Publications by authors named "Barbara Kasprzyk-Hordern"

93 Publications

Stereoselective Bacterial Metabolism of Antibiotics in Environmental Bacteria - A Novel Biochemical Workflow.

Front Microbiol 2021 16;12:562157. Epub 2021 Apr 16.

Department of Chemistry, University of Bath, Bath, United Kingdom.

Although molecular genetic approaches have greatly increased our understanding of the evolution and spread of antibiotic resistance genes, there are fewer studies on the dynamics of antibiotic - bacterial (A-B) interactions, especially with respect to stereochemistry. Addressing this knowledge gap requires an interdisciplinary synthesis, and the development of sensitive and selective analytical tools. Here we describe SAM (stereoselective antimicrobial metabolism) workflow, a novel interdisciplinary approach for assessing bacterial resistance mechanisms in the context of A-B interactions that utilise a combination of whole genome sequencing and mass spectrometry. Chloramphenicol was used to provide proof-of-concept to demonstrate the importance of stereoselective metabolism by resistant environmental bacteria. Our data shows that chloramphenicol can be stereoselectively transformed via microbial metabolism with CAP being subject to extensive metabolic transformation by an environmental bacterial strain. In contrast +)CAP is not metabolised by this bacterial strain, possibly due to the lack of previous exposure to this isomer in the absence of historical selective pressure to evolve metabolic capacity.
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http://dx.doi.org/10.3389/fmicb.2021.562157DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8086513PMC
April 2021

Changes in drug use in European cities during early COVID-19 lockdowns - A snapshot from wastewater analysis.

Environ Int 2021 Mar 26;153:106540. Epub 2021 Mar 26.

Environmental and Public Health Analytical Chemistry, Research Institute for Pesticides and Water, University Jaume I, Castellón, Spain; Institute for Biodiversity and Ecosystem Dynamics, University of Amsterdam, the Netherlands. Electronic address:

The COVID-19 outbreak has forced countries to introduce severe restrictive measures to contain its spread. In particular, physical distancing and restriction of movement have had important consequences on human behaviour and potentially also on illicit drug use and supply. These changes can be associated with additional risks for users, in particular due to reduced access to prevention and harm reduction activities. Furthermore, there have been limitations in the amount of data about drug use which can be collected due to restrictions. To goal of this study was to obtain information about potential changes in illicit drug use impacted by COVID-19 restrictions. Wastewater samples were collected in seven cities in the Netherlands, Belgium, Spain and Italy at the beginning of lockdowns (March-May 2020). Using previously established and validated methods, levels of amphetamine (AMP), methamphetamine (METH), MDMA, benzoylecgonine (BE, the main metabolite of cocaine) and 11-nor-9-carboxy-Δ-tetrahydrocannabinol (THC-COOH, main metabolite of tetrahydrocannabinol (THC)) were measured and compared with findings from previous years. Important differences in levels of consumed drugs were observed across the considered countries. Whilst for some substances and locations, marked decreases in consumption could be observed (e.g., 50% decrease in MDMA levels compared to previous years). In some cases, similar or even higher levels compared to previous years could be found. Changes in weekly patterns were also observed, however these were not clearly defined for all locations and/or substances. Findings confirm that the current situation is highly heterogeneous and that it remains very difficult to explain and/or predict the effect that the present pandemic has on illicit drug use and availability. However, given the current difficulty in obtaining data due to restrictions, wastewater analysis can provide relevant information about the situation at the local level, which would be hard to obtain otherwise.
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http://dx.doi.org/10.1016/j.envint.2021.106540DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7997602PMC
March 2021

New psychoactive substances in several European populations assessed by wastewater-based epidemiology.

Water Res 2021 May 27;195:116983. Epub 2021 Feb 27.

Istituto di Ricerche Farmacologiche Mario Negri IRCCS, Department of Environmental Sciences, Via Mario Negri 2, 20156, Milan, Italy.

Wastewater-based epidemiology (WBE) can be a useful tool to face some of the existing challenges in monitoring the use of new psychoactive substances (NPS), as it can provide objective and updated information. This Europe-wide study aimed to verify the suitability of WBE for investigating the use of NPS. Selected NPS were monitored in urban wastewater by high performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS). The main classical illicit drugs were monitored in the same samples to compare their levels with those of NPS. Raw composite wastewater samples were collected in 2016 and 2017 in 14 European countries (22 cities) following best practice sampling protocols. Methcathinone was most frequent (>65% of the cities), followed by mephedrone (>25% of the cities), and only mephedrone, methcathinone and methylone were found in both years. This study depicts the use of NPS in Europe, confirming that it is much lower than the use of classical drugs. WBE proved able to assess the qualitative and quantitative spatial and temporal profiles of NPS use. The results show the changeable nature of the NPS market and the importance of large WBE monitoring campaigns for selected priority NPS. WBE is valuable for complementing epidemiological studies to follow rapidly changing profiles of use of drugs.
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http://dx.doi.org/10.1016/j.watres.2021.116983DOI Listing
May 2021

Application of wastewater-based epidemiology to investigate stimulant drug, alcohol and tobacco use in Lithuanian communities.

Sci Total Environ 2021 Feb 19;777:145914. Epub 2021 Feb 19.

Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Antwerp, Belgium. Electronic address:

WBE was applied to evaluate illicit drug (i.e. amphetamine, cocaine, MDMA and methamphetamine), alcohol and tobacco use in three Lithuanian cities in 2018 and 2019. Considerable concentrations of methamphetamine and MDMA were found in the three locations, suggesting a specific Lithuanian consumption pattern. Yet, unexpected high concentrations of amphetamine (>4 μg/L) were detected in two samples of Kaunas in 2018. Through the use of chiral analysis and non-target and suspect drug precursor compound screening, these extreme values were confirmed to be the result of direct disposal of amphetamine in the sewers. Furthermore, substantial alcohol use was measured in the three investigated catchment populations of Lithuania with almost 4 standard drinks/day/inhabitant aged 15+ on average in 2019. For tobacco, an average of 5.6 cigarettes/day/inhabitant aged 15+ in 2019 was reported with large discrepancies between WBE figures and sales data, potentially highlighting illegal trade of tobacco products.
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http://dx.doi.org/10.1016/j.scitotenv.2021.145914DOI Listing
February 2021

Occurrence of pharmaceutical residues, personal care products, lifestyle chemicals, illicit drugs and metabolites in wastewater and receiving surface waters of Krakow agglomeration in South Poland.

