Publications by authors named "Richard Bade"

41 Publications

Pholedrine is a marker of direct disposal of methamphetamine.

Sci Total Environ 2021 Aug 30;782:146839. Epub 2021 Mar 30.

Health and Biomedical Innovation, UniSA: Clinical and Health Sciences, University of South Australia, Adelaide 5001, South Australia, Australia. Electronic address:

Consumption of methamphetamine has primarily been estimated in wastewater-based epidemiology by measuring the parent compound. However, this could lead to overestimation when methamphetamine is directly disposed into the sewer system. In this respect, it would be advantageous to measure a specific metabolite of methamphetamine instead. We identified 4-hydroxymethamphetamine (pholedrine) as a potential marker. Stability experiments were performed in both filtered and unfiltered wastewater. Correlations with relative loads in wastewater were used to establish its potential as a marker of direct disposal of methamphetamine, or even as a wastewater-based epidemiology biomarker of methamphetamine consumption. This study then investigated the use of pholedrine in combination with methamphetamine to better detect direct disposal events and its potential as a marker of methamphetamine consumption. Examples from both South Australia and New Zealand exemplify the use of pholedrine to identify potential instances of direct disposal of methamphetamine.
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http://dx.doi.org/10.1016/j.scitotenv.2021.146839DOI Listing
August 2021

International snapshot of new psychoactive substance use: Case study of eight countries over the 2019/2020 new year period.

Water Res 2021 Apr 3;193:116891. Epub 2021 Feb 3.

Health and Biomedical Innovation, UniSA: Clinical and Health Sciences, University of South Australia, Adelaide 5001, South Australia, Australia. Electronic address:

There is considerable concern around the use of new psychoactive substances (NPS), but still little is known about how much they are really consumed. Analysis by forensics laboratories of seized drugs and post-mortem samples as well as hospital emergency rooms are the first line of identifying both 'new' NPS and those that are most dangerous to the community. However, NPS are not necessarily all seized by law enforcement agencies and only substances that contribute to fatalities or serious afflictions are recorded in post-mortem and emergency room samples. To gain a better insight into which NPS are most prevalent within a community, complementary data sources are required. In this work, influent wastewater was analysed from 14 sites in eight countries for a variety of NPS. All samples were collected over the 2019/2020 New Year period, a time which is characterized by celebrations and parties and therefore a time when more NPS may be consumed. Samples were extracted in the country of origin following a validated protocol and shipped to Australia for final analysis using two different mass spectrometric strategies. In total, more than 200 were monitored of which 16 substances were found, with geographical differences seen. This case study is the most comprehensive wastewater analysis study ever carried out for the identification of NPS and provides a starting point for future, ongoing monitoring of these substances.
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http://dx.doi.org/10.1016/j.watres.2021.116891DOI Listing
April 2021

Application of catecholamine metabolites as endogenous population biomarkers for wastewater-based epidemiology.

Sci Total Environ 2021 Apr 14;763:142992. Epub 2020 Oct 14.

University of South Australia, Clinical and Health Sciences (CHS), Health and Biomedical Innovation, South Australia 5000, Australia. Electronic address:

Wastewater-based epidemiology studies use catchment populations to normalise chemical marker mass loads in 24-h composite wastewater samples. However, one of the biggest uncertainties within the field is the accuracy of the population used. A population marker in wastewater may significantly reduce the uncertainty. This study evaluated the catecholamine metabolites - homovanillic acid (HVA) and vanillylmandelic acid (VMA) - as potential population biomarkers. Influent wastewater 24-h composite samples were collected from 38 wastewater catchments from around Australia (representing ~33% of Australia's population), extracted and analysed by liquid chromatography tandem mass spectrometry. Measured mass loads were compared to population sizes determined by mapping catchment maps against high-resolution census data. Both biomarkers correlated with coefficient of determinations (r) of 0.908 and 0.922 for HVA and VMA, respectively. From the regression analysis, a slope (i.e. the daily per-capita excretion) of 1.241 and 1.067 mg.day.person was obtained for HVA and VMA, respectively. The mass load ratio between VMA:HVA were very similar to that reported in literature for urinary analysis among all catchments. Overall, this study provided further evidence that catecholamine metabolites are suitable candidates as population biomarkers for future studies.
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http://dx.doi.org/10.1016/j.scitotenv.2020.142992DOI Listing
April 2021

How the recreational stimulant market has changed: Case study in Adelaide, Australia 2016-2019.

Sci Total Environ 2021 Feb 24;757:143728. Epub 2020 Nov 24.

