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PFAS river export analysis highlights the urgent need for catchment-scale mass loading data

Source apportionment of per- and polyfluoroalkyl substances (PFAS) requires an understanding of the mass loading of these compounds in river basins. However, there is a lack of temporally variable and catchment-scale mass loading data, meaning identification and prioritization of sources of PFAS to rivers for management interventions can be difficult. Here, we analyze PFAS concentrations and loads in the River Mersey to provide the first temporally robust estimates of PFAS export for a European river system and the first estimates of the contribution of wastewater treatment works (WwTWs) to total river PFAS export. We estimate an annual PFAS export of 68.1 kg for the River Mersey and report that the yield of perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA) in the catchment is among the highest recorded globally. Analysis of river and WwTW loads indicates approximately one-third of PFOA emitted from WwTWs is potentially stored in the catchment and approximately half of PFOS transported by the River Mersey may not originate from WwTWs. As governments move toward regulation of PFAS in WwTW effluents, our findings highlight the complexity of PFAS source apportionment and the need for catchment-scale mass loading data. This study indicates that strategies for reducing PFAS loading that focus solely on WwTW effluents may not achieve river water quality targets.

Environmental Science & Technology Letters

Post-Depositional Behavior of Cu in a Metal-Mining Polishing Pond (East Lake, Canada)

The post-depositional behavior of Cu in a gold-mining polishing pond (East Lake, Canada) was assessed after mine closure by examination of porewater chemistry and mineralogy. The near-surface (upper 1.5 cm) sediments are enriched in Cu, with values ranging from 0.4 to 2 wt %. Mineralogical examination revealed that the bulk of the Cu inventory is present as authigenic copper sulfides. Optical microscopy, energy-dispersion spectra, and X-ray data indicate that the main Cu sulfide is covellite (CuS). The formation of authigenic Cu-S phases is supported by the porewater data, which demonstrate that the sediments are serving as a sink for dissolved Cu below sub-bottom depths of 1-2 cm. The zone of Cu removal is consistent with the occurrence of detectable sulfide and the consumption of sulfate. The sediments can be viewed as a passive bioreactor that permanently removes Cu as insoluble copper sulfides. This process is not unlike that which occurs in other forms of bioremediation, such as wetlands and permeable reactive barriers. Above the zone of Cu removal, dissolved Cu maxima in the interfacial porewaters range from 150 to 450 ??g L-1 and reflect the dissolution of a Cu-bearing phase in the surface sediments. The reactive phase is thought to be a component of treatment sludges delivered to the lake as part of cyanide treatment. Flux calculations indicate that the efflux of dissolved Cu from the sediments to the water column (14-51 ??g cm-2 yr-1) can account for the elevated levels of dissolved Cu in lake waters (???50 ??g L-1). Implications for lake recovery are discussed.

Environmental Science & Technology

Economic and health risk trade-offs of swim closures at a Lake Michigan beach

This paper presents a framework for analyzing the economic, health, and recreation implications of swim closures related to high fecal indicator bacteria (FIB) levels. The framework utilizes benefit transfer policy analysis to provide a practical procedure for estimating the effectiveness of recreational water quality policies. Evaluation criteria include the rates of intended and unintended management outcomes, whether the chosen protocols generate closures with positive net economic benefits to swimmers, and the number of predicted illnesses the policy is able to prevent. We demonstrate the framework through a case study of a Lake Michigan freshwater beach using existing water quality and visitor data from 1998 to 2001. We find that a typical closure causes a net economic loss among would-be swimmers totaling $1274-37 030/ day, depending on the value assumptions used. Unnecessary closures, caused by high indicator variability and a 24-h time delay between when samples are taken and the management decision can be made, occurred on 14 (12%) out of 118 monitored summer days. Days with high FIB levels when the swim area is open are also common but do relatively little economic harm in comparison. Also, even if the closure policy could be implemented daily and perfectly without error, only about 42% of predicted illnesses would be avoided. These conclusions were sensitive to the relative values and risk preferences that swimmers have for recreation access and avoiding health effects, suggesting a need for further study of the impacts of recreational water quality policies on individuals.

