Skip to main content
SpringerLink
Log in

Polybrominated diphenyl ethers (PBDEs) and hydroxylated PBDEs in human serum from Shanghai, China: a study on their presence and correlations

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Polybrominated diphenyl ethers (PBDEs) are becoming a public health concern because of their potential toxicity, from endocrine disruption system to neurodevelopmental impairments. Nonetheless, information on their levels in human blood is scarce. In this study, human serum samples collected in Shanghai, China, were analyzed for the concentrations of PBDEs and their hydroxylated metabolites (OH-PBDEs). Eight PBDE congeners and six OH-PBDE congeners were quantified in serum samples by gas chromatography with mass spectrometry (GC-MS) and high-performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). As a result, total PBDE concentration ranged from 0.280 to 12.330 ng g−1 on a lipid weight basis lw (median: 1.100 ng g−1 lw) and the total OH-PBDE level ranged from 0.045 to 0.363 ng g−1 (lw) (median: 0.187 ng g−1 lw). Among them, BDE-47 and 6-OH-BDE-47 were the predominant PBDEs and OH-PBDEs, respectively. In addition, based on the results of the Bartelett X 2 test, BDE-47 significantly (p < 0.05) correlated with BDE-28, BDE-100, BDE-85, and BDE-154, whereas 3′-OH-BDE-7 significantly (p < 0.01) correlated with 3-OH-BDE-47, 2-OH-BDE-68, and 6′-OH-BDE-99. Among all donors, no significant association between age and PBDEs (or OH-PBDEs) was found. Further research on the exposure routes in the environment and metabolic processing of PBDEs in human blood is necessary.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2

Similar content being viewed by others

References

  • Andersson Ö, Blomkvist G (1981) Polybrominated aromatic pollutants found in fish in Sweden. Chemosphere 10(9):1051–1060. https://doi.org/10.1016/0045-6535(81)90216-2

    Article  Google Scholar 

  • Boxtel AL, Kamstra JH, Cenijn PH, Pieterse B, Wagner MJ, Antink M, Krab K, Burg BV, Marsh G, Brouwer A (2008) Microarray analysis reveals a mechanism of phenolic polybrominated diphenylether toxicity in zebrafish. Environ Sci Technol 42(5):1773–1779. https://doi.org/10.1021/es0720863

    Article  Google Scholar 

  • Branchi I, Alleva E, Costa LG (2002) Effects of perinatal exposure to a polybrominated diphenyl ether (PBDE 99) on mouse neurobehavioural development. Neurotoxicology 23(3):375–384. https://doi.org/10.1016/S0161-813X(02)00078-5

    Article  CAS  Google Scholar 

  • Canton RF, Scholten DE, Marsh G, De Jong PC, Van den Berg M (2008) Inhibition of human placental aromatase activity by hydroxylated polybrominated diphenyl ethers (OH-PBDEs). Toxicol Appl Pharmacol 227(1):68–75. https://doi.org/10.1016/j.taap.2007.09.025

    Article  CAS  Google Scholar 

  • Cao J, Lin Y, Guo LH, Zhang AQ, Wei Y, Yang Y (2010) Structure-based investigation on the binding interaction of hydroxylated polybrominated diphenyl ethers with thyroxine transport proteins. Toxicology 277(1-3):20–28. https://doi.org/10.1016/j.tox.2010.08.012

    Article  CAS  Google Scholar 

  • Cesh LS, Elliott KH, Quade S, McKinney MA, Maisoneuve F, Garcelon DK, Sandau CD, Letcher RJ, Williams TD, Elliott JE (2010) Polyhalogenated aromatic hydrocarbons and metabolites: relation to circulating thyroid hormone and retinol in nestling bald eagles (Haliaeetus leucocephalus). Environ Toxicol Chem/SETAC 29:1301–1310

    CAS  Google Scholar 

  • Chen CE, Chen J, Zhao H, Xie Q, Yin Z, Ge L (2010) Levels and patterns of polybrominated diphenyl ethers in children's plasma from Dalian, China. Environ Int 36(2):163–167. https://doi.org/10.1016/j.envint.2009.10.009

    Article  Google Scholar 

  • Chu S, Letcher RJ (2013) Halogenated phenolic compound determination in plasma and serum by solid phase extraction, dansylation derivatization and liquid chromatography-positive electrospray ionization-tandem quadrupole mass spectrometry. J Chromatogr A 1320:111–117. https://doi.org/10.1016/j.chroma.2013.10.068

