Analysis and Distribution of Polycyclic Aromatic Hydrocarbons and Chlorophenols in Sewage and Industrial Wastewater Sludge in Korea

국내 하.폐수슬러지 중 다환방향족탄화수소 및 염화페놀류의 분포 특성

  • Ju, Joon-Hyung (Department of Environment Engineering, Pusan National University) ;
  • Kim, Min-Young (Department of Environment Engineering, Pusan National University) ;
  • Lee, Sung-Hee (Department of Environment Engineering, Pusan National University) ;
  • Oh, Jeong-Eun (Department of Environment Engineering, Pusan National University)
  • Published : 2008.07.31

Abstract

In order to evaluate the levels and distribution patterns, the concentrations of PAHs and chlorophenols were investigated in sludge samples discharged from 6 WWTPs located along Nak-dong river and 7 STPs in Busan, Korea. Levels of 16 PAHs and 19 chlorophenols in sludge samples ranged from 1.28 to 44.9 mg/kg dry wt. and from 213 to 3,850 $\mu$g/kg dry wt., respectively. Levels of PAHs in sludge samples except I5 and S4 were detected lower than those of previous studies. The distribution patterns of PAHs and chlorophenols varied with industrial wastewater sludge samples because industrial wastewater sludge had different industrial input sources. However, the distribution patterns of PAHs and chlorophenols in sewage sludge were pretty similar. Phenanthrene, fluoranthene and pyrene were dominant and the fractions of these 3 PAHs relative to 16 PAHs in sewage sludge ranged from 30.8 to 50.7%. 2-chlorophenol is dominated in most sewage sludge samples and the fraction ranged from 36.0 to 66.8%.

낙동강 유역에 위치한 산업폐수종말처리장에서 채집한 폐수슬러지 시료와 부산 지역 하수처리장에서 채집된 하수슬러지시료를 대상으로 19종의 염화페놀류와 미국 환경보호청(US EPA)에서 우선 오염물질로 지정한 16종의 PAHs를 분석하여 농도 실태 및 분포 특성을 확인하고자 하였다. 분석결과 PAHs는 1.28$\sim$44.9 mg/kg dry wt.의 범위를 보였으며 대부분의 슬러지 시료에서 선행연구와 비슷하거나 낮은 농도를 보였지만 I5와 S4 시료의 경우 매우 높은 농도로 검출되어 슬러지의 종류 및 폐수 발생원에 따라 차이를 보이는 것을 알 수 있었다. 염화페놀류는 213$\sim$3,850 $\mu$g/kg dry wt.로 검출되었으며, 폐수슬러지에서 더 높은 농도로 나타났다. 특히 공단처리수가 하수와 같이 유입되는 하수슬러지 시료의 경우 폐수슬러지와 비슷한 농도수준을 보여 하수보다는 폐수에 의해 이들 물질의 농도가 영향을 받는 것을 알 수 있었다. 또한 슬러지의 종류에 따른 PAHs와 염화페놀류의 분포패턴을 파악하기 위해 주성분분석 및 군집분석을 실시하였다. 폐수슬러지의 경우 폐수가 배출되는 산업의 종류에 따라 서로 다른 분포패턴을 보였지만 하수슬러지는 비교적 유사한 분포패턴을 보였다. 식품산업이 대부분을 차지하는 I6 폐수슬러지 시료의 경우 하수슬러지와 유사한 분포패턴을 보여 폐수 발생원에 의한 영향을 많이 받는 것을 알 수 있었다. 하수슬러지에서 PAHs는 선행연구와 마찬가지로 phenanthrene, pyrene, fluoranthene이 상대적으로 높은 조성비(30.8$\sim$50.7%)를 보였으며, 염화페놀류는 2-chlorophenol이 36.0$\sim$66.8%의 높은 비율로 나타났다.