Environmental Science & Technology

Coastal loading and transport of Escherichia coli at an embayed beach in Lake Michigan

A Chicago beach in southwest Lake Michigan was revisited to determine the influence of nearshore hydrodynamic effects on the variability of Escherichia coli (E. coli) concentration in both knee-deep and offshore waters. Explanatory variables that could be used for identifying potential bacteria loading mechanisms, such as bed shear stress due to a combined wave-current boundary layer and wave runup on the beach surface, were derived from an existing wave and current database. The derived hydrodynamic variables, along with the actual observed E. coli concentrations in the submerged and foreshore sands, were expected to reveal bacteria loading through nearshore sediment resuspension and swash on the beach surface, respectively. Based on the observation that onshore waves tend to result in a more active hydrodynamic system at this embayed beach, multiple linear regression analysis of onshore-wave cases further indicated the significance of sediment resuspension and the interaction of swash with gull-droppings in explaining the variability of E. coli concentration in the knee-deep water. For cases with longshore currents, numerical simulations using the Princeton Ocean Model revealed current circulation patterns inside the embayment, which can effectively entrain bacteria from the swash zone into the central area of the embayed beach water and eventually release them out of the embayment. The embayed circulation patterns are consistent with the statistical results that identified that 1) the submerged sediment was an additional net source of E. coli to the offshore water and 2) variability of E. coli concentration in the knee-deep water contributed adversely to that in the offshore water for longshore-current cases. The embayed beach setting and the statistical and numerical methods used in the present study have wide applicability for analyzing recreational water quality at similar marine and freshwater sites. ?? 2010 American Chemical Society.

Environmental Science & Technology

Factors associated with sources, transport, and fate of chloroform and three other trihalomethanes in untreated groundwater used for drinking water

Multiple lines of evidence for indicating factors associated with the sources, transport, and fate of chloroform and three other trihalomethanes (THMs) in untreated groundwater were revealed by evaluating low-level analytical results and logistic regression results for THMs. Samples of untreated groundwater from wells used for drinking water were collected from 1996-2007 from 2492 wells across the United States and analyzed for chloroform, bromodichloromethane, dibromochloromethane, and bromoform by a low-level analytical method implemented in April 1996. Using an assessment level of 0.02 μg/L, chloroform was detected in 36.5% of public-well samples and 17.6% of domestic-well samples, with most concentrations less than 1 μg/L. Brominated THMs occurred less frequently than chloroform but more frequently in public-well samples than domestic-well samples. For both public and domestic wells, THMs occurred most frequently in urban areas. Logistic regression analyses showed that the occurrence of THMs was related to nonpoint sources such as urban land use and to point sources like septic systems. The frequent occurrence and concentration distribution pattern of THMs, as well as their frequent co-occurrence with other organic compounds and nitrate, all known to have anthropogenic sources, and the positive associations between THM occurrence and dissolved oxygen and recharge indicate the recycling of water that contains THMs and other anthropogenic contaminants.

Environmental Science & Technology

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

Mobilization and transport of soil particles during infiltration experiments in an agricultural field, Shenandoah Valley, Virginia

