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Determination of Freely Dissolved PAHs in Seawater around the Korean Peninsula Using High Speed Rotation-Type Passive Sampling Device

고속회전식 수동형 채집 장치를 이용한 한반도 주변해역에서의 자유용존상 PAHs 측정

  • JANG, YU LEE (Department of Ocean System Engineering, Gyeongsang National University) ;
  • LEE, HYO JIN (Marine Environmental Impact Assessment Center, National Institute of Fisheries Science) ;
  • JEONG, HAEJIN (Department of Ocean System Engineering, Gyeongsang National University) ;
  • JEONG, DA YEONG (Department of Ocean System Engineering, Gyeongsang National University) ;
  • KIM, NA YEONG (Department of Marine Environmental Engineering, Gyeongsang National University) ;
  • KIM, GI BEUM (Department of Marine Environmental Engineering, Gyeongsang National University)
  • 장유리 (경상대학교 해양시스템공학과) ;
  • 이효진 (국립수산과학원 해역이용영향평가센터) ;
  • 정해진 (경상대학교 해양시스템공학과) ;
  • 정다영 (경상대학교 해양시스템공학과) ;
  • 김나영 (경상대학교 해양환경공학과) ;
  • 김기범 (경상대학교 해양환경공학과)
  • Received : 2020.09.10
  • Accepted : 2021.01.05
  • Published : 2021.02.28

Abstract

A new high speed rotation type-passive sampling device (HSR-PSD), which can rotate seawater at high speed and absorb easily and quickly the freely dissolved hydrophobic organic contaminants from seawater, was developed and then applied around the Korean Peninsula. Freely dissolved concentrations (Cfree) of polycyclic aromatic hydrocarbons (PAHs) were determined using the HSR-PSD with low density polyethylene (LDPE) sheets as a passive sampler. Furthermore, dissolved concentrations (Cdissolved) of PAHs in seawater were also obtained from high volume water sampling as a conventional method to account for actual bioavailability. When the LDPE sheets were rotated in the HSR-PSD at 900 rpm, PAHs with log KOW 3.4 ~ 5.2 were equilibrated between the LDPE and water in 5 hours. Although the high molecular weight PAHs with log KOW 5.6 ~ 6.8 was expected to be 2 to 30 days to reach the equilibrium, the Cfree of the PAHs at equilibrium could be corrected using performance reference compounds in 5 hours. Meanwhile, the total Cfree of PAHs were from 0.32 to 1.2 ng/L, which were higher than reported values in other oceans, but lower than in coastal water such as estuary, harbor, or shore. A bioavailability from the detected PAHs was highest at the sampling line near the dumping site of the Yellow Sea. Predicted residual concentrations in biota were relatively higher in offshore including the dumping site than in coastal regions.

본 연구에서는 해수 중 생물에게 실질적으로 이용되어질 수 있는 자유용존상 농도(freely dissolved concentration)를 보다 쉽고 빠르게 검출하고자 해수를 고속으로 회전시키는 수동형 채집 장치를 제작하였다. 이 고속회전식 수동형 채집 장치(high speed rotation-type passive sampling device)를 한반도 주변해역에 적용하여 해수 중 다환방향족탄화수소(polycyclic aromatic hydrocarbons, PAHs)의 자유용존상 농도를 측정하였다. 또한 대용량 해수 채취법(high volume water sampling)으로부터 구한 PAHs의 용존상 농도(dissolved concentration)와 고속회전식 수동형 채집 장치로부터의 자유용존상 농도를 비교하여 생물에게 직접적으로 이용 될 수 있는 비율을 조사하였다. 그 결과, 고속회전식수동형 채집 장치 모터의 회전속도를 900 rpm으로 가동하였을 때, 소수성이 낮은 저분자 PAHs 화합물(log KOW 3.4 ~ 5.2)은 5시간 만에 평형에 도달하였다. 반면 소수성이 비교적 높은 고분자 화합물(log KOW 5.6 ~ 6.8)의 경우, 평형에 도달하는 데 걸리는 시간은 최소 2일에서 한 달 정도 소요될 것으로 예상되었다. 그러나 실행보정물질(performance reference compounds)를 이용할 경우, 5시간 가동만으로도 평형상태에서의 고분자 화합물의 농도 예측이 가능하였다. 수동형 채집 장치를 적용하여 측정된 조사해역에서의 PAHs의 자유용존상 농도는 0.32 ~ 1.2 ng/L으로 다른 대양에서의 농도보다는 높았지만, 항구나 해안과 같은 연안보다는 매우 낮은 수준이었다. 용존상 및 자유용존상이 모두 검출된 PAHs를 대상으로 생물에게 이용 될 수 있는 비율은 서해병 폐기물 배출해역 위치와 인접한 조사구간에서 가장 높았다. 또한 생물 체내 잔류농도를 예측하였을 때, 폐기물 배출해역이 포함된 외해가 연안보다 비교적 높은 것으로 나타났다.

