Fate of alkylbenzenesulfonates and dialkyltetralinsulfonates in sewage contaminated ground water
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Environmental Science & Technology↗
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Size-dependent reactivity of magnetite nanoparticles: a field-laboratory comparison
Logistic challenges make direct comparisons between laboratory- and field-based investigations into the size-dependent reactivity of nanomaterials difficult. This investigation sought to compare the size-dependent reactivity of nanoparticles in a field setting to a laboratory analog using the specific example of magnetite dissolution. Synthetic magnetite nanoparticles of three size intervals, ∼6 nm, ∼44 nm, and ∼90 nm were emplaced in the subsurface of the USGS research site at the Norman Landfill for up to 30 days using custom-made subsurface nanoparticle holders. Laboratory analog dissolution experiments were conducted using synthetic groundwater. Reaction products were analyzed via TEM and SEM and compared to initial particle characterizations. Field results indicated that an organic coating developed on the particle surfaces largely inhibiting reactivity. Limited dissolution occurred, with the amount of dissolution decreasing as particle size decreased. Conversely, the laboratory analogs without organics revealed greater dissolution of the smaller particles. These results showed that the presence of dissolved organics led to a nearly complete reversal in the size-dependent reactivity trends displayed between the field and laboratory experiments indicating that size-dependent trends observed in laboratory investigations may not be relevant in organic-rich natural systems.
Environmental Science & Technology↗
Lacustrine responses to decreasing wet mercury deposition rates: results from a case study in northern Minnesota
We present a case study comparing metrics of methylmercury (MeHg) contamination for four undeveloped lakes in Voyageurs National Park to wet atmospheric deposition of mercury (Hg), sulfate (SO 4 –2 ), and hydrogen ion (H + ) in northern Minnesota. Annual wet Hg, SO 4 –2 , and H + deposition rates at two nearby precipitation monitoring sites indicate considerable decreases from 1998 to 2012 (mean decreases of 32, 48, and 66%, respectively). Consistent with decreases in the atmospheric pollutants, epilimnetic aqueous methylmercury (MeHg aq ) and mercury in small yellow perch (Hg fish ) decreased in two of four lakes (mean decreases of 46.5% and 34.5%, respectively, between 2001 and 2012). Counter to decreases in the atmospheric pollutants, MeHg aq increased by 85% in a third lake, whereas Hg fish increased by 80%. The fourth lake had two disturbances in its watershed during the study period (forest fire; changes in shoreline inundation due to beaver activity); this lake lacked overall trends in MeHg aq and Hg fish . The diverging responses among the study lakes exemplify the complexity of ecosystem responses to decreased loads of atmospheric pollutants.
Minnesota↗
Transformation products and human metabolites of triclocarban and tricllosan in sewage sludge across the United States
Removal of triclocarban (TCC) and triclosan (TCS) from wastewater is a function of adsorption, abiotic degradation, and microbial mineralization or transformation, reactions that are not currently controlled or optimized in the pollution control infrastructure of standard wastewater treatment. Here, we report on the levels of eight transformation products, human metabolites, and manufacturing byproducts of TCC and TCS in raw and treated sewage sludge. Two sample sets were studied: samples collected once from 14 wastewater treatment plants (WWTPs) representing nine states, and multiple samples collected from one WWTP monitored for 12 months. Time-course analysis of significant mass fluxes (α = 0.01) indicate that transformation of TCC (dechlorination) and TCS (methylation) occurred during sewage conveyance and treatment. Strong linear correlations were found between TCC and the human metabolite 2′-hydroxy-TCC ( r = 0.84), and between the TCC-dechlorination products dichlorocarbanilide (DCC) and monochlorocarbanilide ( r = 0.99). Mass ratios of DCC-to-TCC and of methyl-triclosan (MeTCS)-to-TCS, serving as indicators of transformation activity, revealed that transformation was widespread under different treatment regimes across the WWTPs sampled, though the degree of transformation varied significantly among study sites (α = 0.01). The analysis of sludge sampled before and after different unit operation steps (i.e., anaerobic digestion, sludge heat treatment, and sludge drying) yielded insights into the extent and location of TCC and TCS transformation. Results showed anaerobic digestion to be important for MeTCS transformation (37–74%), whereas its contribution to partial TCC dechlorination was limited (0.4–2.1%). This longitudinal and nationwide survey is the first to report the occurrence of transformation products, human metabolites, and manufacturing byproducts of TCC and TCS in sewage sludge.
