Upstream Wastewater Treatment Plant Research Articles

Online trend estimation and detection of trend deviations in sub-sewershed time series of SARS-CoV-2 RNA measured in wastewater

Wastewater surveillance has proven a cost-effective key public health tool to understand a wide range of community health diseases and has been a strong source of information on community levels and spread for health departments throughout the SARS- CoV-2 pandemic. Studies spanning the globe demonstrate the strong association between virus levels observed in wastewater and quality clinical case information of the population served by the sewershed. Few of these studies incorporate the temporal dependence present in sampling over time, which can lead to estimation issues which in turn impact conclusions. We contribute to the literature for this important public health science by putting forward time series methods coupled with statistical process control that (1) capture the evolving trend of a disease in the population; (2) separate the uncertainty in the population disease trend from the uncertainty due to sampling and measurement; and (3) support comparison of sub-sewershed population disease dynamics with those of the population represented by the larger downstream treatment plant. Our statistical methods incorporate the fact that measurements are over time, ensuring correct statistical conclusions. We provide a retrospective example of how sub-sewersheds virus levels compare to the upstream wastewater treatment plant virus levels. An on-line algorithm supports real-time statistical assessment of deviations of virus level in a population represented by a sub-sewershed to the virus level in the corresponding larger downstream wastewater treatment plant. This information supports public health decisions by spotlighting segments of the population where outbreaks may be occurring.

Assessment of bioactive chemicals in wastewater effluents and surface waters using in vitro bioassays in the Nakdong River basin, Korea

Organic micropollutants present in effluents of wastewater treatment plants (WWTPs) can negatively affect the quality of receiving waters or drinking water sources. The present work monitored the concentration of bioactive chemicals using a battery of in vitro bioassays in 14 WWTP effluents, 2 effluent-dominant streams, and 5 river waters in the Nakdong River basin, Korea, for a two-year period. The WWTP effluents showed AR/ERα/TRβ (androgen/estrogen/thyroid hormone) activities at a few to tens ng/L, PAH/PPARγ/p53 (polycyclic-aromatic-hydrocarbon/lipid metabolism/genotoxicity) activities at hundreds ng/L, and PXR/Nrf2 (xenobiotic metabolism/oxidative stress) activities at tens to hundreds μg/L as bioanalytical equivalent concentrations. The concentration level and type of bioactivities were statistically not affected by the source, season, or treatment processes of WWTPs for most endpoints. The effluent-dominant streams showed similar levels of AR/ERα/PAH/PXR/Nrf2 activities compared to the upstream WWTP effluents. The river waters showed lower levels of AR/ERα activities (by factors of 6 or 7) but had only slightly lower PAH/PXR/Nrf2 activities (within factors of 2) than the WWTP effluents when compared based on median concentration. Cytotoxicity was below the quantification limit (0.3 μg/L) in most effluent and river samples. For ERα/PAH/PXR/Nrf2, the median bioactivity levels of the river waters were higher than at least one of the effect-based trigger (EBT) values proposed in the literature. Further monitoring work and reliable/realistic EBT derivation are needed to determine possible ecological risks posed by the observed bioactivities.

Effects of municipal wastewater effluents on the digestive gland microbiome of wild freshwater mussels (Lasmigona costata)

Gut microbial communities are vital for maintaining host health, and are sensitive to diet, environment, and chemical exposures. Wastewater treatment plants (WWTPs) release effluents containing antimicrobials, pharmaceuticals, and other contaminants that may negatively affect the gut microbiome of downstream organisms. This study investigated changes in the diversity and composition of the digestive gland microbiome of flutedshell mussels (Lasmigona costata) from upstream and downstream of two large (service >100,000) WWTPs. Mussel digestive gland microbiome was analyzed following the extraction, PCR amplification, and sequencing of bacterial DNA using the V3-V4 hypervariable regions of the 16 S rRNA gene. Bacterial alpha diversity decreased at sites downstream of the second WWTP and these sites were dissimilar in beta diversity from sites upstream and downstream of the first upstream WWTP. The microbiomes of mussels collected downstream of the first WWTP had increased relative abundances of Actinobacteria, Bacteroidetes, and Firmicutes, with a decrease in Cyanobacteria, compared to upstream mussels. Meanwhile, those collected downstream of the second WWTP increased in Proteobacteria and decreased in Actinobacteria, Bacteroidetes, and Tenericutes. Increased Proteobacteria has been linked to adverse effects in mammals, but their functions in mussels is currently unknown. Finally, effluent-derived bacteria were found in the microbiome of mussels downstream of both WWTPs but not in those from upstream. Overall, results show that the digestive gland microbiome of mussels collected upstream and downstream of WWTPs differed, which has implications for altered host health and the transport of WWTP-derived bacteria through aquatic ecosystems.

