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Contaminants in Aquatic and Terrestrial Environments

Flame Retardant Concentrations Are Lower in College Spaces Meeting the New Furniture Flammability Standard TB117-2013
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Environmental Science & Technology Letters

Cite this: Environ. Sci. Technol. Lett. 2020, 7, 11, 833–839
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https://doi.org/10.1021/acs.estlett.0c00483
Published September 3, 2020

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Abstract

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California’s updated furniture flammability standard, TB117-2013, can be met without the use of chemical flame retardants (FRs). FRs have been associated with neurological damage, reproductive toxicity, thyroid disease, and cancer. We collected dust from classrooms and other nonresidential spaces on four U.S. college campuses that met one of California’s two older FR-reliant standards (TB117, TB133) or the newer TB117-2013. We hypothesized that spaces with TB117-2013-compliant furniture would have lower levels of FRs in dust. We detected all 43 targeted FRs, and FRs were detected in each of the 86 samples. We prioritized 14 FRs for statistical analysis based on their prevalence in dust and use in furniture and textiles. Concentrations of three polybrominated diphenyl ethers (PBDEs), hexabromocyclododecane (HBCDD), and tris(2-chloroethyl) phosphate (TCEP) were significantly lower in TB117-2013 spaces compared to spaces adhering to FR-reliant standards. Concentrations of BDE 209, decabromodiphenylethane (DBDPE), bis(2-ethylhexyl)-3,4,5,6-tetrabromophthalate (BEH-TEBP), hexabromobenzene (HBB), and tetrabromobisphenol A (TBBPA) were significantly lower in spaces meeting TB117-2013 compared to TB133 spaces. We report the highest dust levels of BDE 209, 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (EH-TBB), DBDPE, and TCEP in the U.S. Spaces adhering to the revised standard, TB117-2013, had lower dust concentrations of harmful FRs, suggesting less FR was used in the furnishings.

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Introduction

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In 2013, California revised its primary furniture flammability standard, and it can be met without added flame retardant (FR) chemicals. (1) Previous research has demonstrated that dust concentrations of FRs are influenced by furniture flammability standards that rely on added FR chemicals. (2,3) Therefore, FR dust concentrations are expected to be lower in spaces with furniture adhering to the updated standard.
California’s furniture flammability standards are de facto national standards in the U.S. Prior to 2013, FR chemicals were added to foam in upholstered furniture to meet a California performance-based standard known as Technical Bulletin 117 (TB117). (4) California’s revision of TB117, called TB117-2013, does not rely on added FRs, although it does not preclude their use. The new standard was phased in during 2014 and applied to all residential furniture sold in California starting January 1, 2015. As a result, it is possible for spaces furnished in 2014 and later in California, and therefore most other places in the U.S., to contain furniture meeting TB117-2013. Some places that reference California standards later changed their fire codes to reflect the update. (5,6) Research has found that FR levels were higher in Californians’ blood and house dust compared to levels found in other states, presumably due to California’s earlier and longer enforcement of TB117. (3)
Separately, in 2019, California repealed an outdated and more severe standard called Technical Bulletin 133 (TB133) that applied to furniture in public spaces, (7) which was met with high levels of FRs. (2,8) We previously showed that some FR dust concentrations were higher in college dormitories that met TB133 compared to dormitories that met TB117. (2)
Fire safety scientists have questioned the efficacy of FR use in furniture, and research has shown significant health risks associated with FR exposures. (8−10) Certain polybrominated diphenyl ethers (PBDEs), BDE 47 in particular, alter neurodevelopment in children, leading to decreased IQ. (11,12) They were also found to be associated with higher risk of thyroid disease among women, with stronger effects in postmenopausal women. (13) Studies have found many halogenated organophosphate flame retardants (OPFRs) to be neurotoxic, toxic to development and reproduction, and carcinogenic. (14) Tris(1,3-dichloro-isopropyl) phosphate (TDCIPP) was removed from children’s pajamas in 1978 because it is mutagenic, (15,16) but it remained in wide use, alongside other chlorinated OPFRs, such as tris(2-chloroethyl) phosphate (TCEP), which has carcinogenicity concerns. (17) Hexabromocyclododecane (HBCDD), which was widely used in extruded polystyrene insulation, is considered persistent, bioaccumulative, and toxic (PBT). (18)
We sought to evaluate whether FR concentrations are lower in spaces with furniture complying with the newer standard (TB117-2013) compared to the older standards (TB117 and TB133). We used data collected from nonresidential spaces on college campuses as these spaces are institutionally managed, minimizing variability in the standards used in the space, and typically densely furnished, increasing the FR load. We compared FR concentrations in dust samples collected from classrooms and lecture halls from four U.S. colleges in New England that adhere to TB117, TB133, and TB117-2013, adjusting for room characteristics (e.g., carpeting, number of upholstered furniture pieces). We also evaluated the FR composition of the dust. Previous work on FRs associated with TB117-2013 found that daycares that replaced TB117 nap mats with TB117-2013 nap mats had reductions of dust levels of bis(2-ethylhexyl)-3,4,5,6-tetrabromophthalate (BEH-TEBP), 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (EH-TBB), tris(4-butylphenyl) phosphate (TBPP), and TDCIPP. (19) This study is the first evaluation of the impact of TB117-2013 furniture on FR concentrations in dust.