Environmental Science & Technology↗
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↗
Spatial and temporal patterns in concentrations of perfluorinated compounds in bald eagle nestlings in the Upper Midwestern United States
Perfluorinated chemicals (PFCs) are of concern due to their widespread use, persistence in the environment, tendency to accumulate in animal tissues, and growing evidence of toxicity. Between 2006 and 2011 we collected blood plasma from 261 bald eagle nestlings in six study areas from the upper Midwestern United States. Samples were assessed for levels of 16 different PFCs. We used regression analysis in a Bayesian framework to evaluate spatial and temporal trends for these analytes. We found levels as high as 7370 ng/mL for the sum of all 16 PFCs (∑PFCs). Perfluorooctanesulfonate (PFOS) and perfluorodecanesulfonate (PFDS) were the most abundant analytes, making up 67% and 23% of the PFC burden, respectively. Levels of ∑PFC, PFOS, and PFDS were highest in more urban and industrial areas, moderate on Lake Superior, and low on the remote upper St. Croix River watershed. We found evidence of declines in ∑PFCs and seven analytes, including PFOS, PFDS, and perfluorooctanoic acid (PFOA); no trend in two analytes; and increases in two analytes. We argue that PFDS, a long-chained PFC with potential for high bioaccumulation and toxicity, should be considered for future animal and human studies.
Minnesota, Wisconsin↗
Decreased atmospheric sulfur deposition across the southeastern U.S.: When will watersheds release stored sulfate?
Emissions of sulfur dioxide (SO 2 ) to the atmosphere lead to atmospheric deposition of sulfate (SO 4 2- ), which is the dominant strong acid anion causing acidification of surface waters and soils in the eastern United States (U.S.). Since passage of the Clean Air Act and its Amendments, atmospheric deposition of SO 2 in this region has declined by over 80%, but few corresponding decreases in stream-water SO 4 2- concentrations have been observed in unglaciated watersheds. We calculated SO 4 2- mass balances for 27 forested, unglaciated watersheds from Pennsylvania to Georgia, by using total atmospheric deposition (wet plus dry) as input. Many of these watersheds still retain SO 4 2- , unlike their counterparts in the northeastern U.S. and southern Canada. Our analysis showed that many of these watersheds should convert from retaining to releasing SO 4 2- over the next two decades. The specific years when the watersheds crossover from retaining to releasing SO 4 2- correspond to a general geographical pattern of later net watershed release from north to south. The single most important variable that explained the crossover year was the runoff ratio, defined as the ratio of annual mean stream discharge to precipitation. Percent clay content and mean soil depth were secondary factors in predicting crossover year. The conversion of watersheds from net SO 4 2- retention to release anticipates more widespread reductions in stream-water SO 4 2- concentrations in this region.
Environmental Science & Technology↗
Adverse outcome pathway and risks of anticoagulant rodenticides to predatory wildlife
Despite a long history of successful use, routine application of some anticoagulant rodenticides (ARs) may be at a crossroad due to new regulatory guidelines intended to mitigate risk. An adverse outcome pathway for ARs was developed to identify information gaps and end points to assess the effectiveness of regulations. This framework describes chemical properties of ARs, established macromolecular interactions by inhibition of vitamin K epoxide reductase, cellular responses including altered clotting factor processing and coagulopathy, organ level effects such as hemorrhage, organism responses with linkages to reduced fitness and mortality, and potential consequences to predator populations. Risk assessments have led to restrictions affecting use of some second-generation ARs (SGARs) in North America. While the European regulatory community highlighted significant or unacceptable risk of ARs to nontarget wildlife, use of SGARs in most EU member states remains authorized due to public health concerns and the absence of safe alternatives. For purposes of conservation and restoration of island habitats, SGARs remain a mainstay for eradication of invasive species. There are significant data gaps related to exposure pathways, comparative species sensitivity, consequences of sublethal effects, potential hazards of greater AR residues in genetically resistant prey, effects of low-level exposure to multiple rodenticides, and quantitative data on the magnitude of nontarget wildlife mortality.
