Abstract
Pharmaceuticals and personal care products (PPCPs) can reach soil and aquatic environments through land application of wastewater effluent and agricultural runoff. The objective of this research was to assess the fate of PPCPs at field scale. PPCPs were measured systematically in a wastewater treatment plant (WWTP), and in soil and groundwater receiving treated effluent from the WWTP. A land application site in West Texas was used as the study site; it has received treated wastewater effluent from the WWTP for more than 70 years in order to remove additional nutrients and irrigate non-edible crops. Target compounds (estrone, 17β-estradiol, estriol, 17α-ethynylestradiol, triclosan, caffeine, ibuprofen, and ciprofloxacin) in wastewater, sewage sludge, soil, and groundwater were determined using HPLC/UV with qualitative confirmatory analyses using GC/MS. Samples were collected quarterly over 12 months for wastewater and sludge samples and over 9 months for soil and groundwater samples. Results indicated that concentrations of PPCPs in wastewater influent, effluent, sludge solid phase, and sludge liquid phase were in the range of non-detected (ND)-183 μg/L, ND-83 μg/L, ND-19 μg/g, and ND-50 μg/L, respectively. Concentrations in soil and groundwater samples were in the range of ND-319 ng/g and ND-1,745 μg/L, respectively. GC/MS confirmation data were consistent with the results of HPLC/UV analyses. Overall, data indicate that PPCPs in the wastewater effluent from the WWTP transport both vertically and horizontally in the soil, and eventually reach groundwater following land application of the effluent.
Similar content being viewed by others
References
Allaire, S. E., Castillo, J. D., & Juneau, V. (2006). Sorption kinetics of chlortetracycline and tylosin on sandy loam and heavy clay soils. Journal of Environmental Quality, 35(4), 969–972.
Andersen, H., Siegrist, H., Halling-SØrensen, B., & Ternes, T. A. (2003). Fate of estrogens in a municipal sewage treatment plant. Environmental Science & Technology, 37(18), 4021–4026.
Andersen, H. R., Hansen, M., KjØlholt, J., Stuer-Lauridsen, F., Ternes, T., & Halling-SØrensen, B. (2005). Assessment of the importance of sorption for steroid estrogens removal during activated sludge treatment. Chemosphere, 61(1), 139–146.
Ankley, G. T., Brooks, B. W., Huggett, D. B., & Sumpter, J. P. (2007). Repeating history: pharmaceuticals in the environment. Environmental Science & Technology, 41(24), 8211–8217.
Aranami, K., & Readman, J. W. (2007). Photolytic degradation of triclosan in freshwater and seawater. Chemosphere, 66(6), 1052–1056.
Belden, J. B., Maul, J. D., & Lydy, M. J. (2007). Partitioning and photodegradation of ciprofloxacin in aqueous systems in the presence of organic matter. Chemosphere, 66(8), 1390–1395.
Bester, K. (2005). Fate of triclosan and triclosan-methyl in sewage treatment plants and surface waters. Archives of Environmental Contamination and Toxicology, 49(1), 9–17.
Boxall, A. B. A. (2008). Fate and transport of veterinary medicines in the soil environment. In D. S. Aga (Ed.), Fate of Pharmaceuticals in the Environment and in Water Treatment Systems (pp. 123–137). Florida: CRC.
Buerge, I. J., Poiger, T., Müller, M. D., & Buser, H. R. (2003). Caffeine, an anthropogenic marker for wastewater contamination of surface waters. Environmental Science & Technology, 37(4), 691–700.
Cardoza, L. A., Knapp, C. W., Larive, C. K., Belden, J. B., Lydy, M., & Graham, D. W. (2005). Factors affecting the fate of ciprofloxacin in aquatic field systems. Water, Air, and Soil Pollution, 161(1–4), 383–398.
Casey, F. X. M., Šimůnek, J., Lee, J., Larsen, G. L., & Hakk, H. (2005). Sorption, mobility, and transformation of estrogenic hormones in natural soil. Journal of Environmental Quality, 34(4), 1372–1379.