Evidence that fine particles mobilized and transported in soils and aquifers can have a profound influence on contaminant migration has spawned much interest recently in understanding colloid transport in natural materials. Repeated infiltration experiments on an initially dry field soil were conducted to evaluate rates of mobilization of fine particles over time and to investigate the importance of transient-flow events on particle transport. Water flow was measured in zero-tension lysimeters at 25 cm depth. For repeated infiltration events and for all plots, water flow sharply increased shortly after initial ponding of water at the soil surface, maintained a relatively steady level during the period of ponding, and decreased gradually thereafter. Particle concentrations measured in the pan lysimeters ranged from 7 mg L - 1 to 265 mg L - 1 and were typically on the order of 10 to 100 mg L - 1 . Greatest particle mass flux was observed during the initial infiltration experiment on each plot. During four subsequent infiltration experiments, all conducted within 250 min of the first event, steady mass fluxes were observed that were approximately 70% of the average value seen in the first flush of water through a dry soil, indicating that the supply of mobile soil particles is only sparingly reduced over closely spaced infiltration events. All peak particle concentrations and mass fluxes occurred near either the rising limb or the falling limb of the water flux hydrograph, presumably reflecting the movement of air−water interfaces during imbibition and drainage.

Virginia

Reach-scale monitoring and modeling of rivers--Expanding hydraulic data collection beyond the cross section

For over 125 years, the U.S. Geological Survey streamgage network has provided important hydrologic information about rivers and streams throughout the Nation. Traditional streamgage methods provide reliable stage and streamflow data but typically only monitor stage at a single location in a river and require frequent calibration streamflow measurements. Direct measurements are not always feasible, therefore improved sensors and methods are being deployed at gages to better document streamflow conditions between measurements. The technology and techniques of reach-scale monitoring allow the U.S. Geological Survey to collect more data across the full range of streamflow without requiring that a hydrographer be present. The U.S. Geological Survey Arizona Water Science Center’s reach-scale monitoring program will enhance the Arizona streamgage network with more accurate streamflow measurements and provide more extensive streamflow records and geomorphological datasets for our agency partners and the public. Reach-scale monitoring installations and techniques are applicable to streams of the western United States and likely throughout the Nation.

Arizona

Methane emissions from artificial waterbodies dominate the carbon footprint of irrigation: A study of transitions in the food-energy-water-climate nexus (Spain, 1900-2014)

Irrigation in the Mediterranean region has been used for millennia and has greatly expanded with industrialization. Irrigation is critical for climate change adaptation, but it is also an important source of greenhouse gas emissions. This study analyzes the carbon (C) footprint of irrigation in Spain, covering the complete historical process of mechanization. A 21-fold total, 6-fold area-based, and 4-fold product-based increase in the carbon footprint was observed during the 20th century, despite an increase in water use efficiency. CH 4 emissions from waterbodies, which had not previously been considered in the C footprint of irrigation systems, dominated the emission budget during most of the analyzed period. Technologies to save water and tap new water resources greatly increased energy and infrastructure demand, while improvements in power generation efficiency had a limited influence on irrigation emissions. Electricity production from irrigation dams may contribute to climate change mitigation, but the amount produced in relation to that consumed in irrigation has greatly declined. High uncertainty in CH 4 emission estimates from waterbodies stresses a need for more spatially resolved data and an improved empirical knowledge of the links between water quality, water level fluctuations, and emissions at the regional scale.

Environmental Science & Technology

Clarence Allen talks about the responsibilities in earthquake prediction

Dr. Clarence R. Allen is professor of geology and geophysics at the California Institute of Technology. He has been a member of advisory panels to the Executive Office of the President, National Academy of Sciences, National Science Foundation, U.S Geological Survey, UNESCO, California State Mining and Geology Board, and the California Department of Water Resources. Dr. Allen has been President of both the Geological Society of America and the Seismological Society of America (SSA). The title of this interview is based on his presidential address to the SSA in 1976.