    Article  CAS  Google Scholar 

  • De la Torre A, Pacepavicius G, Martinez MA, Darling C, Muir D, Sherry J, McMaster M, Alaee M (2013) Polybrominated diphenyl ethers and their methoxylated and hydroxylated analogs in Brown Bullhead (Ameiurus nebulosus) plasma from Lake Ontario. Chemosphere 90(5):1644–1651. https://doi.org/10.1016/j.chemosphere.2012.09.005

    Article  Google Scholar 

  • Eguchi A, Nomiyama K, Devanathan G, Subramanian A, Bulbule KA, Parthasarathy P, Takahashi S, Tanabe S (2012) Different profiles of anthropogenic and naturally produced organohalogen compounds in serum from residents living near a coastal area and e-waste recycling workers in India. Environ Int 47:8–16. https://doi.org/10.1016/j.envint.2012.05.003

    Article  CAS  Google Scholar 

  • Eguchi A, Nomiyama K, Minh Tue N, Trang PT, Hung Viet P, Takahashi S, Tanabe S (2015) Residue profiles of organohalogen compounds in human serum from e-waste recycling sites in North Vietnam: association with thyroid hormone levels. Environ Res 137:440–449. https://doi.org/10.1016/j.envres.2015.01.007

    Article  CAS  Google Scholar 

  • Gustavson L, Ciesielski TM, Bytingsvik J, Styrishave B, Hansen M, Lie E, Aars J, Jenssen BM (2015) Hydroxylated polychlorinated biphenyls decrease circulating steroids in female polar bears (Ursus maritimus). Environ Res 138:191–201. https://doi.org/10.1016/j.envres.2015.02.011

    Article  CAS  Google Scholar 

  • Hamers T, Kamstra JH, Sonneveld E, Murk AJ, Kester MH, Andersson PL, Legler J, Brouwer A (2006) In vitro profiling of the endocrine-disrupting potency of brominated flame retardants. Toxicol Sci 92(1):157–173. https://doi.org/10.1093/toxsci/kfj187

    Article  CAS  Google Scholar 

  • Haraguchi K, Kotaki Y, Relox JR, Romero ML, Terada R (2010) Monitoring of naturally produced brominated phenoxyphenols and phenoxyanisoles in aquatic plants from the Philippines. J Agr Food Chem 58(23):12385–12391. https://doi.org/10.1021/jf103001n

    Article  CAS  Google Scholar 

  • Hassanin A, Breivik K, Meijer SN, Steinnes E, Thomas GO, Jones KC (2004) PBDEs in European background soils: levels and factors controlling their distribution. Environ Sci Technol 38(3):738–745. https://doi.org/10.1021/es035008y

    Article  CAS  Google Scholar 

  • He S, Li M, Jin J, Wang Y, Bu Y, Xu M, Yang X, Liu A (2013) Concentrations and trends of halogenated flame retardants in the pooled serum of residents of Laizhou Bay, China. Environ Toxicol Chem / SETAC 32(6):1242–1247. https://doi.org/10.1002/etc.2172

    Article  CAS  Google Scholar 

  • Houde M, Pacepavicius G, Darling C, Fair PA, Alaee M, Bossart GD, Solomon KR, Letcher RJ, Bergman Å, Marsh G (2009) Polybrominated diphenyl ethers and their hydroxylated analogs in plasma of bottlenose dolphins (Tursiops truncatus) from the United States east coast. Environ Toxicol Chem 28(10):2061–2068. https://doi.org/10.1897/09-031.1

    Article  CAS  Google Scholar 

  • Jiang Y, Wang X, Zhu K, Wu M, Sheng G, Fu J (2010) Occurrence, compositional profiles and possible sources of polybrominated diphenyl ethers in urban soils of Shanghai, China. Chemosphere 80(2):131–136. https://doi.org/10.1016/j.chemosphere.2010.04.007

    Article  CAS  Google Scholar 

  • Kang Y, Wang HS, Cheung KC, Wong MH (2011) Polybrominated diphenyl ethers (PBDEs) in indoor dust and human hair. Atmos Environ 45(14):2386–2393. https://doi.org/10.1016/j.atmosenv.2011.02.019

    Article  CAS  Google Scholar 

  • Kim S, Park J, Kim HJ, Lee JJ, Choi G, Choi S, Kim S, Kim SY, Moon HB, Kim S, Choi K (2015) Association between several persistent organic pollutants and thyroid hormone levels in cord blood serum and bloodspot of the newborn infants of Korea. PLoS One 10:125–213

