Evaluation of pharmaceuticals in surface water: reliability of PECs compared to MECs.

Due to the current analytical processes that are not able to measure all the pharmaceutical molecules and to the high costs and the consumption of time to sample and analyze PhACs, models to calculate Predicted Environmental Concentrations (PECs) have been developed. However a comparison between MECs and PECs, taking into account the methods of calculations and peculiarly the parameters included in the calculation (consumption data, pharmacokinetic parameters, elimination rate in STPs and in the environment), is necessary to assess the validity of PECs. MEC variations of sixteen target PhACs [acetaminophen (ACE), amlodipine (AML), atenolol (ATE), caffeine (CAF), carbamazepine (CAR), doxycycline (DOX), epoxycarbamazepine (EPO), fluvoxamine (FLU), furosemide (FUR), hydrochlorothiazide (HYD), ifosfamide (IFO), losartan (LOS), pravastatin (PRA), progesterone (PROG), ramipril (RAM), trimetazidine (TRI)] have been evaluated during one hydrological cycle, from October 2011 to October 2012 and compared to PECs calculated by using an adaptation of the models proposed by Heberer and Feldmann (2005) and EMEA (2006). Comparison of PECs and MECS has been achieved for six molecules: ATE, CAR, DOX, FUR, HYD and PRA. DOX, FUR and HYD present differences between PECs and MECs on an annual basis but their temporal evolutions follow the same trends. PEC evaluation for these PhACs could then be possible but need some adjustments of consumption patterns, pharmacokinetic parameters and/or mechanisms of (bio)degradation. ATE, CAR and PRA are well modeled; PECs can then be used as reliable estimation of concentrations without any reserve.

[1]  B. Roig,et al.  Discharge of pharmaceutical products (PPs) through a conventional biological sewage treatment plant: MECs vs PECs? , 2009, Environment international.

[2]  Anne Togola,et al.  Consequences of treated water recycling as regards pharmaceuticals and drugs in surface and ground waters of a medium-sized Mediterranean catchment. , 2006, Environmental science & technology.

[3]  M. Sauter,et al.  A case study on the correlation of micro-contaminants and potassium in the Leine River (Germany) , 2011 .

[4]  R. Dinsdale,et al.  Illicit drugs and pharmaceuticals in the environment--forensic applications of environmental data, Part 2: Pharmaceuticals as chemical markers of faecal water contamination. , 2009, Environmental pollution.

[5]  Annemarie P van Wezel,et al.  Relating environmental concentrations of pharmaceuticals to consumption: A mass balance approach for the river Rhine. , 2010, Environment international.

[6]  E. Thurman,et al.  Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999-2000: a national reconnaissance. , 2002, Environmental science & technology.

[7]  M. Esperanza,et al.  Zoom sur les substances pharmaceutiques : présence, partition, devenir en station d’épuration , 2011 .

[8]  D. Barceló,et al.  Analysis and occurrence of pharmaceuticals, estrogens, progestogens and polar pesticides in sewage treatment plant effluents, river water and drinking water in the Llobregat river basin (Barcelona, Spain) , 2008 .

[9]  Thomas Heberer,et al.  Contribution of effluents from hospitals and private households to the total loads of diclofenac and carbamazepine in municipal sewage effluents--modeling versus measurements. , 2005, Journal of hazardous materials.

[10]  A Wenzel,et al.  Environmental hazard assessment of pharmaceuticals. , 1997, Regulatory toxicology and pharmacology : RTP.

[11]  Isabel Martí,et al.  Occurrence and fate of emerging wastewater contaminants in Western Balkan Region. , 2008, The Science of the total environment.

[12]  M. Laušević,et al.  Determination of multiple pharmaceutical classes in surface and ground waters by liquid chromatography-ion trap-tandem mass spectrometry. , 2009, Journal of chromatography. A.

[13]  A. Ledin,et al.  Fate of carbamazepine during water treatment. , 2009, Environmental science & technology.

[14]  T. Scheytt,et al.  A New Approach to Calculate EMEA’s Predicted Environmental Concentration for Human Pharmaceuticals in Groundwater at Bank Filtration Sites , 2011 .

[15]  Jörg Römbke,et al.  Environmental fate of pharmaceuticals in water/sediment systems. , 2005, Environmental science & technology.

[16]  D. Grandjean,et al.  Occurrence of several acidic drugs in sewage treatment plants in Switzerland and risk assessment. , 2005, Water research.

[17]  S. Meriç,et al.  Occurrence patterns of pharmaceuticals in water and wastewater environments , 2007, Analytical and bioanalytical chemistry.

