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Development of a cleanup method for polybrominated diphenyl ether (PBDE) in fish by freezing-lipid filtration

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Abstract

A new cleanup method for the determination of brominated flame retardants with an emphasis on polybrominated diphenyl ethers (PBDEs) has been developed for fish tissue sample. This method effectively reduces the sample pretreatment time, labor and required less solvent quantities relative to conventional methods. Freezing-lipid filtration procedure removes approximately 90 % of the lipids in the extract without any significant loss of the PBDEs. A multilayered silica gel column was used for further cleanup of the extracts after freezing-lipid filtration. Multilayered silica gel column chromatography eliminated most of the co-extracted interferences, such as residual lipids and fatty acids. The extracts were analyzed after cleanup by high-resolution gas chromatography/high-resolution mass spectrometry using the isotope dilution method. Tissue samples with 1.6–8.0 and 8.0–40 ppb of PBDE were analyzed using both the sulfuric acid treatment and freezing-lipid filtration cleanup methods in order to evaluate the method performance. Sulfuric acid treatment did not detect 2,4-DiBDE, whereas freezing-lipid filtration detected 2,4-DiBDE but at 50 % recovery. To compare the method, WMF-01 was analyzed via both the sulfuric acid treatment and freezing-lipid filtration cleanup.

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References

  1. Renner R (2000) What fate for brominated fire retardants? Environ Sci Technol 34:223A–226A

    Google Scholar 

  2. de Boer J, de Boer K, Boon JP (2000) The handbook of environmental chemistry, part K, vol 3. Springer, Berlin, pp 61–95

    Google Scholar 

  3. Law RJ, Alaee M, Allchin C, Boon JP, Lebeuf M, Lepom P, Stern GA (2003) Levels and trends of polybrominated diphenylethers and other brominated flame retardants in wildlife. Environ Int 29:757–770

    Article  CAS  Google Scholar 

  4. Meerts IATM, van Zanden JJ, Luijks EAC, van Leeuwen-Bol I, Marsh G, Jakobsson E, Bergman A, Brouwer A (2000) Potent competitive interactions of some brominated flame retardants and related compounds with human transthyretin in vitro. Toxicol Sci 56:95–104

    Article  CAS  Google Scholar 

  5. Richardson VM, Staskal DF, Ross DG, Diliberto JJ, DeVito MJ, Birnbaum LS (2008) Possible mechanisms of thyroid hormone disruption in mice by BDE 47, a major polybrominated diphenyl ether congener. Toxicol Appl Pharmacol 226:244–250

    Article  CAS  Google Scholar 

  6. Bezares-Cruz J, Jafvert CT, Hua I (2004) Solar photodecomposition of decabromodiphenyl ether: products and quantum yield. Environ Sci Technol 38:4149–4156

    Article  CAS  Google Scholar 

  7. Keum YS, Li QX (2005) Reductive debromination of polybrominated diphenyl ethers by zerovalent iron. Environ Sci Technol 39:2280–2286

    Article  CAS  Google Scholar 

  8. Viberg H, Johansson N, Fredriksson A, Eriksson J, Marsh G, Eriksson P (2006) Neonatal exposure to higher brominated diphenyl ethers, hepta-, octa-, or nonabromodiphenyl ether, impairs spontaneous behavior and learning and memory functions of adult mice. Toxicol Sci 92:211–218

    Article  CAS  Google Scholar 

  9. Costa LG, Giordano G (2007) Developmental neurotoxicity of polybrominated diphenyl ether (PBDE) flame retardants. Neurotoxicology 28:1047–1067

    Article  CAS  Google Scholar 

  10. Hale RC, La Guardia MJ, Harvey EP, Mainor TM, Duff WH, Gaylor MO (2002) Polybrominated diphenyl ether flame retardants in Virginia freshwater fishes (USA). Environ Sci Technol 35:4585–4591

    Article  Google Scholar 

  11. Covaci A, Gheorghe A, Voorspoels S, Maervoet J, Steen Redeker E, Blust R, Schepens P (2005) Polybrominated diphenyl ethers, polychlorinated biphenyls and organochlorine pesticides in sediment cores from the Western Scheldt river (Belgium): analytical aspects and depth profiles. Environ Int 31:367–375

    Article  CAS  Google Scholar 

  12. Booij K, Zegers BN, Boon JP (2002) Levels of some polybrominated diphenyl ether (PBDE) flame retardants along the Dutch coast as derived from their accumulation in SPMDs and blue mussels (Mytilus edulis). Chemosphere 46:683–688

