Skip to main content
SpringerLink
Log in

Widespread occurrence and seasonal variation of pharmaceuticals in surface waters and municipal wastewater treatment plants in central Finland

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The presence of five selected pharmaceuticals, consisting of four anti-inflammatory drugs, diclofenac, ibuprofen, ketoprofen, naproxen, and an antiepileptic drug carbamazepine, was determined at four municipal wastewater treatment plants (WWTPs) and in the receiving waterway in central Finland. The samples were taken from influents and effluents of the WWTPs and from surface water of six locations along the water way, including northern Lake Päijänne. In addition, seasonal variation in the area was determined by comparing the concentrations in the winter and summer. The samples were analyzed by liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS) in the multiple reaction monitoring mode. The concentrations in the influents and effluents ranged from hundreds of nanogram per liter to microgram per liter while ranged from tens of nanogram per liter in northern parts of the waterway to hundreds of nanogram per liter in northern Lake Päijänne near the city area. In addition, the concentrations were higher in the winter compared to summer time in surface water due to decreased temperature and solar irradiation. On the other hand, higher concentrations of ibuprofen, ketoprofen, and naproxen were found in summer at the WWTPs, possibly due to seasonal variations in consumption. In conclusion, there are considerable amounts of pharmaceuticals not only in influents and effluents of the WWTPs but also in lake water along the waterway and in northern Lake Päijänne.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10

Similar content being viewed by others

References

  • Andreozzi R, Raffaele M, Nicklas P (2003) Pharmaceuticals in STP effluents and their solar photodegradation in aquatic environment. Chemosphere 50:1319–1330

    Article  CAS  Google Scholar 

  • Arokoski JPA, Lammi MJ, Hyttinen MM, Kiviranta I, Parkkinen JJ, Jurvelin JS, Tammi MI, Helminen HJ (2001) Nivelrikon etiopatogeneesi (In Finnish). Duodecim 117:1617–1626

    CAS  Google Scholar 

  • Barber LB, Keefe SH, Brown GK, Furlong ET, Gray JL, Kolpin DW, Meyer MT, Sandstrom MW, Zaugg SD (2013) Persistence and potential effects of complex organic contaminant mixtures in wastewater-impacted streams. Environ Sci Technol 47:2177–2188

    Article  CAS  Google Scholar 

  • Barceló D (2003) Emerging pollutants in water analysis. Trends Anal Chem 22:xiv–xvi

    Article  Google Scholar 

  • Bartels P, von Tümpling W Jr (2007) Solar radiation influence on the decomposition process of diclofenac in surface waters. Sci Total Environ 374:143–155

    Article  CAS  Google Scholar 

  • Behera SK, Kim HW, Oh J-E, Park H-S (2011) Occurrence and removal of antibiotics, hormones and several other pharmaceuticals in wastewater treatment plants of the largest industrial city of Korea. Sci Total Environ 409:4351–4360

    Article  CAS  Google Scholar 

  • Blair BD, Crago JP, Hedman CJ, Magruder C, Royer LS, Treguer RFJ, Klaper RD (2013) Evaluation of a model for the removal of pharmaceuticals, personal care products, and hormones from wastewater. Sci Total Environ 444C:515–521

    Article  Google Scholar 

  • Bottoni P, Fidente R (2005) Un primo contributo alla problematica dei farmaci come contaminanti delle acque. Ann Ist Super Sanità 41:333–342

    CAS  Google Scholar 

  • Buchberger WW (2007) Novel analytical procedures for screening of drug residues in water, waste water sediment and sludge. Anal Chim Acta 593:129–139

    Article  CAS  Google Scholar 

  • Buser H-R, Poiger T, Müller MD (1999) Occurrence and environmental behavior of the chiral pharmaceutical drug ibuprofen in surface waters and in wastewater. Environ Sci Technol 33:2529–2535

    Article  CAS  Google Scholar 

  • Calza P, Medana C, Padovano E, Giancotti V, Minero C (2013) Fate of selected pharmaceuticals in river waters. Environ Sci Pollut Res 20:2262–2270

    Article  CAS  Google Scholar 

  • 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 40:357–463

    Article  CAS  Google Scholar 

  • Choi K, Kim Y, Park J, Park CK, Kim MY, Kim HS, Kim P (2008) Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River, Korea. Sci Total Environ 405:120–128

    Article  CAS  Google Scholar 

  • Conçalves CMO, Sousa MAD, Alpendurada MFPSPM (2013) Analysis of acidic, basic and neutral pharmaceuticals in river waters: clean-up by 1° 2° amino anion exchange and enrichment using an hydrophilic adsorbent. Intern J Environ Anal Chem 93:1–22

    Article  Google Scholar 

  • Coronado M, De Haro H, Deng X, Rempel MA, Lavado R, Schlenk D (2008) Estrogenic activity and reproductive effects of the UV-filter oxybenzone (2-hydroxy-4-methoxyphenyl-methanone) in fish. Aquat Toxicol 90:182–187