[18]  S. Mabury,et al.  An exposure assessment for selected pharmaceuticals within a watershed in Southern Ontario. , 2006, Chemosphere.

[19]  R. Losier,et al.  The occurrence of acidic drugs and caffeine in sewage effluents and receiving waters from three coastal watersheds in Atlantic Canada. , 2008, The Science of the total environment.

[20]  T. T. ter Laak,et al.  Prediction of concentration levels of metformin and other high consumption pharmaceuticals in wastewater and regional surface water based on sales data. , 2013, The Science of the total environment.

[21]  Jeanne Garric,et al.  Human pharmaceuticals in surface waters. Implementation of a prioritization methodology and application to the French situation. , 2008, Toxicology letters.

[22]  Ran Wang,et al.  Occurrence of veterinary antibiotics in animal wastewater and surface water around farms in Jiangsu Province, China. , 2011, Chemosphere.

[23]  K. Shah,et al.  Effect of pH, chlorobutanol, cysteine hydrochloride, ethylenediaminetetraacetic acid, propylene glycol, sodium metabisulfite, and sodium sulfite on furosemide stability in aqueous solutions. , 1980, Journal of pharmaceutical sciences.

[24]  J. Garric,et al.  Exposure Assessment of Pharmaceuticals and Their Metabolites in the Aquatic Environment: Application to the French Situation and Preliminary Prioritization , 2008 .

[25]  A. Spongberg,et al.  Reconnaissance of selected PPCP compounds in Costa Rican surface waters. , 2011, Water research.

[26]  D. Barceló,et al.  Wastewater treatment plants as a pathway for aquatic contamination by pharmaceuticals in the Ebro river basin (Northeast Spain) , 2007, Environmental toxicology and chemistry.

[27]  E. Michael Thurman,et al.  Response to Comment on “Pharmaceuticals, Hormones, and Other Organic Wastewater Contaminants in U.S. Streams, 1999−2000: A National Reconnaissance” , 2002 .

[28]  T. Tuhkanen,et al.  Elimination of pharmaceuticals in sewage treatment plants in Finland. , 2007, Water research.

[29]  Y. Valcárcel,et al.  Analysis of the presence of cardiovascular and analgesic/anti-inflammatory/antipyretic pharmaceuticals in river- and drinking-water of the Madrid Region in Spain. , 2011, Chemosphere.

[30]  F. Huneau,et al.  Monitoring of trace metals and pharmaceuticals as anthropogenic and socio-economic indicators of urban and industrial impact on surface waters , 2013, Environmental Monitoring and Assessment.

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

[32]  K. Kümmerer,et al.  Summary of Workshop on Fate of Pharmaceuticals in the Environment , 2007 .

[33]  Hélène Budzinski,et al.  Pharmaceuticals in Rivers of Two Regions with Contrasted Socio-Economic Conditions: Occurrence, Accumulation, and Comparison for Ukraine and France , 2012, Water, Air, & Soil Pollution.

[34]  Hélène Budzinski,et al.  Multi-residue analysis of pharmaceutical compounds in aqueous samples. , 2008, Journal of chromatography. A.

[35]  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.

[36]  Marina Coquery,et al.  Évaluer les rendements des stations d’épuration - Apports méthodologiques et résultats pour les micropolluants en filières conventionnelles et avancées , 2011 .

[37]  M. Sauter,et al.  Occurrence and spatial distribution of organic micro-pollutants in a complex hydrogeological karst system during low flow and high flow periods, results of a two-year study. , 2013, The Science of the total environment.

[38]  Rubén I Irusta Mata,et al.  Consumption and occurrence of pharmaceutical and personal care products in the aquatic environment in Spain. , 2013, The Science of the total environment.

[39]  Marta Carballa,et al.  How are pharmaceutical and personal care products (PPCPs) removed from urban wastewaters? , 2008 .

[40]  R. Williams,et al.  A practical demonstration in modelling diclofenac and propranolol river water concentrations using a GIS hydrology model in a rural UK catchment. , 2007, Environmental pollution.

[41]  N Kreuzinger,et al.  Carbamazepine as a possible anthropogenic marker in the aquatic environment: investigations on the behaviour of Carbamazepine in wastewater treatment and during groundwater infiltration. , 2004, Water research.

[42]  Satoshi Takizawa,et al.  Evaluation of pharmaceuticals and personal care products as water-soluble molecular markers of sewage. , 2008, Environmental science & technology.