Sci Total Environ 2021 May 29;768:144360. Epub 2020 Dec 29.

University of Bath, Department of Chemistry, Bath BA2 7AY, United Kingdom. Electronic address:

This is the first study of broad range of chemical classes CECs conducted in the upper Wisla river catchment including the biggest WWTPs in this region and surface waters. The list of compounds is extensive and the paper provides, for the first time, better understanding of environmental burden from PCPCs in Poland. Cumulative contribution of hypertension pharmaceuticals, nonsteroidal anti-inflammatory drugs (NSAIDs) and lifestyle chemicals was 89% and 95% in wastewater influent, and 75% in wastewater effluent at both WWTPs. Significant removal efficiencies, exceeding 90%, were found for parabens, UV filters, NSAIDs, steroid estrogens, plasticizers, antibacterials/antibiotics, stimulants and metabolites and lifestyle chemicals. The comparison of the average mass loads of CECs between the influent and effluent, has shown that 27% and 29% of all detected CECs were removed by less than 50%. An increase of concentrations of CECs in the effluent was observed for 18% and 20% of all detected CECs in Kujawy and Plaszow WWTPs, respectively. Negative mass balances of fexofenadine, venlafaxine, o-desmethyltramadol, ketamine and temazepam were noted within WWTPs, which are a result of dissolution of persistent contaminants accumulated in aggregates and/or back-transformation or de-conjugation of metabolites into parent compounds. 44 CECs were detected in surface waters located upstream and downstream of the WWTPs. The concentrations of compounds were largely dependent on the dilution factor of WWTP discharge. The risk quotation (RQ) values for compounds present in surface waters were calculated in relation to their potential for bioaccumulation. Among compounds with high potential for bioaccumulation, with log K ≥ 4.5, diclofenac, atorvastatin and triclosan were found to be of high risk. Many CECs with high, moderate or even low environmental impact have shown high potential for bioaccumulation and should be considered as priority at the same risk level. Moreover, possible synergistic action is still of concern.
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http://dx.doi.org/10.1016/j.scitotenv.2020.144360DOI Listing
May 2021

A high prevalence of in () and related species in hospital wastewater in South West England.

Microb Genom 2021 03 8;7(3). Epub 2021 Jan 8.

The Milner Centre for Evolution, Department of Biology and Biochemistry, University of Bath, Bath, UK.

species occupy a wide range of environmental and animal niches, and occasionally cause opportunistic infections that are resistant to multiple antibiotics. In particular, () has gained notoriety as a major nosocomial pathogen, due principally to the rise in non-susceptibility to carbapenems and other beta-lactam antibiotics. Whilst it has been proposed that the urban water cycle facilitates transmission of pathogens between clinical settings and the environment, the level of risk posed by resistant strains in hospital wastewater remains unclear. We used whole genome sequencing (WGS) to compare species in contemporaneous samples of wastewater from an English hospital and influent to the associated wastewater treatment plant (WWTP). As we aimed to characterize representative samples of communities, we did not actively select for antibiotic resistance (other than for ampicillin), nor for specific species. Two species, and . () (), were of equal dominance in the hospital wastewater, and four other species were present in low abundance in this sample. In contrast, despite being the species most closely associated with healthcare settings, was the dominant species within the WWTP influent. In total, 29 % of all isolates harboured the gene on a pOXA-48-like plasmid, and these isolates were almost exclusively recovered from the hospital wastewater. This gene was far more common in (68 % of isolates) than in (3.4 % of isolates). In general plasmid-borne, but not chromosomal, resistance genes were significantly enriched in the hospital wastewater sample. These data implicate hospital wastewater as an important reservoir for antibiotic-resistant , and point to an unsuspected role of species within the group in the maintenance and dissemination of plasmid-borne . This article contains data hosted by Microreact.
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http://dx.doi.org/10.1099/mgen.0.000509DOI Listing
March 2021

Estimation of community-wide multi-chemical exposure via water-based chemical mining: Key research gaps drawn from a comprehensive multi-biomarker multi-city dataset.

Environ Int 2021 02 30;147:106331. Epub 2020 Dec 30.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Wessex Water, Bath BA2 7WW, UK.

This paper explores the strong potential of chemical mining of wastewater for markers of community-wide intake of wide-ranging harmful chemicals belonging to several usage groups: industrial chemicals, personal care products, pesticides, illicit drugs, lifestyle chemicals and prescription pharmaceuticals as a proxy for multi-chemical community-wide exposure. An estimation of chemical intake in five contrasting town/cities based in the Avon River catchment in the South-West UK was undertaken. High-resolution spatiotemporal pharmaceutical prescription databases were used for system calibration, both in terms of biomarker selection and its correction factor, as well as for the overall system performance evaluation, both spatially and temporality. Only metabolism data accounting for phase two metabolism provided correct estimates of pharma intake. Using parent compounds as XCRs (xenobiotic compounds residue) was found to overestimate exposure due to an inclusion of directly disposed (unused) drugs. Spatiotemporal trends in XC intake were observed as a result of occupational exposure (higher bisphenol A (BPA) intake during weekday), and lifestyle choices (higher cocaine and pyrethroid pesticides intake during weekend). WBE is not intended to estimate individual exposure to chemicals. It can however provide estimates at a community level, and as a result, it has the potential to be developed into an early warning system, a powerful tool for large scale screening studies identifying communities at risk and in need of high resolution individual testing at a localised scale.
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http://dx.doi.org/10.1016/j.envint.2020.106331DOI Listing
February 2021

Micropollutant fluxes in urban environment - A catchment perspective.