    Article  CAS  Google Scholar 

  • Daneshvar A, Svanfelt J, Kronberg L, Prévost M, Weyhenmeyer GA (2010) Seasonal variations in the occurrence and fate of basic and neutral pharmaceuticals in a Swedish river–lake system. Chemosphere 80:301–309

    Article  CAS  Google Scholar 

  • Daneshvar A, Svanfelt J, Kronberg L, Weyhenmeyer GA (2012) Neglected sources of pharmaceuticals in river water—footprints of a Reggae festival. J Environ Monit 14:596–603

    Article  CAS  Google Scholar 

  • Daughton CG (2002) Environmental stewardship and drugs as pollutants. Lancet 360:1035–1036

    Article  Google Scholar 

  • Daughton CG, Ternes TA (1999) Pharmaceuticals and personal care products in the environment: agents of subtle change? Environ Health Perspect 107:907–938

    Article  CAS  Google Scholar 

  • Díaz-Cruz SM, Llorca M, Barceló D (2008) Organic UV filters and their photodegradates, metabolites and disinfection by-products in the aquatic environment. Trends Anal Chem 27:873–887

    Article  Google Scholar 

  • Fent K, Weston AA, Caminada D (2006) Ecotoxicology of human pharmaceuticals. Aquat Toxicol 76:122–159

    Article  CAS  Google Scholar 

  • Ferrer I, Thurman EM (2010) Identification of a new antidepressant and its glucuronide metabolite in water samples using liquid chromatography/quadrupole time-of-flight mass spectrometry. Anal Chem 82:8161–8168

    Article  CAS  Google Scholar 

  • Finnish Medicines Agency Fimea and Social Insurance Institution (2014) Suomen lääketilasto/ Finnish Statistics on Medicines 2014., http://raportit.nam.fi/raportit/kulutus/kv_laakekulutus.pdf. Accessed 13 July 2015

    Google Scholar 

  • Finnish Medicines Agency Fimea and Social Insurance Institution (2015) List of self-medication packages of medicinal products with market authorisations., http://www.fimea.fi/download/ 22526_Itsehoitovalmistelista.pdf. Accessed 26 August 2015

    Google Scholar 

  • Flaherty CM, Dodson SI (2005) Effects of pharmaceuticals on Daphnia survival, growth, and reproduction. Chemosphere 61:200–207

    Article  CAS  Google Scholar 

  • García del Pozo J, Ramos SE, De Abajo F, Mateos CR (2004) Utilización de los antihipertensivos en España (1995–2001). Rev Esp Cardiol 57:241–249

    Google Scholar 

  • Gros M, Petrović M, Ginebreda A, Barceló D (2010) Removal of pharmaceuticals during wastewater treatment and environmental risk assessment using hazard indexes. Environ Int 36:15–26

    Article  CAS  Google Scholar 

  • Heberer T, Reddersen K, Mechlinski A (2002) From municipal sewage in drinking water: fate and removal of pharmaceuticals residues in the aquatic environment in urban areas. Water Sci Technol 46:81–88

    CAS  Google Scholar 

  • HERTTA (2015) Environmental Information System, Finnish Environmental Institute

    Google Scholar 

  • Herve S (1991) Mussel incubation method for monitoring organochlorine compounds in freshwater recipients of pulp and paper industry. Dissertation, University of Jyväskylä

    Google Scholar 

  • Hignite C, Azarnoff DL (1977) Drugs and drug metabolites as environmental contaminants: chlorophenoxyisobutyrate and salicylic acid in sewage water effluent. Life Sci 20:337–341

    Article  CAS  Google Scholar 

  • Hirsch R, Ternes T, Haberer K, Kratz K-L (1999) Occurrence of antibiotics in the aquatic environment. Sci Total Environ 225:109–118

    Article  CAS  Google Scholar 

  • Holčapek M, Kolářová L, Nobilis M (2008) High-performance liquid chromatography–tandem mass spectrometry in the identification and determination of phase I and phase II drug metabolites. Anal Bioanal Chem 391:59–78

    Article  Google Scholar 

  • Illés E, Takács E, Dombi A, Gajda-Schranz K, Rácz G, Gonter K, Wojnárovits L (2013) Hydroxyl radical induced degradation of ibuprofen. Sci Total Environ 447:286–292

    Article  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Kosjek T, Perko S, Heath E, Kralj B, Žigon D (2011) Application of complementary mass spectrometric techniques to the identification of ketoprofen phototransformation products. J Mass Spectrom 46:391–401

    Article  CAS  Google Scholar 

  • Kostopoulou M, Nikolaou A (2008) Analytical problems and the need for sample preparation in the determination of pharmaceuticals and their metabolites in aqueous environmental matrices. Trends in Anal Chem 27:1023–1035

