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Frequent occurrence of trace organic contaminants in aquatic environments, such as sulfonamide antibiotics in rivers receiving reclaimed water, is concerning. Natural attenuation by soil and sediment is increasingly relied upon. In the case of riverbank filtration for water purification, the reliability of antibiotic attenuation has been called into question due to incomplete understanding of their degradation processes. This study investigated influence of substrates and redox evolution along infiltration path on biotransformation of sulfonamides. Eight sand columns (length: 28 cm) with a riverbed sediment layer at 3-8 cm were fed by groundwater-sourced tap water spiked with 1 µg/L of sulfadiazine (SDZ), sulfamethazine (SMZ), and sulfamethoxazole (SMX) each, with or without amendments of dissolved organic carbon (5 mg-C/L of 1:1 yeast and humics) or ammonium (5 mg-N/L). Two flow rates were tested over 120 days (0.5 mL/min and 0.1 mL/min). Iron-reducing conditions persisted in all columns for 27 days during the initial high flow period due to respiration of sediment organics, evolving to less reducing conditions until the subsequent low flow period to resume more reducing conditions. With surplus substrates, the spatial and temporal patterns of redox conditions differentiated among columns. The removal of SDZ and SMZ in effluents was usually low (15 ± 11%) even with carbon addition (14 ± 9%), increasing to 33 ± 23% with ammonium addition. By contrast, SMX removal was higher and more consistent among columns (46 ± 21%), with the maximum of 64 ± 9% under iron-reducing conditions. When sulfonamide removal was compared between columns for the same redox zones during infiltration, their enhancements were always associated with the availability of dissolved or particulate substrates, suggesting co-metabolism. Manipulation of the exposure time to optimal redox conditions with substrate amendments, rather than to simply prolong the overall residence time, is recommended for nature-based solutions to tackle target antibiotics.

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The use of vacuum-UV/UV (185/254 nm) for trace organic contaminants (TOrCs) elimination during wastewater treatments has attracted much attention. Advanced oxidation processes which combine VUV/UV and additional oxidants (vacuum-UV/UV-based advanced oxidation processes, VUV/UV-AOPs) provide a promising method for eliminating recalcitrant and toxic TOrCs for wastewater reclamation. Researches in this area are increasing but the promoting effects, mechanisms, and influencing factors have not been well summarized. A comprehensive discussion of the limitations of this technique and future research directions is needed. VUV/UV-AOPs have considerable synergistic effects by increasing usage of VUV/UV photons and the oxidant, which increases radical generation. In terms of elimination kinetics, VUV/UV-AOPs outperform conventional UV-AOPs and VUV/UV processes in most cases; a 1.2-87.7-fold increase of the fluence-based kinetic constant is achieved. In terms of energy efficiency per order (EE/O) of TOrCs elimination, the EE/O of VUV/UV-AOPs only accounts for 4% of UV-AOPs and 63% of VUV/UV. However, VUV/UV-AOPs still need to be further investigated. Firstly, although VUV and UV processes have similar radical formation pathways, limited information is available on the quantum yields of photolysis and radical formation of oxidants under VUV irradiation. Secondly, optimization of VUV/UV-AOPs operating conditions, especially oxidant dosage and water-flow patterns, is needed. Thirdly, VUV/UV-AOPs are significantly inhibited by organic and inorganic matters, but the mechanisms of inhibition on VUV/UV scattering, radical quenching, and radical conversion are not well understood. Such inhibition suggests that the use of VUV/UV-AOPs would be limited to relatively clear water treatment, e.g., reverse osmosis effluent for potable water reuse and ultrapure water production. Related research is needed to establish a clearer scheme for VUV/UV-AOPs in terms of the spatial distribution of radical species in the VUV/UV irradiation system and the relevant optimization method for promoting oxidation performance.

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Recharge of urban stormwater has often been limited by the high cost of land and concerns about contamination of groundwater. To provide a possible solution, we developed an electrochemical advanced oxidation system (UV/H2O2) that is compatible with high-capacity stormwater recharge systems (e.g., drywells). The system employed an air-diffusion cathode to generate a H2O2 stock solution (i.e., typically around 600 mM) prior to the storm event. The H2O2 stock solution was then metered into stormwater and converted into hydroxyl radical (•OH) by an ultraviolet lamp. The energy consumption for H2O2 generation was optimized by adjusting the applied current density and adding an inert salt (e.g., Na2SO4) to stormwater. H2O2 in the stock solution was unstable. By mixing the basic H2O2 containing catholyte and the acidic anolyte, the stability increased, enabling generation of the H2O2 stock solution up to three days prior the storm event with loss of less than 20% of the H2O2. Lab-scale experiments and a kinetic model were used to assess the feasibility of the full-scale advanced oxidation system. System performance decreased at elevated concentrations of dissolved organic carbon in stormwater, due to enhanced light reflection and backscattering at the water-air interface in the UV reactor, competition for UV light absorption with H2O2 and the tendency of organic matter to act as a •OH scavenger. The proposed system can be incorporated into drywells to remove greater than 90% of trace organic contaminants under typical operating conditions. The electrical energy per order of the system is estimated to range from 0.5 to 2 kWh/m3, depending on the dissolved organic carbon concentration.