Distribution and characteristics of wastewater treatment plants within the global river network

Abstract. The main objective of wastewater treatment plants (WWTPs) is to remove pathogens, nutrients, organics, and other pollutants from wastewater. After these contaminants are partially or fully removed through physical, biological, and/or chemical processes, the treated effluents are discharged into receiving waterbodies. However, since WWTPs cannot remove all contaminants, especially those of emerging concern, they inevitably represent concentrated point sources of residual contaminant loads into surface waters. To understand the severity and extent of the impact of treated-wastewater discharges from such facilities into rivers and lakes, as well as to identify opportunities of improved management, detailed information about WWTPs is required, including (1) their explicit geospatial locations to identify the waterbodies affected and (2) individual plant characteristics such as the population served, flow rate of effluents, and level of treatment of processed wastewater. These characteristics are especially important for contaminant fate models that are designed to assess the distribution of substances that are not typically included in environmental monitoring programs. Although there are several regional datasets that provide information on WWTP locations and characteristics, data are still lacking at a global scale, especially in developing countries. Here we introduce a spatially explicit global database, termed HydroWASTE, containing 58 502 WWTPs and their characteristics. This database was developed by combining national and regional datasets with auxiliary information to derive or complete missing WWTP characteristics, including the number of people served. A high-resolution river network with streamflow estimates was used to georeference WWTP outfall locations and calculate each plant's dilution factor (i.e., the ratio of the natural discharge of the receiving waterbody to the WWTP effluent discharge). The utility of this information was demonstrated in an assessment of the distribution of treated wastewater at a global scale. Results show that 1 200 000 km of the global river network receives wastewater input from upstream WWTPs, of which more than 90 000 km is downstream of WWTPs that offer only primary treatment. Wastewater ratios originating from WWTPs exceed 10 % in over 72 000 km of rivers, mostly in areas of high population densities in Europe, the USA, China, India, and South Africa. In addition, 2533 plants show a dilution factor of less than 10, which represents a common threshold for environmental concern. HydroWASTE can be accessed at https://doi.org/10.6084/m9.figshare.14847786.v1 (Ehalt Macedo et al., 2021).

Evaluating the impacts of contrasting sewage treatment methods on nutrient dynamics across the River Wensum catchment, UK

Sewage effluent discharged from wastewater treatment plants (WWTPs) is a major driver of nitrogen (N) and phosphorus (P) enrichment, but tertiary treatment methods such as P-stripping have previously been shown to mitigate eutrophication risk. The aim of this study was to evaluate the impacts of sewage effluent discharged from WWTPs with contrasting classifications of tertiary treatment on nutrient dynamics across the River Wensum catchment, UK. River water samples were collected from 20 locations across the catchment at monthly intervals between October 2010 and September 2013, with 677 samples collected in total and analysed for a suite of hydrochemical parameters. The 20 sampling locations were divided into four classifications based on the type of upstream WWTP: (1) no WWTP; (2) WWTPs without P-stripping; (3) WWTPs with and without P-stripping; (4) WWTPs with P-stripping. Results revealed substantial overlaps in riverine nutrient composition making differentiation between classifications difficult. The majority of N (>97%) and P (~75%) was present in dissolved bioavailable forms across all sites and there was no significant difference in total N speciation between classifications. Total P (TP) speciation did, however, reveal higher proportions of particulate P at sites with no WWTP, indicating a greater P contribution of agricultural origin. Ratios of total dissolved to particulate P (TDP:TPP) and chloride concentrations proved effective discriminators of agricultural and sewage P, respectively, but phosphate‑boron ratios (PO4:B) were ineffective discriminators in this catchment. Most importantly, there was no evidence that P-stripping reduced overall TP concentrations downstream of WWTPs, despite evidence of a per capita reduction, nor reduced the proportion of dissolved P released. These findings were attributed to P-stripping facilities serving larger populations and thus releasing greater effluent P load, thereby demonstrating that the presence of tertiary P-stripping alone is insufficient to overcome population pressures and ensure that rivers achieve good hydrochemical status.

