This paper describes the presence of 33 pharmaceuticals and hormones in waters from two sewage treatment plants (STPs) situated in Catalonia, in northeastern Spain. The target compounds were one psychoactive stimulant, one antiepileptic, four analgesics and non-steroidal anti-inflammatories, one lipid regulators, two anti-ulcer agents, nine antibiotics (sulfonamides and macrolides), two beta-blockers, two metabolites, and 11 hormones (free and conjugates). The determination was performed using liquid chromatography coupled to tandem mass spectrometry after enrichment by solid-phase extraction with Oasis HLB sorbent. Most of the pharmaceuticals were found in both influent and effluent samples from the two STPs. The most frequently detected were caffeine, acetaminophen, carbamazepine, diclofenac, ibuprofen, naproxen, sulfamethoxazole, sulfapyridine, sulfathiazole, ranitidine, omeprazole, estrone 3-sulfate, and estradiol 17-glucuronide. Specifically, the highest concentrations found in influents were 19,850 ng/L (acetaminophen), 9,945 ng/L (caffeine), 4,215 ng/L (ibuprofen), 5,695 ng/L (sulfamethoxazole), and 5,140 ng/L (sulfathiazole). Most of the pharmaceuticals present in influent waters were found in effluents at lower concentrations. The highest concentrations in effluents were 970 ng/L (caffeine), 670 ng/L (sulfamethoxazole), 510 ng/L (bezafibrate), and 1,032 ng/L (diclofenac).
This is a preview of subscription content, log in to check access.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
Tax calculation will be finalised during checkout.
Auriol, M., Filali-Meknassi, Y., Tyagi, R. D., Adams, C. D., & Surampalli, R. Y. (2006). Endocrine disrupting compounds removal from wastewater, a new challenge. Process Biochem, 41, 525–539.
Baquero, F., Martínez, J. L., & Cantón, R. (2008). Antibiotics and antibiotic resistance in water environments. Curr Opin Biotechnol, 19, 260–265.
Benítez, F. J., Real, F. J., Acero, J. L., & Roldan, G. (2009). Removal of selected pharmaceuticals in waters by photochemical processes. J Chem Technol Biotechnol, 84, 1186–1195.
Benner, J., & Ternes, T. A. (2009). Ozonation of metoprolol: Elucidation of oxidation pathways and major oxidation products. Environ Sci Technol, 43, 5472–5480.
Benotti, M. J., Trenholm, R. A., Vanderford, B. J., Holady, J. C., Stanford, B. D., & Snyder, S. A. (2009). Pharmaceuticals and endocrine disrupting compounds in U.S. drinking water. Environ Sci Technol, 43, 597–603.
Bolong, N., Ismail, A. F., Salim, M. R., & Matsuura, T. (2009). A review of the effects of emerging contaminants in wastewater and options for their removal. Desalination, 239, 229–246.
Coetsier, C., Lin, L., Roig, B., & Touraud, E. (2007). Integrated approach to the problem of pharmaceutical products in the environment: An overview. Anal Bioanal Chem, 387, 1163–1166.
Conley, J. M., Symes, S. J., Kindelberger, S. A., & Richards, S. M. (2008). Rapid liquid chromatography–tandem mass spectrometry method for the determination of a broad mixture of pharmaceuticals in surface water. J Chromatogr A, 1185, 206–215.
Díaz-Cruz, M. S., García-Galán, M. J., & Barceló, D. (2008). Highly sensitive simultaneous determination of sulfonamide antibiotics and one metabolite in environmental waters by liquid chromatography-quadrupole linear ion trap-mass spectrometry. J Chromatogr A, 1193, 50–59.
Ding, J., Ren, N., Chen, L., & Ding, L. (2009). On-line coupling of solid-phase extraction to liquid-chromatography–tandem mass spectrometry for the determination of macrolide antibiotics in environmental water. Anal Chim Acta, 364, 215–221.
Farré, M., Brix, R., Kuster, M., Rubio, F., Goda, Y., López de Alda, M. J., et al. (2006). Evaluation of commercial immunoassays for the detection of estrogens in water by comparison with high-performance liquid chromatography tandem mass spectrometry HPLC-MS/MS (QqQ). Anal Bioanal Chem, 385, 1001–1011.
Farré, M., Gros, M., Hernández, B., Petrovic, M., Hancock, P., & Barceló, D. (2008a). Analysis of biologically active compounds in water by ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry. Rapid Commun Mass Spectrom, 22, 41–51.
Farré, M., Petrovic, M., Gros, M., Kosjek, T., Martínez, E., Heath, E., et al. (2008b). First interlaboratory exercise on non-steroidal anti-inflammatory drugs analysis in environmental samples. Talanta, 76, 580–590.
Gagnoc, C., & Lajeunesse, A. (2008). Persistence and fate of highly soluble pharmaceutical products in various types of municipal wastewater treatment plants. Waste Manag Environ IV, 109, 799–807.