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Around the globe, on-site wastewater-treatment systems (OWTSs) are critical for rural communities without access to a municipal sewer system. However, their treatment efficiency does not match that of modern wastewater-treatment plants. The impact of OWTS discharge on nearby aquatic ecosystems and their resident fish species is poorly understood. In the present study, larval and adult fathead minnows (Pimephales promelas) and adult sunfish (Lepomis macrochirus) were exposed for 21 days to two trace organic contaminant (TOrC) mixtures replicating water chemistry derived from a previous environmental study. Larval fathead minnows were assessed for survival, growth, predator avoidance, and feeding efficiency. Adult fathead minnows and sunfish were assessed for a suite of physiological endpoints (condition indices, vitellogenin, glucose), histological changes, and fecundity. The only observed effect of TOrC mixture exposure on larval fathead minnows was a decrease in feeding efficiency. Effects were mixed in exposed adult fishes, except for male sunfish which realized a significant induction of vitellogenin (p < 0.05). The consequences of TOrC mixture exposure in the present controlled laboratory study match effects observed in wild-caught sunfish in a corresponding field study. The present study begins to bridge the gap by connecting nonpoint OWTS pollution with biological effects observed in resident lake fish species. Given the effects observed despite the brevity of the laboratory mixture exposure, longer-term studies are warranted to understand the full impacts of OWTS discharge to nearby aquatic ecosystems.  Environ Toxicol Chem 2021;40:3193-3204. © 2021 SETAC. This article has been contributed to by US Government employees and their work is in the public domain in the USA.

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The large number of trace organic contaminants (TrOCs) in wastewater has resulted in severe concerns to human health. Ozonation and UV/H2O2 are widely used to remove TrOCs in wastewater treatment process. Owing to the trace concentrations of TrOCs in wastewater, real-time monitoring of the abatement efficiency of TrOCs through ozonation and UV/H2O2 is quite challenging. Instead of a direct measurement of all the TrOCs, the research community has begun to use different surrogates to monitor the attenuation of TrOCs during AOPs. Various surrogates have been developed over the past few decades. In this review, the different types of surrogates are summarized, including ultraviolet spectroscopy and fluorescence spectroscopy. Strong linear correlations have been found for the removal of TrOCs using AOPs, and the abatement of UV absorption spectroscopy at 254 nm or total fluorescence (TF). Moreover, a two-phase linear correlation can better describe the ozone-resistant TrOCs compared with a single linear correlation. Two different kinds of predictive models exist that use surrogates as the input for ozonation: the regression model and kinetic model. The development of the models requires a further understanding of the impacts of water quality, seasonal variations, and storm events on the kinetic parameters. For the in situ monitoring system, the light-emitting diode (LED) is one of the most promising light sources, although the sensitivity and accuracy still need to be improved.

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Urbanization can dramatically alter stormwater, both the quantity and quality, by engendering larger peak flows and through the introduction of contaminants into runoff. The current study builds on previous research that developed relationships between a suite of nonpoint source contaminants, known as trace organic contaminants (TOrCs), and hydrologic measurements for a series of storms (one site had 15 storms and the other had 19 storms) in Madison, WI, by creating statistical and deterministic models. Correlations and regressions were calculated between TOrC loads and hydrologic measurements for a series of storms for both a commercial site and a high-density residential site. From the regressions, it became evident that loading responses to precipitation were not the same between the two land covers for some TOrCs, indicating varying load responses for TOrCs depending on land cover. The regressions were utilized in the Source Loading and Management Model for Windows (WinSLAMM), an event-based hydrologic and water-quality model, to demonstrate that it can be used to model novel contaminants. The regressions were also used to estimate mean annual loads of TOrCs from all commercial and high-density residential areas in Madison, WI, for the watersheds to which Madison discharges its stormwater. The mean annual loads varied between grams per year to tens of thousands of grams per year depending on the TOrC and watershed. This work will ultimately allow managers to simulate the presence of, establish total maximum daily loads for, and mitigate the loads of TOrCs through stormwater best management practices.

