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Paul M. Bradley

Publications and source records attributed to Paul M. Bradley.

At least 55 records · Page 3Linked to original sources

Public and private tapwater: Comparative analysis of contaminant exposure and potential risk, Cape Cod, Massachusetts, USA

Background Humans are primary drivers of environmental contamination worldwide, including in drinking-water resources. In the United States (US), federal and state agencies regulate and monitor public-supply drinking water while private-supply monitoring is rare; the current lack of directly comparable information on contaminant-mixture exposures and risks between private- and public-supplies undermines tapwater (TW) consumer decision-making. Methods We compared private- and public-supply residential point-of-use TW at Cape Cod, Massachusetts, where both supplies share the same groundwater source. TW from 10 private- and 10 public-supply homes was analyzed for 487 organic, 38 inorganic, 8 microbial indicators, and 3 in vitro bioactivities. Concentrations were compared to existing protective health-based benchmarks, and aggregated Hazard Indices (HI) of regulated and unregulated TW contaminants were calculated along with ratios of in vitro exposure-activity cutoffs. Results Seventy organic and 28 inorganic constituents were detected in TW. Median detections were comparable, but median cumulative concentrations were substantially higher in public supply due to 6 chlorine–disinfected samples characterized by disinfection byproducts and corresponding lower heterotrophic plate counts. Public-supply applicable maximum contaminant (nitrate) and treatment action (lead and copper) levels were exceeded in private-supply TW samples only. Exceedances of health-based HI screening levels of concern were common to both TW supplies. Discussion These Cape Cod results indicate comparable cumulative human-health concerns from contaminant exposures in private- and public-supply TW in a shared source-water setting. Importantly, although this study’s analytical coverage exceeds that currently feasible for water purveyors or homeowners, it nevertheless is a substantial underestimation of the full breadth of contaminant mixtures documented in the environment and potentially present in drinking water. Conclusion Regardless of the supply, increased public engagement in source-water protection and drinking-water treatment, including consumer point-of-use treatment, is warranted to reduce risks associated with long-term TW contaminant exposures, especially in vulnerable populations.

Massachusetts↗

Assessing the ecological functionality and integrity of natural ponds, excavated ponds and stormwater basins for conserving amphibian diversity

Wetlands provide ecological functionality by maintaining and promoting regional biodiversity supporting quality habitat for aquatic organisms. Globally, habitat loss, fragmentation and degradation due to increases in agricultural activities and urban development have reduced or altered geographically isolated wetlands, thus reducing biodiversity. The objective of this study was to assess the relative ecological function and integrity of natural ponds, excavated ponds and stormwater basins in the New Jersey Pinelands, located in the northeastern United States by comparing hydrologic conditions, water quality, pesticide concentrations (water, sediment and tissue) and wetland assemblages including amphibians. Twenty-four wetlands were selected based on surrounding land-use and sampled for a variety of abiotic and biotic variables. Abiotic and biotic wetland variables were similar between natural and excavated ponds, with notable differences between the ponds and stormwater basins. Natural and excavated ponds displayed characteristic Pinelands water quality (low pH, high organic carbon, and low pesticide concentrations), exhibited high ecological integrity and supported native ampbibians. Stormwater basins and degraded ponds surrounded by altered land-use exhibited degraded water quality (high pH, high pesticide concentrations) and were dominated by non-native and introduced plants and amphibians. Results from this study can broadly inform resource conservation strategies for amphibians and other communities with a diverse range of habitat requirements, particularly in areas where conservation and development are competing priorities. To conserve biodiversity in changing landscapes, wetlands with similar functionality and land-use characteristics need to be identified and managed to preserve water quality for species of conservation concern.

