Department Urban Water Management

Wastewater-based epidemiology offers a complementary approach to clinical case-based surveillance of emergent diseases and can help identify regions with infected people to prioritize clinical surveillance strategies. However, tracking emergent diseases in wastewater requires reliance on novel testing assays with uncertain sensitivity and specificity. Limited pathogen shedding may cause detection to be below the limit of quantification or bordering the limit of detection. Here, we investigated how the definition of limit of detection for quantitative polymerase chain reaction (qPCR) impacts epidemiological insights during an mpox outbreak in Switzerland. 365 wastewater samples from three wastewater treatment plants in Switzerland from 9 March through 31 October 2022 were analyzed for mpox DNA using qPCR. We detected mpox DNA in 22% (79 of 365) wastewater samples based on a liberal definition of qPCR detection as any exponentially increasing fluorescence above the threshold. Based on a more restrictive definition as the lowest concentration at which there is 95% likelihood of detection, detection was 1% (5 of 365). The liberal definition shows high specificity (90%) and accuracy (78%), but moderate sensitivity (64%) when benchmarked against available clinical case reporting, which contrasts with higher specificity (98%) but lower sensitivity (10%) and accuracy (56%) of the 95% likelihood definition. Wastewater-based epidemiology applied to an emergent pathogen will require optimizing public health trade-offs between reporting data with high degrees of uncertainty and delaying communication and associated action. Information sharing with relevant public health stakeholders could couple early results with clear descriptions of uncertainty. Impact Statement: When a novel pathogen threatens to enter a community, wastewater-based epidemiology offers an opportunity to track its emergence and spread. However, rapid deployment of methods for to detect a novel pathogen may rely on assays with uncertain sensitivity and specificity. Benchmarking the detection of mpox DNA in Swiss wastewaters with reported clinical cases in 2022, we demonstrate how definitions of detection of a qPCR assay influence epidemiological insights from wastewater. The results highlight the need for information sharing between public health stakeholders that couple early insights from wastewater with descriptions of methodological uncertainty to optimize public health actions.

INTRODUCTION: Influenza infections are challenging to monitor at the population level due to many mild and asymptomatic cases and similar symptoms to other common circulating respiratory diseases, including COVID-19. Methods for tracking cases outside of typical reporting infrastructure could improve monitoring of influenza transmission dynamics. Influenza shedding into wastewater represents a promising source of information where quantification is unbiased by testing or treatment-seeking behaviours. METHODS: We quantified influenza A and B virus loads from influent at Switzerland's three largest wastewater treatment plants, serving about 14% of the Swiss population (1.2 million individuals). We estimated trends in infection incidence and the effective reproductive number (R_e) in these catchments during a 2021/22 epidemic and compared our estimates to typical influenza surveillance data. RESULTS: Wastewater data captured the same overall trends in infection incidence as laboratory-confirmed case data at the catchment level. However, the wastewater data were more sensitive in capturing a transient peak in incidence in December 2021 than the case data. The R_eestimated from the wastewater data was roughly at or below the epidemic threshold of 1 during work-from-home measures in December 2021 but increased to at or above the epidemic threshold in two of the three catchments after the relaxation of these measures. The third catchment yielded qualitatively the same results but with wider confidence intervals. The confirmed case data at the catchment level yielded comparatively less precise R_e estimates before and during the work-from-home period, with confidence intervals that included one before and during the work-fromhome period. DISCUSSION: Overall, we show that influenza RNA in wastewater can help monitor nationwide influenza transmission dynamics. Based on this research, we developed an online dashboard for ongoing wastewater-based influenza surveillance in Switzerland.

Wastewater-based epidemiology (WBE) can provide objective and timely information on the use of new psychoactive substances (NPS), originally designed as legal alternatives of internationally controlled drugs. NPS have rapidly emerged on the global drug market, posing a challenge to drug policy and constituting a risk to public health. In this study, a WBE approach was applied to monitor the use of more than 300 NPS, together with fentanyl and its main metabolite norfentanyl, in influent wastewater collected from 12 European cities during March-June 2021. Quantitative and qualitative analysis of NPS in composite 24 h influent wastewater samples were based on solid phase extraction and liquid chromatography-mass spectrometry. In-sample stability tests demonstrated the suitability of most investigated biomarkers, except for a few synthetic opioids, synthetic cannabinoids and phenetylamines. Fentanyl, norfentanyl and eight NPS were quantified in influent wastewater and at least three substances were found in each city, demonstrating their use in Europe. N,N-dimethyltryptamine and 3-methylmethcathinone (3-MMC) were the most common NPS found, with the latter having the highest mass loads (up to 24.8 mg/day/1000 inhabitants). Seven additional substances, belonging to five categories of NPS, were identified in different cities. Spatial trends of NPS use were observed between cities and countries, and a changing weekly profile of use was observed for 3-MMC. WBE is a useful tool to rapidly evaluate emerging trends of NPS use, complementing common indicators (i.e. population surveys, seizures) and helping to establish measures for public health protection.

Current wastewater-based epidemiology (WBE) studies are predominantly focused on the analysis of urinary biomarkers present in the liquid phase of influent wastewater (IWW). This approach systematically underestimates less polar metabolites, such as cannabis biomarkers. These biomarkers can potentially sorb to and desorb from suspended particulate matter (SPM) present in IWW. This study investigates the bidirectional partitioning of THC[sbnd]COOH between the liquid phase and SPM of IWW by performing multiple sorption experiments using THC[sbnd]COOH-D₉ as a surrogate due to the unavailability of blank SPM and blank IWW. In addition, this study involves the analysis of IWW collected from eight wastewater treatment plants (WWTP) (n = 56) across four European countries, where raw IWW, the liquid phase and SPM were separately analysed to identify potential trends in the fraction of THC[sbnd]COOH in the SPM between and withing the examined locations. Based on the performed sorption experiments, bidirectional partitioning of THC[sbnd]COOH between the liquid phase and SPM was noted, showing partition between both phases when only one of the two phases was spiked. It was illustrated that the concentration of SPM had a notable influence on the THC[sbnd]COOH partitioning between both phases. In addition to the inter location variability (average THC[sbnd]COOH present in the SPM ranged 31–59 %), a substantial intra location variation was also observed, e.g., in one location ranged 17–58 %. While the determination of a correction factor for the amount of THC[sbnd]COOH present in SPM would be ideal, this is challenging, since the amount of SPM is not fixed in all IWW samples. Although SPM has influence on the THC[sbnd]COOH partition, no correlation (p value Spearman correlation = 0.3160) was observed between the SPM concentration and the fraction of THC[sbnd]COOH in the solid phase. Moreover, the collection of homogenized samples is difficult, and the time required to reach an equilibration in partitioning of THC[sbnd]COOH between both IWW phases remains unclear. Due to i) the large inter-and intra-location variation of THC[sbnd]COOH present in the SPM, ii) the variability in SPM concentration in IWW samples, and iii) the time required to reach a partitioning equilibration, an analytical procedure based on liquid-liquid extraction (LLE) that considers both the liquid phase and SPM of IWW is recommended to reduce the overall uncertainty for THC[sbnd]COOH measurement in IWW. It was illustrated that this extraction method is capable to recover the total concentration of THC[sbnd]COOH in both phases.

Combined sewer overflows (CSOs) are an important pathway of organic micropollutants from urban areas to open water bodies. Understanding the temporal dynamics of these micropollutants during overflow events is crucial for applying appropriate sampling methods and implementing effective management strategies. Yet, little is known about the dynamics of micropollutants in CSOs, because most studies report concentrations from single grab samples or event mean concentrations (EMCs). With unique high temporal resolution measurements (3 min), we show the real dynamics of polar organic micropollutants in CSOs of one small (2,700 people: P) and one large (159,000 P) urban catchment, for two micropollutant categories: (i) 33 micropollutants in municipal wastewater and (ii) 13 micropollutants from urban surface runoff. The concentration dynamics depend on the substance source and the catchment size. Indoor substances such as pharmaceuticals show high temporal dynamics with changes of 1 to 2 orders of magnitude within 9 min in the CSO of the small catchment. In contrast, outdoor substances at the small catchment and all substances at the large catchment display considerably lower variation. We tested various time-proportional sampling strategies to assess the range of error when estimating EMCs. We recommend an interval of 3 min to capture the dynamics of indoor substances in CSOs from small catchments. The results highlight that both future monitoring campaigns and the planning and management of urban wet-weather treatment systems will benefit from high temporal sampling resolutions, not only to understand dynamics but also to minimize errors of estimated EMCs.

To inform the development of global wastewater monitoring systems, we surveyed programmes in 43 countries. Most programmes monitored predominantly urban populations. In high-income countries (HICs), composite sampling at centralised treatment plants was most common, whereas grab sampling from surface waters, open drains, and pit latrines was more typical in low-income and middle-income countries (LMICs). Almost all programmes analysed samples in-country, with an average processing time of 2·3 days in HICs and 4·5 days in LMICs. Whereas 59% of HICs regularly monitored wastewater for SARS-CoV-2 variants, only 13% of LMICs did so. Most programmes share their wastewater data internally, with partnering organisations, but not publicly. Our findings show the richness of the existing wastewater monitoring ecosystem. With additional leadership, funding, and implementation frameworks, thousands of individual wastewater initiatives can coalesce into an integrated, sustainable network for disease surveillance—one that minimises the risk of overlooking future global health threats.

BackgroundThroughout the COVID-19 pandemic, SARS-CoV-2 genetic variants of concern (VOCs) have repeatedly and independently arisen. VOCs are characterised by increased transmissibility, increased virulence or reduced neutralisation by antibodies obtained from prior infection or vaccination. Tracking the introduction and transmission of VOCs relies on sequencing, typically whole genome sequencing of clinical samples. Wastewater surveillance is increasingly used to track the introduction and spread of SARS-CoV-2 variants through sequencing approaches.AimHere, we adapt and apply a rapid, high-throughput method for detection and quantification of the relative frequency of two deletions characteristic of the Alpha, Beta, and Gamma VOCs in wastewater.MethodsWe developed drop-off RT-dPCR assays and an associated statistical approach implemented in the R package WWdPCR to analyse temporal dynamics of SARS-CoV-2 signature mutations (spike Δ69-70 and ORF1a Δ3675-3677) in wastewater and quantify transmission fitness advantage of the Alpha VOC.ResultsBased on analysis of Zurich wastewater samples, the estimated transmission fitness advantage of SARS-CoV-2 Alpha based on the spike Δ69-70 was 0.34 (95% confidence interval (CI): 0.30-0.39) and based on ORF1a Δ3675-3677 was 0.53 (95% CI: 0.49-0.57), aligning with the transmission fitness advantage of Alpha estimated by clinical sample sequencing in the surrounding canton of 0.49 (95% CI: 0.38-0.61).ConclusionDigital PCR assays targeting signature mutations in wastewater offer near real-time monitoring of SARS-CoV-2 VOCs and potentially earlier detection and inference on transmission fitness advantage than clinical sequencing.

Wastewater analysis of Δ⁹-tetrahydrocannabinol (THC) biomarkers can provide essential information on trends in cannabis consumption. Although analysis is mostly focused on the aqueous phase, previous studies have illustrated the need of improving the measurements of raw influent wastewater (IWW) considering also suspended solids. This is important for cannabis biomarkers, because a substantial part of them is expected to be found in the suspended solids due to their more lipophilic character compared with other metabolites/drugs included in these types of studies. However, it remains open to which extent trend estimates might be affected by solely analysing the liquid phase. To investigate this aspect, robust analytical methodologies are required to measure both the liquid and solid phases of IWW. In this work, we firstly tested liquid-liquid extraction (LLE) for THC and its major metabolites (THC-OH, and THC-COOH). Using LLE, no filtration or centrifugation step was required for raw IWW analysis, and the three analytes were extracted from both the liquid and the solid phase simultaneously. In parallel, the raw IWW was centrifuged and the obtained solid and liquid phases were analyzed separately: the liquid phase by both LLE and solid phase extraction (SPE) for comparison of data, and the suspended solids by solid-liquid extraction (SLE). The separate analysis of both phases in a number of samples revealed that a significant amount of cannabis biomarkers (ranging from 42 to 90%) was found in the suspended solids. In addition, the total amount of cannabis biomarkers obtained by analysing raw IWW on the one hand, and by separate analysis of the liquid and the solid phases, on the other hand, was in good agreement. Data from this study show that the sole analysis of the liquid phase would lead to a notable underestimation of cannabis biomarkers concentrations in IWW.

Wastewater-based epidemiology (WBE) has emerged as an effective tool for monitoring SARS-CoV-2 dynamics during the COVID-19 pandemic. Here, we add a spatial component to WBE and use it to investigate SARS-CoV-2 spread in the canton of Ticino during the onset of the pandemic in Switzerland (end of February 2020 to beginning of March 2020). Ticino is located at the border to Northern Italy, where a large COVID-19 outbreak occurred in February 2020. Not surprisingly, Ticino was the site of the first clinically confirmed COVID-19 case in Switzerland. We retrospectively analyzed daily influent samples from nine wastewater treatment plants in Ticino that jointly cover an area of 20 km × 60 km and 351,000 people (>99% of the population). Our result is a fine-grained view of the spatiotemporal evolution of the COVID-19 pandemic in this canton. The wastewater analysis revealed that by February 29, 2020, SARS-CoV-2 had already spread to all catchments. At the same time, only four individual cases had been clinically confirmed across the region served by the treatment plants investigated. Our results demonstrate that WBE could serve as a versatile tool to monitor the introduction and spread of an infectious agent on a regional scale. To fully exploit its utility, WBE should be implemented in real time and become an integral part of future disease surveillance efforts.

BACKGROUND: The effective reproductive number, R_e, is a critical indicator to monitor disease dynamics, inform regional and national policies, and estimate the effectiveness of interventions. It describes the average number of new infections caused by a single infectious person through time. To date, R_e estimates are based on clinical data such as observed cases, hospitalizations, and/or deaths. These estimates are temporarily biased when clinical testing or reporting strategies change.
OBJECTIVES: We show that the dynamics of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA in wastewater can be used to estimate R_e in near real time, independent of clinical data and without the associated biases.
METHODS: We collected longitudinal measurements of SARS-CoV-2 RNA in wastewater in Zurich, Switzerland, and San Jose, California, USA. We combined this data with information on the temporal dynamics of shedding (the shedding load distribution) to estimate a time series proportional to the daily COVID-19 infection incidence. We estimated a wastewater-based R_e from this incidence.
RESULTS: The method to estimate R_e from wastewater worked robustly on data from two different countries and two wastewater matrices. The resulting estimates were as similar to the R_e estimates from case report data as R_e estimates based on observed cases, hospitalizations, and deaths are among each other. We further provide details on the effect of sampling frequency and the shedding load distribution on the ability to infer R_e.
DISCUSSION: To our knowledge, this is the first time R_e has been estimated from wastewater. This method provides a low-cost, rapid, and independent way to inform SARS-CoV-2 monitoring during the ongoing pandemic and is applicable to future wastewater-based epidemiology targeting other pathogens.

The continuing emergence of SARS-CoV-2 variants of concern and variants of interest emphasizes the need for early detection and epidemiological surveillance of novel variants. We used genomic sequencing of 122 wastewater samples from three locations in Switzerland to monitor the local spread of B.1.1.7 (Alpha), B.1.351 (Beta) and P.1 (Gamma) variants of SARS-CoV-2 at a population level. We devised a bioinformatics method named COJAC (Co-Occurrence adJusted Analysis and Calling) that uses read pairs carrying multiple variant-specific signature mutations as a robust indicator of low-frequency variants. Application of COJAC revealed that a local outbreak of the Alpha variant in two Swiss cities was observable in wastewater up to 13 d before being first reported in clinical samples. We further confirmed the ability of COJAC to detect emerging variants early for the Delta variant by analysing an additional 1,339 wastewater samples. While sequencing data of single wastewater samples provide limited precision for the quantification of relative prevalence of a variant, we show that replicate and close-meshed longitudinal sequencing allow for robust estimation not only of the local prevalence but also of the transmission fitness advantage of any variant. We conclude that genomic sequencing and our computational analysis can provide population-level estimates of prevalence and fitness of emerging variants from wastewater samples earlier and on the basis of substantially fewer samples than from clinical samples. Our framework is being routinely used in large national projects in Switzerland and the UK.

Wastewater-based epidemiology (WBE) has been shown to coincide with, or anticipate, confirmed COVID-19 case numbers. During periods with high test positivity rates, however, case numbers may be underreported, whereas wastewater does not suffer from this limitation. Here we investigated how the dynamics of new COVID-19 infections estimated based on wastewater monitoring or confirmed cases compare to true COVID-19 incidence dynamics. We focused on the first pandemic wave in Switzerland (February to April, 2020), when test positivity ranged up to 26%. SARS-CoV-2 RNA loads were determined 2–4 times per week in three Swiss wastewater treatment plants (Lugano, Lausanne and Zurich). Wastewater and case data were combined with a shedding load distribution and an infection-to-case confirmation delay distribution, respectively, to estimate infection incidence dynamics. Finally, the estimates were compared to reference incidence dynamics determined by a validated compartmental model. Incidence dynamics estimated based on wastewater data were found to better track the timing and shape of the reference infection peak compared to estimates based on confirmed cases. In contrast, case confirmations provided a better estimate of the subsequent decline in infections. Under a regime of high-test positivity rates, WBE thus provides critical information that is complementary to clinical data to monitor the pandemic trajectory.

Tracking the occurrence of a broad variety of chemicals in the aquatic environment at a high temporal resolution over extended time periods is challenging. Here, we present a transportable platform integrating sample preparation, liquid chromatography-high-resolution mass spectrometry measurement, automated data processing, and remote control and surveillance. The system is capable of quantifying pollutants at 20 min intervals with high sensitivity (limit of quantification down to 10 ng/L) and operated stably on-site over prolonged periods (<3 ppm mass drift over two weeks, <0.3 min retention time drift over six weeks). Field campaigns under different conditions demonstrated unprecedented insights into pollutant dynamics. Time-resolved measurements in a small creek revealed concentration peaks with up to 10-fold exceedances of environmental quality standards. The quantification of illicit drugs and their metabolites in raw wastewater distinguished fractions of consumed and discarded cocaine. Frequency analyses and data mining showed clusters of diurnal, episodic, and possibly industry-related pollutants, including newly identified substances. With this enabling technology the potential for researching and managing chemicals in natural and technical environments can be significantly expanded beyond our current capabilities, for example, real-time control in process engineering and sewer operation (water management and environmental toxicology), industrial surveillance, and wastewater-based epidemiology.