[43]  Barbara Kasprzyk-Hordern,et al.  The occurrence of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs in surface water in South Wales, UK. , 2008, Water research.

[44]  T. Ternes Occurrence of drugs in German sewage treatment plants and rivers 1 Dedicated to Professor Dr. Klaus , 1998 .

[45]  K. Thomas,et al.  The occurrence of selected pharmaceuticals in wastewater effluent and surface waters of the lower Tyne catchment. , 2006, The Science of the total environment.

[46]  F. Borrull,et al.  Pharmaceutical determination in surface and wastewaters using high-performance liquid chromatography-(electrospray)-mass spectrometry. , 2007, Journal of separation science.

[47]  A. V. van Wezel,et al.  Toxicological relevance of emerging contaminants for drinking water quality. , 2010, Water research.

[48]  T. Ginn,et al.  Occurrence and fate of pharmaceutically active compounds in the environment, a case study: Höje River in Sweden. , 2005, Journal of hazardous materials.

[49]  T. Poiger,et al.  Caffeine, an anthropogenic marker for wastewater comtamination of surface waters. , 2003, Environmental science & technology.

[50]  P. Anderson,et al.  Human pharmaceuticals in US surface waters: a human health risk assessment. , 2005, Regulatory toxicology and pharmacology : RTP.

[51]  J. Garric,et al.  Anticancer drugs in surface waters: what can we say about the occurrence and environmental significance of cytotoxic, cytostatic and endocrine therapy drugs? , 2012, Environment international.

[52]  Charles S Wong,et al.  Laboratory calibration and field deployment of the Polar organic chemical integrative sampler for pharmaceuticals and personal care products in wastewater and surface water , 2007, Environmental toxicology and chemistry.

[53]  D. Kolpin,et al.  A national reconnaissance for pharmaceuticals and other organic wastewater contaminants in the United States--II) untreated drinking water sources. , 2008, The Science of the total environment.

[54]  K. Belitz,et al.  Occurrence and concentrations of pharmaceutical compounds in groundwater used for public drinking-water supply in California. , 2011, The Science of the total environment.

[55]  J. Carrera,et al.  Occurrence of 95 pharmaceuticals and transformation products in urban groundwaters underlying the metropolis of Barcelona, Spain. , 2013, Environmental pollution.

[56]  Anna Ledin,et al.  Ecotoxicity of carbamazepine and its UV photolysis transformation products. , 2013, The Science of the total environment.

[57]  J. Sekizawa,et al.  Persistence and partitioning of eight selected pharmaceuticals in the aquatic environment: laboratory photolysis, biodegradation, and sorption experiments. , 2009, Water research.

[58]  D. Calamari,et al.  Methodological approaches for studying pharmaceuticals in the environment by comparing predicted and measured concentrations in River Po, Italy. , 2004, Regulatory toxicology and pharmacology : RTP.

[59]  Jaeweon Cho,et al.  Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters. , 2007, Water research.

[60]  M. Servos,et al.  Behavior and occurrence of estrogens in municipal sewage treatment plants--I. Investigations in Germany, Canada and Brazil. , 1999, The Science of the total environment.

[61]  S. Mabury,et al.  PhetoFate: a new approach in accounting for the contribution of indirect photolysis of pesticides and pharmaceuticals in surface waters. , 2003, Environmental science & technology.

[62]  D. Barceló,et al.  Development of a multi-residue analytical methodology based on liquid chromatography-tandem mass spectrometry (LC-MS/MS) for screening and trace level determination of pharmaceuticals in surface and wastewaters. , 2006, Talanta.

[63]  Adriano Joss,et al.  Biological degradation of pharmaceuticals in municipal wastewater treatment: proposing a classification scheme. , 2006, Water research.

[64]  R. Dinsdale,et al.  Illicit drugs and pharmaceuticals in the environment--forensic applications of environmental data. Part 1: Estimation of the usage of drugs in local communities. , 2009, Environmental pollution.

[65]  D. Barceló,et al.  Environmental risk assessment of pharmaceuticals in rivers: relationships between hazard indexes and aquatic macroinvertebrate diversity indexes in the Llobregat River (NE Spain). , 2010, Environment international.

[66]  D. Barceló,et al.  Occurrence and modeling of pharmaceuticals on a sewage-impacted Mediterranean river and their dynamics under different hydrological conditions. , 2012, The Science of the total environment.

[67]  Klaus Kümmerer,et al.  The presence of pharmaceuticals in the environment due to human use--present knowledge and future challenges. , 2009, Journal of environmental management.

