Occurrence and Removal of Selected Pharmaceuticals and Personal Care Products in Three Wastewater-Treatment Plants

Article

Abstract

Residues of pharmaceuticals and personal care products (PPCPs) have been detected in surface waters. Incomplete removal of these compounds by wastewater-treatment plants (WWTPs) results in their presence in effluents and finally in surface waters. The occurrence and removal of four PPCPs was investigated in three WWTPs in Mississippi, USA, during a period of 1 year. Influent and effluent were sampled from the three WWTPs. Upstream and downstream samples of the WWTPs were also collected. All four PPCPs were detected in all influents where sulfamethoxazole showed the highest concentration levels with a median concentration of 1,640 ng/L, and carbamazepine was detected at the lowest level with a median concentration of 132 ng/L. Different PPCPs were removed to different extents varying from 99 to 100 %. Gemfibrozil showed the highest removal rates (73–100 %), whereas carbamazepine showed the lowest (−99 to −30 %). Secondary activated sludge in oxidation-ditch process showed remarkable PPCP-specific removal rates. Galaxolide was removed more than the other PPCPs, and sulfamethoxazole showed the least removal. Galaxolide was found to be a predominant PPCP in effluent among the PPCPs studied, and it was detected in all downstream (14.1–428.2 ng/L) and upstream (4.1–60.0 ng/L) samples. Sulfamethoxazole was removed more during the summer than the winter season. A clear increase of PPCP concentrations was observed in most downstream samples compared with upstream samples suggesting that discharges from WWTPs are the major source of PPCPs in surface waters.