Konzentrationsspitzen von Pestiziden können von grosser biologischer und regulatorischer Bedeutung sein, werden aber selten und nur mit hohem Aufwand erfasst. Die neue MS²field-Plattform ist eine der ersten mobilen Messinfrastrukturen, die kontinuierliche und zeitlich hochaufgelöste Messungen von Mikroverunreinigungen in umweltrelevanten Konzentrationen im Feld erlaubt. Wie vielfältig Konzentrationsdynamiken von Pestiziden sein können und in welchem Ausmass Spitzenkonzentrationen mit konventionellen Probenahme- und Messtechniken bisher unterschätzt wurden, macht eine Messkampagne in einem landwirtschaftlich stark geprägten Bach sichtbar.

Background and aims Wastewater‐based epidemiology is an additional indicator of drug use that is gaining reliability to complement the current established panel of indicators. The aims of this study were to: (i) assess spatial and temporal trends of population‐normalized mass loads of benzoylecgonine, amphetamine, methamphetamine and 3,4‐methylenedioxymethamphetamine (MDMA) in raw wastewater over 7 years (2011-17); (ii) address overall drug use by estimating the average number of combined doses consumed per day in each city; and (iii) compare these with existing prevalence and seizure data. Design Analysis of daily raw wastewater composite samples collected over 1 week per year from 2011 to 2017. Setting and Participants Catchment areas of 143 wastewater treatment plants in 120 cities in 37 countries. Measurements Parent substances (amphetamine, methamphetamine and MDMA) and the metabolites of cocaine (benzoylecgonine) and of Δ⁹‐tetrahydrocannabinol (11‐nor‐9‐carboxy‐Δ⁹‐tetrahydrocannabinol) were measured in wastewater using liquid chromatography-tandem mass spectrometry. Daily mass loads (mg/day) were normalized to catchment population (mg/1000 people/day) and converted to the number of combined doses consumed per day. Spatial differences were assessed world‐wide, and temporal trends were discerned at European level by comparing 2011-13 drug loads versus 2014-17 loads. Findings Benzoylecgonine was the stimulant metabolite detected at higher loads in southern and western Europe, and amphetamine, MDMA and methamphetamine in East and North-Central Europe. In other continents, methamphetamine showed the highest levels in the United States and Australia and benzoylecgonine in South America. During the reporting period, benzoylecgonine loads increased in general across Europe, amphetamine and methamphetamine levels fluctuated and MDMA underwent an intermittent upsurge. Conclusions The analysis of wastewater to quantify drug loads provides near real‐time drug use estimates that globally correspond to prevalence and seizure data.

Untreated sewer overflows can contaminate receiving waters with micropollutants. Although concentrations of discharged micropollutants can be ecotoxicologically relevant, only limited data is available to assess occurrence and spatial differences among sewer overflow catchments. Therefore, we present an innovative type of data obtained with passive samplers at 20 combined sewer overflow sites (2-7 events per site; 95 events in total). The data sheds light on concentration ranges for 13 representative polar organic micropollutants and shows that micropollutants in both municipal wastewater and stormwater can be relevant sources of contaminants. We identify indicator micropollutants for further studies: benzotriazole (80% interquantile of time-weighted average concentration: 250–4800 ng/L), carbamazepine (33-910 ng/L), diclofenac (78-1000 ng/L), carbendazim (21-900 ng/L), diazinon (2.1-53 ng/L), diuron (22-1100 ng/L), mecoprop (98–5300 ng/L), metolachlor (6-230 ng/L), and terbutryn (29-810 ng/L). These concentration estimates are assumed to be on the safe side for comparison with environmental quality standards (EQS). A majority of sewer overflow sites (13 of 20) show discharge concentrations above acute EQS for at least one micropollutant and thus would have to rely on dilution by receiving waters to not exceed any EQS. The intersite variability among sewer overflows exceed the within-site variability. Hence, future monitoring studies should cover more sewer overflow sites. No correlation could be found with event durations, specific storage volume or land use data, thus showing the complexity of micropollutant occurrence and indicating that other factors led to the observed high spatial variability. In conclusion, our results clearly show the potential relevance of micropollutants in sewer overflows and the need to assess site-specific measures.

Ubiquitous sensing will create many opportunities and threats for urban water management, which are only poorly understood today. To identify the most relevant trends, we conducted a horizon scan regarding how ubiquitous sensing will shape the future of urban drainage and wastewater management. Our survey of the international urban water community received an active response from both the academics and the professionals from the water industry. The analysis of the responses demonstrates that emerging topics for urban water will often involve experts from different communities, including aquatic ecologists, urban water system engineers and managers, as well as information and communications technology professionals and computer scientists. Activities in topics that are identified as novel will either require (i) cross-disciplinary training, such as importing new developments from the IT sector, or (ii) research in new areas for urban water specialists, for example, to help solve open questions in aquatic ecology. These results are, therefore, a call for interdisciplinary research beyond our own discipline. They also demonstrate that the water management community is not yet prepared for the digital transformation, where we will experience a data demand, i.e. a “pull” of urban water data into external services. The results suggest that a lot remains to be done to harvest the upcoming opportunities. Horizon scanning should be repeated on a routine basis, under the umbrella of an experienced polling organization.

Bei Regenwetter werden viele potenziell toxische Schadstoffe aus Aussenhüllen von Gebäuden ausgewaschen und in die Gewässer eingetragen. Unklar ist allerdings, ob einfache lineare Auswaschfunktionen für Mikroschadstoffe aus Gebäudehüllen für Schmutzfrachtsimulationen ausreichend sind. Um Auswaschungen aus beregneten Gebäudehüllen dynamisch zu berechnen, wurde das "COnstruction Material LEAching Model" (COMLEAM) entwickelt, mit dem Mikroverunreinigungen prozess-basiert beschrieben werden. COMLEAM berücksichtigt allerdings keine Transportprozesse in der Siedlungsentwässerung, so dass es bislang nicht möglich ist, Umwelteinflüsse von Gebäudehüllen abzubilden. In dieser Studie wurde daher COMLEAM an das hydrodynamische Niederschlags-Abfluss Modell SWMM gekoppelt. Insbesondere wurden die Unterschiede von dynamischen und linearen Auswaschmodellen untersucht. Für die Verknüpfung der Modelle wurde eine neue Schnittstelle für COMLEAM programmiert, die sowohl einen Export von SWMM-kompatiblen Schmutzfracht-Zeitreihen, als auch Batch-Simulationen ermöglicht. Die Ergebnisse für eine Fallstudie in Fehraltorf (CH), wo Schmutzfrachten und Konzentrationen des Durchwurzelungsschutzmittels Mecoprop vorhergesagt wurden, zeigen grundsätzlich eine befriedigende Übereinstimmung mit zeitlich hochaufgelösten Daten aus einer Messkampagne. Langzeitprognosen mit dem dynamischen COMLEAM Modell liefern in unserem Fall signifikant unterschiedliche Ergebnisse als lineare Auswaschfunktionen. Allerdings sind diese Unterschiede, in unserem Fallbeispiel, ab einem Gebäudealter von 10 Jahren allerdings vernachlässigbar. Sensitivitätsanalyse deuten weiterhin darauf hin, dass Informationen zum Gebäudebestand, und insbesondere das Alter der Gebäude, sehr sensitiv auf die Simulationsresultate sind.

Transformation of biomarkers (or their stability) during sewer transport is an important issue for wastewater-based epidemiology (WBE). Most studies so far have been conducted in the laboratory, which usually employed unrealistic conditions. In the present study, we utilized a pilot sewer system including a gravity pipe and a rising main pipe to investigate the fate of 24 pharmaceutical biomarkers. A programmable logic controller was used to control and monitor the system including sewer operational conditions and wastewater properties. Sequential samples were collected that can represent hydraulic retention time (HRT) of up to 8 h in a rising main and 4 h in a gravity sewer. Wastewater parameters and biomarker concentrations were analysed to evaluate the stability and transformation kinetics. The wastewater parameters of the pilot system were close to the conditions of real sewers. The findings of biomarker transformation were also close to real sewer data with seventeen biomarkers reported as stable while buprenorphine, caffeine, ethyl-sulfate, methadone, paracetamol, paraxanthine and salicylic acid degraded to variable extents. Both zero-order and first-order kinetics were used to model the degradation of unstable biomarkers and interestingly the goodness of fit R² for the zero-order model was higher than the first-order model for all unstable biomarkers in the rising main. The pilot sewer system simulates more realistic conditions than benchtop laboratory setups and may provide a more accurate approach for assessing the in-sewer transformation kinetics and stability of biomarkers.

Niederschlags- und Mischabwasserentlastungen aus Siedlungen tragen zu Mikroverunreinigungen in Gewässern bei. Mit Passivsammlern wurden erstmals Konzentrationsbereiche an 20 Standorten für insgesamt 95 Ereignisse bestimmt, was die Analyse von Unterschieden zwischen Standorten sowie die Identifikation relevanter Eintragspfade unterstützt. An 13 Standorten waren bei mindestens einer Substanz die Konzentrationen im Mischabwasser höher als akute Qualitätskriterien.

Considerable pollutant loads can enter surface waters during rain events. Three factors challenge quantification of these pollutant fluxes using traditional sampling methods: (i) concentration fluctuations; (ii) unknown event duration; and (iii) placement, operation, and maintenance of equipment. Passive samplers offer the advantage of sampling in a continuous mode without power supply. However, variable uptake rates due to environmental factors and desorption in the case of fluctuating concentrations can affect the accuracy of time-weighted average (TWA) concentration estimates. While uncertainties related to environmental factors could be accounted for with additional effort, we can neither control nor quantify the concentration variability. We present measured and modelled concentration profiles at high temporal resolution and provide a systematic approach to assessing deviations from true TWA concentration due to fluctuating concentration profiles. We evaluate sampling of sewer overflows (0.3–14 h) with Chemcatcher and 1-week sampling in rivers. The uncertainty due to fluctuating concentrations is small, and other factors such as chemical analyses and sampler calibration have a similar or higher impact. The uncertainty due to fluctuations clearly increases with the sampling duration, particularly when exceeding the half-life of equilibrium. We conclude that passive sampling can also be used in wastewater systems with potentially high concentration variations.

Contaminants in sewer overflows can contribute to exceedances of environmental quality standards, thus the quantification of contaminants during rainfall events is of relevance. However, monitoring is challenged by i) high spatiotemporal variability of contaminants in events of hard-to-predict durations, and ii) a large number of remote sites, which would imply enormous efforts with traditional sampling equipment. Therefore, we evaluate the applicability of passive samplers (Empore styrene-divinylbenzene reverse phase sulfonated (SDB-RPS)) to monitor a set of 13 polar organic contaminants. We present calibration experiments at high temporal resolution to assess the rate limiting accumulation mechanisms for short events (<36 h), report parameters for typical sewer conditions and compare passive samplers with composite water samples in a field study (three locations, total 10 events). With sampling rates of 0.35–3.5 L/d for 1 h reference time, our calibration results indicate a high sensitivity of passive samplers to sample short, highly variable sewer overflows. The contaminant uptake kinetic shows a fast initial accumulation, which is not well represented with the typical first-order model. Our results indicate that mass transfer to passive samplers is either controlled by the water boundary layer and the sorbent, or by the sorbent alone. Overall, passive sampler concentration estimates are within a factor 0.4 to 3.1 in comparison to composite water samples in the field study. We conclude that passive samplers are a promising approach to monitor a large number of discharge sites although it cannot replace traditional stormwater quality sampling in some cases (e.g. exact load estimates, high temporal resolution). Passive samplers facilitate identifying and prioritizing locations that may require more detailed investigations.

Motivation. Our surface water is impacted by a wide variety of contaminants released through human activities. One contaminant group of concern is micropollutants, which can have eco-toxicological effects in trace concentrations. Micropollutants, for example, include plant protection products and biocides, which are specifically designed to harm organisms. An important input pathway of micropollutants to surface water can be untreated sewer overflows (combined sewer overflows and stormwater outlets). However, the understanding of factors influencing the occurrence and levels of micropollutants is limited and challenged by: i) high spatial differences among sites, ii) a large number of discharge sites and iii) high temporal fluctuating discharge events.

Research objective. This thesis intends to enhance our understanding of micropollutants in sewer overflows. It aims to investigate efficient methods to prioritize sewer overflow sites, which can be potentially harmful for receiving waters. The presented work focuses on the development of model prediction and efficient monitoring approaches and includes the following: i) a Swiss-wide model to assess how many discharge sites may be critical (Chapter 2), ii) fundamentals to develop passive sampling as an alternative monitoring method for short duration sewer overflows (Chapter 3 and 4) and iii) an extended monitoring study covering 20 combined sewer overflows (CSOs) to explore spatial differences among sites (Chapter 5). The main findings of this thesis are presented in the following.

Model-based screening. A dynamic substance flow modeling approach was applied to 2,500 Swiss municipalities, considering micropollutant accumulation and wash-off on urban surfaces. The approach is based on the simplification, that there is one CSO and one stormwater outlet per municipality. The model allows for an estimation of the micropollutant concentration fluctuations in sewer overflows in 10-min resolution. The results show the importance of untreated discharges from sewer overflows as emission into receiving waters. The load contribution to sewer overflows of micropollutants in stormwater (e.g. plant protection products and biocides) is estimated to be considerably higher than of micropollutants in municipal wastewater (e.g. pharmaceuticals and other household chemicals). In addition, the results indicate that up to 83% of all urban catchments have sewer overflows that need to rely on upstream dilution in order to not exceed substance-specific environmental quality standards (EQS). Thus, this nationwide screening approach clearly highlights the need for a more detailed assessment of micropollutants in sewer overflows, and especially, the need for more measured data to allow the development of validated micropollutant prediction models.

Measuring. Difficulties of monitoring sewer overflows with traditional methods are i) high concentration fluctuations with unknown event durations which require a high temporal sampling resolution, ii) many discharge sites and iii) placement, operation, and maintenance of equipment. Hence, passive samplers for polar organic micropollutants are analyzed systematically as a viable alternative to monitor short duration sewer overflows. The main advantage of passive samplers is the continuous accumulation of contaminants from the water phase, with no need for external energy sources nor for immense water sample storage volume. In a first step, the impact of fluctuating concentrations on deviations from true time-weighted average (TWA) concentrations was studied. The results highlight that the deviations induced by fluctuating concentrations are similar or smaller than uncertainties arising from chemical analysis and environmental factors. Understanding the uptake mechanism of micropollutants is one of the most important issues that needs to be resolved to reduce uncertainties in passive sampling data. The uptake experiments in sewer conditions for short duration events (<36h) indicate that the mass transfer is either dominated by the sorbent, or, by a multi-step mechanism. Therefore, a new semi-empirical mixed rate control model is proposed, which can be directly used for future studies under similar conditions. A field validation (3 locations, 10 events) shows that TWA concentration estimates measured by passive samplers are within a factor of 0.4 to 3.1 compared to composite water samples. Hence, the use of upper limit TWA concentration estimates is recommended for compliance checking with EQS. The findings clearly show that passive samplers are suitable to estimate TWA concentration ranges in sewer overflows and, thus facilitate identification of potentially critical discharge sites.

Occurrence of micropollutants. Unique monitoring data from 20 CSO sites was collected with passive samplers. In total 13 polar organic micropollutants were analysed in 95 events (2-7 events per site). The results highlight indicator micropollutants, which were often found in the monitored CSOs and could be used in future monitoring studies: diclofenac, benzotriazole, carbamazepine, diazinon, diuron, carbendazim, mecoprop, metolachlor and terbutryn. Further, our results reveal that the spatial differences among CSO sites are bigger than the inter-event differences within a site for all studied micropollutants. Nevertheless, no significant correlation with land use data could be identified. The results, therefore, suggest that additional factors, most likely the contaminant usage pattern, have a considerable influence on the observed spatial differences. Both municipal wastewater and stormwater contributed to concentrations above the EQS in CSOs (not in the receiving water). In addition, the monitoring with passive samplers indicates that at least 13 out of 20 CSOs show concentrations above EQS in CSOs, and would rely on dilution by receiving waters to not exceed EQS.

Outlook. Overall, the thesis shows the relevance of sewer overflows as a source of micropollutants entering receiving water bodies. The findings can serve as a basis for the development of a systematic and stepwise approach to efficiently identify critical sites. The development of such an approach would require joint efforts by eco-toxicologists, analytical chemists, regulators and wastewater engineers. This approach could be based on a simplified modeling approach as a first indicator, followed by passive sampling to assess micropollutant levels. To enable the widespread application of passive samplers in monitoring programs, regulators’ and operators’ confidence in passive sampling needs to be strengthened with more field validation studies and common guidelines.

Wastewater contains a large range of biological and chemical markers of human activity and exposures. Through systematic collection and analysis of these markers within wastewater samples it is possible to measure the public health of whole populations. The analysis of effluent and biosolids can also be used to understand the release of chemicals from wastewater treatment plants into the environment. Wastewater analysis and comparison with catchment specific data (e.g. demographics) however remains largely unexplored. This manuscript describes a national wastewater monitoring study that combines influent, effluent and biosolids sampling with the Australian Census. An archiving program allows estimation of per capita exposure to and consumption of chemicals, public health information, as well as per capita release of chemicals into the environment. The paper discusses the study concept, critical steps in setting up a coordinated national approach and key logistical and other considerations with a focus on lessons learnt and future applications. The unique combination of archived samples, analytical data and associated census-derived population data will provide a baseline dataset that has wide and potentially increasing applications across many disciplines that include public health, epidemiology, criminology, toxicology and sociology.

