HASTANE ATIKSUYUNA ÖN OKSİDASYON UYGULAMALARI (O3, O3/H2O2): İLAÇ ETKEN MADDELER VE KLASİK KİRLETİCİLERİN AKIBETİ

Abstract

Bu çalışmada psikiyatrik ilaç ve sinir uyarıcılardan dört (karbamazepin (CBZ), primidone (PRM), kafein (CAF), nikotin (NCT)) ve CBZ ve CAF’a ait altı metabolitin (karbamazepin-diol, karbamazepin 10,11-epoksid, 2-hidroksi karbamazepin ve 3-hidroksi karbamazepin, trans-3'-hidroksi kotinin ve N-formilnornikotin) hastane atıksularındaki varlığı ve ozonlama (O3) ve perokson (O3/H2O2) prosesleri ile akıbetleri araştırılmıştır. Bu kapsamda ilaçların analizi HPLC/MS-MS cihazı ile gerçekleştirilmiştir. Yapılan çalışmanın sonuçlarına göre düşük oranda (0,5 mg O3/mg KOİ) sadece ozon dozunda dahi karbamazepin (CBZ) %99,7 oranlarında giderilirken, CAF için benzer giderim verimlilikleri daha yüksek ozon dozlarında (1,5 mg O3/mg KOİ) elde edilmiştir. Perokson prosesinde ise CBZ giderim verimliliği nispeten artış gösterse de (%20), CAF giderimi için benzer pozitif etki gözlemlenmemiştir. İki prosesin mg KOİ başına oksijen oranları dikkate alındığında ozonlama prosesinin tespit edilen ilaçların gideriminde daha etkili bir proses olduğu belirlenmiştir. Ayrıca sadece ozonlama uygulaması ile 1,5 mg O3/mg KOİ oranında %48 KOİ giderimi elde edilmiştir. Bu bağlamda, hastane atıksularının ön oksidasyonunun hem KOİ hem ilaç yüklerinin atıksu arıtma tesislerinde arıtma süreçlerine girmeden önemli seviyelerde azaltılabileceği görülmektedir.

Keywords

• Hastane Atıksukarı
• İleri Oksidasyon
• O3/H2O2
• O3
• İlaç Etken Maddeler.

PRE-OXIDATION APPLICATIONS TO HOSPITAL WASTEWATER (O3, O3/H2O2): FATE OF PHARMACEUTICAL ACTIVE COMPOUNDS (PhACs) AND CONVENTIONAL PARAMETERS

Abstract

In this study, the occurrence of four psychiatric drugs and nerve stimulants (carbamazepine (CBZ), primidone (PRM), caffeine (CAF) and nicotine (NCT)) and six metabolites belonging to CBZ and CAF (cbz-diol, carbamazepine 10,11-epoxide, 2-hydroxy carbamazepine, 3-hydroxy carbamazepine, trans-3'-hydroxy cotinine and N-formylnornicotine) in hospital wastewater and their fate in ozonation (O3) and peroxon (O3/H2O2) processes were determined. In this context, selected drugs analyzed with HPLC/MS-MS. According to obtained results, while removal efficiency of CBZ reached 99.7% in the only ozonation application even lower ozone dose (0.5 mg O3/mg COD), the same removal efficiency for CAF was obtained in higher ozone dose (1,5 mg O3/mg COD). Although peroxon process provided a relatively positive contribution for CBZ removal (%20), the results were not the same for CAF. Considering the oxygen ratios per mg COD of both processes, it was determined that the ozonation process was a more effective process for the removal of the detected drugs compared to peroxon. Additionally, removal efficiencies of COD were determined as 48% in the ratio of 1,5 mg O3/mg COD with the only ozonation process. In this context, obtained results show that both COD and PhAC loads could decrease in important levels with pre-oxidaiton of hospital wastewater without being included to the treatment process in wastewater treatment plants.

Keywords

• Hospital wastewater
• Advanced oxidation
• O3/H2O2
• O3
• Pharmaceutical active compounds.