References

  1. Bartelt-Hunt SL, Snow DD, Damon T, Shockley J, Hoagland K (2009) The occurrence of illicit and therapeutic pharmaceuticals in wastewater effluent and surface waters in Nebraska. Environ Pollut 157:786–791CrossRefGoogle Scholar
  2. Batt AL, Kostich MS, Lazorchak JM (2008) Analysis of ecologically relevant pharmaceuticals in wastewater and surface water using selective solid-phase extraction and UPLC–MS/MS. Anal Chem 80:5021–5030CrossRefGoogle Scholar
  3. Bendz D, Paxeus NA, Ginn TR, Loge FJ (2005) Occurrence and fate of pharmaceutically active compounds in the environment, a case study: Hoje River in Sweden. J Hazard Mater 122:195–204CrossRefGoogle Scholar
  4. Bruce GM, Pleus RC, Snyder SA (2010) Toxicological relevance of pharmaceuticals in drinking water. Environ Sci Technol 44:5619–5626CrossRefGoogle Scholar
  5. Clara M, Gans O, Windhofer G, Krenn U, Hartl W, Braun K et al (2011) Occurrence of polycyclic musks in wastewater and receiving water bodies and fate during wastewater treatment. Chemosphere 82:1116–1123CrossRefGoogle Scholar
  6. Collard HR, Ji K, Lee S, Liu X, Kang S, Kho Y et al (2013) Toxicity and endocrine disruption in zebrafish (Danio rerio) and two freshwater invertebrates (Daphnia magna and Moina macrocopa) after chronic exposure to mefenamic acid. Ecotoxicol Environ Saf 94:80–86CrossRefGoogle Scholar
  7. Daneshvar A, Svanfelt J, Kronberg L, Prevost M, Weyhenmeyer GA (2010) Seasonal variations in the occurrence and fate of basic and neutral pharmaceuticals in a Swedish river–lake system. Chemosphere 80:301–309CrossRefGoogle Scholar
  8. Fang Y, Karnjanapiboonwong A, Chase DA, Wang J, Morse AN, Anderson TA (2012) Occurrence, fate, and persistence of gemfibrozil in water and soil. Environ Toxicol Chem 31:550–555CrossRefGoogle Scholar
  9. Gao L, Shi Y, Li W, Niu H, Liu J, Cai Y (2012) Occurrence of antibiotics in eight sewage treatment plants in Beijing, China. Chemosphere 86:665–671CrossRefGoogle Scholar
  10. Ghosh C, Shinde CP, Chakraborty BS (2012) Influence of ionization source design on matrix effects during LC–ESI–MS/MS analysis. J Chromatogr B 893–894:193–200CrossRefGoogle Scholar
  11. Grover DP, Zhou JL, Frickers PE, Readman JW (2011) Improved removal of estrogenic and pharmaceutical compounds in sewage effluent by full scale granular activated carbon: impact on receiving river water. J Hazard Mater 185:1005–1011CrossRefGoogle Scholar
  12. He YJ, Chen W, Zheng XY, Wang XN, Huang X (2013) Fate and removal of typical pharmaceuticals and personal care products by three different treatment processes. Sci Total Environ 447:248–254CrossRefGoogle Scholar
  13. Kupper T, Plagellat C, Brandli RC, de Alencastro LF, Grandjean D, Tarradellas J (2006) Fate and removal of polycyclic musks, UV filters and biocides during wastewater treatment. Water Res 40:2603–2612CrossRefGoogle Scholar
  14. Kwon JW, Armbrust KL, Vidal-Dorsch D, Bay SM, Xia K (2009) Determination of 17 alpha-ethynylestradiol, carbamazepine, diazepam, simvastatin, and oxybenzone in fish livers. J AOAC Int 92:359–369Google Scholar
  15. Lee CJ, Rasmussen TJ (2006) Occurrence of organic wastewater compounds in effluent-dominated streams in Northeastern Kansas. Sci Total Environ 371:258–269CrossRefGoogle Scholar
  16. Letzel M, Metzner G, Letzel T (2009) Exposure assessment of the pharmaceutical diclofenac based on long-term measurements of the aquatic input. Environ Int 35:363–368CrossRefGoogle Scholar
  17. Lin AY, Plumlee MH, Reinhard M (2006) Natural attenuation of pharmaceuticals and alkylphenol polyethoxylate metabolites during river transport: photochemical and biological transformation. Environ Toxicol Chem 25:1458–1464CrossRefGoogle Scholar
  18. Miao XS, Yang JJ, Metcalfe CD (2005) Carbamazepine and its metabolites in wastewater and in biosolids in a municipal wastewater treatment plant. Environ Sci Technol 39:7469–7475CrossRefGoogle Scholar
  19. Mol HG, van Dam RC, Steijger OM (2003) Determination of polar organophosphorus pesticides in vegetables and fruits using liquid chromatography with tandem mass spectrometry: selection of extraction solvent. J Chromatogr A 1015:119–127CrossRefGoogle Scholar
  20. Nakada N, Shinohara H, Murata A, Kiri K, Managaki S, Sato N et al (2007) Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant. Water Res 41:4373–4382CrossRefGoogle Scholar
  21. Nassef M, Kim SG, Seki M, Kang IJ, Hano T, Shimasaki Y et al (2010a) In ovo nanoinjection of triclosan, diclofenac and carbamazepine affects embryonic development of medaka fish (Oryzias latipes). Chemosphere 79:966–973CrossRefGoogle Scholar
  22. Nassef M, Matsumoto S, Seki M, Khalil F, Kang IJ, Shimasaki Y et al (2010b) Acute effects of triclosan, diclofenac and carbamazepine on feeding performance of Japanese medaka fish (Oryzias latipes). Chemosphere 80:1095–1100CrossRefGoogle Scholar
  23. Parolini M, Quinn B, Binelli A, Provini A (2011) Cytotoxicity assessment of four pharmaceutical compounds on the zebra mussel (Dreissena polymorpha) haemocytes, gill and digestive gland primary cell cultures. Chemosphere 84:91–100CrossRefGoogle Scholar
  24. Radjenovic J, Petrovic M, 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 43:831–841CrossRefGoogle Scholar
  25. Ramirez N, Marce RM, Borrull F (2011) Development of a stir bar sorptive extraction and thermal desorption–gas chromatography–mass spectrometry method for determining synthetic musks in water samples. J Chromatogr A 1218:156–161CrossRefGoogle Scholar