Wastewater studies that provide per capita estimates of consumption (influent) or release (effluent) via wastewater systems rely heavily on accurate population data. This study evaluated the accuracy of Wastewater Treatment Plant (WWTP) reported populations, as well as hydrochemical parameters, against accurate populations from a population census. 104 catchment maps were received from WWTPs, geolocated in geospatial software and overlaid with the smallest area unit of the Australian census, equating to 14.9 million Australians or 64% of the national population. We characterized each catchment for population counts, as well as by age profile, income profile, and education level. For a subset of sites, population estimates using hydrochemical parameters BOD, COD, and dissolved ammonia were evaluated for accuracy against census populations. Population estimates provided by WWTP personnel were on average 18% higher than census-based populations. Furthermore, hydrochemical-based population estimates had high RSD (>44%) for BOD, COD, and ammonium between sites, suggesting that their applicability for use in population estimation may not be appropriate for every WWTP. Catchment age distributions were evaluated and 46% of catchments had skewed age distributions: 6% were skewed older, and 40% were skewed younger. Through this process WWTP catchment populations can be characterized in a way that will enhance the interpretations of per capita estimates.

The impacts of the unintended release of engineered nanomaterials (ENMs) and the resulting exposure to the ecosystems are still poorly understood and intensively debated. In current mass flow models, a global transfer coefficient is used to account for ENMs discharged from sewer systems to surface waters during rain events.
However, different types of sewer systems and specific ENM applications likely require a more elaborate approach to quantify ENM loads entering surface waters during rain events. Therefore, we evaluated the impact of distinguishing between different application areas of ENMs (indoor/outdoor) and different types of sewer systems (combined/separate) on the loads of selected ENMs passing through wastewater systems and reaching the surface water. We applied a dynamic mass flow analysis to eight substances (TiO₂, ZnO, Ag, SiO₂, FeO_x, CuO, CeO₂ and carbon black) for six different sewer system configurations. To estimate the runoff from streets and facades, we used a hydrological model developed for dissolved substances. For areas with separate sewer systems only and ENMs predominantly used in and released from outdoor applications (e.g. CuO, carbon black), up to ~80% of the annual loads entering the sewer systems never reach a sewage treatment plant. Those ENMs are directly discharged to surface waters via stormwater outlets. For combined sewer systems and ENMs mainly applied indoors (e.g. Ag, ZnO), the percentage of ENM bypassing sewage treatment plants remains below 2%. Although the model is setup for Switzerland and other geographical areas will show for example different rain characteristics, the relative importance of the different release pathways will broadly remain the same and the results should, therefore, be transferrable to other countries.

The aim of this paper is to present the first study on spatial and temporal variation in the enantiomeric profile of chiral drugs in eight European cities. Wastewater-based epidemiology (WBE) and enantioselective analysis were combined to evaluate trends in illicit drug use in the context of their consumption vs direct disposal as well as their synthetic production routes. Spatial variations in amphetamine loads were observed with higher use in Northern European cities. Enantioselective analysis showed a general enrichment of amphetamine with the R-(−)-enantiomer in wastewater indicating its abuse. High loads of racemic methamphetamine were detected in Oslo (EF = 0.49 ± 0.02). This is in contrast to other European cities where S-(+)-methamphetamine was the predominant enantiomer. This indicates different methods of methamphetamine synthesis and/or trafficking routes in Oslo, compared with the other cities tested. An enrichment of MDMA with the R-(−)-enantiomer was observed in European wastewaters indicating MDMA consumption rather than disposal of unused drug. MDA's chiral signature indicated its enrichment with the S-(+)-enantiomer, which confirms its origin from MDMA metabolism in humans. HMMA was also detected at quantifiable concentrations in wastewater and was found to be a suitable biomarker for MDMA consumption. Mephedrone was only detected in wastewater from the United Kingdom with population-normalised loads up to 47.7 mg 1000 people⁻¹ day⁻¹. The enrichment of mephedrone in the R-(+)-enantiomer in wastewater suggests stereoselective metabolism in humans, hence consumption, rather than direct disposal of the drug. The investigation of drug precursors, such as ephedrine, showed that their presence was reasonably ascribed to their medical use.

The analysis of illicit drugs in urban wastewater is the basis of wastewater-based epidemiology (WBE), and has received much scientific attention because the concentrations measured can be used as a new non-intrusive tool to provide evidence-based and real-time estimates of community-wide drug consumption. Moreover, WBE allows monitoring patterns and spatial and temporal trends of drug use. Although information and expertise from other disciplines is required to refine and effectively apply WBE, analytical chemistry is the fundamental driver in this field. The use of advanced analytical techniques, commonly based on combined chromatography—mass spectrometry, is mandatory because the very low analyte concentration and the complexity of samples (raw wastewater) make quantification and identification/confirmation of illicit drug biomarkers (IDBs) troublesome. We review the most-recent literature available (mostly from the last 5 years) on the determination of IDBs in wastewater with particular emphasis on the different analytical strategies applied. The predominance of liquid chromatography coupled to tandem mass spectrometry to quantify target IDBs and the essence to produce reliable and comparable results is illustrated. Accordingly, the importance to perform inter-laboratory exercises and the need to analyze appropriate quality controls in each sample sequence is highlighted. Other crucial steps in WBE, such as sample collection and sample pre-treatment, are briefly and carefully discussed. The article further focuses on the potential of high-resolution mass spectrometry. Different approaches for target and non-target analysis are discussed, and the interest to perform experiments under laboratory-controlled conditions, as a complementary tool to investigate related compounds (e.g., minor metabolites and/or transformation products in wastewater) is treated. The article ends up with the trends and future perspectives in this field from the authors’ point of view.

Recent studies have demonstrated the role of biofilms on the stability of drug residues in wastewater. These factors are pertinent in wastewater-based epidemiology (WBE) when estimating community-level drug use. However, there is scarce information on the biotransformation of drug residues in the presence of biofilms and the potential use of transformation products (TPs) as biomarkers in WBE.
The purpose of this work was to investigate the formation of TPs in sewage reactors in the presence of biofilm mimicking conditions during in-sewer transport. Synthetic cathinones (methylenedioxypyrovalerone, methylone, mephedrone) and phenethylamines (4-methoxy-methamphetamine and 4-methoxyamphetamine) were incubated in individual reactors over a 24 h period. Analysis of parent species and TPs was carried out using liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (LC-QToFMS). Identification of TPs was done using suspect and non-target workflows.
In total, 18 TPs were detected and identified with reduction of β-keto group, demethylenation, demethylation, and hydroxylation reactions observed for the synthetic cathinones. For the phenethylamines, N- and O-demethylation reactions were identified. Overall, the experiments showed varying stability for the parent species in wastewater in the presence of biofilms. The newly identified isomeric forms of TPs particularly for methylone and mephedrone can be used as potential target biomarkers for WBE studies due to their specificity and detectability within a 24 h residence time.

The aim of this study was to understand the uncertainty of estimating loads for observed herbicides and nutrients during a flood event and provide guidance on estimator selection. A high-resolution grab sampling campaign (258 samples over 100 h) was conducted during a flood event in a tropical waterway in Queensland, Australia. Ten herbicides and three nutrient compounds were detected at elevated concentrations. Each had a unique chemograph with differences in transport processes (e.g. dependence on flow, dilution processes and timing of concentration pulses). Resampling from the data set was used to assess uncertainty. Bias existed at lower sampling efforts but depended on estimator properties as sampling effort increased: the interpolation, ratio and regression estimators became unbiased. Large differences were observed in precision and the importance of sampling effort and estimator selection depended on the relationship between the chemograph and hydrograph. The variety of transport processes observed and the resultant variability in uncertainty suggest that useful load estimates can only be obtained with sufficient samples and appropriate estimator selection. We provide a rationale to show the latter can be guided across sampling periods by selecting an estimator where the sampling regime or the relationship between the chemograph and hydrograph meet its assumptions: interpolation becomes more correct as sampling effort increases and the ratio becomes more correct as the r² correlation between flux and flow increases (e.g. > 0.9); a stratified composite sampling approach, even with random samples, is a promising alternative.

Wastewater-based epidemiology (WBE) complements existing epidemiologybased estimation techniques and provides objective, evidence-based estimates of illicit drug use. After consumption, biomarkers drugs and their metabolites - excreted to toilets and flushed into urban sewer networks can be measured in raw wastewater samples. The quantified loads can serve as an estimate for the collective consumption of all people contributing to the wastewater sample. This transdisciplinary approach, further explained in this chapter, has developed, matured and is now established for monitoring substances such as cocaine and amphetamine-type stimulants. Research currently underway is refining WBE to new applications including new psychoactive substances (NPS).

Thirty-seven laboratories from 25 countries present the development of an inter-laboratory testing scheme for the analysis of seven illicit drug residues in standard solutions, tap- and wastewater. Almost 10 000 concentration values were evaluated: triplicates of up to five samples and 26 laboratories per year. The setup was substantially improved with experiences gained across the six repetitions (e.g. matrix type, sample conditions, spiking levels). From this, (pre-)analytical issues (e.g. pH adjustment, filtration) were revealed for specific analytes which resulted in formulation of best-practice protocols for inter-laboratory setup and analytical procedures. The results illustrate the effectiveness of the inter-laboratory setup to assess laboratory performance in the framework of wastewater-based epidemiology. The exercise proved that measurements of laboratories were of high quality (>80% satisfactory results for six out of seven analytes) and that analytical follow-up is important to assist laboratories in improving robustness of wastewater-based epidemiology results.

The growing awareness of the relevance of organic microcontaminants on the environment has led to a growing number of studies on attenuation of these compounds in wastewater treatment plants (WWTP) and rivers. However, the effects of the sampling strategies (frequency and duration of composite samples) on the attenuation estimates are largely unknown. Our goal was to assess how frequency and duration of composite samples influence uncertainty of the attenuation estimates in WWTPs and rivers. Furthermore, we also assessed how compound consumption rate and degradability influence uncertainty. The assessment was conducted through simulating the integrated wastewater system of Puigcerdà (NE Iberian Peninsula) using a sewer pattern generator and a coupled model of WWTP and river. Results showed that the sampling strategy is especially critical at the influent of WWTP, particularly when the number of toilet flushes containing the compound of interest is small (≤100 toilet flushes with compound day^-1), and less critical at the effluent of the WWTP and in the river due to the mixing effects of the WWTP. For example, at the WWTP, when evaluating a compound that is present in 50 pulses.d^-1 using a sampling frequency of 15-min to collect a 24-h composite sample, the attenuation uncertainty can range from 94% (0% degradability) to 9% (90% degradability). The estimation of attenuation in rivers is less critical than in WWTPs, as the attenuation uncertainty was lower than 10% for all evaluated scenarios. Interestingly, the errors in the estimates of attenuation are usually lower than those of loads for most sampling strategies and compound characteristics (e.g. consumption and degradability), although the opposite occurs for compounds with low consumption and inappropriate sampling strategies at the WWTP. Hence, when designing a sampling campaign, one should consider the influence of compounds' consumption and degradability as well as the desired level of accuracy in attenuation estimations.

The popularity of new psychoactive substances (NPS) has grown in recent years, with certain NPS commonly and preferentially consumed even following the introduction of preventative legislation. With the objective to improve the knowledge on the use of NPS, a rapid and very sensitive method was developed for the determination of ten priority NPS (N-ethylcathinone, methylenedioxypyrovalerone (MDPV), methylone, butylone, methedrone, mephedrone, naphyrone, 25-C-NBOMe, 25-I-NBOMe and 25-B-NBOMe) in influent wastewater. Sample clean-up and pre-concentration was made by off-line solid phase extraction (SPE) with Oasis MCX cartridges. Isotopically labelled internal standards were used to correct for matrix effects and potential SPE losses. Following chromatographic separation on a C₁₈ column within 6 min, the compounds were measured by tandem mass spectrometry in positive ionization mode. The method was optimised and validated for all compounds. Limits of quantification were evaluated by spiking influent wastewater samples at 1 or 5 ng/L. An investigation into the stability of these compounds in influent wastewater was also performed, showing that, following acidification at pH 2, all compounds were relatively stable for up to 7 days. The method was then applied to influent wastewater samples from eight European countries, in which mephedrone, methylone and MDPV were detected. This work reveals that although NPS use is not as extensive as for classic illicit drugs, the application of a highly sensitive analytical procedure makes their detection in wastewater possible. The developed analytical methodology forms the basis of a subsequent model-based back-calculation of abuse rate in urban areas (i.e. wastewater-based epidemiology).

Monitoring of microbial drinking water quality is a key component for ensuring safety and understanding risk, but conventional monitoring strategies are typically based on low sampling frequencies (e.g., quarterly or monthly). This is of concern because many drinking water sources, such as karstic springs are often subject to changes in bacterial concentrations on much shorter time scales (e.g., hours to days), for example after precipitation events. Microbial contamination events are crucial from a risk assessment perspective and should therefore be targeted by monitoring strategies to establish both the frequency of their occurrence and the magnitude of bacterial peak concentrations. In this study we used monitoring data from two specific karstic springs. We assessed the performance of conventional monitoring based on historical records and tested a number of alternative strategies based on a high-resolution data set of bacterial concentrations in spring water collected with online flow cytometry (FCM). We quantified the effect of increasing sampling frequency and found that for the specific case studied, at least bi-weekly sampling would be needed to detect precipitation events with a probability of >90%. We then proposed an optimized monitoring strategy with three targeted samples per event, triggered by precipitation measurements. This approach is more effective and efficient than simply increasing overall sampling frequency. It would enable the water utility to (1) analyze any relevant event and (2) limit median underestimation of peak concentrations to approximately 10%. We conclude with a generalized perspective on sampling optimization and argue that the assessment of short-term dynamics causing microbial peak loads initially requires increased sampling/analysis efforts, but can be optimized subsequently to account for limited resources. This offers water utilities and public health authorities systematic ways to evaluate and optimize their current monitoring strategies.

Wastewater-based epidemiology is a promising and complementary tool for estimating drug use by the general population, based on the quantitative analysis of specific human metabolites of illicit drugs in urban wastewater. Cannabis is the most commonly used illicit drug and of high interest for epidemiologists. However, the inclusion of its main human urinary metabolite 11-nor-9-carboxy-Δ⁹-tetrahydrocannabinol (THC-COOH) in wastewater-based epidemiology has presented several challenges and concentrations seem to depend heavily on environmental factors, sample preparation and analyses, commonly resulting in an underestimation. The aim of the present study is to investigate, identify and diminish the source of bias when analysing THC-COOH in wastewater. Several experiments were performed to individually assess different aspects of THC-COOH determination in wastewater, such as the number of freeze-thaw cycles, filtration, sorption to different container materials and in-sample stability, and the most suitable order of preparatory steps. Results highlighted the filtration step and adjustment of the sample pH as the most critical parameters to take into account when analysing THC-COOH in wastewater. Furthermore, the order of these initial steps of the analytical procedure is crucial. Findings were translated into a recommended best-practice protocol and an inter-laboratory study was organized with eight laboratories that tested the performance of the proposed procedure. Results were found satisfactory with z-scores ≤ 2.

To which extent illicit drugs are transformed during in-sewer transport, depends on a number of factors: i) substance-specific transformation rates, ii) environmental conditions, iii) point of discharge (location of drug user) and iv) sewer network properties, primarily hydraulic residence time (HRT) and the ratio of biofilm contact area to wastewater volume (A/V_eq).
Assessing associated uncertainties typically requires numerous simulations. Therefore, we propose a new two-step modeling framework: 1) Quantify hydrodynamic conditions. This computationally demanding step was performed once in SWMM to derive HRT and A/V_eq for each potential point of discharge (node) in three catchments of different size. 2) Estimate biomarker loss. In this step, Monte Carlo simulations were performed for defined scenarios. Depending on assumptions about drug user distribution and prevalence, a number of nodes was sampled. For each node an empirical first-order transformation model was applied with flow-path-corresponding HRT and A/V_eq from step 1. Biotic and abiotic transformation rates were sampled from distributions combining variability of different biofilms.
In our modeling study, median losses were >30% for amphetamine, 6-monoacetylmorphine and 6-acetylcodeine in all three catchments with high uncertainty (5%–100% loss), which would imply a systematic underestimation of consumption when neglecting in-sewer processes. Median losses for 21 other investigated biomarkers were <10% with different uncertainty ranges – “no substantial transformation” was confirmed for nine substances in a real sewer segment with a 2-h residence time. Transferability of these results must be tested for other catchments. To further reduce uncertainty, mainly additional knowledge on transformation rates, particularly in biofilm, and their distribution across a sewer network is needed to update model input objectively. Our approach allows efficient testing and, furthermore, can be expanded for many other human biomarkers. Accounting for biomarker stability during in-sewer transport will avoid biased estimates and further improve wastewater-based epidemiology.

High spatio-temporal variability characterizes micropollutants discharged from separate and combined sewers. This challenges monitoring and prediction. We propose passive samplers (Chemcatcher_® for polar, organic substances) as an alternative to active water sampling. Our results indicate sufficient sensitivity of passive samplers for short exposures so that typical rain event durations (<30 h) can be sampled integratively. Although time-weighted average concentrations estimated via passive sampling are higherthan in composite water samples -on average by a factor 2.7 - we conclude that passive sampling is a cost-effective approach to identify locations with critical concentration ranges.

A key uncertainty of wastewater-based epidemiology is the size of the population which contributed to a given wastewater sample. We previously developed and validated a Bayesian inference model to estimate population size based on 14 population markers which: (1) are easily measured and (2) have mass loads which correlate with population size. However, the potential uncertainty of the model prediction due to in-sewer degradation of these markers was not evaluated. In this study, we addressed this gap by testing their stability under sewer conditions and assessed whether degradation impacts the model estimates. Five markers, which formed the core of our model, were stable in the sewers while the others were not. Our evaluation showed that the presence of unstable population markers in the model did not decrease the precision of the population estimates providing that stable markers such as acesulfame remained in the model. However, to achieve the minimum uncertainty in population estimates, we propose that the core markers to be included in population models for other sites should meet two additional criteria: (3) negligible degradation in wastewater to ensure the stability of chemicals during collection; and (4) < 10% in-sewer degradation could occur during the mean residence time of the sewer network.