Contribution of wastewater- versus non-wastewater-derived sources to haloacetonitriles formation potential in a wastewater-impacted river

Population growth and urbanization have led to the increasing presence of treated wastewater effluents in downstream drinking water sources. Drinking water sources influenced by organic matter from upstream wastewater treatment plant (WWTP) effluents are thought prone to the formation of haloacetonitriles (HANs), a group of nitrogenous disinfection by-products (DBPs) that can exhibit higher toxicity than currently regulated carbonaceous DBPs. We develop a framework for studying the HAN formation potential (HAN-FP) considering the WWTP and non-WWTP related sources of HAN precursors, and apply this framework to a representative WWTP-impacted river, the Illinois River, USA. A spatiotemporally-resolved river hydrodynamic and water quality model is developed using HEC-RAS to quantify the contribution of WWTP versus non-WWTP sources of HAN-FP precursors. Results show that non-WWTP sources of HAN-FP are considerable, accounting for up to 78% of HAN-FP concentration. Moreover, the contribution of the two sources varies due to streamflow discharge variability. During lower flows, the contribution of WWTPs drives the high concentration of HAN-FP and during higher flows, the contribution of non-WWTP sources becomes dominant. As a result, a high risk of HAN-FP may exist persistently (HAN-FP concentration is always larger than 9.7 μg/L in this study), not only during low flows but also during high flows due to both wastewater- and non-wastewater-derived HAN-FP sources.

Adding the Mureş River Basin (Transylvania, Romania) to the List of Hotspots with High Contamination with Pharmaceuticals

Background: The Mureș River Basin is a long-term heavily polluted watershed, in a situation of climate changes with decreasing water flow and related decreasing dilution capacity. Here, a mixture of emerging pollutants such as pharmaceuticals were targeted to reveal potential risks regarding the natural lotic ecosystems. Due to the continuous discharge into the environment, pharmaceuticals are gaining persistent organic pollutant characteristics and are considered emerging pollutants. Based on the hazard quotient, this research highlights the dangerous concentrations of carbamazepine, ibuprofen, furosemide, and enalapril in river water. Results: High levels of four pharmaceutical compounds (carbamazepine, ibuprofen, furosemide, and enalapril) and some of their derived metabolites (enalaprilat, carboxyibuprofen, 1-hydroxyibuprofen, and 2-hydroxyibuprofen) were reported in our study in the Mureș River Basin. Overall, pharmaceutical concentrations were found to be highest in the wastewater treatment plant (WWTP) effluent, median downstream of the WWTP, and lowest upstream of the WWTP, as was expected. For all pharmaceutical compounds tested, we recorded concentrations above the limit of quantification (LOQ) in at least one of the sites tested. Carbamazepine exhibited the highest mean values upstream, downstream, and at the WWTP. As expected, the highest concentrations for all the studied pharmaceutical compounds were detected in the WWTP effluent. All Hazard Quotient (HQ) values were below one (on a logarithmic scale in base 10), with the highest values in the WWTP and the lowest in the river upstream of the WWTP. The HQ intervals were in the same range for furosemide, carbamazepine, and ibuprofen at each of the three different sites: upstream WWTP effluent, and downstream. The interval for enalapril stands out as having the lowest HQ at all three sites. Conclusions: Based on these results, the large and complex hydrographical system Mureș River Basin was transformed from a grey area, with little information about pharmaceutical contamination, to a hotspot in terms of contamination with emerging pollutants. Pharmaceutical compound concentrations were found to be the highest in WWTP effluents. The WWTP effluent concentrations were among the highest in Europe, indicating that treatment plants are the primary source of water pollution with pharmaceuticals compounds. The detected levels were higher than the safety limit for carbamazepine and ibuprofen. The determined HQ values imply that the measured levels do pose a threat to the environment for the studied pharmaceuticals. Based on the obtained results, human communities can assess, monitor, predict, and adapt in time to these already-present regional challenges and risks for sustainable use of natural resources, including water and associated products and services.

