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Sarah E. Janssen

Publications and source records attributed to Sarah E. Janssen.

At least 55 records · Page 3Linked to original sources
USGS2022

Assessment of mercury in sediments and waters of Grubers Grove Bay, Wisconsin

Mercury is a global contaminant that can be detrimental to wildlife and human health. Anthropogenic emissions and point sources are primarily responsible for elevated mercury concentrations in sediments and waters. Mercury can physically move and chemically transform in the environment, resulting in biomagnification of mercury, in the form of methylmercury, in the food web and causing elevated mercury concentrations in upper trophic levels. The ability to measure total mercury concentrations in the environment has existed for several decades and makes it possible to detect hotspots that might exist because of ongoing or previous anthropogenic activity. However, recent (within the past 15 years) developments in mass spectrometry have made it possible to complete low level stable isotope analysis allowing for the determination of mercury sources—natural and anthropogenic—in the environment through “fingerprinting.” Grubers Grove Bay in Lake Wisconsin, the focus area of this study, was determined to have elevated mercury levels even after multiple remediation efforts, resulting in its listing on the Federal list of impaired waters pursuant to the Clean Water Act. Adjacent to the bay is the former Badger Army Ammunition Plant, which manufactured ammunition for the U.S. Army during the early and middle 20th century, after which it was put on standby before being fully decommissioned. This study assesses mercury concentrations in the sediments and suspended particulate matter of Grubers Grove Bay, Wiegands Bay, and upstream sites, and in adjacent soils on the former Badger Army Ammunition Plant site. This study confirmed that mercury contamination exists in the sediments of Grubers Grove Bay even after dredging attempts by the U.S. Army. Additionally, using isotope ratios and a two-endmember mixing model, it was determined that soil from within Badger Army Ammunition Plant’s former site contributed a substantial amount of mercury to the bay. This result was supported by an observed gradient of high to low mercury concentrations from the innermost (nearest Badger Army Ammunition Plant) to the outermost (farthest from Badger Army Ammunition Plant) part of the bay.

Wisconsin↗
USGS2022

Methylmercury stable isotopes: New insights on assessing aquatic food web bioaccumulation in legacy impacted regions

Through stable isotope measurements of total mercury (HgT), identification of crucial processes and transformations affecting different sources of mercury (Hg) has become possible. However, attempting to use HgT stable isotopes to track bioaccumulation of Hg sources among different food web compartments can be challenging, if not impossible, when tissues have varying methylmercury (MeHg) contents. We measured HgT and MeHg stable isotope ratios within the lower Fox River to examine how these values differed across the food web and if isotope values in biota were influenced by legacy contamination. We showed that seston, invertebrates, and fish had a large range of δ 202 HgT (−0.74 to 0.15 ‰, n = 11) due to varying MeHg contents in tissues but a commonly conserved MeHg isotope value (δ 202 MeHg ave = 0.01 ± 0.12 ‰, 1 standard deviation, n = 11). We also examined some mathematical approaches to estimate the MeHg isotope values, which were mostly comparable to measured MeHg isotope values in the Fox River, with some exceptions. In this study, we observed that the MeHg isotope values can elucidate links between different food web compartments and provide insight on aquatic Hg cycling that can be masked by the sole use of HgT isotopes in contaminated sites.

Wisconsin↗
USGS2022

Using carbon, nitrogen, and mercury isotope values to distinguish mercury sources to Alaskan lake trout

Lake trout ( Salvelinus namaycush ), collected from 13 remote lakes located in southwestern Alaska, were analyzed for carbon, nitrogen, and mercury (Hg) stable isotope values to assess the importance of migrating oceanic salmon, volcanic activity, and atmospheric deposition to fish Hg burden. Methylmercury (MeHg) bioaccumulation in phytoplankton (5.0–6.9 kg L –1 ) was also measured to quantify the basal uptake of MeHg to these aquatic food webs. Hg isotope values in lake trout revealed that while the extent of precipitation-delivered Hg was similar across the entire study area, volcanic Hg is likely an important additional source to lake trout in proximate lakes. In contrast, migratory salmon ( Oncorhynchus nerka ) deliver little MeHg to lake trout directly, although indirect delivery processes via decay could exist. A high level of variability in carbon, nitrogen, and Hg isotope values indicates niche partitioning in lake trout populations within each lake and that a complex suite of ecological interactions is occurring, complicating the conceptually linear assessment of the contaminant source to the receiving organism. Without connecting energy and contaminant isotope axes, we would not have understood why lake trout from these pristine lakes have highly variable Hg burdens despite consistently low water Hg and comparable age-length dynamics.

