USGS ScienceSearch

Geology topics

David P. Krabbenhoft

Publications and source records attributed to David P. Krabbenhoft.

At least 19 recordsLinked to original sources

Ecological factors decouple Great Lakes fish mercury concentrations trends decadal declines in mercury emissions

Atmospheric mercury (Hg) deposition has been declining in North America but remains the dominant delivery mechanism to the Great Lakes. The Lakes are highly efficient at bioaccumulating methylmercury, making the fish excellent sentinels for tracking shifts in atmospheric Hg deposition. Invasive mussels have altered biogeochemical processes, prey populations and fish dietary strategies asynchronously and to varied extents across the lower four lakes, impacting fish Hg exposure. To test if fish are adapting to new biogeochemical conditions, we analyzed a 40 year fish archive for carbon and nitrogen isotope ratios and amino acid-specific nitrogen isotope ratios. To assess Hg sources, we measured Hg isotope ratios. We reconstructed and compared energetic pathways that impact fish Hg concentrations to Hg-source trends. We found fish-Hg concentrations are declining but not monotonically due to ecological disturbances. Fish-Hg isotope values, unimpacted by ecological disturbance, confirm that sources of bioaccumulated Hg shift contemporaneously with changes in atmospheric Hg concentrations. Across Lakes, the degree of responsiveness to changes in atmospheric Hg concentrations mirrors the proportion of atmospheric-delivered Hg we previously modeled. Changes in both fish concentrations and fish isotope values outpace paleolimnetic reconstructions suggesting declines in atmospheric Hg concentrations impact fish Hg more than sediment.

Great Lakes

Sulfate reduction drives elevated methylmercury formation in water column of eutrophic freshwater lake

Mercury (Hg) contamination of aquatic food webs is controlled in part by the formation and accumulation of toxic and bioaccumulative methylmercury (MeHg). MeHg production is mediated by metabolically diverse microorganisms carrying the hgcAB gene pair, while the demethylation reaction is mediated by several biotic and abiotic processes. However, the relative importance of these two processes on MeHg accumulation and the environmental factors that influence them are poorly characterized, especially in eutrophic environments. In this study, both Hg methylation and MeHg demethylation in a eutrophic freshwater lake were linked to ambient MeHg concentrations and hgcA abundance and expression. High methylation rate potentials indicated in situ MeHg formation was a key source of MeHg to the water column, driven by high hgcA abundance and transcription. Molybdate treatment decreased methylation rate potentials, highlighting the importance of sulfate reduction in driving MeHg formation. Sulfate-reducing bacteria accounted for over 50% of the hgcA gene transcription, despite representing less than 10% of the hgcA -carrying microbial community. An arsR -like transcriptional regulator preceded many hgcA sequences; these were transcriptionally active and linked to lower hgcA expression. Overall, this study elucidates the microbial and biogeochemical processes that influence the in situ formation of MeHg in understudied eutrophic freshwater environments.

Wisconsin

Contrasting magnitude and timing of pulsed aqueous methylmercury bioaccumulation across a reservoir food web

Water column hypoxia is a key process influencing methylmercury (MeHg) production and availability in waterbodies worldwide. During seasonal destratification, large, short-lived pulses of aqueous MeHg may be released into the subsequently mixed water column, but little is known about the fate of these pulses, particularly whether there are concomitant increases in MeHg uptake into aquatic food webs. We examined the magnitude and timing of MeHg uptake across several trophic guilds relative to the reservoir stratification status using biweekly mercury data from water, zooplankton, and fish (Bluegill, Lepomis macrochirus and Smallmouth Bass, Micropterus dolomieu ). Zooplankton MeHg concentrations increased by up to 250% during destratification, concurrent with increases in aqueous MeHg concentrations. Zooplankton and filter-passing MeHg concentrations were positively correlated when the reservoir was mixed ( R 2 = 0.95) and destratifying ( R 2 = 0.57) but not while the reservoir was stratified ( R 2 = 0.21). Mercury concentrations in adult bluegill and juveniles of both fish species increased 20–70% following destratification, with responses lagging 4–8 weeks behind those in water and zooplankton MeHg. Mercury concentrations in piscivorous adult bass varied little over the course of the study. Our findings demonstrate the responsiveness of reservoir food webs to pulses in MeHg availability, suggesting that these pulses could play an important role in biotic MeHg exposure within and downstream of reservoirs.

