Abstract
This work determines the principal environmental pollution pathways of pharmaceuticals on the island of Mallorca (Spain). The evaluation was made on the basis of the quantification of pharmaceutical residues by liquid chromatography–tandem mass spectrometry in several environmental water samples, including wastewater-treatment plant effluents, municipal solid waste landfill leachates, groundwater (GW), and marine water. An overall set of 19 pharmaceuticals has been identified in the environment of the 27 human pharmaceuticals investigated in this study. WWTP effluents are the main source of discharge of the pharmaceuticals into the aquatic environment. The data indicate that reuse of treated domestic wastewater for irrigation (which supplies some 30 % of the total water demand in Mallorca) contributes to the contamination of GW. In addition, leaching from landfills is identified as another, but minor, possible source of introduction of pharmaceuticals to GW aquifers. Finally, WWTP effluents ending in the Mediterranean Sea, primarily highly urbanized coastal areas, cause pharmaceutical residues to occur in marine water bodies.
Similar content being viewed by others
References
Adrover M, Farrús E, Moyà G, Vadell J (2012) Chemical properties and biological activity in soils of Mallorca following twenty years of treated wastewater irrigation. J Environ Manage 95(Suppl):S188–S192
Balearic Islands Government, Ministry of Tourism and Sports (2010) In: Agency BIT (ed) Tourism in the Balearic Islands. Annual Report
Barnes KK, Christenson SC, Kolpin DW, Focazio MJ, Furlong ET, Zaugg SD et al (2004) Pharmaceuticals and other organic waste water contaminants within a leachate plume downgradient of a municipal landfill. Ground Water Monit Remediat 24:119–126
Baumard P, Budzinski H, Garrigues P (1998) Polycyclic aromatic hydrocarbons in sediments and mussels of the western Mediterranean sea. Environ Toxicol Chem 17:765–776
Buszka P, Yeskis D, Kolpin D, Furlong E, Zaugg S, Meyer M (2009) Waste-indicator and pharmaceutical compounds in landfill-leachate-affected ground water near Elkhart, Indiana, 2000–2002. Bull Environ Contam Toxicol 82:653–659
Celiz MD, Tso J, Aga DS (2009) Pharmaceutical metabolites in the environment: analytical challenges and ecological risks. Environ Toxicol Chem 28:2473–2484
Deudero S, Box A, March D, Valencia JM, Grau AM, Tintore J et al (2007) Organic compounds temporal trends at some invertebrate species from the Balearics, Western Mediterranean. Chemosphere 68:1650–1659
Díaz-Cruz MS, Barceló D (2008) Trace organic chemicals contamination in ground water recharge. Chemosphere 72:333–342
Eggen T, Moeder M, Arukwe A (2010) Municipal landfill leachates: a significant source for new and emerging pollutants. Sci Total Environ 408:5147–5157
Essex S, Kent M, Newnham R (2004) Tourism development in Mallorca: is water supply a constraint? J Sustain Tourism 12:4–28
European Environmental Agency (1999) Council directive 1999/31/679/EC of 26 April on the landfill of waste. Report from the EU Commission, Brussels
Farré ML, 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
Giger W (2009) Hydrophilic and amphiphilic water pollutants: using advanced analytical methods for classic and emerging contaminants. Anal Bioanal Chem 393:37–44
Gómez MJ, Petrović M, Fernández-Alba AR, Barceló D (2006) Determination of pharmaceuticals of various therapeutic classes by solid-phase extraction and liquid chromatography–tandem mass spectrometry analysis in hospital effluent wastewaters. J Chromatogr A 1114:224–233
Gómez MJ, Martínez Bueno MJ, Lacorte S, Fernández-Alba AR, Agüera A (2007) Pilot survey monitoring pharmaceuticals and related compounds in a sewage treatment plant located on the Mediterranean coast. Chemosphere 66:993–1002
González Alonso S, Catalá M, Maroto RR, Gil JLR, de Miguel ÁG, Valcárcel Y (2010) Pollution by psychoactive pharmaceuticals in the Rivers of Madrid metropolitan area (Spain). Environ Int 36:195–201
Gracia-Lor E, Sancho JV, Hernández F (2010) Simultaneous determination of acidic, neutral and basic pharmaceuticals in urban wastewater by ultra high-pressure liquid chromatography-tandem mass spectrometry. J Chromatogr A 1217:622–632
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—a review. Chemosphere 36:357–393
Halling-Sørensen B, Lützhøft H-CH, Andersen HR, Ingerslev F (2000) Environmental risk assessment of antibiotics: comparison of mecillinam, trimethoprim and ciprofloxacin. J Antimicrob Chemother 46:53–58
Hansen M, Krogh KA, Halling-Sorensen B, Bjorklund E (2011) Determination of ten steroid hormones in animal waste manure and agricultural soil using inverse and integrated clean-up pressurized liquid extraction and gas chromatography-tandem mass spectrometry. Anal Methods 3:1087–1095
