Refining the estimation of illicit drug consumptions from wastewater analysis: co-analysis of prescription pharmaceuticals and uncertainty assessment.

Wastewater analysis is a promising monitoring tool to estimate illicit drug consumption at the community level. The advantage of this technique over traditional surveys and other surveillance methods has been emphasized in recent studies. However, there are methodological challenges that can affect reliability. The objectives of this study were to systematically reduce and assess uncertainties associated with sampling (through a stringent optimization of the sampling method) and the back calculation of per capita drug consumption (through a refined estimation of the number of people actively contributing to the wastewater in a given period). We applied continuous flow-proportional sampling to ensure the collection of representative raw wastewater samples. Residues of illicit drugs, opioids, prescription pharmaceuticals and one artificial sweetener were analyzed by liquid chromatography coupled with tandem mass spectrometry. A parameter estimating the number of people actively contributing to wastewater over a given period was calculated from the measured loads of prescription pharmaceuticals, their annual consumption and relative excretion data. For the calculation of substance loads in sewage, uncertainties were propagated considering five individual components: sampling, chemical analysis, flow measurements, excretion rates and the number of people contributing to the wastewater. The daily consumption per 1000 inhabitants was estimated to be almost 1000 mg for cannabis and several hundred mg for cocaine, methamphetamine and ecstasy. With the best sampling practice and current chemical analysis, we calculated the remaining uncertainty to be in the range of 20-30% (relative standard deviation, RSD) for the estimation of consumed drug masses in the catchment; RSDs for the per capita consumption were lower (14-24%), as one of the biggest uncertainty components (i.e. error in flow measurements) cancels out in the proposed method for the estimation of the number of people contributing to the daily wastewater volume. In this study, we provide methodological improvements that substantially enhance the reliability of the estimation method--a prerequisite for the application of this technique to meaningfully assess changes in drug consumption and the success of drug intervention strategies in future studies.

[1]  Christian G. Daughton,et al.  Pharmaceuticals and Care Products in the Environment: Scientific and Regulatory Issues , 2001 .

[2]  Franjo Grotenhermen,et al.  Pharmacokinetics and Pharmacodynamics of Cannabinoids , 2003, Clinical pharmacokinetics.

[3]  D. Barceló,et al.  Drugs of abuse and their metabolites in the Ebro River basin: occurrence in sewage and surface water, sewage treatment plants removal efficiency, and collective drug usage estimation. , 2010, Environment international.

[4]  Chris Kostakis,et al.  Population drug use in Australia: a wastewater analysis. , 2011, Forensic science international.

[5]  Paul Griffiths,et al.  The monitoring of drug trends in Australia. , 2003, Drug and alcohol review.

[6]  Christian G. Daughton,et al.  Pharmaceuticals and Personal Care Products in the Environment: Overarching Issues and Overview , 2001 .

[7]  Ettore Zuccato,et al.  Estimating Community Drug Abuse by Wastewater Analysis , 2008, Environmental health perspectives.

[8]  C. Banta-Green,et al.  Eliminating solid phase extraction with large-volume injection LC/MS/MS: analysis of illicit and legal drugs and human urine indicators in U.S. wastewaters. , 2008, Environmental science & technology.

[9]  B. Escher,et al.  Screening method for ecotoxicological hazard assessment of 42 pharmaceuticals considering human metabolism and excretory routes. , 2007, Environmental science & technology.

[10]  Christoph Ort,et al.  Sampling for pharmaceuticals and personal care products (PPCPs) and illicit drugs in wastewater systems: are your conclusions valid? A critical review. , 2010, Environmental science & technology.

[11]  F. Ventura,et al.  Trace determination of cannabinoids and opiates in wastewater and surface waters by ultra-performance liquid chromatography-tandem mass spectrometry. , 2007, Journal of chromatography. A.

[12]  F. Ventura,et al.  Monitoring of opiates, cannabinoids and their metabolites in wastewater, surface water and finished water in Catalonia, Spain. , 2009, Water research.

[13]  Christian G. Daughton,et al.  Illicit Drugs in Municipal Sewage: Proposed New Nonintrusive Tool to Heighten Public Awareness of Societal Use of Illicit-Abused Drugs and Their Potential for Ecological Consequences , 2001 .

[14]  Edward J. Bouwer,et al.  Biodegradation and removal of pharmaceuticals and personal care products in treatment systems: a review , 2009, Biodegradation.

[15]  Ronny Blust,et al.  Cocaine and metabolites in waste and surface water across Belgium. , 2009, Environmental pollution.

[16]  C. Metcalfe,et al.  Illicit drugs in Canadian municipal wastewater and estimates of community drug use. , 2010, Environmental pollution.

[17]  T. Poiger,et al.  Ubiquitous occurrence of the artificial sweetener acesulfame in the aquatic environment: an ideal chemical marker of domestic wastewater in groundwater. , 2009, Environmental science & technology.

