (Larus smithsoniansus) breeding colonies in southern Nova Scotia, Canada. At colonies with dry substrate, THg was significantly higher in soils collected from gull colonies compared to nearby reference soils with no nesting gulls. Further, THg was distinct in soils among study colonies and was likely influenced by biotransport from other nesting seabird species, most notably Leach's storm-petrels (Hydrobates leucorhous). Our research suggests gulls that scavenge on anthropogenic wastes at local industrial sites are biovectors moving THg acquired at these sites to their colonies and may increase the spatial footprint of contaminants from these industries., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Forest harvesting affects dissolved organic matter (DOM) and aqueous mercury inputs as well as the food web structure in small-headwater streams, but how these upstream changes manifest downstream is unclear. To address this uncertainty, we examined DOM quality, autochthony in the caddisfly Hydropsychidae (using δ 2 H), and methylmercury (MeHg) concentrations in stream water and the caddisfly along a longitudinal gradient (first- to fourth-order streams, subcatchments of 50-1900 ha) in paired partially harvested and reference catchments in central Ontario, Canada. Although measures of DOM quality (specific ultraviolet absorbance at 254 nm 2.20-11.62) and autochthony in caddisflies (4.9%-34.0%) varied among sites, no upstream-to-downstream differences in these measures were observed between the paired harvested and reference catchments. In contrast, MeHg levels in stream water (0.06-0.35 ng/L) and caddisflies (29.7-192 µg/kg dry wt) were significantly higher in the upstream sites but not the farthest downstream sites in the harvested catchments compared to the reference catchments. This suggests that while current mitigation measures used by forestry companies did not prevent elevated MeHg in water and invertebrates at smaller spatial scales (subcatchments of 50-400 ha), these upstream impacts did not manifest at larger spatial scales (subcatchments of 800-1900 ha). The present study advances our understanding of spatially cumulative impacts within harvested catchments, which is critical to help forest managers maintain healthy forest streams and their provisioning of aquatic ecosystem services. Environ Toxicol Chem 2022;41:1490-1507. © 2022 SETAC., (© 2022 SETAC.)

Quantifying methylmercury (MeHg) concentrations and uptake at the base of the food web is useful for assessing mercury exposure risk to higher trophic level organisms. Higher MeHg concentrations near the base of the food web may result in more MeHg exposure and accumulation in higher trophic organisms. Here, we analyze MeHg in caddisflies, mayflies, lake water, and sediment collected from two temperate lakes and one brook in Kejimkujik National Park, Nova Scotia, Canada. Overall, caddisfly larvae MeHg (15.38-276.96 ng/g; n = 29) was not significantly correlated with water chemistry. Whereas mayfly naiads MeHg (14.28-166.82 ng/g; n = 31) was positively correlated with water MeHg (r s  = 0.43), negatively correlated with pH (r s  = -0.49), and positively correlated with dissolved organic carbon (DOC; r s  = 0.48). Of the mercury in insect tissues, the %MeHg ranged from 56 to 75 % in caddisfly larvae and 38-47 % in mayfly naiads. MeHg bioaccumulation factors (BAF) varied greatly (water to tissue BAFs = 0.145 × 10 6 -1.054 × 10 6 ; sediment to tissue BAFs = 0.017 × 10 6 -0.541 × 10 6 ). This study highlights the importance of quantifying variations in MeHg bioaccumulation and BAFs of common aquatic insect bioindicators at the base of complex food webs., (Crown Copyright © 2021. Published by Elsevier Ltd. All rights reserved.)

Methylmercury (MeHg) is a toxic and bioaccumulative organo-metallic compound that is naturally produced in many ecosystems. Organisms that occupy the lower trophic positions in food webs may be key factors in the assessment of MeHg biomagnification between ecosystems. Here we present a review of the peer-reviewed literature examining MeHg bioaccumulation in freshwater invertebrates, focused principally on insects. This review aims to characterize the invertebrates that bioaccumulate higher MeHg concentrations and therefore pose a higher risk to upper trophic levels and to clarify which ecosystems are more susceptible to bioaccumulation in lower trophic levels. However, we found that few studies provided robust environmental data (notably water chemistry) as part of their papers, dramatically limiting our ability to test for factors that might contribute to different concentrations of MeHg in invertebrates. We highlight the importance of providing physical and chemical characteristics of study sites in publications examining MeHg bioaccumulation and biomagnification. Adopting the proposed recommendations will improve the available information for future mercury risk assessment analyses., (© 2021. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Methylmercury (MeHg) is a global environmental contaminant that poses significant risks to the health of humans, wildlife, and ecosystems. Assessing MeHg exposure in biota across the landscape and over time is vital for monitoring MeHg pollution and gauging the effectiveness of regulations intended to reduce new mercury (Hg) releases. We used MeHg concentrations measured in museum specimen feathers (collected between 1869 and 2014) and total Hg concentrations (as a proxy for MeHg) of feathers sampled from wild birds (collected between 2008 and 2017) to investigate temporal patterns in exposure over approximately 150 years for North American songbirds. For individual species, we found greater concentrations for samples collected post-2000 compared to those collected during historic times (pre-1900) for six of seven songbird species. Mean feather concentrations measured in samples collected post-2000 ranged between 1.9 and 17 times (mean 6.6) greater than historic specimens. The proportion of individual songbirds with feather concentrations that exceeded modeled toxicity benchmarks increased in samples collected after 1940. Only 2% of individual songbirds collected prior to 1940 had feather concentrations greater than 2.4 μg/g (a toxicity benchmark related to a 10% decrease in nest success) compared to 35% of individuals collected post-1940. Many species included in this study have a vulnerable or near-threatened conservation status, suggesting recovery actions are needed to address mercury pollution.