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Powdered activated carbon (PAC) for organic micro-pollutant (OMP) removal can be applied effectively on wastewater treatment plant (WWTP) effluents by using re-circulation schemes, accumulating the PAC in the system. This technique is complex because several factors are unknown: (i) the PAC concentration in the system, (ii) specific and average contact times of PAC particles, and (iii) PAC particle loadings with target compounds/competing water constituents. Thus, performance projections (e.g. in the lab) are very challenging. We sampled large-scale PAC plants with PAC sludge re-circulation on eight different WWTPs. The PAC plant-induced OMP removals were notably different, even when considering PAC concentrations in proportion to background organic sum parameters. The variability is likely caused by differing PAC products, varying water composition, differently effective plant/re-circulation operation, and variable biodegradation. Plant PAC samples and parts of the PAC plant influent samples were used in laboratory tests, applying multiples (0.5, 1, 2, 4) of the respective large-scale "fresh" PAC doses, and several fixed contact times (0.5, 1, 2, 4, 48 h). The aim was to empirically identify suitable combinations of lab PAC dose (as multiples of the plant PAC dose) and contact time, which represent the PAC plant performances in removing OMPs (for specific OMPs at single locations, and for averages of different OMPs at all locations). E.g., for five well adsorbing, little biodegradable OMPs, plant performances can be projected by using a lab PAC dose of twice the respective full-scale PAC dose and 4 h lab contact time (standard deviation of 13 %-points).

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On-site wastewater treatment systems (OWTSs) are an international wastewater management strategy for rural and semi-rural communities without access to centralized sewage treatment. These systems are a suspected source of trace organic contaminants (TOrCs) that may be responsible for endocrine disrupting effects to resident fish species in Minnesota Lakes. This study assessed localized porewater concentrations of TOrCs in near-shore environments across five Minnesota Lakes. Sampling sites were designated as either likely (HOME) or unlikely (REF) to receive OWTS discharges based on their proximity to shoreline households. Sampling sites also served as sunfish spawning habitats concurrently studied for biological impacts to resident adult males. Two-group hypothesis tests demonstrated significantly (p = .02) higher total TOrC concentrations in HOME (Mean = 841 ng/L) versus REF (Mean = 222 ng/L) sites. HOME sites also contained a wider suite of TOrC detections relative to REF sites. The distance to the nearest household (most proximal distance; MPD) negatively correlated (r = -0.62) with total TOrC concentrations. However, 2,4-D and DEET were major contributors to these total concentrations, suggesting that anthropogenic influence from households may not be exclusively attributed to OWTS discharges. Further, TOrC presence and elevated nitrogen concentrations in REF site porewater suggest additional, non-household TOrC discharges to these lakes. Significantly higher blood concentrations of vitellogenin (p = .03) and 11-ketotestosterone (p = .01) were observed in adult male sunfish captured from HOME versus REF sites. Comparisons between chemical and biological data indicate enhanced bioactive effects of co-contaminants. The findings from this study demonstrate multiple diffuse transport pathways contribute to the presence of biologically active TOrC mixtures in Minnesota Lakes, and mitigation efforts should consider minimizing residential inputs of chemicals associated with both outdoor and OWTS activity.

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We investigated transport mechanisms of trace organic contaminants (TrOCs) through aquaporin thin-film composite forward osmosis (FO) membrane, and membrane stability under extreme conditions with respect to TrOC rejections. Morphology and surface chemistry of the aquaporin membrane were characterised to identify the incorporation of aquaporin vesicles into membrane active layer. Pore hindrance model was used to estimate aquaporin membrane pore size as well as to describe TrOC transport. TrOC transport mechanisms were revealed by varying concentration and type of draw solutions. Experimental results showed that mechanism of TrOC transport through aquaporin-embedded FO membrane was dominated by solution-diffusion mechanism. Non-ionic TrOC rejections were molecular-weight dependent, suggesting steric hindrance mechanisms. On the other hand, ionic TrOC rejections were less sensitive to molecular size, indicating electrostatic interaction. TrOC transport through aquaporin membrane was also subjected to retarded forward diffusion where reverse draw solute flux could hinder the forward diffusion of feed TrOC solutes, reducing their permeation through the FO membrane. Aquaporin membrane stability was demonstrated by either heat treatment or ethanol solvent challenges. Thermal stability of the aquaporin membrane was manifested as a relatively unchanged TrOC rejection before and after the heat treatment challenge test. By contrast, ethanol solvent challenge resulted in a decrease in TrOC rejection, which was evident by the disappearance of the lipid tail of the aquaporin vesicles from infrared spectrum and a notable decrease in the membrane pore size.