    Article  CAS  Google Scholar 

  13. Noren K, Meironyte D (2000) Certain organochlorine and organobromine contaminants in Swedish human milk in perspective of past 20–30 years. Chemosphere 40:1111–1123

    Article  CAS  Google Scholar 

  14. Turner C, Eskilsson CP, Bjorklund E (2002) Collection in analytical-scale supercritical fluid extraction. J Chromatogr A 947:1–22

    Article  CAS  Google Scholar 

  15. Fiddler W, Pensabene JW, Gates RA, Donoghue DJ (1999) Supercritical fluid extraction of organochlorine pesticides in eggs. J Agric Food Chem 47:206–211

    Article  CAS  Google Scholar 

  16. Eskilsson CS, Bjorklund E (2000) Analytical-scale microwave-assisted extraction. J Chromatogr A 902:227–250

    Article  CAS  Google Scholar 

  17. Fitzpatrick LJ, Dean JR (2002) Extraction solvent selection in environmental analysis. Anal Chem 74:74–79

    Article  CAS  Google Scholar 

  18. Ramos E, Kristenson M, Brinkman UATh (2002) Current use of pressurised liquid extraction and subcritical water extraction in environmental analysis. J Chromatogr A 975:3–29

    Article  CAS  Google Scholar 

  19. Castro J, Sanchez-Brunete C, Tadeo J (2001) Multiresidue analysis of insecticides in soil by gas chromatography with electron–capture detection and confirmation by gas chromatography–mass spectrometry. J Chromatogr A 918:371–380

    Article  CAS  Google Scholar 

  20. Thompsen C, Lundanes E, Becher G (2001) A simplified method for determination of tetrabromobisphenol A and polybrominated diphenyl ethers in human plasma and serum. J Sep Sci 24:282–290

    Article  Google Scholar 

  21. Bester K, Biselli S, Ellerichmann T, Huhnerfuss H, Moller K, Rimkus G, Wolf M (1998) Chlorostyrenes in fish and sediment samples from the river Elbe. Chemosphere 37:2459–2471

    Article  CAS  Google Scholar 

  22. Chu S, Covaci A, Voorspeols S, Schepens P (2003) The distribution of octachlorostyrene (OCS) in environmental samples from Europe. J Environ Monit 5:619–625

    Article  CAS  Google Scholar 

  23. Smith LM, Stalling DL, Johnson JL (1984) Determination of part-per-trillion levels of polychlorinated dibenzofurans and dioxins in environmental samples. Anal Chem 56:1830–1842

    Article  CAS  Google Scholar 

  24. Ryan JJ, Lau PY, Pilon JC, Lewis D, McLeod HA, Gervais A (1984) Incidence and levels of 2,3,7,8-tetrachlorodibenzo-p-dioxin in Lake Ontario commercial fish. Environ Sci Technol 18:719–721

    Article  CAS  Google Scholar 

  25. de Boer J, Allchin C, Law R, Zegers B, Boon JP (2001) Method for the analysis of polybrominated diphenylethers in sediments and biota. Trends Anal Chem 20:591–599

    Article  Google Scholar 

  26. Ohta S, Ishizuka D, Nishimura H, Nakao T, Aozosa O, Shimidzu Y, Ochiai F, Kida T, Nishi M, Miyata H (2002) Comparison of polybrominated diphenyl ethers in fish, vegetables, and meats and levels in human milk of nursing women in Japan. Chemosphere 46:689–696

    Article  CAS  Google Scholar 

  27. Hong J, Kim HY, Kim D, Seo J, Kim K (2004) Rapid determination of chlorinated pesticides in fish by freezing-lipid filtration, solid-phase extraction and gas chromatography–mass spectrometry. J Chromatogr A 1038:27–35

    Article  CAS  Google Scholar 

  28. Seo J, Kim HY, Chung BC, Hong J (2005) Simultaneous determination of anabolic steroids and synthetic hormones in meat by freezing-lipid filtration, solid-phase extraction and gas chromatography–mass spectrometry. J Chromatogr A 1067:303–309

    Article  CAS  Google Scholar 

  29. Ahn YG, Seo J, Shin JH, Kim J, Hong J (2006) Development of new cleanup method of polychlorinated dibenzo-p-dioxins/dibenzofurans in fish by freezing-lipid filtration. Anal Chim Acta 576:31–36