J Hazard Mater 2021 01 23;401:123745. Epub 2020 Aug 23.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Water Innovation & Research Centre (WIRC), University of Bath, Bath BA2 7AY, UK. Electronic address:

This study provided a holistic understanding of the sources, fate and behaviour of 142 compounds of emerging concern (CECs) throughout a river catchment impacted by 5 major urban areas. Of the incoming 169.3 kg d of CECs entering the WwTWs, 167.9 kg d were present in the liquid phase of influent and 1.4 kg d were present in the solid phase (solid particulate matter, SPM). Analysis of SPM was important to determine accurate loads of incoming antidepressants and antifungal compounds, which are primarily found in the solid phase. Furthermore, these classes and the plasticiser, bisphenol A (BPA) were the highest contributors to CEC load in digested solids. Population normalised loads showed little variation across the catchment at 154 ± 12 mg d inhabitant indicating that population size is the main driver of CECs in the studied catchment. Across the catchment 154.6 kg d were removed from the liquid phase during treatment processes. CECs discharged into surface waters from individual WwTWs contributed between 0.19 kg d at WwTW A to 7.3 kg d at WwTW E, which correlated strongly with the respective contributing populations. Spatial and temporal variations of individual CECs and their respective classes were found in WwTW influent (both solid (influent) and liquid phases (influent)) throughout the catchment, showing that different urban areas impact the catchment in different ways, with key variables being lifestyle, use of over-the-counter pharmaceuticals and industrial activity. Understanding of both spatial and temporal variation of CECs at the catchment level helped to identify possible instances of direct disposal, as in the case of carbamazepine. Analysis of surface waters throughout the catchment showed increasing mass loads of CECs from upstream of WwTW A to downstream at WwTW D, showing clear individual contributions from WwTWs. Many CECs were ubiquitous throughout the river water in the catchment. Daily loads ranged from 0.005 g d (ketamine, WwTW A) up to 1890.3 g d (metformin, WwTW C) for the 84/138 CECs that were detected downstream of the WwTWs. For metformin this represents the equivalent of ∼1,890 tablets (1,000 mg per tablet) dissolved in the river water downstream of WwTW C.
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http://dx.doi.org/10.1016/j.jhazmat.2020.123745DOI Listing
January 2021

A multi-residue method by supercritical fluid chromatography coupled with tandem mass spectrometry method for the analysis of chiral and non-chiral chemicals of emerging concern in environmental samples.

Anal Bioanal Chem 2020 Sep 9;412(23):5563-5581. Epub 2020 Jul 9.

Department of Chemistry, Faculty of Science, University of Bath, Bath, BA2 7AY, UK.

This manuscript presents the development, validation and application of a multi-residue supercritical fluid chromatography coupled with tandem mass spectrometry method for the analysis of 140 chiral and non-chiral chemicals of emerging concern in environmental samples, with 81 compounds being fully quantitative, 14 semi-quantitative and 45 qualitative, validated according to European Medicine Agency (EMA) guidelines (European Medicines Agency 2019). One unified LC-MS method was used to analyse all analytes, which were split into three injection methods to ensure sufficient peak resolution. The unified method provided an average of 113% accuracy and 4.5% precision across the analyte range. Limits of detection were in the range of 35 pg L-0.7 μg L, in both river water and wastewater, with an average LOD of 33 ng L. The method was combined with solid-phase extraction and applied in environmental samples, showing very good accuracy and precision, as well as excellent chromatographic resolution of a range of chiral enantiomers including beta-blockers, benzodiazepines and antidepressants. The method resulted in quantification of 75% of analytes in at least two matrices, and 56% in the trio of environmental matrices of river water, effluent wastewater and influent wastewater, enabling its use in monitoring compounds of environmental concern, from their sources of origin through to their discharge into the environment.
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http://dx.doi.org/10.1007/s00216-020-02780-9DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7413908PMC
September 2020

(Fluoro)quinolones and quinolone resistance genes in the aquatic environment: A river catchment perspective.

Water Res 2020 Sep 6;182:116015. Epub 2020 Jun 6.

Department of Chemistry, Faculty of Science, University of Bath, Bath, BA2 7AY, United Kingdom, UK. Electronic address:

This study provides an insight into the prevalence of (fluoro)quinolones (FQs) and their specific quinolone qnrS resistance gene in the Avon river catchment area receiving treated wastewater from 5 wastewater treatment plants (WWTPs), serving 1.5 million people and accounting for 75% of inhabitants living in the catchment area in the South West of England.. Ofloxacin, ciprofloxacin, nalidixic acid and norfloxacin were found to be ubiquitous with daily loads reaching a few hundred g/day in wastewater influent and tens of g/day in receiving waters. This was in contrast to other FQs analysed: flumequine, nadifloxacin, lomefloxacin, ulifloxacin, prulifloxacin, besifloxacin and moxifloxacin, which were hardly quantified. Enantiomeric profiling revealed that ofloxacin was enriched with the S-(-)-enantiomer, likely deriving from its prescription as the more potent enantiomerically pure levofloxacin, alongside racemic ofloxacin. While ofloxacin's enantiomeric fraction (EF) remained constant, high stereoselectivity was observed in the case of its metabolite ofloxacin-N-oxide. The removal efficiency of quinolones during wastewater treatment at 5 WWTPs utilising either trickling filters (TF) or activated sludge (AS), was compound and wastewater treatment process dependent, with AS providing better efficiency than TF. The qnrS resistance gene was ubiquitous in wastewater. Its removal was WWTP treatment process dependent with TF performing best and resulting in significant removal of the gene (from 28 to 75%). AS underperformed with only 9% removal in the case of activated sludge and actual increase in the gene copy number within sequencing batch reactors (SBRs). Interestingly, the data suggests that higher removal of antibiotics could be linked with high prevalence of the gene (SBR and WWTP E) and vice versa, low removal of antibiotic is correlated with lower prevalence of the gene in wastewater effluent (TF, WWTP B and D). This is especially prominent in the case of ofloxacin and could indicate that AS might be facilitating antimicrobial resistance (AMR) prevalence to higher extent than TF. Wastewater-based epidemiology (WBE) was also applied to monitor any potential misuse (e.g. direct disposal) of FQs in the catchment. In most cases higher use of antibiotics with respect to official statistics (i.e. ciprofloxacin, ofloxacin) was observed, which suggests that FQs management practice require further attention.
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http://dx.doi.org/10.1016/j.watres.2020.116015DOI Listing
September 2020

Wastewater-based epidemiology combined with local prescription analysis as a tool for temporalmonitoring of drugs trends - A UK perspective.