Earthquake Information Bulletin (USGS)

Differences in neonicotinoid and metabolite sorption to activated carbon are driven by alterations to the insecticidal pharmacophore

Widespread application of neonicotinoids has led to their proliferation in waters. Despite low neonicotinoid hydrophobicity, our prior studies implicated granular activated carbon (GAC) in neonicotinoid removal. Based on known receptor binding characteristics, we hypothesized that the insecticidal pharmacophore influences neonicotinoid sorption. Our objectives were to illuminate drivers of neonicotinoid sorption for parent neonicotinoids (imidacloprid, clothianidin, thiamethoxam, and thiacloprid) and pharmacophore-altered metabolites (desnitro-imidacloprid and imidacloprid urea) to GAC, powdered activated carbon, and carbon nanotubes (CNTs). Neonicotinoid sorption to GAC was extensive and largely irreversible, with significantly greater sorption of imidacloprid than desnitro-imidacloprid. Imidacloprid and imidacloprid urea (electronegative pharmacophores) sorbed most extensively to nonfunctionalized CNTs, whereas desnitro-imidacloprid (positive pharmacophore) sorbed most to COOH-CNTs, indicating the importance of charge interactions and/or hydrogen bonding between the pharmacophore and carbon surface. Water chemistry parameters (temperature, alkalinity, ionic strength, and humic acid) inhibited overall neonicotinoid sorption, suggesting that pharmacophore-driven sorption in real waters may be diminished. Analysis of a full-scale drinking water treatment plant GAC filter influent, effluent, and spent GAC attributes neonicotinoid/metabolite removal to GAC under real-world conditions for the first time. Our results demonstrate that the neonicotinoid pharmacophore not only confers insecticide selectivity but also impacts sorption behavior, leading to less effective removal of metabolites by GAC filters in water treatment.

Environmental Science and Technology

Vertical distribution of microplastics in the water column and surficial sediment from the Milwaukee River basin to Lake Michigan

Microplastic contamination was studied along a freshwater continuum from inland streams to the Milwaukee River estuary to Lake Michigan, and vertically from the water surface, water subsurface and sediment. Microplastics were detected in all 96 water samples and nine sediment samples collected. Results indicated a gradient of polymer presence with depth: low-density particles decreased from water surface to subsurface to sediment, and high-density particles had the opposite result. Polymer identification results indicated water surface and subsurface samples were dominated by low-density polypropylene particles and sediment samples were dominated by more dense polyethylene terephthalate particles. Of the five particle-type categories (fragments, films, foams, pellets/beads and fibers/lines), fibers/lines were the most common particle type and were present in every water and sediment sample collected. Fibers represented 45% of all particles in water samples and were distributed vertically throughout the water column regardless of density. Sediment samples were dominated by black foams (66%, identified as styrene-butadiene rubber, SBR) and to a lesser extent fibers/lines (29%) with approximately 89% of all the sediment particles coming from polymers with densities greater than 1.1 g cm-3. Results demonstrated polymer density influenced partitioning between water surface and subsurface and the underlying surficial sediment and the common practice of sampling only the water surface can result in substantial bias, especially in estuarine, harbor and lake locations where water surface concentrations tend to overestimate mean water column concentrations.

Wisconsin

Measurement of in situ rates of selenate removal by dissimilatory bacterial reduction in sediments

A radioisotope method for measurement of bacteria respiratory reduction of selenate to elemental selenium in aquatic sediments was devised. Sediments were labeled with [75Se]selenate, incubated, and washed, and 75Se0(s) was determined as counts remaining in the sediments. Core profiles of selenate reduction, sulfate reduction, and denitrification were made simultaneously in the sediments of an agricultural wastewater evaporation pond. Most of the in situ selenate reduction (85%) and all the denitrificatation activities were confined to the upper 4-8 cm of the profile, whereas sulfate reduction was greatest below 8 cm (89% of total). The integrated areal rate of selenate reduction was 301 mol m-2 day-1, which results in a turnover of water column selenate in 82.4 days.