    Article  CAS  Google Scholar 

  30. Hagenmaier H, She J, Benz T, Dawidowsky N, Dusterhoft L, Lindig C (1992) Analysis of sewage sludge for polyhalogenated dibenzo-p-dioxins, dibenzofurans, and diphenylethers. Chemosphere 25:1457–1462

    Article  CAS  Google Scholar 

  31. Nácher-Mestre J, Serrano R, Hernández F, Benedito-Palos L, Pérez-Sánchez J (2010) Gas chromatography-mass spectrometric determination of polybrominated diphenyl ethers in complex fatty matrices from aquaculture activities. Anal Chim Acta 664:190–198

    Article  Google Scholar 

  32. Olukunle OI, Okonkwo OJ, Kefeni KK, Lupankwa M (2012) Determination of brominated flame retardants in Jukskei River catchment area in Gauteng, South Africa. Water Sci Technol 65: 743–749

    Article  CAS  Google Scholar 

  33. Xiao Z, Feng J, Shi Z, Li J, Zhao Y, Wu Y (2011) Determination of three brominated flame retardants in human serum using solid-phase extraction coupled with ultra-performance liquid chromatography-tandem mass spectrometry and gas chromatography-mass spectrometry. Chin J Chromatogr (Se Pu) 29: 1165–1172

    CAS  Google Scholar 

  34. Johnson A, Olson N (2001) Analysis and occurrence of polybrominated diphenyl ethers in Washington State freshwater fish. Arch Environ Contam Toxicol 41:339–344

    Article  CAS  Google Scholar 

  35. Zhang Z, Ohiozebau E, Rhind SM (2011) Simultaneous extraction and clean-up of polybrominated diphenyl ethers and polychlorinated biphenyls from sheep liver tissue by selective pressurized liquid extraction and analysis by gas chromatography-mass spectrometry. J Chromatogr A 1218:1203–1209

    Article  CAS  Google Scholar 

  36. Sun J, Liu J, Liu Q, Qu G, Ruan T, Jiang G (2012) Sample preparation method for the speciation of polybrominated diphenyl ethers and their methoxylated and hydroxylated analogues in diverse environmental matrices. Talanta 88:669–676

    Article  CAS  Google Scholar 

  37. Covaci A, de Boer J, Ryan JJ, Voorspoels S, Schepens P (2002) Determination of polybrominated diphenyl ethers and polychlorinated biphenyls in human adipose tissue by large-volume injection-narrow-bore capillary gas chromatography/electron impact low-resolution mass spectrometry. Anal Chem 74:790–798

    Article  CAS  Google Scholar 

  38. Ikonomou MG, Rayne S, Fischer M, Fernandez MP, Cretney W (2002) Occurrence and congener profiles of polybrominated diphenyl ethers (PBDEs) in environmental samples from coastal British Columbia, Canada. Chemosphere 46:649–663

    Article  CAS  Google Scholar 

  39. Wang P, Zhang Q, Wang Y, Wang T, Li X, Ding L, Jiang G (2010) Evaluation of Soxhlet extraction, accelerated solvent extraction and microwave-assisted extraction for the determination of polychlorinated biphenyls and polybrominated diphenyl ethers in soil and fish samples. Anal Chim Acta 662:43–48

    Article  Google Scholar 

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Acknowledgments

This work was supported by outstanding researchers program of Korea Research Foundation (T31750).

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Authors and Affiliations

  1. Korea Basic Science Institute, Seoul, 136-701, Korea

    Jeoung Hwa Shin, Eunjung Bang & Jungju Seo

  2. Department of Biotechnology, College of Nature Science, Chosun University, Gwangju, 501-759, Korea

    Hee Ock Boo

  3. The Institute for Drug Research, School of Pharmacy, The Hebrew University, Hadassah Medical School, 91120, Jerusalem, Israel

    Shela Gorinstein

Authors
  1. Jeoung Hwa Shin
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  2. Hee Ock Boo
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  3. Eunjung Bang
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  4. Shela Gorinstein
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  5. Jungju Seo
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Corresponding authors

Correspondence to Shela Gorinstein or Jungju Seo.

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Shin, J.H., Boo, H.O., Bang, E. et al. Development of a cleanup method for polybrominated diphenyl ether (PBDE) in fish by freezing-lipid filtration. Eur Food Res Technol 235, 295–301 (2012). https://doi.org/10.1007/s00217-012-1758-z

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  • DOI: https://doi.org/10.1007/s00217-012-1758-z

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