Materials and Methods

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Dust Sample Collection

Dust samples were collected from nonresidential spaces from four U.S. colleges in New England. Samples (n = 86) were collected from campuses in Spring 2015, Spring 2016, and Spring 2018. The temporal gap was due to difficulty identifying TB117-2013 spaces. We included a subset of samples (n = 27) from our previous analysis of FRs in college dormitories that were from nonresidential spaces. We collected a total of 86 dust samples from 43 TB133 spaces, 27 TB117 spaces, and 16 TB117-2013 spaces.
Dust was collected using previously published protocols by trained field staff using vacuum cleaners (Dyson, Inc., Chicago, IL) fitted with a custom aluminum crevice tool holding cellulose extraction thimbles (19 mm × 90 mm). (2,20,21) In each space, staff lightly dragged the crevice tool over all room surfaces, including floors, furniture, desks, and window sills, for approximately 30 min to collect dust in thimbles, which were stored in certified glass jars (Environmental Sampling Supply, Dallas, TX) at less than 4 °C prior to shipment to the analytical laboratory.

Dust Sample Analysis

Chemical analysis targeted 43 chemicals, including 12 PBDE congeners, 19 other BFRs, 10 OPFRs, Dechlorane Plus (DP) isomers, and hexabromocyclododecane (HBCDD) isomers (Table S1). Prior to chemical analysis, samples were sieved (<150 μm), weighed, and repackaged for shipment by Southwest Research Institute. Samples were analyzed in three different years, within months of collection.
Analysis comprised two sample preparation methods with three extracts per sample to target a range of FRs with different physicochemical properties. Briefly, samples were fractionated and either analyzed by gas chromatography–electron capture negative ion mass spectrometry (GC–ECNI/MS) and GC–electron impact (EI)/MS or by LC–MS/MS. More details about sample preparation and analysis can be found in Dodson et al. (2) and in the Supporting Information.

Quality Assurance/Quality Control

We used several QA/QC measures to evaluate the accuracy and precision of our measurements and comparability between the data sets. Field or procedural blanks were analyzed in each batch. Results were blank-corrected by subtracting mean blank values from the raw FR values in the samples. Method limits of quantification (LOQs) were calculated as three times the standard deviation of procedural blank values divided by the amount of dust used for analysis. For compounds not detected in blanks, the LOQ was calculated based on a signal-to-noise ratio of 10:1. We replaced nondetect values with the limit of detection (LOD)*detection frequency for the chemical. See Supporting Information for additional details.
We evaluated accuracy using standard reference material (SRM) 2585 (Organic Contaminants in House Dust). For all analytes included in statistical analyses, the average relative difference was less than 27% from the SRM2585 certified or indicative values (Figure SI1). We used SRM and field sample replicates to evaluate precision. Precision for SRM2585 replicates (n = 10) was within 30% for all analytes included in statistical analyses. One field sample from 2018 was split into triplicate samples, and precision was within 24% for analytes included in our analyses, except with higher values for decabromodiphenylethane (DBDPE), BDE 209, tetrabromobisphenol A (TBBPA), BDE 47, and TDCIPP (Table S1).

Additional Data Collection

Trained staff conducted visual inspections of sampling spaces, noting the number, type, and condition of upholstered furniture, flammability standard labels, and carpeting. We solicited information about the furnishings in the sampled spaces from campus administrators.

Data Analysis

We summarized concentrations by flammability standard using descriptive statistics. We prioritized 14 FRs (4 PBDEs, 6 brominated compounds, 3 chlorinated OPFRs, and one nonhalogenated OPFR) for statistical analyses based on their prevalence in this study (detected above the LOQ in at least 60% of samples) and previous research indicating their use in furniture and/or textiles. (22,23) Flame retardant uses in furniture and other products are summarized in Figure SI2.
To compare concentrations across spaces meeting different furniture flammability standards, we estimated linear regression models. To meet the normality assumption, we used natural log-transformed concentrations as the outcome. Our baseline model included dummy variables for TB133 and TB117 (with TB117-2013 the reference group) as explanatory variables. Separately, we ran adjusted models to increase the precision of our estimates, which included covariates assumed to be independently associated with the outcome: carpeting in at least half the room (dichotomous: yes/no) and number of upholstered furniture pieces. Information on carpeting was missing from 17 spaces and on upholstered furniture from 10 spaces (19 spaces missing data out of 86). Observations from these spaces were dropped from the adjusted models. To evaluate the effect of FR levels and standards in rooms furnished before 2005, when PentaBDE was phased out, we stratified our adjusted analysis by spaces furnished after 2004, noting that TB117-2013 spaces were never furnished before 2005. For all three models, significance was determined at alpha = 0.05.
We compared the composition of priority FRs in dust across flammability standards. Because different FRs are likely used (or not used) to meet different standards, we expected the FR composition in dust to vary. Using geometric mean (GM) concentrations, we calculated the proportion of each FR to the total concentration (sum of all GMs). We tested for differences in proportions by standard using a three-sample test for equality of proportions.
Analyses were conducted in R (version 3.6.3; R Development Core Team).