Environmental Science & Technology

Spectroscopic evidence for uranium bearing precipitates in vadose zone sediments at the Hanford 300-area site

Uranium (U) solid-state speciation in vadose zone sediments collected beneath the former North Process Pond (NPP) in the 300 Area of the Hanford site (Washington) was investigated using multi-scale techniques. In 30 day batch experiments, only a small fraction of total U (???7.4%) was released to artificial groundwater solutions equilibrated with 1% pCO2. Synchrotron-based micro-X-ray fluorescence spectroscopy analyses showed that U was distributed among at least two types of species: (i) U discrete grains associated with Cu and (ii) areas with intermediate U concentrations on grains and grain coatings. Metatorbernite (Cu[UO2]2[PO 4]2??8H2O) and uranophane (Ca[UO 2]2[SiO3(OH)]2?? 5H 2O) at some U discrete grains, and muscovite at U intermediate concentration areas, were identified in synchrotron-based micro-X-ray diffraction. Scanning electron microscopy/energy dispersive X-ray analyses revealed 8-10 ??m size metatorbernite particles that were embedded in C-, Al-, and Si-rich coatings on quartz and albite grains. In ??- and bulk-X-ray absorption structure (??-XAS and XAS) spectroscopy analyses, the structure of metatorbernite with additional U-C and U-U coordination environments was consistently observed at U discrete grains with high U concentrations. The consistency of the ??- and bulk-XAS analyses suggests that metatorbernite may comprise a significant fraction of the total U in the sample. The entrapped, micrometer-sized metatorbernite particles in C-, Al-, and Si-rich coatings, along with the more soluble precipitated uranyl carbonates and uranophane, likely control the long-term release of U to water associated with the vadose zone sediments. ?? 2007 American Chemical Society.

Environmental Science & Technology

Occurrence of neonicotinoid insecticides in finished drinking water and fate during drinking water treatment

Neonicotinoid insecticides are widespread in surface waters across the agriculturally-intensive Midwestern US. We report for the first time the presence of three neonicotinoids in finished drinking water and demonstrate their general persistence during conventional water treatment. Periodic tap water grab samples were collected at the University of Iowa over seven weeks in 2016 (May-July) after maize/soy planting. Clothianidin, imidacloprid, and thiamethoxam were ubiquitously detected in finished water samples and ranged from 0.24-57.3 ng/L. Samples collected along the University of Iowa treatment train indicate no apparent removal of clothianidin and imidacloprid, with modest thiamethoxam removal (~50%). In contrast, the concentrations of all neonicotinoids were substantially lower in the Iowa City treatment facility finished water using granular activated carbon (GAC) filtration. Batch experiments investigated potential losses. Thiamethoxam losses are due to base-catalyzed hydrolysis at high pH conditions during lime softening. GAC rapidly and nearly completely removed all three neonicotinoids. Clothianidin is susceptible to reaction with free chlorine and may undergo at least partial transformation during chlorination. Our work provides new insights into the persistence of neonicotinoids and their potential for transformation during water treatment and distribution, while also identifying GAC as an effective management tool to lower neonicotinoid concentrations in finished drinking water.

Environmental Science & Technology Letters

Nature and chlorine reactivity of organic constituents from reclaimed water in groundwater, Los Angeles County, California

The nature and chlorine reactivity of organic constituents in reclaimed water (tertiary-treated municipal wastewater) before, during, and after recharge into groundwater at the Montebello Forebay in Los Angeles County, CA, was the focus of this study. Dissolved organic matter (DOM) in reclaimed water from this site is primarily a mixture of aromatic sulfonates from anionic surfactant degradation, N-acetyl amino sugars and proteins from bacterial activity, and natural fulvic acid, whereas DOM from native groundwaters in the aquifer to which reclaimed water was recharged consists of natural fulvic acids. The hydrophilic neutral N-acetyl amino sugars that constitute 40% of the DOM in reclaimed water are removed during the first 3 m of vertical infiltration in the recharge basin. Groundwater age dating with 3H and 3He isotopes, and determinations of organic and inorganic C isotopes, enabled clear differentiation of recent recharged water from older native groundwater. Phenol structures in natural fulvic acids in DOM isolated from groundwater produced significant trihalomethanes (THM) and total organic halogen (TOX) yields upon chlorination, and these structures also were responsible for the enhanced SUVA and specific fluorescence characteristics relative to DOM in reclaimed water. Aromatic sulfonates and fulvic acids in reclaimed water DOM produced minimal THM and TOX yields.