The use of naturally occurring epiphytic lichens can be an effective tool for regional monitoring of mercury (Hg) and other potentially toxic elements (PTEs). Nova Scotia, Canada is a hotspot for mercury and other trace metal accumulation in ecosystems; partially attributed to long-range transport of air pollution. The relative contribution of local and international sources of Hg to local air in Nova Scotia is unknown. This study assessed the potential of epiphytic lichens (Usnea spp.) as passive samplers for PTE air pollution in Nova Scotia. Lichens (n = 190) collected across mainland Nova Scotia were analyzed for PTEs. Results indicate that there are 3 distinct clusters of PTEs which suggest patterns and sources for each elemental cluster. Hg was correlated with longitude and prevailing wind direction, and Hg was not significantly different in site-specific hotspot sampling nor year of sampling. Our data support the hypothesis that Hg in lichens is from historical and ongoing long-range transport and diffuse emission patterns rather than localized pollution sources. PTE concentrations were shown to have median values that are similar to other remote regions (such as the Antarctic) however the maximum values were observed to be substantially higher for some elements (e.g. lead, cadmium). This research supports the use of lichens as biomonitors and provides a baseline for future monitoring efforts to identify changes in PTE distribution in Nova Scotia with ongoing industrial activity and a changing climate., (Crown Copyright © 2019. Published by Elsevier Ltd. All rights reserved.)

Dissolved gaseous mercury (DGM) production was examined in relation to ultraviolet radiation within a marine aquaculture site in the contaminated Marano and Grado Lagoon (Italy). The measured rates of DGM production relative to time elapsed (17.06 and 20.68 pg h -1 , respectively) were substantially (6-20 times) higher than what has been observed in other marine Hg studies. We measured similar levels of DGM relative to dissolved total mercury (THg D ) (0.84%-8.91%) at these sites in comparison to uncontaminated marine sites, however relative to other moderately-contaminated marine sites in Portugal the % DGM/THg D was high. These results suggest a substantial capacity for Hg volatilization from these highly contaminated lagoons to the atmosphere due to photoreduction mechanisms.

Methylmercury (MeHg) is a neurotoxin and endocrine disruptor that bioaccumulates and biomagnifies through trophic levels, resulting in potentially hazardous concentrations. Although wetlands are known hotspots for mercury (Hg) methylation, the effects of avian biovectors on these processes are poorly understood. We examined Hg speciation and distribution in shallow groundwater and surface water from a raised-bog with over 30years of avian biovector (herring gulls Larus argentatus and great black-backed gulls Larus marinus) colonization and guano input. Compared to the reference site, the avian-impacted bog had elevated concentrations of total dissolved organic carbon (TOC), total Hg, MeHg, phosphate (PO 4 3- , MeHg, As and Cd, but not total mercury (THg), and models suggested that Mn, PO 4 3- , MeHg, As and Cd, but not total mercury (THg), and models suggested that Mn, PO 4 3- , and dissolved TOC were strong predictors of MeHg. Our findings suggest that while these gulls may not be a significant source of Hg, the excess of PO 4 3- (a well recognised component of guano) and the subsequent changes in water chemistry due to avian biovector subsidies may increase net Hg methylation., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Mercury (Hg) is a toxic element which has increased in marine environments for more than a century, due largely to anthropogenic activities, and biomagnifies in food chains to harmful levels in some top predators like waterfowl and seabirds. We analysed total mercury (THg) concentrations in blood, brain and muscle tissue from healthy specimens of 13 coastal and pelagic bird species from eastern and northern Canada to provide a baseline on current concentrations, especially for brain concentrations which are highly underrepresented in the literature. We also examined within and among tissues relationships of THg concentrations within individuals. THg concentrations were generally higher in pelagic species and scavenging gulls, when compared to coastal waterfowl. Brain and muscle tissue had similar concentrations of THg in the birds examined, but both of these tissues had lower concentrations that those found in blood. Our results, and that of a previous study, suggest that body condition has a large influence on blood THg concentrations and should be considered when using blood as a sampling medium. Many of the species we examined had tissue THg above levels known to cause deleterious, sublethal effects in some species., (Copyright © 2018 Elsevier Inc. All rights reserved.)

