Abstract
In the present study, the occurrence of 40 pharmaceuticals belonging to several therapeutic groups was investigated for the first time in hospital effluent, wastewater treatment plant influent and effluent, and seawater in Mahdia, Tunisia. Forty-six samples were collected within a 6-month sampling period. Pharmaceuticals were analyzed using solid-phase extraction followed by ultra-performance liquid chromatography-triple quadrupole mass spectrometry. Thirty-three out of the forty target compounds were detected over a wide concentration of ranges, from nanograms per liter to micrograms per liter, depending on the type of sample. Maximum values were detected for caffeine at 902 μgL−1 in hospital wastewater. This compound, as well as salicylic acid, sulfadiazine, and sulfamethizole, were detected in all samples. The average concentration of total pharmaceuticals in hospital wastewater (340 μgL−1) was higher than those detected in influent and effluent wastewater and seawater (275.11 and 0.2 μgL−1, respectively). Risk quotients (RQs) were also estimated to provide a preliminary environmental risk assessment and results revealed that sulfadiazine, sulfamethoxazole, and fluoxetine could pose medium/high risk to the tested aquatic organisms for maximum measured concentrations in wastewater (including hospital and WWTP samples). Although the measured environmental concentrations (MECs) detected in seawater samples might not pose a toxic effect to the aquatic organisms (except for salicylic acid, sulfamethoxazole and fluoxetine), further researches are needed due to the continuous release of wastewater in the environment and the limited efficiency of wastewater treatment processes.
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References
Afonso-Olivares C, Sosa-Ferrera Z, Santana-Rodríguez JJ (2017) Occurrence and environmental impact of pharmaceutical residues from conventional and natural wastewater treatment plants in Gran Canaria (Spain). Sci Total Environ 599–600:934–943. https://doi.org/10.1016/j.scitotenv.2017.05.058
Al Aukidy M, Verlicchi P, Voulvoulis N (2014) A framework for the assessment of the environmental risk posed by pharmaceuticals originating from hospital effluents. Sci Total Environ 493:54–64. https://doi.org/10.1016/j.scitotenv.2014.05.128
Al Qarni H, Collier P, O’Keeffe J, Akunna J (2016) Investigating the removal of some pharmaceutical compounds in hospital wastewater treatment plants operating in Saudi Arabia. Environ Sci Pollut Res 23(13):13003–13014. https://doi.org/10.1007/s11356-016-6389-7
Alygizakis NA, Gago-Ferrero P, Borova VL, Pavlidou A, Hatzianestis I, Thomaidis NS (2016) Occurrence and spatial distribution of 158 pharmaceuticals, drugs of abuse and related metabolites in offshore seawater. Sci Total Environ 541:1097–1105. https://doi.org/10.1016/j.scitotenv.2015.09.145
ARCHIPLAN-DGAT (2019) Rapport définitif de la 1ère phase de l’étude du Schéma Directeur d’Aménagement et du Développement du Gouvernorat de Mahdia. Janvier.
Arpin-Pont L, Bueno MJ, Gomez E, Fenet H (2016) Occurrence of PPCPs in the marine environment: a review. Environ Sci Pollut Res 23(6):4978–4991. https://doi.org/10.1007/s11356-014-3617-x
Baena-Nogueras RM, Pintado-Herrera MG, González-Mazo E, Lara-Martín PA (2016) Determination of pharmaceuticals in coastal systems using solid phase extraction (SPE) followed by ultra performance liquid chromatography—tandem mass spectrometry (UPLC-MS/MS). Curr Anal Chem 12(3):183–201
Benotti MJ, Brownawell BJ (2007) Distributions of pharmaceuticals in an urban estuary during both dry- and wet-weather conditions. Environ Sci Technol 41(16):5795–5802. https://doi.org/10.1021/es0629965
Benotti MJ, Brownawell BJ (2009) Microbial degradation of pharmaceuticals in estuarine and coastal seawater. Environ Pollut 157(3):994–1002. https://doi.org/10.1016/j.envpol.2008.10.009
Biel-Maeso M, Baena-Nogueras RM, Corada-Fernández C, Lara-Martín PA (2018) Occurrence, distribution and environmentalrisk of pharmaceutically active compounds (PhACs) in coastal and oceanwatersfromtheGulf of Cadiz (SW Spain). Sci Total Environ 612:649–659. https://doi.org/10.1016/j.scitotenv.2017.08.279
