Skip to main content
Log in

Occurrence of pharmaceuticals in municipal wastewater, in the recipient water, and sedimented particles of northern Lake Päijänne

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

Abstract

The presence of five different pharmaceuticals, consisting of four anti-inflammatory and one antiepileptic drug, was determined in influent and effluent of a municipal wastewater treatment plant (WWTP) near the city of Jyväskylä, Finland, and in the receiving water, northern Lake Päijänne. In addition, samples of sedimented particles were collected among water samples from five locations near the discharge point of the treated wastewater. The solid phase extracts (SPEs) of water samples were analyzed by liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS) in the multiple reaction monitoring mode. The studied pharmaceuticals were detected from influent, effluent, and lake water but also in the sedimented particles. The concentrations of carbamazepine, diclofenac, ibuprofen, ketoprofen, and naproxen in Lake Päijänne ranged from 1 to 21 ng L−1, 4 to 209 ng L−1, 5 to 836 ng L−1, 9 to 952 ng L−1, and 2 to 129 ng L−1, respectively. The concentrations of ketoprofen in sedimented particles ranged from 79 to 135 μg g−1 while only trace amounts of other selected pharmaceuticals were detected. The results indicate that the concentrations of pharmaceuticals are affected by the biological and chemical reactions occurring in the wastewater treatment processes but also by the UV light in the photic layer of Lake Päijänne. It can be concluded that considerable amount of selected pharmaceuticals are present in the influent and effluent of municipal WWTP but also in the water phase and sedimented particles of northern Lake Päijänne.

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

Access this article

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

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11

Similar content being viewed by others

References

  • Al-Rifai JH, Gabelish CL, Schäfer AI (2007) Occurrence of pharmaceutically active and non-steroidal estrogenic compounds in three different wastewater recycling schemes in Australia. Chemosphere 69:803–815

    Article  CAS  Google Scholar 

  • 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 

  • Antonić J, Heath E (2007) Determination of NSAIDs in river sediment samples. Anal Bioanal Chem 387:1337–1342

    Article  Google Scholar 

  • Babić S, Ašperger D, Mutavdžić D, Horvat AJM, Kaštelan-Macan M (2006) Solid phase extraction and HPLC determination of veterinary pharmaceuticals in wastewater. Talanta 70:732–738

    Article  Google Scholar 

  • Barceló D (2003) Emerging pollutants in water analysis. Trends Anal Chem 22:14–16

    Article  Google Scholar 

  • Bartels P, Von Tümpling W Jr (2007) Solar radiation 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 pharmaceutical in wastewater treatment plants of the largest industrial city of Korea. Sci Total Environ 409:4351–4360

    Article  CAS  Google Scholar 

  • Bort R, Macé K, Boobis A, Gómez-Lechón M-J, Pfeifer A, Castell J (1999) Hepatic metabolism of diclofenac: role of human CYP in the minor oxidative pathways. Biochem Pharmacol 58:787–796

    Article  CAS  Google Scholar 

  • Brozinski J-M, Lahti M, Meierjohann A, Oikari A, Kronberg L (2013) The anti-inflammatory drugs diclofenac, naproxen and ibuprofen are found in the bile of fish caught downstream of a wastewater treatment plant. Environ Sci Technol 47:342–348

    Article  CAS  Google Scholar 

  • Buchberger WW (2011) Current approaches to trace analysis of pharmaceuticals and personal care products in the environment. J Chromatogr A 1218:603–618

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Carlsson C, Johansson AK, Alvan G, Bergman K, Kühler T (2006) Are pharmaceuticals potent environmental pollutants? Sci Total Environ 364:67–87

    Article  CAS  Google Scholar 

  • Carrara C, Ptacek CJ, Robertson WD, Blowes DW, Moncur MC, Sverko E, Backus S (2008) Fate of pharmaceutical and trace organic compounds in three septic system plumes, Ontario, Canada. Environ Sci Technol 42:2805–2811

    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 40:357–363

    Article  CAS  Google Scholar 

  • Comoretto L, Chiron S (2005) Comparing pharmaceutical and pesticide loads into a small Mediterranean river. Sci Total Environ 349:201–210

