Legacy coal mining impacts downstream ecosystems for decades in the Canadian Rockies.

Mountaintop removal coal mining leaves a legacy of disturbed landscapes and abandoned infrastructure with clear impacts on water resources; however, the intensity and persistence of this water pollution remains poorly characterized. Here we examined the downstream impacts of over a century of coal mining in the Crowsnest Pass (Alberta, Canada). Water samples were collected downstream of two historical coal mines: Tent Mountain and Grassy Mountain. Tent Mountain hosts a partially reclaimed surface mine that closed in 1983. Selenium concentrations downstream of Tent Mountain reached 185 µg/L in a lake below the mine spoil pile, and up to 23 µg/L in Crowsnest Creek, which drains the lake and the mine property. Further downstream, a well-dated sediment core from Crowsnest Lake records increases in sediment, selenium, lead, carbon, nitrogen, and polycyclic aromatic compounds that closely tracked the history of mining at Tent Mountain. In contrast, episodic discharge of mine water from abandoned underground adits at Grassy Mountain drive periodic (but short-term) increases in iron, various metals, and suspended sediment. These results underscore the lasting downstream impacts of abandoned and even reclaimed coal mines.

Tracking historical sources of polycyclic aromatic compounds (PACs) in dated lake sediment cores near in-situ bitumen operations of Cold Lake, Alberta.

Most bitumen in the Alberta oil sands (Canada) is extracted by thermal in-situ recovery. Despite the widespread use of in-situ bitumen extraction, little information is available on the release of petroleum hydrocarbons by this method to adjacent land and water. Here we analyzed the composition and abundance of parent and alkylated polycyclic aromatic compounds (PACs) in 11 radiometrically-dated lake sediment cores collected near in-situ operations at Cold Lake Alberta to assess potential petroleum contamination sources to surrounding lakes over the past century. Like open-pit mining areas, alkylated PACs in Cold Lake sediments were elevated compared to unsubstituted parent PACs and increased coeval with the onset of bitumen extraction in the area. Diagnostic ratios and pyrogenic indices showed that PAC sources to these lake sediments were dominantly pyrogenic, likely from historic forest fires, however they shifted to more petrogenic sources coeval with expanding oil sands extraction at Cold Lake. PACs in sediment from regional lakes are weakly correlated to their proximity to in-situ oil wells, once corrected for lake area. These results suggest that in-situ operations, via diesel-fueled vehicular emissions and the combustion of natural gas for steam generation, are a source of PACs to nearby lakes, but PACs did not exceed Canadian sediment quality guidelines for the protection of aquatic life.

Quantification of Spatial and Temporal Trends in Atmospheric Mercury Deposition across Canada over the Past 30 Years.

Mercury (Hg) is a pollutant of concern across Canada and transboundary anthropogenic Hg sources presently account for over 95% of national anthropogenic Hg deposition. This study applies novel statistical analyses of 82 high-resolution dated lake sediment cores collected from 19 regions across Canada, including nearby point sources and in remote regions and spanning a full west-east geographical range of ∼4900 km (south of 60°N and between 132 and 64°W) to quantify the recent (1990-2018) spatial and temporal trends in anthropogenic atmospheric Hg deposition. Temporal trend analysis shows significant synchronous decreasing trends in post-1990 anthropogenic Hg fluxes in western Canada in contrast to increasing trends in the east, with spatial patterns largely driven by longitude and proximity to known point source(s). Recent sediment-derived Hg fluxes agreed well with the available wet deposition monitoring. Sediment-derived atmospheric Hg deposition rates also compared well to the modeled values derived from the Hg model, when lake sites located nearby (<100 km) point sources were omitted due to difficulties in comparison between the sediment-derived and modeled values at deposition "hot spots". This highlights the applicability of multi-core approaches to quantify spatio-temporal changes in Hg deposition over broad geographic ranges and assess the effectiveness of regional and global Hg emission reductions to address global Hg pollution concerns.

Diet influences on growth and mercury concentrations of two salmonid species from lakes in the eastern Canadian Arctic.