Triclosan export from low-volume sources in an urban to rural watershed

Triclosan (TCS), an emerging contaminant linked to antimicrobial resistance, has been the focus of many surface water studies to date. However, these initial studies have predominantly used sampling locations downstream of large volume (i.e., >0.5 million gallons per day) wastewater treatment plants (WWTPs). This approach overlooks potential inputs from their low volume counterparts as well as non-point sources, such as sewage network leaks, biosolid application to agricultural fields and leach fields associated with septic systems. Here we examine the range of concentrations, overall loading, and potential controls on TCS delivery to the East Branch of the Brandywine Creek (EBBC), a rural to suburban watershed located in southeastern Pennsylvania. TCS measurements were collected from 13 locations in the EBBC during baseflow conditions and immediately following a storm event. A regulatory database review identified WWTP density an order of magnitude greater than the national average, thereby confirming their pervasiveness in rural to urban systems. Detectable concentrations of TCS in the EBBC ranged from 0.2 to 0.6 ng/L during baseflow conditions and 0.5 to over 1000 ng/L following a storm event. The lack of a statistical relationship between TCS concentrations and yields with the number of upstream WWTPs and/or volume of treated effluent during both sampling periods confirm the importance of individual WWTP practices and the volume of the receiving water body, while a positive statistically-significant relationship between TCS concentrations and upstream developed open space following the storm event was likely influenced by runoff of spray-applied treated wastewater and/or sewage network leaks. Furthermore, the presence of detectable concentrations of TCS in sub-watersheds with no WWTP systems implies field applied biosolids or treated wastewater, as well as septic tank related leach fields are all viable sources of TCS. These findings suggest we must greatly expand our consideration of sources for emerging contaminants in waterways.

Wastewater-borne exposure of limnic fish to anticoagulant rodenticides

The recent emergence of second-generation anticoagulant rodenticides (AR) in the aquatic environment emphasizes the relevance and impact of aquatic exposure pathways during rodent control. Pest control in municipal sewer systems of urban and suburban areas is thought to be an important emission pathway for AR to reach wastewater and municipal wastewater treatment plants (WWTP), respectively. To circumstantiate that AR will enter streams via effluent discharges and bioaccumulate in aquatic organisms despite very low predicted environmental emissions, we conducted a retrospective biological monitoring of fish tissue samples from different WWTP fish monitoring ponds exclusively fed by municipal effluents in Bavaria, Germany. At the same time, information about rodent control in associated sewer systems was collected by telephone survey to assess relationships between sewer baiting and rodenticide residues in fish. In addition, mussel and fish tissue samples from several Bavarian surface waters with different effluent impact were analyzed to evaluate the prevalence of anticoagulants in indigenous aquatic organisms.Hepatic AR residues were detected at 12 out of 25 WWTP sampling sites in the low μg/kg range, thereof six sites with one or more second-generation AR (i.e., brodifacoum, difenacoum, bromadiolone). 14 of 18 surveyed sites confirmed sewer baiting with AR and detected hepatic residues matched the reported active ingredients used for sewer baiting at six sites. Furthermore, second-generation AR were detected in more than 80% of fish liver samples from investigated Bavarian streams. Highest total hepatic AR concentrations in these fish were 9.1 and 8.5 μg/kg wet weight, respectively and were observed at two riverine sampling sites characterized by close proximity to upstream WWTP outfalls. No anticoagulant residues were found in fish liver samples from two lakes without known influences of effluent discharges.The findings of our study clearly show incomplete removal of anticoagulants during conventional wastewater treatment and confirm exposure of aquatic organisms via municipal effluents. Based on the demonstrated temporal and spatial coherence between sewer baiting and hepatic AR residues in effluent-exposed fish, sewer baiting in combined sewer systems contributes to the release of active ingredients into the aquatic environment.