Mercury is a globally distributed, environmental contaminant. Quantifying the retention and loss of mercury is integral for predicting mercury-sensitive ecosystems. There is little information on how dissolved organic carbon (DOC) concentrations and particulates affect mercury photoreaction kinetics in freshwater lakes. To address this knowledge gap, samples were collected from ten lakes in Kejimkujik National Park, Nova Scotia (DOC: 2.6-15.4mg/L). Filtered (0.2μm) and unfiltered samples were analysed for gross photoreduction, gross photooxidation, and net reduction rates of mercury using pseudo first-order curves. Unfiltered samples had higher concentrations (p=0.04) of photoreducible divalent mercury (Hg(II) RED ) (mean of 754±253pg/L) than filtered samples (mean of 482±206pg/L); however, gross photoreduction and photooxidation rate constants were not significantly different in filtered or unfiltered samples in early summer. DOC was not significantly related to gross photoreduction rate constants in filtered (R 2 =0.43; p=0.08) and unfiltered (R 2 =0.02; p=0.71) samples; DOC was also not significantly related to gross photooxidation rate constants in filtered or unfiltered samples. However, DOC was significantly negatively related with Hg(II) RED in unfiltered (R 2 =0.53; p=0.04), but not in filtered samples (R 2 =0.04; p=0.60). These trends indicate that DOC is a factor in determining dissolved mercury photoreduction rates and particles partially control available Hg(II) RED in lake water. This research also demonstrates that within these lakes gross photoreduction and photooxidation processes are close to being in balance. Changes to catchment inputs of particulate matter and DOC may alter mercury retention in these lakes and could partially explain observed increases of mercury accumulation in biota., (Copyright © 2017. Published by Elsevier B.V.)

Although estuaries are critical habitats for many aquatic species, the spatial trends of toxic methylmercury (MeHg) in biota from fresh to marine waters are poorly understood. Our objective was to determine if MeHg concentrations in biota changed along a salinity gradient in an estuary. Fourspine Stickleback (Apeltes quadracus), invertebrates (snails, amphipods, and chironomids), sediments, and water were collected from ten sites along the Saint John River estuary, New Brunswick, Canada in 2015 and 2016, with salinities ranging from 0.06 to 6.96. Total mercury (proxy for MeHg) was measured in whole fish and MeHg was measured in a subset of fish, pooled invertebrates, sediments, and water. Stable sulfur (δ 34 S), carbon (δ 13 C), and nitrogen (δ 15 N) isotope values were measured to assess energy sources (S, C) and relative trophic level (N). There were increases in biotic δ 13 C and δ 34 S from fresh to more saline sites and these measures were correlated with salinity. Though aqueous MeHg was higher at the freshwater than more saline sites, only chironomid MeHg increased significantly with salinity. In the Saint John River estuary, there was little evidence that MeHg and its associated risks increased along a salinity gradient., (Copyright © 2018. Published by Elsevier B.V.)

Intertidal sediments of Tagus estuary regularly experiences complex redistribution due to tidal forcing, which affects the cycling of mercury (Hg) between sediments and the water column. This study quantifies total mercury (Hg) and methylmercury (MMHg) concentrations and fluxes in a flooded mudflat as well as the effects on water-level fluctuations on the air-surface exchange of mercury. A fast increase in dissolved Hg and MMHg concentrations was observed in overlying water in the first 10min of inundation and corresponded to a decrease in pore waters, suggesting a rapid export of Hg and MMHg from sediments to the water column. Estimations of daily advective transport exceeded the predicted diffusive fluxes by 5 orders of magnitude. A fast increase in dissolved gaseous mercury (DGM) concentration was also observed in the first 20-30min of inundation (maximum of 40pg L -1 ). Suspended particulate matter (SPM) concentrations were inversely correlated with DGM concentrations. Dissolved Hg variation suggested that biotic DGM production in pore waters is a significant factor in addition to the photochemical reduction of Hg. Mercury volatilization (ranged from 1.1 to 3.3ngm -2 h -1 ; average of 2.1ngm -2 h -1 ) and DGM production exhibited the same pattern with no significant time-lag suggesting a fast release of the produced DGM. These results indicate that Hg sediment/water exchanges in the physical dominated estuaries can be underestimated when the tidal effect is not considered., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Nitrogen and carbon stable isotopes (δ 15 N, δ 13 C) are commonly used to understand mercury (Hg) bioaccumulation and biomagnification in freshwater food webs. Though sulfur isotopes (δ 34 S) can distinguish between energy sources from the water column (aqueous sulfate) and from sediments to freshwater organisms, little is known about whether δ 34 S can help interpret variable Hg concentrations in aquatic species or food webs. Seven acidic lakes in Kejimkujik National Park (Nova Scotia, Canada) were sampled for biota, water, and sediments in 2009 and 2010. Fishes, zooplankton, and macroinvertebrates were analyzed for δ 34 S, δ 15 N, δ 13 C, and Hg (methyl Hg in invertebrates, total Hg in fishes); aqueous sulfate and profundal sediments were analyzed for δ 34 S. Within lakes, mean δ 34 S values in sediments and sulfate differed between 0.53‰ and 1.98‰, limiting their use as tracers of energy sources to the food webs. However, log-Hg and δ 34 S values were negatively related (slopes -0.14 to -0.35, R 2 0.20-0.39, p < 0.001-0.01) through each food web, and slopes were significantly different among lakes (analysis of covariance, lake × δ 34 S interaction term p = 0.04). Despite these relationships, multiple regression analyses within each taxon showed that biotic Hg concentrations were generally better predicted by δ 15 N and/or δ 13 C. The results indicate that δ 34 S values are predictive of Hg concentrations in these food webs, although the mechanisms underlying these relationships warrant further study. Environ Toxicol Chem 2017;36:661-670. © 2016 SETAC., (© 2016 SETAC.)