Alaska↗
USGS2022

Decadal trends of mercury cycling and bioaccumulation within Everglades National Park

Mercury (Hg) contamination has been a persistent concern in the Florida Everglades for over three decades due to elevated atmospheric deposition and the system's propensity for methylation and rapid bioaccumulation. Given declines in atmospheric Hg concentrations in the conterminous United States and efforts to mitigate nutrient release to the greater Everglades ecosystem, it was vital to assess how Hg dynamics responded on temporal and spatial scales. This study used a multimedia approach (water and biota) to examine Hg and methylmercury (MeHg) dynamics across a 76-site network within the southernmost portion of the region, Everglades National Park (ENP), from 2008 to 2018. Atmospheric Hg deposition was evaluated over time using a long-term monitoring station. Hg concentrations across matrices showed that air, water, and biota from the system were inextricably linked. Temporal patterns across matrices were driven primarily by hydrologic and climatic changes in the park and no evidence of a decline in atmospheric Hg deposition from 2008 to 2018 was observed, unlike other regions of the United States. In the Shark River Slough (SRS), excess dissolved organic carbon and sulfate were also consistently delivered from upgradient canals and showed no evidence of decline over the study period. Within the SRS a strong positive correlation was observed between MeHg concentrations in surface water and resident fish. Within distinct geographic regions of ENP (SRS, Marsh, Coastal), the geochemical controls on MeHg dynamics differed and highlighted regions susceptible to higher MeHg bioaccumulation, particularly in the SRS and Coastal regions. This study demonstrates the strong influence that dissolved organic carbon and sulfate loads have on spatial and temporal distributions of MeHg across the ENP. Importantly, improved water quality and flow rates are two key restoration targets of the nearly 30-year Everglades restoration program, which if achieved, this study suggests would lead to reduced MeHg production and exposure.

Florida↗
USGS2022

Tracing the sources and depositional history of mercury to coastal northeastern U.S. lakes

Mercury (Hg) deposition was reconstructed in sediment cores from lakes in two coastal U.S. National Parks: Acadia National Park (ANP) and Cape Cod National Seashore (CCNS), to fill an important spatial gap in Hg deposition records and to explore changing sources of Hg and processes affecting Hg accumulation in these coastal sites. Recent Hg deposition chronology was assessed using (1) a newly developed lead-210 ( 210 Pb) based sediment age model which employs 7 Be to constrain deposition and sediment mixing of 210 Pb-excess, (2) coinciding Pb flux and isotope ratios ( 206 Pb/ 207 Pb), and (3) Hg isotope ratios and their response to changes in Hg flux. At both sites, Hg flux increased substantially from pre-1850 levels, with accumulation in ANP peaking in the 1970s, whereas in CCNS, Hg levels were highest in recent sediments. Negative values of δ 202 Hg and Δ 199 Hg indicated terrestrially-derived Hg was a major constituent of Hg flux to Sargent Mountain Pond, ANP, although recent decreases in Hg flux were in agreement with precipitation Hg records, indicating a rapid watershed response. By contrast, δ 202 Hg and Δ 199 Hg profiles in Long Pond, CNNS reflect direct Hg deposition, but disturbances in the sedimentary record were indicated by bomb fallout radionuclide inventories and by peaks in both Pb and Hg isotope depth profiles. These cores provided poor reconstructions of atmospheric deposition and reveal responses that are decoupled from emissions reduction due to complex post-depositional redistribution of atmospheric metals including Hg. The application of multiple tracers of Hg deposition provide insight into the sources and pathways governing Hg accumulation in these lakes.