Results and Discussion

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Dust Concentrations

We detected all 43 measured FRs (Table SI1). PBDEs were found consistently (detection frequencies: >60% for all). Of the PBDEs, BDE 209 had the highest concentrations, with a maximum of 3,500,000 ng/g (or 3.5 mg/g) and median of 2400 ng/g. The brominated FRs in Firemaster550, a replacement mixture for PentaBDE, were found in nearly all samples along with DBDPE, used in similar applications as DecaBDE. OPFRs were found at the highest levels compared to other FR groups, with tris(2-butoxyethyl) phosphate (TBOEP) found at the highest median concentration of all FRs at 59,000 ng/g. Concentration distributions for all FRs were highly right skewed, with maxima up to 3000 times higher than the median (TCEP).
Median levels of priority FR concentrations were similar to our previous analysis of dormitories. (2) Previously, we reported the highest dust concentrations of several FRs. Maximum concentrations of BDE 209, EH-TBB, DBDPE, TCEP, and TDCIPP were even higher in the current study. To our knowledge, these maxima, except for TDCIPP, are the highest levels measured in indoor dust in the U.S. Comparisons to literature values are listed in Table SI2.

Influence of Flammability Standards on Dust Concentrations

Most PBDE concentrations, including BDE 47 and BDE 99 (used in PentaBDE) and BDE 183 (used in OctaBDE), were significantly higher in TB133 and TB117 spaces compared to TB117-2013 spaces in the baseline model (Figure 1). PentaBDE and OctaBDE mixtures were used in furniture prior to their 2004 phase-out. (22,23) The persistent properties of PentaBDE and OctaBDE, or their presence in nonrenovated articles, may explain their high detection frequencies in TB117-2013 spaces. BDE 209 concentrations were significantly higher in TB133 spaces than TB117-2013 spaces. This is consistent with our previous study that observed higher BDE 209 levels in TB133 spaces than TB117 spaces. (2) BDE 209 was likely used in textile back-coatings in furniture to meet TB133, (24,25) and it was also used extensively in electronic casings. (26)

Figure 1

Figure 1. FR concentrations (ng/g) in spaces (n = 86) adhering to different furniture flammability standards. Estimated marginal means plotted as diamonds with color indicating statistically significant differences compared to TB117-2013 (baseline model). Nondetects are unfilled circles.

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Firemaster 550, which contains two brominated FRs, EH-TBB and BEH-TEBP, along with TPHP, was introduced in 2004 to replace PentaBDE and OctaBDE. (22,23) EH-TBB was significantly higher in TB117 spaces than TB117-2013 spaces. BEH-TEBP was used in other FR mixtures before the introduction of Firemaster 550, (27) possibly explaining its significantly higher levels in TB133 spaces compared to TB117-2013 spaces. We observed no significant differences in TPHP concentrations by standard, likely because of its diverse uses (Figure SI2).
Concentrations of brominated FRs HBB, TBBPA, and DBDPE were significantly higher in TB133 spaces than TB117-2013 spaces. DBDPE is a replacement for BDE 209, so its higher levels in TB133 spaces are not unexpected. TBBPA is a widely used and nonrestricted FR, primarily in reactive and polymeric forms, (14) while HBB is not widely used. However, dust levels may reflect past uses in TB133 spaces or different release rates of TBBPA used in reactive form.
HBCDD was significantly higher in TB133 and TB117 spaces than TB117-2013 spaces. We previously found significantly higher concentrations of HBCDD in dorm rooms meeting TB133 compared to TB117. HBCDD has been used in extruded polystyrene insulation boards, textiles, and electronics, (28,29) and its use has been declining since its listing on the Stockholm Convention in 2013. (18)
Among the chlorinated OPFRs, only TCEP concentrations were significantly different by standard. TCEP was significantly higher in TB133 spaces than TB117-2013 spaces. TDCIPP levels were nonsignificantly lower in TB117-2013 spaces. There were no significant differences for TCIPP by standard, perhaps because it has many other uses besides furniture, such as plastics, rubber, and textiles (Figure SI2).
In the adjusted models the findings were similar, except for TCEP. TCEP concentrations were significantly higher in TB117 spaces compared to TB117-2013 in the adjusted model but not the baseline model, although the direction of the association in both models was the same (Table SI2). The difference is likely due to consistently lower levels of TCEP in TB117 spaces missing carpet information, thus making the TB117 comparison group appear elevated in the adjusted model.