University of South Australia, UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, Adelaide 5000, South Australia, Australia. Electronic address:

The human consumption of stimulant drugs is known to increase over festive periods. In this work, four illicit stimulants: 3,4-methylenedioxymethamphetamine (MDMA), 3,4-methylenedioxyamphetamine (MDA), cocaine and methamphetamine and three new psychoactive substances (NPS): ethylone, mephedrone and N-ethylpentylone were monitored in influent wastewater over the Christmas-New Year period in South Australia from 2016 to 2019 using liquid chromatography-mass spectrometry. The differences in Christmas - New Year consumption between years were evaluated and daily mass loads were compared to the average for that year to determine drug levels over the festive period. Although MDMA, MDA and cocaine showed year-on-year increases, the use over the New Year period was far higher than over the rest of the year, consistent with recreational drug use. These were also the drugs that were used predominantly on weekends during the year. Methamphetamine, which does not have a pattern of predominant weekend use, and the NPS showed variable trends. These results suggest that during holiday periods there are increases in the use of a limited set of drugs only and these can be predicted from patterns of use during the non-holiday periods.
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http://dx.doi.org/10.1016/j.scitotenv.2020.143728DOI Listing
February 2021

What is the drug of choice of young festivalgoers?

Drug Alcohol Depend 2020 11 28;216:108315. Epub 2020 Sep 28.

University of South Australia, UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, Adelaide, SA 5000, Australia. Electronic address:

Background: Drug and alcohol consumption are commonplace at festivals including those aimed at younger attendees. However, there is little quantitative information about the extent of this consumption. This work investigates drug use at a school-leaver festival and how it compares to non-festival weeks.

Methods: Influent wastewater was collected over three consecutive weeks from a location where a school-leaver festival occurs. Multiple liquid chromatography-mass spectrometry methods were used to analyse the use of illicit drugs, pharmaceuticals with abuse potential, new psychoactive substances (NPS), alcohol and cannabis. A method for human neurotransmitter metabolites was also utilised to show the population change and allow the drugs found to be normalised to a population.

Results: A total of 12 compounds were quantifiable: methamphetamine, 3,4-methylenedioxyamphetamine (MDA), 3,4-methylenedioxymethamphetamine (MDMA), alcohol, cannabis, cocaine, morphine, codeine, fentanyl, buprenorphine, oxycodone and nicotine. The NPS methylone was found solely over the festival weekend but at levels below the limit of quantification of the analytical method. The catecholamine metabolites vanillylmandelic acid (VMA) and homovanillic acid (HVA) were found over the entire three weeks, with identical trends - an increase over the festival weekend - indicating a population increase. HVA was used to normalise the drug mass loads to derive a population normalised mass load. Statistical differences using Hedges' g showed large changes in the use of MDMA and MDA over the festival week. Smaller increases were also seen for alcohol and cocaine.

Conclusions: The drugs of choice for the attendees of this school-leaver festival were MDMA and MDA.
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http://dx.doi.org/10.1016/j.drugalcdep.2020.108315DOI Listing
November 2020

Amphetamine dependence in Australia.

Lancet 2020 10;396(10256):957

Clinical and Health Sciences, Health and Biomedical Innovation, University of South Australia, Adelaide, SA 5000, Australia.

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http://dx.doi.org/10.1016/S0140-6736(20)32025-0DOI Listing
October 2020

Changes in alcohol consumption associated with social distancing and self-isolation policies triggered by COVID-19 in South Australia: a wastewater analysis study.

Addiction 2021 06 1;116(6):1600-1605. Epub 2020 Oct 1.

Clinical and Health Sciences, Health and Biomedical Innovation, University of South Australia, Adelaide, Australia.

Aim: To assess the effects of social distancing and social isolation policies triggered by COVID-19 on alcohol consumption using wastewater analysis in Adelaide, South Australia.

Design: Longitudinal quantitative analysis of influent wastewater data for alcohol concentration.

Setting: Adelaide, South Australia.

Participants: Wastewater catchment area representative of 1.1 million inhabitants.

Measurements: Twenty-four hour composite influent wastewater samples were collected from four wastewater treatment plants in Adelaide, South Australia for 7 consecutive days (Wednesday-Tuesday) every 2 months from April 2016-April 2020. The alcohol metabolite ethyl sulfate was measured in samples using chromatography-tandem mass spectrometry. Data were population-weighted adjusted with consumption expressed as standard drinks/day/1000 people. Weekly consumption and weekend to mid-week consumption ratios were analysed to identify changes in weekday alcohol use pattern.

