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USGS2010

Response of a macrotidal estuary to changes in anthropogenic mercury loading between 1850 and 2000

Methylmercury (MeHg) bioaccumulation in marine food webs poses risks to fish-consuming populations and wildlife. Here we develop and test an estuarine mercury cycling model for a coastal embayment of the Bay of Fundy, Canada. Mass budget calculations reveal that MeHg fluxes into sediments from settling solids exceed losses from sediment-to-water diffusion and resuspension. Although measured methylation rates in benthic sediments are high, rapid demethylation results in negligible net in situ production of MeHg. These results suggest that inflowing fluvial and tidal waters, rather than coastal sediments, are the dominant MeHg sources for pelagic marine food webs in this region. Model simulations show water column MeHg concentrations peaked in the 1960s and declined by almost 40% by the year 2000. Water column MeHg concentrations respond rapidly to changes in mercury inputs, reaching 95% of steady state in approximately 2 months. Thus, MeHg concentrations in pelagic organisms can be expected to respond rapidly to mercury loading reductions achieved through regulatory controls. In contrast MeHg concentrations in sediments have steadily increased since the onset of industrialization despite recent decreases in total mercury loading. Benthic food web MeHg concentrations are likely to continue to increase over the next several decades at present-day mercury emissions levels because the deep active sediment layer in this system contains a large amount of legacy mercury and requires hundreds of years to reach steady state with inputs.

Environmental Science & Technology↗

USGS2012

Combined sewer overflows: an environmental source of hormones and wastewater micropollutants

Data were collected at a wastewater treatment plant (WWTP) in Burlington, Vermont, USA, (serving 30,000 people) to assess the relative contribution of CSO (combined sewer overflow) bypass flows and treated wastewater effluent to the load of steroid hormones and other wastewater micropollutants (WMPs) from a WWTP to a lake. Flow-weighted composite samples were collected over a 13 month period at this WWTP from CSO bypass flows or plant influent flows ( n = 28) and treated effluent discharges ( n = 22). Although CSO discharges represent 10% of the total annual water discharge (CSO plus treated plant effluent discharges) from the WWTP, CSO discharges contribute 40–90% of the annual load for hormones and WMPs with high (>90%) wastewater treatment removal efficiency. By contrast, compounds with low removal efficiencies (<90%) have less than 10% of annual load contributed by CSO discharges. Concentrations of estrogens, androgens, and WMPs generally are 10 times higher in CSO discharges compared to treated wastewater discharges. Compound concentrations in samples of CSO discharges generally decrease with increasing flow because of wastewater dilution by rainfall runoff. By contrast, concentrations of hormones and many WMPs in samples from treated discharges can increase with increasing flow due to decreasing removal efficiency.

Environmental Science & Technology↗

USGS2025

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↗

USGS1997

Matrix-enhanced degradation of p,p'-DDT during gas chromatographic analysis: A consideration

Analysis of p,p ‘-DDT in environmental samples requires monitoring the GC-derived breakdown of this insecticide, which produces p,p ‘-DDD and/or p,p ‘-DDE, both also primary environmental degradation products. A performance evaluation standard (PES) containing p,p ‘-DDT but not p,p ‘-DDD or p,p ‘-DDE can be injected at regular intervals throughout an analytical sequence to monitor GC degradation. Some U.S. EPA methods limit GC breakdown of DDT in the PES to ≤20%. GC/MS analysis of large-volume natural water samples fortified with deuterium- and 13 C-labeled p,p ‘-DDT exhibited up to 65% DDT breakdown by the GC inlet. These matrix-enhanced GC degradation amounts substantially exceeded the <20% breakdown levels indicated by bracketing injections of the PES containing unlabeled and labeled DDT. Substantial matrix-enhanced GC degradation was not observed during analysis of a limited number of fractionated bed-sediment extracts containing labeled DDT. Use of isotopically labeled DDT seems to provide an effective tool for monitoring sample-specific DDT breakdown during GC/MS analysis. However, analyte co-elutions render impractical their use in GC/ECD analysis. The oc currence of matrix-enhanced GC degradation might have important implications on data quality and the resultant interpretations of the environmental degradation of DDT and other thermolabile contaminants.

