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Winter accumulation of acidic pharmaceuticals in a Swedish river

Abstract

Purpose

In this study, seasonal variations in the concentration profile of four analgesics and one lipid regulator were monitored on their way from a wastewater treatment plant (WWTP) effluent, along a river, and into a lake.

Methods

From December 2007 to December 2008, water samples were collected monthly (n = 12) from an upstream point, the effluent, four downstream points of the WWTP, and at the point where the river merges with the lake, and the concentrations of ibuprofen, naproxen, bezafibrate, diclofenac, and ketoprofen were determined. The analytical methodology involved solid-phase extraction of the target compounds from water samples followed by liquid chromatography coupled with tandem mass spectrometry for compound separation and detection.

Results

The studied pharmaceuticals were found in the effluent at concentrations ranging from 31 to 1,852 ng l−1 depending on the season. In the river and lake, the concentrations were much lower (6–400 ng l−1) mainly due to dilution but also to a season-dependent contribution from natural transformation processes. The mean mass flow of all analgesics was highest during winter while the highest mean mass flow of the lipid regulator bezafibrate was observed in spring.

Conclusions

The WWTP is the main source of the target compounds in the aquatic environment. The observed winter accumulation signifies the importance of natural transformation processes, which can only be estimated based on mass flow data, on the fate of pharmaceuticals in the environment.

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References

  1. Andreozzi R, Marotta R, Paxéus N (2003) Pharmaceuticals in STP effluents and their solar photodegradation in aquatic environment. Chemosphere 50:1319–1330

  2. Buser HR, Poiger T, Muller MD (1998) Occurrence and fate of the pharmaceutical drug diclofenac in surface waters: rapid photodegradation in a lake. Environ Sci Technol 32:3449–3456

  3. Buser HR, Poiger T, Muller MD (1999) Occurrence and environmental behavior of the chiral pharmaceutical drug ibuprofen in surface waters and in wastewater. Environ Sci Technol 33:2529–2535

  4. Calamari D, Zuccato E, Castiglioni S, Bagnati R, Fanelli R (2003) Strategic survey of therapeutic drugs in the Rivers Po and Lambro in northern Italy. Environ Sci Technol 37:1241–1248

  5. Castiglioni S, Bagnati R, Calamari D, Fanelli R, Zuccato E (2005) A multiresidue analytical method using solid-phase extraction and high-pressure liquid chromatography tandem mass spectrometry to measure pharmaceuticals of different therapeutic classes in urban wastewaters. J Chromatog A 1092:206–215

  6. Castiglioni S, Bagnati R, Fanelli R, Pomati F, Calamari D, Zuccato E (2006) Removal of pharmaceuticals in sewage treatment plants in Italy. Environ Sci Technol 40:357–363

  7. Farréa Ml, Péreza S, Kantiania L, Barceló D (2008) Fate and toxicity of emerging pollutants, their metabolites and transformation products in the aquatic environment. Trends Anal Chem 27:991–1007

  8. Gagné F, Blaise C, André C (2006) Occurrence of pharmaceutical products in a municipal effluent and toxicity to rainbow trout (Oncorhynchus mykiss) hepatocytes. Ecotoxicol Environ Saf 64:329–336

  9. Gros M, Petrovic M, Barcelo D (2006) 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. Talanta 70:678–690

  10. Halling-Sørensen B, Nors Nielsen S, Lanzky PF, Ingerslev F, Holten Lützhøft HC, Jørgensen SE (1998) Occurrence, fate and effects of pharmaceutical substances in the environment—review. Chemosphere 36:357–393

  11. Heberer T (2002) Tracking persistent pharmaceutical residues from municipal sewage to drinking water. J Hydrology 266:175–189

  12. Jones OA, Lester JN, Voulvoulis N (2005) Pharmaceuticals: a threat to drinking water? Trends Biotechnol 23:163–167

  13. Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD, Barber LB, Buxton HT (2002) Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999–2000: a national reconnaissance. Environ Sci Technol 36:1202–1211

  14. Larsson DGJ, de Pedro C, Paxeus N (2007) Effluent from drug manufactures contains extremely high levels of pharmaceuticals. J Hazard Mater 148:751–755

  15. Lindqvist N, Tuhkanen T, Kronberg L (2005) Occurrence of acidic pharmaceuticals in raw and treated sewages and in receiving waters. Water Res 39:2219–2228

  16. Loos R, Wollgast J, Huber T, Hanke G (2007) Polar herbicides, pharmaceutical products, perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), and nonylphenol and its carboxylates and ethoxylates in surface and tap waters around Lake Maggiore in northern Italy. Anal Bioanal Chem 387:1469–1478

