Stability of Illicit Drugs as Biomarkers in Sewers: From Lab to Reality (original) (raw)
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Science of The Total Environment
Stability of the selected urinary biomarkers of six illicit drugs and two therapeutic opioids in municipal wastewater was studied in order to determine errors associated with their possible transformation in the sewer. The stability was assessed in experiments conducted at 10°C and 20°C in order to simulate typical winter and summer temperature conditions in the sewer system. Among fourteen substances tested, the most unstable compounds were morphine-3-β-D glucuronide (MG), 6-acetyl morphine (6-AM), cocaine (COC) and 6-acetyl codeine (6-AC), while all other investigated compounds appeared to be relatively stable over a period of 72h. The transformation of all degradable compounds followed pseudo-first order kinetics with significantly longer half-times (t1/2) at winter conditions. At 20°C, t1/2 of MG, 6-AM, COC and 6-AC was 7h, 87h, 35h and 58h, respectively, while the corresponding t1/2 values at 10°C were 18h, 139h, 173h and 87h. The main transformation mechanism of MG, 6-AM and 6...
Critical review on the stability of illicit drugs in sewers and wastewater samples
Water research, 2016
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....
Environmental Science & Technology, 2019
In-sewer stability of illicit drug biomarkers has been evaluated by several reactor-based studies, but less has beendone in sewer pipes. Experiments conducted in sewer pipes have advantages over lab-scale reactors in providing more realisticbiomarker stability due to theflow and biological dynamics. This study assessed the transportation and transformation of sevenillicit drug biomarker compounds in a pilot-scale rising main and a gravity sewer pipe. Biomarkers presented diverse stabilitypatterns in the pilot sewers, based on which a drug transformation model was calibrated. This model was subsequently validatedusing transformation data sets from the literature, aiming to demonstrate the predictability of the pilot-based transformationcoefficients under varying sewer conditions. Furthermore, transformation coefficients forfive investigated biomarkers weregenerated from four studies, and their prediction capabilities under the pilot-sewer conditions were jointly assessed usingperformance statistics. The transformation model was successful in simulating the in-sewer stability for most illicit drugs.However, further study is required to delineate the sources and pathways for those compounds with potential formations to besimulated in the transformation model. Overall, the transformation model calibrated using the pilot-sewer data is a credible toolfor the application of wastewater-based epidemiology.
Transformation of Illicit Drugs and Pharmaceuticals in Sewer Sediments
Environmental Science & Technology, 2020
In-sewer stability of human excreted biomarkers is a critical factor of wastewater-based epidemiology in back-estimating illicit drug and pharmaceutical use in the community. Biomarker stability has been investigated in sewers with biofilm present, but the understanding in sewer sediments is still lacking. This study for the first time employed a laboratory sediment reactor to measure 18 illicit drug and pharmaceutical biomarkers under gravity sewer environments with the presence of sediment. Biomarkers exhibited various stability patterns due to transformation processes occurring in the bulk wastewater and sediments. The attenuation of a biomarker by sediments is driven by complex processes involving biodegradation, diffusion, and sorption, which is directly proportional to the ratio of sediment surface area against wastewater volume. The sediment-driven transformation coefficients of biomarkers are higher than the accordingly biofilm-mediated rates because of stronger microbial activities in sediments. Additionally, the stability of most biomarkers was insensitive to the natural pH variation in sewers, except for a few compounds (e.g., methadone, ketamine, paracetamol) susceptible to pH changes. In general, this study delineates the stability data of various biomarkers in gravity sewers with sediments, which are novel and long-missing information for wastewater-based epidemiology and improve the reliability of back-estimation in complex sewer networks.
Evaluation of in-sewer transformation of selected illicit drugs and pharmaceutical biomarkers
The Science of the total environment, 2017
Wastewater-based epidemiology (WBE) is considered to be a useful tool for monitoring chemical consumption in the population. However, the lack of information on potential transformation of biomarkers in the sewer system can compromise the accuracy of the consumption estimation. The present study contributes to addressing this issue by investigating the in-sewer stability of biomarkers from a number of commonly used drugs using laboratory sewer reactors that can mimic different sewer conditions. A stable and an unstable chemical (carbamazepine and caffeine) were also used as benchmarking chemicals to reflect the chemical degradation potential in different sewer conditions. The results suggested that ketamine and norketamine were unstable in gravity and rising main sewers, ketamine was unstable in bulk liquid while norketamine was stable under the same condition. Similarly, mephedrone and methylone were unstable in sewer conditions with considerable deviation. Significant loss of bupr...
Environmental science & technology, 2016
Sewer pipelines, although primarily designed for sewage transport, can also be considered as bioreactors. In-sewer processes may lead to significant variations of chemical loadings from source release points to the treatment plant influent. In this study, we assessed in-sewer utilization of growth substrates (primary metabolic processes) and transformation of illicit drug biomarkers (secondary metabolic processes) by suspended biomass. Sixteen drug biomarkers were targeted, including mephedrone, methadone, cocaine, heroin, codeine and tetrahydrocannabinol (THC) and their major human metabolites. Batch experiments were performed under aerobic and anaerobic conditions using raw wastewater, and abiotic biomarker transformation and partitioning to suspended solids and reactor wall were separately investigated under both redox conditions. A process model was identified by combining and extending Wastewater Aerobic/anaerobic Transformations in Sewers model (WATS) and Activated Sludge Mode...
Environmental Science & Technology, 2013
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 backcalculation 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.
Environmental science & technology, 2017
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 est...
Science of The Total Environment, 2019
Endogenous chemicals specific to human metabolism have been suggested to be good candidates for markers of population size in wastewater-based epidemiology (WBE). So far, creatinine is the only endogenous chemical to be assessed against the criteria of in-sewer stability. This study thus aimed to evaluate the fate of three other endogenous compounds, 5-hydroxy indole acetic acid (5-HIAA), cortisol and androstenedione, under different sewer conditions using laboratory-scale sewer reactors. The results showed that while all compounds were stable in wastewater only (i.e. without biofilm), cortisol and androstenedione degraded quickly in sewers with the presence of sewer biofilms. The degradation followed first-order kinetics similar to that of creatinine. In contrast, 5-HIAA was relatively stable in sewer reactors. This study also recognised the impact of wastewater pH on the detectability of 5-HIAA using a LC-MS/MS direct injection method. In samples acidified to pH 2, the method did not allow routine detection/quantification of 5-HIAA whereas in non-acidified samples the method was sufficiently sensitive for routine quantification of 5-HIAA. The stability of 5-HIAA in sewers and the possibility to measure it using a simple and rapid analytical method corroborate that 5-HIAA may be a suitable biomarker for estimation of population size in WBE.