Spatial patterns of water quality impairments from point source nutrient loads in Germany's largest national River Basin (Weser River)

We employed the well-established Horton-Strahler, hierarchical, stream-order (ω) scheme to investigate scaling of nutrient loads (P and N) from ~845 wastewater treatment plants (WWTPs) distributed along the river network in urbanized Weser River, the largest national basin in Germany (~46K km2; ~8.4 million population). We estimated hydrologic and water quality impacts at the reach- and basin-scales, at two steady river discharge conditions (median flow, QR50; low-flow, QR90). Of the five WWTPs class-sizes (1 ≤ k ≤ 5), ~68% discharge to small low-order streams (ω < 3). We found large variations in capacity to dilute WWTP nutrient loads because of variability in (1) treated wastewater discharge (QU) within and among different class-sizes, and (2) river discharge (QR) within low-order streams (ω < 3) resulting from differences in drainage areas. For QR50, reach-scale water quality impairment assessed by nutrient concentration was likely at 136 (~16%) locations for P and 15 locations (~2%) for N. About 90% of these locations were lower-order streams (ω < 3). At QR50 and only with dilution, basin-scale cumulative nutrient loads from multiple upstream WWTPs increase impaired locations to 266 (~32% of total) for P. Considering in-stream uptake decreased P-impaired streams to 225 (~27%), suggesting the dominant role of dilution in the Weser River basin. Role of in-stream uptake diminished along the flow paths, while dilution in larger streams (4 ≤ ω ≤ 7) minimizes the impact of WWTP loads. Under QR90 conditions [(QR50/QR90) ~ 2.5], water quality impaired locations will likely double for the basin-scale analyses. Long-term water quality data suggested that diffuse sources are the primary contributors for water quality impairments in large streams. Our data-modeling synthesis approach is transferable to other urbanized river basins and extends understanding of point source impacts on water quality across spatial scales.

Four decades of water quality change in the upper San Francisco Estuary

Quantitative descriptions of chemical, physical, and biological characteristics of estuaries are critical for developing an ecological understanding of drivers of change. Historical trends and relationships between key species of dissolved inorganic nitrogen (ammonium, nitrate/nitrite, total) from the Delta region of the San Francisco Estuary were modelled with an estuarine adaptation of the Weighted Regressions on Time, Discharge, and Season (WRTDS). Analysis of flow-normalized data revealed trends that were different from those in the observed time-series. Flow-normalized data exhibited changes in magnitude and even reversal of trends relative to the observed data. Modelled trends demonstrated that nutrient concentrations were on average higher in the last twenty years relative to the earlier periods of observation, although concentrations have been slowly declining since the mid-1990s and early 2000s. We further describe mechanisms of change with two case studies that evaluated 1) downstream changes in nitrogen following upgrades at a wastewater treatment plant, and 2) interactions between biological invaders, chlorophyll, macro-nutrients (nitrogen and silica), and flow in Suisun Bay. WRTDS results for ammonium trends showed a distinct signal as a result of upstream wastewater treatment plant upgrades, with specific reductions observed in the winter months during low-flow conditions. Results for Suisun Bay showed that chlorophyll a production in early years was directly stimulated by flow, whereas the relationship with flow in later years was indirect and influenced by grazing pressure. Although these trends and potential causes of change have been described in the literature, results from WRTDS provided an approach to test alternative hypotheses of spatiotemporal drivers of nutrient dynamics in the Delta.

Modeled De Facto Reuse and Contaminants of Emerging Concern in Drinking Water Source Waters.

