Journal of Korean Society of Water and Wastewater (상하수도학회지)

The Korean Society of Water and Wastewater (대한상하수도학회)
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Fate and mass balance of pharmaceuticals of unit processes in a sewage treatment plant

하수처리시설 단위공정별 잔류의약물질 거동 및 물질수지 분석

  • Park, Junwon (Department of Environmental Infrastructure Research, National Institute of Environmental Research) ;
  • Kim, Changsoo (Department of Environmental Infrastructure Research, National Institute of Environmental Research) ;
  • Lee, Wonseok (Department of Environmental Infrastructure Research, National Institute of Environmental Research) ;
  • Lee, Soo-Hyung (Department of Environmental Infrastructure Research, National Institute of Environmental Research) ;
  • Chung, Hyenmi (Department of Environmental Infrastructure Research, National Institute of Environmental Research) ;
  • Jeong, Dong-Hwan (Department of Environmental Infrastructure Research, National Institute of Environmental Research)
  • 박준원 (국립환경과학원 환경기반연구부) ;
  • 김창수 (국립환경과학원 환경기반연구부) ;
  • 이원석 (국립환경과학원 환경기반연구부) ;
  • 이수형 (국립환경과학원 환경기반연구부) ;
  • 정현미 (국립환경과학원 환경기반연구부) ;
  • 정동환 (국립환경과학원 환경기반연구부)
  • Received : 2019.09.04
  • Accepted : 2019.10.14
  • Published : 2019.10.15
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Abstract

In this study, the fate and removal of 15 pharmaceuticals (including stimulants, non-steroidal anti-inflammatory drugs, antibiotics, etc.) in unit processes of a sewage treatment plant (STP) were investigated. Mass loads of pharmaceuticals were 2,598 g/d in the influent, 2,745 g/d in the primary effluent, 143 g/d in the secondary effluent, and 134 g/d in the effluent. The mass loads were reduced by 95% in the biological treatment process, but total phosphorous treatment did not show a significant effect on the removal of most pharmaceuticals. Also, mass balance analysis was performed to evaluate removal characteristics of pharmaceuticals in the biological treatment process. Acetaminophen, caffeine, acetylsalicylic acid, cefradine, and naproxen were efficiently removed in the biological treatment process mainly due to biodegradation. Removal efficiencies of gemfibrozil, ofloxacin, and ciprofloxacin were not high, but their removal was related to sorption onto sludge. This study provides useful information on understanding removal characteristics of pharmaceuticals in unit processes in the STP.