Idaho, Oregon

Connecting tributary mercury loads to nearshore and offshore sediments in Lake Superior

Lake Superior has a vast and largely undeveloped watershed in comparison to the other Great Lakes, which makes it challenging to study mercury (Hg) sources and cycling. To examine Hg inputs to Lake Superior, we conducted an expansive binational assessment in 40 watersheds from a diverse range of landcover types. We further paired tributary Hg data to sediment source portfolios in the nearshore and offshore zones of Lake Superior through partnership with the Great Lakes Sediment Surveillance Program. We observed that total Hg loads were highest in the spring driven by the combination of elevated Hg concentrations and increased water discharge from snowmelt. In addition, total Hg concentrations in tributaries from remote, heavily forested regions, such as Pukaskwa National Park and the Minnesota Northshore, were higher than the Southshore and Thunder Bay regions. Methylmercury concentrations and loads were more spatially dependent, often corresponding to regions with more wetlands (e.g., Michigan Upper Peninsula). We estimated that the total Hg tributary load to Lake Superior in 2021 was 126 kg per year. To further examine the fate of watershed Hg sources, we examined sediments from 28 sites in Lake Superior using Hg stable isotopes. At open water sites, precipitation was the primary Hg source to sediments, but within nearshore sites Hg originated predominantly from watershed runoff. This work further defines the sources and fate of Hg within Lake Superior and highlights how Hg delivery is intrinsically tied to varying hydrologic regimes.

Michigan, Minnesota, Ontario, Wisconsin

Longitudinal and seasonal changes of organic matter sources through a semi-arid river-reservoir system

The quality and quantity of organic matter (OM) in a river system directly affects ecosystem health; thus, managers benefit from an in-depth understanding of the drivers and sources of OM. In the Snake River, a highly altered river-reservoir system in the semi-arid western United States, OM production and loading are key drivers of reservoir anoxia, which leads to several deleterious processes such as mercury methylation. However, sources and quantities of OM to the Snake River, and the effects of impoundment on OM moving through the river-reservoir system, are not well understood. Particulate organic carbon (POC), dissolved organic carbon (DOC), particulate nitrogen (PN), chlorophyll a (chl- a ), and δ 15 N–PN and δ 13 C–POC isotopic ratios were measured bi-weekly for over 2 years at four locations through the Snake River Hells Canyon Reservoir Complex to determine spatial and temporal patterns of OM quantities and sources. POC concentrations increased through the riverine zone upstream of the reservoirs, likely due to in situ primary production and/or inputs from tributaries and agricultural drains; then decreased through the most upstream reservoir likely due to particle settling. Isotopic ratios and other OM source indicators (δ 15 N–PN, δ 13 C–POC, POC:PN, chl- a :POC) show that the dominant source of particulate OM was phytoplankton with seasonal terrestrial/macrophytic inputs. Results highlight the effects of major tributary and agricultural drain inputs, primary production, and impoundment on OM composition and concentration through a large river-reservoir system and may inform water quality management efforts in this and similar systems.

