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Distribution of six anticancer drugs and a variety of other pharmaceuticals, and their sorption onto sediments, in an urban Japanese river

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Abstract

The distributions of 31 pharmaceuticals grouped into nine therapeutic classes, including six anticancer drugs, were investigated in the waters and sediments of an urban river in Japan. The coefficients of sorption (logK d) to the river sediments were also determined from the results of a field survey and laboratory-scale experiment. Three anticancer drugs—bicalutamide, doxifluridine, and tamoxifen—were detected in the river sediments at maximum concentrations of 391, 392, and 250 ng/kg, respectively. In addition, the transformation products of psychotropic carbamazepine (2-hydroxy carbamazepine, acridine, and acridone) were detected in the range of 108 ng/kg (2-hydroxy carbamazepine) to 2365 ng/kg (acridine), and the phytoestrogen glycitein was detected in the range of N.D. to 821 ng/kg. The logK d values of the targeted pharmaceuticals in river sediments in the field survey ranged from 0.5 (theophylline) to 3.3 (azithromycin). These results were in accord with those of the laboratory-scale sorption experiment. To the best of our knowledge, this is the first report of the detection of the anticancer drugs bicalutamide and tamoxifen, the transformation products of carbamazepine (2-hydroxy carbamazepine, acridine, and acridone), and the phytoestrogen genistein in river sediments.

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References

  • Agunbiade FO, Moodley B (2016) Occurrence and distribution pattern of acidic pharmaceuticals in surface water, wastewater, and sediment of the Msunduzi River, Kwazulu-Natal, South Africa. Environ Toxicol Chem 35:36–46

    Article  CAS  Google Scholar 

  • Azuma T, Nakada N, Yamashita N, Tanaka H (2013) Mass balance of anti-influenza drugs discharged into the Yodo River system, Japan, under an influenza outbreak. Chemosphere 93:1672–1677

    Article  CAS  Google Scholar 

  • Azuma T, Ishiuchi H, Inoyama T, Teranishi Y, Yamaoka M, Sato T, Mino Y (2015) Occurrence and fate of selected anticancer, antimicrobial, and psychotropic pharmaceuticals in an urban river in a subcatchment of the Yodo River basin, Japan. Environ Sci Pollut Res 22:18676–18686

    Article  CAS  Google Scholar 

  • Azuma T, Arima N, Tsukada A, Hirami S, Matsuoka R, Moriwake R, Ishiuchi H, Inoyama T, Teranishi Y, Yamaoka M, Mino Y, Hayashi T, Fujita Y, Masada M (2016) Detection of pharmaceuticals and phytochemicals together with their metabolites in hospital effluents in Japan, and their contribution to sewage treatment plant influents. Sci Total Environ 548-549:189–197

    Article  CAS  Google Scholar 

  • Azuma T, Ishida M, Hisamatsu K, Yunoki A, Otomo K, Kunitou M, Shimizu M, Hosomaru K, Mikata S, Mino Y (2017) Fate of new three anti-influenza drugs and one prodrug in the water environment. Chemosphere 169:550–557

    Article  CAS  Google Scholar 

  • Barceló D, Petrovic M (2008) Emerging contaminants from industrial and municipal waste. The handbook of environmental chemistry 5S/2. Springer, Berlin, pp 1–284

    Google Scholar 

  • Barra Caracciolo A, Topp E, Grenni P (2015) Pharmaceuticals in the environment: biodegradation and effects on natural microbial communities. A review. J Pharm Biomed Anal 106:25–36

    Article  CAS  Google Scholar 

  • Besse J-P, Latour J-F, Garric J (2012) Anticancer drugs in surface waters: what can we say about the occurrence and environmental significance of cytotoxic, cytostatic and endocrine therapy drugs? Environ Int 39:73–86

    Article  CAS  Google Scholar 

  • Booker V, Halsall C, Llewellyn N, Johnson A, Williams R (2014) Prioritising anticancer drugs for environmental monitoring and risk assessment purposes. Sci Total Environ 473–474:159–170

