Korean Journal of Soil Science and Fertilizer (한국토양비료학회지)

Korean Society of Soil Science and Fertilizer (한국토양비료학회)
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Concentration and Environmental Loading of Veterinary Antibiotics in Agricultural Irrigation Ditches

  • Kim, Sung-Chul (Department of Bio Environmental Chemistry, Chungnam National University) ;
  • Chung, Doug Young (Department of Bio Environmental Chemistry, Chungnam National University) ;
  • Kim, Kye Hoon (Department of Environmental Horticulture, University of Seoul) ;
  • Lee, Ja Hyun (Rural Development Administration) ;
  • Kim, Hyo Kyung (Rural Development Administration) ;
  • Yang, Jae E. (Department of Biological Environment, Kangwon National University) ;
  • Ok, Yong Sik (Department of Biological Environment, Kangwon National University) ;
  • Almarwei, Yaser A.O. (Department of Biological Environment, Kangwon National University)
  • Received : 2012.09.12
  • Accepted : 2012.12.05
  • Published : 2012.12.31
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Abstract

The concentration of veterinary antibiotics in aqueous and sediment matrices was measured in agricultural irrigation ditches bordering several animal-feeding operations (AFOs) and then compared to its concentration in the watershed. Analytical determination in aqueous samples was based on solid phase extraction (SPE) and appropriate buffer solutions were used to extract residuals in sediment samples. Separation and detection of extracted veterinary antibiotics were performed with high performance liquid chromatograph tandem mass spectrometry (HPLC/MS/MS). In general, higher concentrations of antibiotic were observed in the aqueous phase of irrigation ditches, with the highest concentration of erythromycin hydrochloride (ETM-$H_2O$) of $0.53{\mu}g\;L^{-1}$, than in aqueous watershed samples. In contrast, higher concentrations were measured in river sediment than in irrigation ditch sediment with the highest concentration of oxytetracycline of $110.9{\mu}g\;kg^{-1}$. There was a high calculated correlation ( > 0.95) between precipitation and measured concentration in aqueous samples from the irrigation ditches for five of the ten targeted veterinary antibiotics, indicating that surface runoff could be an important transport mechanism of veterinary antibiotics from field to environment. Further, environmental loading calculation based on measured concentrations in aqueous samples and flow information clearly showed that irrigation ditches were 18 times greater than river. This result suggests the likelihood that veterinary antibiotics can be transported via irrigation ditches to the watershed. The transport via surface runoff and likely environmental loading via irrigation ditches examined in this study helps identify the pathway of veterinary antibiotics residuals in the environment.

