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Multi-analyte method development for analysis of brominated flame retardants (BFRs) and PBDE metabolites in human serum

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Abstract

Commonly, analytical methods measuring brominated flame retardants (BFRs) of different chemical polarities in human serum are labor consuming and tedious. Our study used acidified diatomaceous earth as solid-phase extraction (SPE) adsorbent and defatting material to simultaneously determine the most abundant BFRs and their metabolites with different polarities in human serum samples. The analytes include three types of commercial BFRs, tetrabromobisphenol A (TBBPA), hexabromocyclododecane (HBCD) isomers, and polybrominated biphenyl ethers (PBDEs), and dominant hydroxylated BDE (OH-PBDE) and methoxylated BDE (MeO-PBDE) metabolites of PBDEs. The sample eluents were sequentially analyzed for PBDEs and MeO-BDEs on online gel permeation chromatography/gas chromatography-electron capture-negative ionization mass spectrometry (online GPC GC-ECNI-MS) and for TBBPA, HBCD, and OH-BDEs on liquid chromatography-tandem mass spectrometry (LC-MS/MS). Method recoveries were 67–134% with a relative standard deviation (RSD) of less than 20%. Method detection limits (MDLs) were 0.30–4.20 pg/mL fresh weight (f.w.) for all analytes, except for BDE-209 of 16 pg/mL f.w. The methodology was also applied in a pilot study, which analyzed ten real samples from healthy donors in China, and the majority of target analytes were detected with a detection rate of more than 80%. To our knowledge, it is the first time for us in effectively determining BFRs of most types in one aliquot of human serum samples. This new analytical method is more specific, sensitive, accurate, and time saving for routine biomonitoring of these BFRs and for integrated assessment of health risk of BFR exposure.

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Acknowledgments

Our study was supported by Shanghai Municipal Key Discipline of Public Health (No. 15GWZK0301), Shanghai Municipal Overseas High-End Talent Training (No. GWTD2015S03), Research Grand Award (No. 201540210, Shanghai Municipal Commission of Health and Family Planning, China), Fourth Three-Year Action Plan of System Establishment of Shanghai Municipal Public Health (2016–2018), and National Key Scientific Instrument and Equipment Development Projects (2013YQ150557).

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  1. Dasheng Lu and Yu’e Jin contributed equally to this work

Authors and Affiliations

  1. Shanghai Municipal Center for Disease Control and Prevention, 1380 Zhongshan West Road, Shanghai, 200336, China

    Dasheng Lu, Yu’e Jin, Chao Feng, Yuanjie Lin, Xinlei Qiu, Qian Xu, Yimin Wen & Guoquan Wang

  2. School of Public Health/MOE Key Lab for Public Health, Fudan University, Shanghai, 200032, China

    Dasheng Lu & Zhijun Zhou

  3. California Department of Public Health, Richmond, CA, 94804, USA

    Dongli Wang & Jianwen She

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  1. Dasheng Lu
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Correspondence to Guoquan Wang or Zhijun Zhou.

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The study has been approved by the ethics committee and have been performed in accordance with the institutional guidelines for using animals in the study.

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Lu, D., Jin, Y., Feng, C. et al. Multi-analyte method development for analysis of brominated flame retardants (BFRs) and PBDE metabolites in human serum. Anal Bioanal Chem 409, 5307–5317 (2017). https://doi.org/10.1007/s00216-017-0476-6

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