    Article  Google Scholar 

  • Borgatta M, Waridel P, Decosterd L-A, Buclin T, Chèvre N (2016) Multigenerational effects of the anticancer drug tamoxifen and its metabolite 4-hydroxy-tamoxifen on Daphnia pulex. Sci Total Environ 545–546:21–29

    Article  Google Scholar 

  • Borisover M, Keren Y, Usyskin A, Bukhanovsky N (2016) Effects of γ-irradiation of original and organic matter-amended soils on the sorption of triclosan and diuron from aqueous solutions. Chemosphere 152:62–70

    Article  CAS  Google Scholar 

  • Cavalcanti EB, Segura SG, Centellas F, Brillas E (2013) Electrochemical incineration of omeprazole in neutral aqueous medium using a platinum or boron-doped diamond anode: degradation kinetics and oxidation products. Water Res 47:1803–1815

    Article  CAS  Google Scholar 

  • De Oliveira T, Guégan R, Thiebault T, Milbeau CL, Muller F, Teixeira V, Giovanela M, Boussafir M (2017) Adsorption of diclofenac onto organoclays: effects of surfactant and environmental (pH and temperature) conditions. J Hazard Mater 323(Part A):558–566

    Article  CAS  Google Scholar 

  • Evgenidou EN, Konstantinou IK, Lambropoulou DA (2015) Occurrence and removal of transformation products of PPCPs and illicit drugs in wastewaters: a review. Sci Total Environ 505:905–926

    Article  CAS  Google Scholar 

  • Ferrando-Climent L, Rodriguez-Mozaz S, Barceló D (2014) Incidence of anticancer drugs in an aquatic urban system: from hospital effluents through urban wastewater to natural environment. Environ Pollut 193:216–223

    Article  CAS  Google Scholar 

  • Gmurek M, Olak-Kucharczyk M, Ledakowicz S (2017) Photochemical decomposition of endocrine disrupting compounds – a review. Chem Eng J 310(Part 2):437–456

    Article  CAS  Google Scholar 

  • Golovko O, Koba O, Kodesova R, Fedorova G, Kumar V, Grabic R (2016) Development of fast and robust multiresidual LC-MS/MS method for determination of pharmaceuticals in soils. Environ Sci Polluti Res 23:14068–14077

    Article  CAS  Google Scholar 

  • Hanamoto S, Nakada N, Yamashita N, Tanaka H (2013) Modeling the photochemical attenuation of down-the-drain chemicals during river transport by stochastic methods and field measurements of pharmaceuticals and personal care products. Environ. Sci. Technol. 47:13571–13577

    Article  CAS  Google Scholar 

  • Hanamoto S, Kawakami T, Nakada N, Yamashita N, Tanaka H (2014) Evaluation of the photolysis of pharmaceuticals within a river by 2 year field observations and toxicity changes by sunlight. Environ. Sci. Proc. Imp. 16:2796–2803

    Article  CAS  Google Scholar 

  • Hu X, He K, Zhou Q (2012) Occurrence, accumulation, attenuation and priority of typical antibiotics in sediments based on long-term field and modeling studies. J Hazard Mater 225–226:91–98

    Article  Google Scholar 

  • Japan Sewage Works Association (2016) Statistics of sewerage (in Japanese)

  • Jurado A, López-Serna R, Vázquez-Suné E, Carrera J, Pujades E, Petrovic M, Barceló D (2014) Occurrence of carbamazepine and five metabolites in an urban aquifer. Chemosphere 115:47–53

    Article  CAS  Google Scholar 

  • Kim S-K, Yoon J (2014) Chronological trends of emission, environmental level and human exposure of POPs over the last 10 years (1999–2010) in Korea: implication to science and policy. Sci Total Environ 470–471:1346–1361

    Article  Google Scholar 

  • Koumaki E, Mamais D, Noutsopoulos C (2017) Environmental fate of non-steroidal anti-inflammatory drugs in river water/sediment systems. J Hazard Mater 323(Part A):233–241

    Article  CAS  Google Scholar 

  • Kovalova L, Siegrist H, von Gunten U, Eugster J, Hagenbuch M, Wittmer A, Moser R, McArdell CS (2013) Elimination of micropollutants during post-treatment of hospital wastewater with powdered activated carbon, ozone, and UV. Environ. Sci. Technol. 47:7899–7908