Diet, age, and growth rate influences on fish mercury concentrations were investigated for Arctic char (Salvelinus alpinus) and brook trout (Salvelinus fontinalis) in lakes of the eastern Canadian Arctic. We hypothesized that faster-growing fish have lower mercury concentrations because of growth dilution, a process whereby more efficient growth dilutes a fish's mercury burden. Using datasets of 57 brook trout and 133 Arctic char, linear regression modelling showed fish age and diet indices were the dominant explanatory variables of muscle mercury concentrations for both species. Faster-growing fish (based on length-at-age) fed at a higher trophic position, and as a result, their mercury concentrations were not lower than slower-growing fish. Muscle RNA/DNA ratios were used as a physiological indicator of short-term growth rate (days to weeks). Slower growth of Arctic char, inferred from RNA/DNA ratios, was found in winter versus summer and in polar desert versus tundra lakes, but RNA/DNA ratio was (at best) a weak predictor of fish mercury concentration. Net effects of diet and age on mercury concentration were greater than any potential offset by biomass dilution in faster-growing fish. In these resource-poor Arctic lakes, faster growth was associated with feeding at a higher trophic position, likely due to greater caloric (and mercury) intake, rather than growth efficiency.

Effects of Non-native Fish on Lacustrine Food Web Structure and Mercury Biomagnification along a Dissolved Organic Carbon Gradient.

Although the introduction of non-native fish species has been shown to alter trophic ecology in aquatic ecosystems, there has been limited research on how invasive species alter methylmercury (MeHg) biomagnification in lacustrine food webs. We sampled surface water and biota from 8 lakes in Quebec, Canada, spanning a range of dissolved organic carbon (DOC) concentrations (2.9-8.4 mg/L); 4 lakes were inhabited by native brook trout (Salvelinus fontinalis), and the remaining lakes contained brook trout and a non-native fish, Allegheny pearl dace (Margariscus margarita). Periphyton, zooplankton, macroinvertebrates, and fish were analyzed for: 1) stable carbon (δ13 C) and nitrogen (δ15 N) isotope ratios to delineate food webs, and 2) total Hg (THg) or MeHg. Compared with the brook trout from reference lakes, fish from invaded lakes had higher length-standardized THg concentrations as well as a narrower dietary range and elevated trophic level, inferred from unadjusted δ13 C and δ15 N values, respectively. The rate of Hg biomagnification was similar across invaded and reference lakes, implying little effect of the invasive fish on the trophic transfer of MeHg. Despite differences in food web structure due to pearl dace invasion, DOC was the strongest predictor of brook trout THg levels for all lakes, suggesting that underlying environmental factors exerted a stronger influence on brook trout THg concentrations than the presence of a non-native forage fish. Environ Toxicol Chem 2020;39:2196-2207. © 2020 SETAC.

Mercury methylation and demethylation potentials in Arctic lake sediments.

Mercury (Hg) transformations in sediments are key factors in the Hg exposure pathway for wildlife and humans yet are poorly characterized in Arctic lakes. As the Arctic is rapidly warming, it is important to understand how the rates of Hg methylation and demethylation (wich determine Hg bioavailability) change with temperature in lake sediments. Methylation and demethylation potentials were determined for littoral sediments (2.5 m water depth) in two deep and two shallow lakes in the Canadian Arctic using Hg stable isotope tracers at incubation temperatures of 4, 8, or 16 °C for 24 h. Compared to sediments from other regions, Hg methylation and demethylation potentials in these sediments are low. The maximum depth of the lake from which sediment was collected exerted a stronger influence over methylation potential than sediment Hg concentration or organic matter content; the shallowest lake had the highest Hg methylation potential. Sediments from the shallowest lake also demonstrated the greatest response to the temperature treatments, with significantly higher methylation potentials in the 8 and 16 °C treatments. Sediments from the deep lakes demonstrated greater demethylation potentials than shallow lakes. The methylmercury to total Hg ratio in sediments supported the measured transformation potentials as the lake with the greatest methylation potential had the highest ratio. This study supports previous works indicating that Hg methylation potential may increase as the Arctic warms, but demethylation potential does not respond to warming to the same degree, indicating that Hg methylation may predominate in warming Arctic sediments.

