Occurrence and Distribution of Selected Veterinary Antibiotics in Soils, Sediments and Water Adjacent to a Cattle Manure Composting Facility in Korea

국내 우분 퇴비화 시설 인근 농경지 및 수계 중 Tetracycline 및 Sulfonamide 계열 항생물질의 분포특성

  • Lim, Jung-Eun (Department of Biological Environment, Kangwon National University) ;
  • Kim, Sung-Chul (Department of Biological Environment, Kangwon National University) ;
  • Lee, Hyeon-Yong (Department of Biological Environment, Kangwon National University) ;
  • Kwon, Oh-Kyung (Hazardous Substances Division, National Academy of Agricultural Science) ;
  • Yang, Jae-E. (Department of Biological Environment, Kangwon National University) ;
  • Ok, Yong-Sik (Department of Biological Environment, Kangwon National University)
  • 임정은 (강원대학교 자원생물환경학과) ;
  • 김성철 (강원대학교 자원생물환경학과) ;
  • 이현용 (강원대학교 자원생물환경학과) ;
  • 권오경 (국립농업과학원 유해물질과) ;
  • 양재의 (강원대학교 자원생물환경학과) ;
  • 옥용식 (강원대학교 자원생물환경학과)
  • Received : 2009.07.29
  • Accepted : 2009.08.28
  • Published : 2009.10.31

Abstract

There has been increased concern regarding the release of antibiotics to different environmental compartments due to the possibility of the development of antibiotic resistant bacteria. However, limited information is available regarding the occurrence, fate, and transport of antibiotics in Korea in both the aqueous phase and in solid phases such as sediment and soil. Therefore, this study was conducted to monitor the concentration of released antibiotics in surface water, sediment, and soil adjacent to a cattle manure composting facility in Korea. Specifically, the following six antibiotics were monitored: tetracycline (TC), chlortetracycline (CTC), oxytetracycline (OTC), sulfamethazine (SMT), sulfamethoxazole (SMX), and sulfathiazole (STZ). To extract and quantify the antibiotics from different environmental compartments, solid phase extraction (SPE) and high performance liquid chromatography mass spectrometry (HPLC/MS) techniques were adopted. The concentration of the six antibiotics ranged from below the detection limit (BDL) to 0.71 ${\mu}g$/L in surface water, from BDL to 27.61 ${\mu}g$/L in sediment, and from 0.12 to 157.33 ${\mu}g$/L in soil. In addition, higher concentrations of antibiotics were observed in surface water and sediment at locations closer to the composting facility indicating that composting is the source of the antibiotics found in the environment. Furthermore, higher concentrations of antibiotics were observed in the solid phase (sediment and soil) than the aqueous phase. These findings indicate that the possibility of antibiotic resistant bacteria is increased because such bacteria are more stable in the solid phase. Overall, longterm monitoring of the aqueous phase and solid phase is necessary to gain a better understanding of the impact of antibiotics from source on the environment in Korea.

최근 전 세계적으로 환경 중에 잔류하는 항생물질로 인한 항생물질 내성박테리아의 발현에 대한 우려가 커지고 있다. 그러나 국내의 경우 이에 대한 기초자료 확립을 위한 액상(수질)과 고상(토양, 저질토)에 잔류하는 항생물질의 동태와 이동에 대한 연구는 극히 드문 실정이다. 이에 본 연구에서는 국내 우분 퇴비화 시설에 인접한 농경지 토양과 지표수 및 저질토에 대한 항생물질 모니터링을 실시하여 tetracycline 계열의 항생물질 3종(tetracycline, chlortetracycline, oxytetracycline)과 sulfonamide 계열의 항생물질 3종(sulfamethazine, sulfamethoxazole, sulfathiazole)에 대한 분포특성을 살펴보았다. 항생물질은 고형상추출(SPE, solid phase extraction)을 실시한 후 고성능액체크로마토그래피 질량분석기(HPLC/MS)로 분석하였다. 이를 통해 검출된 환경 중 항생물질의 농도는 지표수에서 BDL ~0.71 ${\mu}g$/L, 저질토에서 BDL ~27.61 ${\mu}g$/L, 농경지 토양에서 0.12~157.33 ${\mu}g$/L 수준으로 나타났으며 퇴비화 시설과 인접한 지점의 시료에서 상대적으로 높은 수준의 항생물질이 검출되었다. 이를 통해 퇴비화 시설이 환경 중에 존재하는 항생물질에 영향을 주고 있음을 알 수 있었다. 한편 수질시료에 비해 저질토와 토양에서 항생물질이 높은 농도로 검출되었으며 이는 항생물질의 물리화학적 특성에 기인하는 것으로 판단되었다. 장기적으로는 저질토와 토양에서 항생물질 내성박테리아 발현이 우려되므로 향후 항생물질의 환경 중 이동 및 잔류특성 평가를 위한 장기 모니터링 연구가 필요할 것으로 판단된다.