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In this study, we investigated the performance of an osmotic membrane bioreactor (OMBR) enabled by a novel biomimetic aquaporin forward osmosis (FO) membrane. Membrane performance and removal of 30 trace organic contaminants (TrOCs) were examined. Results show that the aquaporin FO membrane had better transport properties in comparison with conventional cellulose triacetate and polyamide thin-film composite FO membranes. In particular, the aquaporin FO membrane exhibited much lower salt permeability and thus smaller reverse salt flux, resulting in a less severe salinity build-up in the bioreactor during OMBR operation. During OMBR operation, the aquaporin FO membrane well complemented biological treatment for stable and excellent contaminant removal. All 30 TrOCs selected here were removed by over 85% regardless of their diverse properties. Such high and stable contaminant removal over OMBR operation also indicates the stability and compatibility of the aquaporin FO membrane in combination with activated sludge treatment.

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The impacts of four simulated hazardous events, namely, aeration failure, power loss, and chemical shocks (ammonia or bleach) on the performance of an anoxic-aerobic membrane bioreactor (MBR) receiving real wastewater were investigated. Hazardous events could alter pH and/or oxidation reduction potential of the mixed liquor and inhibit biomass growth, thus affecting the removal of bulk organics, nutrients and trace organic contaminants (TrOC). Chemical shocks generally exerted greater impact on MBR performance than aeration/power failure events, with ammonia shock exerting the greatest impact. Compared to total organic carbon, nutrient removal was more severely affected. Removal of the hydrophilic TrOCs that are resistant and/or occur at high concentrations in wastewater was notably affected. The MBR effectively reduced estrogenicity and toxicity from wastewater, but chemical shocks could temporarily increase the endocrine activity of the effluent. Depending on the chemical shock-dose and the membrane flux, hazardous events can exacerbate membrane fouling.

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Simultaneous nitrification/denitrification and trace organic contaminant (TrOC) removal during wastewater treatment by an integrated anoxic-aerobic MBR was examined. A set of 30 compounds was selected to represent TrOCs that occur ubiquitously in domestic wastewater. The system achieved over 95% total organic carbon (TOC) and over 80% total nitrogen (TN) removal. In addition, 21 of the 30 TrOCs investigated here were removed by over 90%. Low oxidation reduction potential (i.e., anoxic/anaerobic) regimes were conducive to moderate to high (50% to 90%) removal of nine TrOCs. These included four pharmaceuticals and personal care products (primidone, metronidazole, triclosan, and amitriptyline), one steroid hormone (17ß-estradiol-17-acetate), one industrial chemical (4-tert-octylphenol) and all three selected UV filters (benzophenone, oxybenzone, and octocrylene). Internal recirculation between the anoxic and aerobic bioreactors was essential for anoxic removal of remaining TrOCs. A major role of the aerobic MBR for TOC, TN, and TrOC removal was observed.

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BACKGROUND: The widespread utilization of organic compounds in modern society and their dispersion through wastewater have resulted in extensive contamination of source and drinking waters. The vast majority of these compounds are not regulated in wastewater outfalls or in drinking water while trace amounts of certain compounds can impact aquatic wildlife. Hence it is prudent to monitor these contaminants in water sources until sufficient toxicological data relevant to humans becomes available. A method was developed for the analysis of 36 trace organic contaminants (TOrCs) including pharmaceuticals, pesticides, steroid hormones (androgens, progestins, and glucocorticoids), personal care products and polyfluorinated compounds (PFCs) using a single solid phase extraction (SPE) technique with ultra-high performance liquid chromatography coupled to tandem mass spectrometry (UHPLC-MS/MS). The method was applied to a variety of water matrices to demonstrate method performance and reliability. RESULTS: UHPLC-MS/MS in both positive and negative electrospray ionization (ESI) modes was employed to achieve optimum sensitivity while reducing sample analysis time (<20 min) compared with previously published methods. The detection limits for most compounds was lower than 1.0 picogram on the column while reporting limits in water ranged from 0.1 to 15 ng/L based on the extraction of a 1 L sample and concentration to 1 mL. Recoveries in ultrapure water for most compounds were between 90-110%, while recoveries in surface water and wastewater were in the range of 39-121% and 38-141% respectively. The analytical method was successfully applied to analyze samples across several different water matrices including wastewater, groundwater, surface water and drinking water at different stages of the treatment. Among several compounds detected in wastewater, sucralose and TCPP showed the highest concentrations. CONCLUSION: The proposed method is sensitive, rapid and robust; hence it can be used to analyze a large variety of trace organic compounds in different water matrixes.