Maine, Massachusetts↗
USGS2021

Mercury isotope fractionation by internal demethylation and biomineralization reactions in seabirds: Implications for environmental mercury science

A prerequisite for environmental and toxicological applications of mercury (Hg) stable isotopes in wildlife and humans is quantifying the isotopic fractionation of biological reactions. Here, we measured stable Hg isotope values of relevant tissues of giant petrels ( Macronectes spp.). Isotopic data were interpreted with published HR-XANES spectroscopic data that document a stepwise transformation of methylmercury (MeHg) to Hg-tetraselenolate (Hg(Sec) 4 ) and mercury selenide (HgSe) (Sec = selenocysteine). By mathematical inversion of isotopic and spectroscopic data, identical δ 202 Hg values for MeHg (2.69 ± 0.04‰), Hg(Sec) 4 (−1.37 ± 0.06‰), and HgSe (0.18 ± 0.02‰) were determined in 23 tissues of eight birds from the Kerguelen Islands and Adélie Land (Antarctica). Isotopic differences in δ 202 Hg between MeHg and Hg(Sec) 4 (−4.1 ± 0.1‰) reflect mass-dependent fractionation from a kinetic isotope effect due to the MeHg → Hg(Sec) 4 demethylation reaction. Surprisingly, Hg(Sec) 4 and HgSe differed isotopically in δ 202 Hg (+1.6 ± 0.1‰) and mass-independent anomalies (i.e., changes in Δ 199 Hg of ≤0.3‰), consistent with equilibrium isotope effects of mass-dependent and nuclear volume fractionation from Hg(Sec) 4 → HgSe biomineralization. The invariance of species-specific δ 202 Hg values across tissues and individual birds reflects the kinetic lability of Hg-ligand bonds and tissue-specific redistribution of MeHg and inorganic Hg, likely as Hg(Sec) 4 . These observations provide fundamental information necessary to improve the interpretation of stable Hg isotope data and provoke a revisitation of processes governing isotopic fractionation in biota and toxicological risk assessment in wildlife.

Environmental Science and Technology↗
USGS2021

The influence of legacy contamination on the transport and bioaccumulation of mercury within the Mobile River Basin

Past industrial use and subsequent release of mercury (Hg) into the environment have resulted in severe cases of legacy contamination that still influence contemporary Hg levels in biota. While the bioaccumulation of legacy Hg is commonly assessed via concentration measurements within fish tissue, this practice becomes difficult in regions of high productivity and methylmercury (MeHg) production, like the Mobile River Basin, Alabama in the southeastern United States. This study applied Hg stable isotope tracers to distinguish legacy Hg from regional deposition sources in sediments, waters, and fish within the Mobile River. Sediments and waters displayed differences in δ 202 Hg between industrial and background sites, which corresponded to drastic differences in Hg concentration. Sites that were affected by legacy Hg, as defined by δ 202 Hg, produced largemouth bass with lower MeHg content (59–70%) than those captured in the main rivers (>85%). Direct measurements of Hg isotopes and mathematical estimates of MeHg isotope pools in fish displayed similar distinctions between legacy and watershed sources as observed in other matrices. These results indicate that legacy Hg can accumulate directly into fish tissue as the inorganic species and may also be available for methylation within contaminated zones decades after the initial release.

Alabama↗
USGS2021

Examining historical mercury sources in the Saint Louis River estuary: How legacy contamination influences biological mercury levels in Great Lakes coastal regions

Industrial chemical contamination within coastal regions of the Great Lakes can pose serious risks to wetland habitat and offshore fisheries, often resulting in fish consumption advisories that directly affect human and wildlife health. Mercury (Hg) is a contaminant of concern in many of these highly urbanized and industrialized coastal regions, one of which is the Saint Louis River estuary (SLRE), the second largest tributary to Lake Superior. The SLRE has legacy Hg contamination that drives high Hg concentrations within sediments, but it is unclear whether legacy-derived Hg actively cycles within the food web. To understand the relative contributions of legacy versus contemporary Hg sources in coastal zones, Hg, carbon, and nitrogen stable isotope ratios were measured in sediments and food webs of SLRE and the Bad River, an estuarine reference site. Hg stable isotope values revealed that legacy contamination of Hg was widespread and heterogeneously distributed in sediments of SLRE, even in areas lacking industrial Hg sources. Similar isotope values were found in benthic invertebrates, riparian spiders, and prey fish from SLRE, confirming legacy Hg reaches the SLRE food web. Direct comparison of prey fish from SLRE and the Bad River confirmed that Hg isotope differences between the sites were not attributable to fractionation associated with rapid Hg bioaccumulation at estuarine mouths, but due to the presence of industrial Hg within SLRE. The Hg stable isotope values of game fish in both estuaries were dependent on fish migration and diet within the estuaries and extending into Lake Superior. These results indicate that Hg from legacy contamination is actively cycling within the SLRE food web and, through migration, this Hg also extends into Lake Superior via game fish. Understanding sources and the movement of Hg within the estuarine food web better informs restoration strategies for other impaired Great Lakes coastal zones.