Temporal trends, lake-to-lake variation, and climate effects on Arctic char (Salvelinus alpinus) mercury concentrations from six High Arctic lakes in Nunavut, Canada.

Climate warming and mercury (Hg) are concurrently influencing Arctic ecosystems, altering their functioning and threatening food security. Non-anadromous Arctic char (Salvelinus alpinus) in small lakes were used to biomonitor these two anthropogenic stressors, because this iconic Arctic species is a long-lived top predator in relatively simple food webs, and yet population characteristics vary greatly, reflecting differences between lake systems. Mercury concentrations in six landlocked Arctic char populations on Cornwallis Island, Nunavut have been monitored as early as 1989, providing a novel dataset to examine differences in muscle [Hg] among char populations, temporal trends, and the relationship between climate patterns and Arctic char [Hg]. We found significant lake-to-lake differences in length-adjusted Arctic char muscle [Hg], which varied by up to 9-fold. Arctic char muscle [Hg] was significantly correlated to dissolved and particulate organic carbon concentrations in water; neither watershed area or vegetation cover explained differences. Three lakes exhibited significant temporal declines in length-adjusted [Hg] in Arctic char; the other three lakes had no significant trends. Though precipitation, temperature, wind speed, and sea ice duration were tested, no single climate variable was significantly correlated to length-adjusted [Hg] across populations. However, Arctic char Hg in Resolute Lake exhibited a significant correlation with sea ice duration, which is likely closely linked to lake ice duration, and which may impact Hg processing in lakes. Additionally, Arctic char [Hg] in Amituk Lake was significantly correlated to snow fall, which may be linked to Hg deposition. The lack of consistent temporal trends in neighboring char populations indicates that currently, within lake processes are the strongest drivers of [Hg] in char in the study lakes and potentially in other Arctic lakes, and that the influence of climate change will likely vary from lake to lake.

A comparison of factors affecting the small-scale distribution of mercury from artisanal small-scale gold mining in a Zimbabwean stream system.

Artisanal small-scale gold mining (ASGM) operations use mercury liberally in the gold extraction process and account for approximately one quarter of the anthropogenic mercury consumption worldwide. ASGM activities are concentrated in many impoverished and poorly regulated countries such as Zimbabwe, resulting in a number of negative impacts to health and the environment. To examine levels of mercury contamination in one such geographic locality, sediment and tailing samples were collected in a heavily mined watershed in southern Zimbabwe from May-June 2015. Samples were collected from multiple points within the stream system, as well as from around six stamp mills and a single industrial mine in the watershed. GPS point location data were taken for mining operations and sampling sites to examine the spatial patterns of mercury concentration. Data were first analyzed using linear regression and development of a MARS model, followed by application of an ANCOVA model to assess the relationship among mercury concentrations and percent organic material, distance downstream, and distance from potential contamination source. Mercury concentrations within the study area ranged from 6 to 1541 µg/kg dw (mean 142 µg/kg dw). Analyses of mercury concentrations indicated a positive relationship with percent organic material but a negative relationship with distance downstream and distance from potential contamination source. Results from this study help elucidate the relationship between gold production and the spatial scale of mercury contamination in aquatic ecosystems in Africa. These data may lead to a better understanding of the relationship between mercury use and community health, which may aid both the local and global communities in regulating mercury contamination of the environment.

Screening-level risk assessment of methylmercury for non-anadromous Arctic char (Salvelinus alpinus).

