Hydrophobic legacy contaminants like dichlorodiphenyltrichloroethane (DDT) and polychlorinated biphenyls (PCBs) were banned almost half a century ago. While their residues still remain in many ...environmental compartments, they have undergone extensive aging and likely have lower bioaccessibility (the available fraction) compared to fresh residues. However, risk assessment relies heavily on the use of total chemical concentration, rather than accounting for age-diminished bioaccessibility, likely leading to overestimated risks. In this study, we used 24 h Tenax desorption to measure the potential bioaccessibility of DDTs and PCBs in two sediment cores taken from the Palos Verdes Shelf Superfund site in the Pacific Ocean. The total concentrations of DDTs and PCBs from the core located at the sewage outfall (8C) were as high as 41,000–15,700 μg/kg (dry weight, dw) and 530-2600 μg/kg dw, respectively, while those from a location 7 km northeast of the outfall (3C) were 2–3 orders of magnitude lower. Bioaccessibility estimated by 24-h Tenax-aided desorption (F24h) decreased in the order of DDD > DDE > DDT for DDT derivatives, and PCB 52 > PCB 70 > PCB 153 for PCB congeners, showing a negative correlation with their log Kow. Due to the extensive aging, F24h values were <20% of the total chemical concentration for most contaminants and <5% for DDT, DDE and PCB 153, suggesting that aging greatly diminished their bioavailability. However, a quantitative relationship between F24h and sediment age along the vertical profile was not found, likely because the contaminant residues had undergone aging before their offsite transport and deposition onto the ocean floor. As the use of man-made chemicals such as DDT and PCBs was discontinued in the U.S. many decades ago, the reduction in their bioavailability due to aging may be universal and should be taken into consideration to avoid overly conservative risk predictions or unnecessary mitigation interventions.
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•Total concentrations of DDTs and PCBs remains high on the Palos Verdes Shelf.•Aging has greatly diminished bioaccessibility.•Bioavailability should be used during risk assessment versus total concentration.
Although levels of HOCs remain high in the Palos Verdes Shelf sediment, the bioaccessible fractions are extremely low, suggesting limited bioavailability for marine organisms.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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•Order of acute toxicity: Platinum complexes > endocrine therapy agents > antibiotics.•Crustaceans were most sensitive aquatic species to anticancer drugs.•Most of anticancer drugs ...are persistent in the aquatic environment.•Seven anticancer drugs should be priority concerned in the aquatic environment.
Anticancer drugs are a group of therapeutic agents used to enhance cell death in targeted cell types of neoplasia. Because of frequent use and eventual discharge, they have been often detected in wastewater from pharmaceutical factories and hospitals, domestic wastewater, and surface waters. The occurrence of these drugs in aquatic ecosystems and their effects on aquatic organisms have been poorly characterized. This review focuses on the global occurrence of major classes of anticancer drugs in water and sediments of freshwater ecosystems and their ecotoxicological effects at different biological levels. While the availability of data is fairly limited, concentrations of most anticancer drugs range from < 2 ng/L to 762 µg/L in receiving water, while levels in sediments and sludge vary from 0.25 to 42.5 µg/kg. Their detection frequencies were 58%, 52% (78%) and 59% in hospital wastewater, wastewater treatment plant effluents (influents) and surface water, respectively. Predicted log Kow values of vincristine, imatinib mesylate and tamoxifen are higher than 3 and have estimated half-lives>60 d in waters using quantitative structure–activity relationship models, indicating high potential for persistence and bioaccumulation. Based on a species sensitivity distribution evaluation of 9 compounds, crustaceans are most sensitive to anticancer drugs. The most hazardous compound is cisplatin which has a hazard concentration at the 5th percentile. For Daphnia magna, the acute toxicities of major classes of anticancer drugs are ranked as platinum complexes > endocrine therapy agents > antibiotics > antimetabolite agents > alkylating agents. Using hazard quotient analysis based primarily on the lowest observed effect concentrations (LOECs), cyclophosphamide, cisplatin, 5-fluorouracil, imatinib mesylate, bicalutamide, etoposide and paclitaxel have the highest hazard for aquatic organisms. Further research is needed to identify appropriate chronic endpoints for risk assessment thresholds as well as to better understand the mechanisms of action and the potential multigenerational toxicity, and trophic transfer in ecosystems.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