New Jersey↗

In vitro effects-based method and water quality screening model for use in pre- and post-distribution treated waters

Recent urban public water supply contamination events emphasize the importance of screening treated drinking water quality after distribution. In vitro bioassays, when run concurrently with analytical chemistry methods, are effective tools to evaluating the efficacy of water treatment processes and water quality. We tested 49 water samples representing the Chicago Department of Water Management service areas for estrogen, (anti)androgen, glucocorticoid receptor-activating contaminants and cytotoxicity. We present a tiered screening approach suitable to samples with anticipated low-level activity and initially tested all extracts for statistically identifiable endocrine activity; performing a secondary dilution-response analysis to determine sample EC 50 and biological equivalency values (BioEq). Estrogenic activity was detected in untreated Lake Michigan intake water samples using mammalian (5/49; median: 0.21 ng E2Eq/L) and yeast cell (5/49; 1.78 ng E2Eq/L) bioassays. A highly sensitive (anti)androgenic activity bioassay was applied for the first time to water quality screening and androgenic activity was detected in untreated intake and treated pre-distribution samples (4/49; 0.93 ng DHTEq/L). No activity was identified above method detection limits in the yeast androgenic, mammalian anti-androgenic, and both glucocorticoid bioassays. Known estrogen receptor agonists were detected using HPLC/MS-MS (estrone: 0.72-1.4 ng/L; 17α-estradiol: 1.3-1.5 ng/L; 17β-estradiol: 1.4 ng/L; equol: 8.8 ng/L), however occurrence did not correlate with estrogenic bioassay results. Many studies have applied bioassays to water quality monitoring using only relatively small samples sets often collected from surface and/or wastewater effluent. However, to realistically adapt these tools to treated water quality monitoring, water quality managers must have the capacity to screen potentially hundreds of samples in short timeframes. Therefore, we provided a tiered screening model that increased sample screening speed, without sacrificing statistical stringency, and detected estrogenic and androgenic activity only in pre-distribution Chicago area samples.

Illinois, Indiana↗

Multi-region assessment of chemical mixture exposures and predicted cumulative effects in USA wadeable urban/agriculture-gradient streams

Chemical-contaminant mixtures are widely reported in large stream reaches in urban/agriculture-developed watersheds, but mixture compositions and aggregate biological effects are less well understood in corresponding smaller headwaters , which comprise most of stream length, riparian connectivity, and spatial biodiversity. During 2014–2017, the U.S. Geological Survey (USGS) measured 389 unique organic analytes (pharmaceutical, pesticide, organic wastewater indicators) in 305 headwater streams within four contiguous United States (US) regions. Potential aquatic biological effects were evaluated for estimated maximum and median exposure conditions using multiple lines of evidence, including occurrence/concentrations of designed-bioactive pesticides and pharmaceuticals and cumulative risk screening based on vertebrate-centric ToxCast™ exposure-response data and on invertebrate and nonvascular plant aquatic life benchmarks. Mixed-contaminant exposures were ubiquitous and varied, with 78% (304) of analytes detected at least once and cumulative maximum concentrations up to more than 156,000 ng/L. Designed bioactives represented 83% of detected analytes. Contaminant summary metrics correlated strong-positive (rho (ρ): 0.569–0.719) to multiple watershed-development metrics, only weak-positive to point-source discharges (ρ: 0.225–353), and moderate- to strong-negative with multiple instream invertebrate metrics (ρ: −0.373 to −0.652). Risk screening indicated common exposures with high probability of vertebrate-centric molecular effects and of acute toxicity to invertebrates, respectively. The results confirm exposures to broad and diverse contaminant mixtures and provide convincing multiple lines of evidence that chemical contaminants contribute substantially to adverse multi-stressor effects in headwater-stream communities.

Science of the Total Environment↗

Reconnaissance of cumulative risk of pesticides and pharmaceuticals in Great Smoky Mountains National Park streams

The United States (US) National Park Service (NPS) manages protected public lands to preserve biodiversity. Exposure to and effects of bioactive organic contaminants in NPS streams are challenges for resource managers. Recent assessment of pesticides and pharmaceuticals in protected-streams within the urbanized NPS Southeast Region (SER) indicated the importance of fluvial inflows from external sources as drivers of aquatic contaminant-mixture exposures. Great Smoky Mountains National Park (GRSM), lies within SER, has the highest biodiversity and annual visitation of NPS parks, but, in contrast to the previously studied systems, straddles a high-elevation hydrologic divide; this setting limits fluvial-inflows of contaminants but potentially increases visitation-driven contaminant deliveries. We leveraged the unique characteristics of GRSM to test further the importance of fluvial contaminant inflows as drivers of protected-stream exposures and to inform the relative importance of potential additional contaminant transport mechanisms, by comparing the estimated risks of 328 pesticides and pharmaceuticals in water at 16 GRSM stream locations to those estimated previously in SER streams. Extensive mixtures (31 compounds) were only observed in an atypical reach on the boundary of GRSM downstream of a wastewater discharge, while limited mixtures (2–5 compounds) were observed in one stream with elevated visitation pressure (recreational “tube floating”). The insecticide, imidacloprid, used to eradicate hemlock woolly adelgid, was detected in 8 (50%) streams. Infrequent exceedances of a cumulative ToxCast-based, exposure-activity ratio (Σ EAR ) 0.001 screening-level of concern suggested limited risk to non-target, aquatic vertebrates, whereas exceedances of a cumulative benchmark-based, invertebrate toxicity quotient (Σ TQ ) 0.1 screening level at 8 locations indicated generally high risk to invertebrates. The results are consistent with the importance of fluvial transport from extra-park sources as a driver of bioactive-contaminant mixture exposures in protected streams and illustrate the potential additional risks from visitation-driven and tactical-use-pesticides.