Non-anadromous forms of Arctic char (Salvelinus alpinus), those that are restricted to lakes and rivers, typically have higher mercury (Hg) concentrations than anadromous forms, which migrate to and from the sea. Using tissue burden data from the literature and our own analyses, we performed a screening-level risk assessment of methylmercury (MeHg) for non-anadromous Arctic char. Our assessment included 1569 fish distributed across 83 sites. Site-specific mean total Hg concentrations in non-anadromous Arctic char muscle varied considerably from 0.01 to 1.13 µg/g wet weight, with 21% (17 of 83 sites) meeting or exceeding a threshold-effect level in fish of 0.33 µg/g wet weight, and 13% (11 of 83 sites) meeting or exceeding a threshold-effect level in fish of 0.5 µg/g wet weight. Of the sites in exceedance of the 0.33-µg/g threshold, 7 were located in Greenland and 10 in Canada (Labrador, Nunavut, and Yukon). All but one of these sites were located in interfrost or permafrost biomes. Maximum total Hg concentrations exceeded 0.33 µg/g wet weight at 53% of sites (40 of the 75 sites with available maximum Hg values), and exceeded 0.5 µg/g wet weight at 27% (20 of 75 sites). Collectively, these results indicate that certain populations of non-anadromous Arctic char located mainly in interfrost and permafrost regions may be at risk for MeHg toxicity. This approach provides a simple statistical assessment of MeHg risk to non-anadromous Arctic char, and does not indicate actual effects. We highlight the need for studies that evaluate the potential toxic effects of MeHg in non-anadromous Arctic char, as well as those that aid in the development of a MeHg toxic-effect threshold specific to this species of fish. Environ Toxicol Chem 2019;38:489-502. © 2018 SETAC.

Subcellular distributions of trace elements (Cd, Pb, As, Hg, Se) in the livers of Alaskan yelloweye rockfish (Sebastes ruberrimus).

Yelloweye rockfish (Sebastes ruberrimus) is an extremely long-lived species (up to ∼120 years) of fish, which inhabits the coastal waters of Alaska. Due to their long lifespans, yelloweye are known to accumulate high levels of mercury, and potentially other trace elements, in their tissues. Relatively little is known about the subcellular distribution of trace elements in the tissues of yelloweye rockfish; such information can provide important insights into detoxification/toxicity mechanisms at the subcellular level. To address this, we collected yelloweye rockfish (n = 8) from the eastern coast of Prince of Wales Island, Alaska in 2014. We determined the subcellular partitioning of trace elements (cadmium (Cd), lead (Pb), arsenic (As), total mercury (Hg), and selenium (Se)) in yelloweye livers with a partitioning procedure designed to separate liver cells into putative metal-sensitive fractions (cytosolic enzymes, organelles) and detoxified metal fractions (metallothionein or metallothionein-like proteins and peptides, granule-like structures) using differential centrifugation, NaOH digestion, and heat denaturation steps. The resulting fractions were then analyzed for total Hg with a direct Hg analyzer and for trace element concentrations by inductively coupled plasma-mass spectrometry (ICP-MS). For Cd, Pb, and As, the greatest contributions were found in the detoxified fractions, whereas the majority of total Hg was found in sensitive fractions. Selenium, an essential trace element, was distributed to a similar degree between the sensitive and detoxified compartments. Results indicate that although yelloweye sequestered and immobilized potentially toxic elements in detoxified fractions, the extent of binding differed among elements and followed the order: Cd > As > Pb > Hg. In yelloweye rockfish livers, the accumulation of non-essential elements at sensitive sites could lead to deleterious effects at the subcellular level, which should be evaluated in future studies.

Climate, Fire, and Vegetation Mediate Mercury Delivery to Midlatitude Lakes over the Holocene.

The rise in mercury concentrations in lake sediment deposited over the last ∼150 years is widely recognized to have resulted from human activity. However, few studies in the Great Lakes region have used lake sediment to reconstruct atmospheric mercury deposition on millennial time scales. Here we present a 9000-year mercury record from sediment in Copper Falls; a small closed-basin lake on the Keweenaw Peninsula. Prior to abrupt increases in the 19th and 20th centuries, mercury remains at relatively low concentrations for the last 9000 years. Higher mercury fluxes in the early Holocene (3.4 ± 1.1 µg m-2 yr-1) are attributed to drier conditions and greater forest fire occurrence. The gradual decline in mercury flux over the middle to late Holocene (1.9 ± 0.2 µg m-2 yr-1) is interpreted to reflect a transition to wetter conditions, which reduced forest fires, and promoted the development of soil organic matter and deciduous forests that sequestered natural sources of mercury. The Copper Falls Lake record highlights the sensitivity of watersheds to changes in mercury inputs from both human and natural forcings, and provides millennial-scale context for recent mercury contamination that will aid in establishing baseline values for restoration efforts.

