Urinary metabolites of organophosphate flame retardants: temporal variability and correlations with house dust concentrations

John D Meeker, Ellen M Cooper, Heather M Stapleton, Russ Hauser, John D Meeker, Ellen M Cooper, Heather M Stapleton, Russ Hauser

Abstract

Background: A reduction in the use of polybrominated diphenyl ethers (PBDEs) because of human health concerns may result in an increased use of and human exposure to organophosphate flame retardants (OPFRs). Human exposure and health studies of OPFRs are lacking.

Objectives: We sought to define the degree of temporal variability in urinary OPFR metabolites in order to inform epidemiologic study design, and to explore a potential primary source of exposure by examining the relationship between OPFRs in house dust and their metabolites in urine.

Methods: Nine repeated urine samples were collected from 7 men over the course of 3 months and analyzed for bis(1,3-dichloro-2-propyl) phosphate (BDCPP) and diphenyl phosphate (DPP), metabolites of the OPFRs tris(1,3-dichloro-2-propyl) phosphate (TDCPP) and triphenyl phosphate (TPP), respectively. Intraclass correlation coefficients (ICCs) were calculated to characterize temporal reliability. Paired house dust and urine samples were collected from 45 men.

Results: BDCPP was detected in 91% of urine samples, and DPP in 96%. Urinary BDCPP showed moderate-to-strong temporal reliability (ICC range, 0.55-0.72). ICCs for DPP were lower, but moderately reliable (range, 0.35-0.51). There was a weak [Spearman r (r(S)) = 0.31] but significant (p = 0.03) correlation between urinary BDCPP and TDCPP concentrations in house dust that strengthened when nondetects (r(S) = 0.47) were excluded. There was no correlation between uncorrected DPP and TPP measured in house dust (r(S) < 0.1).

Conclusions: Household dust may be an important source of exposure to TDCPP but not TPP. Urinary concentrations of BDCPP and DPP were moderately to highly reliable within individuals over 3 months.

Conflict of interest statement

The authors declare they have no actual or potential competing financial interests.

Figures

Figure 1
Figure 1
Concentrations (ng/mL) in urine from repeated samples collected from seven men over a 3-month period. (A) BDCPP; (B) DPP. Colors represent individual men.
Figure 2
Figure 2
Relationship between house dust OPFR concentrations (ng/g of dust) and uncorrected urinary metabolite concentrations (ng/mL) for 45 study participants with paired samples. (A) TDCPP and BDCPP (rS = 0.31, p = 0.03). (B) TPP and DPP (rS = 0.04, p = 0.8).