Sci Total Environ 2020 Sep 15;735:139433. Epub 2020 May 15.

Department of Chemistry, Faculty of Science, University of Bath, Bath BA2 7AY, United Kingdom. Electronic address:

This paper reports the application of wastewater-based epidemiology (WBE) for the monitoring of one city in the UK in years 2014-2018 as a means of 1) exploring relative temporal changes of illicit drug usage trends across 5 sampling weeks in 5 years, (2) assessing policy impact in reducing drug consumption, focussing particularly on mephedrone, which was classified as a class B drug in the UK in 2010, and the effects of subsequent regulation such as the novel psychoactive substances (NPS) bill of 2016, (3) investigating temporal changes in consumption of prescription pharmaceuticals vs illicit drug usage, and (4) comparing consumption of prescription drugs with WBE to enable more accurate verification of prescription drugs with abuse potential. Mephedrone was quantified only for the first two years of the study, 2014-2015, and remained undetected for the next three years of the study. This shows that given enough time changes in drug policy can have an effect on drug consumption. However, after the introduction of the 2016 NPS bill, between the third and fourth study years, there was an observable increase in the consumption of "classic" drugs of abuse such as cocaine, MDMA and ketamine suggesting a shift away from novel psychoactives. The unique prescription dataset allowed for a more accurate calculation of heroin consumption using morphine by examining other sources morphine. Additionally, for compounds with controlled prescription like methadone, trends in consumption estimated by wastewater and trends in prescription correlated. Wastewater-based epidemiology is a powerful tool for examining whole populations and determining the efficacy and direction of government actions on health, as it can, alongside prescription and wider monitoring data, provide a clear insight into what is being consumed by a population and what action is needed to meet required goals.
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http://dx.doi.org/10.1016/j.scitotenv.2020.139433DOI Listing
September 2020

Future perspectives of wastewater-based epidemiology: Monitoring infectious disease spread and resistance to the community level.

Environ Int 2020 06 4;139:105689. Epub 2020 Apr 4.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Centre for Doctoral Training in Sustainable Chemical Technologies, University of Bath, Bath BA2 7AY, UK. Electronic address:

Infectious diseases are acknowledged as one of the most critical threats to global public health today. Climate change, unprecedented population growth with accelerated rates of antimicrobial resistance, have resulted in both the emergence of novel pathogenic organisms and the re-emergence of infections that were once controlled. The consequences have led to an increased vulnerability to infectious diseases globally. The ability to rapidly monitor the spread of diseases is key for prevention, intervention and control, however several limitations exist for current surveillance systems and the capacity to cope with the rapid population growth and environmental changes. Wastewater-Based Epidemiology (WBE) is a new epidemiology tool that has potential to act as a complementary approach for current infectious disease surveillance systems and an early warning system for disease outbreaks. WBE postulates that through the analysis of population pooled wastewater, infectious disease and resistance spread, the emergence of new disease outbreak to the community level can be monitored comprehensively and in real-time. This manuscript provides critical overview of current infectious disease surveillance status, as well as it introduces WBE and its recent advancements. It also provides recommendations for further development required for WBE application as an effective tool for infectious disease surveillance.
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http://dx.doi.org/10.1016/j.envint.2020.105689DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7128895PMC
June 2020

The role of stereochemistry of antibiotic agents in the development of antibiotic resistance in the environment.

Environ Int 2020 06 3;139:105681. Epub 2020 Apr 3.

Department of Chemistry, University of Bath, BA27AY Bath, United Kingdom. Electronic address:

Antibiotic resistance (ABR) is now recognised as a serious global health and economic threat that is most efficiently managed via a 'one health' approach incorporating environmental risk assessment. Although the environmental dimension of ABR has been largely overlooked, recent studies have underlined the importance of non-clinical settings in the emergence and spread of resistant strains. Despite this, several research gaps remain in regard to the development of a robust and fit-for-purpose environmental risk assessment for ABR drivers such as antibiotics (ABs). Here we explore the role the environment plays in the dissemination of ABR within the context of stereochemistry and its particular form, enantiomerism. Taking chloramphenicol as a proof of principle, we argue that stereoisomerism of ABs impacts on biological properties and the mechanisms of resistance and we discuss more broadly the importance of stereochemistry (enantiomerism in particular) with respect to antimicrobial potency and range of action.
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http://dx.doi.org/10.1016/j.envint.2020.105681DOI Listing
June 2020

Enantiomeric profiling of quinolones and quinolones resistance gene qnrS in European wastewaters.

Water Res 2020 May 10;175:115653. Epub 2020 Mar 10.

Department of Chemistry, Faculty of Science, University of Bath, Bath, BA2 7AY, United Kingdom. Electronic address:

Wastewater-based epidemiology (WBE) was applied for the first time in seven cities across Europe with the aim of estimating quinolones consumption via the analysis of human urinary metabolites in wastewater. This report is also the first pan-European study focussed on the enantiomeric profiling of chiral quinolones in wastewater. By considering loads of (fluoro)quinolones in wastewater within the context of human stereoselective metabolism, we identified cities in Southern Europe characterised by both high usage and direct disposal of unused ofloxacin. In Northern European cities, S-(-)-ofloxacin loads were predominant with respect to R-(+)-ofloxacin. Much more potent, enantiomerically pure S-(-)-ofloxacin was detected in wastewaters from Southern European cities, reflecting consumption of the enantiomerically pure antibiotic. Nalidixic acid, norfloxacin and lomefloxacin were detected in wastewater even though they were not prescribed according to official prescription data. S,S-(-)-moxifloxacin and S,S-(-)-moxifloxacin-N-sulphate were detected in wastewater due to metabolism of moxifloxacin. For the first time, average population-normalised ulifloxacin loads of 22.3 and 1.5 mg day 1000 people were reported for Milan and Castellón as a result of prulifloxacin metabolism. Enrichment of flumequine with first-eluting enantiomer in all the samples indicated animal metabolism rather than its direct disposal. Fluoroquinolone loads were compared with qnrS gene encoding quinolone resistance to correlate usage of fluoroquinolone and prevalence of resistance. The highest daily loads of the qnrS gene in Milan corresponded with the highest total quinolone load in Milan proving the hypothesis that higher usage of quinolones is linked with higher prevalence of quinolone resistance genes. Utrecht, with the lowest quinolones usage (low daily loads) had also one of the lowest daily loads of the qnrS gene. However, a similar trend was not observed in Oslo nor Bristol where higher qnrS gene loads were observed despite low quinolone usage.
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http://dx.doi.org/10.1016/j.watres.2020.115653DOI Listing
May 2020

Spatio-temporal assessment of illicit drug use at large scale: evidence from 7 years of international wastewater monitoring.