    CAS  Google Scholar 

  • Kodavanti PRS, Ward TR (2005) Differential effects of commercial polybrominated diphenyl ether and polychlorinated biphenyl mixtures on intracellular signaling in rat brain in vitro. Toxicol Sci 85(2):952–962. https://doi.org/10.1093/toxsci/kfi147

    Article  CAS  Google Scholar 

  • Kojima H, Takeuchi S, Uramaru N, Sugihara K, Yoshida T, Kitamura S (2009) Nuclear hormone receptor activity of polybrominated diphenyl ethers and their hydroxylated and methoxylated metabolites in transactivation assays using Chinese hamster ovary cells. Environ Health Persp 117(8):1210–1218. https://doi.org/10.1289/ehp.0900753

    Article  CAS  Google Scholar 

  • Kuriyama SN, Wanner A, Fidalgo-Neto AA, Talsness CE, Koerner W, Chahoud I (2007) Developmental exposure to low-dose PBDE-99: tissue distribution and thyroid hormone levels. Toxicology 242(1-3):80–90. https://doi.org/10.1016/j.tox.2007.09.011

    Article  CAS  Google Scholar 

  • Liu J, Luo XJ, LH Y, He MJ, Chen SJ, Mai BX (2010) Polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyles (PCBs), hydroxylated and methoxylated-PBDEs, and methylsulfonyl-PCBs in bird serum from South China. Arch Environ Contam Toxicol 59(3):492–501. https://doi.org/10.1007/s00244-010-9487-4

    Article  CAS  Google Scholar 

  • Lupton SJ, McGarrigle BP, Olson JR, Wood TD, Aga DS (2009) Human liver microsome-mediated metabolism of brominated diphenyl ethers 47, 99, and 153 and identification of their major metabolites. Chem Res Toxicol 22(11):1802–1809. https://doi.org/10.1021/tx900215u

    Article  CAS  Google Scholar 

  • Mizukawa H, Nomiyama K, Kunisue T, Watanabe MX, Subramanian A, Iwata H, Ishizuka M, Tanabe S (2015) Organohalogens and their hydroxylated metabolites in the blood of pigs from an open waste dumping site in south India: association with hepatic cytochrome P450. Environ Res 138:255–263. https://doi.org/10.1016/j.envres.2015.02.012

    Article  CAS  Google Scholar 

  • Mizukawa H, Nomiyama K, Nakatsu S, Yachimori S, Hayashi T, Tashiro Y, Nagano Y, Tanabe S (2013) Species-specific differences in the accumulation features of organohalogen contaminants and their metabolites in the blood of Japanese terrestrial mammals. Environ Pollut 174:28–37. https://doi.org/10.1016/j.envpol.2012.11.004

    Article  CAS  Google Scholar 

  • Moon HB, Kannan K, Lee SJ, Choi M (2007) Atmospheric deposition of polybrominated diphenyl ethers (PBDEs) in coastal areas in Korea. Chemosphere 66(4):585–593. https://doi.org/10.1016/j.chemosphere.2006.09.042

    Article  CAS  Google Scholar 

  • Nomiyama K, Kanbara C, Ochiai M, Eguchi A, Mizukawa H, Isobe T, Matsuishi T, Yamada TK, Tanabe S (2014) Halogenated phenolic contaminants in the blood of marine mammals from Japanese coastal waters. Mar Environ Res 93:15–22. https://doi.org/10.1016/j.marenvres.2013.08.016

    Article  CAS  Google Scholar 

  • Norrgran J, Jones B, Lindquist NG, Bergman A (2012) Decabromobiphenyl, polybrominated diphenyl ethers, and brominated phenolic compounds in serum of cats diagnosed with the endocrine disease feline hyperthyroidism. Arch Environ Con Tox 63(1):161–168. https://doi.org/10.1007/s00244-012-9750-y

    Article  CAS  Google Scholar 

  • Qiu X, Zhu T, Hu J (2010) Polybrominated diphenyl ethers (PBDEs) and other flame retardants in the atmosphere and water from Taihu Lake, East China. Chemosphere 80(10):1207–1212. https://doi.org/10.1016/j.chemosphere.2010.06.013

    Article  CAS  Google Scholar 

  • Qu BL, Yu W, Huang YR, Cai BN, Du LH, Liu F (2015) 6-OH-BDE-47 promotes human lung cancer cells epithelial mesenchymal transition via the AKT/snail signal pathway. Environ Toxicol Phar 39(1):271–279. https://doi.org/10.1016/j.etap.2014.11.022