Idaho, Oregon

Riparian methylmercury production increases riverine mercury flux and food web concentrations

The production and uptake of toxic methylmercury (MeHg) impacts aquatic ecosystems globally. Rivers can be dynamic and difficult systems to study for MeHg production and bioaccumulation, hence identifying sources of MeHg to these systems is both challenging and important for resource management within rivers and main-stem reservoirs. Riparian zones, which are known biogeochemical hotspots for MeHg production, are understudied as potential sources of MeHg to rivers. Here, we present a comprehensive quantification of the hydrologic and biogeochemical processes governing MeHg concentrations, loads, and bioaccumulation at 16 locations along 164 km of the agriculturally intensive Snake River (Idaho, Oregon USA) during summer baseflow conditions, with emphasis on riparian production of MeHg. Approximately one-third of the MeHg load of the Snake River could not be attributed to inflowing waters (upgradient, tributaries, or irrigation drains). Across the study reach, increases in MeHg loads in surface waters were significantly correlated with MeHg concentrations in riparian porewaters, suggesting riparian zones were likely an important source of MeHg to the Snake River. Across all locations, MeHg concentrations in surface waters positively correlated with MeHg concentrations in benthic snails and clams, supporting that riparian produced MeHg was assimilated into local aquatic food webs. This study contributes new insights into riparian MeHg production within rivers which can inform mitigation efforts to reduce MeHg bioaccumulation in fish.

Idaho, Oregon

Geographic drivers of mercury entry into aquatic food webs revealed by mercury stable isotopes in dragonfly larvae

Atmospheric mercury (Hg) emissions and subsequent transport and deposition are major concerns within protected lands, including national parks, where Hg can bioaccumulate to levels detrimental to human and wildlife health. Despite this risk to biological resources, there is limited understanding of the relative importance of different Hg sources and delivery pathways within protected regions. Here, we used Hg stable isotope measurements of a single aquatic bioindicator, dragonfly larvae, to determine if these tracers can resolve spatial patterns in Hg sources, delivery mechanisms, and aquatic cycling at a national scale. Mercury isotope values in dragonfly tissues varied among habitat types (e.g., lentic, lotic, wetland) and geographic location. Photochemical-derived isotope fractionation was habitat-dependent and influenced by factors that impact light penetration directly or indirectly, including dissolved organic matter, canopy cover, and total phosphorus. Strong patterns for Δ 200 Hg emerged in the western US, highlighting the relative importance of wet deposition sources in arid regions in contrast to dry deposition delivery in forested regions. This work highlights the efficacy of dragonfly larvae as biosentinels for Hg isotope studies due to their ubiquity across freshwater ecosystems and ability to track variation in Hg sources and processing attributed to small-scale habitat and large-scale regional patterns.

Environmental Science and Technology

New tools for a legacy problem: How isotope tracers inform area of concern actions in the St. Louis River in Lake Superior

Numerous mercury (Hg) sources can contribute to biological burdens within the Great Lakes, including atmospheric deposition (e.g., precipitation), non-point source land runoff (e.g., watershed), and legacy contamination. Due to these different environmental entry points, it is often difficult to ascertain if legacy Hg contamination contributes to contemporary fish consumption advisories within Areas of Concern (AOCs), as designated by the United States-Canada Great Lakes Water Quality Agreement. In this study, we aimed to assess the contributions of legacy Hg to sediments in nearshore wetland habitats and co-located prey items (dragonfly larvae and yellow perch) within the St. Louis River AOC using Hg stable isotopes. We observed that nearshore sediments had the same Hg source portfolio as previously examined main channel sites. Furthermore, this data confirmed that two major Hg sources were contributing to sediments within nearshore regions of the St. Louis River AOC: legacy and watershed Hg. The contribution of legacy Hg was estimated in biota and demonstrated that up to 64% of the Hg in fish tissue in the lower estuary (St. Louis Bay) was from legacy sources, but that this percentage declined substantially when examining upstream regions of the AOC. These data indicate the influence of legacy Hg to the food web varies spatially within the St. Louis River. We further found that watershed Hg sources are an important Hg contributor to the St. Louis River, which likely applies to other impacted and unimpacted tributaries across the Great Lakes region.