Tennessee↗

Pilot-scale expanded assessment of inorganic and organic tapwater exposures and predicted effects in Puerto Rico, USA

A pilot-scale expanded target assessment of mixtures of inorganic and organic contaminants in point-of-consumption drinking water (tapwater, TW) was conducted in Puerto Rico (PR) to continue to inform TW exposures and corresponding estimations of cumulative human-health risks across the US. In August 2018, a spatial synoptic pilot assessment of than 524 organic, 37 inorganic, and select microbiological contaminant indicators was conducted in 14 locations (7 home; 7 commercial) across PR. A follow-up 3-day temporal assessment of TW variability was conducted in December 2018 at two of the synoptic locations (1 home, 1 commercial) and included daily pre- and post-flush samples. Concentrations of regulated and unregulated TW contaminants were used to calculate cumulative in vitro bioactivity ratios and Hazard Indices (HI) based on existing human-health benchmarks. Synoptic results confirmed that human exposures to inorganic and organic contaminant mixtures, which are rarely monitored together in drinking water at the point of consumption, occurred across PR and consisted of elevated concentrations of inorganic contaminants (e.g., lead, copper), disinfection byproducts (DBP), and to a lesser extent per/polyfluoroalkyl substances (PFAS) and phthalates. Exceedances of human-health benchmarks in every synoptic TW sample support further investigation of the potential cumulative risk to vulnerable populations in PR and emphasize the importance of continued broad characterization of drinking-water exposures at the tap with analytical capabilities that better represent the complexity of both inorganic and organic contaminant mixtures known to occur in ambient source waters. Such health-based monitoring data are essential to support public engagement in source water sustainability and treatment and to inform consumer point-of-use treatment decision making in PR and throughout the US.

Puerto Rico↗

Is there an urban pesticide signature? Urban streams in five U.S. regions share common dissolved-phase pesticides but differ in predicted aquatic toxicity

Pesticides occur in urban streams globally, but the relation of occurrence to urbanization can be obscured by regional differences. In studies of five regions of the United States, we investigated the effect of region and urbanization on the occurrence and potential toxicity of dissolved pesticide mixtures. We analyzed 225 pesticide compounds in weekly discrete water samples collected during 6–12 weeks from 271 wadable streams; development in these basins ranged from undeveloped to highly urbanized. Sixteen pesticides were consistently detected in 16 urban centers across the five regions—we propose that these pesticides comprise a suite of urban signature pesticides (USP) that are all common in small U.S. urban streams. These USPs accounted for the majority of summed maximum pesticide concentrations at urban sites within each urban center. USP concentrations, mixture complexity, and potential toxicity increased with the degree of urbanization in the basin. Basin urbanization explained the most variability in multivariate distance-based models of pesticide profiles, with region always secondary in importance. The USPs accounted for 83% of pesticides in the 20 most frequently occurring 2-compound unique mixtures at urban sites, with carbendazim+prometon the most common. Although USPs were consistently detected in all regions, detection frequencies and concentrations varied by region, conferring differences in potential aquatic toxicity. Potential toxicity was highest for invertebrates (benchmarks exceeded in 51% of urban streams), due most often to the neonicotinoid insecticide imidacloprid and secondarily to organophosphate insecticides and fipronil. Benchmarks were rarely exceeded in urban streams for plants (at 3% of sites) or fish (<1%). We propose that the USPs identified here would make logical core (nonexclusive) constituents for monitoring dissolved pesticides in U.S. urban streams, and that unique mixtures containing imidacloprid, fipronil, and carbendazim are priority candidates for mixtures toxicity testing.

