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.

Chair of Urban Water Management Technische Universität Dresden Dresden Germany

Department of Analytical Chemistry Complutense University of Madrid Madrid Spain

Department of Analytical Environmental and Forensic Sciences King's College London London UK

Department of Aquatic Sciences and Assessment Swedish University of Agricultural Sciences Uppsala Sweden

Department of Chemical Engineering McGill University Montreal Quebec Canada

Department of Chemical Engineering University of Bath Bath UK

Department of Chemistry Laboratory of Analytical Chemistry National and Kapodistrian University of Athens Athens Greece

Department of Chemistry University of Bath Bath UK

Department of Coal Chemistry and Environmental Sciences AGH University of Science and Technology Krakow Poland

Department of Environmental Engineering Faculty of Chemical and Food Technology Slovak University of Technology Bratislava Slovakia

Department of Environmental Engineering Technical University of Denmark Kongens Lyngby Denmark

Department of Environmental Sciences Jožef Stefan Institute Ljubljana Slovenia

Department of Pharmaceutical Sciences Toxicological Center Antwerp Belgium

Department of Pharmacology and Toxicology University of Iceland Reykjavík Iceland

Division for Marine and Environmental Research Rudjer Boskovic Institute Zagreb Croatia

Eawag Urban Water Management Swiss Federal Institute of Aquatic Science and Technology Dübendorf Switzerland

Ecole des Sciences Criminelles University of Lausanne Lausanne Switzerland

Environmental Pollution Control Laboratory Chemistry Department Aristotle University of Thessaloniki Thessaloniki Greece

Faculty of Chemical Sciences Department of Analytical Chemistry Nutrition and Bromatology University of Salamanca Salamanca Spain

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

Faculty of Pharmacy University of Lisbon Lisbon Portugal

Faculty of Technical Sciences Department of Environmental Engineering and Occupational Safety University of Novi Sad Novi Sad Serbia

Food and Environmental Safety Research Group University of Valencia Moncada Spain

Forensic Toxicology National Institute for Health and Welfare Helsinki Finland

IBED University of Amsterdam Amsterdam the Netherlands

Institute for Food Analysis and Research Department of Analytical Chemistry Universidade de Santiago de Compostela Santiago de Compostela Spain

Institute of Clinical Pharmacology Technische Universität Dresden Dresden Germany

Institute of Forensic Research Krakow Poland

Institute of Legal Medicine and Core Facility Metabolomics Medical University of Innsbruck Innsbruck Austria

Istituto di Ricerche Farmacologiche Mario Negri IRCCS Milan Italy

King's Forensics School of Population Health and Environmental Sciences King's College London London UK

KWR Water Research Institute Nieuwegein the Netherlands

National Institute of Legal Medicine and Forensic Sciences Lisbon Portugal

NIREAS International Water Research Center Department of Civil and Environmental Engineering University of Cyprus Nicosia Cyprus

Norwegian Institute for Water Research Oslo Norway

Process and Systems Engineering Center Department of Chemical and Biochemical Engineering Technical University of Denmark Kongens Lyngby Denmark

Queensland Alliance for Environmental Health Sciences The University of Queensland Woolloongabba QLD Australia

Research Institute for Pesticides and Water University Jaume 1 Castellón Spain

School of Pharmacy and Medical Sciences University of South Australia Adelaide South Australia Australia

Unit of Environmental Engineering Ben Gurion University of the Negev Beer Sheva Israel

Université Paris Sud CNRS AgroParisTech Université Paris Saclay Chatenay Malabry France

University of Bern Institute of Plant Sciences Bern Switzerland

University of Puget Sound Tacoma WA USA

Water and Soil Quality Research Group Department of Environmental Chemistry Institute of Environmental Assessment and Water Research Barcelona Spain

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