Precipitation samples have been collected by the National Atmospheric Deposition Program's (NADP) National Trends Network (NTN) using the Aerochem Metrics Model 301 (ACM) collector since 1978. Approximately one-third of the NTN ACM collectors have been replaced with N-CON Systems, Inc. Model ADS 00-120 (NCON) collectors. Concurrent data were collected over 6 years at 12 NTN sites using colocated ACM and NCON collectors in various precipitation regimes. Linear regression models of the colocated data were used to adjust for relative bias between the collectors. Replacement of ACM collectors with NCON collectors resulted in shifts in 10-year seasonal precipitation-weighted mean concentration (PWMC) trend slopes for: cations (−0.001 to −0.007 mgL−1yr−1), anions (−0.009 to −0.028 mgL−1yr−1), and hydrogen ion (+0.689 meqL-1yr−1). Larger shifts in NO3− and SO4−2 seasonal PWMC trend slopes were observed in the Midwest and Northeast US, where concentrations are generally higher than in other regions. Geospatial analysis of interpolated concentration rasters indicated regions of accentuated variability introduced by incorporation of NCON collectors into the NTN.

Synthetic glucocorticoids (GCs) such as dexamethasone (DEX) and prednisolone (PDS) have been used since the 1940s to cure inflammatory and auto-immune disorders. Their use has been linked to a host of deleterious effects in aquatic ecosystems such as osteoporosis in vertebrates, developmental impairments in molluscs and reduced fecundity and growth in cladocerans. Apart from these handful of studies, the effects of GCs on aquatic biota are largely unknown. The present study is a first of its kind aiming to assess the multi-generational exposure effects of DEX and PDS on the life history parameters of Ceriodaphnia dubia (C. dubia). Multigenerational studies have proved to be an advantage in assessing the cumulative damage caused by aquatic toxicants at the population level of the exposed organisms over a period of successive generations using multiple biological endpoints. Test results demonstrated that C. dubia exhibited varied sensitivities towards both the studied chemicals however were more sensitive to DEX with 48-h EC50 (95% confidence interval) of 0.75 mg/L (CI: 0.59–0.92) in comparison to PDS [19 mg/L (CI: 15–23)]. EC10 values for F0 in a multigenerational chronic bioassays were 48 μg/L (CI: 37.4–61) for DEX and 460 μg/L (CI: 341–606) for PDS and in F3 were 2.2 μg/L (CI: 1.6–3.1) for DEX and 31 μg/L (CI: 19.4–46) for PDS. There was a positive trend of increased toxicity followed by reduced life history traits such as fecundity, brood size and time to first brood and intrinsic rate of population increase and body growth (length and area) of C. dubia in the case of both studied chemicals. The results from the current work highlighted the importance of multigenerational studies in identifying the evolutionary responses of stressed non-target aquatic organisms, and data obtained can be further used in developing water quality guidelines.

To better determine phytotoxicity thresholds for metals in the soil, studies should use actual field-contaminated soil samples rather than metal-spiked soil preparations. However, there are surprisingly few such data available for Cu phytotoxicity in field-contaminated soils. Moreover, these studies differ from each other with regards to soil characteristics and experimental setups. This study aimed at more accurately estimating Cu phytotoxicity thresholds using field-collected agricultural soils (Entisols) from areas exposed to contamination from Cu mining. For this purpose, the exposure to Cu was assessed by measuring total soil Cu, soluble Cu, free Cu2+ activity, and Cu in the plant aerial tissues. On the other hand, two bioassay durations (short-term and long-term), three plant species (Avena sativa L., Brassica rapa CrGC syn. Rbr, and Lolium perenne L.), and five biometric endpoints (shoot length and weight, root length and weight, and number of seed pods) were considered. Overall plant growth was best predicted by total Cu content of the soil. Despite some confounding factors, it was possible to determine EC10, EC25 and EC50 of total Cu in the soil. Brassica rapa was more sensitive than Avena sativa for all endpoints, while Lolium perenne was of intermediate sensitivity. For the short-term bioassay (21 days for all three species), the averaged EC10, EC25 and EC50 values of total soil Cu (in mg kg−1) were 356, 621, and 904, respectively. For the long-term bioassay (62 days for oat and 42 days for turnip), the averaged EC10, EC25 and EC50 values of total soil Cu (in mg kg−1) were 355, 513, and 688, respectively. The obtained results indicate that chronic test is a suitable method for assessing Cu phytotoxicity in field-contaminated soils.