References

1. Altman, J., As, R., Zietzschmann, F., Jekel, M., 2014. Direct comparison of ozonation and adsorption onto powdered activated carbon for micropollutant removal in advanced wastewater treatment. Water research, 55, 185-193.
2. Ajo, P., Preis, S., Vornamo, T., Manttari, M., Kallioinen, M., Louhi-Kultanen, M., 2018. Hospital wastewater treatment with pilot-scale pulsed corona discharge for removal of pharmaceutical residues. Journal of Environmental Chemical Engineering, 6, 1569–1577.
3. Argun, M.E., Akkus ̧, M., Ates ̧, H., 2020. Investigation of micropollutants removal from landfill leachate in a full-scale advanced treatment plant in Istanbul city, Turkey. Science of Total Environment, 748.
4. Ates, H., Argun, M.E., 2021. Advanced oxidation of landfill leachate: Removal of micropollutants and identification of by-products. Journal of Hazardous Material, 413, 125326.
5. Aydin, S., Aydin, M.E., Ulvi, A., Kilic H. 2019. Antibiotics in hospital effluents: occurrence, contribution to urban wastewater, removal in a wastewater treatment plant, and environmental risk assessment. Environmental Science and Pollution Research, 26, 544–558.
6. Arslan, A., Veli, S., Bingöl, D., 2014. Use of response surface methodology for pretreatment of hospital wastewater by O3/UV and O3/UV/H2O2 processes. Separation and Purification Technology, 132, 561-567.
7. Arvaniti, O.S., Gkotsis, G., Nika, M-C., Gyparakis, S., Manios, T., Thomaidis, N.S., Fountoulakis, M.S. and Stasinakis, A.S., 2023. Study on the Occurrence of Artificial Sweeteners, Parabens, and Other Emerging Contaminants in Hospital Wastewater Using LC-QToF-MS Target Screening Approach. Water, 15, 936.
8. Azar, A., Jelogir, A., Bidhendi, G., Mehrdadi, N., Zaredar, N., Poshtegal, M., 2010. Investigation of optimal method for hospital wastewater treatment. Journal of Food Agriculture and Environment, 8, 1199–1202.