De facto reuse is the percentage of drinking water treatment plant (DWTP) intake potentially composed of effluent discharged from upstream wastewater treatment plants (WWTPs). Results from grab samples and a De Facto Reuse in our Nation's Consumable Supply (DRINCS) geospatial watershed model were used to quantify contaminants of emerging concern (CECs) concentrations at DWTP intakes to qualitatively compare exposure risks obtained by the two approaches. Between nine and 71 CECs were detected in grab samples. The number of upstream WWTP discharges ranged from 0 to >1,000; comparative de facto reuse results from DRINCS ranged from <0.1 to 13% during average flow and >80% during lower streamflows. Correlation between chemicals detected and DRINCS modeling results were observed, particularly DWTPs withdrawing from midsize water bodies. This comparison advances the utility of DRINCS to identify locations of DWTPs for future CEC sampling and treatment technology testing.

Influence of Bizerte city wastewater treatment plant (WWTP) on abundance and antibioresistance of culturable heterotrophic and fecal indicator bacteria of Bizerte Lagoon (Tunisia)

The waste water treatment plant (WWTP) of the city of Bizerte concentrates different types of chemical and biological pollutants in the Bizerte lagoon (Tunisia). Considering four upstream and downstream WWTP discharge stations, seventy nine, culturable bacterial strains were isolated and identified from water and sediment as fecal coliforms, fecal streptococci, pathogenic staphylococci and non-enterobacteriacea. Fecal coliforms were most abundant (2.5 105 bacteria/mg) in sediment of WWTP discharge. Leuconostoc spp (23.1%) and Chryseomonasluteola (23.1%) were the most prevalent culturable fecal indicator bacteria (FIB) isolated at the upstream discharge stations. However, Staphylococcus xylosus (13.9%) was the most prevalent culturable FIB isolated at the WWTP discharge stations. Moreover, high antibioticresistance phenotypes were present in all sampling stations, but especially in WWTP discharge station in both water and sediment. Resistance levels in water and sediment, respectively were amoxicillin (58.8%; 34.8%), penicillin (50%; 31.6%), oxacillin (60%; 33.3%), cefotaxim (55.2%; 39.1%), ceftazidim (66.7%; 50%), gentamycin (42.9%; 38.9%), tobramycin (50%; 25%), vancomycin (33.3; 71.4%), amikacin (66.7%; 0%) and ciprofloxacin (100%; 100%). Interestingly, ß-lactam antibiotic resistant FIB were mostly isolated from water as well as from sediments of upstream and WWTP discharge station. Canonical correspondence analysis CCA correlating antibiotic resistance profile with the abiotic data showed that, in water column, culturable bacterial strains isolated in upstream WWTP discharge stations were interestingly correlated with the resistance to amikacin, oxacillin, cefotaxim, ciprofloxacin and gentamycin, however, in sediment, they were correlated with the resistance to amoxicillin, oxacillin, céfotaxim and vancomycin. Serious ß-lactams and aminoglycosides acquired resistance appeared mainly in fecal streptococci and pathogen staphylococci groups.

Comparison of dilution factors for German wastewater treatment plant effluents in receiving streams to the fixed dilution factor from chemical risk assessment

Incomplete removal during wastewater treatment leads to frequent detection of compounds such as pharmaceuticals and personal care products in municipal effluents. A fixed standard dilution factor of 10 for effluents entering receiving water bodies is used during the exposure assessment of several chemical risk assessments. However, the dilution potential of German receiving waters under low flow conditions is largely unknown and information is sparse for other European countries. We calculated dilution factors for two datasets differing in spatial extent and wastewater treatment plant (WWTP) size: a national dataset comprising 1225 large WWTPs in Central and Northern Germany and a federal dataset for 678 WWTPs of a single state in Southwest Germany. We found that the fixed factor approach overestimates the dilution potential of 60% and 40% of receiving waters in the national and the federal dataset, with median dilution factors of 5 and 14.5, respectively. Under mean flow conditions, 8% of calculated dilution factors were below 10, with a median dilution factor of 106. We also calculated regional dilution factors that accounted for effluent inputs from upstream WWTPs. For the national and the federal dataset, 70% and 60% of calculated regional dilution factors fell below 10 under mean low flow conditions, respectively. Decrease of regional dilution potential in small receiving streams was mainly driven by the next WWTP upstream with a 2.5 fold drop of median regional dilution factors. Our results show that using the standard dilution factor of 10 would result in the underestimation of environmental concentrations for authorised chemicals by a factor of 3–5 for about 10% of WWTPs, especially during low flow conditions. Consequently, measured environmental concentrations might exceed predicted environmental concentrations and ecological risks posed by effluents could be much higher, suggesting that a revision of current risk assessment practices may be required.