Mercury (Hg) is a ubiquitous heavy metal that occurs naturally in the environment, but its levels have been supplemented for decades by a variety of human activities. Mercury can have serious deleterious effects on a variety of organisms, with top predators being particularly susceptible because methylmercury bioaccumulates and biomagnifies in food webs. Among birds, seabirds can have especially high levels of Hg contamination and Leach's storm-petrels (Oceanodroma leucorhoa), in particular, have amongst the highest known levels. Several populations of Leach's storm-petrels have declined recently in the Northwest Atlantic. The causes of these declines remain uncertain, but the toxic effects of Hg could be a potential factor in this decline. Here, we tested for relationships between adult blood total Hg (THg) concentration and several offspring development parameters, and adult return rate of Leach's storm-petrels breeding on Bon Portage Island (43° 28' N, 65° 44' W), Nova Scotia, Canada, between 2011 and 2015 (blood samples n = 20, 36, 6, 15, and 13 for each year, respectively). Overall, THg levels were elevated (0.78 ± 0.43 μg/g wet wt.) compared to other species of seabirds in this region, and varied significantly among years. However, we found no associations between THg levels and reproductive parameters or adult return rate. Our results indicate that levels of mercury observed in Leach's storm-petrel blood, although elevated, appear not to adversely affect their offspring development or adult return rate on Bon Portage Island.

We investigated the impact of managed retreat on mercury (Hg) biogeochemistry at a site subject to diffuse contamination with Hg. We collected sediment cores from an area of land behind a dyke one year before and one year after it was intentionally breached. These sediments were compared to those of an adjacent mudflat and a salt marsh. The concentration of total mercury (THg) in the sediment doubled after the dyke was breached due to the deposition of fresh sediment that had a smaller particle size, and higher pH. The concentration of methylmercury (MeHg) was 27% lower in the sediments after the dyke was breached. We conclude that coastal flooding during managed retreat of coastal flood defences at this site has not increased the risk of Hg methylation or bioavailability during the first year. As the sediment becomes vegetated, increased activity of Hg-methylating bacteria may accelerate Hg-methylation rate., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Aerobic mercury-resistant bacteria were isolated from the sediments of two highly mercury-polluted areas of the Tagus Estuary (Barreiro and Cala do Norte) and one natural reserve area (Alcochete) in order to test their capacity to transform mercury. Bacterial species were identified using 16S rRNA amplification and sequencing techniques and the results indicate the prevalence of Bacillus sp. Resistance patterns to mercurial compounds were established by the determination of minimal inhibitory concentrations. Representative Hg-resistant bacteria were further tested for transformation pathways (reduction, volatilization and methylation) in cultures containing mercury chloride. Bacterial Hg-methylation was carried out by Vibrio fluvialis, Bacillus megaterium and Serratia marcescens that transformed 2-8% of total mercury into methylmercury in 48h. In addition, most of the HgR bacterial isolates showed Hg(2+)-reduction andHg(0)-volatilization resulting 6-50% mercury loss from the culture media. In summary, the results obtained under controlled laboratory conditions indicate that aerobic Hg-resistant bacteria from the Tagus Estuary significantly affect both the methylation and reduction of mercury and may have a dual face by providing a pathway for pollution dispersion while forming methylmercury, which is highly toxic for living organisms., (Copyright © 2015 Elsevier Inc. All rights reserved.)

Mercury (Hg) is an important environmental contaminant, due to its neurotoxicity and ability to bioaccumulate. The Arctic is a mercury-sensitive region, where organisms can accumulate high Hg concentrations. Snowpack mercury photoredox reactions may control how much Hg is transported with melting Arctic snow. This work aimed to (1) determine the significance of temperature combined with UV irradiation intensity and snow age on Hg(0) flux from Arctic snow and (2) elucidate the effect of temperature on snowpack Hg photoreduction kinetics. Using a Teflon flux chamber, snow temperature, UV irradiation, and snow age were found to significantly influence Hg(0) flux from Arctic snow. Cross-correlation analysis results suggest that UV radiation has a direct effect on Hg(0)flux, while temperature may indirectly influence flux. Laboratory experiments determined that temperature influenced Hg photoreduction kinetics when snow approached the melting point (>-2 °C), where the pseudo-first-order reduction rate constant, k, decreased twofold, and the photoreduced Hg amount, Hg(II)red, increased 10-fold. This suggests that temperature influences Hg photoreduction kinetics indirectly, likely by altering the solid:liquid water ratio. These results imply that large mass transfers of Hg from snow to air may take place during the Arctic snowmelt period, altering photoreducible Hg retention and transport with snow meltwater.