Buerge IJ, Poiger T, Müller MD, Buser HR (2003) Caffeine, an anthropogenic marker for wastewater contamination of surface waters. Environ Sci Technol 37(4):691–700. https://doi.org/10.1021/es020125z
Carraro E, Bonetta S, Bertino C, Lorenzi E, Bonetta S, Gilli G (2016) Hospital effluents management: Chemical, physical, microbiological risks and legislation in different countries. J Environ Manag 168:185–199. https://doi.org/10.1016/j.jenvman.2015.11.021
Coutu S, Wyrsch V, Wynn HK, Rossi L, Barry DA (2013) Temporal dynamics of antibiotics in wastewater treatment plant influent. Sci Total Environ 458:20–26. https://doi.org/10.1016/j.scitotenv.2013.04.017
Desbiolles F, Malleret L, Tiliacos C, Wong-Wah-Chung P, Laffont-Schwob I (2018) Occurrence and ecotoxicological assessment of pharmaceuticals: is there a risk for the Mediterranean aquatic environment? Sci Total Environ 639:1334–1348. https://doi.org/10.1016/j.scitotenv.2018.04.351
Ebele AJ, Abdallah MA, Harrad S (2017) Pharmaceuticals and personal care products (PPCPs) in the freshwater aquatic environment. Emerg Contam 3(1):1–16. https://doi.org/10.1016/j.emcon.2016.12.004
El Morhit M, Yagoubi M, Belmakki A, Zouhdi M (2015) Monthly physicochemical characterization of a hospital effluent according to technical and care activities (Avicenna Rabat-Morocco). World J Pharm Pharm Sci 4(4):247–267
El Tahiri M, Nejjari C, Benaabidate L, Benbrahim KF (2009) Caractérisation des effluents liquides de l’hôpital Al Ghassani, CHU Hassan II de Fès, Maroc. Techniques Hospitalières 64(714):47–50
Escher BI, Baumgartner R, Koller M, Treyer K, Lienert J, McArdell CS (2001) Environmental toxicology and risk assessment of pharmaceuticals from hospital wastewater. Water Res 45(1):75–92. https://doi.org/10.1016/j.watres.2010.08.019
Gao P, Ding Y, Li H, Xagoraraki I (2012) Occurrence of pharmaceuticals in a municipal wastewater treatment plant: mass balance and removal processes. Chemosphere 88(1):17–24. https://doi.org/10.1016/j.chemosphere.2012.02.017
Göbel A, McArdell CS, Suter MJ, Giger W (2004) Trace determination of macrolide and sulfonamide antimicrobials, a human sulphonamide metabolite, and trimethoprim in wastewater using liquid chromatography coupled to electrospray tandem mass spectrometry. Anal Chem 76(16):4756–4764. https://doi.org/10.1021/ac0496603
Golovko O, Kumar V, Fedorova G, Randak T, Grabic R (2014) Seasonal changes in antibiotics, antidepressants/psychiatric drugs, antihistamines and lipid regulators in a wastewater treatment plant. Chemosphere 111:418–426. https://doi.org/10.1016/j.chemosphere.2014.03.132
González-Moreno R, Rodríguez-Mozaz S, Huerta B, Barceló D, León VM (2016) Do pharmaceuticals bioaccumulate in marine molluscs and fish from a coastal lagoon? Environ Res 146:282–298. https://doi.org/10.1016/j.envres.2016.01.001
Harrabi M, DellaGiustina SV, Aloulou F, Rodriguez-Mozaz S, Barceló D, Elleuch B (2018) Analysis of multiclass antibiotic residues in urban wastewater in Tunisia. Environ Nanotechnol Monit Manag 10:163–170. https://doi.org/10.1016/j.enmm.2018.05.006
Heberer T (2002) Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicol Lett 131(1–2):5–17. https://doi.org/10.1016/S0378-4274(02)00041-3
Hedgespeth ML, Sapozhnikova Y, Pennington P, Clum A, Fairey A, Wirth E (2012) Pharmaceuticals and personal care products (PPCPs) in treated wastewater discharges into Charleston Harbor, South Carolina. Sci Total Environ 437:1–9. https://doi.org/10.1016/j.scitotenv.2012.07.076
Houda B, Dorra G, Chafai A, Emna A, Khaled M (2011) Impact of a mixed “industrial and domestic” wastewater effluent on the southern coastal sediments of Sfax (Tunisia) in the Mediterranean Sea. Int J Environ Res 5(3):691–704
Jelic A, Gros M, Ginebreda A, Cespedes-Sánchez R, Ventura F, Petrovic M, Barcelo D (2011) Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Res 45(3):1165–1176. https://doi.org/10.1016/j.watres.2010.11.010