Environmental Science & Technology↗
Bioaccumulation and toxicity of CuO nanoparticles by a freshwater invertebrate after waterborne and dietborne exposures
The incidental ingestion of engineered nanoparticles (NPs) can be an important route of uptake for aquatic organisms. Yet, knowledge of dietary bioavailability and toxicity of NPs is scarce. Here we used isotopically modified copper oxide ( 65 CuO) NPs to characterize the processes governing their bioaccumulation in a freshwater snail after waterborne and dietborne exposures. Lymnaea stagnalis efficiently accumulated 65 Cu after aqueous and dietary exposures to 65 CuO NPs. Cu assimilation efficiency and feeding rates averaged 83% and 0.61 g g –1 d –1 at low exposure concentrations (<100 nmol g –1 ), and declined by nearly 50% above this concentration. We estimated that 80–90% of the bioaccumulated 65 Cu concentration in L. stagnalis originated from the 65 CuO NPs, suggesting that dissolution had a negligible influence on Cu uptake from the NPs under our experimental conditions. The physiological loss of 65 Cu incorporated into tissues after exposures to 65 CuO NPs was rapid over the first days of depuration and not detectable thereafter. As a result, large Cu body concentrations are expected in L. stagnalis after exposure to CuO NPs. To the degree that there is a link between bioaccumulation and toxicity, dietborne exposures to CuO NPs are likely to elicit adverse effects more readily than waterborne exposures.
Environmental Science & Technology↗
Metamorphosis enhances the effects of metal exposure on the mayfly, Centroptilum triangulifer
The response of larval aquatic insects to stressors such as metals is used to assess the ecological condition of streams worldwide. However, nearly all larval insects metamorphose from aquatic larvae to winged adults, and recent surveys indicate that adults may be a more sensitive indicator of stream metal toxicity than larvae. One hypothesis to explain this pattern is that insects exposed to elevated metal in their larval stages have a reduced ability to successfully complete metamorphosis. To test this hypothesis we exposed late-instar larvae of the mayfly, Centroptilum triangulifer , to an aqueous Zn gradient (32–476 μg/L) in the laboratory. After 6 days of exposure, when metamorphosis began, larval survival was unaffected by zinc. However, Zn reduced wingpad development at concentrations above 139 μg/L. In contrast, emergence of subimagos and imagos tended to decline with any increase in Zn. At Zn concentrations below 105 μg/L (hardness-adjusted aquatic life criterion), survival between the wingpad and subimago stages declined 5-fold across the Zn gradient. These results support the hypothesis that metamorphosis may be a survival bottleneck, particularly in contaminated streams. Thus, death during metamorphosis may be a key mechanism explaining how stream metal contamination can impact terrestrial communities by reducing aquatic insect emergence.
Environmental Science & Technology↗
Fractionation of fulvic acid by iron and aluminum oxides: influence on copper toxicity to Ceriodaphnia dubia
This study examines the effect on aquatic copper toxicity of the chemical fractionation of fulvic acid (FA) that results from its association with iron and aluminum oxyhydroxide precipitates. Fractionated and unfractionated FAs obtained from streamwater and suspended sediment were utilized in acute Cu toxicity tests on ,i>Ceriodaphnia dubia. Toxicity test results with equal FA concentrations (6 mg FA/L) show that the fractionated dissolved FA was 3 times less effective at reducing Cu toxicity (EC 50 13 ± 0.6 μg Cu/L) than were the unfractionated dissolved FAs (EC 50 39 ± 0.4 and 41 ± 1.2 μg Cu/L). The fractionation is a consequence of preferential sorption of molecules having strong metal-binding (more aromatic) moieties to precipitating Fe- and Al-rich oxyhydroxides, causing the remaining dissolved FA to be depleted in these functional groups. As a result, there is more bioavailable dissolved Cu in the water and hence greater potential for Cu toxicity to aquatic organisms. In predicting Cu toxicity, biotic ligand models (BLMs) take into account dissolved organic carbon (DOC) concentration; however, unless DOC characteristics are accounted for, model predictions can underestimate acute Cu toxicity for water containing fractionated dissolved FA. This may have implications for water-quality criteria in systems containing Fe- and Al-rich sediment, and in mined and mineralized areas in particular. Optical measurements, such as specific ultraviolet absorbance at 254 nm (SUVA 254 ), show promise for use as spectral indicators of DOC chemical fractionation and inferred increased Cu toxicity.
