The occurrence and spatiotemporal variation of 26 contaminants of emerging concern (CECs) were evaluated in 68 water samples in 2011–2012 in the Zumbro River watershed, Minnesota, U.S.A. Samples were ...collected across a range of seasonal/hydrological conditions from four stream sites that varied in associated land use and presence of an upstream wastewater treatment plant (WWTP). Selected CECs included human/veterinary pharmaceuticals, personal care products, pesticides, phytoestrogens, and commercial/industrial compounds. Detection frequencies and concentrations varied, with atrazine, metolachlor, acetaminophen, caffeine, DEET, and trimethoprim detected in more than 70% of samples, acetochlor, mecoprop, carbamazepine, and daidzein detected in 30%-50% of samples, and 4-nonylphenol, cotinine, sulfamethoxazole, erythromycin, tylosin, and carbaryl detected in 10%–30% of samples. The remaining target CECs were not detected in water samples. Three land use-associated trends were observed for the detected CECs. Carbamazepine, 4-nonylphenol, erythromycin, sulfamethoxazole, tylosin, and carbaryl profiles were WWTP-dominated, as demonstrated by more consistent loading and significantly greater concentrations downstream of the WWTP and during low-flow seasons. In contrast, acetaminophen, trimethoprim, DEET, caffeine, cotinine, and mecoprop patterns demonstrated both seasonally-variable non-WWTP-associated and continual WWTP-associated influences. Surface water studies of CECs often target areas near WWTPs. This study suggests that several CECs often characterized as effluent-associated have additional important sources such as septic systems or land-applied biosolids. Finally, agricultural herbicide (atrazine, acetochlor, and metolachlor) profiles were strongly influenced by agricultural land use and seasonal application-runoff, evident by significantly greater concentrations and loadings at upstream sites and in early summer when application and precipitation rates are greatest. Our results indicate that CEC monitoring studies should consider a range of land uses, seasonality, and transport pathways in relation to concentrations and loadings. This knowledge can augment CEC monitoring programs to result in more accurate source, occurrence, and ecological risk characterizations, more precisely targeted mitigation initiatives, and ultimately, enhanced environmental decision-making.
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•26 CECs measured in 68 water samples from 4 sites in 2011–2012•Some PPCPs and agricultural herbicides were ubiquitously detected.•Land use and seasonality affected the instream concentrations and loading of CECs.•Wastewater, agricultural/upstream, and mixed-source influences were evident.•Understanding land use and temporal factors will enhance CEC monitoring and mitigation.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Despite reports in the literature of superior contaminant degradation in the root-zone of plants, this phenomenon, known as the rhizosphere effect, is poorly understood. We investigated whether root ...exudates could enhance desorption of residual pollutants, thus improving bioavailability and subsequent biodegradation potential. Root exudates were harvested from three species of hydroponically grown plants, and artificial root exudates (AREs) were created using a literature recipe. Aliquots of the exudates were metabolized by soil bacteria to investigate whether biotransformed exudates exhibited different chemical characteristics or had different effects on contaminant bioavailability than ‘raw exudates.’ Slurries of naphthalene-aged soil containing raw exudates had a significantly lower soil-water distribution coefficient (K d) than slurries with metabolized exudates or no-exudate controls, exhibiting median reductions of 50% and 55%, respectively. Raw exudates had a significantly lower surface tension while not increasing overall solubility, indicating the presence of surface-active compounds below the critical micelle concentration; this is a newly observed mechanism of the rhizosphere effect. Exudate samples were characterized by specific UV absorbance, spectral slope, fluorescence index, and excitation–emission matrices. Substantial changes in organic carbon character pre- and postmetabolism, and between harvested exudates and AREs, suggest that AREs are not chemically representative of plant root exudates. Overall, we present evidence that enhanced contaminant desorption in the presence of exudates provides an abiotic contribution to the rhizosphere effect.
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IJS, KILJ, NUK, PNG, UL, UM
Perfluoroalkyl substances (PFAS) are ubiquitous and persistent environmental contaminants, yet knowledge of their biological effects and mechanisms of action is limited. The highest aqueous PFAS ...concentrations are found in areas where bacteria are relied upon for functions such as nutrient cycling and contaminant degradation, including fire-training areas, wastewater treatment plants, and landfill leachates. This research sought to elucidate one of the mechanisms of action of PFAS by studying their uptake by bacteria and partitioning into model phospholipid bilayer membranes. PFAS partitioned into bacteria as well as model membranes (phospholipid liposomes and bilayers). The extent of incorporation into model membranes and bacteria was positively correlated to the number of fluorinated carbons. Furthermore, incorporation was greater for perfluorinated sulfonates than for perfluorinated carboxylates. Changes in zeta potential were observed in liposomes but not bacteria, consistent with PFAS being incorporated into the phospholipid bilayer membrane. Complementary to these results, PFAS were also found to alter the gel-to-fluid phase transition temperature of phospholipid bilayers, demonstrating that PFAS affected lateral phospholipid interactions. This investigation compliments other studies showing that sulfonated PFAS and PFAS with more than seven fluorinated carbons have a higher potential to accumulate within biota than carboxylated and shorter-chain PFAS.