Aim: Analysis of wastewater samples can be used to assess population drug use, but reporting and statistical issues have limited the utility of the approach for epidemiology due to analytical results that are below the limit of quantification or detection. Unobserved or non-quantifiable—censored—data are common and likely to persist as the methodology is applied to more municipalities and a broader array of substances. We demonstrate the use of censored data techniques and account for measurement errors to explore distributions and annual estimates of the daily mean level of drugs excreted per capita.
Measurements: Daily 24-hour composite wastewater samples for 56 days in 2009 were obtained using a random sample stratified by day of week and season for 19 municipalities in the Northwest region of the U.S.
Methods: Methamphetamine, benzoylecgonine (cocaine metabolite), 3,4 methylenedioxymethamphetamine (MDMA), methadone, oxycodone and hydrocodone were identified and quantified in wastewater samples. Four statistical approaches (reporting censoring, Maximum Likelihood Estimation, Kaplan-Meier estimates, or complete data calculations) were used to estimate an annual average, including confidence bounds where appropriate, dependent upon the amount of censoring in the data.
Findings: The proportion of days within a year with censored data varied greatly by drug across the 19 municipalities, with MDMA varying the most (4% to 94% of observations censored). The different statistical approaches each needed to be used given the levels of censoring of measured drug concentrations. Figures incorporating confidence bounds allow visualization of the data that facilitates appropriate comparisons across municipalities.
Conclusions: Results from wastewater sampling that are below detection or quantification limits contain important information and can be incorporated to create a more complete and valid estimate of drug excretion.

Background: Monitoring the scale of pharmaceuticals, illicit and licit drugs consumption is important to assess the needs of law enforcement and public health, and provides more information about the different trends within different countries. Community drug use patterns are usually described by national surveys, sales and seizure data. Wastewater-based epidemiology (WBE) has been shown to be a reliable approach complementing such surveys.
Method: This study aims to compare and correlate the consumption estimates of pharmaceuticals, illicit drugs, alcohol, nicotine and caffeine from wastewater analysis and other sources of information. Wastewater samples were collected in 2015 from 8 different European cities over a one week period, representing a population of approximately 5 million people. Published pharmaceutical sale, illicit drug seizure and alcohol, tobacco and caffeine use data were used for the comparison.
Results: High agreement was found between wastewater and other data sources for pharmaceuticals and cocaine, whereas amphetamines, alcohol and caffeine showed a moderate correlation. methamphetamine and 3,4-methylenedioxymethamphetamine (MDMA) and nicotine did not correlate with other sources of data. Most of the poor correlations were explained as part of the uncertainties related with the use estimates and were improved with other complementary sources of data.
Conclusions: This work confirms the promising future of WBE as a complementary approach to obtain a more accurate picture of substance use situation within different communities. Our findings suggest further improvements to reduce the uncertainties associated with both sources of information in order to make the data more comparable.

Background: Wastewater analysis is an innovative approach that allows monitoring illicit drug use at the community level. This study focused on investigating geographical differences in drug consumption by comparing epidemiological, crime and wastewater data.
Methods: Wastewater samples were collected in 19 cities across Germany and Switzerland during one week, covering a population of approximately 8.1 million people. Self-report data and consumption offences for the investigated areas were used for comparison and to investigate differences between the indicators.
Results: Good agreement between data sources was observed for cannabis and amphetamine-type stimulants, whereas substantial discrepancies were observed for cocaine. In Germany, an important distinction could be made between Berlin, Dortmund and Munich, where cocaine and particularly amphetamine were more prevalent, and Dresden, where methamphetamine consumption was clearly predominant. Cocaine consumption was relatively homogenous in the larger urban areas of Switzerland, although prevalence and offences data suggested a more heterogeneous picture. Conversely, marked regional differences in amphetamine and methamphetamine consumption could be highlighted.
Conclusions: Combining the available data allowed for a better understanding of the geographical differences regarding prevalence, typology and amounts of substances consumed. For cannabis and amphetamine-type stimulants, the complementarity of survey, police and wastewater data could be highlighted, although notable differences could be identified when considering more stigmatised drugs (i.e. cocaine and heroin). Understanding illicit drug consumption at the national scale remains a difficult task, yet this research illustrates the added value of combining complementary data sources to obtain a more comprehensive and accurate picture of the situation.

Introduction and Aims. Illicit drug use is known to occur among inmate populations of correctional (prison) facilities. Conventional approaches to monitor illicit drug use in prisons include random urinalyses (RUA). Conventional approaches are expected to be prone to bias because prisoners may be aware of which days of the week RUAs are conducted. Therefore, we wanted to compare wastewater loads for methamphetamine and cocaine during days with RUA testing and without. Design and Methods. We collected daily 24-h composite samples of wastewater by continuous sampling, computed daily loads for 1 month and compared the frequency of illicit drug detection to the number of positive RUAs. Diurnal data also were collected for 3 days to determine within-day patterns of illicit drugs excretion.Results. Methamphetamine was observed in each sample of prison wastewater with no significant difference in daily mass loads between RUA testing and non-testing days. Cocaine and its major metabolite, benzoylecgonine, were observed only at levels below quantification in prison wastewater. Six RUAs were positive for methamphetamine during the month while none were positive for cocaine out of the 243 RUAs conducted.Discussion and Conclusions. Wastewater analyses offer data regarding the frequency of illicit drug excretion inside the prison that RUAs alone could not detect.

Human land uses and population growth represent major global threats to biodiversity and ecosystem services. Understanding how biological communities respond to multiple drivers of human-induced environmental change is fundamental for conserving ecosystems and remediating degraded habitats. Here, we used a replicated ‘real-world experiment’ to study the responses of invertebrate communities to wastewater perturbations across a land-use intensity gradient in 12 Swiss streams. We used different taxonomy and trait-based community descriptors to establish the most sensitive indicators detecting impacts and to help elucidate potential causal mechanisms of change. First, we predicted that streams in catchments adversely impacted by human land-uses would be less impaired by wastewater inputs because their invertebrate communities should be dominated by pollution-tolerant taxa (‘environmental context’). Second, we predicted that the negative effects of wastewater on stream invertebrate communities should be larger in streams that receive proportionally more wastewater (‘magnitude of disturbance’). In support of the ‘environmental context’ hypothesis, we found that change in the Saprobic Index (a trait-based indicator of tolerance to organic pollution) was associated with upstream community composition; communities in catchments with intensive agricultural land uses (e.g., arable cropping and pasture) were generally more resistant to eutrophication associated with wastewater inputs. We also found support for the ‘magnitude of disturbance’ hypothesis. The SPEAR Index (a trait-based indicator of sensitivity to pesticides) was more sensitive to the relative input of effluent, suggesting that toxic influences of wastewater scale with dilution. Whilst freshwater pollution continues to be a major environmental problem, our findings highlight that the same anthropogenic pressure (i.e., inputs of wastewater) may induce different ecological responses depending on the environmental context and community metrics used. Thus, remediation strategies aiming to improve stream ecological status (e.g., rehabilitating degraded reaches) need to consider upstream anthropogenic influences and the most appropriate indicators of restoration success.

Sampling and analysis of wastewater from municipal wastewater treatment plants (WWTPs) has become a useful tool for understanding exposure to chemicals. Both wastewater based studies and management and planning of the catchment require information on catchment population in the time of monitoring. Recently, a model has been developed and calibrated using selected pharmaceutical and personal care products (PPCPs) measured in influent wastewater for estimating population in different catchments in Australia. The present study aimed at evaluating the feasibility of utilizing this population estimation approach in China. Twenty-four hour composite influent samples were collected from 31 WWTPs in 17 cities with catchment sizes from 200,000–3,450,000 people representing all seven regions of China. The samples were analyzed for 19 PPCPs using liquid chromatography coupled to tandem mass spectrometry in direct injection mode. Eight chemicals were detected in more than 50% of the samples. Significant positive correlations were found between individual PPCP mass loads and population estimates provided by WWTP operators. Using the PPCP mass load modeling approach calibrated with WWTP operator data, we estimated the population size of each catchment with good agreement with WWTP operator values (between 50–200% for all sites and 75–125% for 23 of the 31 sites). Overall, despite much lower detection and relatively high heterogeneity in PPCP consumption across China the model provided a good estimate of the population contributing to a given wastewater sample. Wastewater analysis could also provide objective PPCP consumption status in China.

Wastewater-based epidemiology is increasingly being used as a tool to monitor drug use trends. To minimize costs, studies have typically monitored a small number of days. However, cycles of drug use may display weekly and seasonal trends that affect the accuracy of monthly or annual drug use estimates based on a limited number of samples. This study aimed to rationalize sampling methods for minimizing the number of samples required while maximizing information about temporal trends. A range of sampling strategies were examined: (i) targeted days (e.g., weekends), (ii) completely random or stratified random sampling, and (iii) a number of sampling strategies informed by known weekly cycles in drug use data. Using a time-series approach, analysis was performed for four drugs (MDMA, methamphetamine, cocaine, methadone) collected through a continuous sampling program over 14 months. Results showed, for drugs with weekly cycles (MDMA, methamphetamine and cocaine in this sample), sampling strategies which made use of those weekly cycles required fewer samples to obtain similar information as sampling 5 days per week and had better accuracy than stratified random sampling techniques.

A model to predict the mass flows and concentrations of pharmaceuticals predominantly used in hospitals across a large number of sewage treatment plant (STP) effluents and river waters was developed at high spatial resolution. It comprised 427 geo-referenced hospitals and 742 STPs serving 98% of the general population in Switzerland. In the modeled base scenario, domestic, pharmaceutical use was geographically distributed according to the population size served by the respective STPs. Distinct hospital scenarios were set up to evaluate how the predicted results were modified when pharmaceutical use in hospitals was allocated differently; for example, in proportion to number of beds or number of treatments in hospitals. The hospital scenarios predicted the mass flows and concentrations up to 3.9 times greater than in the domestic scenario for iodinated X-ray contrast media (ICM) used in computed tomography (CT), and up to 6.7 times greater for gadolinium, a contrast medium used in magnetic resonance imaging (MRI). Field measurements showed that ICM and gadolinium were predicted best by the scenarios using number of beds or treatments in hospitals with the specific facilities (i.e., CT and/or MRI). Pharmaceuticals used both in hospitals and by the general population (e.g., cyclophosphamide, sulfamethoxazole, carbamazepine, diclofenac) were predicted best by the scenario using the number of beds in all hospitals, but the deviation from the domestic scenario values was only small. Our study demonstrated that the bed number-based hospital scenarios were effective in predicting the geographical distribution of a diverse range of pharmaceuticals in STP effluents and rivers, while the domestic scenario was similarly effective on the scale of large river-catchments.

Wastewater analysis, or wastewater-based epidemiology, has become a common tool to monitor trends of illicit drug consumption around the world. In this study, we examined trends in cocaine, 3,4-methylenedioxymethamphetamine (MDMA) and methamphetamine consumption by measuring their residues in wastewater from two wastewater treatment plants in Australia (specifically, an urban and a rural catchment, both in South East Queensland) between 2009 and 2015. With direct injection of the samples, target analytes were identified and quantified using liquid chromatography-mass spectrometry. Cocaine and MDMA residues and metabolites were mainly quantifiable in the urban catchment while methamphetamine residues were consistently detected in both urban and rural catchments. There was no consistent trend in the population normalised mass loads observed for cocaine and MDMA at the urban site between 2009 and 2015. In contrast, there was a five-fold increase in methamphetamine consumption over this period in this catchment. For methamphetamine consumption, the rural area showed a very similar trend as the urban catchment starting at a lower baseline. The observed increase in per capita loads of methamphetamine via wastewater analysis over the past six years in South East Queensland provides objective evidence for increased methamphetamine consumption in the Australian population while the use of other illicit stimulants remained relatively stable.

Wastewater-based epidemiology (WBE) applies advanced analytical methods to quantify drug residues in wastewater with the aim to estimate illicit drug use at the population level. Transformation processes during transport in sewers (chemical and biological reactors) and storage of wastewater samples before analysis are expected to change concentrations of different drugs to varying degrees. Ignoring transformation for drugs with low to medium stability will lead to an unknown degree of systematic under- or overestimation of drug use, which should be avoided. This review aims to summarize the current knowledge related to the stability of commonly investigated drugs and, furthermore, suggest a more effective approach to future experiments. From over 100 WBE studies, around 50 mentioned the importance of stability and 24 included tests in wastewater. Most focused on in-sample stability (i.e., sample preparation, preservation and storage) and some extrapolated to in-sewer stability (i.e., during transport in real sewers). While consistent results were reported for rather stable compounds (e.g., MDMA and methamphetamine), a varying range of stability under different or similar conditions was observed for other compounds (e.g., cocaine, amphetamine and morphine). Wastewater composition can vary considerably over time, and different conditions prevail in different sewer systems. In summary, this indicates that more systematic studies are needed to: i) cover the range of possible conditions in sewers and ii) compare results more objectively. To facilitate the latter, we propose a set of parameters that should be reported for in-sewer stability experiments. Finally, a best practice of sample collection, preservation, and preparation before analysis is suggested in order to minimize transformation during these steps.

To estimate drug consumption more reliably, wastewater-based epidemiology would benefit from a better understanding of drug residue stability during in-sewer transport. We conducted batch experiments with real, fresh wastewater and sewer biofilms. Experimental conditions mimic small to medium-sized gravity sewers with a relevant ratio of biofilm surface area to wastewater volume (33 m² m^–3). The influences of biological, chemical, and physical processes on the transformation of 30 illicit drug and pharmaceutical residues were quantified. Rates varied among locations and over time. Three substances were not stable—that is, >20% transformation, mainly due to biological processes—at least for one type of tested biofilm for a residence time ≤2 h: amphetamine, 6-acetylcodeine, and 6-monoacetylmorphine. Cocaine, ecgonine methyl ester, norcocaine, cocaethylene, and mephedrone were mainly transformed by chemical hydrolysis and, hence, also unstable in sewers. In contrast, ketamine, norketamine, O-desmethyltramadol, diclofenac, carbamazepine, and methoxetamine were not substantially affected by in-sewer processes under all tested conditions and residence times up to 12 h. Our transformation rates include careful quantification of uncertainty and can be used to identify situations in which specific compounds are not stable. This will improve accuracy and uncertainty estimates of drug consumption when applied to the back-calculation.

Wet-weather discharges contribute to anthropogenic micropollutant loads entering the aquatic environment. Thousands of wet-weather discharges exist in Swiss sewer systems, and we do not have the capacity to monitor them all. We consequently propose a model-based approach designed to identify critical discharge points in order to support effective monitoring.
We applied a dynamic substance flow model to four substances representing different entry routes: indoor (Triclosan, Mecoprop, Copper) as well as rainfall-mobilized (Glyphosate, Mecoprop, Copper) inputs. The accumulation on different urban land-use surfaces in dry weather and subsequent substance-specific wash-off is taken into account. For evaluation, we use a conservative screening approach to detect critical discharge points. This approach considers only local dilution generated onsite from natural, unpolluted areas, i.e. excluding upstream dilution.
Despite our conservative assumptions, we find that the environmental quality standards for Glyphosate and Mecoprop are not exceeded during any 10-min time interval over a representative one-year simulation period for all 2500 Swiss municipalities. In contrast, the environmental quality standard is exceeded during at least 20% of the discharge time at 83% of all modelled discharge points for Copper and at 71% for Triclosan. For Copper, this corresponds to a total median duration of approximately 19 days per year. For Triclosan, discharged only via combined sewer overflows, this means a median duration of approximately 10 days per year. In general, stormwater outlets contribute more to the calculated effect than combined sewer overflows for rainfall-mobilized substances. We further evaluate the Urban Index (A_{urban,impervious}/A_natural) as a proxy for critical discharge points: catchments where Triclosan and Copper exceed the corresponding environmental quality standard often have an Urban Index >0.03.
A dynamic substance flow analysis allows us to identify the most critical discharge points to be prioritized for more detailed analyses and monitoring. This forms a basis for the efficient mitigation of pollution.

Quantitative measurement of drug consumption biomarkers in wastewater can provide objective information on community drug use patterns and trends. This study presents the measurement of alcohol consumption in 20 cities across 11 countries through the use of wastewater-based epidemiology (WBE), and reports the application of these data for the risk assessment of alcohol on a population scale using the margin of exposure (MOE) approach. Raw 24-h composite wastewater samples were collected over a one-week period from 20 cities following a common protocol. For each sample a specific and stable alcohol consumption biomarker, ethyl sulfate (EtS) was determined by liquid chromatography coupled to tandem mass spectrometry. The EtS concentrations were used for estimation of per capita alcohol consumption in each city, which was further compared with international reports and applied for risk assessment by MOE. The average per capita consumption in 20 cities ranged between 6.4 and 44.3 L/day/1000 inhabitants. An increase in alcohol consumption during the weekend occurred in all cities, however the level of this increase was found to differ. In contrast to conventional data (sales statistics and interviews), WBE revealed geographical differences in the level and pattern of actual alcohol consumption at an inter-city level. All the sampled cities were in the "high risk" category (MOE < 10) and the average MOE for the whole population studied was 2.5. These results allowed direct comparisons of alcohol consumption levels, patterns and risks among the cities. This study shows that WBE can provide timely and complementary information on alcohol use and alcohol associated risks in terms of exposure at the community level.

Wastewater analysis has been demonstrated to be a complementary approach for assessing the overall patterns of drug use by a population while the full potential of wastewater-based epidemiology has yet to be explored. F₂-isoprostanes are a prototype wastewater biomarker to study the cumulative oxidative stress at a community level. In this work, 8-iso-prostaglandin F_2α (8-iso-PGF_2α) was analysed in raw 24 h-composite wastewater samples collected from 4 Norwegian and 7 other European cities in 2014 and 2015. Using the same samples, biomarkers of alcohol (ethyl sulfate) and tobacco (trans-3′-hydroxycotinine) use were also analysed to investigate any possible correlation between 8-iso-PGF_2α and the consumption of the two drugs. The estimated per capita daily loads of 8-iso-PGF_2α in the 11 cities ranged between 2.5 and 9.9 mg/day/1000 inhabitants with a population-weighted mean of 4.8 mg/day/1000 inhabitants. There were no temporal trends observed in the levels of 8-iso-PGF_2α, however, spatial differences were found at the inter-city level correlating to the degree of urbanisation. The 8-iso-PGF_2α mass load was found to be strongly associated with that of trans-3′-hydroxycotinine while it showed no correlation with ethyl sulfate. The present study shows the potential for 8-iso-PGF_2α as a wastewater biomarker for the assessment of community public health.