Heim S, Schwarzbauer J, Littke R (2004) Monitoring of waste deposit derived groundwater contamination with organic tracers. Environ Chem Lett 2:21–25
Holm JV, Ruegge K, Bjerg PL, Christensen TH (1995) Occurrence and distribution of pharmaceutical organic compounds in the groundwater downgradient of a landfill (Grindsted, Denmark). Environ Sci Technol 29:1415–1420
Huerta-Fontela M, Galceran MT, Ventura F (2010) Fast liquid chromatography–quadrupole-linear ion trap mass spectrometry for the analysis of pharmaceuticals and hormones in water resources. J Chromatogr A 1217:4212–4222
Jelić A, Petrović M, Barceló D (2012) Pharmaceuticals in drinking water. Springer, Berlin, pp 1–24
Kuster M, López de Alda MJ, Hernando MD, Petrovic M, Martín-Alonso J, Barceló D (2008) 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). J Hydrol 358:112–123
Luthy RG, Aiken GR, Brusseau ML, Cunningham SD, Gschwend PM, Pignatello JJ et al (1997) Sequestration of hydrophobic organic contaminants by geosorbents. Environ Sci Technol 31:3341–3347
Mateos-Ruiz RM, Lopez-Garcia JM (2003) Retroceso de la intrusión marina debido a la substitución de aguas subterráneas por aguas residuales tratadas para el regadío de una zona agrícola. El Pla de Sant Jordi. Tecnología de la intrusión de agua de mar en los acuíferos costeros: Países mediterráneos. IGME, Madrid
Murray KE, Thomas SM, Bodour AA (2010) Prioritizing research for trace pollutants and emerging contaminants in the freshwater environment. Environ Pollut 158:3462–3471
Nieto A, Borrull F, Pocurull E, Marcé RM (2010) Pressurized liquid extraction: a useful technique to extract pharmaceuticals and personal-care products from sewage sludge. Trends Anal Chem 29:752–764
Oppel J, Broll G, Löffler D, Meller M, Römbke J, Ternes T (2004) Leaching behaviour of pharmaceuticals in soil-testing-systems: a part of an environmental risk assessment for groundwater protection. Sci Total Environ 328:265–273
Pennsylvania Department of Environmental Protection (2005) Environmental Science DatabaseSRC (2005) PhysProp. Organic regulated substances physical and toxicological properties
Pérez-Carrera E, Hansen M, León V, Björklund E, Krogh K, Halling-Sørensen B et al (2010) Multiresidue method for the determination of 32 human and veterinary pharmaceuticals in soil and sediment by pressurized-liquid extraction and LC-MS/MS. Anal Bioanal Chem 398:1173–1184
Richardson SD, Ternes TA (2011) Water analysis: emerging contaminants and current issues. Anal Chem 83:4614–4648
Rodriguez-Navas C, Forteza R, Cerdà V (2012) Use of thermal desorption–gas chromatography–mass spectrometry (TD-GC-MS) on identification of odorant emission focus by volatile organic compounds characterisation. Chemosphere 89:1426–1436
Rodríguez-Navas C, Björklund E, Forteza R, Cerdà V (2012) Volatile organic compounds in landfill odorant emissions on the island of Mallorca. Int J Environ Anal Chem 92:1–16
Runnqvist H, Bak SA, Hansen M, Styrishave B, Halling-Sørensen B, Björklund E (2010) Determination of pharmaceuticals in environmental and biological matrices using pressurised liquid extraction—are we developing sound extraction methods? J Chromatogr A 1217:2447–2470
Schwarzbauer J, Heim S, Brinker S, Littke R (2002) Occurrence and alteration of organic contaminants in seepage and leakage water from a waste deposit landfill. Water Res 36:2275–2287
Simó R, Colom-Altés M, Grimalt JO, Albaigés J (1991) Background levels of atmospheric hydrocarbons, sulphate and nitrate over the western Mediterranean. Atmos Environ A Gen Top 25:1463–1471
Thiele-Bruhn S (2003) Pharmaceutical antibiotic compounds in soils—a review. J Plant Nutr Soil Sci 166:145–167
Verlicchi P, Galletti A, Petrovic M, Barceló D (2010) Hospital effluents as a source of emerging pollutants: an overview of micropollutants and sustainable treatment options. J Hydrol 389:416–428
World Health Organization: Drinking-water Quality Committee (2011) Pharmaceuticals in drinking water. WHO, Geneva
Zhou JL, Zhang ZL, Banks E, Grover D, Jiang JQ (2009) Pharmaceutical residues in wastewater treatment works effluents and their impact on receiving river water. J Hazard Mater 166:655–661
Acknowledgments
The authors acknowledge economic support from the Spanish Ministry of Science and Innovation by the Predoctoral Grant No. BES-2008-003354 and by Project CTQ 2010-15541 as well as the economic support from the Balearic Islands Government. The kind collaboration of all personnel at the waste-management companies involved in this work is sincerely acknowledged.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Rodríguez-Navas, C., Björklund, E., Bak, S.A. et al. Pollution Pathways of Pharmaceutical Residues in the Aquatic Environment on the Island of Mallorca, Spain. Arch Environ Contam Toxicol 65, 56–66 (2013). https://doi.org/10.1007/s00244-013-9880-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s00244-013-9880-x