This study investigated the significant influence of HCO3 – on the degradation of contaminants of emerging concern (CECs) during nitrate photolysis at 254 nm for water reuse applications. The ...second-order rate constants for the reactions between selected contaminants with carbonate radical (CO3 •–) were determined at pH 8.8 and T = 20 °C: estrone ((5.3 ± 1.1) × 108 M–1 s–1), bisphenol A ((2.8 ± 0.2) × 108 M–1 s–1), 17α-ethynylestradiol ((1.6 ± 0.3) × 108 M–1 s–1), triclosan ((4.2 ± 1.4) × 107 M–1 s–1), diclofenac ((2.7 ± 0.7) × 107 M–1 s–1), atrazine ((5.7 ± 0.1) × 106 M–1 s–1), carbamazepine ((4.2 ± 0.01) × 106 M–1 s–1), and ibuprofen ((1.2 ± 1.1) × 106 M–1 s–1). Contributions from UV, reactive nitrogen species (RNS), hydroxyl radical (•OH), and CO3 •– to the CEC decomposition in UV/NO3 – in the presence and absence of HCO3 – were investigated. In addition, possible transformation products and degradation pathways of triclosan, diclofenac, bisphenol A, and estrone in UV/NO3 –/HCO3 – were proposed based on the mass (MS) and MS2 spectra. Significant reduction in the cytotoxicity of bisphenol A was observed after the treatment with UV/NO3 –/HCO3 –.
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IJS, KILJ, NUK, PNG, UL, UM
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•A KEGG analysis in common DEGs of the antibiotics showed the activation of NF-κB.•Low levels of antibiotics induced a NF-κB-mediated immune response.•Induction of cytokines by ...antibiotics were minor when compared to LPS treatment.•Exposure of fish macrophages to low doses of antibiotics activates the NF-kB pathway.
Low doses of antibiotics are ubiquitous in the marine environment and may exert negative effects on non-target aquatic organisms. Using primary macrophages of common carp, we investigated the mechanisms of action following exposure to several common antibiotics; cefotaxime, enrofloxacin, tetracycline, sulfamonomethoxine, and their mixtures, and explored the immunomodulatory effects associated with the nuclear factor-κB (NF-κB) signaling pathway. A KEGG pathway analysis was conducted using the sixty-six differentially expressed genes found in all treatments, and showed that exposure to 100 μg/L of antibiotics could affect regulation of the NF-κB signaling pathway, suggesting that activation of NF-κB is a common response in all four classes of antibiotics. In addition, the four antibiotics induced nf-κb and NF-κB-associated cytokines expression, as verified by qPCR, however, these induction responses by four antibiotics were minor when compared to the same concentration of LPS treatment (100 μg/L). Antagonists of NF-κB blocked many of the immune effects of the antibiotics, providing evidence that NF-κB pathways mediate the actions of all four antibiotics. Moreover, exposure to environmentally relevant, low levels (0.01–100 μg/L) of antibiotics induced a NF-κB-mediated immune response, including endogenous generation of ROS, activity of antioxidant enzymes, as well as expression of cytokine and apoptosis. Moreover, exposure to mixtures of antibiotics presented greater effects on most tested immunological parameters than exposure to a single antibiotic, suggesting additive effects from multiple antibiotics in the environment. This study demonstrates that exposure of fish primary macrophages to low doses of antibiotics activates the NF-kB pathway.