Findings: Estimated weekend alcohol consumption was significantly lower (698 standard drinks/day/1000 people) after self-isolation measures were enforced in April 2020 compared with the preceding sampling period in February 2020 (1047 standard drinks/day/1000 people), P < 0.05. Weekend to midweek consumption ratio was 12% lower than the average ratio compared with all previous sampling periods. April 2020 recorded the lowest alcohol consumption relative to April in previous years, dating back to 2016.

Conclusions: Wastewater analysis suggests that introduction of social distancing and isolation policies triggered by COVID-19 in Adelaide, South Australia, was associated with a decrease in population-level weekend alcohol consumption.
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http://dx.doi.org/10.1111/add.15256DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7537161PMC
June 2021

Determination of prescribed and designer benzodiazepines and metabolites in influent wastewater.

Anal Methods 2020 07 6;12(28):3637-3644. Epub 2020 Jul 6.

University of South Australia, UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, Adelaide 5000, South Australia, Australia.

Benzodiazepines are important prescription pharmaceuticals used to help in the treatment of anxiety and sleep disorders. However, they also have a strong potential for abuse. In this respect, illicit benzodiazepines, i.e. not prescribed in Australia and designer benzodiazepines, which are new compounds that are not legally prescribed in any jurisdiction, have emerged in the illicit Australian market in recent years. Designer benzodiazepines are a new class of new psychoactive substances (NPS) and are particularly dangerous due to limited toxicity information and propensity to be mistaken for conventional benzodiazepines, leading to severe side effects and potentially death. It is therefore important to assess the prevalence of the use of these compounds in the community. The current work presents a validated liquid chromatography-mass spectrometry method for 20 prescribed and designer benzodiazepines and metabolites: 7-amino nimetazepam, alpha-hydroxy alprazolam, alprazolam, clonazepam, delorazepam, deschloroetizolam, diazepam, diclazepam, etizolam, flubromazepam, flunitrazepam, lorazepam, lormetazepam, meclonazepam, midazolam, nimetazepam, nitrazepam, oxazepam, pyrazolam and temazepam. Quetiapine, a prescription sedative drug that has been diverted for non-medical use, was also validated. Limits of quantification were predominantly below 10 ng L, except for the ubiquitous oxazepam, quetiapine and temazepam, which were between 75-300 ng L. Stability, recovery and matrix effects were also examined. Finally, this method was applied to influent wastewater from South Australia, which showed the presence of many benzodiazepines including the NPS etizolam.
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http://dx.doi.org/10.1039/d0ay00560fDOI Listing
July 2020

The complexities associated with new psychoactive substances in influent wastewater: The case of 4-ethylmethcathinone.

Drug Test Anal 2020 Oct 20;12(10):1494-1500. Epub 2020 Jul 20.

UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, University of South Australia, Adelaide, South Australia, Australia.

Consumption of new psychoactive substances (NPS) is an international problem for health, policing, forensic, and analytical laboratories. The transience of these substances in the community, combined with continual slight structural changes to evade legislation makes the elucidation of NPS an analytical challenge. This is amplified in a matrix as complex as wastewater. For that reason, suspect and non-target methodologies, employing high resolution mass spectrometry are the most appropriate current tool to facilitate the identification of new and existing compounds. In the current work, a qualitative screening method of influent wastewater using liquid chromatography-high resolution mass spectrometry showed a strong signal at m/z 192.1382 - identical to that of two NPS standards that were in our method (pentedrone and 4-methylethcathinone), and with identical fragment ions, but the retention times did not match. This work shows the methodology followed to identify this compound, highlighting the challenges of the identifying "new" compounds in influent wastewater.
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http://dx.doi.org/10.1002/dta.2890DOI Listing
October 2020

Anabasine-based measurement of cigarette consumption using wastewater analysis.

Drug Test Anal 2020 Sep 26;12(9):1393-1398. Epub 2020 Jun 26.

UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, University of South Australia, South Australia, Australia.