Keywords

References

  1. Liu, F., Ying, G. G., Tao, R., Zhao, J. L., Yang, J. F., and Zhao, L. F., 'Effects of six selected antibiotics on plant growth and soil microbial and enzymatic activities,' Environ. Pollut., 157(5), 1636-1642(2009) https://doi.org/10.1016/j.envpol.2008.12.021
  2. 최동미, 정지윤, 장문익, 임무혁, 박건상, 홍무기, '식품 중 테트라싸이클린계 항생물질의 분석,' 분석과학, 18(3), 250-256(2005)
  3. Hamscher, G., Sczesny, S., H per, H., and Nau, H., 'Determination of persistent tetracycline residues in soil fertilized with liquid manure by high-performance liquid chromatography with electrospray ionization tandem mass spectrometry,' Analytical Chmistry, 74(7), 1509-1518(2002) https://doi.org/10.1021/ac015588m
  4. K$\ddot{u}$mmerer, K., Antibiotics in the Environment, Pharmaceuticals in the environment. Sources, fate, effects and risks, 3rd ed., K$\ddot{u}$mmerer, K.(Ed), Springer-Verlag Berlin Heidelberg, pp. 75-93(2008)
  5. Seo, Y. H., Choi, J. K., Kim, S. K., Min, H. K., and Jung, Y. S., 'Prioritizing environmental risks of veterinary antibiotics based on the use and the potential to reach environment,' Korean J. Soil Sci. Fertilizer, 40(1), 43-50(2007)
  6. Kim, S. C., and Carlson, K., 'LC-MS2 for quantifying trace amounts of pharmaceutical compounds in soil and sediment matrices,' Trends Anal. Chem., 24(7), 635-644(2005) https://doi.org/10.1016/j.trac.2005.04.006
  7. 하준일, 홍기성, 송시욱, 정석찬, 민영식, 신형철, 이기옥, 임경종, 박종명, '축산 및 수산분야의 항생물질 사용실태 조사,' 한국수의공중보건학회지, 27(4), 205-217(2003)
  8. 식품의약품안전청, 축산용 항생제 관리시스템 구축, 국가항생물질내성안전관리사업 연구보고서(2005)
  9. DANMAP 2007, 'Use of antimicrobial agents and occurrence of antimicrobial resistance in bacteria from food animals, foods and humans in Denmark,' Copenhagen, Denmark(2008)
  10. Veterinary Medicines Directorate (VMD), 'Sales of antimicrobial products authorised for use as veterinary medicines, antiprotozoals, antifungals, growth promoters and coccidiostats, in the UK in 2007,' Woodham Lane, New Haw, UK(2008)
  11. Karci, A., and Balcioglu, I. A., 'Investigation of the tetracycline, sulfonamide, and fluoroquinolone antimicrobial compounds in animal manure and agricultural soils in Turkey,' Sci. Total Environ., 407(16), 4652-4664(2009) https://doi.org/10.1016/j.scitotenv.2009.04.047
  12. Pei, R., Kim, S. C., Carlson, K. H., and Pruden, A., 'Effect of river landscape on the sediment concentrations of antibiotics and corresponding antibiotic resistance genes (ARG),' Water Res., 40(12), 2427-2435(2006) https://doi.org/10.1016/j.watres.2006.04.017
  13. Kim, Y., Jung, J., Kim, M., Park, J., Boxall, A. B. A., and Choi, K., 'Prioritizing veterinary pharmaceuticals for aquatic environment in Korea,' Environ. Toxicol. Pharmacolo., 26(2), 167-176(2008) https://doi.org/10.1016/j.etap.2008.03.006
  14. Boxall, A. B. A., Kolpin, D. W., Halling-S rensen, B., and Tolls, J., 'Are veterinary medicines causing environmental risks?,' Enviorn. Sci. Technol., 37(15), 286A-294A(2003) https://doi.org/10.1021/es032519b
