Simultaneous Determinations of Methoxylated Polybrominated Diphenyl Ethers and Polybrominated Diphenyl Ethers in Dairy Products from China by GC-MS
Science Journal of Analytical Chemistry
Volume 3, Issue 6, November 2015, Pages: 80-90
Received: Sep. 16, 2015;
Accepted: Oct. 4, 2015;
Published: Oct. 23, 2015
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Decong Hu, Hubei Entry-Exit Inspection and Quarantine Bureau of PRC, Wuhan, China; China Certification & Inspection Group HuBei Co., Ltd, Wuhan, China
Xiaozhong Hu, Hubei Entry-Exit Inspection and Quarantine Bureau of PRC, Wuhan, China; China Certification & Inspection Group HuBei Co., Ltd, Wuhan, China
Wei Chen, Hubei Entry-Exit Inspection and Quarantine Bureau of PRC, Wuhan, China; China Certification & Inspection Group HuBei Co., Ltd, Wuhan, China
Hong Wang, Hubei Provincial Supervision and Inspection Research Institute for Products Quality, Wuhan, China
Kuanzheng Zhu, Hubei Provincial Supervision and Inspection Research Institute for Products Quality, Wuhan, China
Bin Wu, Technology Center of Liaoning Entry-Exit Inspection and Quarantine Bureau of PRC, Changjiang Dalian, China
Changjun Lin, Technology Center of Liaoning Entry-Exit Inspection and Quarantine Bureau of PRC, Changjiang Dalian, China
In this paper, the method of simultaneous determinations of methoxylated polybrominated diphenyl ethers and polybrominated diphenyl ethers in dairy products from China was investigated. PBDEs are widely used brominated flame retardant, which are increasingly reported in the environment. MeO-PBDEs are structural analogs to PBDEs, and reported as natural products and novel pollutants present in the environment. A new isotopic dilution GC-MS method was firstly developed to simultaneously determine fourteen PBDEs and eight MeO-PBDEs in dairy products (full cream milk powder, skim milk powder, pure milk and acidophilus milk) in this study. Solvent extraction, gel permeation chromatography (GPC) and silica gel column cleanup were used, some important steps and crucial parameters were modified and intensified compared with other literatures. Besides, the conditions of GC and MS were also optimized. The limits of quantitation values of 1-50, 4-20 μg kg-1 in full cream milk powders, skim milk powders, pure milks and acidophilus milks were calculated for PBDEs and MeO-PBDEs. In addition, good repeatability and accuracy of the whole method were achieved. Moreover, Eighteen kinds of commercial full cream milk powder samples, sixteen skim milk powder samples, twenty pure milk samples and fifteen acidophilus milk samples were collected from local supermarket in Wuhan, Hubei province. These samples were analyzed to determine whether these samples were contaminated by PBDEs and MeO-PBDEs. The method was successfully applied to determine methoxylated polybrominated diphenyl ethers and polybrominated diphenyl ethers in these dairy products. Using the established methods, PBDEs and MeO-PBDEs were not detected in all samples.
Simultaneous Determinations of Methoxylated Polybrominated Diphenyl Ethers and Polybrominated Diphenyl Ethers in Dairy Products from China by GC-MS, Science Journal of Analytical Chemistry.
Vol. 3, No. 6,
2015, pp. 80-90.
De Wit, C.A, An overview of brominated flame retardants in the environment, Chemosphere, 46 (2002) 583–624.
Watanabe, I., Sakai, S.I, Environmental release and behavior of brominated flame retardants, Environment International, 29 (2003) 665–682.
M. Alaee, P. Arias, A. Sjodin, A. Bergman, An overview of commercially used brominated flame retardants, their applications, their use patterns in different countries/regions and possible modes of release, Environ. Int. 29 (2003) 683–689.
R. Alcock, A.J. Sweetman, K. Prevedouros, K.C. Jones, Understanding levels and trends of BDE-47 in the UK and North America: an assessment of principal reservoirs and source inputs, Environ. Int. 29 (2003) 691–698.
B.H. Wilford, T. Harner, J. Zhu, M. Shoeib, K.C. Jones, Passive sampling survey of polybrominated diphenyl ether flame retardants in indoor and outdoor air in Ottawa, Canada: implications for sources and exposure, Environ. Sci. Technol. 38 (2004) 5312–5318.
H. M. Stapleton, N. G. Dodder, J. H. Offenberg, M. M. Schantz, S. A. Wise, Polybrominated diphenyl ethers in house dust and clothes dryer lint, Environ. Sci. Technol. 39 (2005) 925–931.
A. Kirkegaard, A. Bignert, U. Sellstrom, M. Olsson, B. Jansson, C.A. de Wit, Polybrominated diphenyl ethers (PBDEs) and their methoxylated derivates in pike from Swedish waters with emphasis on temporal trends, 1967–2000, Environ. Pollut. 130 (2004) 187–198.