Chenxi, W., Spongberg, A. L., & Witter, J. D. (2008). Determination of the persistence of pharmaceuticals in biosolids using liquid-chromatography tandem mass spectrometry. Chemosphere, 73(4), 511–518.
Christian, T., Schneider, R. J., Färber, H. A., Skutlarek, D., Meyer, M. T., & Goldbach, H. E. (2003). Determination of antibiotic residues in manure, soil, and surface waters. Acta Hydrochimica et Hydrobiologica, 31(1), 36–44.
Chu, S., & Metcalfe, C. D. (2007). Simultaneous determination of triclocarban and triclosan in municipal biosolids by liquid chromatography tandem mass spectrometry. Journal of Chromatography. A, 1164(1–2), 212–218.
Colucci, M. S., Bork, H., & Topp, E. (2001). Persistence of estrogenic hormones in agricultural soils: I. 17β-estradiol and estrone. Journal of Environmental Quality, 30(6), 2070–2076.
Cordy, G. E., Duran, N. L., Bouwer, H., Rice, R. C., Furlong, E. T., Zaugg, S. D., et al. (2004). Do pharmaceuticals, pathogens, and other organic waste water compounds persist when waste water is used for recharge? Ground Water Monitoring and Remediation, 24(2), 58–69.
D’Ascenzo, G., Di Corcia, A., Gentilli, A., Mancini, R., Mastropasqua, R., Nazzari, M., et al. (2003). The Science of the Total Environment, 302(1–3), 199–209.
Daughton, C. G., & Ternes, T. A. (1999). Pharmaceuticals and personal care products in the environment: agent of subtle change? Environmental Health Perspectives, 107(S6), 907–938.
Davis, M.L., & Cornwell, D.F. (1998). Introduction to Environmental Engineering (3rd Ed.). McGraw-Hill Higher Education. ISBN 0-07-015918-1.
Drillia, P., Stamatelatou, K., & Lyberatos, G. (2005). Fate and mobility of pharmaceuticals in solid matrices. Chemosphere, 60(8), 1034–1044.
EPA, U. S. (2000). SW846 test methods. Washington: USEPA.
Gielen, G. J. H. P., Van Den Heuvel, M. R., Clinton, P. W., & Greenfield, L. G. (2009). Factors impacting on pharmaceutical leaching following sewage application to land. Chemosphere, 74(4), 537–542.
Giger, W., Alder, A. C., Golet, E. M., Kohler, H. P. E., McArdell, C. S., Molnar, E., et al. (2003). Occurrence and fate of antibiotics as trace contaminants in wastewaters, sewage sludges and surface waters. Chimia, 57(9), 485–491.
Glassmeyer, S. T., Kolpin, D. W., Furlong, E. T., & Focazio, M. J. (2008). Environmental presence and persistence of pharmaceuticals: An Overview. In D. S. Aga (Ed.), Fate of pharmaceuticals in the environment and in water treatment systems (pp. 3–51). Florida: CRC.
Gross, B., Montgomery-Brown, J., Naumann, A., & Reinhard, M. (2004). Occurrence and fate of pharmaceuticals and alkylphenol ethoxylate metabolites in an effluent-dominated river and wetland. Environmental Toxicology and Chemistry, 23(9), 2074–2083.
Haggard, B. E., Galloway, J. M., Green, W. R., & Meyer, M. T. (2006). Pharmaceuticals and other organic chemicals in selected north-central and northwestern Arkansas streams. Journal of Environmental Quality, 35(4), 1078–1087.
Harrison, E. Z., Oakes, S. R., Hysell, M., & Hay, A. (2006). Organic chemicals in sewage sludges. The Science of the Total Environment, 367(2–3), 481–497.
Heberer, T. (2002a). Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicology Letters, 131(1–2), 5–17.
Heberer, T. (2002b). Tracking persistent pharmaceutical residues from municipal sewage to drinking water. Journal of Hydrology, 266(3–4), 175–189.
Hildebrand, C., Londry, K. L., & Farenhorst, A. (2006). Sorption and desorption of three endocrine disrupters in soils. Journal of Environmental Science and Health. Part B, 41(6), 907–921.