Science of the Total Environment↗

Multiple in-stream stressors degrade biological assemblages in five U.S. regions

Biological assemblages in streams are affected by a wide variety of physical and chemical stressors associated with land-use development, yet the importance of combinations of different types of stressors is not well known. From 2013 to 2017, the U.S. Geological Survey completed multi-stressor/multi-assemblage stream ecological assessments in five regions of the United States (434 streams total). Diatom, invertebrate, and fish communities were enumerated, and five types of potential stressors were quantified: habitat disturbance, excess nutrients, high flows, basic water quality, and contaminants in water and sediment. Boosted regression tree (BRT) models for each biological assemblage and region generally included variables from all five stressor types and multiple stressors types in each model was the norm. Classification and regression tree (CART) models then were used to determine thresholds for each BRT model variable above which there appeared to be adverse effects (multi-metric index (MMI) models only). In every region and assemblage there was a significant inverse relation between the MMI and the number of stressors exerting potentially adverse effects. The number of elevated instream stressors often varied substantially for a given level of land-use development and the number of elevated stressors was a better predictor of biological condition than was development. Using the adverse effects-levels that were developed based on the BRT model results, 68% of the streams had two or more stressors with potentially adverse effects and 35% had four or more. Our results indicate that relatively small increases in the number of stressors of different types can have a large effect on a stream ecosystem.

Science of the Total Environment↗

Effects-based monitoring of bioactive chemicals discharged to the Colorado River before and after a municipal wastewater treatment plant replacement

Monitoring of the Colorado River near the Moab, Utah, wastewater treatment plant (WWTP) outflow has detected pharmaceuticals, hormones, and estrogen-receptor (ER)-, glucocorticoid receptor (GR)-, and peroxisome proliferator-activated receptor-gamma (PPARγ)-mediated biological activities. The aim of the present multi-year study was to assess effects of a WWTP replacement on bioactive chemical (BC) concentrations. Water samples were collected bimonthly, pre- and post-replacement, at 11 sites along the Colorado River upstream and downstream of the WWTP and analyzed for in vitro bioactivities (e.g., agonism of ER, GR, and PPARγ) and BC concentrations; fathead minnows were cage deployed pre- and post-replacement at sites with varying proximities to the WWTP. Before the WWTP replacement, in vitro ER (24 ng 17β-estradiol equivalents/L)-, GR (60 ng dexamethasone equivalents/L)-, and PPARγ-mediated activities were detected at the WWTP outflow but diminished downstream. In March 2018, the WWTP effluent was acutely toxic to the fish, likely due to elevated ammonia concentrations. Following the WWTP replacement, ER, GR, and PPARγ bioactivities were reduced by approximately 60–79%, no toxicity was observed in caged fish, and there were marked decreases in concentrations of many BCs. Results suggest that replacement of the Moab WWTP achieved a significant reduction in BC concentrations to the Colorado River.

Utah↗

Effects of stormwater runoff from selected bridge decks on conditions of water, sediment, and biological quality in receiving waters in South Carolina, 2013 to 2018