Environmental Science & Technology↗
Links between N deposition and nitrate export from a high-elevation watershed in the Colorado Front Range
Long-term patterns of stream nitrate export and atmospheric N deposition were evaluated over three decades in Loch Vale, a high-elevation watershed in the Colorado Front Range. Stream nitrate concentrations increased in the early 1990s, peaked in the mid-2000s, and have since declined by over 40%, coincident with trends in nitrogen oxide emissions over the past decade. Similarities in the timing and magnitude of N deposition provide evidence that stream chemistry is responding to changes in atmospheric deposition. The response to deposition was complicated by a drought in the early 2000s that enhanced N export for several years. Other possible explanations, including forest disturbance, snow depth, or permafrost melting, could not explain patterns in N export. Our results show that stream chemistry responds rapidly to changes in N deposition in high-elevation watersheds, similar to the response observed to changes in sulfur deposition.
Colorado↗
Pesticides in U.S. streams and rivers: occurrence and trends during 1992-2011
During the 20 years from 1992 to 2011, pesticides were found at concentrations that exceeded aquatic-life benchmarks in many rivers and streams that drain agricultural, urban, and mixed-land use watersheds. Overall, the proportions of assessed streams with one or more pesticides that exceeded an aquatic-life benchmark were very similar between the two decades for agricultural (69% during 1992−2001 compared to 61% during 2002−2011) and mixed-land-use streams (45% compared to 46%). Urban streams, in contrast, increased from 53% during 1992−2011 to 90% during 2002−2011, largely because of fipronil and dichlorvos. The potential for adverse effects on aquatic life is likely greater than these results indicate because potentially important pesticide compounds were not included in the assessment. Human-health benchmarks were much less frequently exceeded, and during 2002−2011, only one agricultural stream and no urban or mixed-land-use streams exceeded human-health benchmarks for any of the measured pesticides. Widespread trends in pesticide concentrations, some downward and some upward, occurred in response to shifts in use patterns primarily driven by regulatory changes and introductions of new pesticides.
Environmental Science & Technology↗
Effects of iron on optical properties of dissolved organic matter
Iron is a source of interference in the spectroscopic analysis of dissolved organic matter (DOM); however, its effects on commonly employed ultraviolet and visible (UV–vis) light adsorption and fluorescence measurements are poorly defined. Here, we describe the effects of iron(II) and iron(III) on the UV–vis absorption and fluorescence of solutions containing two DOM fractions and two surface water samples. In each case, regardless of DOM composition, UV–vis absorption increased linearly with increasing iron(III). Correction factors were derived using iron(III) absorption coefficients determined at wavelengths commonly used to characterize DOM. Iron(III) addition increased specific UV absorbances (SUVA) and decreased the absorption ratios ( E 2 : E 3 ) and spectral slope ratios ( S R ) of DOM samples. Both iron(II) and iron(III) quenched DOM fluorescence at pH 6.7. The degree and region of fluorescence quenching varied with the iron:DOC concentration ratio, DOM composition, and pH. Regions of the fluorescence spectra associated with greater DOM conjugation were more susceptible to iron quenching, and DOM fluorescence indices were sensitive to the presence of both forms of iron. Analyses of the excitation–emission matrices using a 7- and 13-component parallel factor analysis (PARAFAC) model showed low PARAFAC sensitivity to iron addition.
Environmental Science & Technology↗
Metamorphosis alters contaminants and chemical tracers in insects: implications for food webs
Insects are integral to most freshwater and terrestrial food webs, but due to their accumulation of environmental pollutants they are also contaminant vectors that threaten reproduction, development, and survival of consumers. Metamorphosis from larvae to adult can cause large chemical changes in insects, altering contaminant concentrations and fractionation of chemical tracers used to establish contaminant biomagnification in food webs, but no framework exists for predicting and managing these effects. We analyzed data from 39 studies of 68 analytes (stable isotopes and contaminants), and found that metamorphosis effects varied greatly. δ 15 N, widely used to estimate relative trophic position in biomagnification studies, was enriched by 1‰ during metamorphosis, while δ 13 C used to estimate diet, was similar in larvae and adults. Metals and polycyclic aromatic hydrocarbons (PAHs) were predominantly lost during metamorphosis leading to 2 to 125-fold higher larval concentrations and higher exposure risks for predators of larvae compared to predators of adults. In contrast, manufactured organic contaminants (such as polychlorinated biphenyls) were retained and concentrated in adults, causing up to 3-fold higher adult concentrations and higher exposure risks to predators of adult insects. Both food web studies and contaminant management and mitigation strategies need to consider how metamorphosis affects the movement of materials between habitats and ecosystems, with special regard for aquatic-terrestrial linkages.