The economic crisis plaguing Greece was expected to impact consumption of pharmaceuticals and illicit drugs – a priori to an unknown extent. We quantified the change of use for various classes of licit and illicit drugs by monitoring Athens’ wastewater from 2010 to 2014. A high increase in the use of psychoactive drugs was detected between 2010 and 2014, especially for antipsychotics (35-fold), benzodiazepines (19-fold), and antidepressants (11-fold). This directly reflects the perceived increase of incidences associated with mental illnesses in the population, as a consequence of severe socioeconomic changes. Other therapeutic classes, like antiepileptics, hypertensives, and gastric and ulcer drugs also showed an increase in use (from 2-fold increase for antiepileptics to 13-fold for hypertensives). In contrast, the overall use of antibiotics and NSAIDs decreased. For mefenamic acid, an almost 28-fold decrease was observed. This finding is likely related to the reduction in drug expenditure applied in public health. A 2-fold increase of methamphetamine use was detected, associated with a cheap street drug called ″sisa″ (related to marginal conducts), which is a health concern. MDMA (5-fold) and methadone (7-fold) use showed also an increase, while cocaine and cannabis estimates did not show a clear trend.

Introduction and Aims. Wastewater analysis (WWA) is intended to be a direct and objective method of measuring substance use in large urban populations. It has also been used to measure prison substance use in two previous studies. The application of WWA in this context has raised questions as to how best it might be used to measure illicit drug use in prisons, and whether it can also be used to measure prescription misuse. We applied WWA to a small regional prison to measure the use of 12 licit and illicit substances. We attempted to measure the non-medical use of methadone and buprenorphine and to compare our findings with the results of the prison's mandatory drug testing (MDT). Design and Methods. Representative daily composite samples were collected for two periods of 12 consecutive days in May to July 2013 and analysed for 18 drug metabolites. Prescription data and MDT results were obtained from the prison and compared with the substance use estimates calculated from WWA data. Results. Daily use of methamphetamine, methadone, buprenorphine and codeine was detected, while sporadic detection of ketamine and methylone was also observed. Overall buprenorphine misuse appeared to be greater than methadone misuse. Discussion and Conclusions. Compared with MDT, WWA provides a more comprehensive picture of prison substance use. WWA also has the potential to measure the misuse of medically prescribed substances. However, a great deal of care must be exercised in quantifying the usage of any substance in small populations, such as in prisons.

Population size is crucial when estimating population-normalized drug consumption (PNDC) from wastewater-based drug epidemiology (WBDE). Three conceptually different population estimates can be used: de jure (common census, residence), de facto (all persons within a sewer catchment), and chemical loads (contributors to the sampled wastewater). De facto and chemical loads will be the same where all households contribute to a central sewer system without wastewater loss. This study explored the feasibility of determining a de facto population and its effect on estimating PNDC in an urban community over an extended period. Drugs and other chemicals were analyzed in 311 daily composite wastewater samples. The daily estimated de facto population (using chemical loads) was on average 32% higher than the de jure population. Consequently, using the latter would systemically overestimate PNDC by 22%. However, the relative day-to-day pattern of drug consumption was similar regardless of the type of normalization as daily illicit drug loads appeared to vary substantially more than the population. Using chemical loads population, we objectively quantified the total methodological uncertainty of PNDC and reduced it by a factor of 2. Our study illustrated the potential benefits of using chemical loads population for obtaining more robust PNDC data in WBDE.

Welchen Wert misst die Bevölkerung der Elimination von Mikroverunreinigungen in den Kläranlagen zu? Aus den Antworten von 1000 Deutschschweizern und Deutschschweizerinnen wurde der wirtschaftliche Nutzen des Ausbaus von Abwasserreinigungsanlagen abgeleitet. Der Vergleich mit den veranschlagten Kosten zeigt, dass der Ausbau in der Schweiz gerechtfertigt ist.

The use of organophosphate esters (PFRs) as flame retardants and plasticizers has increased due to the ban of some brominated flame retardants. There is however some concern regarding the toxicity, particularly carcinogenicity and neurotoxicity, of some of the PFRs. In this study we applied wastewater analysis to assess use of PFRs by the Australian population. Influent samples were collected from eleven wastewater treatment plants (STPs) in Australia on Census day and analysed for PFRs using gas chromatography coupled with mass spectrometry (GC-MS). Per capita mass loads of PFRs were calculated using the accurate Census head counts. The results indicate that tris(2-butoxyethyl) phosphate (TBOEP) has the highest per capita input into wastewater followed by tris(2-chloroisopropyl) phosphate (TCIPP), tris(isobutyl) phosphate (TIBP), tris(2-chloroethyl) phosphate (TCEP) and tris(1,3-dichloroisopropyl) phosphate (TDCIPP). Similar PFR profiles were observed across the Australian STPs and a comparison with European and U.S. STPs indicated similar PFR concentrations. We estimate that approximately 2.1 mg person⁻¹ day⁻¹ of PFRs are input into Australian wastewater which equates to 16 tonnes per annum.

Fluctuations in ammonium (NH₄ ⁺), measured as NH ₄-N loads using an ion-selective electrode installed at the inlet of a sewage treatment plant, showed a distinctive pattern which was associated to weekly (i.e., commuters) and seasonal (i.e., holidays) fluctuations of the population. Moreover, population size estimates based on NH₄-N loads were lower compared to census data. Diurnal profiles of benzoylecgonine (BE) and 11-nor-9-carboxy-δ9-tetrahydrocannabinol (THC-COOH) were shown to be strongly correlated to NH₄-N. Characteristic patterns, which reflect the prolonged nocturnal activity of people during the weekend, could be observed for BE, cocaine, and a major metabolite of MDMA (i.e., 4-hydroxy-3- methoxymethamphetamine). Additional 24 h composite samples were collected between February and September 2013. Per-capita loads (i.e., grams per day per 1000 inhabitants) were computed using census data and NH₄-N measurements. Normalization with NH₄-N did not modify the overall pattern, suggesting that the magnitude of fluctuations in the size of the population is negligible compared to those of illicit drug loads. Results show that fluctuations in the size of the population over longer periods of time or during major events can be monitored using NH₄-N loads: either using raw NH₄-N loads or population size estimates based on NH ₄-N loads, if information about site-specific NH₄-N population equivalents is available.

Contamination of freshwater with micropollutants (MPs) is a growing concern worldwide. Even at very low concentrations, MPs can have adverse effects on aquatic ecosystems and possibly also on human health. Switzerland is one of the first countries to start implementing a national policy to reduce MPs in the effluents of municipal sewage treatment plants (STPs). This paper estimates the benefits of upgrading STPs based on public’s stated preferences. To assess public demand for the reduction of the environmental and health risks of MPs, we conducted a choice experiment in a national online survey. The results indicate that the average willingness to pay per household is CHF 100 (US$ 73) annually for reducing the potential environmental risk of MPs to a low level. These benefits, aggregated over households in the catchment of the STPs to be upgraded, generate a total annual economic value of CHF 155 million (US$ 113 million). This compares with estimated annual costs for upgrading 123 STPs of CHF 133 million (US$ 97 million) or CHF 86 (US$ 63) per household connected to these STPs. Hence, a cost-benefit analysis justifies the investment decision from an economic point of view and supports the implementation of the national policy in the ongoing political discussion.

An important uncertainty when estimating per capita consumption of, for example, illicit drugs by means of wastewater analysis (sometimes referred to as "sewage epidemiology") relates to the size and variability of the de facto population in the catchment of interest. In the absence of a day-specific direct population count any indirect surrogate model to estimate population size lacks a standard to assess associated uncertainties. Therefore, the objective of this study was to collect wastewater samples at a unique opportunity, that is, on a census day, as a basis for a model to estimate the number of people contributing to a given wastewater sample. Mass loads for a wide range of pharmaceuticals and personal care products were quantified in influents of ten sewage treatment plants (STP) serving populations ranging from approximately 3500 to 500 000 people. Separate linear models for population size were estimated with the mass loads of the different chemical as the explanatory variable: 14 chemicals showed good, linear relationships, with highest correlations for acesulfame and gabapentin. De facto population was then estimated through Bayesian inference, by updating the population size provided by STP staff (prior knowledge) with measured chemical mass loads. Cross validation showed that large populations can be estimated fairly accurately with a few chemical mass loads quantified from 24-h composite samples. In contrast, the prior knowledge for small population sizes cannot be improved substantially despite the information of multiple chemical mass loads. In the future, observations other than chemical mass loads may improve this deficit, since Bayesian inference allows including any kind of information relating to population size.

Aims. Quantifying illicit drug loads through wastewater analysis (WWA) is an alternative approach to estimating population drug use. This study investigated the variability of daily drug loads in wastewater and their relationships to environmental factors over an extended period to: (i) explore the suitability of WWA in small populations and (ii) optimize the monitoring design for future studies.
Design, Setting, Participants. Daily wastewater samples (n = 1369 consecutive days) from a German village with approximately 7160 inhabitants.
Measurements. Samples were analysed for cocaine and benzoylecgonine with liquid chromatography-tandem mass spectrometry. Time-series analysis was used to explore the effects of weather and other factors on daily cocaine loads. Subsampling was used to assess monitoring design.
Findings. Cocaine loads [mean = 652 mg_COC/day, standard deviation (SD) = 498 mg_COC/day] increased over the study period, with higher values during winter and spring. Despite high day-to-day variation, loads were significantly higher during weekends [+161 mg_COC/day, 95% confidence interval (CI) = 115–207 mg_COC/day, P < 10⁻⁴] and days with frost (+114 mg_COC/day, 95% CI = 6–223 mg_COC/day, P = 0.039) or snow (+150 mg_COC/day, 95% CI = 46–253 mg_COC/day, P = 0.005). Annual means estimated from 1-week periods were subject to approximately 60% relative error. Increasing sample size and changing sampling from consecutive days to stratified random decreased this uncertainty.
Conclusions. Day-to-day variation and seasonality of drug loads from the few long-term wastewater studies available to date suggest that up to 56 stratified random samples are required to obtain reliable (expected uncertainty around 10%) annual estimates of drug loads. Successfully assessing changes in consumption patterns or relationships to external factors requires larger sample sizes than estimating annual means, which holds true for high-prevalence drugs in small communities and low-prevalence drugs in big cities.

If asked whether you had consumed illicit drugs recently, would you admit it? If yes, could you precisely recall types of drug, times and amounts used? If you were the person commissioned with the task of quantifying drug use, what approach would you use given the social stigma attached with such behavior? We measure drug residues in sewage, which represents urine of entire populations, to provide an objective estimate of total drug use in a region. In transdisciplinary projects, sewage-based results provide valuable information at unrivaled spatiotemporal resolution complementing traditional data.

Aims. To perform wastewater analyses to assess spatial differences and temporal changes of illicit drug use in a large European population.
Design. Analyses of raw wastewater over a 1-week period in 2012 and 2013.
Setting and Participants. Catchment areas of wastewater treatment plants (WWTPs) across Europe, as follows: 2012: 25 WWTPs in 11 countries (23 cities, total population 11.50 million); 2013: 47 WWTPs in 21 countries (42 cities, total population 24.74 million).
Measurements. Excretion products of five illicit drugs (cocaine, amphetamine, ecstasy, methamphetamine, cannabis) were quantified in wastewater samples using methods based on liquid chromatography coupled to mass spectrometry.
Findings. Spatial differences were assessed and confirmed to vary greatly across European metropolitan areas. In general, results were in agreement with traditional surveillance data, where available. While temporal changes were substantial in individual cities and years (P ranging from insignificant to <10⁻³), overall means were relatively stable. The overall mean of methamphetamine was an exception (apparent decline in 2012), as it was influenced mainly by four cities.
Conclusions. Wastewater analysis performed across Europe provides complementary evidence on illicit drug consumption and generally concurs with traditional surveillance data. Wastewater analysis can measure total illicit drug use more quickly and regularly than is the current norm for national surveys, and creates estimates where such data does not exist.

Prison substance use is a major concern for prison authorities and the wider community. Australia has responded to this problem by implementing the National Corrections Drug Strategy. Across Australia, the true extent of prison substance use cannot be determined. As a result, the effectiveness of the interventions employed as part of this strategy cannot be properly assessed. This has important implications for the allocation of corrective services resources and future policy development. This article explores the benefits and limitations, as well as the ethical and practical issues in using wastewater analysis (WWA) to measure levels of substance use in prisons. It reports results from the first application of WWA to an Australian prison, which supports the use of WWA in this context. Given the increasing concern for prescription misuse in prisons, we also highlight the novel use of WWA to measure the extent of prescription misuse by prisoners. The article concludes that as a result of its objectivity, sensitivity and cost-effectiveness, the use of WWA in prisons warrants further consideration in Australia.

The aim of this study was to integrally address the uncertainty associated with all the steps used to estimate community drug consumption through the chemical analysis of sewage biomarkers of illicit drugs. Uncertainty has been evaluated for sampling, chemical analysis, stability of drug biomarkers in sewage, back-calculation of drug use (specific case of cocaine), and estimation of population size in a catchment using data collected from a recent Europe-wide investigation and from the available literature. The quality of sampling protocols and analytical measurements has been evaluated by analyzing standardized questionnaires collected from 19 sewage treatments plants (STPs) and the results of an interlaboratory study (ILS), respectively. Extensive reviews of the available literature have been used to evaluate stability of drug biomarkers in sewage and the uncertainty related to back-calculation of cocaine use. Different methods for estimating population size in a catchment have been compared and the variability among the collected data was very high (7–55%). A reasonable strategy to reduce uncertainty was therefore to choose the most reliable estimation case by case. In the other cases, the highest uncertainties are related to the analysis of sewage drug biomarkers (uncertainty as relative standard deviation; RSD: 6–26% from ILS) and to the back-calculation of cocaine use (uncertainty; RSD: 26%). Uncertainty can be kept below 10% in the remaining steps, if specific requirements outlined in this work are considered. For each step, a best practice protocol has been suggested and discussed to reduce and keep to a minimum the uncertainty of the entire procedure and to improve the reliability of the estimates of drug use.

Models for predicting the fate of micropollutants (MPs) in wastewater treatment plants (WWTPs) have been developed to provide engineers and decision-makers with tools that they can use to improve their understanding of, and evaluate how to optimize, the removal of MPs and determine their impact on the receiving waters. This paper provides an overview of such models, and discusses the impact of regulation, engineering practice and research on model development. A review of the current status of MP models reveals that a single model cannot represent the wide range of MPs that are present in wastewaters today, and that it is important to start considering classes of MPs based on their chemical structure or ecotoxicological effect, rather than the individual molecules. This paper identifies potential future research areas that comprise (i) considering transformation products in MP removal analysis, (ii) addressing advancements in WWTP treatment technologies, (iii) making use of common approaches to data acquisition for model calibration and (iv) integrating ecotoxicological effects of MPs in receiving waters.

Discharge of silver nanoparticles (Ag-NP) from textiles and cosmetics, todays major application areas for metallic Ag-NP, into wastewater is inevitable. Transformation and removal processes in sewers and wastewater treatment plants (WWTP) will determine the impact of Ag-NP on aquatic and terrestrial environments, via the effluents of the WWTP and via the use of digested sludge as fertilizer. We thus conducted experiments addressing the behavior of Ag-NP in sewers and in WWTP.
We spiked Ag-NP to a 5 km long main trunk sewer and collected 40 wastewater samples after 500 m, 2400 m and 5000 m each according to the expected travel times of the Ag-NP. Excellent mass closure of the Ag derived by multiplying the measured Ag concentrations times the volumetric flow rates indicate an efficient transport of the Ag-NP without substantial losses to the sewer biofilm. Ag-NP reacted with raw wastewater in batch experiments were sulfidized to roughly 15% after 5 h reaction time as revealed by X-ray absorption spectroscopy (XAS). However, acid volatile sulfide (AVS) concentrations were substantially higher in the sewer channel (100 μM) compared to the batch experiments (3 μM; still sufficient to sulfidize spiked 2 μM Ag) possibly resulting in a higher degree of sulfidation in the sewer channel. We further investigated the removal efficiency of 10 nm and 100 nm Ag- and gold (Au)-NP coated with citrate or polyvinylpyrrolidone in activated sludge batch experiments. We obtained very high removal efficiencies (∼99%) irrespective of size and coating for Ag- and Au-NP, the latter confirming that the particle type was of minor importance with respect to the degree of NP removal. We observed a strong size dependence of the sulfidation kinetics. We conclude that Ag-NP discharged to the wastewater stream will become sulfidized to various degrees in the sewer system and are efficiently transported to the WWTP. The sulfidation of the Ag-NP will continue in the WWTP, but primarily depending on the size the Ag-NP, may not be complete. Very high removal efficiencies in the WWTP will divert most of the Ag-NP mass flow to the digester and only a small fraction of the Ag will be released to surface waters.

The measurement of illicit drug metabolites in raw wastewater is increasingly being adopted as an approach to objectively monitor population-level drug use, and is an effective complement to traditional epidemiological methods. As such, it has been widely applied in western countries. In this study, we utilised this approach to assess drug use patterns over nine days during April 2011 in Hong Kong. Raw wastewater samples were collected from the largest wastewater treatment plant serving a community of approximately 3.5 million people and analysed for excreted drug residues including cocaine, ketamine, methamphetamine, 3,4-methylenedioxymethamphetamine (MDMA) and key metabolites using liquid chromatography coupled with tandem mass spectrometry. The overall drug use pattern determined by wastewater analysis was consistent with that have seen amongst people coming into contact with services in relation to substance use; among our target drugs, ketamine (estimated consumption: 1400–1600 mg/day/1000 people) was the predominant drug followed by methamphetamine (180–200 mg/day/1000 people), cocaine (160–180 mg/day/1000 people) and MDMA (not detected). The levels of these drugs were relatively steady throughout the monitoring period. Analysing samples at higher temporal resolution provided data on diurnal variations of drug residue loads. Elevated ratios of cocaine to benzoylecgonine were identified unexpectedly in three samples during the evening and night, providing evidence for potential dumping events of cocaine. This study provides the first application of wastewater analysis to quantitatively evaluate daily drug use in an Asian metropolitan community. Our data reinforces the benefit of wastewater monitoring to health and law enforcement authorities for strategic planning and evaluation of drug intervention strategies.