Minnesota, Wisconsin↗
USGS2021

Stable isotope fractionation reveals similar atomic-level controls during aerobic and anaerobic microbial Hg transformation pathways

Mercury (Hg) is a global pollutant and potent neurotoxin that bioaccumulates in food webs as monomethylmercury (MeHg). The production of MeHg is driven by anaerobic and Hg redox cycling pathways, such as Hg reduction, which control the availability of Hg to methylators. Anaerobes play an important role in Hg reduction in methylation hot spots, yet their contributions remain underappreciated due to how challenging these pathways are to study in the absence of dedicated genetic targets and low levels of Hg 0 in anoxic environments. In this study, we used Hg stable isotope fractionation to explore Hg reduction during anoxygenic photosynthesis and fermentation in the model anaerobe Heliobacterium modesticaldum Ice1. We show that cells preferentially reduce lighter Hg isotopes in both metabolisms, leading to mass-dependent fractionation, but mass-independent fractionation commonly induced by UV-visible light is absent. Due to the variability associated with replicate experiments, we could not discern whether dedicated physiological processes drive Hg reduction during photosynthesis and fermentation. However, we demonstrate that fractionation is affected by the interplay between pathways controlling Hg recruitment, accessibility, and availability alongside metabolic redox reactions. The combined contributions of these processes lead to isotopic enrichment during anoxygenic photosynthesis that is in between the values reported for anaerobic respiratory microbial Hg reduction and abiotic photoreduction. Isotope enrichment during fermentation is closer to what has been observed in aerobic bacteria that reduce Hg through dedicated detoxification pathways. Our work suggests that similar controls likely underpin diverse microbe-mediated Hg transformations that affect Hg’s fate in oxic and anoxic habitats.

Applied and Environmental Microbiology↗
USGS2020

Mercury methylation genes identified across diverse anaerobic microbial guilds in a eutrophic sulfate-enriched lake

Mercury (Hg) methylation is a microbially mediated process that converts inorganic Hg into bioaccumulative, neurotoxic methylmercury (MeHg). The metabolic activity of methylating organisms is highly dependent on biogeochemical conditions, which subsequently influences MeHg production. However, our understanding of the ecophysiology of methylators in natural ecosystems is still limited. Here, we identified potential locations of MeHg production in the anoxic, sulfidic hypolimnion of a freshwater lake. At these sites, we used shotgun metagenomics to characterize microorganisms with the Hg-methylation gene hgcA . Putative methylators were dominated by hgcA sequences divergent from those in well-studied, confirmed methylators. Using genome-resolved metagenomics, we identified organisms with hgcA (hgcA+) within the Bacteroidetes and the recently described Kiritimatiellaeota phyla. We identified hgcA+ genomes derived from sulfate-reducing bacteria, but these accounted for only 22% of hgcA+ genome coverage. The most abundant hgcA+ genomes were from fermenters, accounting for over half of the hgcA gene coverage. Many of these organisms also mediate hydrolysis of polysaccharides, likely from cyanobacterial blooms. This work highlights the distribution of the Hg-methylation genes across microbial metabolic guilds and indicate that primary degradation of polysaccharides and fermentation may play an important but unrecognized role in MeHg production in the anoxic hypolimnion of freshwater lakes.

Environmental Science and Technology↗
USGS2020

Insights into mercury source identification and bioaccumulation using stable isotope approaches in the Hannibal Pool of the Ohio River

