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Using a time-of-travel sampling approach to quantify per- and polyfluoroalkyl substances (PFAS) stream loading and source inputs in a mixed-source, urban catchment

Understanding per- and polyfluoroalkyl substances (PFAS) mass distribution in surface and groundwater systems can support source prioritization, load reduction, and water management. Thirteen sites within an urban catchment were sampled utilizing a time-of-travel sampling approach to minimize the influence of subdaily fluctuations in mass from PFAS point sources and to quantify PFAS and ancillary chemical loads from various PFAS sources. A larger increase in perfluoroalkyl sulfonate (PFSA) loads (8 to 11 μg/s, up to 618%) than in perfluoroalkyl carboxylate (PFCA) loads (no change to 3.4 μg/s, up to 122%) was observed at sites below tributaries influenced by military bases with known groundwater discharge. Point discharges from two sewage treatment plants (STPs) resulted in increases in PFCA and PFSA loads that were similar (6 and 10 μg/s respectively) below the first STP and greater for PFCA compared to PFSA loads (23 and 13 μg/s respectively) below the second STP. Overall, percent increases in total PFAS load ranged from 20 to 277% for military base inputs and 44 to 77% for STP inputs. A focus catchment that represents only 14% (76.9 km 2 ) of the drainage area at the most downstream site (544 km 2 ) accounted for about 70% of PFSA and 40% of PFCA loads observed at the most downstream site. Results show that by using a time-of-travel sampling approach in mixed, urban settings with several PFAS sources, it is possible to quantify stream loads from individual PFAS sources, thereby improving source attribution and providing actionable data for water-resource managers.

ACS ES&T Water↗

Naegleria fowleri detected in Grand Teton National Park hot springs

The free-living thermophilic amoeba Naegleria fowleri ( N. fowleri ) causes the highly fatal disease primary amoebic meningoencephalitis. The environmental conditions that are favorable to the growth and proliferation of N. fowleri are not well-defined, especially in northern regions of the United States. In this study, we used culture-based methods and multiple molecular approaches to detect and analyze N. fowleri and other Naegleria spp. in water, sediment, and biofilm samples from five hot spring sites in Grand Teton National Park, Wyoming, U.S.A. These results provide the first detections of N. fowleri in Grand Teton National Park and provide new insights into the distribution of pathogenic N. fowleri and other nonpathogenic Naegleria spp. in natural thermal water systems in northern latitudes.

Wyoming↗

Detection of Naegleria fowleri in thermally impacted recreational waters of western United States national parks

Naegleria fowleri is a thermophilic free-living amoeba (FLA) and the causative agent of primary amoebic meningoencephalitis, posing public health risks in warm freshwater environments. This multiyear, multiagency study surveyed 40 thermally impacted recreational waters across five western United States national parks and recreation areas–Yellowstone National Park, Grand Teton National Park, Olympic National Park, Newberry National Volcanic Monument, and Lake Mead National Recreation Area–to assess N. fowleri presence, concentration, and associated environmental conditions. A total of 185 water samples were analyzed by qPCR and Sanger sequencing, revealing widespread detection of N. fowleri in 34% of samples with positive detections from Lake Mead, Yellowstone, and Grand Teton hot springs and thermally impacted waters, with concentrations ranging from 4.9 to 115.7 cells/L. Multiple codetections of N. fowleri with nonpathogenic species including Naegleria australiensis were identified, suggesting they may inhabit similar ecological niches in the natural systems in contrast to engineered systems. These findings indicate that N. fowleri is present in thermally impacted areas across the western United States and underscore the use of enhanced monitoring, public awareness, and risk management strategies in thermally influenced recreational waters.

Arizona, Nevada, Oregon, Washington, Wyoming↗

Concentration dependency of PFOS bioaccumulation by freshwater benthic algae

Although perfluorooctanesulfonic acid (PFOS) has been voluntarily phased out, it remains the most abundant and frequently detected PFAS compound in biota worldwide. A deeper understanding of how PFOS enters the aquatic food web at the energetic base is needed to better characterize and predict the general patterns of PFAS trophic transfer. Research on bioaccumulation by primary producers remains limited. Because diatoms (Bacillariophyta) are often dominant constituents of aquatic biofilms, we exposed freshwater benthic diatoms ( Mayamaea atomus ) to a range of PFOS concentrations (0.01–100 μg/L) for 7 days in a controlled laboratory experiment to investigate PFAS bioaccumulation patterns. We quantified PFOS in water and algal matrices using liquid chromatography-tandem mass spectrometry and calculated bioconcentration factors (BCFs). Log PFOS concentrations in diatoms increased linearly with log 10 exposure concentration, corresponding to a sublinear relationship in arithmetic space. Consequently, BCF values decreased, from 4,831 to 174 L/kg, with increasing PFOS exposure, indicating concentration-dependent bioaccumulation consistent with higher-order organisms (e.g., Crustacea, Mollusca, Chordata). This pattern complicates the use of BCF for predictive purposes and may lead to mis-estimations of risk. Even as PFOS declines in the environment, algae will likely continue to accumulate and transfer PFOS and other PFAS to higher trophic levels.

