Abstract
The present study deals with the assessment of the fate of an emerging contaminant (diclofenac), present in the subsurface environment at specific concentration levels, and its biodegradation potential under different environmental configurations. Diclofenac is a widely consumed nonsteroidal anti-inflammatory drug used as a painkiller prescribed as pills or ointments and among the most frequently detected pharmaceuticals in wastewater treatment plants’ effluents. Fermentative/methanogenic cultures were enriched from previously contaminated sediment samples. Although partial biodegradation was achieved in all enrichment cultures, complete degradation was not observed. The results reflected that less than 6% of the diclofenac sorbed on the solid phase and the rest was either biotransformed (25–40%) or remained in the liquid phase (55–70%) at the end of 45-day incubation period. Although partial cometabolic degradation of diclofenac occurred in the presence of glucose, biodegradation was not observed in the presence of readily biodegradable carbon source (i.e., acetate). Diclofenac concentration up to 1000 µg/L did not affect the methanogenic activity of the enriched culture. The results of this study will have a significant impact in the designation of the permitted concentration limits of diclofenac before the discharge through wastewater treatment plants.
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References
APHA (2005) Standard methods for the examination of water and wastewater, 21st edn. American Public Health Association, American Water Works Association/Water Environment Federation, Washington, DC
Aydin E, Talinli I (2013) Analysis, occurrence and fate of commonly used pharmaceuticals and hormones in the Buyukcekmece Watershed, Turkey. Chemosphere 90:2004–2012
Calasan J, Mijatovic V, Horvat O, Varga J, Sabo A, Stilinovic N (2011) The outpatient utilization of non-steroidal anti-inflammatory drugs in South Backa District, Serbia. Int J Clin Pharm 33:246–251
Chang HL, Alvarez-Cohen L (1995) Model for the cometabolic biodegradation of chlorinated organics. Environ Sci Technol 29(9):2357–2367
Corada-Fernández C, Jiménez-Martínez J, Candela L, González-Mazo E, Lara-Martín PA (2015) Occurrence and spatial distribution of emerging contaminants in the unsaturated zone. Case study: Guadalete River basin (Cadiz, Spain). Chemosphere 119:S131–S137
EC (2012) Report from the commission to the European Parliament and the Council on the outcome of the review of Annex X to Directive 2000/60/EC of the European Parliament and of the Council on priority substances in the field of water policy. http://ec.europa.eu/environment/water/water-dangersub/pdf/com_2011_875.pdf. Accessed Jan 2015
Einsiedl F, Radke M, Maloszewski P (2010) Occurrence and transport of pharmaceuticals in a karst groundwater system affected by domestic wastewater treatment plants. J Contam Hydrol 117(1–4):26–36
EU (2015) Commission implementing decision (EU) 2015/495 of 20 March 2015. Establishing a watch list of substances for Union-wide monitoring in the field of water policy pursuant to Directive 2008/105/EC of the European Parliament and of the Council. http://eur-lex.europa.eu/legal-content/EN/TXT/?uri=uriserv%3AOJ.L_.2015.078.01.0040.01.ENG. Accessed Feb 2017
Fatta-Kassinos D, Hapeshi E, Achilleos A, Meric S, Gros M, Petrovic M, Barcelo D (2011) Existence of pharmaceutical compounds in tertiary treated urban wastewater that is utilized for reuse applications. Water Resour Manag 25:1183–1193
Fountoulakis M, Drillia P, Stamatelatou K, Lyberatos G (2004) Toxic effect of pharmaceuticals on methanogenesis. Water Sci Technol 50(5):335–340
Jelic A, Gros M, Ginebreda A, Cespedes-Sanchez R, Ventura F, Petrovic M, Barcelo D (2011) Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment. Water Res 45:1165–1176
Kimura K, Hara H, Watanabe Y (2007) Elimination of selected acidic pharmaceuticals from municipal wastewater by an activated sludge system and membrane bioreactors. Environ Sci Technol 41:3708–3714
Kunkel U, Radke M (2012) Fate of pharmaceuticals in rivers: deriving a benchmark dataset at favorable attenuation conditions. Water Res 46(17):5551–5565