  26. Reiner JL, Berset JD, Kannan K (2007) Mass flow of polycyclic musks in two wastewater treatment plants. Arch Environ Contam Toxicol 52:451–457CrossRefGoogle Scholar
  27. Rosal R, Rodriguez A, Perdigon-Melon JA, Petre A, Garcia-Calvo E, Gomez MJ et al (2010) Occurrence of emerging pollutants in urban wastewater and their removal through biological treatment followed by ozonation. Water Res 44:578–588CrossRefGoogle Scholar
  28. Santos JL, Aparicio I, Callejon M, Alonso E (2009) Occurrence of pharmaceutically active compounds during 1-year period in wastewaters from four wastewater treatment plants in Seville (Spain). J Hazard Mater 164:1509–1516CrossRefGoogle Scholar
  29. Saravanan M, Ramesh M (2013) Short and long-term effects of clofibric acid and diclofenac on certain biochemical and ionoregulatory responses in an Indian major carp, Cirrhinus mrigala. Chemosphere 93:388–396CrossRefGoogle Scholar
  30. Segura PA, Gagnon C, Sauve S (2007) A fully automated on-line preconcentration and liquid chromatography–tandem mass spectrometry method for the analysis of anti-infectives in wastewaters. Anal Chim Acta 604:147–157CrossRefGoogle Scholar
  31. Sim WJ, Lee JW, Lee ES, Shin SK, Hwang SR, Oh JE (2011) Occurrence and distribution of pharmaceuticals in wastewater from households, livestock farms, hospitals and pharmaceutical manufactures. Chemosphere 82:179–186CrossRefGoogle Scholar
  32. Snider SA (2008) Occurrence, treatment, and toxicological relevance of EDCs and pharmaceuticals in water. Ozone Sci Eng 30:65–69CrossRefGoogle Scholar
  33. Spongberg AL, Witter JD (2008) Pharmaceutical compounds in the wastewater process stream in Northwest Ohio. Sci Total Environ 397:148–157CrossRefGoogle Scholar
  34. Sui Q, Huang J, Deng S, Yu G, Fan Q (2010) Occurrence and removal of pharmaceuticals, caffeine and DEET in wastewater treatment plants of Beijing, China. Water Res 44:417–426CrossRefGoogle Scholar
  35. 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 45:3341–3348CrossRefGoogle Scholar
  36. Thomas PM, Foster GD (2005) Tracking acidic pharmaceuticals, caffeine, and triclosan through the wastewater treatment process. Environ Toxicol Chem 24:25–30CrossRefGoogle Scholar
  37. Tong AY, Peake BM, Braund R (2011) Disposal practices for unused medications around the world. Environ Int 37:292–298CrossRefGoogle Scholar
  38. United States Environmental Protection Agency (2011) Pharmaceuticals and personal care products (PPCPs). http://epa.gov/ppcp. Accessed 14 Feb 2013
  39. Van Eeckhaut A, Lanckmans K, Sarre S, Smolders I, Michotte Y (2009) Validation of bioanalytical LC–MS/MS assays: evaluation of matrix effects. J Chromatogr B 877:2198–2207CrossRefGoogle Scholar
  40. Vieno N, Tuhkanen T, Kronberg L (2007a) Elimination of pharmaceuticals in sewage treatment plants in Finland. Water Res 41:1001–1012CrossRefGoogle Scholar
  41. Vieno NM, Harkki H, Tuhkanen T, Kronberg L (2007b) Occurrence of pharmaceuticals in river water and their elimination in a pilot-scale drinking water treatment plant. Environ Sci Technol 41:5077–5084CrossRefGoogle Scholar
  42. Westerhoff P, Yoon Y, Snyder S, Wert E (2005) Fate of endocrine-disruptor, pharmaceutical, and personal care product chemicals during simulated drinking water treatment processes. Environ Sci Technol 39:6649–6663CrossRefGoogle Scholar
  43. Winkler M, Headley JV, Peru KM (2000) Optimization of solid-phase microextraction for the gas chromatographic–mass spectrometric determination of synthetic musk fragrances in water samples. J Chromatogr A 903:203–210CrossRefGoogle Scholar
  44. Xu B, Mao D, Luo Y, Xu L (2011) Sulfamethoxazole biodegradation and biotransformation in the water–sediment system of a natural river. Bioresour Technol 102:7069–7076CrossRefGoogle Scholar
  45. Yan Q, Gao X, Chen Y-P, Peng X-Y, Zhang Y-X, Gan X-M et al (2014) Occurrence, fate and ecotoxicological assessment of pharmaceutically active compounds in wastewater and sludge from wastewater treatment plants in Chongqing, the Three Gorges Reservoir Area. Sci Total Environ 470–471:618–630Google Scholar
  46. Yang SF, Lin CF, Lin AY, Hong PK (2011) Sorption and biodegradation of sulfonamide antibiotics by activated sludge: experimental assessment using batch data obtained under aerobic conditions. Water Res 45:3389–3397CrossRefGoogle Scholar
  47. Yu Y, Wu L (2012) Analysis of endocrine disrupting compounds, pharmaceuticals and personal care products in sewage sludge by gas chromatography–mass spectrometry. Talanta 89:258–263CrossRefGoogle Scholar
  48. Zhou JL, Zhang ZL, Banks E, Grover D, Jiang JQ (2009) Pharmaceutical residues in wastewater treatment works effluents and their impact on receiving river water. J Hazard Mater 166:655–661CrossRefGoogle Scholar
  49. Zhou LJ, Ying GG, Liu S, Zhao JL, Yang B, Chen ZF et al (2013) Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China. Sci Total Environ 452–453:365–376CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media New York 2013

Authors and Affiliations

  1. 1.Mississippi State Chemical LaboratoryMississippi State UniversityMississippi StateUSA
  2. 2.Department of Biochemistry and Molecular Biology, Entomology and Plant PathologyMississippi State UniversityMississippi StateUSA

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