Intensive exploitation and transport of oil and derivatives are increasing the risk of coastal contamination by either dramatic disasters or diffuse sources. Tools for monitoring diffuse contamination, such as diesel oil that leaks from marine vessels are much needed. We experimentally tested the efficiency of antioxidant biomarkers as indicators of chronic exposure to diesel oil in a mudflat from the subtropical Bay of Paranaguá, in southern Brazil. We examined the effects of three successive diesel oil spills, with two weeks of recovery time between exposures, on the edible clam Anomalocardia flexuosa. Previous studies have highlighted its potential as a bioindicator species for diesel oil contamination in subtropical and tropical ecosystems. Endpoints measured in gill and digestive gland homogenates included the activity of antioxidant enzymes SOD, GPx, GST and levels of lipid peroxides. PAHs concentration in sediments and soft tissue were also quantified. GST and SOD were the most responsive biomarkers to the exposure. There were significant but non–cumulative departures from control levels in organisms from treated samples, which were, in all cases, more common 48 h after each experimental spill. Biomarker responses were more evident in the digestive gland than in gills. This work validated the short–term responsiveness of biomarkers as measures of repeated pulsed in situ exposure to low concentrations of diesel oil. For their routine implementation into monitoring programs for tropical estuaries our general recommendations are 1) to include several reference sites, 2) to analyze biomarker data using a logarithmic–scale and 3) to interpret deviations from “normal” activity as multiplicative interval differences.

The environmental safety of cerium (Ce) applications in many fields has been debated for almost a century because the cellular effects of environmental Ce on living organisms remain largely unclear. Here, using new, interdisciplinary methods, we surprisingly found that after Ce(III) treatment, Ce(III) was first recognized and anchored on the plasma membrane in leaf cells. Moreover, some trivalent Ce(III) was oxidized to tetravalent Ce(IV) in this organelle, which activated pinocytosis. Subsequently, more anchoring sites and stronger valence-variable behavior on the plasma membrane caused stronger pinocytosis to transport Ce(III and IV) into the leaf cells. Interestingly, a great deal of Ce was bound on the pinocytotic vesicle membrane; only a small amount of Ce was enclosed in the pinocytotic vesicles. Some pinocytic vesicles in the cytoplasm were deformed and broken. Upon breaking, pinocytic vesicles released Ce into the cytoplasm, and then these Ce particles self-assembled into nanospheres. The aforementioned special behaviors of Ce decreased the fluidity of the plasma membrane, inhibited the cellular growth of leaves, and finally, decreased plant yield. In summary, our findings directly show the special cellular behavior of Ce in plant cells, which may be the cellular basis of plant yield reduction induced by environmental Ce.

Many regulatory screening level exposure assessments are based on simple large scale conceptual scenarios. However, exposure, and therefore risks associated with chemicals, are characterised by high spatial variability. The Scenario assembly tool (ScenAT) is a global screening level model to enable spatially resolved local predictions of environmental concentrations of home and personal care chemicals. It uses the European Union Technical Guidance Document (TGD) equation to predict local scale freshwater concentrations (predicted environmental concentrations - PECs) of chemicals discharged via wastewater. ScenAT uses Geographic Information System (GIS) layers for the underlying socio-economic (population) and environmental parameters (per capita water use, sewage treatment plant connectivity, dilution factor). Using a probabilistic approach, we incorporate sources of uncertainty in the input data (tonnage estimation, removal in sewage treatment plants and seasonal variability in dilution factors) for two case-study chemicals: the antimicrobial triclosan (TCS) and the anionic surfactant linear alkylbenzene sulphonate (LAS). We then compare model estimates of wastewater and freshwater concentrations of TCS and LAS to UK monitoring data. Comparison showed that modeled PECs were on average higher than mean measured data for TCS and LAS by a factor 1.8 and 1.4, respectively. Considering the uncertainty associated with both model and monitoring data, the use of a probabilistic approach using the ScenAT model for screening assessment is reasonable. The combination of modelled and monitoring data enables the contextualisation of monitoring data. Spatial PECs can be used to identify areas of elevated concentration for further refined assessment.A probabilistic approach for large scale screening assessments to contextualise monitoring data for risk assessment.

Diluted bitumen (dilbit) from Alberta oil sands (Canada) is transported across major continental watersheds, yet little is known about its toxicity to fish if spilled into aquatic environments. The toxicity of Cold Lake (CLB) dilbit was assessed for medaka embryos (Oryzias latipes) exposed to water accommodated fractions (WAF) and chemically-enhanced WAF (CEWAF) using Corexit®EC9500A as dispersant. The effects of CLB toxicity were similar to conventional crude oils and Access Western Blend (AWB) dilbit. The prevalence of malformations and cyp1a mRNA synthesis in hatched fish increased monotonically with concentration during WAF and CEWAF treatments and provided a novel indicator of dilbit PAH toxicity. Apart from nfe2 (an antioxidant transcription factor), there were no statistically significant monotonic exposure-responses of ahr, arnt2, cat, sod, gpx, gst, gsr, g6pdh, p53, and hsp70 transcripts at total polycyclic aromatic hydrocarbons (TPAH) concentrations bracketing EC50s for embryotoxicity (WAF ≅ 3 μg/L; CEWAF ≅ 0.1 μg/L TPAH). Based on measured TPAH concentrations in exposure test solutions, CLB dilbit was 6–10 fold more toxic to medaka than AWB during chronic exposures. Lack of direct monotonic gene transcription responses to increasing oil concentrations during exposures that were embryotoxic suggests that the capacity of the oxidative stress response is limited in earlier lifestages or that differences exist among species in mechanisms of toxicity. This study provides a comparative framework for identifying suitable biomarkers and toxicity methods for those fish species in sensitive lifestages at highest risk of Canadian oil sands dilbit exposure following a spill in the freshwater environment.