Mercury (Hg) concentrations are a concern in the Canadian Arctic, because they are relatively high compared to background levels and to similar species farther south, and are increasing in many wildlife species. Among marine birds breeding in the Canadian Arctic, Hg concentrations have been monitored regularly in eggs and intermittently in livers, but feathers have generally not been used as an indicator of Hg exposure or burden. We examined Hg concentrations in six marine bird species in the Canadian Arctic. Ivory gull Pagophila eburnea, feather Hg was exceptionally high, while glaucous gull Larus hyperboreus feather Hg was unexpectedly low, and ratios of feather THg to egg THg varied across species. The proportion of total Hg that was comprised of methyl Hg in ivory gull feathers was lower than in other species, and may be related to photo-demethylation or keratin breakdown in semi-opaque feather tissue., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Recurring polynyas are important areas of biological productivity and feeding grounds for seabirds and mammals in the Arctic marine environment. In this study, we examined food web structure (using carbon and nitrogen isotopes, δ(13)C and δ(15)N) and mercury (Hg) bioaccumulation and biomagnification in a small recurring polynya ecosystem near Nasaruvaalik Island (Nunavut, Canada). Methyl Hg (MeHg) concentrations increased by more than 50-fold from copepods (Calanus hyperboreus) to Arctic terns (Sterna paradisaea), the abundant predators at this site. The biomagnification of MeHg through members of the food web - using the slope of log MeHg versus δ(15)N - was 0.157 from copepods (C. hyperboreus) to fish. This slope was higher (0.267) when seabird chicks were included in the analyses. Collectively, our results indicate that MeHg biomagnification is occurring in this small polynya and that its trophic transfer is at the lower end of the range of estimates from other Arctic marine ecosystems. In addition, we measured Hg concentrations in some poorly studied members of Arctic marine food webs [e.g. Arctic alligatorfish (Ulcina olrikii) and jellyfish, Medusozoa], and found that MeHg concentrations in jellyfish were lower than expected given their trophic position. Overall, these findings provide fundamental information about food web structure and mercury contamination in a small Arctic polynya, which will inform future research in such ecosystems and provide a baseline against which to assess changes over time resulting from environmental disturbance., (Copyright © 2014 Elsevier B.V. All rights reserved.)

In temperate regions of Canada, mercury (Hg) concentrations in biota and the magnitude of Hg biomagnification through food webs vary between neighboring lakes and are related to water chemistry variables and physical lake features. However, few studies have examined factors affecting the variable Hg concentrations in landlocked Arctic char (Salvelinus alpinus) or the biomagnification of Hg through their food webs. We estimated the food web structure of six high Arctic lakes near Resolute Bay, Nunavut, Canada, using stable carbon (δ(13)C) and nitrogen (δ(15)N) isotopes and measured Hg (total Hg (THg) in char, the only fish species, and methylmercury (MeHg) in chironomids and zooplankton) concentrations in biota collected in 2010 and 2011. Across lakes, δ(13)C showed that benthic carbon (chironomids) was the dominant food source for char. Regression models of log Hg versus δ(15)N (of char and benthic invertebrates) showed positive and significant slopes, indicting Hg biomagnification in all lakes, and higher slopes in some lakes than others. However, no principal components (PC) generated using all water chemistry data and physical characteristics of the lakes predicted the different slopes. The PC dominated by aqueous ions was a negative predictor of MeHg concentrations in chironomids, suggesting that water chemistry affects Hg bioavailability and MeHg concentrations in these lower-trophic-level organisms. Furthermore, regression intercepts were predicted by the PCs dominated by catchment area, aqueous ions, and MeHg. Weaker relationships were also found between THg in small char or MeHg in pelagic invertebrates and the PCs dominated by catchment area, and aqueous nitrate and MeHg. Results from these high Arctic lakes suggest that Hg biomagnification differs between systems and that their physical and chemical characteristics affect Hg concentrations in lower-trophic-level biota., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Soils are a source of elemental mercury (Hg(0)) to the atmosphere, however the effects of soil temperature and moisture on Hg(0) formation is not well defined. This research quantifies the effect of varying soil temperature (278-303 K), moisture (15-80% water filled pore space (WFPS)) and sterilization on the kinetics of Hg(0) formation in forested soils of Nova Scotia, Canada. Both, the logarithm of cumulative mass of Hg(0) formed in soils and the reduction rate constants (k values) increased with temperature and moisture respectively. Sterilizing soils significantly (p < 0.05, n = 10) decreased the percent of total Hg reduced to Hg(0). We describe the fundamentals of Hg(0) formation in soils and our results highlight two key processes: (i) a fast abiotic process that peaks at 45% WFPS and depletes a small pool of Hg(0) and; (ii) a slower, rate limiting biotic process that generates a large pool of reducible Hg(II)., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Dragonflies (Odonata: Anisoptera) are an important component of both aquatic and terrestrial food webs and are vectors for methylmercury (MeHg) biomagnification. Variations in mercury content with life stage and body regions may affect the relative transfer of mercury to aquatic or terrestrial food webs; however, there has been little research on this subject. Also, little is known about mercury bioaccumulation in different body regions of dragonflies. To address these knowledge gaps, dragonfly naiads, adults, and exuviae were collected at 2 lakes in Kejimkujik National Park, Nova Scotia, Canada, and mercury concentrations in different life stages and body regions were quantified. Mean whole body concentrations of MeHg were substantial in naiads (232 ± 112 ng g(-1) dry wt, n = 66), emerging adults (236 ± 50 ng g(-1) dry wt, n = 10), and mature adults (231 ± 74 ng g(-1) dry wt, n = 20). Mean MeHg concentrations in exuviae (5.6 ± 4.3 ng g(-1), n = 32) were 40-fold lower than in naiads and adults. Emerging adults had 2-fold to 2.5-fold higher Hg(II) concentrations than naiads, mature adults, and exuviae. In body regions of both naiads and adults, some abdomens contained significantly higher concentrations of Hg(II) than heads or thoraces, and this trend was consistent across families. Across families, Aeshnidae had significantly higher concentrations of MeHg and total Hg than Gomphidae and Libellulidae, but not higher than Cordulidae. The Hg(II) concentrations were lower in Aeshnidae and Libellulidae than in Gomphidae and Cordulidae. Shedding of exuviae presents a possible mechanism for mercury detoxification, but mercury concentrations and burdens in exuviae are low in comparison with naiads and adults. Dragonfly adults retain a high potential for transferring substantial amounts of MeHg to their predators., (© 2014 SETAC.)