Addiction 2020 01 23;115(1):109-120. Epub 2019 Oct 23.

Faculty of Fisheries and Protection of Waters, University of South Bohemia in Ceske Budejovice, Zatisi, Czech Republic.

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 Δ -tetrahydrocannabinol (11-nor-9-carboxy-Δ -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.
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http://dx.doi.org/10.1111/add.14767DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6973045PMC
January 2020

Multi-residue ultra-performance liquid chromatography coupled with tandem mass spectrometry method for comprehensive multi-class anthropogenic compounds of emerging concern analysis in a catchment-based exposure-driven study.

Anal Bioanal Chem 2019 Nov 7;411(27):7061-7086. Epub 2019 Sep 7.

Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY, UK.

This paper presents a new multi-residue method for the quantification of more than 142 anthropogenic compounds of emerging concern (CECs) in various environmental matrices. These CECs are from a wide range of major classes including pharmaceuticals, household, industrial and agricultural. This method utilises ultra-performance liquid chromatography coupled with tandem mass spectrometry (UPLC-MS/MS) for analysis of five matrices (three liquid and two solid) from wastewater treatment processes and the surrounding environment. Relative recoveries were predominantly between 80 and 120%; however, due to the complexity of the matrices used in this work, not all compounds were recovered in all matrices, from 138/142 analytes in surface water to 96/142 analytes in digested solids. Method quantification limits (MQLs) ranged from 0.004 ng L (bisoprolol in surface water) to 3118 ng L (creatinine in wastewater treatment work (WwTW) influent). The overall method accuracy was 107.0%, and precision was 13.4%. To test its performance, the method was applied to the range of environmental matrices at WwTWs in South West England. Overall, this method was found to be suitable for application in catchment-based exposure-driven studies, as, of the total number of analytes quantifiable in each matrix, 61% on average was found to be above their corresponding MQL. The results confirm the need for analysing both the liquid and solid compartments within a WwTW to prevent under-reporting of concentrations.
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http://dx.doi.org/10.1007/s00216-019-02091-8DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6838033PMC
November 2019

Stereoisomeric profiling of chiral pharmaceutically active compounds in wastewaters and the receiving environment - A catchment-scale and a laboratory study.

Environ Int 2019 06 11;127:558-572. Epub 2019 Apr 11.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Water Innovation & Research Centre (WIRC), University of Bath, Bath BA2 7AY, UK. Electronic address:

Chiral pharmaceutically active compounds (cPACs) are not currently governed by environmental regulation yet are expected to be in the future. As cPACs can exert stereospecific toxicity in the aquatic environment, it is essential to better understand their stereoselective behaviour here. Therefore, this study aims to provide a new perspective towards comprehensive evaluation of cPACs at a river catchment level, including their stereochemistry as a chemical phenomenon driving fate of chiral molecules in the environment. A large spatial and temporal monitoring program was performed in Southwest England. It included 5 sewage treatment works and the receiving waters of the largest river catchment in Southwest England. Simultaneously, lab-scale microcosm studies in simulated activated sludge bioreactors and river water microcosm were performed to evaluate stereoselective degradation of cPACs. A multi-residue enantioselective method allowed the analysis of a total of 18 pairs of enantiomers and 3 single enantiomers in wastewater and river water samples. Our monitoring program revealed: (1) spatial and temporal variations of cPACs in influent wastewaters resulting from different patterns of usage as well as an (2) enantiomeric enrichment of cPACs, likely due to human metabolism, despite their commercialization as racemic mixtures. A similar chiral signature was observed in effluent and receiving waters. Stereoselective degradation was observed in trickling filters (TF) for naproxen, ketoprofen, cetirizine and 10,11-dihydroxy-10-hydroxycarbamazepine, in sequencing batch reactors (SBR) for ifosfamide and in activated sludge (AS) for cetirizine. The extent of enantiomer-specific fate was wastewater treatment dependent in the case of naproxen (TF showed higher stereoselectivity than AS and SBR) and cetirizine (TF and AS showed higher stereoselectivity than SBR) due to differing microbial population. Furthermore, stereoselective degradation of naproxen was highly variable among STWs using similar treatments (TF) and operating in the same region. Microbial stereoselective degradation was also confirmed by both activated and river water simulated microcosm for chloramphenicol, ketoprofen, indoprofen, naproxen and 10,11-dihydroxy-10-hydroxycarbamazepine. Results from our large scale river catchment monitoring study and lab simulated microcosm show wide-ranging implications of enantiomerism of cPACs on environmental risk assessment (ERA). As two enantiomers of the same compound show different biological effects (e.g. toxicity), their non-racemic presence in the environment might lead to inaccurate ERA. This is because current ERA approaches do not require analysis at enantiomeric level.
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http://dx.doi.org/10.1016/j.envint.2019.03.050DOI Listing
June 2019

An ultra-high-performance liquid chromatography tandem mass spectrometry method for oxidative stress biomarker analysis in wastewater.

Anal Bioanal Chem 2019 Apr 23;411(11):2261-2271. Epub 2019 Feb 23.

Department of Chemistry, University of Bath, Bath, BA2 7AY, UK.