Minnesota, Wisconsin

Habitat and dissolved organic carbon modulate variation in the biogeochemical drivers of mercury bioaccumulation in dragonfly larvae at the national scale

We paired mercury (Hg) concentrations in dragonfly larvae with water chemistry in 29 U.S. national parks to highlight how ecological and biogeochemical context (habitat, dissolved organic carbon [DOC]) influence drivers of Hg bioaccumulation. Although prior studies have defined influences of biogeochemical variables on Hg production and bioaccumulation, it has been challenging to determine their influence across diverse habitats, regions, or biogeochemical conditions within a single study. We compared global (i.e., all sites), habitat-specific, and DOC-class models to illuminate how these controls on biotic Hg vary. Although the suite of important biogeochemical factors across all sites (e.g., aqueous Hg, DOC, sulfate [SO42−], and pH) was consistent with general findings in the literature, contrasting the restricted models revealed more nuanced controls on biosentinel Hg. Comparing habitats, aqueous (filtered) total mercury (THg) and SO42− were important in lentic systems whereas aqueous (filtered) methylmercury (MeHg), DOC, pH, and SO42− were important in lotic and wetland systems. The ability to identify important variables varied among habitats, with less certainty in lentic (model weight (W) = 0.05) than lotic (W = 0.11) or wetland habitats (W = 0.23), suggesting that biogeochemical drivers of bioaccumulation are more variable, or obscured by other aspects of Hg cycling, in these habitats. Results revealed a contrast in the importance of aqueous MeHg versus aqueous THg between DOC-classes: in low-DOC sites (<8.5 mg/L), availability of upstream inputs of MeHg appeared more important for bioaccumulation; in high-DOC sites (>8.5 mg/L) THg was more important, suggesting a link to in-situ controls on bioavailability of Hg for MeHg production. Mercury bioaccumulation (indicated by bioaccumulation factor) was more efficient in low DOC-class sites, likely due to reduced partitioning of aqueous MeHg to DOC. Together, findings highlight substantial variation in the drivers of Hg bioaccumulation and suggest consideration of these factors in natural resource management and decision-making.

Science of the Total Environment

Increased mercury concentrations in walleye and yellow perch in lakes invaded by zebra mussels

Zebra mussels ( Dreissena polymorpha ) are invasive species that alter ecosystems and food webs with the potential to affect aquatic mercury cycling and bioaccumulation in fishes, although the effect of zebra mussels on fish tissue mercury has not been tested in inland lakes. We assessed differences in fish tissue mercury concentrations and food webs in Minnesota lakes with and without zebra mussels while controlling for other lake and watershed characteristics. Mercury concentrations in adult walleye ( Sander vitreus ) and yellow perch ( Perca flavescens ) were 72 % and 157 % higher, respectively, in lakes containing zebra mussels compared to uninvaded lakes. Mercury in young of year (age-0) fish was also elevated, with mercury concentrations 97 % and 82 % higher in age-0 walleye and yellow perch, respectively, in zebra mussel lakes. Walleye mercury concentrations exceeded 0.22 ppm — a threshold triggering more restrictive human consumption advisories for sensitive populations — at a 23 % smaller size, and average-sized walleye (420 mm) exceeded this threshold at a rate of 77 % in invaded lakes, compared to 35 % in uninvaded lakes. Walleye and yellow perch relied more on littoral resources in lakes with zebra mussels but did not feed at meaningfully higher trophic levels. Increased fish tissue mercury in lakes invaded by zebra mussels have consequential implications for fisheries and human health.

Minnesota

Competition between dissolved organic matter and freshwater plankton control methylmercury isotope fractionation during uptake and photochemical demethylation