Mercury contamination in river systems due to historic and current Hg releases is a persistent concern for both wildlife and human health. In larger rivers, like the Ohio River, USA, it is difficult to directly link Hg discharges to bioaccumulation due to the existence of multiple industrial Hg sources as well as the varied dietary and migratory habits of biota. To better understand how industrial effluent influences the cycling and bioaccumulation of Hg within the Ohio River, Hg stable isotope analysis was applied to various nonbiological and biological media. High Hg concentrations in suspended particulate matter suggest this vector was the largest contributor of Hg to the water column, and distinct Hg source signatures were observed in effluent particulates from different industrial processes, such as chlor‐alkali activity (δ 202 Hg = −0.52‰) and coal power plant discharge (δ 202 Hg = −1.39‰). Despite this distinction, average sediments (δ 202 Hg = −1.00 ± 0.23‰) showed intermediate isotopic signatures that suggest the accumulation of a mixed Hg source driven by multiple industrial discharges. Biota in the system were shown to have a conserved range of δ 202 Hg and estimation approaches related these signatures back to particulate matter within Hannibal Pool. Mussels were found to conserve Hg isotopes signatures independently of food web drivers and served as ideal water column indicators of bioaccumulated Hg sources. This study highlights the complexity of Hg cycling within an industrialized river and shows that an isotope tracer approach can provide insight to water column sources of Hg. Integr Environ Assess Manag 2021;17:233−242. Published 2020. This article is a US Government work and is in the public domain in the USA.

Ohio↗
USGS2020

Resolving atmospheric mercury loading and source trends from isotopic records of remote North American lake sediments

The strongest evidence for anthropogenic alterations to the global mercury (Hg) cycle comes from historical records of mercury deposition preserved in lake sediments. Hg isotopes have added a new dimension to these sedimentary archives, promising additional insights into Hg source apportionment and biogeochemical processing. Presently, most interpretations of historical changes are constrained to a small number of locally contaminated ecosystems. Here, we describe changes in natural Hg isotope records from a suite of dated sediment cores collected from various remote lakes of North America. In nearly all cases, the rise in industrial-use Hg is accompanied by an increase in δ 202 Hg and Δ 199 Hg values. These trends can be attributed to large-scale industrial emission of Hg into the atmosphere and are consistent with positive Δ 199 Hg values measured in modern-day precipitation and modeled increases in δ 202 Hg values from global emission inventories. Despite similar temporal trends among cores, the baseline isotopic values vary considerably among the different study regions, likely attributable to differences in the fractionation produced in situ as well as differing amounts of atmospherically delivered Hg. Differences among the study lakes in precipitation and watershed size provide an empirical framework for evaluating Hg isotopic signatures and global Hg cycling.

North America↗
USGS2020

Tracing the uptake of Hg(II) in an iron-reducing bacterium using mercury stable isotopes

Anaerobic microorganisms play a key role in the biological mercury (Hg) cycle due to their ability to produce bioaccumulative neurotoxic methylmercury (MeHg). However, despite recent advances, how bacteria accumulate inorganic Hg [Hg(II)] prior to methylation is largely unknown. In this study, we applied Hg stable isotopes to measure changes in cellular compartments of Geobacter sulfurreducens and a nonmethylating mutant strain to investigate intracellular transport of Hg(II). Both strains accumulated intracellular Hg(II) that was lower in δ 202 Hg relative to dissolved extracellular Hg(II), demonstrating mass-dependent fractionation during uptake. Hg reduction by the mutant strain (50% Hg concentration loss in 24 h) resulted in higher δ 202 Hg values of cellular Hg than in wild-type cells. Further observations showed increasing δ 202 Hg values in dissolved extracellular MeHg and Hg(II) but decreasing δ 202 Hg values of intracellular Hg(II) in wild-type G. sulfurreducens suggesting that external Hg pools may be the proximate source of Hg for methylation in this bacterium. This investigation demonstrates that cellular uptake is comprised of multiple processes and transformations that influence Hg(II) prior to methylation, which can impart distinct isotopic signatures to Hg(II) and MeHg pools in the environment.

Environmental Science and Technology Letters↗
USGS2020

Mercury, cadmium, copper, arsenic, and selenium measurements in the feathers of adult eastern brown pelicans (Pelecanus occidentalis carolinensis) and chicks in multiple breeding grounds in the northern Gulf of Mexico