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This study aimed to understand the effect of different dissolved oxygen (DO) concentrations on the abundance and performance of nitrifying bacteria in full-scale wastewater treatment bioreactors, ...particularly during the winter when nitrifying bacterial activity is often negligible. Biomass samples were collected from three parallel full-scale bioreactors with low DO concentrations (<1.3 mg/ L) and from two full-scale bioreactors with higher DO concentrations (~4.0 and ~2.3 mg/ L). The relative abundance of nitrifying bacteria was determined by sequencing of PCR-amplified 16S rRNA gene fragments. In the three bioreactors with low DO concentrations, effluent ammonia concentrations sharply increased with a decline in temperature below approximately 17 °C, while the bioreactors with high DO concentrations showed stable nitrification regardless of temperature. Even with the decline in nitrification during the winter in the three low DO bioreactors, the relative abundance of ammonia oxidizing bacteria (mostly Nitrosomonas spp.) was curiously maintained. The relative abundance of nitrite oxidizing bacteria was similarly maintained, although there were substantial seasonal fluctuations in the relative abundance values of Nitrospira spp. versus Nitrotoga spp. This research suggests that nitrification activity can be controlled during the winter via DO to produce better effluent quality with high DO concentrations or to reduce aeration costs with a concomitant decline in nitrification activity.
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•Nitrification was inhibited at low dissolved oxygen concentrations and temperatures.•Nitrification performance was continuous at higher dissolved oxygen concentrations.•Nitrifying biomass levels were sustained, independent of nitrification performance.•Nitrospira spp. were prominent year-round at higher dissolved oxygen concentrations.•Nitrotoga spp. were prominent during the summer but scarce during the winter.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
AbstractStorm-water pollutants are widely recognized as a major cause of surface water quality degradation. Most storm-water treatment efforts have focused on capture of particles and ...particle-associated pollutants, but oftentimes half or more of pollutant loads can be attributed to the dissolved phase. Dissolved pollutants are more mobile, bioavailable, and are captured via different mechanisms than particles. Low-impact development storm-water control measures such as bioretention are being used to infiltrate storm water to reduce storm-water volume as well as to capture storm-water pollutants. Bioretention systems have proven effective at capturing both dissolved and particulate storm-water pollutants. Herein the authors present a state-of-the-art review of dissolved storm-water pollutant sources and typical concentrations, removal mechanisms, and fate in bioretention cells covering three pollutant classes: (1) nutrients (i.e., phosphorus and nitrogen), (2) toxic metals, and (3) organic compounds, including emerging contaminants. Also discussed are recent innovations in bioretention design to enhance dissolved pollutant removal, such as media amendments, saturated zones for promoting denitrification, and vegetation for stimulating biodegradation. Current knowledge gaps and recommendations for future research directions are also discussed.
•A model was developed to predict N removal for encapsulated cells.•The model includes diffusion, sorption, reaction, and growth within the encapsulant.•Observed increases in biomass in the outer ...zone was captured by the model.•The reactor performance was accurately predicted.•The methodology developed can optimize encapsulated systems for N removal.
Encapsulation is a promising technology to retain and protect autotrophs for biological nitrogen removal. One-dimensional biofilm models have been used to describe encapsulated systems; they do not, however, incorporate chemical sorption to the encapsulant nor do they adequately describe cell growth and distribution within the encapsulant. In this research we developed a new model to describe encapsulated growth and activity of Nitrosomonas europaea, incorporating ammonium sorption to the alginate encapsulant. Batch and continuous flow reactors were used to verify the simulation results. Quantitative PCR and cross-section fluorescence in situ hybridization were used to analyze the growth and spatial distribution of the encapsulated cells within alginate. Preferential growth of Nitrosomonas near the surface of the encapsulant was predicted by the model and confirmed by experiments. The modeling and experimental results also suggested that smaller encapsulants with a larger surface area to volume ratio would improve ammonia oxidation. Excessive aeration caused the breakage of the encapsulant, resulting in unpredicted microbial release and washout. Overall, our modeling approach is flexible and can be used to engineer and optimize encapsulated systems for enhanced biological nitrogen removal. Similar modeling approaches can be used to incorporate sorption of additional species within an encapsulant, additional nitrogen-converting microorganisms, and the use of other encapsulation materials.