Keywords

References

  1. 환경부, 2008. 황해 환경오염 특성평가 및 감시체계 개발, 522 pp.
  2. Adams, R.G., R. Lohmann, L.A. Fernandez, J.K. MacFarlane and P.M. Gschwend, 2007. Polyethylene Devices: Passive samplers for measuring dissolved hydrophobic organic compounds in aquatic environments. Environ. Sci. Technol., 41: 1317-1323. https://doi.org/10.1021/es0621593
  3. Allan, I.J., H.C. Nilsson, I. Tjensvoll, C. Bradshaw and K. Naes, 2011. Mobile passive sampler: Concept for a novel mode of exposure. Environ. Pollut., 159: 2393-2397. https://doi.org/10.1016/j.envpol.2011.06.039
  4. Allan, S.E., B.W. Smith and K.A. Anderson, 2012. Impact of the Deepwater Horizon oil spill on bioavailable polycyclic aromatic hydrocarbons in Gulf of Mexico coastal waters. Environ. Sci. Technol., 46: 2033-2039. https://doi.org/10.1021/es202942q
  5. Apell, J.N. and P.M. Gschwend, 2014. Validating the use of performance reference compounds in passive samplers to assess porewater concentrations in sediment beds. Environ. Sci. Technol., 48: 10301-10307. https://doi.org/10.1021/es502694g
  6. Apell, J.N., A.P. Tcaciuc and P.M. Gschwend, 2016. Understanding the rates of nonpolar organic chemical accumulation into passive samplers deployed in the environment: Guidance for passive sampler deployments. Integr. Environ. Assess. Manag., 12: 486-492. https://doi.org/10.1002/ieam.1697
  7. Bao, L.J., S.P. Xu, Y. Liang and E.Y. Zeng, 2012. Development of a low-density polyethylene-containing passive sampler for measuring dissolved hydrophobic organic compounds in open waters. Environ. Toxicol. Chem., 31: 1012-1018. https://doi.org/10.1002/etc.1788
  8. Booij, K. and F. Smedes, 2010. An lmproved method for estimating in situ sampling rates of nonpolar passive samplers. Environ, Sci. Technol., 44: 6789-6794. https://doi.org/10.1021/es101321v
  9. Booij, K., F. Smedes and E.M. Van Weerle, 2002. Spiking of performance reference compounds in low density polyethylene and silicone passive water samplers. Chemosphere, 46: 1157-1161. https://doi.org/10.1016/S0045-6535(01)00200-4
  10. Booij, K., R. van Bommel, H.M. van Aken, H. van Haren, G.J.A. Brummer and H. Ridderinkhof, 2014. Passive sampling of nonpolar contaminants at three deep-ocean sites. Environ. Pollut., 195: 101-108. https://doi.org/10.1016/j.envpol.2014.08.013
  11. Cai, M., M. Duan, J. Guo, M. Liu, A. Qi, Y. Lin and J. Liang, 2018. PAHs in the Northern South China Sea: Horizontal transport and downward export on the continental shelf. Mar. Chem., 202: 121-129. https://doi.org/10.1016/j.marchem.2018.03.004
  12. Choi, M., Y. Park, H.B. Moon, J. Yu and H.G. Choi, 2010. Distribution of fecal sterols, nonylphenol, and polycyclic aromatic hydrocarbons in surface water from Masan Bay, Korea. Fish Aqua. Sci., 13: 236-243. https://doi.org/10.5657/fas.2010.13.3.236
  13. Cornelissen, G., A. Pettersen, D. Broman, P. Mayer and G.D. Breedveld, 2008. Field testing of equilibrium passive samplers to determine freely dissolved native polycyclic aromatic hydrocarbon concentrations. Environ. Toxicol. Chem., 27: 499-508. https://doi.org/10.1897/07-253.1
  14. Fernandez, L.A., W. Lao, K.A. Maruya, C. White and R.M. Burgess, 2012. Passive sampling to measure baseline dissolved persistent organic pollutant concentrations in the water column of the palos verdes shelf superfund site. Environ. Sci. Technol., 46: 11937-11947. https://doi.org/10.1021/es302139y