Community tobacco use can be monitored over time using wastewater-based epidemiological approaches by estimating the mass loads of nicotine and its metabolites, cotinine, or hydroxycotinine, in wastewater. However, due to the use of nicotine in smoking cessation products, other sources of nicotine contribute to cotinine and hydroxycotinine loads. The use of nicotine replacement therapies could vary in space and time and mask the true rates of tobacco consumption. Therefore, this work evaluated the content of tobacco specific markers, anatabine and anabasine, in cigarettes, in urine of smokers, and in wastewater. The results indicated that the anabasine content in both licit and illicit cigarettes in Australia is less variable than anatabine and is therefore considered a better measure of tobacco consumption. A study determining the excretion of tobacco-specific alkaloids of smoking and non-smoking volunteers gave an average urinary mass load of anabasine of 4.38 μg/L/person and a daily mass load of 1.13 μg/day/person. Finally, this was compared with the mass loads of anabasine from wastewater-based epidemiology data of 3 μg/day/person to estimate cigarette rates in a South Australian city: equivalent to 2.6 cigarettes/person/day. The rate of decline of cigarette use was greater when using anabasine as a measure of consumption compared with cotinine. This is the first study to estimate the rate of anabasine excretion, which can be used to estimate tobacco use independent of therapeutically prescribed nicotine.
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http://dx.doi.org/10.1002/dta.2874DOI Listing
September 2020

Towards an efficient method for the extraction and analysis of cannabinoids in wastewater.

Talanta 2020 Sep 18;217:121034. Epub 2020 Apr 18.

Health and Biomedical Innovation, UniSA: Clinical and Health Sciences, University of South Australia, Adelaide, 5001, Australia. Electronic address:

Owing to the risks and dangers of xenobiotic cannabinoids (phyto and synthetic), studies are required to evaluate community consumption. The analysis of excreted cannabinoids in wastewater can provide information about community consumption for a defined catchment area. The recovery of cannabinoids from complex wastewater matrices is difficult due to the hydrophobic properties of these compounds. In this study, a liquid chromatography tandem mass spectrometry (LC-MS/MS) method was optimised for the recovery of 30 cannabinoids from wastewater, including the cannabis urinary biomarker 11-nor-9-carboxy-Δ-tetrahydrocannabinol (THC-COOH), cannabidiol (CBD), and a variety of different generational synthetic cannabinoids and metabolites. Method validation assessed criteria including linearity, selectivity, recovery, ion-suppression, filtration losses and matrix effect. Two sample preparation approaches-liquid-liquid extraction (LLE) and solid phase extraction (SPE)-were compared, with comparable limits of quantification between 0.001 and 0.5 µg L in wastewater. Filtration was found to reduce the recovery for many of the investigated cannabinoids, where up to 97% of analyte was lost. The method was applied to 15 different catchment areas across Australia to gauge the community use of the cannabinoids in this study. The cannabis biomarker THC-COOH was quantified at all locations, and cannabidiol was measured at eight catchment areas. Three synthetic cannabinoids were detected at the limit of detection: 5-fluoro APINACA, JWH-073 (4-hydroxypentyl), and MDMB-CHMICA.
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http://dx.doi.org/10.1016/j.talanta.2020.121034DOI Listing
September 2020

Determining changes in new psychoactive substance use in Australia by wastewater analysis.

Sci Total Environ 2020 Aug 7;731:139209. Epub 2020 May 7.

University of South Australia, UniSA: Clinical and Health Sciences, Health and Biomedical Innovation, Adelaide 5000, South Australia, Australia. Electronic address:

Measuring community consumption of new psychoactive substances (NPS) is notoriously difficult to assess by traditional means such as surveys and seizure data. Previously, we used the approach to demonstrate the prevalence of NPS on a national scale. In the current study we explored the temporal resolution for the analysis of NPS in wastewater from Australia. Samples covering all States and Territories in Australia and both metropolitan and regional areas and were collected bimonthly from October 2017-June 2018 and October 2019-February 2020. A qualitative screening method was applied, screening for 201 NPS. In total, 15 substances were found from a variety of classes of NPS. The most prevalent class was synthetic cathinones, with pentylone, N-ethylpentylone and ethylone found in all periods in at least one site in the earlier sampling period, as well as the amphetamine-like paramethoxyamphetamine (PMA). In the latter period, synthetic cathinones were also the most prevalent, including eutylone, marking the first time that this compound has been detected in wastewater. This study shows the application of wastewater analysis to detect outbreaks of NPS use and temporal differences among sites.
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http://dx.doi.org/10.1016/j.scitotenv.2020.139209DOI Listing
August 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

Determination of 21 synthetic cathinones, phenethylamines, amphetamines and opioids in influent wastewater using liquid chromatography coupled to tandem mass spectrometry.

Talanta 2020 Feb 18;208:120479. Epub 2019 Oct 18.

