DOI QR코드

DOI QR Code

Polycyclic Aromatic Hydrocarbons in Industrial Organic Sludge from Wastewater Treatment Facilities in Korea

폐수처리시설에서 발생된 유기성 슬러지에 함유된 다환방향족탄화수소의 농도 특성

  • Nam, Seong-Nam (Resource Recirculation Research Division, National Institute of Environmental Research) ;
  • Lee, Mi-Young (Resource Recirculation Research Division, National Institute of Environmental Research) ;
  • Yeon, Jinmo (Resource Recirculation Research Division, National Institute of Environmental Research) ;
  • Jeon, Taewan (Resource Recirculation Research Division, National Institute of Environmental Research) ;
  • Shin, Sun Kyoung (Resource Recirculation Research Division, National Institute of Environmental Research)
  • 남성남 (국립환경과학원 자원순환연구과) ;
  • 이미영 (국립환경과학원 자원순환연구과) ;
  • 연진모 (국립환경과학원 자원순환연구과) ;
  • 전태완 (국립환경과학원 자원순환연구과) ;
  • 신선경 (국립환경과학원 자원순환연구과)
  • Received : 2012.07.13
  • Accepted : 2012.08.29
  • Published : 2012.08.30

Abstract

This study presents the concentrations of the polycyclic aromatic hydrocarbons (PAHs) listed as priority pollutants by United States Environmental Protection Agency (US EPA), in 98 sludges from 54 industrial wastewater treatment facilities of South Korea. The mean concentrations of ${\Sigma}_{16}PAHs$ were ranged from 32.5 ${\mu}g/kg-dw$ to 1189.3 ${\mu}g/kg-dw$ by industries, and the highest content was found in the petrochemical industry, followed by chemical, clothing manufacturing and dying, pulp and papermaking, secondary wastewater treatment, and food/beverage producing industries. Comparisons to the EU and Danish standards of ${\Sigma}_{16}PAHs$ in sewage sludge for land application showed only two samples (one from petrochemical, and the other from chemical industry) exceeded the limits. ANOVA test with PAH concentrations as variables revealed no statistically significant influences by industrial types and sampling time (i.e., seasonal variations). Pearson correlations between individual PAHs showed strong relationships (r>0.7) among 4-ring PAHs. Concentrations of acenaphthylene, anthracene, fluoranthene, benzo(a)anthracene, benzo(f)fluoranthene, benzo(k)fluoranthene, benzo(a)pyrene presented strong correlations to ${\Sigma}_{16}PAHs$. Principal component analysis discriminated entire samples into three groups by two principal components (PC1 and PC2) with 70% of data variations, in which industrial types were not of importance, but a dominance of certain PAHs. Samples in group-I, which is high PC1 and low PC2, were characterized by a dominance of 2-ring PAHs, and in group-II, PC1 and PC2 showed a linear relation, was dominant 4-ring PAHs. Group-III with low PC1 and high PC2 includes 17 samples showing a noticeably high contribution of 3-ring PAHs to ${\Sigma}_{16}PAHs$. This study provides concentrations of PAHs in industrial sludges collected from a wide variety of sources (six industrial types) and two seasons of sampling events, and the comparison of ${\Sigma}_{16}PAHs$ with other studies are also discussed.

이 연구에서는 우리나라에서 유기성 슬러지의 배출량이 많은 6개 주요 산업 업종의 54개 사업장에서 채취한 98개 폐수처리 슬러지에 대하여 PAHs 함량을 조사하였다. 슬러지에 대한 해양배출허용기준과 비교시 C업종의 슬러지는 Nap에 대하여 제1기준과 제2기준을 모두 초과하는 시료가 1건, PC업종의 슬러지에서 Ant와 Fla에 대하여 제2기준을 초과하는 시료가 1건 있었다. ${\Sigma}_{16}PAHs$는 PC> C > CD> PP >WS > FB업종의 순으로 높았다. 슬러지의 육상 이용시 ${\Sigma}_{16}PAHs$ 함량농도를 규제하는 EU와 덴마크의 기준과 비교하였을 때 EU의 기준은 PC업종에서 1건, 덴마크 기준은 C업종과 PC업종에서 각 1건의 시료가 초과하였다. 7종 발암성 PAHs에 대한 ${\Sigma}_7PAHs$은 상대적으로 PC, CD, C업종에서 높게, PP, WS업종에서 낮았으며, FB업종에서는 검출되지 않았다. 슬러지에서의 PAHs의 농도에 대한 ANOVA 분석결과 발생업종과 채취시기에 의한 영향은 없는 것으로 나타났다. 개별 PAHs간 상관분석결과 4-ring 이상의 HMW PAHs 농도간에 상관성이 높았다. ${\Sigma}_{16}PAHs$와는 0.7 이상의 높은 상관성을 갖는 PAHs는 Acy, Ant, Fla, B(a)A, B(f)F, B(a)P 이었다. 주성분분석의 결과 98개의 슬러지는 전체 데이터의 약 70%의 설명력을 갖는 두 개의 주성분에 의해 세 개의 그룹으로 특성별로 분리될 수 있었다. 국내/외 선행연구와의 비교 결과 ${\Sigma}_{16}PAHs$는 스위스의 연구 결과와 비슷하였다.