Environmental Science & Technology↗

USGS2004

When synthetic chemicals degrade in the environment: What are the absolute fate, effects, and potential risks to humans and the ecosystem?

Various processes degrade synthetic chemicals—pesticides, pharmaceuticals, biocides, and industrials—in the environment ( 1 , 2 ). Consequently, the environment may be exposed to a mixture of the parent compounds and any resulting degradation products (degradates). Recent advances in analytical methodology and greater access to analytical standards have advanced degradates research ( 3 , 4 ). Specifically, research on pesticides has found degradates in surface water ( 5 – 10 ), groundwater ( 11 – 13 ), precipitation ( 14 – 16 ), air ( 17 , 18 ), and sediment ( 19 , 20 ). Pharmaceuticals and detergent degradates also exist in the environment ( 21 – 23 ). Figure 1 shows that degradates were detected as often as or more frequently than the parent compound. Although some regulatory schemes require information about the impacts of degradates on human and environmental health, that information does not exist for many compounds ( 25 , 26 ). Pesticides are the exception. In this article, we bring together the available data to address the environmental behavior of degradates and their effects on organisms and discuss how to identify substances of potential concern. In addition, we cite gaps in the current knowledge and make recommendations for future research requirements. While the article focuses on pesticides, we believe these observations can be extended to biologically active compounds and some industrial substances.

Environmental Science & Technology↗

USGS2016

Regional monitoring programs in the United States: Synthesis of four case studies from Pacific, Atlantic, and Gulf Coasts

Water quality monitoring is a cornerstone of environmental protection and ambient monitoring provides managers with the critical data they need to take informed action. Unlike site-specific monitoring that is at the heart of regulatory permit compliance, regional monitoring can provide an integrated, holistic view of the environment, allowing managers to obtain a more complete picture of natural variability and cumulative impacts, and more effectively prioritize management actions. By reviewing four long-standing regional monitoring programs that cover portions of all three coasts in the United States – Chesapeake Bay, Tampa Bay, Southern California Bight, and San Francisco Bay – important insights can be gleaned about the benefits that regional monitoring provides to managers. These insights include the underlying reasons that make regional monitoring programs successful, the challenges to maintain relevance and viability in the face of ever-changing technology, competing demands and shifting management priorities. The lessons learned can help other managers achieve similar successes as they seek to establish and reinvigorate their own monitoring programs.

California, Delaware, Florida, Maryland, New Jerse↗

USGS2002

VOCs, pesticides, nitrate, and their mixtures in groundwater used for drinking water in the United States

Samples of untreated groundwater from 1255 domestic drinking-water wells and 242 public supply wells were analyzed as part of the National Water-Quality Assessment Program of the U.S. Geological Survey between 1992 and 1999. Wells were sampled to define the regional quality of the groundwater resource and, thus, were distributed geographically across large aquifers, primarily in rural areas. For each sample, as many as 60 volatile organic compounds (VOCs), 83 pesticides, and nitrate were analyzed. On the basis of previous studies, nitrate concentrations as nitrogen ≥3 mg/L were considered to have an anthropogenic origin. VOCs were detected more frequently (44%) than pesticides (38%) or anthropogenic nitrate (28%). Seventy percent of the samples contained at least one VOC, pesticide, or anthropogenic nitrate; 47% contained at least two compounds; and 33% contained at least three compounds. The combined concentrations of VOCs and pesticides ranged from about 0.001 to 100 μg/L, with a median of 0.02 μg/L. Water from about 12% of the wells contained one or more compounds that exceeded U.S. Environmental Protection Agency drinking-water standards or human health criteria, primarily because of nitrate concentrations exceeding the maximum contaminant level in domestic wells. A mixture is defined as a unique combination of two or more particular compounds, regardless of the presence of other compounds that may occur in the same sample. There were 100 mixtures (significantly associated with agricultural land use) that had a detection frequency between 2% and 19%. There were 302 mixtures (significantly associated with urban land use) that had a detection frequency between 1% and <2%. Only 14 compounds (seven VOCs, six pesticides, and nitrate) contributed over 95% of the detections in these 402 mixtures; however, most samples with these mixtures also contain a variety of other compounds.