The U.S. Geological Survey, in cooperation with the South Carolina Department of Transportation, investigated the effects of stormwater runoff from bridge decks on stream water quality conditions in South Carolina. The investigation assessed 5 bridges in 3 physiographic provinces in South Carolina (Piedmont, Upper Coastal Plain, and Lower Coast Plain) that had a range of bridge, traffic, and hydrologic characteristics. The five selected South Carolina bridge sites (coincident with U.S. Geological Survey stations) and corresponding highways were Lynches River at Effingham (station 02132000; U.S. Highway 52), North Fork Edisto River at Orangeburg (station 02173500; U.S. Highway 301), Turkey Creek above Huger (station 02172035; South Carolina Highway 41), South Fork Edisto River near Denmark (station 02173000; U.S. Highway 321), and Fishing Creek at Highway 5 below York (station 021473415; South Carolina Highway 5). Bridge decks at the selected sites used open chutes, scuppers, and downspouts to drain stormwater directly into the receiving water at evenly spaced intervals. Stream water, sediment, and biological samples were collected and analyzed for a variety of constituents to evaluate the stream conditions for this study. Five to six stream samples were collected at transects upstream and downstream from each selected bridge site using the equal-width-increment technique during observable stormwater runoff. Routine samples of the receiving waters were collected 12 to 14 times at the upstream transect during nonstorm conditions. Samples were analyzed for physical properties, suspended sediment, nutrients, major ions, trace metals, polycyclic aromatic hydrocarbons, and Escherichia coli . Bridge-deck sediment and streambed sediment at upstream and downstream transects were collected once at each bridge site and analyzed for metals and semivolatile organic compounds that include polycyclic aromatic hydrocarbons. Benthic macroinvertebrate community surveys were conducted once using Hester-Dendy multiplate artificial substrate samplers deployed at multiple upstream and downstream transects concurrently. Statistical analysis of the water-quality data determined that stormwater runoff from bridges did not significantly degrade physical properties, nor nutrient, trace-metal, Escherichia coli , and suspended-sediment concentrations at the selected sites beyond the variability at the upstream transect (no bridge influence) during the study period. During storm sampling at the bridge sites, water-quality conditions were statistically similar upstream and downstream from each bridge, except for greater turbidity, total nitrogen, and total organic nitrogen plus ammonia concentrations found downstream from the bridge site on Fishing Creek; higher total chromium concentrations detected downstream from the bridge site on Turkey Creek; and increased Escherichia coli concentrations found downstream from the bridge site on the North Fork Edisto River. Total recoverable lead, cadmium, and copper concentrations were the only trace metals that periodically exceeded the South Carolina Department of Health and Environmental Control freshwater aquatic-life criteria at some bridge sites (lead, copper, and cadmium in Turkey Creek; cadmium and lead in Fishing Creek; lead in the South Fork Edisto River and Lynches River), but the exceedances occurred more frequently during routine sampling upstream from the bridge sites than during storm sampling at upstream and downstream transects. In general, stormwater runoff from the bridge decks did not seem to be the major source of metal enrichment in receiving waters during the study period. North Fork and South Fork Edisto Rivers and Turkey Creek had only one storm sample that exceeded South Carolina Department of Health and Environmental Control recreational criterion for Escherichia coli at both the upstream and downstream locations, while Fishing Creek had more frequent exceedances. Polycyclic aromatic hydrocarbons were detected infrequently in the stream samples. In general, sediment trace-metal concentrations were below the threshold and probable effect concentration at all bridge sites, except for the chromium concentration (45.1 milligrams per kilogram) detected upstream from the bridge site on Fishing Creek that exceeded the threshold effect concentration of 43.4 milligrams per kilogram. Based on enrichment ratios less than 1.5, bridge-deck runoff did not seem to be affecting trace-metal accumulation in the streambed sediment downstream from the bridge sites, except for lead at the bridge site on the Lynches River and manganese at the bridge site on Fishing Creek. Individual polycyclic aromatic compound concentrations and the sum of 18 compounds did not exceed any threshold and probable effect concentrations, indicating polycyclic aromatic hydrocarbon concentrations in the streambed sediment at downstream and upstream transects were not likely to affect the health of benthic macroinvertebrate communities. Although the cumulative polycyclic aromatic hydrocarbon concentrations in downstream sediment at the sites on Turkey and Fishing Creeks were well below the threshold effect concentration of 1,610 micrograms per kilogram, the 3- to 100-fold increase in downstream concentrations indicated a strong probability of a bridge-deck runoff source. Overall, benthic macroinvertebrate community health downstream from the bridge sites did not seem to be affected by bridge-deck runoff based on several multivariate analyses that indicated statistically similar benthic macroinvertebrate communities at upstream and downstream transects. Of the five bridge sites in this study, the site on Turkey Creek seemed to have the least healthy benthic macroinvertebrate communities because of the lowest Ephemeroptera, Plecoptera, and Trichoptera spp. (mayflies, stoneflies, and caddisflies, respectively) taxa, species richness, and diversity; and the highest biotic indices, indicative of poorer ecological health, at upstream and downstream transects. This ecological finding was not unexpected because of seasonal periods of negligible flow when dissolved-oxygen concentrations fell below 4 milligrams per liter during the study period. Of the five bridge sites in this study, the site on the South Fork Edisto River seemed to have healthier benthic macroinvertebrate communities because of the greater mean Ephemeroptera, Plecoptera, and Trichoptera spp. taxa; and lower mean biotic indices at upstream and downstream transects.