Holbrook, R. D., Novak, J. T., Grizzard, T. J., & Love, N. G. (2002). Estrogen receptor agonist fate during wastewater and biosolids treatment processes: a mass balance analysis. Environmental Science & Technology, 36(21), 4533–4539.
Jacobsen, A. M., Lorenzen, A., Chapman, R., & Topp, E. (2005). Persistence of testosterone and 17β-estradiol in soils receiving swine manure or municipal biosolids. Journal of Environmental Quality, 34(3), 861–871.
Karnjanapiboonwong, A., Morse, A. N., Maul, J. D., & Anderson, T. A. (2010). Sorption of estrogens, triclosan, and caffeine in a sandy loam and a silt loam soil. Journal of Soils and Sediments. doi:10.1007/s11368-010-0223-5.
Kim, S., Weber, A. S., Batt, A., & Aga, D. S. (2008). Removal of pharmaceuticals in biological wastewater treatment plants. In D. S. Aga (Ed.), Fate of pharmaceuticals in the environment and in water treatment systems (pp. 349–361). Florida: CRC.
Kinney, C. A., Furlong, E. T., Werner, S. L., & Cahill, J. D. (2006). Presence and distribution of wastewater-derived pharmaceuticals in soil irrigated with reclaimed water. Environmental Toxicology and Chemistry, 25(2), 317–326.
Kirk, L. A., Tyler, C. R., Lye, C. M., & Sumpter, J. P. (2002). Changes in estrogenic and androgenic activities at different stages of treatment in wastewater treatment works. Environmental Toxicology and Chemistry, 21(5), 972–979.
Kolpin, D. W., Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B., et al. (2002). Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999–2000: a national reconnaissance. Environmental Science & Technology, 36(6), 1202–1211.
Kreuzinger, N., Clara, M., Strenn, B., & Kroiss, H. (2004). Relevance of the sludge retention time (SRT) as design criteria for wastewater treatment plants for the removal of endocrine disruptors and pharmaceuticals from wastewater. Water Science and Technology, 50(5), 149–156.
Kreuzinger, N., Clara, M., Strenn, B., & Vogel, B. (2004). Investigation on the behaviour of selected pharmaceuticals in the groundwater after infiltration of treated wastewater. Water Science and Technology, 50(2), 221–228.
Kümmerer, K. (2004). Pharmaceuticals in the environment: sources, fate, effects, and risk (2nd ed.). Berlin: Springer.
Kvanli, D. M., Marisetty, S., Anderson, T. A., Jackson, W. A., & Morse, A. N. (2008). Monitoring estrogen compounds in wastewater recycling systems. Water, Air, and Soil Pollution, 188(1–4), 31–40.
Lee, H. B., Peart, T. E., & Svoboda, M. L. (2007). Determination of ofloxacin, norfloxacin, and ciprofloxacin in sewage by selective solid-phase extraction, liquid chromatography with fluorescence determination, and liquid chromatography-tandem mass spectrometry. Journal of Chromatography. A, 1139(1), 45–52.
Lin, A. Y. C., & Reinhard, M. (2005). Photodegradation of common environmental pharmaceuticals and estrogens in river water. Environmental Toxicology and Chemistry, 24(6), 1303–1309.
Machatha, S. G., & Yalkowsky, S. H. (2005). Comparison of the octanol/water partition coefficients calculated by ClogP®, ACDlogP and KowWin® to experimentally determined values. International Journal of Pharmaceutics, 294(1–2), 185–192.
Mansell, J., & Drewes, J. E. (2004). Fate of steroidal hormones during soil-aquifer treatment. Ground Water Monitoring and Remediation, 24(2), 94–101.
Mansell, J., Drewes, J. E., & Rauch, T. (2004). Removal mechanisms of endocrine disrupting compounds (steroids) during soil aquifer treatment. Water Science and Technology, 50(2), 229–237.
Matamoros, V., Duhec, A., Albaigés, J., & Bayona, J. M. (2009). Photodegradation of carbamazepine, ibuprofen, ketoprofen, and 17α-ethinylestradiol (EE2) in fresh and seawater. Water, Air, and Soil Pollution, 196(1–4), 161–168.