Lake-sediment record of PAH, mercury, and fly-ash particle deposition near coal-fired power plants in Central Alberta, Canada.

We report a historical record of atmospheric deposition in dated sediment cores from Hasse Lake, ideally located near both currently and previously operational coal-fired power plants in Central Alberta, Canada. Accumulation rates of spheroidal carbonaceous particles (SCPs), an unambiguous marker of high-temperature fossil-fuel combustion, in the early part of the sediment record (pre-1955) compared well with historical emissions from one of North America's earliest coal-fired power plants (Rossdale) located ∼43 km to the east in the city of Edmonton. Accumulation rates in the latter part of the record (post-1955) suggested inputs from the Wabamun region's plants situated ∼17-25 km to the west. Increasing accumulation rates of SCPs, polycyclic aromatic hydrocarbons (PAHs) and Hg coincided with the previously documented period of peak pollution in the Wabamun region during the late 1960s to early 1970s, although Hg deposition trends were also similar to those found in western North American lakes not directly affected by point sources. A noticeable reduction in contaminant inputs during the 1970s is attributed in part to technological improvements and stricter emission controls. The over one hundred-year historical record of coal-fired power plant emissions documented in Hasse Lake sediments has provided insight into the impact that both environmental regulations and changes in electricity output have had over time. This information is crucial to assessing the current and future role of coal in the world's energy supply.

Mercury in tunas and blue marlin in the North Pacific Ocean.

Models and data from the North Pacific Ocean indicate that mercury concentrations in water and biota are increasing in response to (global or hemispheric) anthropogenic mercury releases. In the present study, we provide an updated record of mercury in yellowfin tuna (Thunnus albacares) caught near Hawaii that confirms an earlier conclusion that mercury concentrations in these fish are increasing at a rate similar to that observed in waters shallower than 1000 m. We also compiled and reanalyzed data from bigeye tuna (Thunnus obesus) and blue marlin (Makaira nigricans) caught near Hawaii in the 1970s and 2000s. Increases in mercury concentrations in bigeye tuna are consistent with the trend found in yellowfin tuna, in both timing and magnitude. The data available for blue marlin do not allow for a fair comparison among years, because mercury concentrations differ between sexes for this species, and sex was identified (or reported) in only 3 of 7 studies. Also, mercury concentrations in blue marlin may be insensitive to modest changes in mercury exposure, because this species appears to have the ability to detoxify mercury. The North Pacific Ocean is a region of both relatively high rates of atmospheric mercury deposition and capture fisheries production. Other data sets that allow temporal comparisons in mercury concentrations, such as pacific cod (Gadus macrocephalus) in Alaskan waters and albacore tuna (Thunnus alalunga) off the US Pacific coast, should be explored further, to aid in understanding human health and ecological risks and to develop additional baseline knowledge for assessing changes in a region expected to respond strongly to reductions in anthropogenic mercury emissions. Environ Toxicol Chem 2017;36:1365-1374. © 2017 SETAC.

Relationship among mercury concentration, growth rate, and condition of northern pike: A tautology resolved?

Methylmercury is a bioaccumulative contaminant that biomagnifies in aquatic food webs and adversely affects the health of freshwater fish. Previous studies have documented an inverse relationship between fish condition and concentration of mercury in fish. However, this relationship may be a result of slow-growing fish accumulating large amounts of methylmercury rather than the effects of methylmercury on fish condition and growth. An evaluation was conducted of the relationship among fish condition, growth, and mercury concentration in northern pike Esox lucius from 26 lakes in the western region of the Laurentian Great Lakes (USA-Canada). The relative weight (an index of fish condition) of northern pike was inversely related to mercury concentration in the axial muscle. The concentration of mercury in standard-size northern pike increased with fish age and suggested that fast-growing fish accumulated less mercury than slow-growing fish. However, there was no relationship between the mean relative weight of northern pike in each population and mean age or mercury concentration of standard-size northern pike. These results suggest that the relationship between mercury and fish condition is not because of the effects of mercury on rate of growth, but rather because slow-growing fish bioaccumulate greater concentrations of mercury than fast-growing fish of the same length. Environ Toxicol Chem 2016;35:2910-2915. © 2016 SETAC.