ACS ES&T Water↗

Metal release from manganese nodules in anoxic seawater and implications for deep-sea mining dewatering operations

The potential mining of deep-sea polymetallic nodules has been gaining increasing attention due to their enrichment in metals essential for a low-carbon future. To date, there have been few scientific studies concerning the geochemical consequences of dewatered mining waste discharge into the pelagic water column, which can inform best practices in future mining operations. Here, we report the results of laboratory incubation experiments that simulate mining discharge into anoxic waters such as those that overlie potential mining sites in the North Pacific Ocean. We find that manganese nodules are reductively dissolved, with an apparent activation energy of 42.8 kJ mol –1 , leading to the release of associated metals in the order manganese > nickel > copper > cobalt > cadmium > lead. The composition of trace metals released during the incubation allows us to estimate a likely trace metal budget from the simulated dewatering waste plume. These estimates suggest that released cobalt and copper are the most enriched trace metals within the plume, up to ∼15 times more elevated than the background seawater. High copper concentrations can be toxic to marine organisms. Future work on metal toxicity to mesopelagic communities could help us better understand the ecological effects of these fluxes of trace metals.

ACS ES&T Water↗

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

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

Wisconsin↗

A universal method for the simultaneous determination of environmental pollutants in marine biological samples: Per- and polyfluoroalkyl substances and antibiotics as a case study

Conventional detection technologies for environmental contaminants have primarily focused on providing accurate qualitative and quantitative evaluations for single pollutant types, leading to increased costs and an inability to satisfy the growing demand for detecting a broader spectrum of pollutants. Here, we introduced a novel analytical method to simultaneously measure the concentration levels of diverse environmental pollutants, characterized by their distinct properties, across complex biological samples. Per- and polyfluoroalkyl substances (PFAS) and antibiotics were used as a case study due to their frequency of detection in the environment and known impacts Our method harnesses the salting-out effect of sodium chloride on proteins within the muscle tissues of 178 marine species, which significantly reduces the addition of extraneous substances, mitigates matrix interference, and avoids reliance on solid-phase extraction or dispersive extraction agents. The method provides a simultaneous pretreatment for the detection of several compounds, with detection limits from 0.002 to 0.41 ng/g dry weight, which are substantially lower than conventional methods. Overall, this method streamlines efficiency, decreases costs, lessens matrix effects, and sets a solid groundwork for future applications in the concurrent detection of a broader spectrum of environmentally pertinent pollutants with varied characteristics.

ACS ES&T Water↗

From transcriptomic dysregulation to behavioral impairment: Mechanistic effects of weathered Brazilian oil on early life stage fish

The 2019–2020 oil spill along the northeastern coast of Brazil affected coastal reef ecosystems and the organisms that inhabit these environments. To characterize the toxicity of persistent weathered oil residues to early life stage fish, embryonic zebrafish ( Danio rerio ) were exposed to environmentally relevant concentrations of a water-accommodated fraction (WAF) prepared from weathered oil recovered following the spill. Embryos were exposed from 24 to 168 h postfertilization (hpf) to low (2.14 μg ∑PAH 60 L –1 ) and high (17.1 μg ∑PAH 60 L –1 ) concentrations representative of chronic postspill exposure conditions. Transcriptomic profiling revealed early alterations in pathways associated with connective tissue, cardiovascular, and respiratory development at 48 hpf, which corresponded with a significant reduction in heart rate at 72 hpf. By 96 and 168 hpf, molecular responses shifted toward visual system dysfunction, including pathways related to photoreceptor development and phototransduction. Histological evaluation confirmed significant thinning of retinal layers, consistent with impaired retinal development or photoreceptor degeneration. These structural changes translated to functional impairment, as larvae exhibited a 40% reduction in optokinetic response. These integrated analyses identify mechanistic targets of weathered oil toxicity and establish molecular to behavioral relationships that improve understanding of chronic oil spill impacts on early life stage fish.

Pernambuco↗