Maria Ospina1, Nayana K Jayatilaka2, Lee-Yang Wong2, Paula Restrepo2, Antonia M Calafat2. 1. Division of Laboratory Sciences, National Center for Environmental Health, Centers for Disease Control and Prevention, 4770 Buford Hwy, MS F17, Atlanta, GA 30341, USA. Electronic address: meo3@cdc.gov. 2. Division of Laboratory Sciences, National Center for Environmental Health, Centers for Disease Control and Prevention, 4770 Buford Hwy, MS F17, Atlanta, GA 30341, USA.
Abstract
BACKGROUND: Use of organophosphate flame retardants (OPFRs) including tris(1,3-dichloro-2-propyl) phosphate, triphenyl phosphate, tris(1-chloro-2-propyl) phosphate, and tris-2-chloroethyl phosphate, in consumer products is on the rise because of the recent phase out of polybrominated diphenyl ether (PBDE) flame retardants. Some of these chemicals are also used as plasticizers or lubricants in many consumer products. OBJECTIVES: To assess human exposure to these chlorinated and non-chlorinated organophosphates, and non-PBDE brominated chemicals in a representative sample of the U.S. general population 6years and older from the 2013-2014 National Health and Nutrition Examination Survey (NHANES). METHODS: We used solid-phase extraction coupled to isotope dilution high-performance liquid chromatography-tandem mass spectrometry after enzymatic hydrolysis of conjugates to analyze 2666 NHANES urine samples for nine biomarkers: diphenyl phosphate (DPHP), bis(1,3-dichloro-2-propyl) phosphate (BDCIPP), bis-(1-chloro-2-propyl) phosphate (BCIPP), bis-2-chloroethyl phosphate (BCEP), di-n-butyl phosphate (DNBP), di-p-cresylphosphate (DpCP), di-o-cresylphosphate (DoCP), dibenzyl phosphate (DBzP), and 2,3,4,5-tetrabromobenzoic acid (TBBA). We calculated the geometric mean (GM) and distribution percentiles for the urinary concentrations (both in micrograms per liter [μg/L] and in micrograms per gram of creatinine). We only calculated GMs for analytes with an overall weighted frequency of detection >60%. For those analytes, we also a) determined weighted Pearson correlations among the log10-transformed concentrations, and b) used regression models to evaluate associations of various demographic parameters with urinary concentrations of these biomarkers. RESULTS: We detected BDCIPP and DPHP in approximately 92% of study participants, BCEP in 89%, DNBP in 81%, and BCIPP in 61%. By contrast, we detected the other biomarkers much less frequently: DpCP (13%), DoCP (0.1%), TBBA (5%), and did not detect DBzP in any of the participants. Concentration ranges were highest for DPHP (<0.16-193μg/L), BDCIPP (<0.11-169μg/L), and BCEP (<0.08-110μg/L). Regardless of race/ethnicity, 6-11year old children had significantly higher BCEP adjusted GMs than other age groups. Females had significantly higher DPHP and BDCIPP adjusted GM than males, and were more likely than males to have DPHP concentrations above the 95th percentile (odds ratio=3.61; 95% confidence interval, 2.01-6.48). CONCLUSIONS: Our results confirm findings from previous studies suggesting human exposure to OPFRs, and demonstrate, for the first time, widespread exposure to several OPFRs among a representative sample of the U.S. general population 6years of age and older. The observed differences in concentrations of certain OPFRs biomarkers by race/ethnicity, in children compared to other age groups, and in females compared to males may reflect differences in lifestyle and exposure patterns. These NHANES data can be used to stablish a nationally representative baseline of exposures to OPFRs and when combined with future 2-year survey data, to evaluate exposure trends. Published by Elsevier Ltd.
BACKGROUND: Use of organophosphateflame retardants (OPFRs) including tris(1,3-dichloro-2-propyl) phosphate, triphenyl phosphate, tris(1-chloro-2-propyl) phosphate, and tris-2-chloroethyl phosphate, in consumer products is on the rise because of the recent phase out of polybrominated diphenyl ether (PBDE) flame retardants. Some of these chemicals are also used as plasticizers or lubricants in many consumer products. OBJECTIVES: To assess human exposure to these chlorinated and non-chlorinated organophosphates, and non-PBDE brominated chemicals in a representative sample of the U.S. general population 6years and older from the 2013-2014 National Health and Nutrition Examination Survey (NHANES). METHODS: We used solid-phase extraction coupled to isotope dilution high-performance liquid chromatography-tandem mass spectrometry after enzymatic hydrolysis of conjugates to analyze 2666 NHANES urine samples for nine biomarkers: diphenyl phosphate (DPHP), bis(1,3-dichloro-2-propyl) phosphate (BDCIPP), bis-(1-chloro-2-propyl) phosphate (BCIPP), bis-2-chloroethyl phosphate (BCEP), di-n-butyl phosphate (DNBP), di-p-cresylphosphate (DpCP), di-o-cresylphosphate (DoCP), dibenzyl phosphate (DBzP), and 2,3,4,5-tetrabromobenzoic acid (TBBA). We calculated the geometric mean (GM) and distribution percentiles for the urinary concentrations (both in micrograms per liter [μg/L] and in micrograms per gram of creatinine). We only calculated GMs for analytes with an overall weighted frequency of detection >60%. For those analytes, we also a) determined weighted Pearson correlations among the log10-transformed concentrations, and b) used regression models to evaluate associations of various demographic parameters with urinary concentrations of these biomarkers. RESULTS: We detected BDCIPP and DPHP in approximately 92% of study participants, BCEP in 89%, DNBP in 81%, and BCIPP in 61%. By contrast, we detected the other biomarkers much less frequently: DpCP (13%), DoCP (0.1%), TBBA (5%), and did not detect DBzP in any of the participants. Concentration ranges were highest for DPHP (<0.16-193μg/L), BDCIPP (<0.11-169μg/L), and BCEP (<0.08-110μg/L). Regardless of race/ethnicity, 6-11year old children had significantly higher BCEP adjusted GMs than other age groups. Females had significantly higher DPHP and BDCIPP adjusted GM than males, and were more likely than males to have DPHP concentrations above the 95th percentile (odds ratio=3.61; 95% confidence interval, 2.01-6.48). CONCLUSIONS: Our results confirm findings from previous studies suggesting human exposure to OPFRs, and demonstrate, for the first time, widespread exposure to several OPFRs among a representative sample of the U.S. general population 6years of age and older. The observed differences in concentrations of certain OPFRs biomarkers by race/ethnicity, in children compared to other age groups, and in females compared to males may reflect differences in lifestyle and exposure patterns. These NHANES data can be used to stablish a nationally representative baseline of exposures to OPFRs and when combined with future 2-year survey data, to evaluate exposure trends. Published by Elsevier Ltd.