Land application of animal manure is a common agricultural practice potentially leading to dispersal and propagation of antibiotic resistance genes (ARGs) in environmental settings. However, the fate of resistome in agro-ecosystems over time following application of different manure sources has never been compared systematically. Here, soil microcosm incubation was conducted to compare effects of poultry, cattle and swine manures spiked with or without the antibiotic tylosin on the temporal changes of soil ARGs. The high-throughput quantitative PCR detected a total of 185 unique ARGs, with Macrolide-Lincosamide-Streptogramin B resistance as the most frequently encountered ARG type. The diversity and abundance of ARGs significantly increased following application of manure and manure spiked with tylosin, with more pronounced effects observed in the swine and poultry manure treatments than in the cattle manure treatment. The level of antibiotic resistance gradually decreased over time in all manured soils but was still significantly higher in the soils treated with swine and poultry manures than in the untreated soils after 130 days’ incubation. Tylosin-amended soils consistently showed higher abundances of ARGs than soils treated with manure only, suggesting a strong selection pressure of antibiotic-spiked manure on soil ARGs. The relative abundance of ARGs had significantly positive correlations with integrase and transposase genes, indicative of horizontal transfer potential of ARGs in manure and tylosin treated soils. Our findings provide evidence that application of swine and poultry manures might enrich more soil ARGs than cattle manure, which necessitates the appropriate treatment of raw animal manures prior to land application to minimise the spread of environmental ARGs.

Acrylamide-induced immunotoxicity and allergic dermatitis have been reported in animal experiments and clinical reports, respectively. However, epidemiological evidence from the general population is limited.The purpose of the present study was to estimate the associations between acrylamide exposure and allergy-related outcomes in the general US population.A total of 6982 subjects were selected from the National Health and Nutrition Examination Survey 2005–2006 (NHANES). Internal exposure was measured by the hemoglobin adducts of acrylamide (HbAA) and its metabolite glycidamide (HbGA). Allergy-related outcomes including asthma, hay fever, allergy, itchy rash, sneeze, wheeze and eczema were obtained by self-administered questionnaires. Allergic sensitization was assessed by the total immunoglobulin E (IgE) levels. The associations of HbAA and HbGA quartiles with allergy-related outcomes were calculated using logistic regression models with multivariable adjustments. Analyses were additionally stratified according to age, gender and serum cotinine levels.When setting quartile 1 of HbAA as reference, the odds ratios (ORs) [95% confidence intervals (CIs)] of quartile 2 to 4 for eczema were 1.18 (0.79–1.76), 1.14 (0.73–1.78) and 1.58 (1.14–2.18), respectively (ptrend = 0.002). Individuals at the highest quartile of HbGA had significantly elevated likelihoods of itchy rash (OR = 1.37, 95% CI = 1.02–1.83, ptrend = 0.032) and eczema (OR = 1.45, 95% CI = 1.06–1.97, ptrend = 0.044). The stratification analyses indicated various results in different subgroups.This study indicated significant associations between HbAA and HbGA levels and the likelihoods of allergy-related outcomes in the general US population, depending on age, gender and smoke exposure status. These findings suggested potential public health concerns for the widespread exposure to acrylamide.

Very few ecotoxicological studies have been performed on long-term exposure under controlled conditions, hence limiting the assessment of the impact of chronic and diffuse chemical pressures on the health of aquatic organisms. In this study, an ecotoxicoproteomic approach was used to assess the integrated response and possible acclimation mechanisms in Gammarus fossarum following chronic exposures to Cd, Cu or Pb, at environmentally realistic concentrations (i.e. 0.25, 1.5 and 5 μg/L respectively). After 10-week exposure, changes in protein expression were investigated in caeca of control and exposed males. Gel-free proteomic analyses allowed for the identification of 35 proteins involved in various biological functions, for which 23 were significantly deregulated by metal exposures. The protein deregulation profiles were specific to each metal, providing evidence for metal-specific action sites and responses of gammarids. Among the tested metals, Cu was the most toxic in terms of mortality, probably linked with persistent oxidative stress. Moulting and osmoregulation were the major biological functions affected by Cu in the long-term. In Pb-exposed gammarids, significant deregulations of proteins involved in immune response and cytoskeleton were observed. Reproduction appears to be strongly affected in gammarids chronically exposed to Cd or Pb. Besides, modified expressions of several proteins involved in energy transfer and metabolism highlighted important energetic reshuffling to cope with chronic metal exposures. These results support the fact that metallic pressures induce a functional and energetic cost for individuals of G. fossarum with potential repercussions on population dynamics. Furthermore, this ecotoxicoproteomic study offers promising lines of enquiry in the development of new biomarkers that could make evidence of long-term impacts of metals on the health of organisms.