9. Blanch, A.R., Caplin, J.L., Iversen, A., Kuehn, I., Manero, A., Taylor, H.D., Vilanova, X., 2003. Comparison of enterococcal populations related to urban and hospital wastewater in various climatic and geographic European regions. Journal of Applied Microbiology, 94, 994e1002.
10. Boillot, C., Bazin, C., Tissot-Guerraz, F., Droguet, J., Perraud, M., Cetre, J. C., Trepo, D., Perrodin, Y., 2008. Daily physicochemical, microbiological and ecotoxicological fluctuations of a hospital effluent according to technical and care activities. Science of The Total Environment, 403, 13-129.
11. Casas, M.E., Chhetri, R.K., Ooi, G., Hansen, K.M.S., Litty, K., Christensson, M., Kragelund, C., Andersen, H.R., Bester, K., 2015. Biodegradation of pharmaceuticals in hospital wastewater by staged Moving Bed Biofilm Reactors (MBBR). Water Research, 83 (2015) 293–302.
12. Chen-Lin, A.Y., Fang Hsueh, J.H., Andy Hong, P. K., 2015. Removal of antineoplastic drugs cyclophosphamide, ifosfamide, and 5-fluorouracil and a vasodilator drug pentoxifylline from wastewaters by ozonation. Environmental Science and Pollution Research, 22, 508-515.
13. Chiarello, M., Minetto, L., Giustina, S.V.D., Beal, L.L., Moura, S., 2016. Popular pharmaceutical residues in hospital wastewater: quantification and qualification of degradation products by mass spectroscopy after treatment with membrane bioreactor. Environmental Science and Pollution Research, 23, pages 16079–16089.
14. Chitnis, V., Chitnis, S., Vaidya, K., Ravikant, S., Patil, S., Chitnis, D.S. 2004. Bacterial population changes in hospital effluent treatment plant in central India. Water Research, 38, 441–447.
15. Dolu T., 2021. Farmasötı̇klerı̇n İlerı̇ Bı̇yolojı̇k Atıksu Arıtma Tesı̇sı̇ndekı̇ Akıbetlerı̇, Membran Prosesler İle Gı̇derı̇mlerı̇ Ve Farklı Tarımsal Uygulamalar İle Toprak Ve Bı̇tkı̇lere Geçı̇şlerı̇, Doktora Tezi, Konya Teknik Üniversitesi, Türkiye.
16. Dolu, T. and Nas, B., 2023a. Dissemination of nonsteroidal anti-inflammatory drugs (NSAIDs) and metabolites from wastewater treatment plant to soils and agricultural crops via real-scale different agronomic practices. Environmental Research, 227, 115731.
17. Dolu, T., Nas, B., 2023b. Full-scaleanaerobicdigestionofsewagesludges:fateevaluationof pharmaceuticals and main metabolites. Journal of Water Process Engineering, 51, 103366. Ferre-Aracil, F., Valcárcel, Y., Negreira, N., López de Alda, M., Barceló, D., Cardona, S.C., Navarro-Laboulais, J., 2016. Ozonation of hospital raw wastewaters for cytostatic compounds removal. Kinetic modelling and economic assessment of the process, Science of the Total Environment, 556, 70-79.
18. Golovko, O., Kumar, V., Fedorova, G., Randak, T. ve Grabic, R., 2014. Seasonal changes in antibiotics, antidepressants/psychiatric drugs, antihistamines and lipid regulators in a wastewater treatment plant. Chemosphere, 111, 418-426.
19. Gonzalez, P., 2021. Understanding Phosphorus”, Chemicals Incorporated 13560 Colombard Court, Fontana, CA 92337, https://www.cheminc.com/post/understanding-phosphorus, Access date: 16 Nisan 2023.
20. Gomez, M.J., Agüera, A., Mezcua, M., Hurtado, J., Mocholi, F., Fernandez-Alba, A.R., 2007. Simultaneous analysis of neutral and acidic pharmaceuticals as well as related compounds by gas chromatography–tandem mass spectrometry in wastewater. Talanta, 73, 314–320.
21. Gönder, Z.B., Kara, E.M., Celik, B.O., Vergili, I., Kaya, Y., Altinkum, S.M., Bagdatli, Y., Yilmaz, G., 2021. Detailed characterization, antibiotic resistance and seasonal variation of hospital wastewater. Environmental Science and Pollution Research, 28(13), 16380-16393.
22. Gracia-Lor, E., Sancho, J. V., Serrano, R. ve Hernández, F., 2012. Occurrence and removal of pharmaceuticals in wastewater treatment plants at the Spanish Mediterranean area of Valencia. Chemosphere, 87 (5), 453-462.