This study examines mercury exposure in bats across the northeast U.S. from 2005 to 2009. We collected 1,481 fur and 681 blood samples from 8 states and analyzed them for total Hg. A subset (n = 20) are also analyzed for methylmercury (MeHg). Ten species of bats from the northeast U.S. are represented in this study of which two are protected by the Endangered Species Act (ESA 1973) and two other species are pending review. There are four objectives in this paper: (1) to examine correlates to differences in fur-Hg levels among all of the sampling sites, including age, sex, species, and presence of a Hg point source; (2) define the relationship between blood and fur-Hg levels and the factors that influence that relationship including age, sex, species, reproductive status, and energetic condition; (3) determine the relationships between total Hg and MeHg in five common eastern bat species; and (4) assess the distribution of Hg across bat populations in the northeast. We found total blood and fur mercury was eight times higher in bats captured near point sources compared to nonpoint sources. Blood-Hg and fur-Hg were well correlated with females on average accumulating two times more Hg in fur than males. On average fur MeHg accounted for 86 % (range 71-95 %) of the total Hg in bat fur. Considering that females had high Hg concentrations, beyond that of established levels of concern, suggests there could be negative implications for bat populations from high Hg exposure since Hg is readily transferred to pups via breast milk. Bats provide an integral part of the ecosystem and their protection is considered to be of high priority. More research is needed to determine if Hg is a stressor that is negatively impacting bat populations.

The polychaete worm Nereis diversicolor engineers its environment by creating oxygenated burrows in anoxic intertidal sediments. The authors carried out a laboratory microcosm experiment to test the impact of polychaete burrowing and feeding activity on the lability and methylation of mercury in sediments from the Bay of Fundy, Canada. The concentration of labile inorganic mercury and methylmercury in burrow walls was elevated compared to worm-free sediments. Mucus secretions and organic detritus in worm burrows increased labile mercury concentrations. Worms decreased sulfide concentrations, which increased Hg bioavailability to sulfate-reducing bacteria and increased methylmercury concentrations in burrow linings. Because the walls of polychaete burrows have a greater interaction with organisms, and the overlying water, the concentrations of mercury and methylmercury they contain is more toxicologically relevant to the base of a coastal food web than bulk samples. The authors recommend that researchers examining Hg in marine environments account for sediment dwelling invertebrate activity to more fully assess mercury bioavailability., (Copyright © 2013 SETAC.)