  15. Fernandez, L.A., W. Lao, K.A. Maruya and R.M. Burgess, 2014. Calculating the diffusive flux of persistent organic pollutants between sediments and the water column on the palos verdes shelf superfund site using polymeric passive samplers. Environ. Sci. Technol., 48: 3925-3934. https://doi.org/10.1021/es404475c
  16. Gao, X., P. Huang, Q. Huang, K. Rao, Z. Lu, Y. Xu, G.W. Gabrielsen, I. Hallanger, M. Ma and Z. Wang, 2019. Organophosphorus flame retardants and persistent, bioaccumulative, and toxic contaminants in Arctic seawaters: On-board passive sampling coupled with target and non-target analysis. Environ. Pollut., 253: 1-10. https://doi.org/10.1016/j.envpol.2019.06.094
  17. Huckins, J.N., M.W. Tubergen and G.K. Manuweera, 1990. Semipermeable membrane devices containing model lipid: A new approach to monitoring the bioavaiiability of lipophilic contaminants and estimating their bioconcentration potential. Chemosphere, 20: 533-552. https://doi.org/10.1016/0045-6535(90)90110-F
  18. Huckins, J.N., J.D. Petty, J.A. Lebo, F.V. Almeida, K. Booij, D.A. Alvarez, W.L. Cranor, R.C. Clark and B.B. Mogensen, 2002. Development of the permeability/performance reference compound approach for in situ calibration of semipermeable membreane devices. Environ. Sci. Technol., 36: 85-91. https://doi.org/10.1021/es010991w
  19. Huckins, J.N., J.D. Petty and K. Booij, 2006. Monitors of Organic Chemicals in the Environment: Semipermeable Membrane Devices. Springer Science & Business Media, New York.
  20. Interstate Technology & Regulatory Council (ITRC), 2011. Incorporating bioavailability considerations into the evaluation of contaminated sediment sites, 162 pp.
  21. Jeong, D.Y., Y.L. Jang, H.J. Lee, H.J. Jeong, N.Y. Kim, J.H. Won and G.B. Kim, 2020. Optimization of ex-situ experiment and application in contaminated sediment for determination of the freely dissolved concentration of polycyclic aromatic hydrocarbons. J. Korean Soc. Mar. Environ. Energy, 23: 109-116. https://doi.org/10.7846/jkosmee.2020.23.3.109
  22. Joyce, A.S., M.S. Pirogovsky, R.G. Adams, W. Lao, D. Tsukada, C.L. Cash, J.F. Haw and K.A. Maruya, 2015. Using performance reference compound-corrected polyethylene passive samplers and caged bivalves to measure hydrophobic contaminants of concern in urban coastal seawaters. Chemosphere, 127: 10-17. https://doi.org/10.1016/j.chemosphere.2014.12.067
  23. Joyce, A.S. and R.M. Burgess, 2018. Using performance reference compounds to compare mass transfer calibration methodologies in passive samplers deployed in the water column. Environ. Toxicol. Chem., 37: 2089-2097. https://doi.org/10.1002/etc.4167
  24. Ju, J.H., I.S. Lee, W.J. Sim, H. Eun and J.E. Oh, 2009. Analysis and evaluation of chlorinated persistent organic compounds and PAHs in sludge in Korea. Chemosphere, 74: 441-447. https://doi.org/10.1016/j.chemosphere.2008.09.059
  25. Kim, G.B. and H.M. Stapleton, 2010. PBDEs, methoxylated PBDEs and HBCDs in Japanese common squid (Todarodes pacificus) from Korean offshore waters. Mar. Pollut. Bull., 60: 935-940. https://doi.org/10.1016/j.marpolbul.2010.03.025
  26. Kim, N.Y., Y.L. Jang, H. Jeong, D.Y. Jeong and G.B. Kim, 2020. Applicability of vinyl wrap (linear low density polyethylene) as a new passive sampler: Measurement of freely dissolved polycyclic aromatic hydrocarbons in the offshore. J. Korean Soc. Mar. Environ. Energy, 23: 277-285. https://doi.org/10.7846/JKOSMEE.2020.23.4.277