Mazellier, P., Méité, L., & Laat, D. E. (2008). Photodegradation of the steroid hormones 17β-estradiol (E2) and 17α-ethinylestradiol (EE2) in dilute aqueous solution. Chemosphere, 73(8), 1216–1223.
McAvoy, D. C., Schatowitz, B., Jacob, M., Hauk, A., & Eckhoff, W. S. (2002). Measurement of triclosan in wastewater treatment systems. Environmental Toxicology and Chemistry, 21(7), 1323–1329.
Monteiro, S. C., & Boxall, A. B. (2009). Factors affecting the degradation of pharmaceuticals in agricultural soils. Environmental Toxicology and Chemistry, 28(12), 2546–2554.
Nakada, N., Tanishima, T., Shinohara, H., Kiri, K., & Takada, H. (2006). Pharmaceutical chemicals and endocrine disrupters in municipal wastewater in Tokyo and their removal during activated sludge treatment. Water Research, 40(17), 3297–3303.
Nakada, N., Kiri, K., Shinohara, H., Harada, A., Kuroda, K., Takizawa, S., et al. (2008). Evaluation of pharmaceuticals and personal care products as water-soluble molecular markers of sewage. Environmental Science & Technology, 42(17), 6347–6353.
Oppel, J., Broll, G., Löffler, D., Meller, M., Römbke, J., & Ternes, T. (2004). Leaching behavior of pharmaceuticals in soil-testing-systems: a part of an environmental risk assessment for groundwater protection. The Science of the Total Environment, 328(1–3), 265–273.
Osenbrück, K., Gläser, H. R., Knöller, K., Weise, S. M., Möder, M., Wennrich, R., et al. (2007). Sources and transport of selected organic micropollutants in urban groundwater underlying the city of Halle (Saale), Germany. Water Research, 41(15), 3259–3270.
Overcash, M., Sims, R. C., Sims, J. L., & Nieman, J. K. C. (2005). Beneficial reuse of sustainability: the fate of organic compounds in land-applied waste. Journal of Environmental Quality, 34(1), 29–51.
Pedersen, J. A., Soliman, M., & Suffet, I. H. M. (2005). Human pharmaceuticals, hormones, and personal care product ingredients in runoff from agricultural fields irrigated with treated wastewater. Journal of Agricultural and Food Chemistry, 53(5), 1625–1632.
Phillips, G., Johnson, B. E., & Ferguson, J. (1990). The loss of antibiotic activity of ciprofloxacin by photodegradation. The Journal of Antimicrobial Chemotherapy, 26(6), 783–789.
Polar, J.A. (2007). The fate of pharmaceuticals after wastewater treatment. Florida Water Resources Journal, June, 26–31
Rodriguez-Mozaz, S., López de Alda, M. J., & Barceló, D. (2004). Monitoring of estrogens, pesticides and bisphenol A in natural waters and drinking water treatment plants by solid-phase extraction-liquid chromatography-mass spectrometry. Journal of Chromatography. A, 1045(1–2), 85–92.
Sangsupan, H. A., Radcliffe, D. E., Hartel, P. G., Jenkins, M. B., Vencill, W. K., & Cabrera, M. L. (2006). Sorption and transport of 17β-estradiol and testosterone in undisturbed soil columns. Journal of Environmental Quality, 35(6), 2261–2272.
Scheytt, T., Mersmann, P., Lindstädt, R., & Heberer, T. (2005). Determination of sorption coefficients of pharmaceutically active substances carbamazepine, diclofenac, and ibuprofen, in sandy sediments. Chemosphere, 60(2), 245–253.
Scheytt, T. J., Mersmann, P., & Heberer, T. (2006). Mobility of pharmaceuticals carbamazepine, diclofenac, ibuprofen, and propyphenazone in miscible-displacement experiments. Journal of Contaminant Hydrology, 83(1–2), 53–69.