Influence of Flammability Standards on Dust Concentrations after 2004

When we stratified our analysis to include only spaces furnished after 2004, we still observed that TB117-2013 spaces had significantly lower FR levels for BDE 99, BDE 183, and TCEP compared to both TB133 and TB117 spaces (Table SI3). However, we no longer observed significantly lower FR levels between TB133 spaces furnished after 2004 compared to TB117-2013 spaces for BDE 47, BEH-TBEP, and DBDPE. Similarly, HBCDD concentrations were no longer significantly lower in TB117 spaces furnished after 2004 compared to TB117-2013 spaces. The smaller sample size (67 samples compared to 86) for the post-2004 furnished spaces likely reduced statistical power, causing some observations to become nonsignificant. BDE 209 concentrations were significantly higher in TB117 spaces furnished after 2004 than in TB117-2013 spaces. This could be due to an increase in BDE 209 use after 2004, before its scheduled phase-out in 2013 in the U.S. (30)

Dust Composition by Flammability Standard

The composition of FRs in dust varied by flammability standard (Figure 2). The proportion of PBDEs varied significantly by standard; PBDEs comprised approximately 36% of the FR concentrations of the dust in TB133 spaces, 17% of dust in TB117 spaces, and 6% of dust in TB117-2013 spaces. Because all TB117-2013 spaces were renovated after the PentaBDE phase-out, this is consistent with FR use trends. BDE 209 comprised nearly 89% of the PBDEs in TB133 spaces and 40% in TB117 spaces, consistent with its use in furniture to meet TB133. The proportion of chlorinated OPFRs was relatively consistent (38%–39%) in TB133 and TB117 spaces and slightly, yet significantly, lower in TB117-2013 spaces. Among chlorinated OPFRs, the proportion of TCIPP was highest in the TB117-2013 spaces (56%). The proportion of TPHP, a nonchlorinated OPFR, was significantly highest in TB117-2013 spaces. Both TCIPP and TPHP have other uses unrelated to furniture; one of the largest uses of TCIPP is in spray foam insulation. (31)

Figure 2

Figure 2. FR composition in spaces adhering to different furniture flammability standards. Proportions are GM of each chemical to sum of GMs for all chemicals (top bar graph).

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Limitations

This study evaluated the impact of TB117-2013 on a broad range of FRs in university settings in the U.S., making it one of the first studies to evaluate the effect of the new standard on exposures. Because our data set included only 16 dust samples from two campuses with TB117-2013 spaces, we are not able to generalize our findings to all TB117-2013 spaces, and the small sample size is a limitation of our study. We relied on communications with campus administrators to understand flammability standard adherence, though we did not have information on whether FRs were used in the TB117-2013 furniture. This may have created the possibility for misclassification of TB117-2013 spaces that may have had furniture with FRs. We did not have data on FRs or standards used in other components in each space, such as electronics or insulation, nor complete data on date of refurbishment of each space, cleaning practices, or age of the building, and these unaccounted-for factors may influence FR concentrations in the spaces.

Implications

This is the first study, to our knowledge, to demonstrate that FR dust concentrations are lower in spaces adhering to the newer furniture flammability standard TB117-2013. The lower dust concentrations of FRs in TB117-2013 spaces suggest those spaces confer lower body burdens and associated health effects to occupants, compared to TB117 and TB133 spaces. More generally, this study adds to evidence that furniture flammability standards affect FR exposures via dust. When flammability standards for consumer products are developed or updated, potential exposure to and toxicity of FRs that could be used to meet such standards should be evaluated. It is also important to highlight that nonchemical methods, such as automatic sprinklers, smoke detectors, smoking bans, and use of inherently less flammable materials are important contributors to fire safety.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.estlett.0c00483.

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Author Information

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  • Corresponding Author
  • Authors
    • Adrian Covaci - Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium;  Orcidhttp://orcid.org/0000-0003-0527-1136
    • Giulia Poma - Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium;  Orcidhttp://orcid.org/0000-0003-0597-2653
    • Kristin Knox - Silent Spring Institute, Suite 302, 320 Nevada Street, Newton, Massachusetts 20460, United States
    • Joseph G. Allen - Harvard T.H. Chan School of Public Health, Boston, Massachusetts 02215, United States;  Orcidhttp://orcid.org/0000-0003-2702-5550
    • Jose Cedeno-Laurent - Harvard T.H. Chan School of Public Health, Boston, Massachusetts 02215, United States
    • Ruthann A. Rudel - Silent Spring Institute, Suite 302, 320 Nevada Street, Newton, Massachusetts 20460, United States
    • Robin E. Dodson - Silent Spring Institute, Suite 302, 320 Nevada Street, Newton, Massachusetts 20460, United States;  Orcidhttp://orcid.org/0000-0001-7356-9511
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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This work was supported by the John Merck Fund, the Fine Fund, the Hoffman Program on Chemicals and Health, and charitable donations to Silent Spring Institute. We thank the participating colleges and M. Dashko, L. Swetschinski, L. Borth, and K. Vilardi for assistance with sampling and C. Christia for help with the sample analysis.

References

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This article references 31 other publications.