Reported herein is the development of an analytical method for the detection of four oxidative stress biomarkers in wastewater using ultra-high-performance liquid chromatography coupled with tandem mass spectrometry (UHPLC-MS/MS) and solid phase extraction (SPE). The following four biomarkers of oxidative stress and lipid peroxidation have been investigated: hydroxynonenal-mercapturic acid (HNE-MA), 8-iso-prostglandin F2beta (8-iso-PGF), 8-nitroguanine (8-NOGua) and 8-hydroxy-2-deoxyguanosine (8-OHdG). The method showed very good performance: accuracy (> 87%), precision (> 90%), method quantification limits (1.3-3.0 ng L) and biomarker stability in wastewater in the case of HNE-MA, 8-OHdG and 8-iso-PGF. In contrast, 8-NOGua was found to be less stable in wastewater, which affected its method performance: accuracy (> 63%), precision (> 91%) and method quantification limits (85.3 ng L). Application of the developed method resulted in, for the first time, HNE-MA being successfully observed and quantified within wastewater over a study period of a week (displayed average daily loads per capita of 48.9 ± 4.1 mg/1000/people/day). 8-iso-PGF was detected with good intensity but could not be quantified due to co-elution with other isomers. 8-OHdG was detected, albeit at < MQL. This study demonstrates the potential for expanding on the possible endogenous biomarkers of health used in urban water fingerprinting to aid in measuring health in near-real time on a community-wide scale.
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http://dx.doi.org/10.1007/s00216-019-01667-8DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6459808PMC
April 2019

Estimation of community-wide exposure to bisphenol A via water fingerprinting.

Environ Int 2019 04 25;125:1-8. Epub 2019 Jan 25.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK. Electronic address:

Molecular epidemiology in human biomonitoring allows for verification of public exposure to chemical substances. Unfortunately, due to logistical difficulties and high cost, it evaluates only small study groups and as a result does not provide comprehensive large scale community-wide exposure data. Wastewater fingerprinting utilizing metabolic biomarkers of exposure that are excreted collectively by studied populations into urine and ultimately into the community's wastewater, provides a timely alternative to traditional approaches. This study aimed to provide comprehensive spatiotemporal community-wide exposure to bisphenol A (BPA, including BPA intake) using wastewater fingerprinting. Wastewater fingerprinting was undertaken using high resolution mass spectrometry retrospective data mining of characteristic BPA human metabolism marker (bisphenol A sulphate), applied to a large geographical area of 2000 km and a population of ~1.5 million served by 5 WWTPs (wastewater treatment plants) accounting for >75% of the overall population in the studied catchment. Community-wide BPA intake was found to be below temporary tolerable daily intake (t-TDI) level of 4 μg kg day set by the European Food Safety Agency (EFSA) suggesting overall low exposure at 3 WWTPs serving residential areas with low industrial/commercial presence. However, at two WWTPs serving communities with higher industrial/commercial presence, higher BPA sulphate loads corresponding to higher (up to 14 times) BPA intakes (exceeding 10 μg kg day at one WWTP and reaching 50 μg kg day at the second WWTP) were observed and they are likely linked with occupational exposure. Characteristic temporal variations of BPA intake were noted in most studied WWTPs with the lowest intake occurring during weekends and the highest during weekdays.
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http://dx.doi.org/10.1016/j.envint.2018.12.048DOI Listing
April 2019

A new analytical framework for multi-residue analysis of chemically diverse endocrine disruptors in complex environmental matrices utilising ultra-performance liquid chromatography coupled with high-resolution tandem quadrupole time-of-flight mass spectrometry.

Anal Bioanal Chem 2019 Jan 22;411(3):689-704. Epub 2018 Nov 22.

Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY, UK.

This manuscript presents a comprehensive analytical framework for identification and quantification of chemically diverse endocrine disrupting chemicals (EDCs) used in personal care and consumer products in diverse solid and liquid environmental matrices with an ultimate goal of evaluating public exposure to EDCs via water fingerprinting. Liquid chromatography coupled with tandem quadrupole time-of-flight mass spectrometry (UHPLC-ESI-MS/MS) was used for targeted analysis of selected EDCs as well as to identify and quantify a few metabolites using post-acquisition data mining. Solid-phase extraction (SPE) was applied to liquid matrices in order to reduce matrix effects and provide required sample concentration and ultimately, high sensitivity and selectivity of measurements. SPE recoveries in liquid samples ranged from 49 to 140% with method quantification limits not exceeding 1 ng L for the majority of EDCs. Microwave-assisted extraction (MAE) was applied to solid samples and when followed by SPE, it permitted the analysis of EDCs in digested sludge. MAE/SPE recoveries varied from 11 to 186% and MQLs between 0.03 and 8.1 ng g with the majority of compounds showing MQLs below 2 ng g. Mass error for quantifier and qualifier ions was below 5 ppm when analysing river water and effluent wastewater and below 10 ppm when analysing influent wastewater and solid samples. The method was successfully applied to environmental samples, with 33 EDCs identified and quantified in wastewater and receiving waters. In addition, several EDCs were found in digested sludge, which confirms that for a more comprehensive understanding of exposure patterns and environmental impact, analysis of solids cannot be neglected. Finally, post-acquisition data mining permitted the identification and quantification of a metabolite of BPA and the identification of a metabolite of 4-Cl-3-methylphenol. Graphical abstract ᅟ.
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http://dx.doi.org/10.1007/s00216-018-1483-yDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6338708PMC
January 2019

Assessment of bisphenol-A in the urban water cycle.