    Article  CAS  Google Scholar 

  • Ren G, Yu Z, Ma S, Zheng K, Wang Y, Wu M, Sheng G, Fu J (2011) Determination of polybrominated diphenyl ethers and their methoxylated and hydroxylated metabolites in human serum from electronic waste dismantling workers. Anal Methods 3(2):408–413. https://doi.org/10.1039/C0AY00571A

    Article  CAS  Google Scholar 

  • Sepúlveda A, Schluep M, Renaud FG, Streicher M, Kuehr R, Hagelüken C, Gerecke AC (2010) A review of the environmental fate and effects of hazardous substances released from electrical and electronic equipments during recycling: examples from China and India. Environ Impact Assess Rev 30(1):28–41. https://doi.org/10.1016/j.eiar.2009.04.001

    Article  Google Scholar 

  • Sjödin A, Jones RS, Focant JF, Lapeza C, Wang RY, McGahee EE, Zhang Y, Turner WE, Slazyk B, Needham LL (2004) Retrospective time-trend study of polybrominated diphenyl ether and polybrominated and polychlorinated biphenyl levels in human serum from the United States. Environ Health Persp 112(6):654–658. https://doi.org/10.1289/ehp.6826

    Article  Google Scholar 

  • Sjödin A, Wong LY, Jones RS, Park A, Zhang Y, Hodge C, DiPietro E, McClure C, Turner W, Needham LL (2008) Serum concentrations of polybrominated diphenyl ethers (PBDEs) and polybrominated biphenyl (PBB) in the United States population: 2003–2004. Environ Sci Technol 42(4):1377–1384. https://doi.org/10.1021/es702451p

    Article  Google Scholar 

  • Thuresson K, Höglund P, Hagmar L, Sjödin A, Bergman Å, Jakobsson K (2006) Apparent half-lives of hepta- to decabrominated diphenyl ethers in human serum as determined in occupationally exposed workers. Environ. Health Persp 114(2):176–181. https://doi.org/10.1289/ehp.8350

    Article  CAS  Google Scholar 

  • Wan Y, Jones PD, Wiseman S, Chang H, Chorney D, Kannan K, Zhang K, JY H, Khim JS, Tanabe S (2010) Contribution of synthetic and naturally occurring organobromine compounds to bromine mass in marine organisms. Environ Sci Technol 44(16):6068–6073. https://doi.org/10.1021/es100914r

    Article  CAS  Google Scholar 

  • Wan Y, Wiseman S, Chang H, Zhang X, Jones PD, Hecker M, Kannan K, Tanabe S, Hu J, Lam MH (2009) Origin of hydroxylated brominated diphenyl ethers: natural compounds or man-made flame retardants? Environ Sci Technol 43(19):7536–7542. https://doi.org/10.1021/es901357u

    Article  CAS  Google Scholar 

  • Wang C, Lin Z, Dong Q, Lin Z, Lin K, Wang J, Huang J, Huang X, He Y, Huang C (2012a) Polybrominated diphenyl ethers (PBDEs) in human serum from Southeast China. Ecotox Environ Safe 78:206–211. https://doi.org/10.1016/j.ecoenv.2011.11.016

    Article  CAS  Google Scholar 

  • Wang H, Chen Z, Ho K, Ge L, Du J, Lam MW, Giesy JP, Wong M, Wong CK (2012b) Hydroxylated and methoxylated polybrominated diphenyl ethers in blood plasma of humans in Hong Kong. Environ Int 47:66–72. https://doi.org/10.1016/j.envint.2012.06.004

    Article  CAS  Google Scholar 

  • Wiseman SB, Wan Y, Chang H, Zhang X, Hecker M, Jones PD, Giesy JP (2011) Polybrominated diphenyl ethers and their hydroxylated/methoxylated analogs: environmental sources, metabolic relationships, and relative toxicities. Mar Pollut Bull 63(5-12):179–188. https://doi.org/10.1016/j.marpolbul.2011.02.008

    Article  CAS  Google Scholar 

  • Wu MH, Xu BT, Xu G, Wang MN, Ma J, Pan CY, Sun R, Han T, Tang L (2017) Occurrence and profiles of polybrominated diphenyl ethers (PBDEs) in riverine sediments of Shanghai: a combinative study with human serum from the locals. Environ Geochem Health 39(4):729–738