Isotope fractionation related to photochemical reactions and planktonic uptake at the base of the food web is a major uncertainty in the biological application of mercury (Hg) stable isotopes. In freshwater systems, it is unclear how competitive interactions among methylmercury (MeHg), dissolved organic matter (DOM), and phytoplankton govern the magnitude of mass-dependent and mass-independent fractionation. This study investigated how DOM alters rates of planktonic MeHg uptake and photodegradation and corresponding Hg isotope fractionation in the presence of freshwater phytoplankton species, Raphidocelis subcapitata . Outdoor sunlight exposure experiments utilizing R. subcapitata were performed in the presence of different DOM samples using environmentally relevant ratios of MeHg-DOM thiol groups. The extent of Δ 199 Hg in phytoplankton incubations (2.99‰ St. Louis River HPOA, 1.88‰ Lake Erie HPOA) was lower compared to paired abiotic control experiments (4.29 and 2.86‰, respectively) after ∼30 h of irradiation, resulting from cell shading or other limiting factors reducing the extent of photodemethylation. Although the Δ 199 Hg/Δ 201 Hg ratio was uniform across experiments (∼1.4), Δ 199 Hg/δ 202 Hg slopes varied dramatically (from −0.96 to 15.4) across incubations with R. subcapitata and DOM. In addition, no evidence of Hg isotope fractionation was observed within R. subcapitata cells. This study provides a refined examination of Hg isotope fractionation markers for key processes occurring in the lower food web prior to bioaccumulation, critical for accurately accounting for the photochemical processing of Hg isotopes across a wide spectrum of freshwater systems.

ACS Earth and Space Chemistry

Reservoir stratification modulates the influence of impoundments on fish mercury concentrations along an arid land river system

Impoundment is among the most common hydrologic alterations with impacts on aquatic ecosystems that can include effects on mercury (Hg) cycling. However, landscape-scale differences in Hg bioaccumulation between reservoirs and other habitats are not well characterized nor are the processes driving these differences. We examined total Hg (THg) concentrations of Smallmouth Bass ( Micropterus dolomieu ) collected from reservoir, tailrace, and free-flowing reaches along an 863 km segment of the Snake River, USA, a semiarid river with 22 impoundments along its course. Across three size-classes (putative 1-year-old, first reproductive, and harvestable sized fish), THg concentrations in reservoirs and tailraces averaged 76% higher than those in free-flowing segments. Among reservoirs, THg concentrations were highest in reservoirs with inconsistent stratification patterns, 47% higher than annually stratified, and 144% higher than unstratified reservoirs. Fish THg concentrations in tailraces immediately downstream of stratified reservoirs were higher than those below unstratified (38–130%) or inconsistently stratified (32–79%) reservoirs. Stratification regimes influenced the exceedance of fish and human health benchmarks, with 52–80% of fish from stratifying reservoirs and downstream tailraces exceeding a human consumption benchmark, compared to 6–17% where stratification did not occur. These findings suggest that impoundment and stratification play important roles in determining the patterns of Hg exposure risk across the landscape.

Environmental Science & Technology

Linking meso-scale spatial variation in methylmercury production to bioaccumulation in tidal marsh food webs

Differences in sediment biogeochemistry among tidal marsh features with different hydrological and geomorphological characteristics, including marsh interiors, marsh edges, first-order channels, and third-order channels, can result in spatial variation in MeHg production and availability. To better understand the link between MeHg production in sediments and bioaccumulation in primary and secondary consumer invertebrates and fish, we characterized mesoscale spatial variation in sediment biogeochemistry and MeHg concentrations of sediments, water, and consumer tissues among marsh features. Our results indicated that marsh interiors had biogeochemical conditions, including greater concentrations of organic matter and sulfate reduction rates, that resulted in greater MeHg concentrations in sediments and surface water particulates from marsh interiors compared to other features. Tissue MeHg concentrations of consumers also differed among features, with greater concentrations from marsh edges and interiors compared to channels. This spatial mismatch of MeHg concentrations in sediments and water compared to those in consumers may have resulted from differences in behavior and physiology among consumers that influenced the spatial scale over which MeHg was integrated into tissues. Our results highlight the importance of sampling across a suite of marsh features and considering the behavioral and physiological traits of sentinel taxa for contaminant monitoring studies.