23. Hansen, K.M.S., Spiliotopoulou, A., Chhetri, R.K., Casas, M.E., Bester, K., Andersen, H.R., 2016. Ozonation for source treatment of pharmaceuticals in hospital wastewater – Ozone lifetime and required ozone dose. Chemical Engineering Journal, 290, 507-514.
24. Hörsch, P., Speck, A., Frimmel, F.H., 2003. Combined advanced oxidation and biodegradation of industrial effluents from the production of stilbene-based fluorescent whitening agents. Water Research, 37(11), 2748-2756.
25. Karakaş, İ., Kaya, Y., Vergili, İ., Özçelep, Z. B., Yılmaz, G., 2022. Hastane atiksularindaki mikrokirleticiler ve mikrokirleticilerin membran biyoreaktörlerde giderimi. Mühendislik Bilimleri ve Tasarım Dergisi, 10(2), 722-739.
26. Khan, N.A., Khan, A.H., Ahmed, S., Farooqi, I.H., Alam, S.S., Ali, I., Bokhari, A., Mubashir, M., 2022. Efficient removal of ibuprofen and ofloxacin pharmaceuticals using biofilm reactors for hospital wastewater treatment. Chemosphere, 298, 134243.
27. Kosma, C. I., Lambropouolu, D. A., Albanis, T. A. 2010. Occurrence and removal of PPCPs in municipal and hospital wastewaters in Greece. Journal of Hazardous Materials, 179, 804-817.
28. Kovalova, L., Siegrist, H., Singer, H., Wittmer, A., McArdell, C.S., 2012. Hospital wastewater treatment by membrane bioreactor: performance and efficiency for organic micropollutant elimination. Environmental Science&Technology, 46, 1536e1545.
29. Kovalova, L., Siegrist, H., von Gunten, U., Eugster, J., Hagenbuch, M., Wittmer, A., Moser, R., McArdell, C.S., 2013. Elimination of micropollutants during post-treatment of hospital wastewater with powdered activated carbon, ozone, and UV. Environmental Science&Technology, 47, 7899e7908.
30. Kumari, A., Maurya, N.S., Tiwari, B. 2020. Hospital wastewater treatment scenario around the globe. Current Developments in Biotechnology and Bioengineering, 549–570.
31. Langlais, B., Reckhow, D. ve R. Brink, D., 1991. Ozone in Water Treatment, Lewis Publisher.
32. Lee, Y., Kovalova, L., McArdell, C.S., von Gunten, U., 2014. Prediction of micropollutant elimination during ozonation of a hospital wastewater effluent. Water Research, 64, 134–148
33. Nas, B., Dolu, T., Argun, M.E., Yel, E., Ates ̧, H., Koyuncu, S., 2021. Comparison of advanced biological treatment and nature-based solutions for the treatment of pharmaceutically active compounds (PhACs): a comprehensive study for wastewater and sewage sludge. Science of Total Environment, 779, 146344.
34. Nieto-Juárez, J. I., Torres-Palma, R. A., Botero-Coy, A. M. ve Hernández, F., 2021, Pharmaceuticals and environmental risk assessment in municipal wastewater treatment plants and rivers from Peru. Environment International, 155, 106674.
35. Nguyen, T.T., Bui, X.T., Luu, V.P., Nguyen, P.D., Guo, W., Ngo, H.H., 2017. Removal of antibiotics in sponge membrane bioreactors treating hospital wastewater: comparison between hollow fiber and flat sheet membrane systems. Bioresource Technology, 240, 42–49.
36. Majumder, A., Gupta, A.K., Ghosal, P.S., Varma, M., 2021. A review on hospital wastewater treatment: A special emphasis on occurrence and removal of pharmaceutically active compounds, resistant microorganisms, and SARS-CoV-2. Journal of Environmental Chemical Engineering, 9(2), 104812.
37. Ogava, K., Umetsu, Y., Kamimura, K., 2020. Changes in the absorption spectra and colour of tetraphenylporphyrins after redox reactions, Journal of Chemical Research, 44(9-10), 613-61.
38. Olmez-Hanci, T., Dogruel, S. Allar Emek, A. D., Eropak Yılmazer, C., Çınar, S., Kiraz, O., Citil, E., Koc Orhon, A., Siltu, E., Gucver, S. M., Karahan Ozgun, O., Tanik, A. and Yetis U. 2020. Performance of ozone and peroxone on the removal of endocrine disrupting chemicals (EDCs) coupled with cost analysis. Water Science & Technology, 82(4), 640-650.