School of Pharmacy and Medical Sciences, University of South Australia, Adelaide, South Australia, 5000, Australia. Electronic address:

Human consumption of illicit novel psychoactive substances (NPS) is a continuing problem. New derivatives are constantly appearing, circumventing national and international laws. The use of these compounds tend to be sporadic and many are consumed as mixtures, meaning very low amounts of each are detectable at any one time. The analysis of excreted NPS in wastewater provides information on community prevalence. A wastewater-based epidemiology approach has been applied in the current study for the quantification of 21 NPS. These include three phenethylamines (25B-NBOMe, 25C-NBOMe, 25I-NBOMe), ten synthetic cathinones (3-ethylmethcathinone (3-EMC), 3-methylbuphedrone, 3-methylmethcathinone (3-MMC), 4-fluoromethcathinone (4-FMC), 4-methylbuphedrone, 4-methylethcathinone (4-MEC), buphedrone, butylone, N-ethylpentylone and pentylone), five synthetic opioid analgesics (AH-7921, butyryl fentanyl, furanyl fentanyl, U-47700 and valeryl fentanyl) as well as the synthetic amphetamine 4-fluoroamphemtaine (4-FA), ketamine analogue methoxetamine and methiopropamine. Limits of detection were between 0.01 and 0.5 ng/L and limits of quantification were between 0.05 and 1 ng/L. The method was applied to wastewater samples from South Australia collected over the Christmas-New Year period when recreational drug use tends to be high. Seven NPS (butylone, butyryl fentanyl, furanyl fentanyl, methoxetamine, N-ethylpentylone, pentylone and valeryl fentanyl) were found, with N-ethylpentylone showing the highest mass loads at 36 mg/day/1000 inhabitants.
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http://dx.doi.org/10.1016/j.talanta.2019.120479DOI Listing
February 2020

A sensitive analytical method for the measurement of neurotransmitter metabolites as potential population biomarkers in wastewater.

J Chromatogr A 2020 Feb 14;1612:460623. Epub 2019 Oct 14.

School of Pharmacy and Medical Sciences, University of South Australia, Adelaide, South Australia 5000, Australia.

Wastewater-based epidemiology is a growing research field which provides valuable information on community drug use and chemical exposure. One parameter critical to estimations of drug use is the catchment area population. A population biomarker could be used to provide this information. This study evaluated the analytical suitability of three endogenous biomarkers of human activity: the serotonin metabolite 5-hydroxyindoleacetic acid (5-HIAA) which has previously been proposed and two further candidates, the catecholamine metabolites vanillylmandelic acid (VMA) and homovanillic acid (HVA). An analytical method involving derivatization was developed and validated for two candidates, 5-HIAA and HVA by liquid chromatography - mass spectrometry. The best performance was obtained for VMA as the underivatized analyte. The derivatized extracts produced a 100 times better sensitivity. The three neurotransmitter metabolites were evaluated as population biomarkers in wastewater samples. All were stable in sample, not lost upon filtration and showed stable inter-day mass loads over seven days for a metropolitan wastewater treatment plant. When applied to a small community during a festival period, mass loads of both HVA and VMA reflected the increase in the catchment population, whilst 5-HIAA proved to be more variable.
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http://dx.doi.org/10.1016/j.chroma.2019.460623DOI Listing
February 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

Harnessing the Power of the Census: Characterizing Wastewater Treatment Plant Catchment Populations for Wastewater-Based Epidemiology.

Environ Sci Technol 2019 Sep 22;53(17):10303-10311. Epub 2019 Aug 22.

Queensland Alliance for Environmental Health Science , The University of Queensland , 20 Cornwall Street , Woolloongabba , Queensland 4102 , Australia.

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.
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http://dx.doi.org/10.1021/acs.est.9b03447DOI Listing
September 2019

Simultaneous determination of 24 opioids, stimulants and new psychoactive substances in wastewater.

MethodsX 2019 19;6:953-960. Epub 2019 Apr 19.

School of Pharmacy and Medical Sciences, University of South Australia, Adelaide, South Australia, 5000, Australia.

Wastewater-based epidemiology has become a reputable means to estimate drug consumption within a community. However, these methods typically focus solely on illicit drugs or a single chemical family, with multi-class methods out of favour due to the increased analytical challenges. •A sensitive liquid chromatography - mass spectrometry method was developed for the simultaneous determination of 24 opioids, stimulants and new psychoactive substances in influent wastewater.•Filtered wastewater samples, preserved with sodium metabisulfite, were pretreated and 1000 times concentrated using off-line solid phase extraction.•The method was optimised and fully validated for all compounds, with limits of quantification between 0.2 and 300 ng/L.
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http://dx.doi.org/10.1016/j.mex.2019.04.016DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6500910PMC
April 2019

LC-HRMS suspect screening to show spatial patterns of New Psychoactive Substances use in Australia.

Sci Total Environ 2019 Feb 28;650(Pt 2):2181-2187. Epub 2018 Sep 28.