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References

  1. Alexander, J.T., Hai, F.I., and Al-aboud, T.M. (2012). Chemical coagulation-based processes for trace organic contaminant removal: Current state and future potential, J. Environ. Manage., 111, 195-207. https://doi.org/10.1016/j.jenvman.2012.07.023
  2. Andreozzi, R., Caprio, V., Ciniglia, C., De Champdore, M., Lo Giudice, R., Marotta, R., and Zuccato, E. (2004). Antibiotics in the environment: Occurrence in Italian STPs, fate, and preliminary assessment on algal toxicity of amoxicillin, Environ. Sci. Technol., 38, 6832-6838. https://doi.org/10.1021/es049509a
  3. Ashfaq, M., Li, Y., Wang, Y., Chen, W., Wang, H., Chen, X., Wu, W., Huang, Z., Yu, C.P., and Sun, Q. (2017). Occurrence, fate, and mass balance of different classes of pharmaceuticals and personal care products in an anaerobic-anoxic-oxic wastewater treatment plant in Xiamen, China, Water Res., 123, 655-667. https://doi.org/10.1016/j.watres.2017.07.014
  4. Baalbaki, Z., Sultana, T., Maere, T., Vanrolleghem, P.A., Metcalfe, C.D., and Yargeau, V. (2016). Fate and mass balance of contaminants of emerging concern during wastewater treatment determined using the fractionated approach, Sci. Total Environ., 573, 1147-1158. https://doi.org/10.1016/j.scitotenv.2016.08.073
  5. Behera, S.K., Kim, H.W., Oh, J.E., and Park, H.S. (2011). Occurrence and removal of antibiotics, hormones and several other pharmaceuticals in wastewater treatment plants of the largest industrial city of Korea, Sci. Total Environ., 409, 4351-4360. https://doi.org/10.1016/j.scitotenv.2011.07.015
  6. Bourdat-Deschamps, M., Leang, S., Bernet, N., Daudin, J., and Nelieu, S. (2014). Multi-residue analysis of pharmaceuticals in aqueous environmental samples by online solid-phase extraction-ultra-high-performance liquid chromatography-tandem mass spectrometry: Optimisation and matrix effects reduction by quick, easy, cheap, effective, rugged and safe extraction, J. Chromatography A, 1349, 11-23. https://doi.org/10.1016/j.chroma.2014.05.006
  7. Carballa, M., Omil, F., Lema, J.M., Llompart, M., Garcia-Jares, C., Rodriguez, I., Gomez, M., and Ternes, T. (2004). Behavior of pharmaceuticals, cosmetics and hormones in a sewage treatment plant, Water Res., 38, 2918-2926. https://doi.org/10.1016/j.watres.2004.03.029
  8. Conkle, J.L., White, J.R., and Metcalfe, C.D. (2008). Reduction of pharmaceutically active compounds by a lagoon wetland wastewater treatment system in Southeast Louisiana, Chemosphere, 73, 1741-1748. https://doi.org/10.1016/j.chemosphere.2008.09.020
  9. Gao, J., Huang, J., Chen, W., Wang, B., Wang, Y., Deng, S., and Yu, G. (2016). Fate and removal of typical pharmaceutical and personal care products in a wastewater treatment plant from Beijing: a mass balance study, Front. Environ. Sci. Eng., 10(3), 491-501. https://doi.org/10.1007/s11783-016-0837-y
  10. Gao, P., Ding, Y., Li, H., and Xagoraraki, I. (2012). Occurrence of pharmaceuticals in a municipal wastewater treatment plant: Mass balance and removal processes, Chemosphere, 88, 17-24. https://doi.org/10.1016/j.chemosphere.2012.02.017
  11. Golet, E.M., Xifra, I., Siegrist, H., Alder, A.C., and Giger, W. (2003). Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil, Environ. Sci. Technol., 37, 3243-3249. https://doi.org/10.1021/es0264448
  12. Gracia-Lor, E., Sancho, J.V., Serrano, R., and Hernandez, F. (2012). Occurrence and removal of pharmaceuticals in wastewater treatment plants at the Spanish Mediterranean area of Valencia, Chemosphere, 87, 453-462. https://doi.org/10.1016/j.chemosphere.2011.12.025
  13. Guerra, P., Kim, M., Shah, A., Alaee, M., and Smyth, S.A. (2014). Occurrence and fate of antibiotic, analgesic/anti-inflammatory, and antifungal compounds in five wastewater treatment processes, Sci. Total Environ., 473-474, 235-243. https://doi.org/10.1016/j.scitotenv.2013.12.008
  14. Jelic, A., Gros, M., Ginebreda, A., Cespedes-Sanchez, R., Ventura, F., Petrovic, M., and Barcelo, D. (2011). Occurrence, partition and removal of pharmaceuticals in sewage water and sludge during wastewater treatment, Water Res., 45, 1165-1176. https://doi.org/10.1016/j.watres.2010.11.010