Sci Total Environ 2019 Feb 5;650(Pt 1):900-907. Epub 2018 Sep 5.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Water Innovation & Research Centre (WIRC), University of Bath, Bath BA2 7AY, UK. Electronic address:

The plasticizer bisphenol-A (BPA) is common to municipal wastewaters and can exert toxicity to exposed organisms in the environment. Here BPA concentration at 5 sewage treatment works (STW) and distribution throughout a river catchment in South West UK were investigated. Sampling sites included influent and effluent wastewater (n = 5), river water (n = 7) and digested sludge (n = 2) which were monitored for 7 consecutive days. Findings revealed average BPA loads in influent wastewater at two STWs were 10-37 times greater than the other wastewaters monitored. Concentrations up to ~100 μg L were measured considerably higher than previously reported for municipal wastewaters. Temporal variability throughout the week (i.e., highest concentrations during weekdays) suggests these high concentrations are linked with industrial activity. Despite ≥90% removal during wastewater treatment, notable concentrations remained in tested effluent (62-892 ng L). However, minimal impact on BPA concentrations in river water was observed for any of the effluents. The maximum BPA concentration found in river water was 117 ng L which is considerably lower than the current predicted no effect concentration of 1.6 μg L. Nevertheless, analysis of digested sludge from sites which received these elevated BPA levels revealed average concentrations of 4.6 ± 0.3 and 38.7 ± 5.4 μg g. These sludge BPA concentrations are considerably greater than previously reported and are attributed to the high BPA loading in influent wastewater. A typical sludge application regime to agricultural land would result in a predicted BPA concentration of 297 ng g in soil. Further studies are needed on the toxicological thresholds of exposed terrestrial organisms in amended soils to better assess the environmental risk here.
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http://dx.doi.org/10.1016/j.scitotenv.2018.09.011DOI Listing
February 2019

Multi-residue analysis of chiral and achiral trace organic contaminants in soil by accelerated solvent extraction and enantioselective liquid chromatography tandem-mass spectrometry.

J Chromatogr A 2018 Oct 19;1572:62-71. Epub 2018 Aug 19.

School of Pharmacy and Life Sciences, Robert Gordon University, Aberdeen, AB10 7GJ, United Kingdom.

Reported here is the first analytical methodology for the enantiomeric determination of chiral trace organic contaminants (TOrCs) in soil. Direct enantioselective separations were achieved on a Chirobiotic V2 column operated in polar ionic mode. Initial screening of vancomycin stationary phases found Chirobiotic V2 better suited for multi-residue separation of chiral TOrCs than Chirobiotic V due to differences in the ligand linkage chemistry. Simultaneous enantioseparation of beta-blockers, beta-agonists, anti-depressants, anti-histamines and stimulants was achieved for the first time. This included the first separation of chlorpheniramine enantiomers with a method suitable for environmental analysis (i.e., coupled to MS). Investigation of mobile phase composition found the concentration of liophilic ions had the greatest influence on enantioseparations and of most importance during method development. The optimized method achieved simultaneous separation of salbutamol, propranolol, atenolol, amphetamine, chlorpheniramine and fluoxetine enantiomers with satisfactory resolution (>1.0). For completeness, such methods also need to support analysis of achiral TOrCs. Therefore three achiral TOrCs (carbamazepine, carbamazepine 10,11 epoxide and triclocarban) were included to demonstrate the methods suitability. Method recoveries for all analytes ranged from 76 to 122% with method quantitation limits (MQLs) <1 ng g. Application of the method to soil microcosm studies revealed stereoselective degradation of chiral TOrCs for the first time. For example, S(+)-amphetamine degraded at a faster rate than its corresponding enantiomer leading to an enrichment of R(-)-amphetamine. Therefore to better understand the risk posed from TOrCs on the terrestrial environment, chiral species need profiled at the enantiomeric level. This can now be addressed using the proposed methodology whilst simultaneously profiling achiral TOrCs.
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http://dx.doi.org/10.1016/j.chroma.2018.08.034DOI Listing
October 2018

Verifying community-wide exposure to endocrine disruptors in personal care products - In quest for metabolic biomarkers of exposure via in vitro studies and wastewater-based epidemiology.

Water Res 2018 10 14;143:117-126. Epub 2018 Jun 14.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK. Electronic address:

This study aimed to identify human specific metabolites of selected known or suspected endocrine disruptors (EDCs), mainly UV filters, used in personal care and consumer products whose metabolism has hardly been explored and to select suitable candidate biomarkers for human exposure studies using wastewater based epidemiology (WBE). The analysis of metabolic biomarkers of target chemicals is crucial in order to distinguish between internal and external exposure, since many sources contribute to chemicals being discharged into wastewater. This was achieved through the employment of a new analytical framework for verification of biomarkers of exposure to chemicals combining human biomonitoring and water fingerprinting. Eight EDCs with unknown metabolic pathways (benzophenone-1 (BP-1); benzophenone-2 (BP-2); 4,4'-dihydroxybenzophenone (4,4'-DHBP); 4-benzylphenol (4-BenzPh); homosalate (HO); octocrylene (OC); 3-benzylidene camphor (3-BC), and two EDCs with known metabolism (bisphenol A (BPA) and benzophenone-3 (BP-3)) were tested. The biotransformation observed consisted mainly of phase I processes such as hydrolysis and hydroxylation together with phase II conjugation reactions such as sulphation and glucuronidation. Only two chemicals (BP-1, BP-3) were identified in urine and three chemicals (BPA, BP-1, BP-3) in wastewater. Five newly discovered metabolites (HO-Met1, OC-Met1, 4-BenzPh-Met4, 4-BenzPh-Met5 and 4-BenzPh-Met6) and one previously known metabolite (BPA-Met3) were detected in tested urine/wastewater samples from five WWTPs serving large communities ranging between 17 and 100 thousand inhabitants. The presence of metabolic biotransformation products of OC, 4-BenzPh, BPA and HO in wastewater provides evidence for internal exposure of studied populations to these chemicals.
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http://dx.doi.org/10.1016/j.watres.2018.06.028DOI Listing
October 2018

Wastewater Analysis for Community-Wide Drugs Use Assessment.

Handb Exp Pharmacol 2018;252:543-566

Department of Chemistry, University of Bath, Bath, UK.

Wastewater-based epidemiology (WBE) complements existing epidemiology-based 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).
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http://dx.doi.org/10.1007/164_2018_111DOI Listing
June 2019

Enantioselective fractionation of fluoroquinolones in the aqueous environment using chiral liquid chromatography coupled with tandem mass spectrometry.

Chemosphere 2018 Sep 4;206:376-386. Epub 2018 May 4.

Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY, United Kingdom. Electronic address:

This paper aims to examine the multiresidue enantiomeric profiling of (fluoro)quinolones and their metabolites in solid and liquid environmental matrices using chiral HPLC-MS/MS method and a CHIRALCEL OZ-RH column. Simultaneous chiral separation was obtained for chiral ofloxacin and its main metabolites ofloxacin-N-oxide and desmethyl-ofloxacin; moxifloxacin; the prodrug prulifloxacin and its active compound ulifloxacin; flumequine; nadifloxacin and R-(+)-besifloxacin. Achiral antibiotics (ciprofloxacin, norfloxacin and nalidixic acid) were also included in the method to enable the analysis of all targeted quinolones within one analytical run. Satisfactory enantiomeric resolution (Rs ≥ 1) was obtained for five out of eight chiral drugs enabling quantitative analysis. The overall performance of the method was satisfactory with a method precision <20%, relative recoveries >70% for most of the analytes and method detection limits (MDL) at low ng L levels (0.1 < MDL (ng L)< 6.4, 0.1 < MDL (ng L)< 6.6 and 0.1 < MDL (ng L)< 7.0 in influent, effluent and river waters for 83% compounds, 0.01 < MDL (ng g)< 4.9 in solids for 91% compounds). Enantiomeric profiling from a week-long monitoring campaign in the UK showed that (±)-ofloxacin was found to be racemic in upstream waters but it was enriched with S-(-)-enantiomer in wastewater and in receiving waters. This could be due to the fact that ofloxacin can be used both as a racemate and as a S-(-)-enantiomer. Its consumption was further confirmed by the chiral signature of the investigated ofloxacin metabolites. As a result, alterations in the enantiomeric composition of antibiotics could influence not only their activity and toxicity in the environment, but also could induce changes in the microbial communities constantly exposed to them.
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http://dx.doi.org/10.1016/j.chemosphere.2018.05.005DOI Listing
September 2018

Comparison of phosphodiesterase type V inhibitors use in eight European cities through analysis of urban wastewater.

Environ Int 2018 06 3;115:279-284. Epub 2018 Apr 3.

KWR Watercycle Research Institute, Chemical Water Quality and Health, P.O. Box 1072, 3430 BB Nieuwegein, The Netherlands; Institute for Biodiversity and Ecosystem Dynamics, University of Amsterdam, P.O. Box 94248, 1090 GE Amsterdam, The Netherlands. Electronic address:

In this work a step forward in investigating the use of prescription drugs, namely erectile dysfunction products, at European level was taken by applying the wastewater-based epidemiology approach. 24-h composite samples of untreated wastewater were collected at the entrance of eight wastewater treatment plants serving the catchment within the cities of Bristol, Brussels, Castellón, Copenhagen, Milan, Oslo, Utrecht and Zurich. A validated analytical procedure with direct injection of filtered aliquots by liquid chromatography-tandem mass spectrometry was applied. The target list included the three active pharmaceutical ingredients (sildenafil, tadalafil and vardenafil) together with (bio)transformation products and other analogues. Only sildenafil and its two human urinary metabolites desmethyl- and desethylsildenafil were detected in the samples with concentrations reaching 60 ng L. The concentrations were transformed into normalized measured loads and the estimated actual consumption of sildenafil was back-calculated from these loads. In addition, national prescription data from five countries was gathered in the form of the number of prescribed daily doses and transformed into predicted loads for comparison. This comparison resulted in the evidence of a different spatial trend across Europe. In Utrecht and Brussels, prescription data could only partly explain the total amount found in wastewater; whereas in Bristol, the comparison was in agreement; and in Milan and Oslo a lower amount was found in wastewater than expected from the prescription data. This study illustrates the potential of wastewater-based epidemiology to investigate the use of counterfeit medication and rogue online pharmacy sales.
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http://dx.doi.org/10.1016/j.envint.2018.03.039DOI Listing
June 2018

Publisher Correction: A new approach towards biomarker selection in estimation of human exposure to chiral chemicals: a case study of mephedrone.

Sci Rep 2018 Mar 6;8(1):4295. Epub 2018 Mar 6.

Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY, United Kingdom.

A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.
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http://dx.doi.org/10.1038/s41598-018-22367-wDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5840424PMC
March 2018

Biotic phase micropollutant distribution in horizontal sub-surface flow constructed wetlands.

Sci Total Environ 2018 Jul 27;630:648-657. Epub 2018 Feb 27.

Department of Chemistry, University of Bath, Bath BA2 7AY, UK; Water Innovation & Research Centre (WIRC), University of Bath, Bath BA2 7AY, UK. Electronic address:

The distribution of micropollutants in biotic phases of horizontal sub-surface flow (HSSF) constructed wetlands was investigated. 88 diverse micropollutants (personal care products, pharmaceuticals and illicit drugs) were monitored for in full-scale HSSF steel slag and gravel beds to assess their fate and behaviour during tertiary wastewater treatment. Of the studied micropollutants 54 were found in receiving and treated wastewaters. Treatment reduced concentrations of several micropollutants by >50% (removal range -112% to 98%) and resulted in changes to the stereo-isomeric composition of chiral species. For example, stereo-selective changes were observed for 3,4-methylenedioxymethamphetamine (MDMA) and atenolol during HSSF constructed wetland treatment for the first time. Analysis of sludge present within the HSSF beds found 37 micropollutants to be present. However, concentrations for the majority of these micropollutants were not considered high enough to suggest partitioning into sludge was a contributing mechanism of removal. Nevertheless the preservative methylparaben was found at 2772mgbed. Its daily removal from wastewater of 3.4mgd indicates partitioning and accumulation in sludge contributes to its removal. Other micropollutants found at high levels in sludge (relative to their overall removals) were the antidepressants sertraline and fluoxetine, and the metabolite desmethylcitalopram. Furthermore, process balances indicated uptake and metabolism by Phragmites australis (Cav.) Trin. ex Steud did not contribute significantly to micropollutant removal. However analysis of plant tissues evidenced uptake, metabolism and accumulation of recalcitrant micropollutants such as ketamine and carbamazepine. It is considered that the rate of uptake was too slow to have a notable impact on removal at the 14h hydraulic retention time. Despite evidence of other removal mechanisms at play (e.g., partitioning into sludge and plant uptake), findings indicate biodegradation is the dominant mechanism of micropollutant removal in HSSF constructed wetlands.
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http://dx.doi.org/10.1016/j.scitotenv.2018.02.242DOI Listing
July 2018