The amounts of trace metals and metalloids that have been introduced into aquatic ecosystems due to anthropogenic activities have increased in recent decades. Some of these elements like mercury are easily transferred from one trophic level to another and can accumulate to toxic quantities in organisms at the top of aquatic food webs. For this reason, seabirds like the Eastern brown pelican (Pelecanus occidentalis carolinensis ) are susceptible to heavy metal and metalloid toxicity and may warrant periodic monitoring. Mercury, cadmium, copper, arsenic and selenium were measured in the feathers of adult brown pelicans and chicks in several breeding colonies (Shamrock Island, Chester Island, Marker 52 Island, North Deer Island, Raccoon Island, Felicity Island, Gaillard Island, Audubon Island, and Ten Palms Island) in the Northern Gulf of Mexico. Overall, most chicks and adults examined had mercury levels in feathers that were below the concentration range in which birds show symptoms of mercury toxicity. However, chicks in the Audubon Island and Ten Palms Island colonies displayed mercury levels that were 3 times higher than values observed in 5 other colonies. In addition, several adults and chicks displayed selenium concentrations that are above what is considered safe for birds. Cadmium quantities in feathers were below levels that trigger toxicity in birds. Similarly, arsenic measurements were at quantities below the average of what has been reported for birds living in contaminated sites. Finally, we identify pelican breeding colonies that may warrant monitoring due to elevated levels of contaminants.

Alabama, Florida, Louisiana,Texas↗
USGS2020

The assessment and remediation of mercury contaminated sites: A review of current approaches

Remediation of mercury (Hg) contaminated sites has long relied on traditional approaches, such as removal and containment/capping. Here we review contemporary practices in the assessment and remediation of industrial-scale Hg contaminated sites and discuss recent advances. Significant improvements have been made in site assessment, including the use of XRF to rapidly identify the spatial extent of contamination, Hg stable isotope fractionation to identify sources and transformation processes, and solid-phase characterization (XAFS) to evaluate Hg forms. The understanding of Hg bioavailability for methylation has been improved by methods such as sequential chemical extractions and porewater measurements, including the use of diffuse gradient in thin-film (DGT) samplers. These approaches have shown varying success in identifying bioavailable Hg fractions and further study and field applications are needed. The downstream accumulation of methylmercury (MeHg) in biota is a concern at many contaminated sites. Identifying the variables limiting/controlling MeHg production—such as bioavailable inorganic Hg, organic carbon, and/or terminal electron acceptors (e.g. sulfate, iron) is critical. Mercury can be released from contaminated sites to the air and water, both of which are influenced by meteorological and hydrological conditions. Mercury mobilized from contaminated sites is predominantly bound to particles, highly correlated with total sediment solids (TSS), and elevated during stormflow. Remediation techniques to address Hg contamination can include the removal or containment of Hg contaminated materials, the application of amendments to reduce mobility and bioavailability, landscape/waterbody manipulations to reduce MeHg production, and food web manipulations through stocking or extirpation to reduce MeHg accumulated in desired species. These approaches often rely on knowledge of the Hg forms/speciation at the site, and utilize physical, chemical, thermal and biological methods to achieve remediation goals. Overall, the complexity of Hg cycling allows many different opportunities to reduce/mitigate impacts, which creates flexibility in determining suitable and logistically feasible remedies.

Science of the Total Environment↗
USGS2019

Isolation of methylmercury using distillation and anion-exchange chromatography for isotopic analyses in natural matrices

The development of mercury (Hg) stable isotope measurements has enhanced the study of Hg sources and transformations in the environment. As a result of the mixing of inorganic Hg (iHg) and methylmercury (MeHg) species within organisms of the aquatic food web, understanding species-specific Hg stable isotopic compositions is of significant importance. The lack of MeHg isotope measurements is due to the analytical difficulty in the separation of the MeHg from the total Hg pool, with only a few methods having been tested over the past decade with varying degrees of success, and only a handful of environmentally relevant measurements. Here, we present a novel anion-exchange resin separation method using AG 1-X4 that further isolates MeHg from the sample matrix, following a distillation pretreatment, in order to obtain ambient MeHg stable isotopic compositions. This method avoids the use of organic reagents, does not require complex instrumentation, and is applicable across matrices. Separation tests across sediment, water, and biotic matrices showed acceptable recoveries (98 ± 5%, n = 54) and reproducible δ 202 Hg isotope results (2 SDs ≤ 0.15‰) down to 5 ng of MeHg. The measured MeHg pools in natural matrices, such as plankton and sediments, showed large deviations from the non-speciated total Hg measurement, indicating that there is an important isotopic shift during methylation that is not recorded by typical measurements, but is vital in order to assess sources of Hg during bioaccumulation.

Analytical and Bioanalytical Chemistry↗
USGS2019

Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ 202 Hg increased (0.4‰) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ 202 Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

Lake Michigan↗