Lahti M, Oikari A (2011) Microbial transformation of pharmaceuticals naproxen, bisoprolol, and diclofenac in aerobic and anaerobic environments. Arch Environ Contam Toxicol 61:202–210
Li J, Dodgen L, Ye Q, Gan J (2013) Degradation kinetics and metabolites of carbamazepine in soil. Environ Sci Technol 47(8):3678–3684
Oaks JL, Gilbert M, Virani MZ, Watson RT, Meteyer CU, Rideout BA, Shivaprasad HL, Ahmed S, Chaudhry MJ, Arshad M, Mahmood S, Ali A, Khan AA (2004) Diclofenac residues as the cause of vulture population decline in Pakistan. Nature 427:630–633
Okutman Tas D, Pavlostathis SG (2007) The influence of iron reduction on the reductive biotransformation of pentachloronitrobenzene. Eur J Soil Biol 43:264–275
Okutman Tas D, Pavlostathis SG (2010) Microbial transformation of pentachloronitrobenzene under nitrate reducing conditions. Biodegradation 21:691–702
Onesios KM, Bouwer EJ (2012) Biological removal of pharmaceuticals and personal care products during laboratory soil aquifer treatment simulation with different primary substrate concentrations. Water Res 46(7):2365–2375
Ozdemir G, Aydin E, Topuz E, Yangin-Gomec C, Okutman-Tas D (2015) Acute and chronic responses of denitrifying culture to diclofenac. Bioresour Technol 176:112–120
Pasquini L, Merlin L, Hassenboehler C, Munoz JF, Pons MN, Görner T (2013) Impact of certain household micropollutants on bacterial behavior toxicity tests/study of extracellular polymeric substances in sludge. Sci Total Environ 463–464:355–365
Queiroz FB, Brandt EMF, Aquino SF, Chernicharo CAL, Afonso RJCF (2012) Occurrence of pharmaceuticals and endocrine disruptors in raw sewage and their behavior in UASB reactors operated at different hydraulic retention times. Water Sci Technol 66(12):2562–2569
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
Rozman D, Hrkal Z, Eckhardt P, Novotná E, Boukalová Z (2015) Pharmaceuticals in groundwaters: a case study of the psychiatric hospital at Horní Beřkovice, Czech Republic. Environ Earth Sci 73(7):3775–3784
Sari S, Ozdemir G, Yangin Gömec C, Zengin GE, Topuz E, Aydin E, Pehlivanoglu-Mantas E, Okutman Tas D (2014) Seasonal variation of diclofenac concentration and its relation with wastewater characteristics at two municipal wastewater treatment plants in Turkey. J Hazard Mater 272:155–164
Schwaiger J, Ferling H, Mallow U, Wintermayr H, Negele RD (2004) Toxic effects of the non-steroidal anti-inflammatory drug diclofenac. Part I: histopathological alterations and bioaccumulation in rainbow trout. Aquat Toxicol 68:141–150
Sui Q, Huang J, Deng S, Chen W, Yu G (2011) Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in different biological wastewater treatment processes. Environ Sci Technol 45:3341–3348
Symsaris EC, Fotidis IA, Stasinakis AS, Angelidaki I (2015) Effects of triclosan, diclofenac, and nonylphenol on mesophilic and thermophilic methanogenic activity and on the methanogenic communities. J Hazard Mater 291:45–51
Syracuse Research Corporation Physprop database (2010) PhysProp Database, Environmental Science Center: Syracuse, NY. http://www.syrres.com. Accessed Nov 2015
Ternes TA, Bonerz M, Herrmann N, Teiser B, Andersen HR (2007) Irrigation of treated wastewater in Braunschweig, Germany: an option to remove pharmaceuticals and musk fragrances. Chemosphere 66(5):894–904
Topuz E, Sari S, Ozdemir G, Aydin E, Pehlivanoglu-Mantas E, Okutman Tas D (2014) Optimization of diclofenac quantification from wastewater treatment plant sludge by ultrasonication assisted extraction. J Chromatogr B 958:48–54
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This work was funded by the Scientific and Technological Research Council of Turkey (TUBITAK, Project # 110Y319) and Istanbul Technical University, Scientific Research Projects Fund (Project # 36258).
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Tas, D.O., Sari, S., Aydın, E. et al. Fate and biodegradability potential of an emerging micropollutant diclofenac in subsurface environment. Int. J. Environ. Sci. Technol. 15, 1201–1210 (2018). https://doi.org/10.1007/s13762-017-1485-x
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DOI: https://doi.org/10.1007/s13762-017-1485-x