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    Dorman, D. C.; Chiu, W.; Hales, B. F.; Hauser, R.; Johnson, K. J.; Mantus, E.; Martel, S.; Robinson, K. A.; Rooney, A. A.; Rudel, R.; Sathyanarayana, S.; Schantz, S. L.; Waters, K. M. Polybrominated diphenyl ether (PBDE) neurotoxicity: a systematic review and meta-analysis of animal evidence. J. Toxicol. Environ. Health, Part B 2018, 21 (4), 269– 289,  DOI: 10.1080/10937404.2018.1514829
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    11
    Polybrominated diphenyl ether (PBDE) neurotoxicity: a systematic review and meta-analysis of animal evidence
    Dorman, David C.; Chiu, Weihsueh; Hales, Barbara F.; Hauser, Russ; Johnson, Kamin J.; Mantus, Ellen; Martel, Susan; Robinson, Karen A.; Rooney, Andrew A.; Rudel, Ruthann; Sathyanarayana, Sheela; Schantz, Susan L.; Waters, Katrina M.
    Journal of Toxicology and Environmental Health, Part B: Critical Reviews (2018), 21 (4), 269-289CODEN: JTECFR; ISSN:1093-7404. (Taylor & Francis, Inc.)
    A review. A recent systematic review (SR) and meta-anal. of human studies found an assocn. between prenatal serum polybrominated di-Ph ethers (PBDE) concns. and a decrease in the IQ of children. A SR of exptl. developmental animal PBDE-mediated neurotoxicity studies was performed in the present study. Outcomes assessed included measures related to learning, memory, and attention, which parallel the intelligence-related outcomes evaluated in the human studies SR. PubMed, Embase, and Toxline were searched for relevant exptl. non-human mammalian studies. Evaluation of risk of bias (RoB) and overall body of evidence followed guidance developed by the National Toxicol. Program. Animal studies using varying designs and outcomes were available for BDEs 47, 99, 153, 203, 206, and 209 and the tech. mixt. DE-71. Study reporting of methods and results was often incomplete leading to concerns regarding RoB. A meta-anal. of 6 Morris water maze studies showed evidence of a significant increase in last trial latency (effect size of 25.8 [CI, 20.3 to 31.2]) in PBDE-exposed animals with low heterogeneity. For most endpoints, there were unexplained inconsistencies across studies and no consistent evidence of a dose-response relationship. There is a "moderate" level of evidence that exposure to BDEs 47, 99, and 209 affects learning. For other PBDEs and other endpoints, the level of evidence was "low" or "very low". The meta-anal. led to stronger conclusions than that based upon a qual. review of the evidence. The SR also identified RoB concerns that might be remedied by better study reporting.
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  12. 12
    Lam, J.; Lanphear, B. P.; Bellinger, D.; Axelrad, D. A.; McPartland, J.; Sutton, P.; Davidson, L.; Daniels, N.; Sen, S.; Woodruff, T. J. Developmental PBDE Exposure and IQ/ADHD in Childhood: A Systematic Review and Meta-analysis. Environ. Health Perspect. 2017, 125 (8), 086001,  DOI: 10.1289/EHP1632
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    12
    Developmental PBDE Exposure and IQ/ADHD in Childhood: A Systematic Review and Meta-analysis
    Lam Juleen; Sutton Patrice; Daniels Natalyn; Woodruff Tracey J; Lanphear Bruce P; Bellinger David; Axelrad Daniel A; McPartland Jennifer; Davidson Lisette; Sen Saunak
    Environmental health perspectives (2017), 125 (8), 086001 ISSN:.
    BACKGROUND: In the United States, one in six children are affected by neurodevelopmental disorders, and polybrominated diphenyl ethers (PBDEs) in flame-retardant chemicals are measured ubiquitously in children. OBJECTIVE: We conducted a systematic a systematic review regarding developmental exposure to PBDEs and intelligence or Attention Deficit/Hyperactivity Disorder (ADHD) and attention-related behavioral conditions in humans. METHODS: We searched articles published up to 26 September 2016, and included original studies that quantified exposures to PBDEs incurred any time in proximity to conception or during in utero, perinatal, or childhood time periods. We evaluated the risk of bias of individual studies and the overall quality and strength of the evidence according to the Navigation Guide systematic review methodology. We established criteria in advance to identify studies that could be combined using random effects meta-analyses (DerSimonian-Laird method). RESULTS: Fifteen studies met the inclusion criteria; 10 studies met the criteria for intelligence and nine for attention-related problems. We rated studies generally with "low" to "probably low" risk of bias and rated the overall body of evidence as "moderate" quality with "sufficient" evidence for an association between Intelligence Quotient (IQ) and PBDEs. Our meta-analysis of four studies estimated a 10-fold increase (in other words, times 10) in PBDE exposure associated with a decrement of 3.70 IQ points (95% confidence interval: 0.83, 6.56). We concluded the body of evidence was of "moderate" quality for ADHD with "limited" evidence for an association with PBDEs, based on the heterogeneity of association estimates reported by a small number of studies and the fact that chance, bias, and confounding could not be ruled out with reasonable confidence. CONCLUSION: We concluded there was sufficient evidence supporting an association between developmental PBDE exposure and reduced IQ. Preventing developmental exposure to PBDEs could help prevent loss of human intelligence. https://doi.org/10.1289/EHP1632.