  • Wu MH, Pei JC, Zheng M, Tang L, Bao YY, BT X, Sun R, Sun YF, Xu G, Lei JQ (2015) Polybrominated diphenyl ethers (PBDEs) in soil and outdoor dust from a multi-functional area of Shanghai: levels, compositional profiles and interrelationships. Chemosphere 118:87–95

    Article  CAS  Google Scholar 

  • Xu BT, Wu MH, Pan CY, Sun Y, Yuan DB, Tang L, Xu G (2017) Aquatic photolysis of hydroxylated polybromodiphenyl ethers under direct UV irradiation: a case study of 2′-HO-BDE-68. Environ Sci Pollut Res 24:14409–14416

    Article  CAS  Google Scholar 

  • Xu P, Lou X, Ding G, Shen H, Wu L, Chen Z, Han J, Wang X (2015) Effects of PCBs and PBDEs on thyroid hormone, lymphocyte proliferation, hematology and kidney injury markers in residents of an e-waste dismantling area in Zhejiang, China. Sci Total Environ 536:215–222. https://doi.org/10.1016/j.scitotenv.2015.07.025

    Article  CAS  Google Scholar 

  • Yu ZQ, Zheng KW, Ren GF, Zheng YY, Ma ST, Peng PG, Wu MH, Sheng GY, Fu JM (2010) Identification of hydroxylated octa and nona-bromodiphenyl ethers in human serum from electronic waste dismantling workers. Environ Sci Technol 44:3979–3985

    Article  CAS  Google Scholar 

  • Zeng YH, Luo XJ, Chen HS, Chen SJ, Wu JP, Mai BX (2013) Method for the purification of polybrominated diphenyl ethers in sediment for compound-specific isotope analysis. Talanta 111:93–97. https://doi.org/10.1016/j.talanta.2013.02.036

    Article  CAS  Google Scholar 

  • Zhou Y, Chen Q, Du X, Yin G, Qiu Y, Ye L, Zhu Z, Zhao J (2016) Occurrence and trophic magnification of polybrominated diphenyl ethers (PBDEs) and their methoxylated derivatives in freshwater fish from Dianshan Lake, Shanghai, China. Environ Pollut 219:932–938. https://doi.org/10.1016/j.envpol.2016.09.043

    Article  CAS  Google Scholar 

  • Zhu L, Ma B, Hites RA (2009) Brominated flame retardants in serum from the general population in northern China. Environ Sci Technol 43(18):6963–6968. https://doi.org/10.1021/es901296t

    Article  CAS  Google Scholar 

  • Zota AR, Park JS, Wang Y, Petreas M, Zoeller RT, Woodruff TJ (2011) Polybrominated diphenyl ethers, hydroxylated polybrominated diphenyl ethers, and measures of thyroid function in second trimester pregnant women in California. Environ Sci Technol 45(18):7896–7790. https://doi.org/10.1021/es200422b

    Article  CAS  Google Scholar 

Download references

Funding

This work was financially supported by the National Natural Science Foundation of China (41430644, 41473090, 11605111 and 41173120) and by Program for Changjiang Scholars and Innovative Research Team in University (IRT13078).

Author information

Authors and Affiliations

  1. Institute of Applied Radiation, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, People’s Republic of China

    Bentuo Xu, Minghong Wu, Chenyuan Pan, Liang Tang & Gang Xu

  2. Yinyuan Hospital, Jiading District, Shanghai, 201800, People’s Republic of China

    Mingnan Wang

  3. School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, 518055, People’s Republic of China

    Wenhui Qiu

Authors
  1. Bentuo Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Minghong Wu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Mingnan Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Chenyuan Pan
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Wenhui Qiu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Liang Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Gang Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Gang Xu.

Additional information

Responsible editor: Hongwen Sun

Highlights

• PBDEs and OH-PBDEs in human serum samples were quantified.

• BDE-47 and 6-OH-BDE-47 were predominant congeners in most of human serum samples.

• We evaluated the relation between PBDE and OH-PBDE concentrations in human serum.

Electronic supplementary material

ESM 1

(DOCX 189 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Xu, B., Wu, M., Wang, M. et al. Polybrominated diphenyl ethers (PBDEs) and hydroxylated PBDEs in human serum from Shanghai, China: a study on their presence and correlations. Environ Sci Pollut Res 25, 3518–3526 (2018). https://doi.org/10.1007/s11356-017-0709-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-017-0709-4

Keywords

Search

Navigation