Environmental Science & Technology↗

USGS2014

Hydrological controls on methylmercury distribution and flux in a tidal marsh

The San Francisco Estuary, California, contains mercury (Hg) contamination originating from historical regional gold and Hg mining operations. We measured hydrological and geochemical variables in a tidal marsh of the Palo Alto Baylands Nature Preserve to determine the sources, location, and magnitude of hydrological fluxes of methylmercury (MeHg), a bioavailable Hg species of ecological and health concern. Based on measured concentrations and detailed finite-element simulation of coupled surface water and saturated-unsaturated groundwater flow, we found pore water MeHg was concentrated in unsaturated pockets that persisted over tidal cycles. These pockets, occurring over 16% of the marsh plain area, corresponded to the marsh root zone. Groundwater discharge (e.g., exfiltration) to the tidal channel represented a significant source of MeHg during low tide. We found that nonchannelized flow accounted for up to 20% of the MeHg flux to the estuary. The estimated net flux of filter-passing (0.45 μm) MeHg toward estuary was 10 ± 5 ng m –2 day –1 during a single 12-h tidal cycle, suggesting an annual MeHg load of 1.17 ± 0.58 kg when the estimated flux was applied to present tidal marshes and planned marsh restorations throughout the San Francisco Estuary.

Environmental Science & Technology↗

USGS2005

Why is metal bioaccumulation so variable? Biodynamics as a unifying concept

Ecological risks from metal contaminants are difficult to document because responses differ among species, threats differ among metals, and environmental influences are complex. Unifying concepts are needed to better tie together such complexities. Here we suggest that a biologically based conceptualization, the biodynamic model, provides the necessary unification for a key aspect in risk: metal bioaccumulation (internal exposure). The model is mechanistically based, but empirically considers geochemical influences, biological differences, and differences among metals. Forecasts from the model agree closely with observations from nature, validating its basic assumptions. The biodynamic metal bioaccumulation model combines targeted, high-quality geochemical analyses from a site of interest with parametrization of key physiological constants for a species from that site. The physiological parameters include metal influx rates from water, influx rates from food, rate constants of loss, and growth rates (when high). We compiled results from 15 publications that forecast species-specific bioaccumulation, and compare the forecasts to bioaccumulation data from the field. These data consider concentrations that cover 7 orders of magnitude. They include 7 metals and 14 species of animals from 3 phyla and 11 marine, estuarine, and freshwater environments. The coefficient of determination ( R 2 ) between forecasts and independently observed bioaccumulation from the field was 0.98. Most forecasts agreed with observations within 2-fold. The agreement suggests that the basic assumptions of the biodynamic model are tenable. A unified explanation of metal bioaccumulation sets the stage for a realistic understanding of toxicity and ecological effects of metals in nature.

Environmental Science & Technology↗

USGS2011

Sulfur in the South Florida ecosystem: Distribution, sources, biogeochemistry, impacts, and management for restoration