Sihem Ben Hassinea, Walid Ben Ameura, Ethel Eljarratb, Damià Barcelób, Soufiane Touila, Mohamed Ridha Drissa, Methoxylated polybrominated diphenyl ethers (MeO-PBDE) in human milk from Bizerte, Tunisia, Environmental research 138 (2015) 32-37.
D. Handayani, R. A. Edrada, P. Proksch, V. Wray, L. Witte, R. W. Van Soest, Four new bioactive polybrominated diphenyl ethers of the sponge Dysidea herbacea from West Sumatra, Indonesia, Journal of Natural Products, 60 (1997) 1313–1316.
Wen-Long Lia, Hong Qia, Wan-Li Maa, Li-Yan Liua, Zhi Zhangb, Mohammed O.A. Mohammeda, Wei-Wei Songa, Zifeng Zhanga, Yi-Fan Lia, Brominated flame retardants in Chinese air before and after the phase out of polybrominated diphenyl ethers, Atmospheric Environment, 117 (2015) 156–161.
L. Weijs, S. Losada, K. Das, L. Roosens, P.J. Reijnders, J.F. Santos, H. Neels, R. Blust, A. Covaci, Biomagnification of naturally-produced methoxylated polybrominated diphenyl ethers (MeO-PBDEs) in harbour seals and harbour porpoises from the southern North Sea, Environment Iinternational, 35 (2009) 893–899.
B.C. Kelly, M.G. Ikonomou, J.D. Blair, FAPC. Gobas, Hydroxylated and methoxylated polybrominated diphenyl ethers in a Canadian Arctic marine food web, Environmental Science & Technology, 42 (2008) 7069–7077.
C.L. Feng, Y.P. Xu, Y. He, Q. Luo, J.M. Zha, Z.J. Wang, Debrominated and methoxylated polybrominated diphenyl ether metabolites in rainbow trout (Oncorhynchus mykiss) after exposure to decabromodiphenyl ether, Journal of Environmental Sciences, 22 (2010) 1425–1434.
P. Haglund, D.R. Zook, H.R. Buser, J. Hu, Identification and quantification of polybrominated diphenyl ethers and methoxy-polybrominated diphenyl ethers in Baltic biota, Environmental Science & Technology, 31 (1997) 3281–3287.
U. Nordlof, B. Helander, A. Bignert, L. Asplund, Levels of brominated flame retardants and methoxylated polybrominated diphenyl ethers in eggs of white-tailed sea eagles breeding in different regions of Sweden, Science of the Total Environment, 409 (2010) 238–246.
S. Losada, F.J. Santos, A. Covaci, M.T. Galceran, Gas chromatography–ion trap tandem mass spectrometry method for the analysis of methoxylated polybrominated diphenyl ethers in fish, Journal of Chromatography A, 1217 (2010) 5253–5260.
W.B. Ameur, S.B. Hassine, E. Eljarrat, Y.E. Megdiche, S. Trabelsi, B. Hammami, D. Barcelo, M.R. Driss, Polybrominated diphenyl ethers and their methoxylated analogs in mullet (Mugil cephalus) and sea bass (Dicentrarchus labrax) from Bizerte Lagoon, Tunisia, Marine Environmental Research, 72 (2011) 258–264.
J.T. Sun, J.Y. Liu, Q. Liu, G.B. Qu, T. Ruan, G.B. Jiang, Sample preparation method for the speciation of polybrominated diphenyl ethers and their methoxylated and hydroxylated analogues in diverse environmental matrices, Talanta, 88 (2012) 669–676.
K. Lofstrand, X.T. Liu, D. Lindqvist, S. Jensen, L. Asplund, Seasonal variations of hydroxylated and methoxylated brominated diphenyl ethers in blue mussels from the Baltic Sea, Chemosphere, 84 (2011) 527–532.
G.B. Kim, H.M. Stapleton, PBDEs, methoxylated PBDEs and HBCDs in Japanese common squid (Todarodes pacificus) from Korean offshore waters, Marine Pollution Bulletin, 60 (2010) 935–940.
A. Rotander, B. van Bavel, F. Riget, G.A. Auðunsson, A. Polder, G.W. Gabrielsen, G. Víkingsson, B. Mikkelsen, M. Dam, Methoxylated polybrominated diphenyl ethers (MeO-PBDEs) are major contributors to the persistent organobromine load in sub-Arctic and Arctic marine mammals, 1986–2009, Science of the Total Environment, 416 (2012) 482–489.
P.O. Darnerud, G.S. Eriksen, T. Johannesson, P.B. Larsen, M. Viluksela, Polybrominated diphenyl ethers: occurrence, dietary exposure and toxicology, Environmental Health Perspectives, 109 (2001) 49–68.
Liqin Yua, Zhihua Hanb, Chunsheng Liu, A review on the effects of PBDEs on thyroid and reproduction systems in fish, General and Comparative Endocrinology, 219 (2015) 64–73.