Polychaete worms are abundant in many mudflats but their importance to coastal food web Hg biomagnification is not known. We sampled sediments and polychaete worms from mudflats in the Bay of Fundy to investigate the bioaccumulation of mercury (Hg) and methylmercury (MeHg) in the coastal invertebrate food web. Hg concentrations in the sediments were low (<20 μg kg(-1)). Labile Hg (methanol/KOH sediment extraction) in surface sediments (0-1 cm) was positively correlated with Hg bioaccumulation by surface sediment-ingesting polychaetes but, surprisingly, there was a negative correlation between δ(15)N (i.e. trophic level) and THg bioaccumulation factors in polychaete worms. Worms feeding on deeper sediments contained the greatest MeHg concentrations (69.6 μg kg(-1)). Polychaetes are an important vector for Hg biomagnification to the coastal avian food web. This research demonstrates that feeding depth and method of feeding are more important than trophic position or sediment Hg concentrations for predicting Hg bioaccumulation., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Mercury (Hg) contamination in aquatic systems remains a global concern because the organic form, methyl Hg (MeHg), can biomagnify to harmful concentrations in fish, fish-eating wildlife, and humans. Food web transfer of MeHg has been explored using models of log MeHg versus relative trophic position (nitrogen isotopes, δ(15)N), but regression slopes vary across systems for unknown reasons. In this study, MeHg biomagnification was determined for 11 lake food webs in Kejimkujik National Park, Nova Scotia, Canada, and compared to physical and chemical lake characteristics using principal component and multiple regression analyses. MeHg biomagnification (regression slopes of log MeHg versus baseline-adjusted δ(15)N for fishes and invertebrates) varied significantly across lakes and was higher in systems with lower aqueous nutrient/MeHg/chloride scores. This is one of the largest, consistent data sets available on MeHg biomagnification through temperate lake food webs and the first study to use a principal component and multiple regression approach to understand how lake chemical and physical characteristics interact to affect biomagnification among systems. Overall, our results show that the magnitude of MeHg biomagnification through lake food webs is related to the chemical and physical characteristics of the systems, but the underlying mechanisms warrant further investigation.

Uncertainties in projected ultraviolet (UV) radiation may lead to future increases in UV irradiation of freshwater lakes. Because dissolved organic carbon (DOC) is the main binding phase for mercury (Hg) in freshwater lakes, an increase in DOC photo-oxidation may affect Hg speciation and bioavailability. We quantified the effect of DOC concentration on the rate of abiotic DOC photo-oxidation for five lakes (DOC=3.27-12.3 mg L(-1)) in Kejimkujik National Park, Canada. Samples were irradiated with UV-A or UV-B radiation over a 72-h period. UV-B radiation was found to be 2.36 times more efficient at photo-oxidizing DOC than UV-A, with energy-normalized rates of dissolved inorganic carbon (DIC) production ranging from 3.8×10(-5) to 1.1×10(-4) mg L(-1)J(-1) for UV-A, and from 6.0×10(-5) to 3.1×10(-4) mg L(-1)J(-1) for UV-B. Energy normalized rates of DIC production were positively correlated with DOC concentrations. Diffuse integrated attenuation coefficients were quantified in situ (UV-A K(d)=0.056-0.180 J cm(-1); UV-B K(d)=0.015-0.165 J cm(-1)) and a quantitative depth-integrated model for yearly DIC photo-production in each lake was developed. The model predicts that, UV-A produces between 3.2 and 100 times more DIC (1521-2851 mg m(-2) year(-1)) than UV-B radiation (29.17-746.7 mg m(-2) year(-1)). Future increases in UV radiation may increase DIC production and increase Hg bioavailability in low DOC lakes to a greater extent than in high DOC lakes., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

We present pseudofirst order rate constants for gross photoreduction and gross photooxidation of mercury in surface water from the open Atlantic Ocean, determined under controlled laboratory conditions. Experiments using both unfiltered and filtered ocean water were carried out to characterize the importance of microbes and colloids on reaction kinetics. Results indicate that reduction and oxidation of mercury in ocean water does not follow a simple two-species reversible reaction pathway. We suggest two possible redox pathways that reproduce the pattern of dissolved gaseous mercury (DGM) concentrations observed in our laboratory experiments, and evaluate them using a controlled outdoor experiment. In both proposed pathways Hg(0), the major constituent of DGM, is converted to an unidentified oxidized species that is different from the reducible form present initially. This reaction step plays a major role in the net formation of DGM in our experiments. Our results represent new quantitative information about the gross reaction kinetics for both reduction and oxidation of mercury in open ocean surface water. Pseudofirst order rate constants for reduction reactions that form DGM were determined to be in the range of 0.15-0.93 h(-1) and pseudofirst order rate constants for oxidation of Hg(0) to be in the range of 0.4-1.9 h(-1). Microbes and colloids did not appreciably influence the reduction and oxidation kinetics.

Diurnal patterns for dissolved gaseous mercury (DGM) concentration, mercury flux, several water variables (pH, oxidation reduction potential (ORP), water temperature), and meteorological variables (wind speed, air temperature, % relative humidity, solar radiation) were measured in two lakes with contrasting dissolved organic carbon (DOC) concentrations in Kejimkujik Park, Nova Scotia. A continuous analysis system made it possible to measure quick changes in DGM over time. Consistently higher DGM concentrations were found in the high DOC lake as compared to the low DOC lake. An examination of current mercury flux models using this quantitative data indicated some good correlations between the date and predicted flux (r ranging from 0.27 to 0.83) but generally poor fit (standard deviation of residuals ranging from 0.97 to 3.39). Cross-correlation analysis indicated that DGM dynamics changed in response to solar radiation with lag-times of 65 and 90 min. This relationship with solar radiation was used to develop new predictive models of DGM and mercury flux dynamics for each lake. We suggest that a generalized approach using time-shifted solar radiation date to predict DGM can be incorporated into existing mercury flux models. It is clear from the work presented that DOC and wind speed may also play important roles in DGM and mercury flux dynamics, and these roles have not been adequately accounted for in current predictive models.