[68]  M. Benotti,et al.  Distributions of pharmaceuticals in an urban estuary during both dry- and wet-weather conditions. , 2007, Environmental science & technology.

[69]  B. Kasprzyk-Hordern,et al.  Spatial and temporal occurrence of pharmaceuticals and illicit drugs in the aqueous environment and during wastewater treatment: new developments. , 2013, The Science of the total environment.

[70]  J. Tarazona,et al.  Occurrence of pharmaceutically active compounds in surface waters of the Henares-Jarama-Tajo River system (Madrid, Spain) and a potential risk characterization. , 2010, The Science of the total environment.

[71]  M. Carballa,et al.  Comparison of predicted and measured concentrations of selected pharmaceuticals, fragrances and hormones in Spanish sewage. , 2008, Chemosphere.

[72]  D. Larsson,et al.  Effluent from drug manufactures contains extremely high levels of pharmaceuticals. , 2007, Journal of hazardous materials.

[73]  A. Togola Présence et devenir des substances pharmaceutiques dans les écosystèmes aquatiques , 2006 .

[74]  D. Kolpin,et al.  A national reconnaissance of pharmaceuticals and other organic wastewater contaminants in the United States--I) groundwater. , 2008, The Science of the total environment.

[75]  H. Singer,et al.  Simultaneous quantification of neutral and acidic pharmaceuticals and pesticides at the low-ng/l level in surface and waste water. , 2001, Journal of chromatography. A.

[76]  Thomas Heberer,et al.  Tracking persistent pharmaceutical residues from municipal sewage to drinking water , 2002 .

[77]  C. Cren-olivé,et al.  Screening of pharmaceuticals and hormones at the regional scale, in surface and groundwaters intended to human consumption. , 2011, Environmental pollution.

[78]  T. Tuhkanen,et al.  Occurrence of acidic pharmaceuticals in raw and treated sewages and in receiving waters. , 2005, Water research.

[79]  G. Khachatourians,et al.  Agricultural use of antibiotics and the evolution and transfer of antibiotic-resistant bacteria. , 1998, CMAJ : Canadian Medical Association journal = journal de l'Association medicale canadienne.

[80]  M. Prévost,et al.  Seasonal variations in the occurrence and fate of basic and neutral pharmaceuticals in a Swedish river-lake system. , 2010, Chemosphere.

[81]  D. Voutsa,et al.  Passive sampling of selected endocrine disrupting compounds using polar organic chemical integrative samplers. , 2008, Environmental pollution.

[82]  Hing-Biu Lee,et al.  Determination of endocrine-disrupting phenols, acidic pharmaceuticals, and personal-care products in sewage by solid-phase extraction and gas chromatography-mass spectrometry. , 2005, Journal of chromatography. A.

[83]  Kyungho Choi,et al.  Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River, Korea. , 2008, The Science of the total environment.

[84]  M. Birkved,et al.  Environmental risk assessment of human pharmaceuticals in Denmark after normal therapeutic use. , 2000, Chemosphere.

[85]  H. E. Williams,et al.  Kinetics and Degradation Products for Direct Photolysis of β-Blockers in Water , 2007 .

[86]  H. Gardarsdottir,et al.  Seasonal patterns of initiating antidepressant therapy in general practice in the Netherlands during 2002-2007. , 2010, Journal of affective disorders.

[87]  J. Santos,et al.  Presence of pharmaceutically active compounds in Doñana Park (Spain) main watersheds. , 2010, Journal of hazardous materials.

[88]  J. Conley,et al.  Spatial and temporal analysis of pharmaceutical concentrations in the upper Tennessee River basin. , 2008, Chemosphere.

[89]  Vimal Kumar,et al.  De-conjugation behavior of conjugated estrogens in the raw sewage, activated sludge and river water. , 2012, Journal of hazardous materials.

[90]  Z. Moldovan Occurrences of pharmaceutical and personal care products as micropollutants in rivers from Romania. , 2006, Chemosphere.

[91]  R Hirsch,et al.  Occurrence of antibiotics in the aquatic environment. , 1999, The Science of the total environment.

[92]  T. Steger-Hartmann,et al.  Biological degradation of cyclophosphamide and its occurrence in sewage water. , 1997, Ecotoxicology and environmental safety.

[93]  R. Fanelli,et al.  Identification of the pharmaceuticals for human use contaminating the Italian aquatic environment. , 2005, Journal of hazardous materials.

[94]  K. Thomas,et al.  Environmental assessment of Norwegian priority pharmaceuticals based on the EMEA guideline. , 2008, Ecotoxicology and environmental safety.