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  13. 13
    Allen, J. G.; Gale, S.; Zoeller, R. T.; Spengler, J. D.; Birnbaum, L.; McNeely, E. PBDE flame retardants, thyroid disease, and menopausal status in U.S. women. Environ. Health 2016, 15 (1), 60,  DOI: 10.1186/s12940-016-0141-0
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    13
    PBDE flame retardants, thyroid disease, and menopausal status in U.S. women
    Allen, Joseph G.; Gale, Sara; Zoeller, R. Thomas; Spengler, John D.; Birnbaum, Linda; McNeely, Eileen
    Environmental Health (London, United Kingdom) (2016), 15 (), 60/1-60/9CODEN: EHAGAB; ISSN:1476-069X. (BioMed Central Ltd.)
    Background: Women have elevated rates of thyroid disease compared to men. Environmental toxicants have been implicated as contributors to this dimorphism, including polybrominated di-Ph ethers (PBDEs), flame retardant chems. that disrupt thyroid hormone action. PBDEs have also been implicated in the disruption of estrogenic activity, and estrogen levels regulate thyroid hormones. Post-menopausal women may therefore be particularly vulnerable to PBDE induced thyroid effects, given low estrogen reserves. The objective of this study was to test for an assocn. between serum PBDE concns. and thyroid disease in women from the United States (U.S.), stratified by menopause status. Methods: Serum PBDE concns. (BDEs 47, 99, 100 and 153) from the National Health and Examn. Survey (NHANES) and reports on thyroid problems were available in the NHANES 2003-2004 cycle. Odds ratios (ORs) were calcd. using multivariate logistic regression models accounting for population-weighted survey techniques and controlling for age, body mass index (BMI), education, smoking, alc. consumption and thyroid medication. Menopause status was obtained by self-reported absence of menstruation in the previous 12 mo and declared menopause. Results: Women in the highest quartile of serum concns. for BDEs 47, 99, and 100 had increased odds of currently having thyroid disease (ORs: 1.5, 1.8, 1.5, resp.) compared to the ref. group (1st and 2nd quartiles combined); stronger assocns. were obsd. when the anal. was restricted to postmenopausal women (ORs: 2.2, 3.6, 2.0, resp.). Conclusion: Exposure to BDEs 47, 99, and 100 is assocd. with thyroid disease in a national sample of U.S. women, with greater effects obsd. post-menopause, suggesting that the disruption of thyroid signaling by PBDEs may be enhanced by the altered estrogen levels during menopause.
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  14. 14
    Blum, A.; Behl, M.; Birnbaum, L. S.; Diamond, M. L.; Phillips, A.; Singla, V.; Sipes, N. S.; Stapleton, H. M.; Venier, M. Organophosphate Ester Flame Retardants: Are They a Regrettable Substitution for Polybrominated Diphenyl Ethers?. Environ. Sci. Technol. Lett. 2019, 6 (11), 638– 649,  DOI: 10.1021/acs.estlett.9b00582
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    14
    Organophosphate Ester Flame Retardants: Are They a Regrettable Substitution for Polybrominated Diphenyl Ethers?
    Blum, Arlene; Behl, Mamta; Birnbaum, Linda S.; Diamond, Miriam L.; Phillips, Allison; Singla, Veena; Sipes, Nisha S.; Stapleton, Heather M.; Venier, Marta
    Environmental Science & Technology Letters (2019), 6 (11), 638-649CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
    A review to det. whether organophosphate ester flame retardants (OPFR) are a better choice (better alternative) than polybrominated di-Ph ether flame retardants (PBDE) by comparing the two over a range of properties is given. OPFR exposure is ubiquitous to humans and indoor/outdoor; they now often occur at higher concns. than PBDE peak exposure concns. Toxicity testing, epidemiol. study, and risk assessment data all suggest there are health concerns at current exposure levels for halogenated and non-halogenated OPFR. With the large no. of OPFR in use, producers can move toward healthier, safer products by developing innovative ways to reduce fire risks for electronics enclosures, upholstered furniture, building materials, and other consumer products with no added flame retardants. Topics discussed include: introduction; environmental behavior; indoor behavior and human exposure; toxicity and health effects; epidemiol. evidence; looking forward; supporting information (plasma bio-equiv. using high through-put toxicokinetic modeling).
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  15. 15
    Gold, M. D.; Blum, A.; Ames, B. N. Another flame retardant, tris-(1,3-dichloro-2-propyl)-phosphate, and its expected metabolites are mutagens. Science 1978, 200 (4343), 785– 7,  DOI: 10.1126/science.347576
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    15
    Another flame retardant, tris-(1,3-dichloro-2-propyl)phosphate, and its expected metabolites are mutagens