Scientific Investigations Report↗

Methylmercury-Total mercury ratios in predator and primary consumer insects from Adirondack streams (New York, USA)

Mercury (Hg) is a global pollutant that affects biota in remote settings due to atmospheric deposition of inorganic Hg, and its conversion to methylmercury (MeHg), the bioaccumulating and toxic form. Characterizing biotic MeHg is important for evaluating aquatic ecosystem responses to changes in Hg inputs. Aquatic insects possess many qualities desired for MeHg biomonitoring, but are not widely used, largely because of limited information regarding percentages of total mercury (THg) composed of MeHg (i.e., MeHg%) in various taxa. Here, we examine taxonomic, spatial, and seasonal variation in MeHg% of stream-dwelling predator and primary-consumer insects from nine streams in the Adirondack region (NY, USA). Predator MeHg% was high (median 94%) and did not differ significantly among five taxa. MeHg% in selected dragonflies (the most abundant predators, Odonata: Aeshnidae and Libellulidae) exhibited little seasonal and spatial variation, and THg concentration was strongly correlated with aqueous (filtered) MeHg (FMeHg; r s = 0.76). In contrast, MeHg% in primary consumers—shredders (northern caddisflies [Trichoptera: Limnephilidae]) and scrapers (flathead mayflies [Ephemeroptera: Heptageniidae]), were lower (medians 52% and 35%, respectively), and differed significantly between taxa, among sites, and seasonally. Correlations of THg with FMeHg were weak (shredders, r s = 0.45, p = 0.09) or not significant (scrapers, p = 0.89). The higher MeHg% of predators corresponded with their higher trophic positions (indicated by nitrogen stable isotopes). Results suggest obligate predators hold the most promise for the use of THg as a surrogate for MeHg biomonitoring with aquatic insects within the Adirondack region.

Adirondack Mountains↗

Multi-region assessment of pharmaceutical exposures and predicted effects in USA wadeable urban-gradient streams

Human-use pharmaceuticals in urban streams link aquatic-ecosystem health to human health. Pharmaceutical mixtures have been widely reported in larger streams due to historical emphasis on wastewater-treatment plant (WWTP) sources, with limited investigation of pharmaceutical exposures and potential effects in smaller headwater streams. In 2014–2017, the United States Geological Survey measured 111 pharmaceutical compounds in 308 headwater streams (261 urban-gradient sites sampled 3–5 times, 47 putative low-impact sites sampled once) in 4 regions across the US. Simultaneous exposures to multiple pharmaceutical compounds (pharmaceutical mixtures) were observed in 91% of streams (248 urban-gradient, 32 low-impact), with 88 analytes detected across all sites and cumulative maximum concentrations up to 36,142 ng/L per site. Cumulative detections and concentrations correlated to urban land use and presence/absence of permitted WWTP discharges, but pharmaceutical mixtures also were common in the 75% of sampled streams without WWTP. Cumulative exposure-activity ratios (EAR) indicated widespread transient exposures with high probability of molecular effects to vertebrates. Considering the potential individual and interactive effects of the detected pharmaceuticals and the recognized analytical underestimation of the pharmaceutical-contaminant (unassessed parent compounds, metabolites, degradates) space, these results demonstrate a nation-wide environmental concern and the need for watershed-scale mitigation of in-stream pharmaceutical contamination.

Alabama, California, Connecticut, Georgia, Delawar↗

Evaluating the potential role of bioactive chemicals on the distribution of invasive Asian carp upstream and downstream from river mile 278 in the Illinois waterway