School of Pharmacy and Medical Sciences, University of South Australia, Adelaide 5001, Australia. Electronic address:

New Psychoactive Substances (NPS) are an ever-changing class of compounds designed to imitate the effects of current recreational drugs. Such a diverse market is difficult to assess by traditional means, while collected information can become obsolete before it is available. Wastewater-based epidemiology is one technique which can capture information on where and when NPS appear at the community level. The aim of this study was to identify NPS in wastewater samples using a suspect screening approach. Weekend samples were collected from 50 wastewater treatment plants from Australian capital cities and regional areas across all eight States and Territories and screened against a database containing almost 200 NPS. A total of 22 different NPS were found across all regional and metropolitan wastewater treatment plants. Results showed that the most detected compounds were of the cathinone class, with both Alpha-PVP and methcathinone found in every region. In addition, five different synthetic cannabinoids were detected, at least once in half of the regions analysed. Herein, we report the first comprehensive nationwide analysis of NPS and show the utility of liquid chromatography-high resolution mass spectrometry screening for delivering spatial information of the NPS being consumed in communities.
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http://dx.doi.org/10.1016/j.scitotenv.2018.09.348DOI Listing
February 2019

Investigating the appearance of new psychoactive substances in South Australia using wastewater and forensic data.

Drug Test Anal 2019 Feb 12;11(2):250-256. Epub 2018 Sep 12.

School of Pharmacy and Medical Sciences, University of South Australia, Adelaide, 5001, Australia.

New psychoactive substances (NPS) have increased in use and popularity worldwide. Wastewater analysis has been successfully applied to evaluate illicit drugs use within a population. However, for NPS, such an approach may be limited due to low doses of NPS combined with their ever-changing composition and usage. The dynamic nature of the NPS market means use may be opportunistic, infrequent, and with few users. Hence, the use of complementary information sources is recommended to improve the knowledge on NPS consumption. The aim of this study was to investigate the changing landscape of NPS use on a community scale by combining wastewater analysis and forensic toxicology. Forensic analysis provided specific information on NPS prevalence in post-mortem blood samples in Adelaide, South Australia over five years, while wastewater analysis showed community use over the same period. A qualitative liquid chromatography--high resolution mass spectrometry method was initially used to screen the wastewater samples. A total of 24 NPS were found: 6 in wastewater only, 13 in forensic post-mortem toxicology samples only, and 5 in both. As these results showed the presence of NPS, a targeted method was subsequently employed to quantify levels of these NPS in wastewater. Temporal trends were found in wastewater with distinct tendencies for synthetic cathinones visible over the period studied.
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http://dx.doi.org/10.1002/dta.2484DOI Listing
February 2019

Investigating the correlation between wastewater analysis and roadside drug testing in South Australia.

Drug Alcohol Depend 2018 06 10;187:123-126. Epub 2018 Apr 10.

School of Pharmacy and Medical Sciences, University of South Australia, GPO Box 2471, Adelaide, SA 5001, Australia. Electronic address:

Background: The societal impact of drug use is well known. An example is when drug-intoxicated drivers increase the burden on policing and healthcare services.

Methods: This work presents the correlation of wastewater analysis (using UHPLC-MS/MS) and positive roadside drug testing results for methamphetamine, 3,4-methylenedioxymethamphetamine (MDMA) and cannabis from December 2011-December 2016 in South Australia.

Results: Methamphetamine and MDMA showed similar trends between the data sources with matching increases and decreases, respectively. Cannabis was relatively steady based on wastewater analysis, but the roadside drug testing data started to diverge in the final part of the measurement period.

Conclusions: The ability to triangulate data as shown here validates both wastewater analysis and roadside drug testing. This suggests that changes in overall population drug use revealed by WWA is consistent and proportional with changes in drug-driving behaviours. The results show that, at higher levels of drug use as measured by wastewater analysis, there is an increase in drug driving in the community and therefore more strain on health services and police.
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http://dx.doi.org/10.1016/j.drugalcdep.2018.02.030DOI Listing
June 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

Enantiomeric profiling of chiral illicit drugs in a pan-European study.

Water Res 2018 03 1;130:151-160. Epub 2017 Dec 1.

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

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 day. 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.
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http://dx.doi.org/10.1016/j.watres.2017.11.051DOI Listing
March 2018

Qualitative and quantitative temporal analysis of licit and illicit drugs in wastewater in Australia using liquid chromatography coupled to mass spectrometry.

Anal Bioanal Chem 2018 Jan 6;410(2):529-542. Epub 2017 Dec 6.