    Gold, Marian Deborah; Blum, Arlene; Ames, Bruce N.
    Science (Washington, DC, United States) (1978), 200 (4343), 785-7CODEN: SCIEAS; ISSN:0036-8075.
    The flame retardant tris(1,3-dichloro-2-propyl) phosphate (Fyrol FR2) [13674-87-8] was a mutagen in the Salmonella-mammalian tissue homogenate tests after it was activated by mouse or rat liver homogenate. The expected enzymic hydrolysis product, 1,3-dichloro-2-propanol [96-23-1] was similarly a mutagen after activation by liver homogenate. A proposed metabolite of the flame retardant, 1,3-dichloro-2-propanone [534-07-6] was a potent mutagen in the absence of such activation. A flame retardant with a similar structure, tris(2,3-dibromopropyl) phosphate (tris-BP), was shown previously to be a mutagen, to cause sterility in animals, to be a carcinogen, and to be absorbed through human skin. These and other flame retardants have characteristic nuclear magnetic resonance spectra that can be used to det. which flame retardant is present in com. purchased sleepwear. Sleepwear treated with tris-BP, Fyrol FR2, and other chem. additives was being sold in late 1977.
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  16. 16
    Sanders, H. J. Flame Retardants: Government Regulations and Public Emphasis on Safety Provide the Impetus for an Expanding industry. Chem. Eng. News 1978, 56 (17), 22– 36,  DOI: 10.1021/cen-v056n017.p022
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  17. 17
    Chemicals Considered or Listed Under Proposition 65: Tris(2-chloroethyl) Phosphate. https://oehha.ca.gov/proposition-65/chemicals/tris2-chloroethyl-phosphate (accessed July 23, 2020).
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    The New POPs under the Stockholm Convention. http://chm.pops.int/TheConvention/ThePOPs/TheNewPOPs/tabid/2511/Default.aspx (accessed July 23, 2020),.
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  19. 19
    Stubbings, W. A.; Schreder, E. D.; Thomas, M. B.; Romanak, K.; Venier, M.; Salamova, A. Exposure to brominated and organophosphate ester flame retardants in U.S. childcare environments: Effect of removal of flame-retarded nap mats on indoor levels. Environ. Pollut. 2018, 238, 1056– 1068,  DOI: 10.1016/j.envpol.2018.03.083
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    19
    Exposure to brominated and organophosphate ester flame retardants in U.S. childcare environments: Effect of removal of flame-retarded nap mats on indoor levels
    Stubbings, W. A.; Schreder, E. D.; Thomas, M. B.; Romanak, K.; Venier, M.; Salamova, A.
    Environmental Pollution (Oxford, United Kingdom) (2018), 238 (), 1056-1068CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
    We assessed exposure to 39 brominated and 16 organophosphate ester flame retardants (FRs) from both dust and indoor air at seven childcare centers in Seattle, USA, and investigated the importance of nap mats as a source of these chems. Many childcare centers serving young children use polyurethane foam mats for the childrens naptime. Until recently, the vast majority of these mats sold in the United States contained flame-retarded polyurethane foam to meet California Tech. Bulletin 117 (TB117) requirements. With the 2013 update of TB117, allowing manufacturers to meet flammability stds. without adding FRs to filling materials, FR-free nap mats have become widely available. We conducted an intervention study by actively switching out FR-treated nap mats with FR-free nap mats and measuring FR levels in indoor air and dust before and after the switch-out. The predominant FRs found in dust and indoor air were 2-ethylhexyl tetrabromobenzoate (EHTBB) and tris(1-chloro-2-propyl) phosphate (TCIPP), resp. Nap mat samples analyzed from four of the six centers contained a Firemaster mixt., while one mat was predominantly treated with tris(1,3-dichloroisopropyl) phosphate (TDCIPP) and the other contained no detectable target FRs. After replacement, there was a significant decrease (p = 0.03-0.09) in median dust concns. for bis(2-ethylhexyl) tetrabromophthalate (BEHTBP), EHTBB, tris(4-butylphenyl) phosphate (TBPP), and TDCIPP with redns. of 90%, 79%, 65%, and 42%, resp. These findings suggest that the nap mats were an important source of these FRs to dust in the investigated childcare environments and that a campaign of swapping out flame-retarded mats for FR-free ones would reduce exposure to these chems. While calcd. exposure ests. to the investigated FRs via inhalation, dust ingestion, and dermal absorption were below established ref. dose values, they are likely underestimated when considering the toddlers direct contact to the mats and personal cloud effects.
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  20. 20
    Rudel, R. A.; Brody, J. G.; Spengler, J. C.; Vallarino, J.; Geno, P. W.; Sun, G.; Yau, A. Identification of selected hormonally active agents and animal mammary carcinogens in commercial and residential air and dust samples. J. Air Waste Manage. Assoc. 2001, 51 (4), 499– 513,  DOI: 10.1080/10473289.2001.10464292
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    20