  15. Klein, E.Y., Boeckel, T.P.V., Martinez, E.M., Pant, S., Gandra, S., Levin, S.A., Goossens, H., and Laxminarayan, R. (2018). Global increase and geographic convergence in antibiotic consumption between 2000 and 2015, Proc. Natl. Acad. Sci., 115(15), E3463-E3470. https://doi.org/10.1073/pnas.1717295115
  16. Luo, Y., Guo, W., Ngo, H.H., Nghiem, L.D., Hai, F.I., Zhang, J., Liang, S., and Wang, X.C. (2014). A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment, Sci. Total Environ., 473-474, 619-641. https://doi.org/10.1016/j.scitotenv.2013.12.065
  17. Matamoros, V., and Salvado, V. (2013). Evaluation of a coagulation/flocculation-lamellar clarifier and filtration-UV-chlorination reactor for removing emerging contaminants at full-scale wastewater treatment plants in Spain, J. Environ. Manage., 117, 96-102. https://doi.org/10.1016/j.jenvman.2012.12.021
  18. Nakada, N., Hanamoto, S., Jurgens, M.D., Johnson, A.C., Bowes, M.J., and Tanaka, H. (2017). Assessing the population equivalent and performance of wastewater treatment through the ratios of pharmaceuticals and personal care products present in a river basin: Application to the River Thames basin, UK, Sci. Total Environ., 575, 1100-1108. https://doi.org/10.1016/j.scitotenv.2016.09.180
  19. Park, J., Yamashita, N., Park, C., Shimono, T., Takeuchi, D.M., and Tanaka, H. (2017). Removal characteristics of pharmaceuticals and personal care products: comparison between membrane bioreactor and various biological treatment processes, Chemosphere, 179, 347-358. https://doi.org/10.1016/j.chemosphere.2017.03.135
  20. Park, J., Kim, C., Ju, B., Lee, W., Chung, H., and Jeong, D. (2018). Evaluation and application of pretreatment methods for pharmaceuticals and personal care products in the solid phase of sewage samples, J. Korean Soc. Water Wastewater, 32(6), 559-572. https://doi.org/10.11001/jksww.2018.32.6.559
  21. Radjenovic, J., Petrovic, M., and Barcelo, D. (2009). Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge (CAS) and advanced membrane bioreactor (MBR) treatment, Water Res., 43, 831-841. https://doi.org/10.1016/j.watres.2008.11.043
  22. Rodayan, A., Majewsky, M., and Yargeau, V. (2014). Impact of approach used to determine removal levels of drugs of abuse during wastewater treatment, Sci. Total Environ., 487, 731-739. https://doi.org/10.1016/j.scitotenv.2014.03.080
  23. Rossini, D., Ciofi, L., Ancillotti, C., Checchini, L., Bruzzoniti, M.C., Rivoira, L., Fibbi, D., Orlandini, S., and Del Bubba, M. (2016). Innovative combination of QuEChERS extraction with on-line solid-phase extract purification and pre-concentration, followed by liquid chromatography-tandem mass spectrometry for the determination of non-steroidal anti-inflammatory drugs and their metabolites in sewage sludge, Anal. Chim. Acta, 935, 269-281. https://doi.org/10.1016/j.aca.2016.06.023
  24. Salgado, R., Marques, R., Noronha, J.P., Carvalho, G., Oehmen, A., and Reis, M.A.M. (2012). Assessing the removal of pharmaceuticals and personal care products in a full-scale activated sludge plant, Environ. Sci. Pollut. Res., 19, 1818-1827. https://doi.org/10.1007/s11356-011-0693-z
  25. Shrivastava, A. and Gupta, V.B. (2011). Methods for the determination of limit of detection and limit of quantitation of the analytical methods, Chron. Young Sci., 2(1), 21-25. https://doi.org/10.4103/2229-5186.79345
  26. Wang, Y., Li, Y., Hu, A., Rashid, A., Ashfaq, M., Wang, Y., Wang, H., Luo, H., Yu, C.P., and Sun, Q. (2018). Monitoring, mass balance and fate of pharmaceuticals and personal care products in seven wastewater treatment plants in Xiamen City, China, J. Hazard. Mater., 354, 81-90. https://doi.org/10.1016/j.jhazmat.2018.04.064
  27. Xie, W.Y., McGrath, S.P., Su, J.Q., Hirsch, P.R., Clark, I.M., Shen, Q., Zhu, Y.G., and Zhao, F.J. (2016). Long-term impact of field applications of sewage sludge on soil antibiotic resistome, Environ. Sci. Technol., 50, 12602-12611. https://doi.org/10.1021/acs.est.6b02138
  28. Verlicchi, P., Al Aukidy, M., and Zambello, E. (2012). 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