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Plastic debris is an emerging worldwide threat to marine biota. Marine species may face unique challenges in low-flow estuarine systems with a high abundance of “macro-sized” (>4.75 mm) plastic due ...to the leaching of constituents and adsorbed contaminants. To simulate this leaching process, plastic samples recovered from the North Pacific Gyre along with corresponding UV-irradiated virgin plastic and non-irradiated virgin plastic counterparts were incubated in saltwater for 30 days at ambient temperatures ranging from 17 to 25 °C. Following solid-phase extraction, water samples were fractionated with sequential methanol elution from 10 to 100% and evaluated using in vitro assays assessing estrogen receptor (ER) and aryl hydrocarbon receptor (AhR) activities. In vivo responses (vitellogenin vtg and cytochrome p450 1A cyp1a mRNA) were measured following 5-day exposures in Japanese medaka (Oryzias latipes) larvae (3 days post hatch). Estrogenic plasticizers, co-planar PCBs and PAHs were quantified in the extracts using targeted GC–MS/MS and UPLC-MS/MS. In vitro estrogenicity showed highest activity in the 70% methanol fraction for all plastic leachate exposures. Whole extract in vitro estradiol equivalent (EEQ) values were 4.34 ± 2.65, 8.79 ± 2.09 and 13.78 ± 3.64 ng/L, for virgin plastic, UV-irradiated virgin plastic and North Pacific Gyre-recovered plastic, respectively (mean ± SD). Significant vtg induction was observed in medaka larvae exposed to leachate extracts from North Pacific Gyre-recovered plastic and UV-irradiated virgin plastic (9.9-fold, p = 0.039 and 10.1-fold, p = 0.042, respectively). Chemically-determined EEQ values were also localized in the 70% methanol fraction. Whole leachate extract chemical EEQ values were 0.33 ± 0.07, 1.64 ± 0.62 and 11.4 ± 2.13 ng/L, for virgin plastic, UV-irradiated virgin plastic and North Pacific Gyre-recovered plastic, respectively. In-vitro AhR activity was highest in the 70% methanol elution with greater activity in North Pacific Gyre-recovered plastic than in virgin plastic and UV-irradiated virgin plastic (toxic equivalency TEQ = 1.06 ± 0.54, 0.38 ± 0.07 and 0.71 ± 0.47 ng/L, respectively). CYP1A mRNA was significantly induced in larval medaka exposed to North Pacific Gyre-recovered plastic leachates (17.8-fold, p = 0.02) while exposure to virgin plastic and UV-irradiated virgin plastic leachates caused no significant change. Chemically-determined TEQ analysis for AhR indicated highest activity in the 90% methanol fraction for all leachates, with whole extract in vitro TEQs being 1.47 ± 0.87, 0.03 ± 0.05 and 0.42 ± 0.38 ng/L for North Pacific Gyre-recovered plastic, virgin plastic and UV-irradiated virgin plastic, respectively. These results indicate that weathering and UV radiation release estrogenic plasticizers and demonstrate the ability for plastics to transport adsorbed persistent organic pollutants at eco-toxicologically relevant concentrations.
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•North Pacific Gyre plastic leached higher in vitro and chemical EEQ and TEQ than “virgin” and irradiated “virgin” plastic.•North Pacific Gyre plastic leachates significantly induced cyp1a and VTG mRNA in Oryzias latipes.•UV radiation enhanced desorption of BPA, OP and PCBs from virgin plastic and induced VTG mRNA in Oryzias latipes.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The Deepwater Horizon (DWH) incident resulted in extensive oiling of the pelagic zone and shoreline habitats of many commercially important fish species. Exposure to the water-accommodated fraction ...(WAF) of oil from the spill causes developmental toxicity through cardiac defects in pelagic fish species. However, few studies have evaluated the effects of the oil on near-shore estuarine fish species such as red drum (Sciaenops ocellatus). Following exposure to a certified weathered slick oil (4.74 μg/L ∑PAH50) from the DWH event, significant sublethal impacts were observed ranging from impaired nervous system development average 17 and 22% reductions in brain and eye area at 48 h postfertilization (hpf), respectively to abnormal cardiac morphology (100% incidence at 24, 48, and 72 hpf) in red drum larvae. Consistent with the phenotypic responses, significantly differentially expressed transcripts, enriched gene ontology, and altered functions and canonical pathways predicted adverse outcomes in nervous and cardiovascular systems, with more pronounced changes at later larval stages. Our study demonstrated that the WAF of weathered slick oil of DWH caused morphological abnormalities predicted by a suite of advanced bioinformatic tools in early developing red drum and also provided the basis for a better understanding of molecular mechanisms of crude oil toxicity in fish.