    Article  CAS  Google Scholar 

  • Kumar V, Hanamoto S, Johnson AC, Yamashita N, Nakada N, Tanaka H (2014) Elevated risk from estrogens in the Yodo River basin (Japan) in winter and ozonation as a management option. Environ Sci Proc Imp 16:232–238

    Article  CAS  Google Scholar 

  • Kuzmanović M, Ginebreda A, Petrović M, Barceló D (2015) Risk assessment based prioritization of 200 organic micropollutants in 4 Iberian rivers. Sci Total Environ 503–504:289–299

    Article  Google Scholar 

  • Lake Biwa-Yodo River Water Quality Preservation Organization, Japan (2016) BYQ (Lake Biwa-Yodo River Water Quality Preservation Organization) Report on water environment in Biwa Lake-Yodo River System 2014 (in Japanese), pp 1–94

  • Leal RMP, Alleoni LRF, Tornisielo VL, Regitano JB (2013) Sorption of fluoroquinolones and sulfonamides in 13 Brazilian soils. Chemosphere 92:979–985

    Article  CAS  Google Scholar 

  • Leclercq M, Mathieu O, Gomez E, Casellas C, Fenet H, Hillaire-Buys D (2009) Presence and fate of carbamazepine, oxcarbazepine, and seven of their metabolites at wastewater treatment plants. Arc Environ Contam Toxicol 56:408–415

    Article  CAS  Google Scholar 

  • Lei X, Lu J, Liu Z, Tong Y, Li S (2015) Concentration and distribution of antibiotics in water–sediment system of Bosten Lake, Xinjiang. Environ Sci Pollut Res 22:1670–1678

    Article  CAS  Google Scholar 

  • Li W, Shi Y, Gao L, Liu J, Cai Y (2012) Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China. Chemosphere 89:1307–1315

    Article  CAS  Google Scholar 

  • Lopes C, Persat H, Babut M (2012) Transfer of PCBs from bottom sediment to freshwater river fish: a food-web modelling approach in the Rhône River (France) in support of sediment management. Ecotoxicol Environ Safe 81:17–26

    Article  CAS  Google Scholar 

  • López-Serna R, Jurado A, Vázquez-Suñé E, Carrera J, Petrović M, Barceló D (2013) Occurrence of 95 pharmaceuticals and transformation products in urban groundwaters underlying the metropolis of Barcelona, Spain. Environ Pollut 174:305–315

    Article  Google Scholar 

  • Magnusson M, Heimann K, Ridd M, Negri AP (2013) Pesticide contamination and phytotoxicity of sediment interstitial water to tropical benthic microalgae. Water Res 47:5211–5221

    Article  CAS  Google Scholar 

  • Matongo S, Birungi G, Moodley B, Ndungu P (2015) Occurrence of selected pharmaceuticals in water and sediment of Umgeni River, KwaZulu-Natal, South Africa. Environ Sci Pollut Res 22:10298–10308

    Article  CAS  Google Scholar 

  • Ministry of Health Labour and Welfare, Japan (2014) Vital statistics in Japan (in Japanese), pp 1–59

  • Ministry of Health Labour and Welfare, Japan (2016) Annual report on statistics of production by pharmaceutical industry in 2014 (in Japanese) Available from http://www.mhlw.go.jp/topics/yakuji/2014/nenpo/index.html. Accessed 5 Apr 2017

  • Narumiya M, Nakada N, Yamashita N, Tanaka H (2013) Phase distribution and removal of pharmaceuticals and personal care products during anaerobic sludge digestion. J Hazard Mater 260:305–312

    Article  CAS  Google Scholar 

  • Negreira N, Mastroianni N, López de Alda M, Barceló D (2013) Multianalyte determination of 24 cytostatics and metabolites by liquid chromatography–electrospray–tandem mass spectrometry and study of their stability and optimum storage conditions in aqueous solution. Talanta 116:290–299

    Article  CAS  Google Scholar 

  • Negreira N, de Alda ML, Barceló D (2014) Cytostatic drugs and metabolites in municipal and hospital wastewaters in Spain: filtration, occurrence, and environmental risk. Sci Total Environ 497-498:68–77