Sedlak, D. L., & Pinkston, K. E. (2001). Factors affecting the concentrations of pharmaceuticals released to the aquatic environment. Water Resources Update, 120, 56–64.
Snyder, S. A., Leising, J., Westerhoff, P., Yoon, Y., Mash, H., & Vanderford, B. (2004). Biological and physical attenuation of endocrine disruptors and pharmaceuticals: implications for water reuse. Ground Water Monitoring and Remediation, 24(2), 108–118.
Snyder, S. A., Lei, H., & Wert, E. C. (2008). Removal of endocrine disruptors and pharmaceuticals during water treatment. In D. S. Aga (Ed.), Fate of pharmaceuticals in the environment and in water treatment systems (pp. 229–259). Florida: CRC.
Ternes, T., Bonerz, M., & Schmidt, T. (2001). Determination of neutral pharmaceuticals in wastewater and rivers by liquid chromatography-electrospray tandem mass spectrometry. Journal of Chromatography. A, 938(1–2), 175–185.
Thomas, P. M., & Foster, G. D. (2004). Determination of nonsteroidal anti-inflammatory drugs, caffeine, and triclosan in wastewater by gas chromatography-mass spectrometry. Journal of Environmental Science and Health Part A, 39(8), 1969–1978.
Thomas, P. M., & Foster, G. D. (2005). Tracking acidic pharmaceuticals, caffeine, and triclosan through the wastewater treatment process. Environmental Toxicology and Chemistry, 24(1), 25–30.
Thomas, A. T., Andersen, H., Gilberg, D., & Bonerz, M. (2002). Determination of estrogens in sludge and sediments by liquid extraction and GC/MS/MS. Analytical Chemistry, 74(14), 3498–3504.
Thompson, A., Griffin, P., Stuetz, R., & Cartmell, E. (2005). The fate and removal of triclosan during wastewater treatment. Water Environment Research, 77(1), 63–67.
Topp, E., Hendel, J., Lu, Z., & Chapman, R. (2006). Biodegradation of caffeine in agricultural soil. Canadian Journal of Soil Science, 86(3), 533–544.
Uslu, M. Ö., Yediler, A., Balcioğlu, I. A., & Schulte-Hostede, S. (2008). Analysis and sorption behavior of fluoroquinolones in solid matrices. Water, Air, and Soil Pollution, 190(1–4), 55–63.
Waltman, E. L., Venables, B. J., & Waller, W. T. (2006). Triclosan in a North Texas wastewater treatment plant and the influent and effluent of an experimental constructed wetland. Environmental Toxicology and Chemistry, 25(2), 367–372.
Xu, J., Chen, W., Wu, L., Green, R., & Chang, A. C. (2009). Leachability of some emerging contaminants in reclaimed municipal wastewater-irrigated turf grass fields. Environmental Toxicology and Chemistry, 28(9), 1842–1850.
Xuan, R., Blassengale, A. A., & Wang, Q. (2008). Degradation of estrogenic hormones in a silt loam soil. Journal of Agricultural and Food Chemistry, 56(19), 9152–9158.
Ying, G. G., & Kookana, R. S. (2005). Sorption and degradation of estrogen-like-endocrine disrupting chemicals in soil. Environmental Toxicology and Chemistry, 24(10), 2640–2645.
Ying, G. G., & Kookana, R. S. (2007). Triclosan in wastewaters and biosolids from Australian wastewater treatment plants. Environment International, 33(2), 199–205.
Ying, G.G., Kookana, R., & Waite, T.D. (2004). Endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in reclaimed water in Australia. Australian water conservation and reuse research program. ISBN 0643091807
Acknowledgments
This study was partially funded by the Texas Water Resources Institute (TWRI) and the US EPA. Special thanks to individuals for assisting in sample collection and access to the WRP and the LAS.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Karnjanapiboonwong, A., Suski, J.G., Shah, A.A. et al. Occurrence of PPCPs at a Wastewater Treatment Plant and in Soil and Groundwater at a Land Application Site. Water Air Soil Pollut 216, 257–273 (2011). https://doi.org/10.1007/s11270-010-0532-8
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11270-010-0532-8