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

The first comprehensive assessment of 34 solid phase extraction sorbents is presented for organic explosive residues in wastewater prior to analysis with liquid chromatography-high resolution accurate mass spectrometry (LC-HRMS). A total of 18 explosives were selected including nitramines, nitrate esters, nitroaromatics and organic peroxides. Three polymeric divinylbenzene-based sorbents were found to be most suitable and one co-polymerised with n-vinyl pyrrolidone offered satisfactory recoveries for 14 compounds in fortified wastewater (77-124%). Limits of detection in matrix ranged from 0.026-23μgL-1 with R2≥0.98 for most compounds. The method was applied to eight 24-h composite wastewater samples from a London wastewater works and one compound, 2,4-dinitrotoluene, was determined over five days between 332 and 468g day-1 (225-303ngL-1). To further exploit the suspect screening capability, 17 additional explosives, precursors and transformation products were screened in spiked wastewater samples. Of these, 14 were detected with recoveries from 62 to 92%, highlighting the broad applicability of the method. To our knowledge, this represents the first screen of explosives-related compounds in wastewater from a major European city. This method also allows post-analysis detection of new or emerging compounds using full-scan HRMS datasets to potentially identify and locate illegal manufacture of explosives via wastewater analysis.

The development, characterisation and application of a new analytical method for multi-residue PPCP determination in the freshwater amphipod, Gammarus pulex are presented. Analysis was performed using pulverised liquid extraction (PuLE), solid phase extraction (SPE) and liquid chromatography-tandem mass spectrometry (LC-MS/MS). Qualitative method performance offered excellent limits of detection at <20 ng g(-1) for 18 out of 29 compounds. For quantitative application, linearity and precision were considered acceptable for 10 compounds across the ng-μg g(-1) range (R2≥0.99; ≤20% relative standard deviation respectively). The method was applied to the analysis of G. pulex and river water sourced from six tributaries of the River Thames. Carbamazepine, diazepam, nimesulide, trimethoprim and warfarin were determined in G. pulex samples at low ng g(-1) (dry weight) concentrations across these sites. Temazepam and diclofenac were also detected, but were not quantifiable. Six pharmaceuticals were quantified in surface waters across the eight sites at concentrations ranging from 3 to 344 ng L(-1). The possibility for confirmatory detection and subsequent quantification of pharmaceutical residues in benthic organisms such as G. pulex will enable further understanding on the susceptibility and ecological effects of PPCPs in the aquatic environment.