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http://dx.doi.org/10.11001/jksww.2018.32.6.559

Evaluation and application of pretreatment methods for pharmaceuticals and personal care products in the solid phase of sewage samples  

Park, Junwon (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Kim, Changsoo (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Ju, Byoungkyu (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Lee, Wonseok (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Chung, Hyenmi (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Jeong, Dong-Hwan (National Institute of Environmental Research, Water Supply and Sewerage Research Division)
Publication Information
Journal of Korean Society of Water and Wastewater / v.32, no.6, 2018 , pp. 559-572 More about this Journal
Abstract
The aim of this study was to evaluate pretreatment methods for 27 pharmaceuticals and personal care products (PPCPs) in various sewage samples using a modified quick, easy, cheap, effective, rugged, and safe (QuEChERS) and online solid-phase extraction with LC-MS/MS. Extraction efficiencies of PPCPs in the solid phase under different experimental conditions were evaluated, showing that the highest recoveries were obtained with the addition of sodium sulfate and ethylenediaminetetraacetic acid disodium salt dehydrate in acidified conditions. The recoveries of target compounds ranged from 91 to 117.2% for liquid samples and from 61.3 to 137.2% for solid samples, with a good precision. The methods under development were applied to sewage samples collected in two sewage treatment plants (STPs) to determine PPCPs in liquid and solid phases. Out of 27 PPCPs, more than 19 compounds were detected in liquid samples (i.e., influent and effluent) of two STPs, with concentration ranges of LOQ-33,152 ng/L in influents and LOQ-4,523 ng/L in effluents, respectively. In addition, some PPCPs such as acetylsalicylic acid, ibuprofen, and ofloxacin were detected at high concentrations in activated sludge as well as in excess sludge. This methodology was successfully applied to sewage samples for the determination of the target compounds in STPs.
Keywords
Method validation; Online SPE; Pharmaceuticals and personal care products; Pretreatment method; Sewage treatment plants;
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1 Anastassiades, M., Lehotay, S.J., Stajnbaher, D., and Schenck, F.J. (2003). Fate and easy multiresidue method employing acetonitrile extraction/partitioning and "dispersive solid-phase-extraction" for the determination of pesticide residues in produce, J. AOAC Int., 86(2), 412-431.
2 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.   DOI
3 Association of Analytical communities (AOAC) International (2011). AOAC Official Method 2007.01 pesticide residues in foods by acetonitrile extraction and partitioning with magnesium sulfate, Off. Methods Anal. AOAC Int., 90, 17-26.
4 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.   DOI
5 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 chromatographytandem mass spectrometry: Optimisation and matrix effects reduction by quick, easy, cheap, effective, rugged and safe extraction, J. Chromatography A, 1349, 11-23.   DOI
6 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.   DOI
7 Goh, S.X.L., Duarah, A., Zhang, L., Snyder, S.A., and Lee, H.K. (2016). Online solid phase extraction with liquid chromatography-tandem mass spectrometry for determination of estrogens and glucocorticoids in water, J. Chromatography A, 1465, 1-9.   DOI
8 Daughton, C.G. and Ternes, T.A. (1999). Pharmaceuticals and personal care products in the environment: agents of subtle change?, Environ. Health Perspect., 107, 907-938.   DOI
9 European Committee for Standardization (CEN) (2008). Foods of plant origin - determination of pesticide residues using GC-MS and/or LC-MS/MS following acetonitrile extraction/partitioning and clean-up by dispersive SPE - QuEChERS-method, EN 15662, 24, 1-83.
10 Gabet-Giraud, V., Miege, C., Choubert, J.M., Ruel, S.M., and Coquery, M. (2010). Occurrence and removal of estrogens and beta blockers by various processes in wastewater treatment plants, Sci. Total Environ., 408, 4257-4269.   DOI
11 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.   DOI
12 Guo, C., Wang, M., Xiao, H., Huai, B., Wang, F., Pan, G., Liao, X., and Liu, Y. (2016). Development of a modified QuEChERS method for the determination of veterinary antibiotics in swine manure by liquid chromatography tandem mass spectrometry, J. Chromatography B, 1027, 110-118.   DOI
13 Hwang, Y., Shin, S., and Park, J. (2013). Development of the analytical method for residual pharmaceuticals in raw water using online sample preconcentration with high resolution LC-ESI/Orbitrap MS, J. Korean Soc. Water Environ., 29(3), 409-419.