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(6):1202–1211. https://doi.org/10.1021/es011055j
Kristofco LA, Brooks BW (2017) Global scanning of antihistamines in the environment: analysis of occurrence and hazards in aquatic systems. Sci Total Environ 592:477–487. https://doi.org/10.1016/j.scitotenv.2017.03.120
Kümmerer K (2001) Drugs in the environment: emission of drugs, diagnostic aids and disinfectants into wastewater by hospitals in relation to other sources—a review. Chemosphere 45(6–7):957–969. https://doi.org/10.1016/S0045-6535(01)00144-8
Lahti M, Brozinski JM, Segner H, Kronberg L, Oikari A (2012) Bioavailability of pharmaceuticals in waters close to wastewater treatment plants: use of fish bile for exposure assessment. Environ Toxicol Chem 31(8):1831–1837. https://doi.org/10.1002/etc.1879
Lindholm-Lehto PC, Ahkola HS, Knuutinen JS, Herve SH (2015) Occurrence of pharmaceuticals in municipal wastewater, in the recipient water, and sedimented particles of northern Lake Päijänne. Environ Sci Pollut Res 22(21):17209–17223. https://doi.org/10.1007/s11356-015-4908-6
Mazzitelli JY, Budzinski H, Cachot J, Geffard O, Marty P, Chiffre A, François A, Bonnafe E, Geret F (2018) Evaluation of psychiatric hospital wastewater toxicity: what is its impact on aquatic organisms. Environ Sci Pollut Res 25(26):26090–26102. https://doi.org/10.1007/s11356-018-2501-5
McEachran AD, Shea D, Bodnar W, Nichols EG (2016) Pharmaceutical occurrence in groundwater and surface waters in forests land-applied with municipal wastewater. Environ Toxicol Chem 35(4):898–905. https://doi.org/10.1002/etc.3216
Mendoza A, Aceña J, Pérez S, De Alda ML, Barceló D, Gil A, Valcárcel Y (2015) Pharmaceuticals and iodinated contrast media in a hospital wastewater: a case study to analyse their presence and characterise their environmental risk and hazard. Environ Res 140:225–241. https://doi.org/10.1016/j.envres.2015.04.003
Moslah B, Hapeshi E, Jrad A, Fatta-Kassinos D, Hedhili A (2018) Pharmaceuticals and illicit drugs in wastewater samples in north-eastern Tunisia. Environ Sci Pollut Res 25(19):18226–18241. https://doi.org/10.1007/s11356-017-8902-z
Muter O, Ingus P, Selga T, Berzins A, Gudra D, Radovica-Spalvina I, Fridmanis D, Bartkevics V (2017) Removal of pharmaceuticals from municipal wastewaters at laboratory scale by treatment with activated sludge and biostimulation. Sci Total Environ 584:402–413. https://doi.org/10.1016/j.scitotenv.2017.01.023
Nasri E, Machreki M, Beltifa A, Aroui S, Ghorbel A, Saad A, Feriani A, Borgi MA, Ghazouani L, Sire O, Balcázar JL (2017) Cytotoxic effects of seven Tunisian hospital wastewaters on the proliferation of human breast cancer cell line MDA-231: correlation with their chemical characterization. Environ Sci Pollut Res 24(25):20422–20428. https://doi.org/10.1007/s11356-017-9717-7
Osorio V, Larrañaga A, Aceña J, Pérez S, Barceló D (2016) Concentration and risk of pharmaceuticals in fresh water systems are related to the population density and the livestock units in Iberian Rivers. Sci Total Environ 540:267–277. https://doi.org/10.1016/j.scitotenv.2015.06.143
Packer JL, Werner JJ, Latch DE, McNeill K, Arnold WA (2003) Photochemicalfate of pharmaceuticals in the environment: naproxen, diclofenac, clofibricacid and ibuprofen. Aquat Sci 65:342–351. https://doi.org/10.1007/s00027-003-0671-8
Santos LH, Gros M, Rodriguez-Mozaz S, Delerue-Matos C, Pena A, Barcelo D, Montenegro MC (2013) Contribution of hospital effluents to the load of pharmaceuticals in urban wastewaters: identification of ecologically relevant pharmaceuticals. Sci Total Environ 461:302–316. https://doi.org/10.1016/j.scitotenv.2013.04.077
Simons FE, Simons KJ (2011) Histamine and H1-antihistamines: celebrating a century of progress. J Allergy Clin Immunol 128(6):1139–1150. https://doi.org/10.1016/j.jaci.2011.09.005
Tahrani L, Van Loco J, Ben Mansour H, Reyns T (2016) Occurrence of antibiotics in pharmaceutical industrial wastewater, wastewater treatment plant and sea waters in Tunisia. J Water Health 14(2):208–213