Sulfur is broadly recognized as a water quality issue of significance for the freshwater Florida Everglades. Roughly 60% of the remnant Everglades has surface water sulfate concentrations above 1 mg l-1, a restoration performance measure based on present sulfate levels in unenriched areas. Highly enriched marshes in the northern Everglades have average sulfate levels of 60 mg l-1. Sulfate loading to the Everglades is principally a result of land and water management in South Florida. The highest concentrations of sulfate (average 60-70 mg l-1) in the ecosystem are in canal water in the Everglades Agricultural Area (EAA). Potential sulfur sourcesin the watershed are many, but geochemical data and a preliminary sulfur mass balance for the EAA are consistent with sulfur presently used in agricultural, and sulfur released by oxidation of organic EAA soils (including legacy agricultural applications and natural sulfur) as the primary sources of sulfate enrichment in the EAA canals. Sulfate loading to the Everglades increases microbial sulfate reduction in soils, leading to more reducing conditions, greater cycling of nutrients in soils, production of toxic sulfide, and enhanced methylmercury (MeHg) production and bioaccumulation. Wetlands are zones of naturally high MeHg production, but the combination of high atmospheric mercury deposition rates in South Florida and elevated sulfate loading leads to increased MeHg production and MeHg risk to Everglades wildlife and human consumers. Sulfate from the EAA drainage canals penetrates deep into the Everglades Water Conservation Areas, and may extend into Everglades National Park. Present plans to restore sheet flow and to deliver more water to the Everglades may increase overall sulfur loads to the ecosystem, and move sulfate-enriched water further south. However, water management practices that minimize soil drying and rewetting cycles can mitigate sulfate release during soil oxidation. A comprehensive Everglades restoration strategy should include reduction of sulfur loads as a goal because of the many detrimental impacts of sulfate on the ecosystem. Monitoring data show that the ecosystem response to changes in sulfate levels is rapid, and strategies for reducing sulfate loading may be effective in the near term. A multifaceted approach employing best management practices for sulfur in agriculture, agricultural practices that minimize soil oxidation, and changes to stormwater treatment areas that increase sulfate retention could help achieve reduced sulfate loads to the Everglades, with resulting benefits.

Florida↗

USGS2017

Reassessment of the Upper Fremont Glacier ice-core chronologies by synchronizing of ice-core-water isotopes to a nearby tree-ring chronology

The Upper Fremont Glacier (UFG), Wyoming, is one of the few continental glaciers in the contiguous United States known to preserve environmental and climate records spanning recent centuries. A pair of ice cores taken from UFG have been studied extensively to document changes in climate and industrial pollution (most notably, mid-19th century increases in mercury pollution). Fundamental to these studies is the chronology used to map ice-core depth to age. Here, we present a revised chronology for the UFG ice cores based on new measurements and using a novel dating approach of synchronizing continuous water isotope measurements to a nearby tree-ring chronology. While consistent with the few unambiguous age controls underpinning the previous UFG chronologies, the new interpretation suggests a very different time scale for the UFG cores with changes of up to 80 years. Mercury increases previously associated with the mid-19th century Gold Rush now coincide with early-20th century industrial emissions, aligning the UFG record with other North American mercury records from ice and lake sediment cores. Additionally, new UFG records of industrial pollutants parallel changes documented in ice cores from southern Greenland, further validating the new UFG chronologies while documenting the extent of late 19th and early 20th century pollution in remote North America.

Environmental Science & Technology↗

USGS2023

Perfluorooctanesulfonate adversely affects a mayfly (Neocloeon triangulifer) at environmentally realistic concentrations

Of the emerging contaminant types thought to threaten freshwater biota, per- and polyfluoroalkyl substances appear to be particularly widespread, and limited studies conducted with these compounds thus far indicate insects may be particularly sensitive to them. This study investigated the short- and long-term effects of two commonly detected compounds on the laboratory-reared mayfly Neocloeon triangulifer in water only exposures. In acute tests, the mayfly was approximately 85-fold more sensitive to perfluorooctanesulfonate (PFOS) and 7-fold more sensitive to perfluorooctanoic acid (PFOA) than the next most sensitive species reported in the literature. In 14 day and full-life chronic PFOS toxicity tests, the lowest 10% effect concentration was 0.272 μg of PFOS/L, which is lower than any previous reports to the best of our knowledge, but consistent in demonstrating the sensitivity of insects to this compound. Conversely, N. triangulifer was not particularly chronically sensitive to PFOA. This study demonstrates the risks of environmentally relevant concentrations of PFOS to a freshwater insect and suggests that investigation of the toxicity of more compounds with different carbon-chain lengths and functional groups to freshwater insects is needed.