Aims: To examine changes in illicit drug consumption between peak holiday season (23 December-3 January) in Australia and a control period two months later in a coastal urban area, an inland semi-rural area and an island populated predominantly by vacationers during holidays. Design: Analysis of representative daily composite wastewater samples collected from the inlet of the major wastewater treatment plant in each area. Setting: Three wastewater treatment plants. Participants: Wastewater treatment plants serviced approximately 350 000 persons in the urban area, 120 000 in the semi-rural area and 1100-2400 on the island. Measurements: Drug residues were analysed using liquid chromatography coupled to a tandem mass spectrometer. Per capita drug consumption was estimated. Changes in drug use were quantified using Hedges' g. Findings: During the holidays, cannabis consumption in the semi-rural area declined (g=-2.8) as did methamphetamine (-0.8), whereas cocaine (+1.5) and ecstasy (+1.6) use increased. In the urban area, consumption of all drugs increased during holidays (cannabis +1.6, cocaine +1.2, ecstasy +0.8 and methamphetamine +0.3). In the vacation area, methamphetamine (+0.7), ecstasy (+0.7) and cocaine (+1.1) use increased, but cannabis (-0.5) use decreased during holiday periods. Conclusions: While the peak holiday season in Australia is perceived as a period of increased drug use, this is not uniform across all drugs and areas. Substantial declines in drug use in the semi-rural area contrasted with substantial increases in urban and vacation areas. Per capita drug consumption in the vacation area was equivalent to that in the urban area, implying that these locations merit particular attention for drug use monitoring and harm minimisation measures.

Introduction and Aims. Wastewater analysis provides a non-intrusive way of measuring drug use within a population. We used this approach to determine daily use of conventional illicit drugs [cannabis, cocaine, methamphetamine and 3,4-methylenedioxymethamphetamine (MDMA)] and emerging illicit psychostimulants (benzylpiperazine, mephedrone and methylone) in two consecutive years (2010 and 2011) at an annual music festival. Design and Methods. Daily composite wastewater samples, representative of the festival, were collected from the on-site wastewater treatment plant and analysed for drug metabolites. Data over 2 years were compared using Wilcoxon matched-pair test. Data from 2010 festival were compared with data collected at the same time from a nearby urban community using equivalent methods. Results. Conventional illicit drugs were detected in all samples whereas emerging illicit psychostimulants were found only on specific days. The estimated per capita consumption of MDMA, cocaine and cannabis was similar between the two festival years. Statistically significant (P < 0.05; Z = −2.0–2.2) decreases were observed in use of methamphetamine and one emerging illicit psychostimulant (benzyl piperazine). Only consumption of MDMA was elevated at the festival compared with the nearby urban community. Discussion and Conclusions. Rates of substance use at this festival remained relatively consistent over two monitoring years. Compared with the urban community, drug use among festival goers was only elevated for MDMA, confirming its popularity in music settings. Our study demonstrated that wastewater analysis can objectively capture changes in substance use at a music setting without raising major ethical issues. It would potentially allow effective assessments of drug prevention strategies in such settings in the future.

This paper provides a comprehensive summary on modelling of micro-pollutants' (MPs) fate and transport in wastewater. It indicates the motivations of MP modelling and summarises and illustrates the current status. Finally, some recommendations are provided to improve and diffuse the use of such models. In brief, we conclude that, in order to predict the contaminant removal in centralised treatment works, considering the dramatic improvement in monitoring and detecting MPs in wastewater, more mechanistic approaches should be used to complement conventional, heuristic and other fate models. This is crucial, as regional risk assessments and model-based evaluations of pollution discharge from urban areas can potentially be used by decision makers to evaluate effluent quality regulation, and assess upgrading requirements, in the future.

Mit dem Abwasser gelangen pro Jahr rund 41 000 t Stickstoff (N) in die Schweizer Kläranlagen. Davon werden heute etwa 18 000 t in den ARA eliminiert. Mit Hilfe einer Kombination von neu entwickelten Reinigungsverfahren, die zum Teil bereits gut etabliert und auf dem Stand der Technik sind, liessen sich die Oberflächengewässer im Inland um weitere 6600 t Stickstoff entlasten, wie die vorliegende Studie zeigt. Bei Ausschöpfung des Reduktionspotenzials in den 160 grösseren ARA ist mit Gesamtinvestitionen von 344 Mio. Franken und jährlichen Betriebskosten von 27 Mio. Franken zu rechnen.

The assessment of potential impacts of wastewater effluent discharges in freshwater systems requires an understanding of the likely degrees of dilution and potential zones of influence. In this study, four tracers commonly present in wastewater effluents were monitored to compare their relative effectiveness in determining areas in freshwater systems that are likely to be impacted by effluent discharges. The four tracers selected were the human pharmaceutical carbamazepine, anthropogenic gadolinium, fluorescent-dissolved organic matter (fDOM), and electrical conductivity (EC). The four tracers were monitored longitudinally in two distinct freshwater systems receiving wastewater effluents, where one site had a high level of effluent dilution (effluent <1 % of total flow) and the other site had a low level of effluent dilution (effluent ∼50 % of total flow). At both sites, the selected tracers exhibited a similar pattern of response intensity downstream of discharge points relative to undiluted wastewater effluent, although a number of anomalies were noted between the tracers. Both EC and fDOM are non-specific to human influences, and both had a high background response, relative to the highly sensitive carbamazepine and anthropogenic gadolinium responses, although the ease of measuring EC and fDOM would make them more adaptable in highly variable systems. However, the greater sensitivity and selectivity of carbamazepine and gadolinium would make their combination with EC and fDOM as tracers of wastewater effluent discharges highly desirable to overcome potential limitations of individual tracers.

Drug concentrations in composite municipal wastewater samples and census-based estimates of population are used to derive daily loads of illicit substances that are indexed to population. However, such estimates do not provide information on the diurnal trends of substance excretion nor can they account for changes in population. To address these limitations, a series of 1 h composites created by sampling wastewater influent at 6 min intervals was collected over four consecutive days at a single wastewater treatment plant. Creatinine (a urinary indicator), caffeine, methamphetamine, benzoylecgonine (BZE), and cocaine were analyzed by liquid chromatography/tandem mass spectrometry (LC-MS/MS). Diurnal trends and between-day trends were substance specific and related to the number of estimated doses and excretory half-life. Normalization to creatinine yielded trends in substances that differed significantly from non-normalized trends by accounting for changes in population within the municipality studied. Increases in normalized substance excretion observed during early morning hours originate from individuals among the resident population of the municipality due to the absence of commuters.

Mit 17,8 Millionen Einwohnern ist Nordrhein-Westfalen das bevölkerungsreichste Bundesland in Deutschland. Durch die hohe Besiedlungsdichte, insbesondere in industriellen Ballungsgebieten wie dem Ruhrgebiet, ist der Druck auf die Gewässer durch die Wassernutzung und Abwas-sereinleitung verhältnismäßig groß. Bei Niedrigwasser führen viele Gewässer einen Abwasseranteil (gereinigtes Abwasser aus kommunalen Kläranlagen) von mehr als 10%.
Mit dem gereinigten kommunalen Abwasser werden Rückstände von Arzneimitteln, Bioziden und Haushaltschemikalien, sogenannte Mikroschadstoffe, in die Oberflächengewässer einge-tragen. Aufgrund der hohen Abwasserbelastung der nordrhein-westfälischen Fliessgewässer, ist auch die Problematik der Mikroschadstoffe für Nordrhein-Westfalen von besonderer Rele-vanz. In diesem Projekt wurde für Arzneimittel und weitere Mikroschadstoffe aus kommunalen Kläranlagen mit einem Stoffflussmodell eine flächendeckende Übersicht zur Belastungslage erstellt und der aktuelle Handlungsbedarf aufgezeigt. Es wurden dabei rund 650 Kläranlagen mit einer Größe >50 Einwohnerwerten (EW) berücksichtigt. Mit dem Stoffflussmodell wurden sowohl die Stoffflüsse als auch die Konzentrationen im Gewässer direkt unterhalb der Einleit-stellen der Kläranlagen berechnet. [...]

Aims: To discuss ethical issues that may arise in using WWA to monitor illicit drug use in the general population and in entertainment precincts, prisons, schools and work-places. Method: Review current applications of WWA and identify ethical and social issues that may be raised with current and projected future uses of this method. Results: Wastewater analysis (WWA) of drug residues is a promising method of monitoring illicit drug use that may overcome some limitations of other monitoring methods. When used for monitoring purposes in large populations, WWA does not raise major ethical concerns because individuals are not identified and the prospects of harming residents of catchment areas are remote. When WWA is used in smaller catchment areas (entertainment venues, prisons, schools or work-places) their results could, possibly, indirectly affect the occupants adversely. Researchers will need to take care in reporting their results to reduce media misreporting. Fears about possible use of WWA for mass individual surveillance by drug law enforcement officials are unlikely to be realized, but will need to be addressed because they may affect public support adversely for this type of research. Conclusions: Using wastewater analysis to monitor illicit drug use in large populations does not raise major ethical concerns, but researchers need to minimize possible adverse consequences in studying smaller populations, such as workers, prisoners and students.

Hospitals are considered as major sources of pharmaceutical residues discharged to municipal wastewater, but recent experimental studies showed that the contribution of hospitals to the loads of selected, quantifiable pharmaceuticals in sewage treatment plant (STP) influents was limited. However such conclusions are made based on the experimental analysis of pharmaceuticals in hospital wastewater which is hindered by a number of factors such as access to suitable sampling sites, difficulties in obtaining representative samples and availability of analytical methods. Therefore, this study explores a refined and extended consumption-based approach to predict the contribution of six selected Australian hospitals to the loads of 589 pharmaceuticals in municipal wastewater. In addition, the possibility that hospital-specific substances are present at levels that may pose a risk for human health was evaluated. For 63 to 84% of the pharmaceuticals investigated, the selected hospitals are not a major point source with individual contributions likely to be less than 15% which is in line with previous experimental studies. In contrast, between 10 and 20% of the pharmaceuticals consumed in the selected hospitals are exclusively used in these hospitals. For these hospital-specific substances, 57 distinct pharmaceuticals may cause concerns for human health as concentrations predicted in hospital effluents are less than 100-fold lower than effect thresholds. However, when concentrations were predicted in the influent of the corresponding STP, only 12 compounds (including the antineoplastic vincristine, the antibiotics tazobactam and piperacillin) remain in concentration close to effect thresholds, but further decrease is expected after removal in STP, dilution in the receiving stream and drinking water treatment. The results of this study suggest that risks of human exposure to the pharmaceuticals exclusively administered in the investigated hospitals are limited and decentralised wastewater treatment at these sites would not have a substantial impact on pharmaceutical loads entering STPs, and finally the environment. Overall, our approach demonstrates a unique opportunity to screen for pharmaceuticals used in hospitals and identifying priority pollutants in hospital wastewater explicitly accounting for site-specific conditions. Being based on consumption and loads discharged by hospitals into municipal wastewater, it is not limited by 1) the big effort to obtain representative samples from sewers, 2) the availability of sensitive chemical analysis or 3) a pre-selection of consumption data (e.g. consumption volume).

Two projects will be presented within this talk. First, a national wide model will be discussed for the prediction of mass flows of pharmaceuticals within the river system of Switzerland. Second, a mass flux study of organic micropollutants performed in rivers downstream of the Megacity Beijing will be presented.

To date it is unknown how pumps in sewer systems influence micropollutant loads at the scale of minutes to hours. This is important to design sampling campaigns: i) collecting representative composite samples, ii) experimentally determining peak loads or iii) dynamically evaluating wastewater treatment plant performance.
Hydrodynamic models which could simulate pollutographs become available for an increasing number of catchments. However, computationally it remains demanding to run simulations at high temporal resolution for a large number of conduits. Furthermore, also in complex models pumps are typically only modelled as one conceptual node, i.e. no spatial differentiation only volume. Furthermore, particularly for micropollutants, long measured input time series at sufficiently high temporal resolution are missing. In this paper we present a conceptual model to assess any combination of sub-catchments and lift stations. In gravity systems the number of wastewater packets containing the substance of interest generated at the source - i.e. toilets and other household appliances - determines the variability of the pollutograph. However, in the effluent of sub-catchments with pumps, the variability is independent of the number of generated wastewater packets but heavily depending on the properties and operation of the lift station.

Illicit drug use results in considerable social and economic costs to Australia (Collins & Lapsley 2008) but the magnitude of use is inherently difficult to measure. Besides being a clandestine behaviour, drug use in the community is not static and can peak at certain events (such as music festivals; Hesse, Tutenges & Schliewe 2010) or celebratory times of the year (such as New Year Eve; van Nuijs et al. 2011). Drug trends are triangulated across monitoring systems that employ different research methods and a mix of strengths with respect to, among other things, timeliness, reliability, drug-specificity and sample size (see Griffith & Mounteney 2010).

Regenwassereinleitungen und Mischwasserentlastungen tragen erheblich zu den Frachten im Gewässer bei. Die Situationsanalyse charakterisiert diese Emissionen für Mikroverunreinigungen aus dem häuslichen Abwasser und dem Regenabfluss. Die Modellergebnisse weisen substanzabhängig auf kritische Stellen in kleinen und mittelgrossen Gewässern in verdichteten Siedlungsräumen hin.

Certain rainfall mobilized micropollutants have been found in relevant concentrations in various water bodies across Switzerland. To distinguish contributions by sewage treatment plants and combined sewer overflows, extensive and expensive measurement campaigns would be necessary. Indicators could be used to optimize such campaigns if they are able to give a sound estimate of the local emission. In this framework a dynamic substance flow analysis was carried out. It is able to use information on land-use to calculate the loads discharged via combined sewer overflows (CSOs). The overall model results show, that combined sewer overflow emissions of urban areas are an important contribution to the pollutant load in surface waters. Especially for pollutants washed off from impervious areas, such as roofs or facades, loads were estimated to be in the same range as the loads discharged towards the sewage treatment plants. E.g. for Mecroprop, which originates primarily from buildings and gardens, it was found, that CSOs are a major contributor to urban emissions. Referring to the load entering the sewer more than 70% of the load from buildings and more than 60% of the load originating from gardens leave the sewer systems via CSOs. Furthermore, the results showed that size of the population indicates the emission of Triclosan and Copper while the impervious area is an indicator for the release of Mecoprop and Glyphosat.

Dieses Faktenblatt hat die Ziele (i) den heutigen Kenntnisstand zu diffusen Emissionen von Mikroverunreinigungen aus Siedlungen zusammenzufassen und (ii) die Relevanz der Niederschlagswassereinleitungen auf lokaler und nationaler Ebene zu beurteilen. Dazu wurde Literatur ausgewertet und eine System- und Stoffflussanalyse durchgeführt. Die Untersuchung fokussiert auf diffuse urbane Stoff- und Quellenkombinationen, die über Mischwasserentlastungen und Regenwassereinleitungen (zusammen nachstehend als „Niederschlagswassereinleitungen“ bezeichnet) in die aquatische Umwelt gelangen. [...]

Über die Transformation von Mikroverunreinigungen in Kanalisationssystemen ist bislang wenig bekannt. Aus diesem Grund will die vorliegende Bachelorarbeit aufzuzeigen, wie gross Abbauraten von solchen anthropogenen Stoffen sein müssten, damit am Ende eines Versuchskanals ein Abbau messbar ist. Dazu wurden mehrere Tracerexperimente ausgewertet. Die Tracerexperimente waren vorgängig von der EAWAG durchgeführt worden. Als Versuchskanal diente der fünf Kilometer lange Glattstollen, welcher das Abwasser durch den Zürichberg zur Abwasserreinigungsanlage Werdhölzli transportiert. Der Abwasserkanal ist für die Experimente ideal, da keine seitlichen Zuflüsse vorhanden sind.
Für die Auswertung der Tracerexperimente wurde das Computerprogramm Aquasim 2.1 verwendet. Der Abwasserkanal wurde sowohl als Advective-Diffusive Reactor Compartment (Modell 1) als auch als River-Section Compartment (Modell 2) modelliert. Anschliessend wurden die Modelle mittels Daten aus den Tracerexperimenten kalibriert. Als Grundlage dazu diente das Massenerhaltungsgesetz. Für die hydraulische Kalibrierung wurde bei beiden Modellen die Dispersion geschätzt. Zusätzlich wurde beim Modell 1 die Geschwindigkeit und beim Modell 2 der hydraulischen Widerstandsbeiwert nach Strickler ermittelt. Anschliessend wurde ein linearer Abbauprozess hinzugefügt. Durch das Variieren verschiedener Abbauraten konnte die verbleibende Konzentration fünf Kilometer nach Zudosierung berechnet und verglichen werden.
Das Modell 1 und 2 unterscheiden sich prinzipiell in der Wahl des Kompartiments. Gewisse Variablen müssen dadurch unterschiedlich definiert werden. Die Resultate zum Abbau indizieren, dass das Modell 2 genauere Ergebnisse liefert. Beide Modelle zeigen bei der Parameterschätzung ähnliche Resultate. Dies zeigt, dass auch die Modellierung des Kanals als Advektive-Diffusive Reactor Compartment (Modell 1) für eine solide Abschätzung der Parameter sowie zur Quantifizierung des Abbaus verwendet werden kann. Modell 1 ist insbesondere vorzuziehen, falls Angaben zum Durchmesser oder Gefälle fehlen.
Die Auswertung der Tracerversuche ergab, dass sich der Dispersionskoeffizient zwischen 0.11 – 0.29 m²/s befindet. Nach Rieckermann et al. (2005) ist in Abwasserkanälen ein mittlerer Dispersionskoeffizient von 0.16 m²/s üblich. Die ermittelten Werte sind somit durchaus realistisch.
Für die Quantifizierung des Abbaus wurden Abbauraten zwischen 0.1/d und 24/d betrachtet. Die Berechnungen ergaben, dass bei einer Abbaurate von 24/d am Ende des Versuchskanals etwa 90 % der Zudosiermenge abgebaut werden. Allerdings sind die Abbauraten von Mikroverunreinigungen viel geringer. Eine Abbaurate von 0.1/d oder noch kleiner ist realistischer (Joss et al., 2006). Dabei würden ungefähr 1.2 % abgebaut werden. Dies entspricht keinem erheblichen Abbau und könnte, je nach Substanz und Genauigkeit des Messinstruments, knapp oder gar nicht registriert werden.
Bei der Transformation von Mikroverunreinigungen in Abwasserkanälen spielt, neben dem Abbau, auch die Sorption eine Rolle. Durch die Erweiterung der Modelle mit einem Biofilm - Reaktor sowie einem Prozess, der die Sorption beschreibt, könnte das Verhalten der Mikroverunreinigungen in Kanalisationssytemen noch detaillierter betrachtet werden.