Tahrani L, Van Loco J, Anthonissen R, Verschaeve L, Ben Mansour H, Reyns T (2017) Identification and risk assessment of human and veterinary antibiotics in the wastewater treatment plants and the adjacent sea in Tunisia. Water Sci Technol 76(11):3000–3021
Togola A, Budzinski H (2008) Multi-residue analysis of pharmaceutical compounds in aqueous samples. J Chromatogr 1177(1):150–158. https://doi.org/10.1016/j.chroma.2007.10.105
Tran NH, Reinhard M, Gin KY (2018) Occurrence and fate of emerging contaminants in municipal wastewater treatment plants from different geographical regions—a review. Water Res 133:182–207. https://doi.org/10.1016/j.watres.2017.12.029
Verlicchi P, Zambello E (2016) Predicted and measured concentrations of pharmaceuticals in hospital effluents. Examination of the strengths and weaknesses of the two approaches through the analysis of a case study. Sci Total Environ 565:82–94. https://doi.org/10.1016/j.scitotenv.2016.04.165
Verlicchi P, Al Aukidy M, Galletti A, Petrovic M, Barceló D (2012a) Hospital effluent: Investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Sci Total Environ 430:109–118. https://doi.org/10.1016/j.scitotenv.2012.04.055
Verlicchi P, Al Aukidy M, Zambello E (2012b) Occurrence of pharmaceutical compounds in urban wastewater: removal, mass load and environmental risk after a secondary treatment—a review. Sci Total Environ 429:123–155. https://doi.org/10.1016/j.scitotenv.2012.04.028
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(21):8220–8226. https://doi.org/10.1021/es051124k
Weigel S, Kuhlmann J, Hühnerfuss H (2002) Drugs and personal care products as ubiquitous pollutants: occurrence and distribution of clofibric acid, caffeine and DEET in the North Sea. Sci Total Environ 295(1–3):131–141. https://doi.org/10.1016/S0048-9697(02)00064-5
WHO (2012) Pharmaceuticals in drinking-water [WWW Document]. WHO. http://www.who.int/water-sanitation-health/publications/2012/pharmaceuticals/en/. Accessed 2.20 Feb. 17.
Wille K, Noppe H, Verheyden K, Bussche JV, De Wulf E, Van Caeter P, Janssen CR, De Brabander HF, Vanhaecke L (2010) Validation and application of an LC-MS/MS method for the simultaneous quantification of 13 pharmaceuticals in seawater. Anal Bioanal Chem 397(5):1797–1808. https://doi.org/10.1007/s00216-010-3702-z
Yilmaz G, Kaya Y, Vergili I, Gönder ZB, Özhan G, Celik BO, Altinkum SM, Bagdatli Y, Boergers A, Tuerk J (2017) Characterization and toxicity of hospital wastewaters in Turkey. Environ Monit Assess 189(2):55. https://doi.org/10.1007/s10661-016-5732-2
Yu Y, Wu L, Chang AC (2013) Seasonal variation of endocrine disrupting compounds, pharmaceuticals and personal care products in wastewater treatment plants. Sci Total Environ 442:310–316. https://doi.org/10.1016/j.scitotenv.2012.10.001
Zhang R, Zhang G, Zheng Q, Tang J, Chen Y, Xu W, Zou Y, Chen X (2012) Occurrence and risks of antibiotics in the Laizhou Bay, China: impacts of river discharge. Ecotoxicol Environ Saf 80:208–215. https://doi.org/10.1016/j.ecoenv.2012.03.002
Zhang Y, Tian Z, Liu M, Shi ZJ, Hale L, Zhou J, Yang M (2015) High concentrations of the antibiotic spiramycin in wastewater lead to high abundance of ammonia-oxidizing archaea in Nitrifying Populations. Environ Sci Technol 49(15):9124–9132. https://doi.org/10.1021/acs.est.5b01293
Zheng Q, Zhang R, Wang Y, Pan X, Tang J, Zhang G (2012) Occurrence and distribution of antibiotics in the Beibu Gulf, China: impacts of river discharge and aquaculture activities. Mar Environ Res 78:26–33. https://doi.org/10.1016/j.marenvres.2012.03.007
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Afsa, S., Hamden, K., Lara Martin, P.A. et al. Occurrence of 40 pharmaceutically active compounds in hospital and urban wastewaters and their contribution to Mahdia coastal seawater contamination. Environ Sci Pollut Res 27, 1941–1955 (2020). https://doi.org/10.1007/s11356-019-06866-5
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DOI: https://doi.org/10.1007/s11356-019-06866-5