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IJS, KILJ, NUK, PNG, UL, UM
Organophosphate esters (OPEs) have been in use as flame retardants for many decades, with their actual usage varying over time. Knowledge of the emission history of OPEs is valuable for improving our ...prediction of their environmental loadings and associated risks. In this study, concentrations and compositions of 10 OPEs were measured in three dated sediment cores from the Palos Verdes Shelf (PVS) off the coast of Los Angeles, which has been impacted by wastewater treatment plant (WWTP) effluents for over a century. The total OPE concentrations varied from 0.68 to 1064 ng/g along the sediment profile, with two apparent peaks. The first peak occurred in the 1970s, coinciding with peak emissions from WWTPs. The second peak appeared in the 2000s and was possibly attributed to increased consumption of OPEs as replacement flame retardants. Since downward movement of OPEs in the PVS sediment bed was retarded by their slow desorption, the reconstructed history likely provided an accurate picture of OPE emissions in Southern California and North America. These findings suggest that the near-shore marine sediments affected by WWTP effluents could serve as an environmental proxy documenting history in OPE use and emissions.
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IJS, KILJ, NUK, PNG, UL, UM
The Salton Sea, the largest inland surface water body in California, has been designated as a sensitive ecological area by federal and state governments. Its two main tributaries, the New River and ...Alamo River are impacted by urban and agriculture land use wastes. The purpose of this study was to temporally and spatially evaluate the ecological risks of contaminants of concern in water, sediments and fish tissues. A total of 229 semivolatile organic compounds and 12 trace metals were examined. Among them Selenium, DDTs, PAHs, PCBs, chlorpyrifos and some current-use pesticides such as pyrethroids exceeded risk thresholds. From 2002 to 2012, measurements of chlorpyrifos in sediments generally declined and were not observed after 2009 at the river outlets. In contrast, pyrethroid concentrations in sediments rose consistently after 2009. In water samples, the outlets of the two rivers showed relatively higher levels of contamination than the main water body of the Salton Sea. However, sediments of the main water body of the Salton Sea showed relatively higher sediment concentrations of contaminants than the two rivers. This was particularly true for selenium which showed reductions in concentrations from 2002 to 2007, but then gradual increases to 2012. Consistent with water evaluations, contaminant concentrations in fish tissues tended to be higher at the New River boundary and at the drainage sites for the Alamo River compared to sites along each river. The persistent contaminants DDTs, PAHs, chlorpyrifos and several pyrethroid insecticides were associated with the toxicity of sediments and water collected from the rivers. Overall, assessment results suggested potential ecological risk in sediments of the Salton Sea as well as in water and fish from the two rivers.
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•Persistent toxics are prevalent in the Salton Sea and its two main tributary rivers.•Contaminant levels in water and fish are higher in the rivers than the Sea.•Sediment chlorpyrifos declined, pyrethroid and selenium increased from 2007 to 2012.•DDT, PAH, chlorpyrifos and pyrethroids are associated with in vivo toxicity.•Exceedance of thresholds suggests potential ecological risk in the Sea and rivers.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
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•Plant accumulation of four CECs and their methylated or demethylated counterparts was measured.•Methylated counterparts showed comparative or greater accumulation in Arabidopsis ...cells and wheat plant.•Demethylated derivatives exhibited more limited uptake or translocation.•Methylation/demethylation influenced plant accumulation by altering physicochemical properties.•Transformation products need to be included for holistic risk assessment.
Contaminants of emerging concern (CECs) as well as their transformation products (TPs) are often found in treated wastewater and biosolids, raising concerns about their environmental risks. Small changes in chemical structure, such as the addition or loss of a methyl group, as the result of methylation or demethylation reaction, may significantly alter a chemical’s physicochemical properties. In this study, we evaluated the difference in accumulation and translocation between four CECs and their respective methylated or demethylated derivatives in plant models. Suspended Arabidopsis thaliana cell culture and wheat seedlings were cultivated in nutrient solutions containing individual compounds at 1 mg/L. The methylated counterparts were generally more hydrophobic and showed comparative or greater accumulation in both plant models. For example, after 1 h incubation, methylparaben was found in A. thaliana cells at levels two orders of magnitude greater than demethylated methylparaben. In contrast, the demethylated counterparts, especially those with the addition of a hydroxyl group after demethylation, showed decreased plant uptake and limited translocation. For example, acetaminophen and demethylated naproxen were not detected in the shoots of wheat seedlings after hydroponic exposure. Results from this study suggest that common transformations such as methylation and demethylation may affect the environmental fate of CECs, and should be considered to obtain a more comprehensive understanding of risks of CECs in the environment.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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