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References

  1. Blackwell, P.A., H.H. Lutzhoft, H.P. Ma, B. Halling-Sorensen, A.B.A. Boxwell, and Kay, P. 2004. Ultrasonic extraction of veterinary antibiotics from soils and pig slurry with SPE clean-up and LC-UV and fluorescence detection. Talanta, 64:1058-1064. https://doi.org/10.1016/j.talanta.2004.05.006
  2. Bruhn, S.T. 2003. Pharmaceutical antibiotic compounds in soils - a review. Journal of Plant Nutrition and Soil Science, 166:145 - 167. https://doi.org/10.1002/jpln.200390023
  3. Burkhardt, M., C. Stamm, C. Waul, H. Singer, and S. Muller. 2005. Surface runoff and transport of sulfonamide antibiotics and tracers on manured grassland. Journal of Environmental Quality, 34:1363-1371. https://doi.org/10.2134/jeq2004.0261
  4. Campagnolo, E.R., K.R. Johnson, A. Karpati, C.S. Rubin, D.W. Kolpin, M.T. Meyer, and J.E. Esteban. 2002. Antimicrobial residuals in animal waste and water resources proximal to large-scale swine and poultry feeding operations. Science of the Total Environment, 299:89 - 95. https://doi.org/10.1016/S0048-9697(02)00233-4
  5. Castiglioni, S., R. Bagnati, R. Fanelli, F. Pomati, D. Calamari, and E. Zuccato. 2006. Removal of pharmaceuticals in sewage treatment plants in Italy. Environmental Science and Technology, 40:357-363. https://doi.org/10.1021/es050991m
  6. Chee-Sanford, J.C., R.I. Aminov, I.J. Krapac, N. Garrigues-Jeanjean, and R.I. Mackie. 2001. Occurrence and diversity of tetracycline resistance genes in lagoons and groundwatr underlying two swine production facilities. Applied and Environmental Microbiology, 67:1494-1502. https://doi.org/10.1128/AEM.67.4.1494-1502.2001
  7. Cromwell, G. 2002. Why and how antibiotics are used in swine production. Animal Biotechnology, 13:7. https://doi.org/10.1081/ABIO-120005767
  8. Davis, J.G., C.C. Truman, S.C. Kim, J.C. Ascough, and K. Carlson. 2006. Antibiotic transport via runoff and soil loss. Journal of Environmental Quality, 35:2250-2260. https://doi.org/10.2134/jeq2005.0348
  9. Diaz-Cruz, M.S., M.J.L. Alda, and D. Barcelo. 2003. Environmental behavior and analysis of veterinary and human drugs in soils, sediment and sludge. TRAC Trends in Analytical Chemistry, 22:340-351. https://doi.org/10.1016/S0165-9936(03)00603-4
  10. Gobel, A., C.S. McArdell, M.J.F. Suter, and W. Giger. 2004. Trace determination of macrolide and sulfonamide antimicrobials, a human sulfonamide metabolite, and trimethoprim in wastewater using liquid chromatography coupled to electrospray tandem mass spectrometry. Analytical Chemistry, 76:4756-4764. https://doi.org/10.1021/ac0496603
  11. Haller, M.Y., S.R. Muller, C.S. McArdell, A.C. Alder, and M.J.-F. Suter. 2002. Quantification of veterinary antibiotics (sulfonamides and trimethoprim) in animal manure by liquid chromatography-mass spectrometry. Journal of Chromatography A, 952:111 - 120. https://doi.org/10.1016/S0021-9673(02)00083-3
  12. Hamscher, G., S. Sczesny, H. Hoper, and H. Nau. 2002. Determination of persistent tetracycline residues in soil fertilized with liquid manure by high performance liquid chromatography with electrospray ionization tandem mass spectrometry. Analytical Chemistry, 74:1509-1518. https://doi.org/10.1021/ac015588m
  13. Heberer, T. 2002. Occurrence, fate, and removal of pharmaceutical residues in the aquatic environment: a review of recent research data. Toxicology Letters, 131:5-17. https://doi.org/10.1016/S0378-4274(02)00041-3
  14. Hirsch, R., T. Ternes, K. Hanerer, and Kratz, K.L. 1999. Occurrence of antibiotics in the aquatic environment. Science of the Total Environment, 225:109-118. https://doi.org/10.1016/S0048-9697(98)00337-4
  15. Jacobsen, A.M., B. Halling-Sorensen, F. Ingerslev, and S.H. Gansen. 2004. Simultaneous extraction of tetracycline, macrolide and sulfonamide antibiotics from agricultural soils using pressurised liquid extraction, followed by solid-phase extraction and liquid chromatography-tandem mass spectrometry. Journal of Chromatography A, 1038:157-170. https://doi.org/10.1016/j.chroma.2004.03.034
  16. Kay, P., P.A. Blackwell, and A.B.A. Boxall. 2004. Fate of veterinary antibiotics in a macroporous tile drained clay soils. Environmental Toxicology and Chemistry, 23:1136-1144. https://doi.org/10.1897/03-374
  17. Kay, P., P.A. Blackwell, and Boxall, A.B.A. 2005a. A lysimeter experiment to investigate the leaching of veterinary antibiotics through a clay soil and comparison with field data. Environmental Pollution, 134:333-341. https://doi.org/10.1016/j.envpol.2004.07.021
  18. Kay, P., P.A. Blackwell, and A.B.A. Boxall. 2005b. Transport of veterinary antibiotics in overland flow following the application of slurry to arable land. Chemosphere, 59:951-959. https://doi.org/10.1016/j.chemosphere.2004.11.055