Two non-native carp species have invaded the Illinois Waterway and are a threat to Great Lakes ecosystems. Poor water quality in the upper Illinois Waterway, may be a factor contributing to the stalling of the carp population front near river mile 278. In 2015, the U.S. Geological Survey collected 4 sets of water samples from two sites upstream and 4 sites downstream from river mile 278, and one tributary. Each sample was analyzed for up to 649 unique parameters of which 287 were detected including 96 pesticides, 62 pharmaceuticals, 39 wastewater indicator compounds, 29 metals, 19 volatile organic compounds (VOCs), six disinfection by-products (DBPs), five hormones, and five carboxylic acids. Potential for bioactivity was estimated by comparing chemical concentrations to aquatic life or human health criteria and to in-vitro bioactivity screening results in the U.S EPA ToxCast™ database. The resulting hazard quotients and exposure-activity ratios (EARs) are toxicity indexes, that can be used to rank potential bioactivity of individual chemicals and chemical mixtures. This analysis indicates that several bioactive chemicals (BCs) including: carbendazim, 2,4-D, metolachlor, terbuthylazine, and acetochlor (pesticides); 1,4-dioxane (VOC); metformin, diphenhydramine, sulfamethoxazole, tramadol, fexofenadine, and the anti-depressants (pharmaceuticals); bisphenol A, 4-nonylphenol, galaxolide, 4-tert-octylphenol (wastewater indicator chemical); lead and boron (metals); and estrone (hormone) all occur in the upper Illinois Waterway at concentrations that produce elevated EARs values and may be adversely affecting carp reproduction and health. The clear differences in water quality upstream and downstream from river mile 278 with higher contaminant concentrations and potential bioactivity upstream could represent a barrier to carp range expansion.

Illinois↗

Landfill leachate contributes per-/poly-fluoroalkyl substances (PFAS) and pharmaceuticals to municipal wastewater

Widespread disposal of landfill leachate to municipal sewer infrastructure in the United States calls for an improved understanding of the relative organic-chemical contributions to the wastewater treatment plant (WWTP) waste stream and associated surface-water discharge to receptors in the environment. Landfill leachate, WWTP influent, and WWTP effluent samples were collected from three landfill-WWTP systems and compared with analogous influent and effluent samples from two WWTPs that did not receive leachate. Samples were analyzed for 73 per-/poly-fluoroalkyl substances (PFAS), 109 pharmaceuticals, and 21 hormones and related compounds. PFAS were detected more frequently in leachate (92%) than in influent (55%). Total PFAS concentrations in leachate (93,100 ng/L) were more than ten times higher than in influent (6,950 ng/L), and effluent samples (3,730 ng/L). Concentrations of bisphenol A; the nonprescription pharmaceuticals cotinine, lidocaine, nicotine; and the prescription pharmaceuticals amphetamine, carisoprodol, pentoxifylline, and thiabendazole were an order of magnitude higher in landfill leachate than WWTP influent. Leachate load contributions for PFAS (0.78 to 31 g/d), bisphenol A (0.97 to 8.3 g/d), and nonprescription (2.0 to 3.1 g/d) and prescription (0.48 to 2.5 g/d) pharmaceuticals to WWTP influent were generally low (<10 g/d) for most compounds because of high influent-to-leachate volumetric ratios (0.983). No clear differences in concentrations were apparent between effluents from WWTPs receiving landfill leachate and those that did not receive landfill leachate.

Environmental Science: Water Research & Technology↗

Projected urban growth in the Southeastern USA puts small streams at risk

Future land-use development has the potential to profoundly affect the health of aquatic ecosystems in the coming decades. We developed regression models predicting the loss of sensitive fish (R2=0.39) and macroinvertebrate (R2=0.64) taxa as a function of urban and agricultural land uses and applied them to projected urbanization of the rapidly urbanizing Piedmont ecoregion of the southeastern USA for 2030 and 2060. The regression models are based on a 2014 investigation of water quality and ecology of 75 wadeable streams across the region. Based on these projections, stream kilometers experiencing >50% loss of sensitive fish and invertebrate taxa will nearly quadruple to 19,500 and 38,950 km by 2060 (16 and 32% of small stream kilometers in the region), respectively. Uncertainty was assessed using the 20 and 80% probability of urbanization for the land-use projection model and using the 95% confidence intervals for the regression models. Adverse effects on stream health were linked to elevated concentrations of contaminants and nutrients, low dissolved oxygen, and streamflow alteration, all associated with urbanization. The results of this analysis provide a warning of potential risks from future urbanization and perhaps some guidance on how those risks might be mitigated.