  27. Kim, S.K. and D.H. Chae, 2016. Seasonal variation in diffusive exchange of polycyclic aromatic hydrocarbons across the air-seawater interface in coastal urban area. Mar. Pollut. Bull., 109: 221-229. https://doi.org/10.1016/j.marpolbul.2016.05.078
  28. Lao, W., K.A. Maruya and D. Tsukada, 2019. An exponential model based new approach for correcting aqueous concentrations of hydrophobic organic chemicals measured by polyethylene passive samplers. Sci. Total Environ., 646: 11-18. https://doi.org/10.1016/j.scitotenv.2018.07.192
  29. Lohmann, R. and D. Muir, 2010. Global aquatic passive sampling (AQUA-GAPS): Using passive samplers to monitor POPs in the waters of the world. Environ. Sci. Technol., 44: 860-864. https://doi.org/10.1021/es902379g
  30. Lohmann, R., 2012. Critical review of low-density polyethylene's partitioning and diffusion coefficients for trace organic contaminants and implications for its use as a passive sampler. Environ. Sci. Technol., 46: 606-618. https://doi.org/10.1021/es202702y
  31. Ma, M., Z. Feng, C. Guan, Y. Ma, H. Xu and H. Li, 2001. DDT, PAH and PCB in sediments from the intertidal zone of the Bohai Sea and the Yellow Sea. Mar. Pollut. Bull., 42: 132-136. https://doi.org/10.1016/S0025-326X(00)00118-1
  32. Monteyne, E., P. Roose and C.R. Janssen, 2013. Application of a silicone rubber passive sampling technique for monitoring PAHs and PCBs at three Belgian coastal harbours. Chemosphere, 91: 390-398. https://doi.org/10.1016/j.chemosphere.2012.11.074
  33. Moschet, C., E.L.M. Vermeirssen, R. Seiz, H. Pfefferli and J. Hollender, 2014. Picogram per liter detections of pyrethroids and organophosphates in surface waters using passive sampling. Water Res., 66: 411-422. https://doi.org/10.1016/j.watres.2014.08.032
  34. Ohura, T., H. Sakakibara, I. Watanabe, W.J. Shim, P.M. Manage and K.S. Guruge, 2015. Spatial and vertical distributions of sedimentary halogenated polycyclic aromatic hydrocarbons in moderately polluted areas of Asia. Environ. Pollut., 196: 331-340. https://doi.org/10.1016/j.envpol.2014.10.028
  35. Ortega-Calvo, J.J., J. Harmsen, J.R. Parsons, K.T. Semple, M.D. Aitken, C. Ajao, C. Eadsforth, M. Galay-Burgos, R. Naidu, R. Oliver, W.J.G.M. Peijnenburg, J. Römbke, G. Streck and B. Versonnen, 2015. From bioavailability science to regulation of organic chemicals. Environ. Sci. Technol., 49: 10255-10264. https://doi.org/10.1021/acs.est.5b02412
  36. Park, J.M., S.B. Lee, J.P. Kim, M.J. Kim, O.S. Kwon and D.I. Jung, 2009. Behavior of PAHs from sewage sludge incinerators in Korea. Waste Manage., 29: 690-695. https://doi.org/10.1016/j.wasman.2008.08.015
  37. Perron, M.M., R.M. Burgess, E.M. Suuberg, M.G. Cantwell and K.G. Pennell, 2013. Performance of passive samplers for monitoring estuarine water column concentrations: 1. Contaminants of concern. Environ. Toxicol. Chem., 32: 2182-2189. https://doi.org/10.1002/etc.2321
  38. Perugini, M., P. Visciano, A. Giammarino, M. Manera, W.D. Nardo and M. Amorena, 2007. Polycyclic aromatic hydrocarbons in marine organisms from the Adriatic Sea, Italy. Chemosphere, 66: 1904-1910. https://doi.org/10.1016/j.chemosphere.2006.07.079
  39. RIVM (National Institute for Public Health and the Environment), 2012. Environmental risk limits for polycyclic aromatic hydrocarbons (PAHs) for direct aquatic, benthic, and terrestrial toxicity, 337 pp.