    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 

  • Derksen JGM, Rijs GBJ, Jongbloed RH (2004) Diffuse pollution of surface water by pharmaceutical products. Water Sci Technol 49:213–221

    CAS  Google Scholar 

  • Destandau E, Vial J, Jardy A, Hennion M-C, Bonnet D, Lancelin P (2005) Development and validation of a reversed-phase liquid chromatography method for the quantitative determination of carboxylic acids in industrial reaction mixtures. J Chromatogr A 1088:49–56

    Article  CAS  Google Scholar 

  • Donner E, Kosjek T, Qualmann S, Kusk KO, Heath E, Revitt DM, Ledin A, Andersen HR (2013) Ecotoxicity of carbamazepine and its UV photolysis transformation products. Sci Total Environ 443:870–876

    Article  CAS  Google Scholar 

  • Farré M, Pérez S, Kantiani 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

    Article  Google Scholar 

  • Fatta D, Nikolaou A, Achilleos A, Meriç S (2007) Analytical methods for tracing pharmaceutical residues in water and wastewater. Trends Anal Chem 26:515–533

    Article  CAS  Google Scholar 

  • Finnish Medicines Agency Fimea and Social Insurance Institution (2013) Suomen lääketilasto/ Finnish Statistics on Medicines 2013. http://www.fimea.fi/download/27596_SLT_2013_net.pdf. Accessed 23 February 2015

  • Gebhardt W, Schröder HF (2007) Liquid chromatography–(tandem) mass spectrometry for the follow-up of the elimination of persistent pharmaceuticals during wastewater treatment applying biological wastewater treatment and advanced oxidation. J Chromatogr A 1160:34–43

    Article  CAS  Google Scholar 

  • Grenni P, Patrolecco L, Ademollo N, Di Lenola M, Caracciolo AB (2014) Capability of the natural microbial community in a river water ecosystem to degrade the drug naproxen. Environ Sci Pollut Res 21:13470–13479

    Article  CAS  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 

  • Gros M, Rodríguez-Mozaz S, Barceló D (2012) Fast and comprehensive multi-residue analysis of a broad range of human and veterinary pharmaceuticals and some of their metabolites in surface and treated waters by ultra-high-performance liquid chromatography coupled to quadrupole-linear ion trap tandem mass spectrometry. J Chromatogr A 1248:104–121

    Article  CAS  Google Scholar 

  • Heberer T (2002) Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicol Lett 131:5–17

    Article  CAS  Google Scholar 

  • HERTTA (2013) Environmental Information System, Finnish Environmental Institute

  • Käkölä J, Alén R (2006) A fast method for determining low-molecular-mass aliphatic carboxylic acids by high-performance liquid chromatography–atmospheric pressure chemical ionization mass spectrometry. J Sep Sci 29:1996–2003

    Article  Google Scholar 

  • Kallio J-M, Lahti M, Oikari A, Kronberg L (2010) Metabolites of the aquatic pollutant diclofenac in fish bile. Environ Sci Technol 44:7213–7219

    Article  CAS  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 U.S. Streams, 1999-2000: a national reconnaissance. Environ Sci Technol 36:1202–2011

    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 

  • Kümmerer K (2001) Pharmaceuticals in the environment—sources, fate, effect and risks. Springer, New York

    Google Scholar 

  • Larsen TA, Lienert J, Joss A, Siegrist H (2004) How to avoid pharmaceuticals in the aquatic environment. J Biotechnol 113:295–304

    Article  CAS  Google Scholar 

  • Li J, Dodgen L, Ye Q, Gan J (2013) Degradation kinetics and metabolites of carbamazepine in soil. Environ Sci Technol 47:3678–3684

    Article  CAS  Google Scholar 

  • Lin AY-C, Reinhard M (2005) Photodegradation of common environmental pharmaceuticals and estrogens in river water. Toxicol Environ Chem 24:1303–1305