  17. Metcalfe CD, Koenig BG, Bennie DT, Servos M, Ternes TA, Hirsch R (2003a) Occurrence of neutral and acidic drugs in the effluents of Canadian sewage treatment plants. Environ Toxicol Chem 22:2872–2880

  18. Metcalfe CD, Miao X-S, Koenig BG, Struger J (2003b) Distribution of acidic and neutral drugs in surface waters near sewage treatment plants in the lower Great Lakes, Canada. Environ Toxicol Chem 22:2881–2889

  19. Ollers S, Singer HP, Fassler P, Muller SR (2001) Simultaneous quantification of neutral and acidic pharmaceuticals and pesticides at the low-ng/l level in surface and waste water. J Chromatog A 911:225–234

  20. Peng X, Yu Y, Tang C, Tan J, Huang Q, Wang Z (2008) Occurrence of steroid estrogens, endocrine-disrupting phenols, and acid pharmaceutical residues in urban riverine water of the Pearl River Delta, South China. Sci Total Environ 397:158–166

  21. Pharma Professional Service (2009) http://www.phaps.com. Accessed 1 July 2009

  22. SRC PhysProp Database (2009) Interactive PhysProp Database Demo. http://esc.syrres.com/interkow/physsdemo.htm. Accessed 01 July 2009

  23. Rabiet M, Togola A, Brissaud F, Seidel JL, Budzinski H, Elbaz-Poulichet F (2006) Consequences of treated water recycling as regards pharmaceuticals and drugs in surface and ground waters of a medium-sized Mediterranean catchment. Environ Sci Technol 40:5282–5288

  24. Ternes TA (1998) Occurrence of drugs in German sewage treatment plants and rivers. Water Res 32:3245–3260

  25. Tixier C, Singer HP, Oellers S, Muller SR (2003) Occurrence and fate of carbamazepine, clofibric acid, diclofenac, ibuprofen, ketoprofen, and naproxen in surface waters. Environ Sci Technol 37:1061–1068

  26. Triebskorn R, Casper H, Heyd A, Eikemper R, Kohler H-R, Schweiger J (2004) Toxic effects of the non-steroidal anti-inflammatory drug diclofenac. Part II. Cytological effects in liver, kidney, gills and intestine of rainbow trout (Oncorhynchus mykiss). Aquat Toxicol 68:151–166

  27. Vieno N (2006) Occurrence of pharmaceuticals in Finnish sewage treatment plants, surface waters, and their elimination in drinking water treatment processes. Dissertation, Tampere University of Technology

  28. Vieno NM, Tuhkanen T, Kronberg L (2005) Seasonal variation in the occurrence of pharmaceuticals in effluents from a sewage treatment plant and in the recipient water. Environ Sci Technol 39:8220–8226

  29. Vieno N, Tuhkanen T, Kronberg L (2007) Elimination of pharmaceuticals in sewage treatment plants in Finland. Water Res 41:1001–1012

  30. Viglino L, Aboulfadl K, Daneshvar Mahvelat A, Prévost M, Sauvé S (2008) On-line solid phase extraction and liquid chromatography/tandem mass spectrometry to quantify pharmaceuticals, pesticides and some metabolites in wastewaters, drinking, and surface waters. J Environ Monitor 10:482–489

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Acknowledgment

The authors would like to thank The Swedish Research Council for Environment, Agricultural Sciences, and Spatial Planning (Formas) for financial support of this project. Dr. Jerker Fick is acknowledged for contributing in the early planning of this project and providing the internal standards. Professor Michèle Prévost is also greatly thanked for reviewing the manuscript and her helpful comments.

Author information

Correspondence to Leif Kronberg.

Additional information

Responsible editor: Zhihong Xu

Electronic supplementary material

Below is the link to the electronic supplementary material.

ESM Table 1

ESI–MS optimized parameters for the acidic compounds (DOC 36 kb)

ESM Table 2

SPE–LC–MS/MS method validation parameters (DOC 28 kb)

ESM Table 3

The measured concentration of the studied compounds in the effluent of the WWTP (DOC 39 kb)

ESM Table 4

The measured concentration of the studied compounds in the samples collected along the River Fyris (DOC 129 kb)

ESM Table 5

The measured concentration of the studied compounds in the Lake Mälaren (DOC 40 kb)

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Daneshvar, A., Svanfelt, J., Kronberg, L. et al. Winter accumulation of acidic pharmaceuticals in a Swedish river. Environ Sci Pollut Res 17, 908–916 (2010). https://doi.org/10.1007/s11356-009-0261-y

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Keywords

  • Winter
  • Pharmaceutical
  • WWTP
  • River
  • Sweden