Gebhardt, W., & Schroder, H. F. (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.
Göbel, A., Ardell, C. S. M., Suter, M., & Giger, W. (2004). Trace determination of macrolide and sulfonamide antimicrobial, a human sulfonamide metabolite, and trimethoprim in wastewater using liquid chromatography coupled to electrospray tandem mass spectrometry. Anal Chem, 76, 4756–4764.
Gros, M., Petrovic, M., & Barceló, D. (2006). Multi-residue analytical methods using LC-tandem MS for the determination of pharmaceuticals in environmental and wastewater samples: A review. Anal Bioanal Chem, 386, 941–952.
Gros, M., Pizzolato, T. M., Petrovic, M., López de Alda, M. J., & Barceló, D. (2008). Trace level determination of β-blockers in waste waters by highly selective molecularly imprinted polymers extraction followed by liquid chromatography-quadrupole-linear ion trap mass spectrometry. J Chromatogr A, 1189, 374–384.
Gros, M., Petrovic, M., & Barceló, D. (2009). Tracing pharmaceutical residues of different therapeutic classes in environmental waters by using liquid chromatography/quadrupole-linear ion trap mass spectrometry and automated library searching. Anal Chem, 81, 898–912.
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.
Hernández, F., Sancho, J. V., Ibañez, M., & Guerrero, C. (2007). Antibiotic residue determination in environmental waters by LC-MS. Trends Anal Chem, 26, 466–485.
Hernando, M. D., Mezcua, M., Gómez, M. J., Malato, O., Aguera, A., & Fernández-Alba, A. R. (2004). Comparative study of analytical methods involving gas chromatography–mass spectrometry after derivatization and gas chromatography–tandem mass spectrometry for the determination of selected endocrine disrupting compounds in wastewaters. J Chromatogr A, 1047, 129–135.
Hernando, M. D., Heat, E., Petrovic, M., & Barceló, D. (2006). Trace-level determination of pharmaceutical residues by LC-MS-MS in natural and treated waters. A pilot-survey study. Anal Bioanal Chem, 385, 985–991.
Hilton, M. J., & Thomas, K. V. (2003). Determination of selected human pharmaceutical compounds in effluent and surface water samples by high-performance liquid chromatography–electrospray tandem mass spectrometry. J Chromatogr A, 1015, 129–141.
Huerta-Fontela, M., Galceran, M. T., Martín-Alonso, J., & Ventura, F. (2008). Occurrence of psychoactive stimulatory drugs in wastewaters in north-eastern Spain. Sci Total Environ, 397, 31–40.
Karthikeyan, K. G., & Meyer, M. T. (2006). Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ, 361, 196–207.
Khalaf, H., Salste, L., Karlsson, P., Ivarsson, P., Jass, J., & Olsson, P. E. (2009). In vitro analysis of inflammatory responses following environmental exposure to pharmaceuticals and inland waters. Sci Total Environ, 407, 1452–1460.
Kuster, M., López de Alda, M. J., Hernando, M. D., Petrovic, M., Martín-Alonso, J., & Barceló, D. (2008). Analysis and occurrence of pharmaceuticals, estrogens, progestrogens and polar pesticides in sewage treatment plant effluents, river water and drinking water in the Llobregat river basin (Barcelona, Spain). J Hidrol, 358, 112–123.
Kvanli, D. M., Marisetty, S., Anderson, T. A., Jackson, W. A., & Morse, A. N. (2008). Monitoring estrogen compounds in wastewater recycling systems. Water Air Soil Pollut, 188, 31–40.
Lacey, C., McMahon, G., Bones, J., Barron, L., Morrissey, A., & Tobin, J. M. (2008). An LC-MS method for the determination of pharmaceutical compounds in wastewater treatment plant influent and effluent samples. Talanta, 75, 1089–1097.
Managaki, S., Murata, A., Takada, H., Tuyen, B. C., & Chiem, N. H. (2007). Distribution of macrolides, sulfonamides, and trimethoprim in tropical waters: Ubiquitous occurrence of veterinary antibiotics in the Mekong Delta. Environ Sci Technol, 41, 8004–8010.
Nakada, N., Shinohara, H., Murata, A., Kiri, K., Managaki, S., Sato, N., et al. (2007). Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant. Water Res, 41, 4373–4382.
Nieto, A., Borrull, F., Pocurull, E., & Marcé, R. M. (2008). Determination of natural and synthetic estrogens and their conjugates in sewage sludge by pressurized liquid extraction and liquid chromatography–tandem mass spectrometry. J Chromatogr A, 1213, 224–230.
Nikolaou, A., Meric, S., & Fatta, D. (2007). Occurrence patterns of pharmaceuticals in water and wastewater environments. Anal Bioanal Chem, 387, 1225–1234.
Pedrouzo, M., Reverté, S., Borrull, F., Pocurull, E., & Marcé, R. M. (2007). Pharmaceutical determination in surface and wastewaters using high-performance liquid chromatography–(electrospray)-mass spectrometry. J Sep Sci, 30, 297–303.