PLoS ONE↗

Predictive analysis using chemical-gene interaction networks consistent with observed endocrine activity and mutagenicity of U.S. streams

In a recent U.S. Geological Survey/U.S. Environmental Protection Agency study assessing >700 organic compounds in 38 streams, in vitro assays indicated generally low estrogen, androgen, and glucocorticoid receptor activities, but identified 13 surface waters with 17β estradiol equivalent (E2Eq) activities greater than the 1 ng/L level of concern for feminization of male fish. Among the 36 samples assayed for mutagenicity in the Salmonella bioassay (reported here), 25% were considered mutagenic (statistically significant slope and at least a two-fold increase in revertants/plate). Endocrine and mutagenic activities of the water samples were well correlated with each other and with the total number and cumulative concentrations of detected chemical contaminants. To test the predictive utility of knowledgebase-leveraging approaches, site-specific predicted chemical-gene (pCGA) and predicted analogous pathway-linked (pPLA) association networks identified in the Comparative Toxicogenomics Database were compared with observed endocrine/mutagenic bioactivities. We evaluated pCGA/pPLA patterns among sites by cluster analysis and principal component analysis and grouped the pPLA into broad mode-of-action classes. Measured E2Eq and mutagenic activities correlated well with predicted pathways. The pPLA analysis also revealed correlations with signaling, metabolic, and regulatory groups, suggesting that other effects pathways may be associated with chemical contaminants in these waters and indicating the need for broader bioassay coverage to assess potential adverse impacts.

Environmental Science & Technology↗

Mixed-chemical exposure and predicted effects potential in wadeable southeastern USA streams

Complex chemical mixtures have been widely reported in larger streams but relatively little work has been done to characterize them and assess their potential effects in headwaterstreams. In 2014, the United States Geological Survey (USGS) sampled 54 Piedmont streams over ten weeks and measured 475 unique organic compounds using five analytical methods. Maximum and median exposure conditions were evaluated in relation to watershed characteristics and for potential biological effects using multiple lines of evidence. Results demonstrate that mixed-contaminant exposures are ubiquitous and varied in sampled headwater streams. Approximately 56% (264) of the 475 compounds were detected at least once across all sites. Cumulative maximum concentrations ranged 1,922–162,346 ng L −1 per site. Chemical occurrence significantly correlated to urban land use but was not related to presence/absence of wastewater treatment facility discharges. Designed bioactive chemicals represent about 2/3rd of chemicals detected, notably pharmaceuticals and pesticides, qualitative evidence for possible adverse biological effects. Comparative Toxicogenomics Database chemical-gene associations applied to maximum exposure conditions indicate >12,000 and 2,900 potential gene targets were predicted at least once across all sites for fish and invertebrates, respectively. Analysis of cumulative exposure-activity ratios provided additional evidence that, at a minimum, transient exposures with high probability of molecular effects to vertebrates were common. Finally, cumulative detections and concentrations correlated inversely with invertebrate metrics from in-stream surveys. The results demonstrate widespread instream exposure to extensive contaminant mixtures and compelling multiple lines of evidence for adverse effects on aquatic communities.

Science of the Total Environment↗

Exposure and potential effects of pesticides and pharmaceuticals in protected streams of the US National Park Service southeast Region

Globally protected areas offer refugia for a broad range of taxa including threatened and endangered species. The United States National Park Service (NPS) manages public lands to preserve biodiversity, but increasing park visitation and development of surrounding landscapes increase exposure to and effects from bioactive contaminants. The risk (exposure and hazard) to NPS protected-stream ecosystems within the highly urbanized southeast region (SER) from bioactive contaminants was assessed in five systems based on 334 pesticide and pharmaceutical analytes in water and 119 pesticides in sediment. Contaminant mixtures were common across all sampled systems, with approximately 24% of the unique analytes (80/334) detected at least once and 15% (49/334) detected in half of the surface-water samples. Pharmaceuticals were observed more frequently than pesticides, consistent with riparian buffers and concomitant spatial separation from non-point pesticide sources in four of the systems. To extrapolate exposure data to biological effects space, site specific cumulative exposure-activity ratios (ΣEAR) were calculated for detected surface-water contaminants with available ToxCast data; common exceedances of a 0.001 ΣEAR effects-screening threshold raise concerns for molecular toxicity and possible, sub-lethal effects to non-target, aquatic vertebrates. The results illustrate the need for continued management of protected resources to reduce contaminant exposure and preserve habitat quality, including prioritization of conservation practices (riparian buffers) near stream corridors and increased engagement with upstream/up-gradient property owners and municipal wastewater facilities.

Alabama, Florida, Georgia, Kentucky, Mississippi, ↗