  19. Kim, S.C. and K. Carlson. 2007. Quantification of human and veterinary antibiotics in water and sediment using SPE/LC/MS/MS. Analytical and Bioanalytical Chemistry, 387:1301-1315. https://doi.org/10.1007/s00216-006-0613-0
  20. Kim, S.C. and K.H. Carlson. 2006. Occurrence of ionophore antibiotics in water and sediments of a mixed-landscape watershed. Water Research, 40:2549-2560. https://doi.org/10.1016/j.watres.2006.04.036
  21. Kim, Y.H., T.M. Heinze, S.J. Kim, and C.E. Cerniglia. 2004. Adsorption and clay-catalyzed degradation of erythromycin A on homoionic clays. Journal of Environmental Quality, 33:257-264. https://doi.org/10.2134/jeq2004.2570
  22. Kolpin, D.W., E.T. Furlong, M.T. Meyer, E.M. Thurman, S.D., Zaugg, L.B. Barber, and H.T. Buxton. 2002. Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999-2000: A National Reconnaissance. Environmental Science and Technology, 36:1202 - 1211. https://doi.org/10.1021/es011055j
  23. Lidberg, R.H., K. Bjorklund, R. Rendahl, M.I. Johansson, M. Tysklind, and B.A.V. Andersson. 2007. Environmental risk assessment of antibiotics in the Swedish environment with emphasis on sewage treatment plants. Water Research, 41:613-619. https://doi.org/10.1016/j.watres.2006.11.014
  24. Liguoro, M.D., V. Cibin, F. Capolongo, B. Halling-sorensen, and C. Montesissa. 2003. Use of oxytetracycline and tylosin in intensive calf farming: evaluation of transfer to manure and soil. Chemosphere, 52:203-212. https://doi.org/10.1016/S0045-6535(03)00284-4
  25. Lindsey, M.E., M. Meyer, and E.M. Thurman. 2001. Analysis of trace levels of sulfonamides and tetracycline antimicrobials in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometry. Analytical Chemistry, 73:4640-4646. https://doi.org/10.1021/ac010514w
  26. McArdell, C.S., E. Molnar, M.J.F. Suter, and W. Giger. 2003. Occurrence and fate of macrolide antibiotics in wastewater treatment plants and in the glatt valley watershed, Switzerland. Environmental Science and Technology, 37:5479-5486. https://doi.org/10.1021/es034368i
  27. Mellon, M., C. Benbrook, and K.L. Benbrook. 2001. Hogging it: Estimation of antimicrobial abuse in livestock. Union of Concerned Scientists.
  28. Pedersen, J.A., M. Soliman, and I.H. Suffet. 2005. Human pharmaceuticals, hormons, and personal care product ingredients in runoff from agricultural fields irrigated with treated wastewater. Journal of Agricultural and Food Chemistry, 53:1625-1632. https://doi.org/10.1021/jf049228m
  29. Pei, R., S.C. Kim, K.H. Carlson, and A. Pruden. 2006. Effect of river landscape on the sediment concentration of antibiotics and corresponding antibiotic resistance genes (ARG). Water Research, 40:2427-2435. https://doi.org/10.1016/j.watres.2006.04.017
  30. Richardson, M.L. and J.M. Bowron. 1985. The fate of pharmaceutical chemicals in the aquatic environment. Journal of Pharmacy and Pharmacology, 37:1 - 12. https://doi.org/10.1111/j.2042-7158.1985.tb04922.x
  31. Rooklidge, S.J. 2004. Environmental antimicrobial contamination from terraccumulation and diffuse pollution pathways. Science of the Total Environment, 325:1-13. https://doi.org/10.1016/j.scitotenv.2003.11.007
  32. Schlusener, M.P., K. Bester, and M. Spiteller. 2003. Determination of antibiotics such as macrolide, ionophores and tiamulin in liquid manure by HPLC-MS/MS. Analytical and Bioanalytical Chemistry, 375:942-947. https://doi.org/10.1007/s00216-003-1838-9
  33. Sengelov, G., Y. Agerso, B. Halling-Sorensen, S.B. Baloda, J.S. Anderson, and L.B. Jensen. 2003. Bacterial antibiotic resistance levels in Danish farmland as a result of treatment with pig manure slurry. Environment International, 28:587-595. https://doi.org/10.1016/S0160-4120(02)00084-3
  34. Storteboom, H.N., S.-C. Kim, K.C. Doesken, K.H. Carlson, J.G. Davis, and A. Pruden. 2007. Response of antibiotics and resistance genes to high-intensity and low-intensity manure management. Journal of Environmental Quality, 36:1695-1703. https://doi.org/10.2134/jeq2007.0006
  35. Thiele-Bruhn, S. 2003. Pharmaceutical antibiotic compounds in soil - a review. Journal of Plant Nutrition and Soil Science, 166:145-167. https://doi.org/10.1002/jpln.200390023
  36. Tolls, J. 2001. Sorption of veterinary pharmaceuticals in soils: A review. Environmental Science and Technology, 35:3397-3406. https://doi.org/10.1021/es0003021
  37. USDA. 2003. Qualitative Identification of Tetracyclines in Tissues. United States Department of Agriculture Food Safety and Inspection Service.
  38. Zhu, J., D.D. Snow, D.A. Cassada, S.J. Monson, and Spalding, R.F. 2001. Analysis of oxytetracycline, tetracycline, and chlorotetracycline in water using solid-phase extraction and liquid chromatography tandem mass spectrometry. Journal of Chromatography A, 928:177 - 186. https://doi.org/10.1016/S0021-9673(01)01139-6

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