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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 evaluated the occurrence and distribution of 15 contaminants of emerging concern (CECs) in stream water and sediments in the Zumbro River watershed in Minnesota and compared these with ...sub-watershed land uses. Sixty pairs of sediment and water samples were collected across all seasons from four stream sites for over two years and analyzed for selected personal care products, pesticides, human and veterinary medications, and phytoestrogens. Spatial and temporal analyses indicate that pharmaceuticals and personal care products (urban/residential CECs) are significantly elevated in water and/or sediment at sites with greater population density (>100people/km2) and percentage of developed land use (>8% of subwatershed area) than those with less population density and land area under development. Significant spatial variations of agricultural pesticides in water and sediment were detectable, even though all sites had a high percentage of agricultural land use. Seasonality in CEC concentration was observed in water but not in sediment, although sediment concentrations of three CECs did vary between years. Average measured non-equilibrium distribution coefficients exceeded equilibrium hydrophobic partitioning-based predictions for 5 of the 7 detected CECs by at least an order of magnitude. Agreement of measured and predicted distribution coefficients improved with increasing hydrophobicity and in-stream persistence. The more polar and degradable CECs showed greater variability in measured distributions across different sampling events. Our results confirm that CECs are present in urban and agricultural stream sediments, including those CECs that would typically be thought of as non-sorptive based on their log Kow values. These results and the observed patterns of sediment and water distributions augment existing information to improve prediction of CEC fate and transport, leading to more accurate assessments of exposure and risk to surface water ecosystems.
•Sediment–water distributions of CECs were not governed by hydrophobic partitioning.•Water concentrations exhibited seasonal variation; sediment concentrations did not.•Spatial variations correlated with land use for many CECs in water and/or sediment.•Hydrophobicity and persistence affected predictability of distribution coefficients.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Triclosan is a widespread antimicrobial agent that accumulates in anaerobic digesters used to treat the residual solids generated at municipal wastewater treatment plants; there is very little ...information, however, about how triclosan impacts microbial communities in anaerobic digesters. We investigated how triclosan impacts the community structure, function and antimicrobial resistance genes in lab-scale anaerobic digesters. Previously exposed (to triclosan) communities were amended with 5, 50, and 500 mg/kg of triclosan, corresponding to the median, 95th percentile, and 4-fold higher than maximum triclosan concentration that has been detected in U.S. biosolids. Triclosan amendment caused all of the Bacteria and Archaea communities to structurally diverge from that of the control cultures (based on ARISA). At the end of the experiment, all triclosan-amended Archaea communities had diverged from the control communities, regardless of the triclosan concentration added. In contrast, over time the Bacteria communities that were amended with lower concentrations of triclosan (5 mg/kg and 50 mg/kg) initially diverged and then reconverged with the control community structure. Methane production at 500 mg/kg was nearly half the methane production in control cultures. At 50 mg/kg, a large variability in methane production was observed, suggesting that 50 mg/kg may be a tipping point where function begins to fail in some communities. When previously unexposed communities were exposed to 500 mg triclosan/kg, function was maintained, but the abundance of a gene encoding for triclosan resistance (mexB) increased. This research suggests that triclosan could inhibit methane production in anaerobic digesters if concentrations were to increase and may also select for resistant Bacteria. In both cases, microbial community composition and exposure history alter the influence of triclosan.
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IJS, KILJ, NUK, PNG, UL, UM
Understanding the sources, transport, and spatiotemporal variability of contaminants of emerging concern (CECs) is important for understanding risks and developing monitoring and mitigation ...strategies. This study used mass balances to compare wastewater treatment plant (WWTP) and upstream sources of 16 CECs to a mixed-use watershed in Minnesota, under different seasonal and hydrological conditions. Three distinct CEC groups emerged with respect to their source proportionality and instream behavior. Agricultural herbicides and daidzein inputs were primarily via upstream routes with the greatest loadings and concentrations during high flows. Trimethoprim, mecoprop, nonprescription pharmaceuticals, and personal care products entered the system via balanced/mixed pathways with peak loadings and concentrations in high flows. Carbaryl, 4-nonylphenol, and the remaining prescription pharmaceuticals entered the system via WWTP effluent with relatively stable loadings across sampling events. Mass balance analysis based on multiple sampling events and sites facilitated CEC source comparisons and may therefore prove to be a powerful tool for apportioning sources and exploring mitigation strategies.
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