The evasion of elemental mercury represents a significant pathway for reducing the level of this potentially toxic material in aquatic ecosystems. The evasion rate is controlled by the concentration of dissolved gaseous mercury (DGM) across the air-water interface, water, and air temperature as well as wind speed. Here we investigate the role of microbial mercury oxidation and reduction in regulating DGM diel patterns in two freshwater lakes, Jack's Lake and Lake Ontario. Three replicate diurnal cycles of DGM in Brookes Bay, Jack's Lake peaked at 313 fM between 9:00 to 10:30 and decreased to 79.6 fM by 16:00. Microbial mercury reductase activity (converts Hg2+ to Hg0) increased with DGM concentrations and mercury oxidase activity (converts Hg0 to Hg2+) increased as DGM concentrations decreased in the mid-afternoon. This illustrates that mercury oxidase activity was linked to hydrogen peroxide (H2O2) diurnal patterns. Thirty minutes after spiking Lake Ontario water with H2O2, mercury oxidase activity increased by 250% and by 60 min, DGM decreased to 28% of its initial value. Two hours after the H2O2 spike, mercury oxidase activity had declined, but mercury reductase activity and DGM both increased. Four hours after the spike, mercury reductase and DGM levels had returned to original levels. Our results are consistent with the following sequence of events. In the morning, microbial activity produces DGM (in addition to any DGM formed through photoreduction of Hg2+). As photochemically produced H2O2 increases in concentration it induces the biologically mediated decrease in DGM concentrations throughout the afternoon. To predict concentration of DGM in surface waters and flux rates to the atmosphere, the contribution of photoreduction and photooxidation must be placed in context with reduction and oxidation rates due to microbial activity.

A survey of the comparative cytological effects of growth in the presence of mercury by a group of mercury-resistant bacterial cultures and a characterization of the process of bacterial adaptation to Hg2+ ion was accomplished. Mercury resistance was found to be dependent upon the ability to volatilize mercury from the medium and upon the amount of mercury accumulated by the cells. The results indicate that most cultures which adapt to growth in the presence of HgCl2 exhibit extensive morphological abnormalities. Significant effects are delay in the onset of growth and cell division and numerous structural irregularities associated with cell wall and cytoplasmic membrane synthesis and function. A detailed analysis of the adaptation process and the resulting effects on morphology was performed on an Enterobacter sp. During the period preceding active multiplication, a selection for mercury-resistant mutants occurred. It was also demonstrated that growth commenced only at a specific threshold concentration of HG2+.

An investigation of mercury-resistant bacteria was undertaken to determine their role in the accumulation of mercury in a simplified food chain. Oysters (Crassostrea virginica) were maintained in a closed system, sealed aquarium with stirred, aerated water containing 10 mug of 203-HgCl2 per liter. Uptake of 203-Hg by oysters held under control conditions was compared with that of 203-Hg uptake by oysters under similar conditions except that mercury-accumulating and mercury-metabolizing species of Pseudomonas, isolated from Chesapeake Bay, were added to the experimental oysters. After incubation for 4 days, the major portion ofthe 203-Hg in the water column was found to be associated with the microparticulate fraction, corresponding to a rise in total viable count. Mercury accumulation in the oysters was significantly higher in the gill and visceral tissue than other tissue. Mercury concentrations were 200 times greater in tissue fractions of oysters dosed with mercury-metabolizing bacteria compared with the oysters held under control conditions without mercury-metabolizing bacteria.

Selected cultures of mercury-resistant bacteria degrade the fungicide-slimicide phenylmercuric acetate. By means of a closed system incorporating a flameless atomic absorption spectrophotometer and a vapor phase chromatograph, it was demonstrated that elemental mercury vapor and benzene were products of phenylmercuric acetate degradation.

Methyl mercury (MeHg) bioaccumulation in lower-trophic-level organisms and its subsequent biomagnification through food webs differs in magnitude among lakes and results in intraspecific variability of MeHg in top predator fishes. Understanding these differences is critical given the reproductive and neurotoxic effects of MeHg on fishes and their predators, including humans. In this study we characterized the food webs of five lakes in New Brunswick, Canada, supporting Brook Trout (Salvelinus fontinalis) using measures of relative trophic position (δ15N) and carbon sources (δ13C), determined the concentrations of MeHg in invertebrates and total Hg (THg) in fishes, and quantified MeHg biomagnification from primary to tertiary consumers. Methyl Hg and THg concentrations were highest in biota from lakes with lower pH. The trophic magnification slopes (TMS; log Hg versus δ15N) varied significantly among lakes (0.12-0.20; ANCOVA, p=0.031). When combined with data from other salmonid lakes in temperate and Arctic Canada (n=36), among-system variability in TMS was best, but weakly, positively predicted by aqueous total phosphorous (p = 0.028, R2adj = 0.109). These results suggest that lake productivity directly or indirectly influences the biomagnification of MeHg through diverse food webs supporting salmonids.