  40. Sacks, V.P. and R. Lohmann, 2012, Freely dissolved PBDEs in water and porewater of an urban estuary, Environ. Pollut., 162: 287-293. https://doi.org/10.1016/j.envpol.2011.11.028
  41. Sun, C., T. Soltwedel, E. Bauerfeind, D.A. Adelman and R. Lohmann, 2016. Depth profiles of persistent organic pollutants in the North and Tropical Atlantic Ocean. Environ. Sci. Technol., 50: 6172-6179. https://doi.org/10.1021/acs.est.5b05891
  42. United States Environmental Protection Agency (USEPA), 2012. Guidelines for using passive samplers to monitor organic contaminants at superfund sediment sites, 32 pp.
  43. United States Environmental Protection Agency (USEPA), 2017. Laboratory, field, and analytical procedures for using passive sampling in the evaluation of contaminated sediments: User's manual, 153 pp.
  44. Vrana, B., G. Mills, R. Greenwood, J. Knutsson, K. Svensson and G. Morrison, 2005. Performance optimisation of a passive sampler for monitoring hydrophobic organic pollutants in water. J. Environ. Monit., 7, 612-620. https://doi.org/10.1039/b419070j
  45. Wang, Q., F. Peng, Y. Chen, L. Jin, J. Lin, X. Zhao, J. Yin and J.Y. Li, 2019. Heavy metals and PAHs in an open fishing area of the East China Sea: Multimedia distribution, source diagnosis, and dietary risk assessment. Environ. Sci. Pollut. Res., 26: 21140-21150. https://doi.org/10.1007/s11356-019-05355-z
  46. Ya, M., L. Xu, Y. Wu., Y. Li, S. Zhao and X. Wang, 2018. Fossil fuel-derived polycyclic aromatic hydrocarbons in the Taiwan Strait, China, and fluxes across the air-water interface. Environ. Sci. Technol., 52: 7307-7316. https://doi.org/10.1021/acs.est.8b01331
  47. Yoon, S.J., S. Hong, S. Kim, J. Lee, T. Kim, B. Kim, B.O. Kwon, Y. Zhou, B. Shi, P. Liu, W. Hu, B. Huang, T. Wang and J.S. Khim, 2020. Large-scale monitoring and ecological risk assessment of persistent toxic substances in riverine, estuarine, and coastal sediments of the Yellow and Bohai seas. Environ. Int., 137: 105517. https://doi.org/10.1016/j.envint.2020.105517
  48. You, J., P.F. Landrum and M.J. Lydy, 2006. Comparison of chemical approaches for assessing bioavailability of sediment-associated contaminants. Environ. Sci. Technol., 40: 6348-6353. https://doi.org/10.1021/es060830y
  49. Zhao, W., M. Cai, D. Adelman, M. Khairy, P. August and R. Lohmann, 2018. Land-use-based sources and trends of dissolved PBDEs and PAHs in an urbanized watershed using passive polyethylene samplers. Environ. Pollut., 238: 573-580. https://doi.org/10.1016/j.envpol.2018.02.057