Environmental Science and Technology

Metabolically diverse microorganisms mediate methylmercury formation under nitrate-reducing conditions in a dynamic hydroelectric reservoir

Brownlee Reservoir is a mercury (Hg)-impaired hydroelectric reservoir that exhibits dynamic hydrological and geochemical conditions and is located within the Hells Canyon Complex in Idaho, USA. Methylmercury (MeHg) contamination in fish is a concern in the reservoir. While MeHg production has historically been attributed to sulfate-reducing bacteria and methanogenic archaea, microorganisms carrying the hgcA gene are taxonomically and metabolically diverse and the major biogeochemical cycles driving mercury (Hg) methylation are not well understood. In this study, Hg speciation and redox-active compounds were measured throughout Brownlee Reservoir across the stratified period in four consecutive years (2016–2019) to identify the location where and redox conditions under which MeHg is produced. Metagenomic sequencing was performed on a subset of samples to characterize the microbial community with hgcA and identify possible links between biogeochemical cycles and MeHg production. Biogeochemical profiles suggested in situ water column Hg methylation was the major source of MeHg. These profiles, combined with genome-resolved metagenomics focused on hgcA -carrying microbes, indicated that MeHg production occurs in this system under nitrate- or manganese-reducing conditions, which were previously thought to preclude Hg-methylation. Using this multidisciplinary approach, we identified the cascading effects of interannual variability in hydrology on the redox status, microbial metabolic strategies, abundance and metabolic diversity of Hg methylators, and ultimately MeHg concentrations throughout the reservoir. This work expands the known conditions conducive to producing MeHg and suggests that the Hg-methylation mitigation efforts by nitrate or manganese amendment may be unsuccessful in some locations.

Idaho

National-scale assessment of total gaseous mercury isotopes across the United States

With the 2011 promulgation of the Mercury and Air Toxics Standards by the U.S. Environmental Protection Agency, and the successful negotiation by the United Nations Environment Program of the Minamata Convention, emissions of mercury (Hg) have declined in the United States. While the declines in atmospheric Hg concentrations in North America are encouraging, linking the declines to changing domestic and global source portfolios remains challenging. To address these research gaps, the U.S. Geological Survey initiated the first national-scale effort to establish a baseline of total gaseous mercury stable isotope values at 31 sites distributed across the United States. Results indicated that unique Hg sources, such as Hg evasion from an elemental Hg contaminated site or free tropospheric intrusions in high altitude sites, were distinguishable from background atmospheric values. Minor gradients were observed across the nation, with regions of heavy industrial activity demonstrating lower δ 202 Hg, but no consistent changes in other isotopes such as Δ 199 Hg and Δ 200 Hg were observed. Furthermore, δ 202 Hg was impacted by foliar uptake and senescence but trends varied between forested regions in the northeastern and midwestern United States. These data demonstrate regional emission sources and other environmental variables can impact total gaseous Hg (TGM) isotope values, highlighting the need to characterize atmospheric Hg isotopes over larger geographical areas to evaluate changes related to national and international Hg regulations.

JGR Atmospheres

Understanding drivers of mercury in lake trout (Salvelinus namaycush), a top-predator fish in southwest Alaska's parklands

Mercury (Hg) is a widespread element and persistent pollutant, harmful to fish, wildlife, and humans in its organic, methylated form. The risk of Hg contamination is driven by factors that regulate Hg loading, methylation, bioaccumulation, and biomagnification. In remote locations, with infrequent access and limited data, understanding the relative importance of these factors can pose a challenge. Here, we assessed Hg concentrations in an apex predator fish species, lake trout (Salvelinus namaycush), collected from 14 lakes spanning two National Parks in southwest Alaska, U.S.A. We then examined factors associated with the variation in fish Hg concentrations using a Bayesian hierarchical model. We found that total Hg concentrations in water were consistently low among lakes (0.11–0.50 ng L− 1). Conversely, total Hg concentrations in lake trout spanned a thirty-fold range (101–3046 ng g− 1 dry weight), with median values at 7 lakes exceeding Alaska’s human consumption threshold. Model results showed that fish age and, to a lesser extent, body condition best explained variation in Hg concentration among fish within a lake, with Hg elevated in older, thinner lake trout. Other factors, including plankton methyl Hg content, fish species richness, volcano proximity, and glacier loss, best explained variation in lake trout Hg concentration among lakes. Collectively, these results provide evidence that multiple, hierarchically nested factors control fish Hg levels in these lakes.