The analysis of sewage for urinary biomarkers of illicit drugs is a promising and complementary approach for estimating the use of these substances in the general population. For the first time, this approach was simultaneously applied in 19 European cities, making it possible to directly compare illicit drug loads in Europe over a 1-week period. An inter-laboratory comparison study was performed to evaluate the analytical performance of the participating laboratories. Raw 24-hour composite sewage samples were collected from 19 European cities during a single week in March 2011 and analyzed for the urinary biomarkers of cocaine, amphetamine, ecstasy, methamphetamine and cannabis using in-house optimized and validated analytical methods. The load of each substance used in each city was back-calculated from the measured concentrations. The data show distinct temporal and spatial patterns in drug use across Europe. Cocaine use was higher in Western and Central Europe and lower in Northern and Eastern Europe. The extrapolated total daily use of cocaine in Europe during the study period was equivalent to 356. kg/day. High per capita ecstasy loads were observed in Dutch cities, as well as in Antwerp and London. In general, cocaine and ecstasy loads were significantly elevated during the weekend compared to weekdays. Per-capita loads of methamphetamine were highest in Helsinki and Turku, Oslo and Budweis, while the per capita loads of cannabis were similar throughout Europe. This study shows that a standardized analysis for illicit drug urinary biomarkers in sewage can be applied to estimate and compare the use of these substances at local and international scales. This approach has the potential to deliver important information on drug markets (supply indicator).

Probabilistic material flow analysis and graph theory were combined to calculate predicted environmental concentrations (PECs) of engineered nanomaterials (ENMs) in Swiss rivers: 543 river sections were used to assess the geographical variability of nano-TiO₂, nano-ZnO and nano-Ag, and flow measurements over a 20-year period at 21 locations served to evaluate temporal variation. A conservative scenario assuming no ENM removal and an optimistic scenario covering complete ENM transformation/deposition were considered. ENM concentrations varied by a factor 5 due to uncertain ENM emissions (15%–85% quantiles of ENM emissions) and up to a factor of 10 due to temporal river flow variations (15%–85% quantiles of flow). The results indicate highly variable local PECs and a location- and time-dependent risk evaluation. Nano-TiO₂ median PECs ranged from 11 to 1′623 ng L⁻¹ (conservative scenario) and from 2 to 1′618 ng L⁻¹ (optimistic scenario). The equivalent values for nano-ZnO and nano-Ag were by factors of 14 and 240 smaller.

Wastewater analysis is a promising monitoring tool to estimate illicit drug consumption at the community level. The advantage of this technique over traditional surveys and other surveillance methods has been emphasized in recent studies. However, there are methodological challenges that can affect reliability. The objectives of this study were to systematically reduce and assess uncertainties associated with sampling (through a stringent optimization of the sampling method) and the back calculation of per capita drug consumption (through a refined estimation of the number of people actively contributing to the wastewater in a given period). We applied continuous flow-proportional sampling to ensure the collection of representative raw wastewater samples. Residues of illicit drugs, opioids, prescription pharmaceuticals and one artificial sweetener were analyzed by liquid chromatography coupled with tandem mass spectrometry. A parameter estimating the number of people actively contributing to wastewater over a given period was calculated from the measured loads of prescription pharmaceuticals, their annual consumption and relative excretion data. For the calculation of substance loads in sewage, uncertainties were propagated considering five individual components: sampling, chemical analysis, flow measurements, excretion rates and the number of people contributing to the wastewater. The daily consumption per 1000 inhabitants was estimated to be almost 1000 mg for cannabis and several hundred mg for cocaine, methamphetamine and ecstasy. With the best sampling practice and current chemical analysis, we calculated the remaining uncertainty to be in the range of 20–30% (relative standard deviation, RSD) for the estimation of consumed drug masses in the catchment; RSDs for the per capita consumption were lower (14–24%), as one of the biggest uncertainty components (i.e. error in flow measurements) cancels out in the proposed method for the estimation of the number of people contributing to the daily wastewater volume. In this study, we provide methodological improvements that substantially enhance the reliability of the estimation method – a prerequisite for the application of this technique to meaningfully assess changes in drug consumption and the success of drug intervention strategies in future studies.

Wastewater production, like many other engineered and environmental processes, is inherent stochastic in nature and requires the use of complex stochastic models, for example, to predict realistic patterns of down-the-drain chemicals or pharmaceuticals and personal care products. Up until now, a formal method of statistical inference has been lacking for many of those models, where explicit likelihood functions were intractable. In this Article, we investigate Approximate Bayesian Computation (ABC) methods to infer important parameters of stochastic environmental models. ABC methods have been recently suggested to perform model-based inference in a Bayesian setting when model likelihoods are analytically or computationally intractable and have not been applied to environmental systems analysis or water quality modeling before. In a case study, we investigate the performance of three different algorithms to infer the number of wastewater pulses contained in three high-resolution data series of benzotriazole and total nitrogen loads in sewers. We find that all algorithms perform well and that the uncertainty in the inferred number of corresponding wastewater pulses varies between 6% and 28%. In our case, the results are more sensitive to substance characteristics than to catchment properties. Although the application of ABC methods requires careful tuning and attention to detail, they have a great general potential to update stochastic model parameters with monitoring data and improve their predictive capabilities.

The kinetics of oxidation and disinfection processes during ozonation in a full-scale reactor treating secondary wastewater effluent were investigated for seven ozone doses ranging from 0.21 to 1.24 g O₃ g⁻¹ dissolved organic carbon (DOC). Substances reacting fast with ozone, such as diclofenac or carbamazepine (k_P,O3 > 10⁴ M⁻¹), were eliminated within the gas bubble column, except for the lowest ozone dose of 0.21 g O₃ g⁻¹ DOC. For this low dose, this could be attributed to short-circuiting within the reactor. Substances with lower ozone reactivity (k_P,O3 < 10⁴ M⁻¹ s⁻¹) were only fully eliminated for higher ozone doses.
The predictions of micropollutant oxidation based on coupling reactor hydraulics with ozone chemistry and reaction kinetics were up to a factor of 2.5 higher than full-scale measurements. Monte Carlo simulations showed that the observed differences were higher than model uncertainties. The overestimation of micropollutant oxidation was attributed to a protection of micropollutants from ozone attack by the interaction with aquatic colloids. Laboratory-scale batch experiments using wastewater from the same full-scale treatment plant could predict the oxidation of slowly-reacting micropollutants on the full-scale level within a factor of 1.5. The Rct value, the experimentally determined ratio of the concentrations of hydroxyl radicals and ozone, was identified as a major contribution to this difference.
An increase in the formation of bromate, a potential human carcinogen, was observed with increasing ozone doses. The final concentration for the highest ozone dose of 1.24 g O₃ g⁻¹ DOC was 7.5 μg L⁻¹, which is below the drinking water standard of 10 μg L⁻¹. N-Nitrosodimethylamine (NDMA) formation of up to 15 ng L⁻¹ was observed in the first compartment of the reactor, followed by a slight elimination during sand filtration. Assimilable organic carbon (AOC) increased up to 740 μg AOC L⁻¹, with no clear trend when correlated to the ozone dose, and decreased by up to 50% during post-sand filtration. The disinfection capacity of the ozone reactor was assessed to be 1–4.5 log units in terms of total cell counts (TCC) and 0.5 to 2.5 log units for Escherichia coli (E. coli). Regrowth of up to 2.5 log units during sand filtration was observed for TCC while no regrowth occurred for E. coli. E. coli inactivation could not be accurately predicted by the model approach, most likely due to shielding of E. coli by flocs.

Within the framework of the “Micropoll Strategy” project of the Swiss Federal Environmental Agency, the suitability of ozonation as an additional treatment stage for the removal of organic trace elements was tested at the Regensdorf wastewater treatment plant. With ozone doses of 0.60 g O₃/g DOC already, a large portion of the organic trace elements could no longer be detected in the plant run-off. Only for a few, very persistent compounds (like iodized radio-opaque substances or atrazine), the removal rates amounted to only about 50 percent, even with high ozone doses (1.16 g O₃ /g DOC). Eco-toxicological methods were used to prove that a clear reduction in summary effects (like e.g. oestrogen effects or the effect of insecticides) took place. In two tests, negative effects were measured directly after ozonation, but they disappeared again after the final sand filter. Oxidation by-products (such as assimilable organic carbon or N-Nitrosodimethylamine [NDMA]) were also reduced through sand filtration. This underlines the importance of a biologically active stage downstream of the ozonation stage, for example a sand filtration stage. The pilot operation also showed that an ozonation stage at a municipal wastewater treatment plant is technically feasible and economically reasonable.

The analysis of 87 peer-reviewed journal articles reveals that sampling for pharmaceuticals and personal care products (PPCPs) and illicit drugs in sewers and sewage treatment plant influents is mostly carried out according to existing tradition or standard laboratory protocols. Less than 5% of all studies explicitly consider internationally acknowledged guidelines or methods for the experimental design of monitoring campaigns. In the absence of a proper analysis of the system under investigation, the importance of short-term pollutant variations was typically not addressed. Therefore, due to relatively long sampling intervals, potentially inadequate sampling modes, or insufficient documentation, it remains unclear for the majority of reviewed studies whether observed variations can be attributed to “real” variations or if they simply reflect sampling artifacts. Based on results from previous and current work, the present paper demonstrates that sampling errors can lead to overinterpretation of measured data and ultimately, wrong conclusions. Depending on catchment size, sewer type, sampling setup, substance of interest, and accuracy of analytical method, avoidable sampling artifacts can range from “not significant” to “100% or more” for different compounds even within the same study. However, in most situations sampling errors can be reduced greatly, and sampling biases can be eliminated completely, by choosing an appropriate sampling mode and frequency. This is crucial, because proper sampling will help to maximize the value of measured data for the experimental assessment of the fate of PPCPs as well as for the formulation and validation of mathematical models. The trend from reporting presence or absence of a compound in “clean” water samples toward the quantification of PPCPs in raw wastewater requires not only sophisticated analytical methods but also adapted sampling methods. With increasing accuracy of chemical analyses, inappropriate sampling increasingly represents the major source of inaccuracy. A condensed step-by-step Sampling Guide is proposed as a starting point for future studies.

Ozonation as an advanced treatment for micropollutant removal was tested full-scale on the wastewater treatment plant (WWTP) Regensdorf during 16 months. This experiment has been conducted within the project „Strategy Micropoll“ of the Swiss Federal Office for the Environment (FOEN). Ozonation eliminated a broad range of organic micropollutants and various ecotoxicological effects. The pilot study also showed that the implementation of an ozonation step in an existing WWTP is feasible, both technically and economically. [...]

Auf der Abwasserreinigungsanlage (ARA) Regensdorf wurde im Rahmen des Projekts „Strategie Micropoll“ des Bundesamts für Umwelt (BAFU) während 16 Monaten die Eignung der Ozonung als zusätzliche Reinigungsstufe für die Entfernung von Mikroverunreinigungen getestet. Dabei konnte ein breites Spektrum problematischer organischer Spurenstoffe entfernt werden. Gleichzeitig wurden verschiedene unerwünschte ökotoxikologische Wirkungen eliminiert. Der Versuchsbetrieb zeigte, dass eine Ozonungsstufe auf einer kommunalen ARA technisch machbar und wirtschaftlich vertretbar ist. [...]

Der Eintrag von organischen Spurenstoffen aus der Siedlungsentwässerung ist aktuell eine besondere Herausforderung für den Gewässerschutz. Im Rahmen des Projekts "Strategie Micro-Poll" des Schweizer Bundesamts für Umwelt werden weitergehende Maßnahmen auf Kläranlagen zur Reduktion des Eintrags problematischer Stoffe diskutiert. Dabei stehen zurzeit die Ozonung und die Behandlung mit Pulveraktivkohle im Vordergrund. In einer Teilstudie des Projekts wurden für sechs ausgewählte Kläranlagen unterschiedlicher Größe die Kosten für Bau und Betrieb dieser zwei Verfahren berechnet sowie die Kosten für Kläranlagen anderer Größen interpoliert. Die Mehrkosten gegenüber der herkömmlichen Reinigung belaufen sich, je nach Anlagengröße, auf 5 bis 25 Prozent. Anschließend wurden die Gesamtkosten für die Schweiz für verschiedene Szenarien bestimmt. Die Gesamtkosten für den Ausbau der größten Anlagen sowie der Ausbau aller Anlagen, bei denen das Qualitätsziel für Diclofenac im Gewässer überschritten ist, würden für die Schweiz auf 115 bis 180 Millionen Schweizer Franken pro Jahr oder 15 bis 24 Schweizer Franken pro Einwohner jährlich geschätzt. Die Mehrkosten werden somit als vertretbar angesehen. Für eine konkrete Umsetzung müssen im Einzelfall jedoch sorgfältige Kosten-Nutzen-Betrachtungen vorgenommen werden.

Tertiary treatment of wastewater with ozone is a promising technique for removing residual micropollutants that remain after secondary biological treatment. We monitored the performance of a full-scale ozonation reactor on a sewage treatment plant in Switzerland with a screening battery of bioassays. Six toxicity endpoints were selected that covered non-specific toxicity, as well as selected receptor-mediated modes of action and reactive toxicity. Non-specific toxicity was assessed with two bioassays, the bioluminescence inhibition of the marine luminescent bacterium Vibrio Fischeri and the growth inhibition of the green algae Pseudokirchneriella subcapitata. Treatment efficiency was around 90% for the secondary treatment, but only 65% and 76% for the ozonation step in the two non-specific endpoints, respectively. This finding is consistent with this type of oxidation reaction because ozone only modifies the organic molecules but does not mineralize them fully leaving residual toxicity of the transformation products. In contrast, the specific receptor-mediated endpoints of inhibition of photosystem II in algae and estrogenicity were largely reduced by ozonation. While compounds inhibiting photosynthesis proved to be rather recalcitrant toward biological treatment with only 47% removal, an additional 86% removal by ozonation yielded an overall treatment efficiency in the entire treatment chain of 89%. The effect on estrogenicity, quantified with the yeast estrogen screen, was even more significant: A treatment efficiency of 95% in the secondary treatment, 86% during ozonation plus a small effect by biological sand filtration yielded an overall treatment efficiency of 99.5%. Insecticides that inhibit acetylcholinesterase were fairly resistant to degradation, but an overall treatment efficiency of 91% was achieved in two steps: 72% in biological treatment and 60% during ozonation. Finally, no significant genotoxicity was observed with the umuC test after ozonation, while the influent showed a genotoxic response when it was enriched by a factor of 15 to 60. Treatment efficiency increased with the ozone dose and remained virtually unchanged over ozone doses above 500 g ozone per kg dissolved organic carbon. The reduction of toxicity can be rationalized by the chemical oxidation processes likely to occur for each group of chemicals that are typical for a given mode of toxic action. For comparison, tertiary treatment with powdered activated carbon was also evaluated, which poses a viable alternative to ozonation with respect to removal of micropollutants.

Over the past few years a situation analysis on micropollutants in watercourses has been carried out on the initiative of the FOEN through various research projects. This report summarises the results of these studies.
The research groups obtained more detailed knowledge of the pollution situation, enabling them to make reliable model predictions and indicate possible options for action, their anticipated effects and the resultant costs –
with particular focus on the technical optimization of municipal waste water treatment. It became evident that significant reductions in micropollutant levels can only be made by combining a number of measures on multiple levels.

The removal efficiency for 220 micropollutants was studied at the scale of a municipal wastewater treatment plant (WWTP) upgraded with post-ozonation followed by sand filtration. During post-ozonation, compounds with activated aromatic moieties, amine functions, or double bonds such as sulfamethoxazole, diclofenac, or carbamazepine with second-order rate constants for the reaction with ozone >10⁴ M⁻¹ s⁻¹ at pH 7 (fast-reacting) were eliminated to concentrations below the detection limit for an ozone dose of 0.47 g O₃ g⁻¹ dissolved organic carbon (DOC). Compounds more resistant to oxidation by ozone such as atenolol and benzotriazole were increasingly eliminated with increasing ozone doses, resulting in >85% removal for a medium ozone dose (0.6 g O₃ g⁻¹ DOC). Only a few micropollutants such as some X-ray contrast media and triazine herbicides with second-order rate constants <10² M⁻¹ s⁻¹ (slowly reacting) persisted to a large extent. With a medium ozone dose, only 11 micropollutants of 55 detected in the secondary effluent were found at >100 ng L⁻¹. The combination of reaction kinetics and reactor hydraulics, based on laboratory- and full-scale data, enabled a quantification of the results by model calculations. This conceptual approach allows a direct upscaling from laboratory- to full-scale systems and can be applied to other similar systems. The carcinogenic by-products N-nitrosodimethylamine (NDMA) (≤14 ng L⁻¹) and bromate (<10 μg L⁻¹) were produced during ozonation, however their concentrations were below or in the range of the drinking water standards. Furthermore, it could be demonstrated that biological sand filtration is an efficient additional barrier for the elimination of biodegradable compounds formed during ozonation such as NDMA. The energy requirement for the additional post-ozonation step is about 0.035 kWh m⁻³, which corresponds to 12% of a typical medium-sized nutrient removal plant (5 g DOC m⁻³).