Spatiotemporal patterns of mercury accumulation in lake sediments of western North America.

For the Western North America Mercury Synthesis, we compiled mercury records from 165 dated sediment cores from 138 natural lakes across western North America. Lake sediments are accepted as faithful recorders of historical mercury accumulation rates, and regional and sub-regional temporal and spatial trends were analyzed with descriptive and inferential statistics. Mercury accumulation rates in sediments have increased, on average, four times (4×) from 1850 to 2000 and continue to increase by approximately 0.2µg/m(2) per year. Lakes with the greatest increases were influenced by the Flin Flon smelter, followed by lakes directly affected by mining and wastewater discharges. Of lakes not directly affected by point sources, there is a clear separation in mercury accumulation rates between lakes with no/little watershed development and lakes with extensive watershed development for agricultural and/or residential purposes. Lakes in the latter group exhibited a sharp increase in mercury accumulation rates with human settlement, stabilizing after 1950 at five times (5×) 1850 rates. Mercury accumulation rates in lakes with no/little watershed development were controlled primarily by relative watershed size prior to 1850, and since have exhibited modest increases (in absolute terms and compared to that described above) associated with (regional and global) industrialization. A sub-regional analysis highlighted that in the ecoregion Northwestern Forest Mountains, <1% of mercury deposited to watersheds is delivered to lakes. Research is warranted to understand whether mountainous watersheds act as permanent sinks for mercury or if export of "legacy" mercury (deposited in years past) will delay recovery when/if emissions reductions are achieved.

Subcellular distribution of trace elements and liver histology of landlocked Arctic char (Salvelinus alpinus) sampled along a mercury contamination gradient.

We sampled landlocked Arctic char (Salvelinus alpinus) from four lakes (Small, 9-Mile, North, Amituk) in the Canadian High Arctic that span a gradient of mercury contamination. Metals (Hg, Se, Tl, and Fe) were measured in char tissues to determine their relationships with health indices (relative condition factor and hepatosomatic index), stable nitrogen isotope ratios, and liver histology. A subcellular partitioning procedure was employed to determine how metals were distributed between potentially sensitive and detoxified compartments of Arctic char livers from a low- and high-mercury lake (Small Lake and Amituk Lake, respectively). Differences in health indices and metal concentrations among char populations were likely related to differences in feeding ecology. Concentrations of Hg, Se, and Tl were highest in the livers of Amituk char, whereas concentrations of Fe were highest in Small and 9-Mile char. At the subcellular level we found that although Amituk char had higher concentrations of Tl in whole liver than Small Lake char, they maintained a greater proportion of this metal in detoxified fractions, suggesting an attempt at detoxification. Mercury was found mainly in potentially sensitive fractions of both Small and Amituk Lake char, indicating that Arctic char are not effectively detoxifying this metal. Histological changes in char livers, mainly in the form of melano-macrophage aggregates and hepatic fibrosis, could be linked to the concentrations and subcellular distributions of essential or non-essential metals.

Embryotoxicity of maternally transferred methylmercury to fathead minnows (Pimephales promelas).

Mercury (Hg) is a ubiquitous environmental contaminant and potent neurotoxin. In aquatic environments, Hg can be transformed into methylmercury (MeHg), which bioaccumulates in aquatic food webs, including fish. Methylmercury has been shown to transfer from female fish to developing eggs; however, relatively little is known regarding the effects of maternally transferred MeHg on fish embryos. The present study evaluated the effects of maternally transferred MeHg on fathead minnow (Pimephales promelas) embryos. Embryos were collected from adult fatheads exposed for 30 d to 1 of 3 diets spiked with MeHg: a control diet (0.02 ppm Hg dry wt), a low diet (0.87 ppm Hg dry wt), or a high diet (5.5 ppm Hg dry wt). No effects on spawning frequency, clutch size, or total egg output were observed. In embryos, Hg concentration was a function of female diet and the duration (number of days) of female exposure. Compared with controls, embryos from the low-diet treatment displayed altered embryonic movement patterns (hyperactivity) and decreased time to hatch. Embryos from the high-diet treatment had delayed hatching and increased mortality compared with the other treatments. Collectively, these results suggest that maternally transferred Hg may impact survival, behavior, and developmental milestones of the embryo-larval stages of fish. Environ Toxicol Chem 2016;35:1436-1441. © 2015 SETAC.