Keywords

References

  1. 환경부, "2010 전국폐기물 발생 및 처리현황" (2011).
  2. European Commission, Organic Contaminants in Sewage Sludge for Agricultural Use, 2001, http://ec.europa.eu/environment/waste/sludge/pdf/organics_in_sludge.pdf (accessed June 2012).
  3. EU report on sludge management, 2010 http://ec.europa.eu/ environment/waste/sludge/pdf/part_iii_report.pdf (accessed February, 2012).
  4. United States Environmental Protection Agency (US EPA), 40 CFR Part 503, Standards for the Use and Disposal of Sewage Sludge (the Part 503 rule), (1993).
  5. 국립환경과학원, "폐수처리시설에서 발생하는 유기성 슬러지의 재활용 활성화 방안에 관한 연구(II)," (2011).
  6. Khalili, N. R., Scheff, P. A. and Holsen, T. M., "PAH source fingerprints for coke ovens, diesel and gasoline engines, highway tunnels and wood combustion emissions," Atmospheric Environ., 29(4), 533-542(1995). https://doi.org/10.1016/1352-2310(94)00275-P
  7. Joa, K., Panova, E., Irha, N., Teinemaa, E., Lintelmann, J. and Kirso, U., "Determination of polycyclic aromatic hydrocarbons (PAHs) in oil shale processing wastes: current practice and new trends," 26(1) 59-72(2009).
  8. International Society for Polycyclic Aromatic Compounds 2003, PAH sturcture/properites, http://www.ispac.org/Links.htm.
  9. Online website, Chemfate database, http://esc.syrres.com/efdb/ Chemfate.htm (accessed June 2012).
  10. TOXNET (Toxicology Data Network), http://toxnet.nlm.nih. gov/
  11. Mackay, D. and Shiu, W. Y., "Aqueous solubility of polynuclear aromatic hydrocarbons," J. Chem. Eng. Data, 22(4), 399-402(1977). https://doi.org/10.1021/je60075a012
  12. Brownawell, B. J., "The role of colloidal organic matter in the marine geochemistry of PCBs, PhD dissertation," Massachusettes Institute of Technology, 1986.
  13. Mackay, D., Shiu, W. Y. and Ma, K. C., Illustrated Handbook of Physico-Chemical Properties and Environmental Fate for Organic Chemicals, Part 3. Lewis, Chelsea, MI, USA. 1992.
  14. 국토해양부, 해양환경관리법, 2012.
  15. Council of the European Community (CEC), 2000, Working document on sludge, third draft, Brussels
  16. Madsen, T., Kristensen, P., Samso-Petersen, I., Torslov, J. and Sasmussen, J. O., Application of sludge on farmlandquality objectives, level of contamination and environmental risk assessment, Specialty conference on management and fate of toxic organics in sludge applied to land. Copenhagen, 4/30-5/2, 1997.
  17. Jolliffe, I. T., "Principal Component Analysis. 2nd Edition ed. 2002: Springer-Verlag," New York.
  18. 이강영, 정창수, 김영일, 이현경, 홍기훈, "우리나라 하수 및 폐수 처리 슬러지의 다환방향족탄화수소의 함량," 한국환경과학회지, 14(4), 413-425(2005)
  19. Ju, J.-H., Lee, I.-S., Sim, W.-J., Eun H. and Oh, J.-E., "Analysis and evaluation of chlorinated persistant organic compounds and PAHs in sludge in Korea," Chemosphere, 74, 441-447(2009) https://doi.org/10.1016/j.chemosphere.2008.09.059
  20. Abad, E., Martinez, K., Planas, C., Palacios, O., Caixach, J. and Rivera, J., "Priority organic pollutants assessment of sludges for agricultural purposes," Chemosphere, 61, 1358-1369 (2005).
  21. Berset, J. D. and Holzer, R., "Quantitative determination of polycyclic aromatic hydrocarbons, polychlornated biphenyls and organochlorine pesticides in sewage sludges using supercritical fluid extraction and mass spectrometric detection," J. Chromatography A, 852, 545-558(1999). https://doi.org/10.1016/S0021-9673(99)00641-X
  22. Blanchard, M., Teil, M. J., Ollivon, D., Legenti, L. and Chevreuil, M., "Polyaromatic hydrocarbons and polychlorobiphenyls in wastewaters and sewage sludges from the Paris area (France)," Environ. Res., 95, 184-197(1999).
  23. Stevens, J. L., Northcott, G. L., Stern, G. A., Tomy, G. T. and 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, 462-467(2003). https://doi.org/10.1021/es020161y
  24. Baran, S. and Oleszczuk, P., "The concentration of polycyclic aromatic hydrocarbons in sewage sludge in relation to the amount and origin of purified sewage," Polish J. Environ. Studies, 12, 523-529(2003).
  25. Jiries, A., Hussani, H. and Lintelmann, J., "Determination of polycyclic aromatic hydrocarbons in wastewater, sediments, sludge and plants in Karak province," Jordan, Water, Air, and Soil Pollut., 121, 217-228(2000). https://doi.org/10.1023/A:1005257207607
  26. Salihoglu, N. K., Salihoglu, G., Tasdemir, Y., Cindoruk, S. S., Yolsal, D., Ogulmus, R. and Karaca, G., "Comparison of Polycyclic Aromatic Hydrocarbons Levels in Sludges from Municipal and Industrial Wastewater Treatment Plants," Arch. Environ. Contam. Toxicol., 58(3), 523-534(2010). https://doi.org/10.1007/s00244-009-9389-5
  27. Cai, Q.-Y., Mo, C.-H., Wu, Q.-T., Zeng, Q.-Y. and Katsoyiannis, A., "Occurrence of organic contaminants in sewage sludges from eleven wastewater treatment plants, China," Chemosphere, 68, 1751-1762(2007). https://doi.org/10.1016/j.chemosphere.2007.03.041