Environmental Science & Technology↗
Bacterial pathogen gene abundance and relation to recreational water quality at seven Great Lakes beaches
Quantitative assessment of bacterial pathogens, their geographic variability, and distribution in various matrices at Great Lakes beaches are limited. Quantitative PCR (qPCR) was used to test for genes from E. coli O157:H7 ( eae O157 ), shiga-toxin producing E. coli ( stx2 ), Campylobacter jejuni ( mapA ), Shigella spp. ( ipaH ), and a Salmonella enterica -specific ( SE ) DNA sequence at seven Great Lakes beaches, in algae, water, and sediment. Overall, detection frequencies were mapA > stx2 > ipaH > SE > eae O157 . Results were highly variable among beaches and matrices; some correlations with environmental conditions were observed for mapA , stx2 , and ipaH detections. Beach seasonal mean mapA abundance in water was correlated with beach seasonal mean log 10 E. coli concentration. At one beach, stx2 gene abundance was positively correlated with concurrent daily E. coli concentrations. Concentration distributions for stx2 , ipaH , and mapA within algae, sediment, and water were statistically different (Non-Detect and Data Analysis in R). Assuming 10, 50, or 100% of gene copies represented viable and presumably infective cells, a quantitative microbial risk assessment tool developed by Michigan State University indicated a moderate probability of illness for Campylobacter jejuni at the study beaches, especially where recreational water quality criteria were exceeded. Pathogen gene quantification may be useful for beach water quality management.
Environmental Science & Technology↗
Mississippi River nitrate loads from high frequency sensor measurements and regression-based load estimation
Accurately quantifying nitrate (NO 3 – ) loading from the Mississippi River is important for predicting summer hypoxia in the Gulf of Mexico and targeting nutrient reduction within the basin. Loads have historically been modeled with regression-based techniques, but recent advances with high frequency NO 3 – sensors allowed us to evaluate model performance relative to measured loads in the lower Mississippi River. Patterns in NO 3 – concentrations and loads were observed at daily to annual time steps, with considerable variability in concentration-discharge relationships over the two year study. Differences were particularly accentuated during the 2012 drought and 2013 flood, which resulted in anomalously high NO 3 – concentrations consistent with a large flush of stored NO 3 – from soil. The comparison between measured loads and modeled loads (LOADEST, Composite Method, WRTDS) showed underestimates of only 3.5% across the entire study period, but much larger differences at shorter time steps. Absolute differences in loads were typically greatest in the spring and early summer critical to Gulf hypoxia formation, with the largest differences (underestimates) for all models during the flood period of 2013. In additional to improving the accuracy and precision of monthly loads, high frequency NO 3 – measurements offer additional benefits not available with regression-based or other load estimation techniques.
Louisiana↗
Using chromate to investigate the impact of natural organics on the surface reactivity of nanoparticulate magnetite
Chromate was used as a chemical probe to investigate the size-dependent influence of organics on nanoparticle surface reactivity. Magnetite–chromate sorption experiments were conducted with ∼90 and ∼6 nm magnetite nanoparticles in the presence and absence of fulvic acid (FA), natural organic matter (NOM), and isolated landfill leachate (LL). Results indicated that low concentrations (1 mg/L) of organics had no noticeable impact on chromate sorption, whereas concentrations of 50 mg/L or more resulted in decreased amounts of chromate sorption. The adsorption of organics onto the magnetite surfaces interfered equally with the ability of the 6 and 90 nm particles to sorb chromate from solution, despite the greater surface area of the smaller particles. Results indicate the presence of organics did not impact the redox chemistry of the magnetite–chromate system over the duration of the experiments (8 h), nor did the organics interact with the chromate in solution. Brunauer–Emmett–Teller (BET) and scanning electron microscopy (SEM) results indicate that the organics blocked the surface reactivity by occupying surface sites on the particles. The similarity of results with FA and NOM suggests that coverage of the reactive mineral surface is the main factor behind the inhibition of surface reactivity in the presence of organics.
Environmental Science & Technology↗