    Article  CAS  Google Scholar 

  • Nie M, Yan C, Dong W, Liu M, Zhou J, Yang Y (2015) Occurrence, distribution and risk assessment of estrogens in surface water, suspended particulate matter, and sediments of the Yangtze Estuary. Chemosphere 127:109–116

    Article  CAS  Google Scholar 

  • OECD (2000) Adsorption-desorption using a batch equilibrium method, OECD guideline for the testing of chemicals No. 106., pp 1–45

  • Oliveira TS, Murphy M, Mendola N, Wong V, Carlson D, Waring L (2015) Characterization of pharmaceuticals and personal care products in hospital effluent and waste water influent/effluent by direct-injection LC-MS-MS. Sci Total Environ 518–519:459–478

    Article  Google Scholar 

  • Orias F, Bony S, Devaux A, Durrieu C, Aubrat M, Hombert T, Wigh A, Perrodin Y (2015) Tamoxifen ecotoxicity and resulting risks for aquatic ecosystems. Chemosphere 128:79–84

    Article  CAS  Google Scholar 

  • Osaka Prefectural Government, Japan (2016) Survey results based on water quality measurement (in Japanese). Available from http://www.pref.osaka.lg.jp/kankyohozen/osaka-wan/kokyo-status.html. Accessed 5 Apr 2017

  • Pan M, Chu LM (2016) Adsorption and degradation of five selected antibiotics in agricultural soil. Sci Total Environ 545–546:48–56

    Article  Google Scholar 

  • Patrolecco L, Capri S, Ademollo N (2015) Occurrence of selected pharmaceuticals in the principal sewage treatment plants in Rome (Italy) and in the receiving surface waters. Environ Sci Pollut Res 22:5864–5876

    Article  CAS  Google Scholar 

  • Pereira AMPT, Silva LJG, Lino CM, Meisel LM, Pena A (2016) Assessing environmental risk of pharmaceuticals in Portugal: an approach for the selection of the Portuguese monitoring stations in line with directive 2013/39/EU. Chemosphere 144:2507–2515

    Article  CAS  Google Scholar 

  • Petrović M, Škrbić B, Živančev J, Ferrando-Climent L, Barcelo D (2014) Determination of 81 pharmaceutical drugs by high performance liquid chromatography coupled to mass spectrometry with hybrid triple quadrupole–linear ion trap in different types of water in Serbia. Sci Total Environ 468–469:415–428

    Article  Google Scholar 

  • Polesel F, Lehnberg K, Dott W, Trapp S, Thomas KV, Plósz BG (2015) Factors influencing sorption of ciprofloxacin onto activated sludge: experimental assessment and modelling implications. Chemosphere 119:105–111

    Article  CAS  Google Scholar 

  • Prasse C, Schlüsener MP, Schulz R, Ternes TA (2010) Antiviral drugs in wastewater and surface waters: a new pharmaceutical class of environmental relevance? Environ Sci Technol 44:1728–1735

    Article  CAS  Google Scholar 

  • Radović T, Grujić S, Petković A, Dimkić M, Laušević M (2015) Determination of pharmaceuticals and pesticides in river sediments and corresponding surface and ground water in the Danube River and tributaries in Serbia. Environ Monit Asses 187:4092

    Article  Google Scholar 

  • Radović TT, Grujić SD, Kovačević SR, Laušević MD, Dimkić MA (2016) Sorption of selected pharmaceuticals and pesticides on different river sediments. Environ Sci Pollut Res 23:25232–25244

    Article  Google Scholar 

  • Rogers HR (1996) Sources, behaviour and fate of organic contaminants during sewage treatment and in sewage sludges. Sci Total Environ 185:3–26

    Article  CAS  Google Scholar 

  • Sangster JL, Oke H, Zhang Y, Bartelt-Hunt SL (2015) The effect of particle size on sorption of estrogens, androgens and progestagens in aquatic sediment. J Hazard Mater 299:112–121

    Article  CAS  Google Scholar 

  • Schlüsener MP, Hardenbicker P, Nilson E, Schulz M, Viergutz C, Ternes TA (2015) Occurrence of venlafaxine, other antidepressants and selected metabolites in the Rhine catchment in the face of climate change. Environ Pollut 196:247–256