Keywords

References

  1. Harrison, E. Z., Oakes, S. R., Hysell, M., Hay, A., 'Organic chemicals in sewage sludges,' Sci. Total Environ., 367(2-3), 481-497(2006) https://doi.org/10.1016/j.scitotenv.2006.04.002
  2. 환경부, '환경통계연감'(2006)
  3. 환경부, '전국 폐기물 발생 및 처리 현황'(2005)
  4. Abad, E., Martinez, K., Planas, C., Palacios, O., Caixach, J., Rivera, J., 'Priority organic pollutant assessment of sludges for agricultural purposes,' Chemosphere, 61(9), 1358-1369(2005) https://doi.org/10.1016/j.chemosphere.2005.03.018
  5. Bright, D. A., Healey, N., 'Contaminant risks from biosolids land application: Contemporary organic contaminant levels in digested sewage sludge from five treatment plants in Greater Vancouver, British Columbia,' Environ. Pollut., 126(1), 39-49(2003) https://doi.org/10.1016/S0269-7491(03)00148-9
  6. Klopffer, W., 'Environmental hazard assessment of chemicals and products. Part V. Anthropogenic chemicals in sewage sludge,' Chemosphere, 33(6), 1067-1081(1996) https://doi.org/10.1016/0045-6535(96)00247-0
  7. Pereira, M. S., Kuch, B., 'Heavy metals, PCDD/F and PCB in sewage sludge samples from two wastewater treatment facilities in Rio de Janeiro State, Brazil,' Chemosphere, 60(7), 844-853(2005) https://doi.org/10.1016/j.chemosphere.2005.01.079
  8. Dudzinska, M. R., Czerwinski, J., Staszowska, A., 'Timerelated trends in PCDD/F levels in sewage sludge in southeastern Poland,' Organohalogen Compd., 68, 1047-1050 (2006)
  9. Eljarrat, E., Caixach, J., Rivera, J., 'Evaluation of dioxin contamination in sewage sludge discharges on coastal sediments from Catalonia, Spain,' Water Res., 35(11), 2799-2803(2001) https://doi.org/10.1016/S0043-1354(00)00566-2
  10. Fuentes, M. J., Font, R., Gomez-Rico, M. F., Molto, J., 'Multivariant statistical analysis of PCDD/FS in sewage sludges from different areas of the Valencian Community (Spain),' Chemosphere, 67(7), 1423-1433(2007) https://doi.org/10.1016/j.chemosphere.2006.10.005
  11. Martinez, K., Abad, E., Adrados, M. A., Saulo, J., Palacios, O., Austrui, J. R., Caixach, J., Rivera, J., 'PCDD/F assessment in waste water trearment plant sludges and related matrices,' Organohalogen Compd., 68, 1087-1090 (2006)
  12. Rivera, J., Eljarrat, E., Espadaler, I., Martrat, M. G., Caixach, J., 'Determination of PCDF/PCDD in sludges from a drinking water treatment plant influence of chlorination treatment,' Chemosphere, 34(5-7), 989-997(1997) https://doi.org/10.1016/S0045-6535(97)00401-3
  13. Sanz, P., Concejero, M. A., Martinez, M. A., Navarro, I., Torre, A., 'Determination of PCDD/F levels in spanish sewage sludge for being applied as raw in composting and agriculture,' Organohalogen Compd., 68, 1099-1102 (2006)
  14. Eljarrat, E., Caixach, J., Rivera, J., 'A comparison of TEQ contributions from PCDDs, PCDFs and dioxin-like PCBs in sewage sludges from Catalonia, Spain,' Chemosphere, 51(7), 595-601(2003) https://doi.org/10.1016/S0045-6535(02)00785-3
  15. Stevens, J., Green, N. J. L., Jones, K. C., 'Survey of PCDD/Fs and non-ortho PCBs in UK sewage sludges,' Chemosphere, 44(6), 1455-1462(2001) https://doi.org/10.1016/S0045-6535(00)00474-4
  16. Stevens, J. L., Northcott, G. L., Stern, G. A., Tomy, G. T., Jones K. C., 'PAHs, PCBs, PCNs, organochlorine pesticides, synthetic musks, and polychlorinated n-alkanes in U.K. sewage sludge: survey results and implications,' Environ. Sci. Technol., 37(3), 462-467(2003) https://doi.org/10.1021/es020161y
  17. Oleszczuk P., 'Persistence of polycyclic aromatic hydrocarbons( PAHs) in sewage sludge-amended soil,' Chemosphere, 65(9), 1616-1626(2006) https://doi.org/10.1016/j.chemosphere.2006.03.007
  18. 김종훈., '하수슬러지와 토양 중 다핵방향족 탄화수소의 정량,' 분석과학, 13(3), 357-367(2000)
  19. 남재작, 소규호, 박우균, 조남준, 이상학, '가스크로마토그래피-이온트랩질량분석법을 이용한 하수슬러지 중 다핵방향족탄화수소(PAHs) 함량 분석,' 한국환경과학회지, 11(4), 367-373(2002)
  20. 이강영, 정창수, 김영일, 이현경, 홍기훈, '우리나라 하수 및 폐수 처리 슬러지의 다환방향족탄화수소의 함량,' 한국환경과학회지, 14(4), 413-425(2005) https://doi.org/10.5322/JES.2005.14.4.413
  21. EU, 'Working Document on Sludge 3rd Draft,' Unpublished, p19
  22. U.S. Environmental Protection Agency Home Page, http://www.epa.gov/waterscience/methods/pollutants.htm, June(2008)
  23. 한국과학기술정보연구원, '비산재로부터 다이옥신의 제거기술'(2004)
  24. Lewis, R. J., 'Hawley's Condensed Chemical Dictionary,' 12th ed. New York, Van Nostrand Rheinhold Co., p. 270(1993)
  25. Helmuth J., 'Chlorophenols and nonylphenols in sewage sludges. Part 2. Did contents of pentachlorophenol and nonylphenols reduce?,' Acta Hydroch. Hydrob., 26(6), 344-348(1998) https://doi.org/10.1002/(SICI)1521-401X(199811)26:6<344::AID-AHEH344>3.0.CO;2-9
  26. Wild, S. R., Harrad, S. J., Jones, K. C., 'Chlorophenols in digested U.K. sewage sludges,' Inst. Environ. Biol. Sci., Water Res., 27(10), 1527-1534(1993)
  27. Lega, R., Ladwig, G., Meresz, O., Clement, R. E., Crawford, G., Salemi, R., Jones, Y., 'Quantiotative determination of organic priority pollutants in sewage sludge by GC/MS,' Chemosphere, 34(8) 1705-1712(1997) https://doi.org/10.1016/S0045-6535(97)00027-1