Authors: Nele Van den Eede; Gregg Tomy; Fang Tao; Thor Halldorson; Stuart Harrad; Hugo Neels; Adrian Covaci Journal: Chemosphere Date: 2015-10-23 Impact factor: 7.086
Authors: Kate Hoffman; Amelia Lorenzo; Craig M Butt; Linda Adair; Amy H Herring; Heather M Stapleton; Julie L Daniels Journal: Environ Int Date: 2016-10-13 Impact factor: 9.621
Authors: Nadeem Ali; Alin C Dirtu; Nele Van den Eede; Emma Goosey; Stuart Harrad; Hugo Neels; Andrea 't Mannetje; Jonathan Coakley; Jeroen Douwes; Adrian Covaci Journal: Chemosphere Date: 2012-04-30 Impact factor: 7.086
Authors: Courtney C Carignan; Michael D McClean; Ellen M Cooper; Deborah J Watkins; Alicia J Fraser; Wendy Heiger-Bernays; Heather M Stapleton; Thomas F Webster Journal: Environ Int Date: 2013-03-20 Impact factor: 9.621
Authors: Molly L Kile; Richard P Scott; Steven G O'Connell; Shannon Lipscomb; Megan MacDonald; Megan McClelland; Kim A Anderson Journal: Environ Res Date: 2016-03-03 Impact factor: 6.498
Authors: Heather M Stapleton; Smriti Sharma; Gordon Getzinger; P Lee Ferguson; Michelle Gabriel; Thomas F Webster; Arlene Blum Journal: Environ Sci Technol Date: 2012-11-28 Impact factor: 9.028
Authors: Kylie R Baldwin; Allison L Phillips; Brian Horman; Sheryl E Arambula; Meghan E Rebuli; Heather M Stapleton; Heather B Patisaul Journal: Sci Rep Date: 2017-08-02 Impact factor: 4.379
Authors: Brett T Doherty; Kate Hoffman; Alexander P Keil; Stephanie M Engel; Heather M Stapleton; Barbara D Goldman; Andrew F Olshan; Julie L Daniels Journal: Environ Res Date: 2018-10-30 Impact factor: 6.498
Authors: Subham Dasgupta; Vanessa Cheng; Sara M F Vliet; Constance A Mitchell; David C Volz Journal: Environ Sci Technol Date: 2018-09-10 Impact factor: 9.028
Authors: Arlene Blum; Mamta Behl; Linda Birnbaum; Miriam L Diamond; Allison Phillips; Veena Singla; Nisha S Sipes; Heather M Stapleton; Marta Venier Journal: Environ Sci Technol Lett Date: 2019-10-21
Authors: Cheryl Fairfield Estill; Jonathan Slone; Alexander C Mayer; Kaitlyn Phillips; John Lu; I-Chen Chen; Annette Christianson; Robert Streicher; Mark J La Guardia; Nayana Jayatilaka; Maria Ospina; Antonia M Calafat Journal: J Occup Environ Hyg Date: 2019-05-21 Impact factor: 2.155
Authors: Carolyn M Poutasse; Julie B Herbstman; Mark E Peterson; Jana Gordon; Peter H Soboroff; Darrell Holmes; Dezere Gonzalez; Lane G Tidwell; Kim A Anderson Journal: Environ Sci Technol Date: 2019-07-10 Impact factor: 9.028
Authors: Mary E Ingle; Deborah Watkins; Zaira Rosario; Carmen M Vélez Vega; Gredia Huerta-Montanez; Antonia M Calafat; Maria Ospina; José F Cordero; Akram Alshawabkeh; John D Meeker Journal: Environ Res Date: 2019-09-23 Impact factor: 6.498
Authors: Stephanie Kim; Nabil Rabhi; Benjamin C Blum; Ryan Hekman; Kieran Wynne; Andrew Emili; Stephen Farmer; Jennifer J Schlezinger Journal: Arch Toxicol Date: 2020-07-18 Impact factor: 5.153