The presence of nitrosamines in wastewater might pose a risk to water resources even in countries where chlorination or chloramination are hardly used for water disinfection. We studied the variation of concentrations and removal efficiencies of eight N-nitrosamines among 21 full-scale sewage treatment plants (STPs) in Switzerland and temporal variations at one of these plants. N-nitrosodimethylamine (NDMA) was the predominant compound in STP primary effluents with median concentrations in the range of 5–20 ng/L, but peak concentrations up to 1 μg/L. N-nitrosomorpholine (NMOR) was abundant in all plants at concentrations of 5–30 ng/L, other nitrosamines occurred at a lower number of plants at similar levels. From concentrations in urine samples and domestic wastewater we estimated that human excretion accounted for levels of <5 ng/L of NDMA and <1 ng/L of the other nitrosamines in municipal wastewater, additional domestic sources for <5 ng/L of NMOR. Levels above this domestic background are probably caused by industrial or commercial discharges, which results in highly variable concentrations in sewage. Aqueous removal efficiencies in activated sludge treatment were in general above 40% for NMOR and above 60% for the other nitrosamines, but could be lower if concentrations were below 8–15 ng/L in primary effluent. We hypothesize that substrate competition in the cometabolic degradation explains the occurrence of such threshold concentrations. An additional sand filtration step resulted in a further removal of nitrosamines from secondary effluents even at low concentrations. Concentrations released to surface waters were largely below 10 ng/L, suggesting a low impact on Swiss water resources and drinking water generation considering the generally high environmental dilution and possible degradation. However, local impacts in case a larger fraction of wastewater is present cannot be ruled out.

Installation and maintenance of flow gauging stations to assess wastewater dilution in small creeks is expensive. The method outlined in this paper provides a flexible and cheap alternative for situations with dilution factors smaller than 10 and unambiguous flow direction. It is shown that conductivity profiles from three sampling locations enable accurate identification of the dilution factor with an uncertainty of ±10–30%. Furthermore, much insight can be gained on the temporal behavior of both, the receiving water and the wastewater treatment system by combined analysis of conductivity and temperature data. In this case study the data also enabled identification and tracking down of illegal polluters.

A model based on graph theory was developed to efficiently evaluate the impact of the effluent from 742 wastewater treatment plants (WWTPs) on micropollutant loading throughout all river catchments in Switzerland. Model results agree well with measured loads for 12 compounds in river water samples, revealing mean predictive accuracy factors between 0.8 and 3.4. Subsequently, pollutant concentrations were predicted for river sections downstream from 543 WWTPs where hydrological information was available, and compared with recent recommendations for water quality criteria. At base flow conditions, carbamazepine concentrations (parent compound only) are ubiquitously below a water quality criterion of 0.5 μg L⁻¹. In contrast, the sum of diclofenac and its metabolites is expected to exceed the corresponding water quality criterion of 0.1 μg L⁻¹ in 224 river sections. If diclofenac cannot be eliminated at the source, the model suggests a directed upgrade of 173 WWTPs to meet the condition that concentrations are never to exceed this water quality criterion.

Little is known about the significance of hospitals as point sources for emission of organic micropollutants into the aquatic environment. A mass flow analysis of pharmaceuticals and diagnostics used in hospitals was performed on the site of a representative Swiss cantonal hospital. Specifically, we analyzed the consumption of iodinated X-ray contrast media (ICM) and cytostatics in their corresponding medical applications of radiology and oncology, respectively, and their discharge into hospital wastewater and eventually into the wastewater of the municipal wastewater treatment plant. Emission levels within one day and over several days were found to correlate with the pharmacokinetic excretion pattern and the consumed amounts in the hospital during these days. ICM total emissions vary substantially from day to day from 255 to 1259 g/d, with a maximum on the day when the highest radiology treatment occurred. Parent cytostatic compounds reach maximal emissions of 8−10 mg/d. A total of 1.1%, 1.4%, and 3.7% of the excreted amounts of the cytostatics 5-fluorouracil, gemcitabine, and 2′,2′-difluorodeoxyuridine (main metabolite of gemcitabine), respectively, were found in the hospital wastewater, whereas 49% of the total ICM was detected, showing a high variability among the compounds. These recoveries can essentially be explained by the high amount administered to out-patients (70% for cytostatics and 50% for ICM); therefore, only part of this dose is expected to be excreted on-site. In addition, this study emphasizes critical issues to consider when sampling in hospital sewer systems. Flow proportional sampling over a longer period is crucial to compute robust hospital mass flows.

Fluorochemicals are persistent contaminants that are globally distributed in air, water, sediments, and biota. Wastewater treatment plants (WWTPs) play an important role in mitigating pollutant releases from municipalities to aquatic and terrestrial environments. However, because WWTPs are point sources of fluorochemicals, it is important to understand their contribution to fluorochemical burdens in the greater context of watersheds. To this end, over a 1 week period, the mass flows of 11 fluorochemicals from seven WWTPs that discharge effluent into the Glatt River in Switzerland were measured and compared to the measured mass flows within the Glatt River. Overall, the fluorochemicals were not removed efficiently during wastewater treatment. Effluents from WWTPs and Glatt River water were dominated by perfluorooctane sulfonate, which was detected in all samples, followed by perfluorohexane sulfonate and perfluorooctanoate. The mass flows of fluorochemicals emanating from WWTPs were found to be conserved within the 35 km Glatt River, which indicates that input from the WWTPs is additive and that removal within the Glatt River is not significant. Per capita discharges of fluorochemicals were calculated from the populations served by the WWTPs studied; the values determined also account for the fluorochemical content of Lake Greifen (Greifensee), which is a lake at the headwaters of the Glatt River that also receives treated wastewater.

Down-the-drain household chemicals are mostly discharged intermittently (i.e. with water pulses, e.g. pharmaceuticals from toilet flushing) and well soluble micropollutants can, therefore, be subject to significantly high short-term fluctuations. It is not known how these fluctuations are attenuated by sorption to sewer sediments or biofilm. First, we investigated in this paper the effect of sorption for substances with high, medium and low affinity to particulate matter based on computational experiments. For substances with high K_oc we found that the additional attenuation of a load pattern due to sorption is in the same order of magnitude as caused by dispersion in a typical main sewer. The mass flux between wastewater and the first biofilm layer was identified as the most sensitive parameter. Furthermore, the interplay of systematic, slow diurnal variations does not affect short-term fluctuations. Second, during rain events partial erosion of the biofilm can lead to increased micropollutant loads for substances with high K_oc. This increase is in the same order of magnitude as diurnal variations of the loads in the liquid phase and the TSS.

In recent years, human and veterinary pharmaceuticals have received much attention as pollutants of water bodies or drinking water resources due to possible negative effects on humans or the ecosystem even at very low concentrations. Over the last 10 years, considerable progress has been made regarding the knowledge of the exposure of water bodies to those drugs. This review summarizes the present understanding in this broad and interdisciplinary field incorporating contributions ranging from trace analytics to spatially distributed modelling of point-source and diffuse pollution. It discusses the main factors and processes controlling the environmental fate of pharmaceuticals from their usage to their spatial and temporal occurrence in water bodies. The current research is still rather phenomenological and further advancement of the field requires more integrated, quantitative mass flux analyses. Such analyses should also consider the explicit incorporation of uncertainties that appropriately reflect the current limited understanding and data availability.

Sampling and analytical chemistry are costly, and therefore, measurements can only provide limited information in space and time on the occurrence of micropollutants in surface waters. What would the picture look like, if one measured in rivers downstream of all wastewater treatment plants? To make a prediction of pollutant loads from urban drainage a national mass flux model has been developed. For more than 100 wastewater treatment plants, the dilution factor of treated wastewater during dry weather conditions is smaller than 10. For specific substances, this can lead to the exceedance of critical concentrations in rivers. Furthermore, the model allows the calculation of different scenarios. Whole river catchments are taken inter consideration.

Most commercially available auto-sampling devices do not support a continuous flow-proportional sampling mode, which would conceptually be the best for collecting representative composite samples. Instead different discrete sampling modes are available. Household chemicals can show considerable random short-term variations. With the anticorrosive benzotriazole, relating to a middle-frequent household activity, we show that, besides an accurate flow meter, mainly three factors are decisive for the representativeness of a substance's average load: the substance's load pattern, the sampling frequency and the length of the composite sample. When the sampling intervals are 10 minutes or longer, errors in the order of ±40% (standard deviation) or more have to be accepted, if the substance of interest is contained in a low number of wastewater pulses (i.e. the level of household activity). This particularly holds true for specific pharmaceuticals e.g. carbamazepine. Ammonium would be less critical, because it relates to a larger number of sources in the same catchment.

Introduction
A large number of substances, contained in pharmaceuticals, personal care products and other household chemicals, are comfortably disposed of in sanitary appliances. Collected in the sewer system and partly eliminated in wastewater treatment plants they are then released to a certain extent into the aquatic environment. Many of these compounds belong to the category of micropollutants, which can have adverse effects on living organisms already in very low concentrations. Since no clear causal relationship between observed changes of ecosystems and the presence of micropollutants could be established, scientists combine monitoring with laboratory data. While experiments in the laboratory can be performed under controlled conditions it is very difficult to assess the complex situation in the environment. It is not only a hand full of micropollutants, but rather hundreds. To measure environmental concentrations of all these compounds over a relevant period of time is impossible. Therefore, predictive models are needed to forecast environmental concentrations. The input to these kinds of models, are emission data. Their acquisition is a tedious task. [...]

Einleitung
Medikamente, Körperpflegemittel und viele andere Haushaltprodukte enthalten eine grosse Anzahl chemischer Substanzen. Diese werden nach ihrer Anwendung bequem in sanitären Einrichtungen wie Toilette, Bad, Geschirrspül- oder Waschmaschine entsorgt. Mit dem Abwasser werden sie in der Kanalisation gesammelt und in die Kläranlagen transportiert. Einige werden gut eliminiert, andere hingegen können nur teilweise oder gar nicht abgebaut werden und gelangen so in die natürlichen Gewässer. Viele dieser chemischen Verbindungen gehören zu Kategorie der so genannten „Mikroverunreinigungen“, welche bereits in tiefsten Konzentrationen negative Auswirkung auf aquatische Lebewesen haben können. Bis heute konnten keine eindeutigen Zusammenhänge zwischen dem Auftreten von Mikroverun-reinigungen und beobachteten Veränderungen aquatischer Populationen aufgezeigt werden. Deshalb kombinieren Wissenschaftler Laborergebnisse mit Umweltdaten. Während Labor-experimente unter weitest gehend kontrollierten Bedingungen durchgeführt werden können, ist es äusserst schwierig, die komplexe Situation in der Umwelt zu erfassen. Es handelt sich bei den Mikroverunreinigungen nicht nur um eine Hand voll, sondern eher um hunderte von kritischen Substanzen. Das Messen von Umweltkonzentrationen all dieser Stoffe über eine genügend lange Periode ist unmöglich. Darum braucht es Modelle, um diese Umwelt konzentrationen abschätzen zu können. Die Eingangsgrössen zu solchen Modellen sind Emissionsdaten. Diese zu erheben ist eine mühsame Aufgabe. [...]

In urbanized areas large quantities of synthetic organic compounds are being used which can inevitably enter both municipai waste water end receiving water bodies. Many of these substances can be detected in aqueous systems at very low concentrations (nano- to microgram per litre). These so-called rnicropollutants are seen as a further challenge tor the field of water protection. The new project «Strategy MicroPoll» of the Swiss Federal Office tor the Environment (FOEN) is gathering evidence to determine a basis for policy decision-making with regard to micropollutants in municipal waste water.

The legal criteria for the design of CSO structures can be set at different levels of sophistication. Applying emission based criteria the performances of three design alternatives are compared by using different strategies to account for variability and parameter uncertainty. The importance of separating these two effects is highlighted and the decision processes are explored. Additionally, the consequences of different kind of criteria are discussed with respect to the stakeholders involved.

Les critères légaux pour le dimensionnement de bassins de rétention peuvent être placés à différents niveaux de sophistication. En appliquant un critère d'émission, trois alternatives de dimensionnement sont comparées en employant différentes stratégies de prise en compte de la variabilité et de l'incertitude de paramètre. L'importance de séparer ces deux effets est accentuée et les procédés de décision sont explorés. En outre, les conséquences de différents critères sont examinées en ce qui concerne les stakeholders.

In wastewater treatment and environmental risk assessments increasing attention is paid to the fate of micropollutants. These are time-consuming, expensive and difficult to detect and quantify. If a substance's load or concentration is subject to high dynamic fluctuations, it is demanding to take representative samples, especially when the "variation" is unknown. Therefore, we developed a concept to model stochastic load variations in sewer systems. We gathered readily available information from existing databases (population and consumption data) and combined it with the characteristics of household activities and appliances. We succeeded in predicting realistic short-term variations of benzotriazole (contained in dishwasher detergents) and validated them with a high-frequency measuring campaign. Benzotriazole stands as an example for other household chemicals, which cannot be measured so easily. All required information used within this case study is also available for other substances and catchments. This allows the forecast of stochastic load variations for many chemical compounds of interest. It helps to plan measuring campaigns, to estimate discharged loads from combined sewer overflows and to have a characteristic input for modeling purposes.

In this paper, 60 tracer experiments in 37 different sewer reaches have been analyzed for longitudinal dispersion under dry weather flow conditions. It was found that dispersion coefficients of sewers are two to three orders of magnitude smaller than those measured in rivers and do not differ much from system to system. Suitable equations were identified to predict reasonable dispersion coefficients in sewer reaches with uniform geometry and stable flow conditions, For engineering applications that require a high degree of accuracy the performance of tracer measurements is recommended.

In der vorliegenden Diplomarbeit geht es darum, die Schwankungen der Urinfracht in der Kanalisation zu untersuchen. Dazu wurde mittels eines mathematischen Modells ein Bezug zwischen der menschlichen Aktivität „urinieren“ und der Urinfracht in der Kanalisation hergestellt. Es geht dabei nicht darum den Tagesgang zu modellieren, sondern vielmehr aufzuzeigen, dass die Urinfracht in der Kanalisation starken kurzfristigen Schwankungen unterliegt und dass diese mit relativ geringem Aufwand vorhergesagt werden können. Mit einer Messkampagne soll überprüft werden, ob die modellierte Ganglinie mit der Realität übereinstimmt. Als Einzugsgebiet wurde das Dorf Wangen ZH gewählt. Beim gewählten Punkt in der Kanalisation sind 1063 Einwohner angeschlossen und die Fliessdistanz beträgt zwischen 52 und 965 Meter. Zur Modellierung der Urinfracht wurde ein bewusst einfach gehaltenes Advektions-Dispersions-Modell verwendet. Urin wird dabei durch den Parameter Stickstoff modelliert und gemessen. Dies ist möglich, da über 80% des in der Kanalisation vorhandenen Stickstoffs aus dem Urin stammt. Jeder Person wurde zufällig ein Zeitpunkt für den Toilettengang, eine Fliessdistanz, eine Urin-Stickstoff-Menge und eine Zeitdauer für den Urinpuls zugeteilt. Die Werte für diese Eigenschaften wurden aus der Literatur, einfachen Messungen und anderen Daten bestimmt. Die Urinpulse wurde dann um die Fliesszeit verschoben, einer Dispersion unterworfen und beim gewählten Punkt in der Kanalisation aufsummiert. Mit einer Monte Carlo Simulation wurden 200 Frachten-Ganglinien modelliert.
An einem Wochentag wurden zwischen 8:10 und 9:20 Uhr die Stickstoffkonzentration und der Durchfluss, im Abstand von 45 Sekunden, gemessen. Daraus wurde die Zeitreihe für die Urinfracht berechnet. Um die Messunsicherheiten zu berücksichtigen wurde ein mathematisches Modell erstellt, das jedem Wert der Zeitreihe zufällig eine Messabweichung zuteilt. Mit einer Monte Carlo Simulation wurden wiederum 200 Frachten-Ganglinien modelliert.
Anhand eines optischen Vergleiches und mit statistischen Kennwerten wurden die je 200 Frachten-Ganglinien miteinander verglichen. Sie zeigten optisch sowie für den Mittelwert, und damit für die Massenbilanz, eine sehr gute Übereinstimmung. Als weitere statistische Kennwerte dienten die Standardabweichung, die Anzahl der Nulldurchgänge sowie die Autokorrelation. In einem weiteren Analyse-Schritt wurden die Differenzen zwischen sich folgenden Werten der Ganglinien gebildet. Auch die Differenzen-Ganglinien wurden mit denselben statistischen Kennwerten untersucht. Für keinen dieser Kennwerte zeigten die gemessene und die modellierten Ganglinien eine starke Abweichung und für die meisten war die Übereinstimmung sehr gut.
Mit dieser Arbeit konnte gezeigt werden, dass das Muster der Urinfracht in der Kanalisation mit einem einfachen mathematischen Modell vorausgesagt werden kann. Für die Bestimmung der Parameter genügt es Angaben aus der Literatur und anderen vorhandenen Daten, sowie Werte aus einfachen Messungen zu verwenden. Die zeitintensivste Arbeit ist dabei die Literaturrecherche. Da das Modell einfach gehalten wurde, kann es ohne Probleme auf andere Einzugsgebiete oder Stoffe übertragen werden.
Für ein kleines Einzugsgebiet von gut 1000 Einwohnern konnte gezeigt werden, dass die Urinfracht starken kurzfristigen Schwankungen unterliegt. Innerhalb von gut 2 Minuten wurde eine Frachtzunahme um den Faktor 3 beobachtet. Diese kurzfristigen Frachten-Änderungen müssen bei Messkampagnen berücksichtigt werden, um grosse Fehler bei der Frachtenbestimmung zu vermeiden.