School of Pharmacy and Medical Sciences, University of South Australia, GPO Box 2471, Adelaide, South Australia, 5001, Australia.

The combination of qualitative and quantitative bimonthly analysis of pharmaceuticals and illicit drugs using liquid chromatography coupled to mass spectrometry is presented. A liquid chromatography-quadrupole time of flight instrument equipped with Sequential Window Acquisition of all THeoretical fragment-ion spectra (SWATH) was used to qualitatively screen 346 compounds in influent wastewater from two wastewater treatment plants in South Australia over a 14-month period. A total of 100 compounds were confirmed and/or detected using this strategy, with 61 confirmed in all samples including antidepressants (amitriptyline, dothiepin, doxepin), antipsychotics (amisulpride, clozapine), illicit drugs (cocaine, methamphetamine, amphetamine, 3,4-methylenedioxymethamphetamine (MDMA)), and known drug adulterants (lidocaine and tetramisole). A subset of these compounds was also included in a quantitative method, analyzed on a liquid chromatography-triple quadrupole mass spectrometer. The use of illicit stimulants (methamphetamine) showed a clear decrease, levels of opioid analgesics (morphine and methadone) remained relatively stable, while the use of new psychoactive substances (methylenedioxypyrovalerone (MDPV) and Alpha PVP) varied with no visible trend. This work demonstrates the value that high-frequency sampling combined with quantitative and qualitative analysis can deliver. Graphical abstract Temporal analysis of licit and illicit drugs in South Australia.
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http://dx.doi.org/10.1007/s00216-017-0747-2DOI Listing
January 2018

Estimation of caffeine intake from analysis of caffeine metabolites in wastewater.

Sci Total Environ 2017 Dec 8;609:1582-1588. Epub 2017 Aug 8.

IRCCS - Istituto di Ricerche Farmacologiche "Mario Negri", Department of Environmental Health Sciences, Via La Masa 19, 20156 Milan, Italy. Electronic address:

Caffeine metabolites in wastewater were investigated as potential biomarkers for assessing caffeine intake in a population. The main human urinary metabolites of caffeine were measured in the urban wastewater of ten European cities and the metabolic profiles in wastewater were compared with the human urinary excretion profile. A good match was found for 1,7-dimethyluric acid, an exclusive caffeine metabolite, suggesting that might be a suitable biomarker in wastewater for assessing population-level caffeine consumption. A correction factor was developed considering the percentage of excretion of this metabolite in humans, according to published pharmacokinetic studies. Daily caffeine intake estimated from wastewater analysis was compared with the average daily intake calculated from the average amount of coffee consumed by country per capita. Good agreement was found in some cities but further information is needed to standardize this approach. Wastewater analysis proved useful to providing additional local information on caffeine use.
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http://dx.doi.org/10.1016/j.scitotenv.2017.07.258DOI Listing
December 2017

Wastewater-based epidemiology to assess pan-European pesticide exposure.

Water Res 2017 09 21;121:270-279. Epub 2017 May 21.

IRCCS - Istituto di Ricerche Farmacologiche "Mario Negri", Department of Environmental Health Sciences, Via La Masa 19, 20156, Milan, Italy. Electronic address:

Human biomonitoring, i.e. the determination of chemicals and/or their metabolites in human specimens, is the most common and potent tool for assessing human exposure to pesticides, but it suffers from limitations such as high costs and biases in sampling. Wastewater-based epidemiology (WBE) is an innovative approach based on the chemical analysis of specific human metabolic excretion products (biomarkers) in wastewater, and provides objective and real-time information on xenobiotics directly or indirectly ingested by a population. This study applied the WBE approach for the first time to evaluate human exposure to pesticides in eight cities across Europe. 24 h-composite wastewater samples were collected from the main wastewater treatment plants and analyzed for urinary metabolites of three classes of pesticides, namely triazines, organophosphates and pyrethroids, by liquid chromatography-tandem mass spectrometry. The mass loads (mg/day/1000 inhabitants) were highest for organophosphates and lowest for triazines. Different patterns were observed among the cities and for the various classes of pesticides. Population weighted loads of specific biomarkers indicated higher exposure in Castellon, Milan, Copenhagen and Bristol for pyrethroids, and in Castellon, Bristol and Zurich for organophosphates. The lowest mass loads (mg/day/1000 inhabitants) were found in Utrecht and Oslo. These results were in agreement with several national statistics related to pesticides exposure such as pesticides sales. The daily intake of pyrethroids was estimated in each city and it was found to exceed the acceptable daily intake (ADI) only in one city (Castellon, Spain). This was the first large-scale application of WBE to monitor population exposure to pesticides. The results indicated that WBE can give new information about the "average exposure" of the population to pesticides, and is a useful complementary biomonitoring tool to study population-wide exposure to pesticides.
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http://dx.doi.org/10.1016/j.watres.2017.05.044DOI Listing
September 2017

Prediction of Collision Cross-Section Values for Small Molecules: Application to Pesticide Residue Analysis.