Environmental Science & Technology Letters↗

USGS2013

Novel and non-traditional use of stable isotope tracers to study metal bioavailability from natural particles

We devised a novel tracing approach that involves enriching test organisms with a stable metal isotope of low natural abundance prior to characterizing metal bioavailability from natural inorganic particles. In addition to circumventing uncertainties associated with labeling natural particles and distinguishing background metals, the proposed "reverse labeling" technique overcomes many drawbacks inherent to using radioisotope tracers. Specifically, we chronically exposed freshwater snails (Lymnaea stagnalis) to synthetic water spiked with Cu that was 99.4% 65 Cu to increase the relative abundance of 65 Cu in the snail’s tissues from 32% to >80%. The isotopically enriched snails were then exposed to benthic algae mixed with Cu-bearing Fe–Al particles collected from the Animas River (Colorado), an acid mine drainage impacted river. We used 63 Cu to trace Cu uptake from the natural particles and inferred their bioavailability from calculation of Cu assimilation into tissues. Cu assimilation from these particles was 44%, indicating that 44% of the particulate Cu was absorbed by the invertebrate. This demonstrates that inorganic particulate Cu can be bioavailable. The reverse labeling approach shows great potential in various scientific areas such as environmental contamination and nutrition for addressing questions involving uptake of an element that naturally has multiple isotopes.

Environmental Science & Technology↗

USGS2023

Airport deicers: An unrecognized source of phosphorus loading in receiving waters

Airport ice control products contributed to total phosphorus (TP) loadings in a study of surface water runoff at a medium-sized airport from 2015 to 2021. Eleven airport ice control products had TP concentrations from 1–807 mg L –1 in liquid formulas, while solid pavement deicer had a TP concentration of 805 mg kg –1 . Product application data, formula TP concentrations, and surface water sampling results were used to estimate TP concentration and loading contributions from these ice control products to receiving streams. Airport ice control products were found to contribute to TP in 84% of the water samples collected at downstream sites during deicing events, and TP concentrations at those sites exceeded aquatic life benchmarks in 70% of samples collected during deicing. A receiving stream 6 km downstream had TP attributed to airport ice control sources in 78% of the samples. TP loadings at an upstream site and the receiving stream site were greatest during the largest runoff events as is typical in urban runoff, but this pattern was not always followed at airport outfall sites due to the influence of TP in deicer products. Products analyzed in this study are used at airports across the United States and abroad, and findings suggest that airport deicers could represent a previously unrecognized source of phosphorus to adjacent waterways.

Wisconsin↗

USGS2019

Using age tracers and decadal sampling to discern trends in nitrate, arsenic and uranium in groundwater beneath irrigated cropland

Repeat sampling and age tracers were used to examine trends in nitrate, arsenic and uranium concentrations in groundwater beneath irrigated cropland. Much higher nitrate concentrations in shallow modern groundwater were observed at both the Columbia Plateau and High Plains sites (median values of 10.2 and 15.4 mg/L as N, respectively) than in groundwater that recharged prior to the onset of intensive irrigation (median values of <1 and <4 mg/L as N, respectively). Repeat sampling of these well networks indicates that high nitrate concentrations in modern, shallow groundwater have been sustained for decades, posing a future risk to older, deeper groundwater used for drinking water. In fact, nitrate concentrations in older modern water (30-60 years since recharge) at the High Plains site have increased in the last decade. Groundwater irrigated areas in the Columbia Plateau tend to have higher nitrate concentrations than surface-water irrigated areas suggesting that repeated dissolution of land applied fertilizer during recirculation may be an important factor causing high nitrate concentrations in groundwater. Mobilization of uranium and arsenic by land surface activities is suggested by the higher concentrations of these constituents in modern, shallow groundwater than in older, deeper groundwater at the Columbia Plateau site. Bicarbonate concentrations in modern groundwater are positively correlated with uranium (r=0.72, p<0.01), suggesting bicarbonate may mobilize uranium in this system. A positive correlation between arsenic and phosphorus concentrations in modern groundwater (r=0.55, p<0.01) suggests that phosphate from fertilizer outcompetes arsenate for sorption sites, mobilizing sorbed arsenic derived from past pesticide use or other sources.