[18]  Steve Carter,et al.  Determining the fraction of pharmaceutical residues in wastewater originating from a hospital. , 2010, Water research.

[19]  Adrian Covaci,et al.  Illicit drug consumption estimations derived from wastewater analysis: a critical review. , 2011, The Science of the total environment.

[20]  Ettore Zuccato,et al.  Identification and measurement of illicit drugs and their metabolites in urban wastewater by liquid chromatography-tandem mass spectrometry. , 2006, Analytical chemistry.

[21]  D. Barceló,et al.  Analysis of drugs of abuse and their human metabolites in water by LC-MS2: A non-intrusive tool for drug abuse estimation at the community level , 2008 .

[22]  Willi Gujer,et al.  Estimating sewer leakage from continuous tracer experiments. , 2007, Water research.

[23]  B. Lloyd,et al.  Qld Drug Trends 2006: Findings from the Illicit Drug Reporting System (IDRS) , 2003 .

[24]  Ronny Blust,et al.  Spatial and temporal variations in the occurrence of cocaine and benzoylecgonine in waste- and surface water from Belgium and removal during wastewater treatment. , 2009, Water research.

[25]  F. Ventura,et al.  Occurrence of psychoactive stimulatory drugs in wastewaters in north-eastern Spain. , 2008, The Science of the total environment.

[26]  M Thomann Quality evaluation methods for wastewater treatment plant data. , 2008, Water science and technology : a journal of the International Association on Water Pollution Research.

[27]  M. Fischman,et al.  Urinary excretion of ecgonine methyl ester, a major metabolite of cocaine in humans. , 1984, Journal of analytical toxicology.

[28]  Marilyn A Huestis,et al.  Urinary MDMA, MDA, HMMA, and HMA excretion following controlled MDMA administration to humans. , 2009, Journal of analytical toxicology.

[29]  B. Paull,et al.  Using environmental analytical data to estimate levels of community consumption of illicit drugs and abused pharmaceuticals. , 2007, Journal of environmental monitoring : JEM.

[30]  Randall C. Baselt,et al.  Disposition of toxic drugs and chemicals in man , 1982 .

[31]  H. Neels,et al.  Can cocaine use be evaluated through analysis of wastewater? A nation-wide approach conducted in Belgium. , 2009, Addiction.

[32]  Antonio Pflüger,et al.  The costs of tobacco, alcohol and illicit drug abuse to Australian society in 2004/05: summary version , 2008 .

[33]  Y. Lévi,et al.  Estimation of illicit drugs consumption by wastewater analysis in Paris area (France). , 2010, Forensic science international.

[34]  M. Huestis,et al.  Urine testing for cocaine abuse: metabolic and excretion patterns following different routes of administration and methods for detection of false-negative results. , 2003, Journal of analytical toxicology.

[35]  S. Belknap,et al.  Urinary excretion of cocaine, benzoylecgonine, and ecgonine methyl ester in humans. , 1988, Journal of analytical toxicology.

[36]  Christoph Ort,et al.  Sampling for PPCPs in wastewater systems: comparison of different sampling modes and optimization strategies. , 2010, Environmental science & technology.

[37]  I. Senta,et al.  Illicit drugs in wastewater of the city of Zagreb (Croatia)--estimation of drug abuse in a transition country. , 2010, Environmental pollution.

[38]  Alan D. Lopez,et al.  Comparative quantification of health risks. Global and regional burden of disease attributable to selected major risk factors. Volume 1. , 2004 .

[39]  F. Ventura,et al.  Ultraperformance liquid chromatography-tandem mass spectrometry analysis of stimulatory drugs of abuse in wastewater and surface waters. , 2007, Analytical chemistry.

[40]  Ronny Blust,et al.  Sewage epidemiology--a real-time approach to estimate the consumption of illicit drugs in Brussels, Belgium. , 2011, Environment international.

[41]  E. Cone,et al.  Cocaine metabolism and urinary excretion after different routes of administration. , 1998, Therapeutic drug monitoring.

[42]  C. Daughton Illicit drugs: contaminants in the environment and utility in forensic epidemiology. , 2011, Reviews of environmental contamination and toxicology.

[43]  D. Calamari,et al.  Cocaine in surface waters: a new evidence-based tool to monitor community drug abuse , 2005, Environmental health : a global access science source.

[44]  R. Fanelli,et al.  Mass spectrometric analysis of illicit drugs in wastewater and surface water. , 2008, Mass spectrometry reviews.

[45]  J. Choubert,et al.  Fate of pharmaceuticals and personal care products in wastewater treatment plants--conception of a database and first results. , 2009, Environmental pollution.

[46]  S. R. Howell,et al.  Metabolic disposition of 14C-venlafaxine in mouse, rat, dog, rhesus monkey and man. , 1993, Xenobiotica; the fate of foreign compounds in biological systems.