  15. Martinez-Carballo, E., Gonzalez-Barreiro, C., Scharf, S., and Gans, O., 'Environmental monitoring study of selected veterinary antibiotics in animal manure and soils Austria,' Environ. Pollut., 148(2), 570-579(2007) https://doi.org/10.1016/j.envpol.2006.11.035
  16. Pailler, J. Y., Krein, A., Pfister, L., Hoffmann, L., and Guignard, C., 'Solid phase extraction coupled to liquid chromatographytandem mass spectrometry analysis of sulfonamides, tetracyclines, analgesics and hormones in surface water and wastewater in Luxembourg,' Sci. Total Environ., 407(16), 4736-4743(2009) https://doi.org/10.1016/j.scitotenv.2009.04.042
  17. Choi, K., Kim, Y., Park, J., Park, C. K., Kim, M., Kim, H. S., and Kim, P., 'Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River, Korea,' Sci. Total Environ., 405(1-3), 120-128(2008) https://doi.org/10.1016/j.scitotenv.2008.06.038
  18. Christian, T., Schneider, R. J., F rber, H. A., Skutlarek, D., Meyer, M. T., and Goldbach, H. E., 'Determination of antibiotic residues in manure, soil, and surface waters,' Acta hydrochim. hydrobiol., 31(1), 36-44(2003) https://doi.org/10.1002/aheh.200390014
  19. Kolpin, D. W., Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B., and Buxton, H. T., 'Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999-2000: a national reconnaissance,' Environ. Sci. Technol., 36(6), 1202-1211(2002) https://doi.org/10.1021/es011055j
  20. 옥용식, 작물재배환경에서 중금속 및 항생물질의 안정성 평가, 농업과학기술개발공동연구사업 연차보고서, 농촌진흥청(2008)
  21. Awad, Y. M., Kim, S. C., Lim, J. E., Lee, H. Y., Kim, T. S., Yang, J. E., and Ok, Y. S., Novel approaches for monitoring and remediation of human and veterinary antibiotics in soil and water: a critical review, The 5th International Joint Symposium between Japan and Korea: The Recent Status and Perspectives of Food System, Agricultural Environment and Biology in 2008, Chungnam National University, Daejeon, pp. 134-147(2008)
  22. Okuda, T., Kobayashi, Y., Nagao, R., Yamashita, N., Tanaka, H., Tanaka, S., Fujii, S., Konishi, C., and Houwa, I., 'Removal efficiency of 66 pharmaceuticals during wastewater treatment process in Japan,' Water Sci. Technol., 57(1), 65-71(2008) https://doi.org/10.2166/wst.2008.822
  23. Watkinson, A. J., Murby, E. J., and Costanzo, S. D., 'Removal of antibiotics in conventional and advanced wastewater treatment: Implications for environmental discharge and wastewater recycling,' Water Res., 41(18), 4164-4176(2007) https://doi.org/10.1016/j.watres.2007.04.005
  24. 이현용, 임정은, 권오경, 김성철, 서영호, 양재의, 옥용식, '토양 및 수질 중 항생제 처리기술에 관한 최근 연구동향,' 농생명과학연구, 20, 45-54(2009)
  25. 김성철, 이현용, 임정은, 김종진, 김동국, 용석호, 권오경, 양재의, 옥용식, '돈분 퇴비의 부숙화 정도에 따른 잔류항생제의 저감효율 평가,' 2008 대한환경공학회 추계학술연구발표회 논문요약집, 대한환경공학회, 서울, pp. 169(2008)