Presence of pharmaceuticals in the Lis river (Portugal): Sources, fate and seasonal variation

The occurrence of 33 pharmaceuticals and metabolites was evaluated along the Lis river and in the influents and effluents of two wastewater treatment plants (WWTPs) located along the river. Results indicate that pharmaceuticals, such as ibuprofen, ketoprofen, carbamazepine and fluoxetine, and the metabolite salicylic acid are widespread along the Lis river, showing 100% of detection frequency, at levels up to 1.3μgL–1. The number of molecules detected increased along the river, with 11 molecules in the source, 15 upstream WWTP 1, 16 downstream WWTP 1 and upstream WWTP 2 and 19 downstream WWTP 2. The highest concentrations were often found downstream near the river mouth. Different possible sources of contamination of the Lis river were identified, namely WWTP effluents, untreated wastewaters and livestock production. Nevertheless, the discharge of WWTP effluents appeared to be the most pronounced, given that, in general, it was noticed an increase in the concentration of pharmaceuticals downstream of the WWTPs. WWTP effluents contributed with a total mass load of pharmaceuticals into the Lis river between 470 and 2317mg/d/1000 inhabitants. Non-steroidal anti-inflammatory drugs/analgesics were the therapeutic group with a high contribution to the total mass load of pharmaceuticals entering the Lis river, followed by psychiatric drugs and antibiotics. No seasonal variation was observed for the detected concentrations of pharmaceuticals. At the levels detected in the Lis river, sulfamethoxazole, clarithromycin, azithromycin and ibuprofen showed to have potential risk for aquatic organisms. These findings show that further studies embracing different environmental compartments (water, sediment and biota) are needed, in order to evaluate the partition/distribution of pharmaceuticals, their metabolites and transformation products in the environment as well as to predict their possible impact to non-target organisms and, in a last instance, to human health.

Occurrence, removal, and environmental impacts of emerging contaminants detected in water and wastewater in Southern Ontario—Part I: occurrence and removal

A comprehensive study was conducted at two wastewater treatment plants (WWTPs) and one water treatment plant (WTP) in Windsor, Ontario, Canada. The occurrence of 220 emerging and legacy compounds, their removal efficiencies by the existing treatment processes, and their potential environmental impacts were studied. The results are reported in a two part paper. In this part (I), the occurrence and removal efficiencies are presented. Three of the 47 target pharmaceutically active compounds (PhACs) and endocrine disrupting compounds (EDCs) contributed 89–96% of the total concentration of PhACs/EDCs in the WWTP influents. They were acetaminophen, ibuprofen, and naproxen. The existing treatment processes successfully removed between 95 and 98% of ‘all’ PhACs/EDCs, primarily due to the high removal rates of these three analgesics. Concentrations of PhACs/EDCs detected at the WTP intake were two to three orders of magnitude lower than those in the effluent of the upstream WWTP. These concentrations remained relatively unchanged in the finished drinking water, indicating the WTP's low removal efficiency for trace amounts of them. Polybrominated diphenyl ethers (PBDEs) were detected at concentrations as high as 150 ng/L (for PBDE-209) in the WWTPs’ influent, and removed at 86–96% efficiency. PDBE effluent concentrations were mostly below 1 ng/L at both WWTPs, with a maximum of 9 ng/L for PBDE-209. Octylphenol, nonylphenol, and nonylphenol ethoxylates concentrations were monitored in one WWTP's effluent, and ranged between undetectable and 286 ng/L (LoDs varied between 1.3 and 15.2 ng/L).

Sources and transport of contaminants of emerging concern: A two-year study of occurrence and spatiotemporal variation in a mixed land use watershed

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.