California

Isotopically modified nanoparticles for enhanced detection in bioaccumulation studies

This work presents results on synthesis of isotopically enriched (99% 65 Cu) copper oxide nanoparticles and its application in ecotoxicological studies. 65 CuO nanoparticles were synthesized as spheres (7 nm) and rods (7 × 40 nm). Significant differences were observed between the reactivity and dissolution of spherical and rod shaped nanoparticles. The extreme sensitivity of the stable isotope tracing technique developed in this study allowed determining Cu uptake at exposure concentrations equivalent to background Cu concentrations in freshwater systems (0.2–30 μg/L). Without a tracer, detection of newly accumulated Cu was impossible, even at exposure concentrations surpassing some of the most contaminated water systems (>1 mg/L).

Environmental Science & Technology

Methods of practice and guidelines for using survey-grade global navigation satellite systems (GNSS) to establish vertical datum in the United States Geological Survey

Geodetic surveys have evolved through the years to the use of survey-grade (centimeter level) global positioning to perpetuate and post-process vertical datum. The U.S. Geological Survey (USGS) uses Global Navigation Satellite Systems (GNSS) technology to monitor natural hazards, ensure geospatial control for climate and land use change, and gather data necessary for investigative studies related to water, the environment, energy, and ecosystems. Vertical datum is fundamental to a variety of these integrated earth sciences. Essentially GNSS surveys provide a three-dimensional position x, y, and z as a function of the North American Datum of 1983 ellipsoid and the most current hybrid geoid model. A GNSS survey may be approached with post-processed positioning for static observations related to a single point or network, or involve real-time corrections to provide positioning "on-the-fly." Field equipment required to facilitate GNSS surveys range from a single receiver, with a power source for static positioning, to an additional receiver or network communicated by radio or cellular for real-time positioning. A real-time approach in its most common form may be described as a roving receiver augmented by a single-base station receiver, known as a single-base real-time (RT) survey. More efficient real-time methods involving a Real-Time Network (RTN) permit the use of only one roving receiver that is augmented to a network of fixed receivers commonly known as Continually Operating Reference Stations (CORS). A post-processed approach in its most common form involves static data collection at a single point. Data are most commonly post-processed through a universally accepted utility maintained by the National Geodetic Survey (NGS), known as the Online Position User Service (OPUS). More complex post-processed methods involve static observations among a network of additional receivers collecting static data at known benchmarks. Both classifications provide users flexibility regarding efficiency and quality of data collection. Quality assurance of survey-grade global positioning is often overlooked or not understood and perceived uncertainties can be misleading. GNSS users can benefit from a blueprint of data collection standards used to ensure consistency among USGS mission areas. A classification of GNSS survey qualities provide the user with the ability to choose from the highest quality survey used to establish objective points with low uncertainties, identified as a Level I, to a GNSS survey for general topographic control without quality assurance, identified as a Level IV. A Level I survey is strictly limited to post-processed methods, whereas Level II, Level III, and Level IV surveys integrate variations of a RT approach. Among these classifications, techniques involving blunder checks and redundancy are important, and planning that involves the assessment of the overall satellite configuration, as well as terrestrial and space weather, are necessary to ensure an efficient and quality campaign. Although quality indicators and uncertainties are identified in post-processed methods using CORS, the accuracy of a GNSS survey is most effectively expressed as a comparison to a local benchmark that has a high degree of confidence. Real-time and post-processed methods should incorporate these "trusted" benchmarks as a check during any campaign. Global positioning surveys are expected to change rapidly in the future. The expansion of continuously operating reference stations, combined with newly available satellite signals, and enhancements to the conterminous geoid, are all sufficient indicators for substantial growth in real-time positioning and quality thereof.

Techniques and Methods