References

    1. Birnbaum LS, Bergman Å. Brominated and chlorinated flame retardants: the San Antonio Statement. Environ Health Perspect. 2010;118:A514–A515. [Editorial]
    1. Boeniger MF, Lowry LK, Rosenberg J. Interpretation of urine results used to assess chemical exposure with emphasis on creatinine adjustments: a review. Am Ind Hyg Assoc J. 1993;54(10):615–627.
    1. Cooper EM, Covaci A, van Nuijs AL, Webster TF, Stapleton HM. Analysis of the flame retardant metabolites bis(1,3-dichloro-2-propyl) phosphate (BDCPP) and diphenyl phosphate (DPP) in urine using liquid chromatography–tandem mass spectrometry. Anal Bioanal Chem. 2011;401(7):2123–2132.
    1. Cooper EM, Stapleton HM. Metabolism of organophosphate flame retardants by human liver microsomes and porcine esterase [Abstract]. In: Proceedings of the Society of Environmental Toxicology and Chemistry (SETAC) North America 32nd Annual Meeting, November 13–17, 2011. Abstract MP010. Boston, MA. [Abstract]. 2012. Available: (accessed 2 August 2012)
    1. DiGangi J, Blum A, Bergman Å, de Wit CA, Lucas D, Mortimer D, et al. San Antonio Statement on brominated and chlorinated flame retardants. Environ Health Perspect. 2010;118:A516–A518.
    1. Dishaw LV, Powers CM, Ryde IT, Roberts SC, Seidler FJ, Slotkin TA, et al. Is the PentaBDE replacement, tris (1,3-dichloro-2-propyl) phosphate (TDCPP), a developmental neurotoxicant? Studies in PC12 cells. Toxicol Appl Pharmacol. 2011;256(3):281–289.
    1. Hankinson SE, Manson JE, Spiegelman D, Willett WC, Longcop C, Speizer FE. Reproducibility of plasma hormone levels in post-menopausal women over a 2–3 year period. Cancer Epidemiol Biomarkers Prev. 1995;4:649–654.
    1. Hauser R, Meeker JD, Park S, Silva MJ, Calafat AM. Temporal variability of urinary phthalate metabolite levels in men of reproductive age. Environ Health Perspect. 2004;112:1734–1740.
    1. Johnson PI, Stapleton HM, Sjödin A, Meeker JD. Relationships between polybrominated diphenyl ether concentrations in house dust and serum. Environ Sci Technol. 2010;44(14):5627–5632.
    1. Lynn RK, Wong K, Garvie-Gould C, Kennish JM. Disposition of the flame retardant, tris(1,3-dichloro-2-propyl) phosphate, in the rat. Drug Metab Dispos. 1981;9(5):434–441.
    1. Mahalingaiah S, Meeker JD, Pearson KR, Calafat AM, Ye X, Petrozza J, et al. Temporal variability and predictors of urinary bisphenol A concentrations in men and women. Environ Health Perspect. 2008;116:173–178.
    1. Makiguchi K, Satoh T, Kakuchi T. Diphenyl phosphate as an efficient cationic organocatalyst for controlled/living ring-opening polymerization of delta-valerolactone and epsilon-caprolactone. Macromolecules. 2011;44(7):1999–2005.
    1. Meeker JD, Barr DB, Ryan L, Herrick RF, Bennett DH, Bravo R, et al. Temporal variability of urinary levels of nonpersistent insecticides in adult men. J Expo Anal Environ Epidemiol. 2005;15(3):271–281.
    1. Meeker JD, Godfrey-Bailey L, Hauser R. Relationships between serum hormone levels and semen quality among men from an infertility clinic. J Androl. 2007;28(3):397–406.
    1. Meeker JD, Stapleton HM. House dust concentrations of organophosphate flame retardants in relation to hormone levels and semen quality parameters. Environ Health Perspect. 2010;118:318–323.
    1. Nomeir AA, Kato S, Matthews HB. The metabolism and disposition of tris(1,3-dichloro-2-propyl) phosphate (Fyrol FR-2) in the rat. Toxicol Appl Pharmacol. 1981;57(3):401–413.
    1. Rosner B. 2000. Fundamentals of Biostatistics. 5th ed. Pacific Grove, CA:Duxbury Press.
    1. Sasaki K, Suzuki T, Takeda M, Uchiyama M. Metabolism of phosphoric acid triesters by rat liver homogenate. Bull Environ Contam Toxicol. 1984;33(3):281–288.
    1. Shaw SD, Blum A, Weber R, Kannan K, Rich D, Lucas D, et al. Halogenated flame retardants: Do the fire safety benefits justify the risks? Rev Environ Health. 2010;25(4):261–305.
    1. Stapleton HM, Eagle S, Sjödin A, Webster TF. Serum PBDEs in a North Carolina toddler cohort: associations with handwipes, house dust, and socioeconomic variables. Environ Health Perspect. 2012;120:1049–1054.
    1. Stapleton HM, Klosterhaus S, Eagle S, Fuh J, Meeker JD, Blum A, et al. Detection of organophosphate flame retardants in furniture foam and U.S. house dust. Environ Sci Technol. 2009;43(19):7490–7495.
    1. Stapleton HM, Klosterhaus S, Keller A, Ferguson PL, van Bergen S, Cooper E, et al. Identification of flame retardants in polyurethane foam collected from baby products. Environ Sci Technol. 2011;45(12):5323–5331.
    1. U.S. Environmental Protection Agency. Furniture Flame Retardancy Partnership: Environmental Profiles of Chemical Flame-Retardant Alternatives for Low-Density Polyurethane Foam. Chemical Hazard Reviews, Vol. 2. Washington, DC:U.S. EPA. 2005. Available: [accessed 22 March 2013]
    1. Van den Eede N, Dirtu AC, Neels H, Covaci A. Analytical developments and preliminary assessment of human exposure to organophosphate flame retardants from indoor dust. Environ Int. 2011;37(2):454–461.
    1. van der Veen I, de Boer J. Phosphorus flame retardants: properties, production, environmental occurrence, toxicity and analysis. Chemosphere. 2012;88(10):1119–1153.
    1. Watkins DJ, McClean MD, Fraser AJ, Weinberg J, Stapleton HM, Sjödin A, et al. Impact of dust from multiple microenvironments and diet on pentaBDE body burden. Environ Sci Technol. 2012;46(2):1192–1200.

Source: PubMed

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