P. Eriksson, E. Jakobsson, A. Fredriksson, Brominated flame retardants: a novel class of developmental neurotoxicants in our environment, Environmental Health Perspectives, 109 (2001) 903–908.
H. Viberg, A. Fredriksson, P. Eriksson, Neonatal exposure to the brominated flame retardant 2,2’,4,4’,5-pentabromodiphenyl ether causes altered susceptibility in the cholinergic transmitter system in the adult mouse, Toxicology Sciences, 67 (2002) 104–107.
H. Viberg, A. Fredriksson, P. Eriksson, Neonatal exposure to polybrominated diphenyl ether (PBDE 153) disrupts spontaneous behaviour, impairs learning and memeory, and decreases hippocampal cholinergic receptors in adult mice, Toxicology and applied pharmacology, 192 (2003) 95–106.
T. Zhou, M.M. Taylor, M.J. DeVito, K.M. Crofton, Developmental exposure to brominated diphenyl ethers results in thyroid hormone disruption, Toxicology Sciences, 66 (2002) 105–116.
I. Branchi, E. Alleva, L.G. Costa, Effects of perinatal exposure to a polybrominated diphenyl ether (PBDE-99) on mouse neurobehavioural development, Neurotoxicology, 23 (2002) 375–384.
I. Branchi, F. Capone, E. Alleva, L.G. Costa, Polybrominated diphenyl ethers: neurobehavioral effects following developmental exposure, Neurotoxicology, 24 (2003) 449–462.
T. Reistad, F. Fonnum, E. Mariussen, Neurotoxicity of the pentabrominated diphenyl ether mixture, DE-71, and hexabromocyclododecane (HBCD) in rat cerebellar granule cells in vitro, Archives of Toxicology, 80 (2006) 785–796.
F. Madia, G. Giordano, V. Fattori, A. Vitalone, I. Branchi, F. Capone, L.G. Costa, Differential in vitro neurotoxicity of the flame retardant PBDE-99 and of the PCB Aroclor 1254 in human astrocytoma cells, Toxicology Letters, 154 (2004) 11–21.
X.Z. Hu, Y. Xu, D.C. Hu, Y. Hui, F.X. Yang, Apoptosis induction on human hepatoma cells Hep G2 of decabrominated diphenyl ether (PBDE-209), Toxicol. Lett. 171 (2007) 19–28.
Y.H. He, M.B. Murphy, R.M.K. Yu, M.H.W. Lam, M. Hecker, J.P. Giesy, R.S.S. Wu, P.K.S. Lam, Effects of 20 PBDE metabolites on steroidogenesis in the H295R cell line, Toxicol. Lett. 176 (2008) 230–238.
R.F. Song, Y.H. He, M.B. Murphy, L.W.Y. Yeung, R.M.K. Yu, M.H.W. Lam, P.K.S. Lam, M. Hecker, J.P. Giesy, S.S. WuRudolf, W.B. Zhang, G.Y. Sheng, J.M. Fu, Effects of fifteen PBDE metabolites, DE71, DE79 and TBBPA on steroidogenesis in the H295R cell line, Chemosphere 71 (2008) 1888–1894.
X.Z. Hu, D.C. Hu, Q. Song, J. Li, P. Wang, S.F. Guo, Analysis and occurrences of perfluorinated compounds in agricultural and aquatic products and water from China, J. Liq. Chromatogr. R. T. 34 (2011) 2196–2210.
X.Z. Hu, D.C. Hu, Q. Song, J. Li, P. Wang, Determinations of hexabromocyclododecane (HBCD) isomers in channel catfish, crayfish, hen eggs and fish feeds from China by isotopic dilution LC–MS/MS, Chemosphere 82 (2011) 698–707.
S. Lacorte, M.G. Ikonomou, M. Fischer, A comprehensive gas chromatography coupled to high resolution mass spectrometry based method for the determination of polybrominated diphenyl ethers and their hydroxylated and methoxylated metabolites in environmental samples; Journal of Chromatography A, 1217 (2010) 337–347.
Kato Yoshihisa, Okada Syohei, Atobe Kazutaka, Endo Tetsuya, Matsubara Futoshi, Oguma Takayoshi and Haraguchi Koichi, Simultaneous Determination by APCI-LC/MS/MS of Hydroxylated and Methoxylated Polybrominated Diphenyl Ethers Found in Marine Biota, Anal. Chem, 81 (2009) 5942–5948.
Shi Zhixiong, Jiao Yang, Hu Yue, Sun Zhiwei, Zhou Xianqing, Feng Jinfang, Li Jingguang, Wu Yongning, Levels of tetrabromobisphenol A, hexabromocyclododecanes and polybrominated diphenyl ethers in human milk from the general population in Beijing, China, Science of the Total Environment, 10–18 (2013) 452–453.