14 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.   DOI
15 Joss, A., Zabczynski, S., Gobel, A., Hoffmann, B., Loffler, D., McArdell, C.S., Ternes, T.A., Thomsen, A., and Siegrist, H. (2006). Biological degradation of pharmaceuticals in municipal wastewater treatment: Proposing a classification scheme, Water Res., 40, 1686-1696.   DOI
16 Khan, G.A., Lindberg, R., Grabic, R., and Fick, J. (2012). The development and application of a system for simultaneously determining anti-infectives and nasal decongestants using on-line solid-phase extraction and liquid chromatographytandem mass spectrometry, J. Pharmacol. Biomed. Anal., 66, 24-32.   DOI
17 Kim, J.W., Yoon, S.M., Lee. S.J., Narumiya, M., Nakada, N., Han, I.S., and Tanaka, H. (2012). Occurrence and fate of PPCPs wastewater treatment plants in Korea, Proceedings of 2nd International Conference on Environment and Industrial Innovation, 2-3 June, 2012, Singapore.
18 Lindsey, M.E., Meyer, M., and Thurman, E.M. (2001). Analysis of trace levels of sulfonamide and tetracycline antimicrobials in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometry, Anal. Chem., 73, 4640-4646.   DOI
19 Lopez-Serna, R., Perez, S., Ginebreda, A., Petrovic, M., and Barcelo, D. (2010). Fully automated determination of 74 pharmaceuticals in environmental and waste waters by online solid phase extraction-liquid chromatographyelectrospray-tandem mass spectrometry, Talanta, 83, 410-424.   DOI
20 Marshall, A.J. and Piddock, L.J. (1994). Interaction of divalent cations, quinolones and bacteria, J. Antimicrob. Chemother., 34 (4), 465-483.   DOI
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.   DOI
22 National Institute of Environmental Research. (2012). A study of discharge source and variation for pharmaceuticals in the environment (V), 1-6.
23 Pailler, J.Y., Krein, A., Pfister, L., Hoffmann, L., and Guignard, C. (2009). Solid phase extraction coupled to liquid chromatography-tandem mass spectrometry analysis of sulfonamides, tetracyclines, analgesics and hormones in surface water and wastewater in Luxembourg, Sci. Total Environ., 407, 4736-4743.   DOI
24 Panditi, V.R., Batchu, S.R., and Gardinali, P.R. (2013). Online solid-phase extraction-liquid chromatography-electrospraytandem mass spectrometry determination of multiple classes of antibiotics in environmental and treated waters, Anal. Bioanal. Chem., 405, 5953-5964.   DOI
25 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.   DOI
26 Ponce-Robles, L., Rivas, G., Esteban, B., Oller, I., Malato, S., and Aguera, A. (2017). Determination of pesticides in sewage sludge from an agro-food industry using QuEChERS extraction followed by analysis with liquid chromatography-tandem mass spectrometry, Anal. Bioanal. Chem., 409, 6181-6193.   DOI
27 Ternes, T.A. and Joss, A. (2006). Human pharmaceuticals, hormones and fragrances, IWA, 203-206.
28 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 chromatographytandem mass spectrometry for the determination of non-steroidal anti-inflammatory drugs and their metabolites in sewage sludge, Anal. Chim. Acta, 935, 269-281.   DOI
29 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.   DOI
30 Sui, Q., Zhao, W., Cao, X., Lu, S., Qiu, Z., Gu, W., and Yu, G. (2015). Pharmaceuticals and personal care products in the leachates from a typical landfill reservoir of municipal solid waste in Shanghai, China: occurrence and removal by a full-scale membrane reactor, J. Hazard. Mater., 323, 99-108.
31 Tran, N.H., Chen, H., Reinhard, M., Mao, F., and Gin, K.Y.H. (2016). Occurrence and removal of multiple classes of antibiotics and antimicrobial agents in biological wastewater treatment processes, Water Res., 104, 461-472.   DOI
32 Trenholm, R.A., Vanderford, B.J., and Snyder, S.A. (2009). On-line solid phase extraction LC-MS/MS analysis of pharmaceutical indicators in water: A green alternative to conventional methods, Talanta, 79, 1425-1432.   DOI
33 US EPA. (2007). Method 1694: Pharmaceuticals and Personal Care Products in Water, Soil, Sediment, and Biosolids by HPLC/MS/MS, US EPA, Washington D.C., USA.
34 Vieno, N., Tuhkanen, T., and Kronberg, L. (2007). Elimination of pharmaceuticals in sewage treatment plants in Finland, Water Res., 41, 1001-1012.   DOI
35 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.   DOI