    Article  Google Scholar 

  • Silva BFD, Jelic A, López-Serna R, Mozeto AA, Petrovic M, Barceló D (2011) Occurrence and distribution of pharmaceuticals in surface water, suspended solids and sediments of the Ebro River basin, Spain. Chemosphere 85:1331–1339

    Article  Google Scholar 

  • Taheran M, Brar SK, Verma M, Surampalli RY, Zhang TC, Valero JR (2016) Membrane processes for removal of pharmaceutically active compounds (PhACs) from water and wastewaters. Sci Total Environ 547:60–77

    Article  CAS  Google Scholar 

  • Tiedeken EJ, Tahar A, McHugh B, Rowan NJ (2017) Monitoring, sources, receptors, and control measures for three European Union watch list substances of emerging concern in receiving waters—a 20 year systematic review. Sci Total Environ 574:1140–1163

    Article  CAS  Google Scholar 

  • Toolaram AP, Kümmerer K, Schneider M (2014) Environmental risk assessment of anti-cancer drugs and their transformation products: a focus on their genotoxicity characterization-state of knowledge and short comings. Mutat Res 760:18–35

    Article  CAS  Google Scholar 

  • Tran NH, Chen H, Reinhard M, Mao F, Gin KY-H (2016) Occurrence and removal of multiple classes of antibiotics and antimicrobial agents in biological wastewater treatment processes. Water Res 104:461–472

    Article  CAS  Google Scholar 

  • Vasquez MI, Lambrianides A, Schneider M, Kümmerer K, Fatta-Kassinos D (2014) Environmental side effects of pharmaceutical cocktails: what we know and what we should know. J Hazard Mater 279:169–189

    Article  CAS  Google Scholar 

  • Venkatesan AK, Pycke BFG, Barber LB, Lee KE, Halden RU (2012) Occurrence of triclosan, triclocarban, and its lesser chlorinated congeners in Minnesota freshwater sediments collected near wastewater treatment plants. J Hazard Mater 229–230:29–35

    Article  Google Scholar 

  • Verbyla ME, Mihelcic JR (2015) A review of virus removal in wastewater treatment pond systems. Water Res 71:107–124

    Article  CAS  Google Scholar 

  • Wu C, Zhang K, Huang X, Liu J (2016) Sorption of pharmaceuticals and personal care products to polyethylene debris. Environ Sci Pollut Res 23:8819–8826

    Article  CAS  Google Scholar 

  • Xiang L, Wu X-L, Jiang Y-N, Yan Q-Y, Li Y-W, Huang X-P, Cai Q-Y, Mo C-H (2016) Occurrence and risk assessment of tetracycline antibiotics in soil from organic vegetable farms in a subtropical city, south China. Environ Sci Pollut Res 23:13984–13995

    Article  CAS  Google Scholar 

  • Yi Y, Wang Z, Zhang K, Yu G, Duan X (2008) Sediment pollution and its effect on fish through food chain in the Yangtze River. Int J Sediment Res 23:338–347

    Article  Google Scholar 

  • Zhang Y, Xu J, Zhong Z, Guo C, Li L, He Y, Fan W, Chen Y (2013) Degradation of sulfonamides antibiotics in lake water and sediment. Environ Sci Pollut Research 20:2372–2380

    Article  CAS  Google Scholar 

  • Zhou J, Broodbank N (2014) Sediment-water interactions of pharmaceutical residues in the river environment. Water Res 48:61–70

    Article  CAS  Google Scholar 

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Acknowledgements

We thank the staff of the STPs for sampling the water. We also acknowledge the River Foundation and the Ministry of Education, Culture, Sports, Science, and Technology of Japan for funding in the form of research grants and scholarships.

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Correspondence to Takashi Azuma.

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Azuma, T., Arima, N., Tsukada, A. et al. Distribution of six anticancer drugs and a variety of other pharmaceuticals, and their sorption onto sediments, in an urban Japanese river. Environ Sci Pollut Res 24, 19021–19030 (2017). https://doi.org/10.1007/s11356-017-9525-0

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