Anal Chem 2017 06 7;89(12):6583-6589. Epub 2017 Jun 7.

Research Institute for Pesticides and Water, University Jaume I , Avda. Sos Baynat s/n, E-12071 Castellón, Spain.

The use of collision cross-section (CCS) values obtained by ion mobility high-resolution mass spectrometry has added a third dimension (alongside retention time and exact mass) to aid in the identification of compounds. However, its utility is limited by the number of experimental CCS values currently available. This work demonstrates the potential of artificial neural networks (ANNs) for the prediction of CCS values of pesticides. The predictor, based on eight software-chosen molecular descriptors, was optimized using CCS values of 205 small molecules and validated using a set of 131 pesticides. The relative error was within 6% for 95% of all CCS values for protonated molecules, resulting in a median relative error less than 2%. In order to demonstrate the potential of CCS prediction, the strategy was applied to spinach samples. It notably improved the confidence in the tentative identification of suspect and nontarget pesticides.
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http://dx.doi.org/10.1021/acs.analchem.7b00741DOI Listing
June 2017

Monitoring a large number of pesticides and transformation products in water samples from Spain and Italy.

Environ Res 2017 07 14;156:31-38. Epub 2017 Mar 14.

RCCS - Istituto di Ricerche Farmacologiche "Mario Negri", Environmental Biomarkers Unit, Food Toxicology Laboratory, Department of Environmental Health Sciences, Via La Masa 19, 20156 Milan, Italy. Electronic address:

Assessing the presence of pesticides in environmental waters is particularly challenging because of the huge number of substances used which may end up in the environment. Furthermore, the occurrence of pesticide transformation products (TPs) and/or metabolites makes this task even harder. Most studies dealing with the determination of pesticides in water include only a small number of analytes and in many cases no TPs. The present study applied a screening method for the determination of a large number of pesticides and TPs in wastewater (WW) and surface water (SW) from Spain and Italy. Liquid chromatography coupled to high-resolution mass spectrometry (HRMS) was used to screen a database of 450 pesticides and TPs. Detection and identification were based on specific criteria, i.e. mass accuracy, fragmentation, and comparison of retention times when reference standards were available, or a retention time prediction model when standards were not available. Seventeen pesticides and TPs from different classes (fungicides, herbicides and insecticides) were found in WW in Italy and Spain, and twelve in SW. Generally, in both countries more compounds were detected in effluent WW than in influent WW, and in SW than WW. This might be due to the analytical sensitivity in the different matrices, but also to the presence of multiple sources of pollution. HRMS proved a good screening tool to determine a large number of substances in water and identify some priority compounds for further quantitative analysis.
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http://dx.doi.org/10.1016/j.envres.2017.03.013DOI Listing
July 2017

Measuring biomarkers in wastewater as a new source of epidemiological information: Current state and future perspectives.

Environ Int 2017 Feb 27;99:131-150. Epub 2016 Dec 27.

Research Institute for Pesticides and Water, Universitat Jaume I, Castellon, Spain. Electronic address:

The information obtained from the chemical analysis of specific human excretion products (biomarkers) in urban wastewater can be used to estimate the exposure or consumption of the population under investigation to a defined substance. A proper biomarker can provide relevant information about lifestyle habits, health and wellbeing, but its selection is not an easy task as it should fulfil several specific requirements in order to be successfully employed. This paper aims to summarize the current knowledge related to the most relevant biomarkers used so far. In addition, some potential wastewater biomarkers that could be used for future applications were evaluated. For this purpose, representative chemical classes have been chosen and grouped in four main categories: (i) those that provide estimates of lifestyle factors and substance use, (ii) those used to estimate the exposure to toxicants present in the environment and food, (iii) those that have the potential to provide information about public health and illness and (iv) those used to estimate the population size. To facilitate the evaluation of the eligibility of a compound as a biomarker, information, when available, on stability in urine and wastewater and pharmacokinetic data (i.e. metabolism and urinary excretion profile) has been reviewed. Finally, several needs and recommendations for future research are proposed.
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http://dx.doi.org/10.1016/j.envint.2016.12.016DOI Listing
February 2017