    Article  CAS  Google Scholar 

  • Kotnik K, Kosjek T, Krajnc U, Heath E (2014) Trace analysis of benzophenone-derived compounds in surface waters and sediments using solid-phase extraction and microwave-assisted extraction followed by gas chromatography–mass spectrometry. Anal Bioanal Chem 406:3179–3190

    Article  CAS  Google Scholar 

  • Krogerus K, Liukko N, Juntunen J, Kotamäki N, Nieminen P, Huttula T (2013) Purkuputken siirron vaikutukset vedenlaatuun Pohjois-Päijänteellä Coherens-malliarvio (in Finnish)., Finnish Environment Institute 12/2013

    Google Scholar 

  • Kümmerer K (2004) Resistance in the environment. J Antimicrob Chemother 54:311–320

    Article  Google Scholar 

  • Kunkel U, Radke M (2012) Fate of pharmaceuticals in rivers: deriving a benchmark dataset at favorable attenuation conditions. Water Res 46:5551–5565

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Lemus JA, Blanco G, Grande J, Arroyo B, García-Montijano M, Martínez F (2008) Antibiotics threaten wildlife: circulating quinolone residues and disease in Avian scavengers. PloS One 3:e1444

    Article  Google Scholar 

  • Li H, Helm PA, Metcalfe CD (2010a) Sampling in the Great Lakes for pharmaceutical, personal care products, and endcrine-disrupting substances using the passive polar organic chemical integrative sampler. Environ Toxicol Chem 29:751–762

    Article  CAS  Google Scholar 

  • Li D, Yu T, Zhang Y, Yang M, Li Z, Liu M, Qi R (2010b) Antibiotic resistance characteristics of environmental bacteria from an oxytetracycline production wastewater treatment plant and the receiving river. App Environ Microbiol 76:3444–3451

    Article  CAS  Google Scholar 

  • Lindholm PC, Knuutinen JS, Ahkola HSJ, Herve SH (2014) Analysis of trace pharmaceuticals and related compounds in municipal wastewaters by preconcentration, chromatography, derivatization, and separation methods. Bioresources 9:3688–3732

    Article  Google Scholar 

  • Lindholm-Lehto PC, Knuutinen JS, Ahkola HSJ, Herve SH (2015a) Occurrence of pharmaceuticals in municipal wastewater, in the recipient water and sediment. Environ Sci Pollut Res 22:17209–17223

    Article  CAS  Google Scholar 

  • Lindholm-Lehto PC, Knuutinen JS, Ahkola HSJ, Herve SH (2015b) Refractory organic pollutants and toxicity in pulp and paper mill wastewaters. Environ Sci Pollut Res 22:6473–6499

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Loos R, Wollgast J, Huber T, Hanke G (2007) Polar herbicides, pharmaceutical products, perfluorooctanesulfonate (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

    Article  CAS  Google Scholar 

  • Madureira TV, Barreiro JC, Rocha MJ, Rocha E, Cass QB, Tiritan ME (2010) Spatiotemporal distribution of pharmaceuticals in the Douro River estuary (Portugal). Sci Total Environ 408:5513–5520

    Article  CAS  Google Scholar 

  • Middleton JH, Salierno JD (2013) Antibiotic resistance in triclosan tolerant fecal coliforms isolated from surface waters near wastewater treatment plant outflows (Morris County, NJ, USA). Ecotoxicol Environ Saf 88:79–88

    Article  CAS  Google Scholar 

  • Moreno-González R, Rodríguez-Mozaz S, Gros M, Pérez-Cánovas E, Barceló D, León VM (2014) Input of pharmaceuticals through coastal surface watercourses into a Mediterranean lagoon (Mar Menor, SE Spain): sources and seasonal variations. Sci Total Environ 490:59–72

    Article  Google Scholar 

  • Munaron D, Tapie N, Budzinski H, Andral B, Gonzalez JL (2012) Pharmaceuticals, alkylphenols and pesticides in Mediterranean coastal waters: results from a pilot survey using passive samplers. Estuar Coast Shelf Sci 114:82–92

    Article  CAS  Google Scholar 

  • Nelson ED, Do H, Lewis RS, Carr SA (2011) Diurnal variability of pharmaceutical, personal care product, estrogen and alkylphenol concentrations in effluent from a tertiary wastewater treatment facility. Environ Sci Technol 45:1228–1234

    Article  CAS  Google Scholar 

  • Packer JL, Werner JJ, Latch DE, McNeill K, Arnold WA (2003) Photochemical fate of pharmaceuticals in the environment: naproxen, diclofenac, clofibric acid, and ibuprofen. Aquat Sci 65:342–351