Pedrouzo, M., Borrull, F., Marcé, R. M., & Pocurull, E. (2008). Simultaneous determination of macrolides, sulfonamides, and other pharmaceuticals in water samples by solid-phase extraction and LC-(ESI)MS. J Sep Sci, 31, 2182–2188.
Pedrouzo, M., Borrull, F., Pocurull, E., & Marcé, R. M. (2009). Estrogens and their conjugates: Determination in water samples by solid-phase extraction and liquid chromatography–tandem mass spectrometry. Talanta, 78, 1327–1331.
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.
Radjenovic, J., Petrovic, M., Ventura, F., & Barceló, D. (2008). Rejection of pharmaceuticals in nanofiltration and reverse osmosis membrane drinking water treatment. Water Res, 42, 3601–3610.
Rodríguez-Mozaz, S., López de Alda, M. J., & Barceló, D. (2004). Picogram per liter level determination of estrogens in natural waters and waterworks by a fully automated on-line solid-phase extraction-liquid chromatography–electrospray tandem mass spectrometry method. Anal Chem, 76, 6998–7006.
Servos, M. R., Bennie, D. T., Burnison, B. K., Jurkovic, A., McInnis, R., Neheli, T., et al. (2005). Distribution of estrogens, 17β-estradiol and estrone, in Canadian municipal wastewater treatment plants. Sci Total Environ, 336, 155–170.
Sponberg, A. L., & Witter, J. D. (2008). Pharmaceutical compounds in the wastewater process stream in northwest Ohio. Sci Total Environ, 397, 148–157.
Ternes, T. A., Bonerz, M., Herrmann, N., Teiser, B., & Andersen, H. R. (2007). Irrigation of treated wastewater in Braunschweig, Germany: An option to remove pharmaceuticals and musk fragrances. Chemosphere, 66, 894–904.
Tixier, C., Singer, H. P., Oellers, S., & Müller, S. (2003). Occurrence and fate of carbamazepine, clofibric acid, diclofenac, ibuprofen, ketoprofen, and naproxen in surface waters. Environ Sci Technol, 37, 1061–1068.
Vanderford, B. J., & Snyder, S. A. (2006). Analysis of pharmaceuticals in water by isotope dilution liquid chromatography/tandem mass spectrometry. Environ Sci Technol, 40, 7312–7320.
Viglino, L., Aboulfadl, K., Prévost, M., & Sauvé, S. (2008). Analysis of natural and synthetic estrogenic endocrine disruptors in environmental waters using online preconcentration coupled with LC-APPI-MS/MS. Talanta, 76, 1088–1096.
Vulliet, E., Wiest, L., Baudot, R., & Grenier-Loustalot, M. F. (2008). Multi-residue analysis of steroids at sub-ng/L levels in surface and ground-waters using liquid chromatography coupled to tandem mass spectrometry. J Chromatogr A, 1210, 84–91.
Wu, C., Spongberg, A. L., & Witter, J. D. (2008). Use of solid phase extraction and liquid chromatography–tandem mass spectrometry for simultaneous determination of various pharmaceuticals in surface water. Int J Environ Anal Chem, 88, 1033–1048.
Xu, X., Roman, J. M., Veenstra, T. D., Van Anda, J., Ziegler, R. G., & Issaq, H. J. (2006). Analysis of fifteen estrogen metabolites using packed column supercritical fluid chromatography–mass spectrometry. Anal Chem, 78, 1553–1558.
Ye, Z., & Weinberg, H. S. (2007). Trace analysis of trimethoprim and sulfonamide, macrolide, quinolone and tetracycline antibiotics in chlorinated drinking water using liquid chromatography electrospray tandem mass spectrometry. Anal Chem, 79, 1135–1144.
Zhao, X., & Metcalfe, C. D. (2008). Characterizing and compensating for matrix effects using atmospheric pressure chemical ionization liquid chromatography–tandem mass spectrometry: Analysis of neutral pharmaceuticals in wastewater. Anal Chem, 80, 2010–2017.
Zhou, J. L., Zhang, Z. L., Banks, E., Grover, D., & Jiang, J. Q. (2009). Pharmaceutical residues in wastewater treatment works effluents and their impact on receiving river water. J Hazard Mater, 166, 655–661.
Zwiener, C. (2007). Occurrence and analysis of pharmaceuticals and their transformation products in drinking water treatment. Anal Bioanal Chem, 387, 1159–1162.
This study was funded by the Dirección General de Investigación of the Ministry of Science and Technology, project CTM2008-06847-C02-01/TECNO. The authors wish to thank the personnel of the sewage treatment plants for the sampling facilities.
About this article
Cite this article
Pedrouzo, M., Borrull, F., Pocurull, E. et al. Presence of Pharmaceuticals and Hormones in Waters from Sewage Treatment Plants. Water Air Soil Pollut 217, 267–281 (2011). https://doi.org/10.1007/s11270-010-0585-8