The role of melano-macrophage aggregates in the storage of mercury and other metals: an example from yelloweye rockfish (Sebastes ruberrimus).

Melano-macrophage aggregates, collections of specialized cells of the innate immune system of fish, are considered a general biomarker for contaminant toxicity. To elucidate further the relationship between macrophage aggregates and metals exposure, yelloweye rockfish (Sebastes ruberrimus), a long-lived species, were sampled from the east and west coasts of Prince of Wales Island, Alaska. Metals concentrations in livers (inorganic Hg, methyl mercury, Se, Ni, Cd, Cu, Zn) and spleens (inorganic Hg and methyl mercury) were determined, as well as their correlations with melano-macrophage aggregate area. Sections of liver tissue were analyzed by laser ablation-inductively coupled plasma-mass spectrometry to determine how metals were spatially distributed between hepatocytes and macrophage aggregates. The concentration of inorganic Hg in whole tissue was the best predictor of macrophage area in yelloweye livers and spleens. Macrophage aggregates had higher relative concentrations than most metals compared with the surrounding hepatocytes. However, not all metals were accumulated to the same degree, as evidenced by differences in the ratios of metals in macrophages compared with hepatocytes. Laser ablation data were corroborated with the results of X-ray synchrotron fluorescence imaging of a yelloweye liver section. Hepatic macrophage aggregates in yelloweye rockfish may play an important role in the detoxification and storage of Hg and other metals.

Increase in mercury in Pacific yellowfin tuna.

Mercury is a toxic trace metal that can accumulate to levels that threaten human and environmental health. Models and empirical data suggest that humans are responsible for a great deal of the mercury actively cycling in the environment at present. Thus, one might predict that the concentration of mercury in fish should have increased dramatically since the Industrial Revolution. Evidence in support of this hypothesis has been hard to find, however, and some studies have suggested that analyses of fish show no change in mercury concentration. By compiling and re-analyzing published reports on yellowfin tuna (Thunnus albacares) caught near Hawaii (USA) over the past half century, the authors found that the concentration of mercury in these fish currently is increasing at a rate of at least 3.8% per year. This rate of increase is consistent with a model of anthropogenic forcing on the mercury cycle in the North Pacific Ocean and suggests that fish mercury concentrations are keeping pace with current loading increases to the ocean. Future increases in mercury in yellowfin tuna and other fishes can be avoided by reductions in atmospheric mercury emissions from point sources.

Atmospheric Hg emissions from preindustrial gold and silver extraction in the Americas: a reevaluation from lake-sediment archives.

Human activities over the last several centuries have transferred vast quantities of mercury (Hg) from deep geologic stores to actively cycling earth-surface reservoirs, increasing atmospheric Hg deposition worldwide. Understanding the magnitude and fate of these releases is critical to predicting how rates of atmospheric Hg deposition will respond to future emission reductions. The most recently compiled global inventories of integrated (all-time) anthropogenic Hg releases are dominated by atmospheric emissions from preindustrial gold/silver mining in the Americas. However, the geophysical evidence for such large early emissions is equivocal, because most reconstructions of past Hg-deposition have been based on lake-sediment records that cover only the industrial period (1850-present). Here we evaluate historical changes in atmospheric Hg deposition over the last millennium from a suite of lake-sediment cores collected from remote regions of the globe. Along with recent measurements of Hg in the deep ocean, these archives indicate that atmospheric Hg emissions from early mining were modest as compared to more recent industrial-era emissions. Although large quantities of Hg were used to extract New World gold and silver beginning in the 16th century, a reevaluation of historical metallurgical methods indicates that most of the Hg employed was not volatilized, but rather was immobilized in mining waste.