  26. 손희종, 정종문, 노재순, 유평종, 'GAC 공정에서의 Sulfonamide계 항생물질 흡착특성,' 대한환경공학회지, 30(4), 401-408(2008)
  27. 손희종, 정종문, 황영도, 노재순, 유평종, '활성탄 재질 및 사용연수에 따른 Tetracycline계 항생물질 흡착특성,' 대한환경공학회지, 30(9), 925-932(2008)
  28. 김 균, 김정한, 이성규, 김용화, '농약의 물리화학적 특성연구 (I) Captafol의 수용성, 가수분해, 증기압, 옥탄올/물 분배계수,' 한국농화학회지, 40(1), 71-75(1997)
  29. Kim, S. C., and Carlson, K., 'Temporal and spatial treands in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices,' Environ. Sci. Technol., 41(1), 50-57(2007) https://doi.org/10.1021/es060737+
  30. Tolls, J., 'Sorption of veterinary pharmaceuticals in soils: a review,' Environ. Sci. Technol., 35(17), 3397-3406(2001) https://doi.org/10.1021/es0003021
  31. 한국환경정책평가연구원(KEI), 의약물질의 환경위해성 평가체계 구축 방안. 연구보고서(2006)
  32. Loftsson, T., and Hreinsdottir, D., 'Determination of aqueous solubility by heating and equilibration: a technical note,' AAPS PharmSciTech, 7(1), E1-E4(2006) https://doi.org/10.1208/pt070101
  33. Kim, S. C., and Carlson, K., 'Quantification of human and veterinary antibiotics in water and sediment using SPE/LC/MS/MS,' Anal. Bioanal. Chem., 387(4), 1301-1315(2007) https://doi.org/10.1007/s00216-006-0613-0
  34. 농업과학기술원, 토양 및 식물체 분석법(2000)
  35. 환경부, 수질오염공정시험방법(2007)
  36. Hirsch, R., Ternes, T., Haberer, K., and Kratz, K. -L., 'Occurrence of antibiotics in the aquatic environment,' Sci. Total Envion., 225(1-2), 109-118(1999) https://doi.org/10.1016/S0048-9697(98)00337-4
  37. Watkinson, A. J., Murby, E. J., Kolpin, D. W., and Costanzo, S. D., 'The occurrence of antibiotics in an urban watershed: From wastewater to drinking water,' Sci. Total Envion., 407(8), 2711-2723(2009) https://doi.org/10.1016/j.scitotenv.2008.11.059
  38. Calamari, D., Zuccato, E., Castiglioni, S., Bagnati, R., and Fanelli, R., 'Strategic survey of therapeutic drugs in the Rivers Po and Lambro in northern Italy,' Environ. Sci. Technol., 37(7), 1241-1248(2003) https://doi.org/10.1021/es020158e
  39. Kim, S. D., Cho, J., Kim, I. S., Vanderford, B. J., and Snyder, S. A., 'Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters,' Water Res., 41(5), 1013-1021(2007) https://doi.org/10.1016/j.watres.2006.06.034
  40. Managaki, S., Murata, A., Takada, H., Tuyen, B. C., and Chiem, N. H., 'Distribution of macrolides, sulfonamides, and trimethoprim in tropical waters: ubiquitous occurrence of veterinary antibiotics in the Mekong Delta,' Environ. Sci. Technol., 41(23), 8004-8010(2007) https://doi.org/10.1021/es0709021
  41. Kim, S. C., Occurrence, fate, and transport of human and veterinary antibiotics in the watershed, Ph.D thesis, Colorado State University, Fort Collins, Colorado, USA(2006)
  42. Diaz-Cruz, M. S., and Barcelo, D., 'Determination of antimicrobial residues and metabolites in the aquatic environment by liquid chromatography tandem mass spectrometry,' Anal. Bioanal. Chem., 386(4), 973-985(2006) https://doi.org/10.1007/s00216-006-0444-z