Alaska

The influence of short-term temporal variability on the efficacy of dragonfly larvae as mercury biosentinels

Mercury (Hg) exposure to fish, wildlife, and humans is widespread and of global concern, thus stimulating efforts to reduce emissions. Because the relationships between rates of inorganic Hg loading, methylmercury (MeHg) production, and bioaccumulation are extremely complex and challenging to predict, there is a need for reliable biosentinels to understand the distribution of Hg in the environment and monitor the effectiveness of reduction efforts. However, it is important to assess how temporal and spatial variation at multiple scales influences the efficacy of specific biosentinels. Seasonal and interannual variation in total Hg (THg) concentrations of dragonfly larvae were examined in relation to spatial variability among 21 sites in two U.S. national parks with contrasting ecologies and Hg deposition patterns. Dragonfly THg differed among sampling events at 17 of the 21 sites, but by an average of only 20.4 % across events, compared to an average difference of 52.7 % among sites. Further, THg concentrations did not follow consistent seasonal patterns across sites or years, suggesting that the observed temporal variation was unlikely to bias monitoring efforts. Importantly, for a specific site, there was no difference in % MeHg in dragonflies among sampling events. Finally, there was significant temporal variability in the biogeochemical factors (aqueous inorganic Hg, aqueous MeHg, DOC, SO 4 , and pH) influencing dragonfly THg, with the importance of individual factors varying by 2.4 to 4.3-fold across sampling events. Despite these results, it is noteworthy that the observed temporal variation in dragonfly THg concentrations was neither large nor consistent enough to bias spatial assessments. Thus, although this temporal variation may provide insights into the processes influencing biological Hg concentrations, it is unlikely to impair the use of dragonflies as biosentinels for monitoring spatial or temporal patterns at scales relevant to most mitigation efforts.

Science of the Total Environment

Mercury sources and budget for the Snake River above a hydroelectric reservoir complex

Understanding sources of mercury (Hg) and methylmercury (MeHg) to a water body is critical for management but is often complicated by poorly characterized Hg inputs and in situ processes, such as inorganic Hg methylation. In this study, we determined inorganic Hg and MeHg concentrations and loads (filter-passing and particulate fractions) for a semi-arid 164-kilometer stretch of the Snake River above the Hells Canyon Complex, a Hg-impaired hydroelectric reservoir complex on the Idaho-Oregon border, and used water quality measurements and Hg stable isotope ratios to create a comprehensive Hg source budget for the river. Results show that whereas most of the streamflow to the study reach comes from the main branch of the Snake River (i.e., the upstream watershed), major tributaries within the study reach contribute a greater proportion of inorganic Hg and MeHg loads. Mercury stable-isotope analyses highlight that Hg within the tributaries is predominantly associated with geologic deposits and snowmelt sources, the latter reflecting wet deposition. Surprisingly, irrigation return drains contribute 40–50 % of particulate inorganic Hg loads despite being ≤4.3 % of the overall water budget. Together, tributaries and irrigation return drains account for 97–100 % of the inorganic Hg and streamflow to the study reach, but ~65 % of the MeHg, indicating in-stream and riparian methylation may be an important and previously unrecognized source of MeHg. Streamflow, total suspended solids, dissolved organic carbon, and agricultural land cover were found to be important controls on the mobilization and transport of different Hg species and fractions. This study represents the first fluvial budget for Hg in the Snake River that accounts for particulate and filter-passing Hg species from both major tributaries and irrigation return drains, and expands our understanding of Hg sources and methylation processes within semi-arid environments. This information is critical to inform management decisions related to elevated Hg burdens in biota.

Idaho, Nevada, Oregon