    Article  CAS  Google Scholar 

  • Phillips PJ, Smith SG, Kolpin DW, Zaugg SD, Buxton HT, Furlong ET, Esposito K, Stinson B (2010) Pharmaceutical formulation facilities as sources of opioids and other pharmaceuticals to wastewater treatment plant effluents. Environ Sci Technol 44:4910–4916

    Article  CAS  Google Scholar 

  • Quintana JB, Weiss S, Reemtsma T (2005) Pathways and metabolites of microbial degradation of selected acidic pharmaceutical and their occurrence in municipal wastewater treated by a membrane bioreactor. Water Research 39:2654–2664

    Article  CAS  Google Scholar 

  • Santos JL, Aparicio I, Callejón M, Alonso E (2009) Occurrence of pharmaceutically active compounds during 1-year period in wastewaters from four wastewater treatment plants in Seville (Spain). J Hazard Mater 164:1509–1516

    Article  CAS  Google Scholar 

  • Silva BF, Jelic A, López-Serna R, Mozeto AA, Petrovic M, Barceló D (2011) Occurrence and distribution of pharmaceuticals in surface water, suspended solids and sediments of the Ebro river basin, Spain. Chemosphere 85:1331–1339

    Article  Google Scholar 

  • Statistics Finland (2015) Age distribution in municipalities., http://www.stat.fi/tup/kunnat/tilastot _aakkosittain.html. Accessed 26 August 2015

    Google Scholar 

  • Stumpf M, Ternes T, Haberer K, Baumann W (1998) Isolierung von Ibuprofen-Metaboliten und deren Bedeutung als Kontaminanten in der aquatischen Umwelt. [Isolation of ibuprofen-metabolites and their importance as pollutants of the aquatic environment]. Vom Wasser 91:291–303

    CAS  Google Scholar 

  • Swapna KM, Rajesh R, Lakshmanan PT (2012) Incidence of antibiotic residues in farmed shrimps from the southern states of India. Indian J Fish 41:344–347

    CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Urase T, Kikuta T (2005) Separate estimation of adsorption and degradation pf pharmaceutical substances and estrogens in the activated sludge process. Water Res 39:1289–1300

    Article  CAS  Google Scholar 

  • 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

    Article  CAS  Google Scholar 

  • Vogna D, Marotta R, Andreozzi R, Napolitano A, d’Ischia M (2004) Kinetic and chemical assessment of the UV/H2O2 treatment of antiepileptic drug carbamazepine. Chemosphere 54:497–505

    Article  CAS  Google Scholar 

  • Yamamoto H, Nakamura Y, Moriguchi S, Honda Y, Tamura I, Hirata Y, Hayashi A, Sekizawa J (2009) Persistence and partitioning of eight selected pharmaceuticals in the aquatic environment: laboratory photolysis, biodegradation, and sorption experiments. Water Res 43:351–362

    Article  CAS  Google Scholar 

  • Zuccato E, Calamari D, Natangelo M, Fanelli R (2000) Presence of therapeutic drugs in the environment. Lancet 355:1789–1790

    Article  CAS  Google Scholar 

  • Zuccato E, Castiglioni S, Fanelli R, Reitano G, Bagnati R, Chiabrando C, Pomati F, Rossetti C, Calamari D (2006) Pharmaceuticals in the environment in Italy: causes, occurrence, effects and control. Environ Sci Pollut Res 13:15–21

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors would like to thank for the financial support from Maa-ja vesitekniikan tuki ry. In addition, the cooperation during sampling with Nab Labs Oy, Nenäinniemi WWTP (Jyväskylän Seudun Puhdistamo Oy), Äänekoski WWTP (Äänekosken Energia Oy), and Saarilampi and Pylkönmäki WWTPs (Saarijärven Vesihuolto Oy) is gratefully acknowledged.

Author information

Authors and Affiliations

  1. Department of Chemistry, University of Jyväskylä, P.O. Box 35, FI-40014, Jyväskylä, Finland

    Petra C. Lindholm-Lehto & Juha S. Knuutinen

  2. Finnish Environment Institute (SYKE), Laboratory Centre, Ecotoxicology and Risk Assessment, Survontie 9A, FI-40500, Jyväskylä, Finland

    Heidi S. J. Ahkola & Sirpa H. Herve

Authors
  1. Petra C. Lindholm-Lehto
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Heidi S. J. Ahkola
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Juha S. Knuutinen
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Sirpa H. Herve
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Petra C. Lindholm-Lehto.

Additional information

Responsible editor: Hongwen Sun

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Lindholm-Lehto, P.C., Ahkola, H.S.J., Knuutinen, J.S. et al. Widespread occurrence and seasonal variation of pharmaceuticals in surface waters and municipal wastewater treatment plants in central Finland. Environ Sci Pollut Res 23, 7985–7997 (2016). https://doi.org/10.1007/s11356-015-5997-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-015-5997-y

Keywords

Search

Navigation