Environmental Science and Technology↗

USGS2011

Probability of detecting perchlorate under natural conditions in deep groundwater in California and the Southwestern United States

We use data from 1626 groundwater samples collected in California, primarily from public drinking water supply wells, to investigate the distribution of perchlorate in deep groundwater under natural conditions. The wells were sampled for the California Groundwater Ambient Monitoring and Assessment Priority Basin Project. We develop a logistic regression model for predicting probabilities of detecting perchlorate at concentrations greater than multiple threshold concentrations as a function of climate (represented by an aridity index) and potential anthropogenic contributions of perchlorate (quantified as an anthropogenic score, AS). AS is a composite categorical variable including terms for nitrate, pesticides, and volatile organic compounds. Incorporating water-quality parameters in AS permits identification of perturbation of natural occurrence patterns by flushing of natural perchlorate salts from unsaturated zones by irrigation recharge as well as addition of perchlorate from industrial and agricultural sources. The data and model results indicate low concentrations (0.1-0.5 μg/L) of perchlorate occur under natural conditions in groundwater across a wide range of climates, beyond the arid to semiarid climates in which they mostly have been previously reported. The probability of detecting perchlorate at concentrations greater than 0.1 μg/L under natural conditions ranges from 50-70% in semiarid to arid regions of California and the Southwestern United States to 5-15% in the wettest regions sampled (the Northern California coast). The probability of concentrations above 1 μg/L under natural conditions is low (generally <3%).

California↗

USGS1996

Comparison of Eh and H2 measurements for delineating redox processes in a contaminated aquifer

Measurements of oxidation-reduction potential ( E h ) and concentrations of dissolved hydrogen (H 2 ) were made in a shallow groundwater system contaminated with solvents and jet fuel to delineate the zonation of redox processes. E h measurements ranged from +69 to -158 mV in a cross section of the contaminated plume and accurately delineated oxic from anoxic groundwater. Plotting measured E h and pH values on an equilibrium stability diagram indicated that Fe(III) reduction was the predominant redox process in the anoxic zone and did not indicate the presence of methanogenesis and sulfate reduction. In contrast, measurements of H 2 concentrations indicated that methanogenesis predominated in heavily contaminated sediments near the water table surface (H 2 ∼ 7.0 nM) and that the methanogenic zone was surrounded by distinct sulfate-reducing (H 2 ∼ 1-4 nM) and Fe(III)-reducing (H 2 ∼ 0.1-0.8 nM) zones. The presence of methanogenesis, sulfate reduction, and Fe(III) reduction was confirmed by the distribution of dissolved oxygen, sulfate, Fe(II), and methane in groundwater. These results show that H 2 concentrations were more useful for identifying anoxic redox processes than E h measurements in this groundwater system. However, H 2 -based redox zone delineations are more reliable when H 2 concentrations are interpreted in the context of electron-acceptor (oxygen, nitrate, sulfate) availability and the presence of final products [Fe(II), sulfide, methane] of microbial metabolism.

Environmental Science & Technology↗

USGS1998

Polychlorinated dibenzo-p-dioxin and dibenzofuran concentration profiles in sediment and fish tissue of the Willamette Basin, Oregon

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F) are highly hydrophobic compounds that have been implicated as carcinogens and, more recently, as estrogen disrupters. An occurrence and distribution study of these compounds in the Willamette Basin, Oregon, was conducted by the U.S. Geological Survey as part of the National Water-Quality Assessment Program. Bed sediment was collected from 22 sites; fish tissue was collected from eight sites. PCDD/F were found to be ubiquitous in Willamette Basin sediment. A distinct homolog profile, dominated by octachlorodibenzo-p-dioxin, was observed in sediment throughout the basin. The PCDD homolog profile was consistent at all sites, regardless of total PCDD/F concentration, presence of point sources, subbasin size, geographic location or land use. Principal components analysis revealed a gradient among the homolog profiles that showed increasing dominance of highly chlorinated congeners where human and industrial activity increased. Tissue and bed sediment obtained from the same site did not have similar PCDD/F concentrations or homolog profiles. Fish tissue showed enrichment in less chlorinated congeners and congeners with chlorine substitutions in the 2, 3, 7 and 8 positions.

Environmental Science & Technology↗