39. Ooi, G.T.H., Tang, K., Chhetri, R.K., Kaarsholm, K.M.S, Sundmark, K., Kragelund, C., Litty, K., Christensen, A., Lindholst, S., Sund, C., Christensson, M., Bester, K., Andersen, H. R., 2018. Biological removal of pharmaceuticals from hospital wastewater in a pilot-scale staged moving bed biofilm reactor (MBBR) utilising nitrifying and denitrifying processes. Bioresource Technology, 267, 677–687.
40. Pariente, M.I., Segura, Y., Alvarez-Torrellas, S., Casas, J.A., dePedro, Z.M., Diaz, E., García, J., Lopez-Munoz, M.J., Marugan, J., Mohedano, A.F., Molina, R., Munoz, M., Pablos, C., Perdigon-Melon, J.A., Petre, A.L., Rodríguez, J.J., Tobajas, M., Martínez, F., 2022. Critical review of technologies for the on-site treatment of hospital wastewater: From conventional to combined advanced processes. Journal of Environmental Management, 320, 115769.
41. Prasertkulsak, S., Chiemchaisri, C., Chiemchaisri, W., Itonaga, T., Yamamoto, K., 2016. Removals of pharmaceutical compounds from hospital wastewater in membrane bioreactor operated under short hydraulic retention time. Chemosphere, 150, 624-631.
42. Piras, F., Santoro, O., Pastore, T., Pio, I., De Dominicis, E., Gritti, E., Caricato, R.,Lionetto, M.G., Mele, G., Santoro, D., 2020. Controlling micropollutants in tertiary municipal wastewater by O3/H2O2, granular biofiltration and UV254/H2O2 for potable reuse applications. Chemosphere, 239, 124635.
43. Prieto-Rodríguez, L., Oller, I., Klamerth, N. Agüera, A. Rodríguez, E.M., Malato, S., 2013. Application of solar AOPs and ozonation for elimination of micropollutants in municipal wastewater treatment plant effluents, Water Research, 47(4), 1521-1528.
44. Rosal, R., Rodríguez, A., Perdigón-Melón, J.A., Petre, A., García-Calvo, E., Gómez, M.J., Agüera, A., Fernández-Alba, A.R., 2009. Degradation of caffeine and identification of the transformation products generated by ozonation, Chemosphere, 74, 825–831. Rosal, R., Rodríguez, A., Perdigón-Melón, J.A., Petre, A., García-Calvo, E., Gómez, M.J., Agüera, A., Fernández-Alba, A.R., 2010. Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation. Water Research, 44(2), 578-588.
45. Schuts, E.C., Boyd, A., Muller, A.E., Mouton, J.V., Prins, J.M., 2021. The Effect of Antibiotic Restriction Programs on Prevalence of Antimicrobial Resistance: A Systematic Review and Meta-Analysis, Open Forum Infectious Diseases, 8(4).
46. Souza, F.S., Da Silva, V.V., Rosin, C.K., Hainzenreder, L., Arenzon, A., Pizzolato, T., Jank, L., Féris, L.A. 2018. Determination of pharmaceutical compounds in hospital wastewater and their elimination by advanced oxidation processes. Journal of Environmental Science and Health, Part A, 53(3), 213-221.
47. Souza, D.M., Reichert, J.F., do Nascimento, V.R., Martins, A.F., 2022. Ozonation and UV photolysis for removing anticancer drug residues from hospitalwastewater. Journal Of Environmental Science and Health, Part A, 5788), 635-644.
48. Wen, X., Ding, H., Huang, X., Lui, R., 2004. Treatment of hospital wastewater using a submerged membrane bioreactor. Process Biochemistry, 39, 1427-1431.
49. Verlicchi, P., Galletti, A., Petrovic, M., Barcelo, D., 2010. Hospital effluents as a source of emerging pollutants: an overview of micropollutants and sustainable treatment options. Journal of Hydrology, 389, 416-428.
50. Yuan, S., Jiang, X., Xia, X., Zhang, H., Zheng, S., 2013. Detection, occurrence and fate of 22 psychiatric pharmaceuticals in psychiatric hospital and municipal wastewater treatment plants in Beijing, China. Chemosphere, 90, 2520–2525
51. Zheng J, Su C, Zhou J, Xu L, Qian Y, Chen H., 2017. Effects and mechanisms of ultraviolet, chlorination, and ozone disinfection on antibiotic resistance genes in secondary effluents of municipal wastewater treatment plants. Chemical Engineering Journal, 317, 309-316.