    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  CAS  Google Scholar 

  • Lindholm-Lehto PC, Knuutinen JS, Ahkola HSJ, Herve SH (2015) 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 sewage and in receiving waters. Water Res 39:2219–2228

    Article  CAS  Google Scholar 

  • Loos R, Gawlik BM, Locoro G, Rimaviciute E, Contini S, Bidoglio G (2008) EU-wide survey of polar organic persistent pollutants in European river waters. Environ Pollut 157:561–568

    Article  Google Scholar 

  • López-Serna R, Pérez S, Ginebreda A, Petrović M, Barceló D (2010) Fully automated determination of 74 pharmaceuticals in environmental and waste waters by online solid phase extraction–liquid chromatography-electrospray–tandem mass spectrometry. Talanta 83:410–424

    Article  Google Scholar 

  • Massmann G, Dünnbier U, Heberer T, Taute T (2008) Behaviour and redox sensitivity of pharmaceutical residues during bank filtration—investigation of phenazone-type residues. Chemosphere 71:1476–1485

    Article  CAS  Google Scholar 

  • Mills GA, Vrana B, Allan I, Alvarez DA, Huckins JN, Greenwood R (2007) Trends in monitoring pharmaceuticals and personal-care products in the aquatic environment by use of passive sampling devices. Anal Bioanal Chem 387:1153–1157

    Article  CAS  Google Scholar 

  • Mompelat S, Le Bot B, Thomas O (2009) Occurrence and fate of pharmaceutical products and by-products, from resource to drinking water. Environ Int 35:803–814

    Article  CAS  Google Scholar 

  • Nikolaou A, Meric S, Fatta D (2007) Occurrence patterns of pharmaceuticals in water and wastewater environments. Anal Bioanal Chem 387:1225–1234

    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 Res 39:2654–2664

    Article  CAS  Google Scholar 

  • Santos JL, Aparicio I, Alonso E, Callejón M (2005) Simultaneous determination of pharmaceutically active compounds in wastewater samples by solid phase extraction and high-performance liquid chromatography with diode array and fluorescence detectors. Anal Chim Acta 550:116–122

    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 

  • Schwarzenbach RP, Escher BI, Fenner K, Hofstetter TB, Johnson CA, von Gunten U, Wehrli B (2006) The challenge of micropollutants in aquatic systems. Science 313:1072–1077

    Article  CAS  Google Scholar 

  • Seifrtová M, Nováková L, Lino C, Pena A, Solich P (2009) An overview of analytical methodologies for the determination of antibiotics in environmental waters. Anal Chim Acta 649:158–179

    Article  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 

  • Stumpf M, Ternes T, Wilken R-D, Rodrigues SV, Baumann W (1999) Polar drug residues in sewage and natural waters in the state of Rio de Janeiro, Brazil. Sci Total Environ 225:135–141

    Article  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Ternes TA, Stüber J, Herrmann N, McDowell D, Ried A, Kampmann M, Teiser B (2003) Ozonation: a tool for removal of pharmaceuticals, contrast media and musk fragrances from wastewater? Water Res 37:1976–1982

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Vieno N, Sillanpää M (2014) Fate of diclofenac in municipal wastewater treatment plant—a review. Environ Int 69:28–39

    Article  CAS  Google Scholar 

  • Vieno N, 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 

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

    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 

  • Weigel S, Berger U, Jensen E, Kallenborn R, Thoresen H, Hühnerfuss H (2004) Determination of selected pharmaceuticals and caffeine in sewage and seawater from Tromsø/Norway with emphasis on ibuprofen and its metabolites. Chemosphere 56:583–592

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors would like to acknowledge the financial support from Maa- ja vesitekniikan tuki ry.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Petra C. Lindholm-Lehto.

Additional information

Responsible editor: Roland Kallenborn

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. Occurrence of pharmaceuticals in municipal wastewater, in the recipient water, and sedimented particles of northern Lake Päijänne. Environ Sci Pollut Res 22, 17209–17223 (2015). https://doi.org/10.1007/s11356-015-4908-6

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-015-4908-6

Keywords

Navigation