Increasing nitrate concentrations in streams draining into Lake Ontario

Abstract Nitrate (NO 3 -N) concentrations in offshore waters of Lake Ontario increased by approximately 60% between the 1970s and 2000s, although the drivers are unclear. Here, we show that NO 3 -N concentrations also increased significantly in at least one season at 13 of 15 large southern Ontario tributaries (8.4 to 2779 km 2 ) that drain into Lake Ontario and have no known upstream wastewater treatment plants. Average NO 3 -N concentrations more than doubled between the 1970s and 2000s at some streams. Only the two most urbanized streams did not show any increase in NO 3 -N and NO 3 -N declined at the most urbanized catchment in this study (Sheridan Creek; 92% urban). Agriculture is the predominant form of human activity at the 13 watersheds where NO 3 -N increased, accounting for 51–71% of total land cover. Both the total area of agricultural land and the type of agriculture have changed dramatically in southern Ontario; and these shifts could alter nutrient transfer to waterways. Specifically, shifts in agriculture towards more N-demanding annual row crops like corn could result in higher NO 3 -N leakage to streams, and the impact of this form of land use change on nutrient export requires further investigation. Overall, these results suggest that changes in tributary loading may have contributed to recent observations of increasing NO 3 -N levels in offshore waters of Lake Ontario.

Spatial and temporal variation in de facto wastewater reuse in drinking water systems across the U.S.A.

De facto potable reuse occurs when treated wastewater is discharged into surface waters upstream of potable drinking water treatment plant (DWTP) intakes. Wastewater treatment plant (WWTP) discharges may pose water quality risks at the downstream DWTP, but additional flow aids in providing a reliable water supply source. In this work de facto reuse is analyzed for 2056 surface water intakes serving 1210 DWTPs across the U.S.A. that serve greater than 10,000 people, covering approximately 82% of the nation’s population. An ArcGIS model is developed to assess spatial relationships between DWTPs and WWTPs, with a python script designed to perform a network analysis by hydrologic region. A high frequency of de facto reuse occurrence was observed; 50% of the DWTP intakes are potentially impacted by upstream WWTP discharges. However, the magnitude of de facto reuse was seen to be relatively low, where 50% of the impacted intakes contained less than 1% treated municipal wastewater under average streamflow conditions. De facto reuse increased greatly under low streamflow conditions (modeled by Q95), with 32 of the 80 sites yielding at least 50% treated wastewater, this portion of the analysis is limited to sites where stream gauge data was readily available.

Seasonal and temporal patterns of NDMA formation potentials in surface waters

The seasonal and temporal patterns of N-nitrosodimethylamine (NDMA) formation potentials (FPs) were examined with water samples collected monthly for 21 month period in 12 surface waters. This long term study allowed monitoring the patterns of NDMA FPs under dynamic weather conditions (e.g., rainy and dry periods) covering several seasons. Anthropogenically impacted waters which were determined by high sucralose levels (>100 ng/L) had higher NDMA FPs than limited impacted sources (<100 ng/L). In most sources, NDMA FP showed more variability in spring months, while seasonal mean values remained relatively consistent. The study also showed that watershed characteristics played an important role in the seasonal and temporal patterns. In the two dam-controlled river systems (SW A and G), the NDMA FP levels at the downstream sampling locations were controlled by the NDMA levels in the dams independent of either the increases in discharge rates due to water releases from the dams prior to or during the heavy rain events or intermittent high NDMA FP levels observed at the upstream of dams. The large reservoirs and impoundments on rivers examined in this study appeared serving as an equalization basin for NDMA precursors. On the other hand, in a river without an upstream reservoir (SW E), the NDMA levels were influenced by the ratio of an upstream wastewater treatment plant (WWTP) effluent discharge to the river discharge rate. The impact of WWTP effluent decreased during the high river flow periods due to rain events. Linear regression with independent variables DOC, DON, and sucralose yielded poor correlations with NDMA FP (R2 < 0.27). Multiple linear regression analysis using DOC and log [sucralose] yielded a better correlation with NDMA FP (R2 = 0.53).