    Identification of selected hormonally active agents and animal mammary carcinogens in commercial and residential air and dust samples
    Rudel, Ruthann A.; Brody, Julia G.; Spengler, John D.; Vallarino, Jose; Geno, Paul W.; Sun, Gang; Yau, Alice
    Journal of the Air & Waste Management Association (2001), 51 (4), 499-513CODEN: JAWAFC; ISSN:1096-2247. (Air & Waste Management Association)
    To characterize typical indoor exposure to chems. of interest for research on breast cancer and other hormonally-mediated health outcomes, methods were developed to analyze air and dust for target compds. identified as animal mammary carcinogens or hormonally-active agents and that are used in com. or consumer products or building materials. These methods were applied to a small no. of residential and com. environments to begin to characterize the extent of exposure to these classes of compds. Phenolic compds. (nonylphenol, octylphenol, bisphenol A, and the methoxychlor metabolite, 2,2-bis (p-hydroxyphenyl)-1,1,1-trichloroethane [HPTE]), were extd., derivatized, and analyzed by gas chromatog./mass spectrometry (GC/MS)-selective ion monitoring (SIM). Selected phthalates, pesticides, polycyclic arom. hydrocarbons (PAH), and polychlorinated biphenyls (PCB) were extd. and analyzed by GC/MS-SIM. Residential and workplace samples showed detectable concns. of 12 pesticides in dust and 7 in air samples. Phthalates were abundant in dust (0.3-524 μg/g) and air (0.005-2.8 μg/m3). Nonylphenol and its mono- and di-ethoxylates were prevalent in dust (0.82-14 μg/g) along with estrogenic phenols, such as bisphenol A and o-Ph phenol. In this 7-sample pilot study, 33 of 86 target compds. were detected in dust, and 24 of 57 target compds. were detected in air. In a single sample from 1 home, 27 target compds. were detected in dust and 15 in air, providing an indication of chem. mixts. to which humans are typically exposed.
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  21. 21
    Rudel, R. A.; Camann, D. E.; Spengler, J. D.; Korn, L. R.; Brody, J. G. Phthalates, alkylphenols, pesticides, polybrominated diphenyl ethers, and other endocrine-disrupting compounds in indoor air and dust. Environ. Sci. Technol. 2003, 37 (20), 4543– 53,  DOI: 10.1021/es0264596
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    Phthalates, Alkylphenols, Pesticides, Polybrominated Diphenyl Ethers, and Other Endocrine-Disrupting Compounds in Indoor Air and Dust
    Rudel, Ruthann A.; Camann, David E.; Spengler, John D.; Korn, Leo R.; Brody, Julia G.
    Environmental Science and Technology (2003), 37 (20), 4543-4553CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Endocrine-disrupting compds. (EDC) have widespread consumer uses, yet little is known about indoor exposure. Indoor air and dust was sampled in 120 homes and analyzed for 89 org. EDC: 52 compds. were detected in air and 66 were detected in dust. These are the first reported measurements in residential environments for >30 of these compds., including several detected at highest concns. The no. of compds. detected/home was 13-28 in air and 6-42 in dust. The most abundant compds. in air included phthalates (plasticizers, emulsifiers), o-phenylphenol (disinfectant), 4-nonylphenol (detergent metabolite), and 4-tert-butylphenol (adhesive), with typical concns. of 50-1500 ng/m3. Penta- and tetrabrominated di-Ph ethers (flame retardants) were frequently detected in dust, and 2,3-dibromo-1-propanol, the carcinogenic intermediate of a flame retardant banned in 1977, was detected in air and dust. A total of 23 pesticides were detected in air and 27 were detected in dust; the most abundant were permethrins and the synergist, piperonyl butoxide; banned pesticides (heptachlor, chlordane, methoxychlor, DDT) were also frequently detected, suggesting limited indoor degrdn. Detected concns. exceeded government health-based guidelines for 15 compds.; however, no guidelines are available for 28 compds. and existing guidelines do not consider endocrine effects. Results provided a basis to prioritize toxicol. and exposure research for individual EDC and mixts. and provided new tools for exposure assessment in health studies.
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  22. 22
    Dodson, R. E.; Perovich, L. J.; Covaci, A.; Van den Eede, N.; Ionas, A. C.; Dirtu, A. C.; Brody, J. G.; Rudel, R. A. After the PBDE phase-out: a broad suite of flame retardants in repeat house dust samples from California. Environ. Sci. Technol. 2012, 46 (24), 13056– 66,  DOI: 10.1021/es303879n
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    After the PBDE Phase-Out: A Broad Suite of Flame Retardants in Repeat House Dust Samples from California
    Dodson, Robin E.; Perovich, Laura J.; Covaci, Adrian; Van den Eede, Nele; Ionas, Alin C.; Dirtu, Alin C.; Brody, Julia Green; Rudel, Ruthann A.
    Environmental Science & Technology (2012), 46 (24), 13056-13066CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Higher house dust polybrominated di-Ph ether (PBDE) flame retardant (FR) concns. have been reported in California vs. other parts of the world due to the state furniture flammability std.; however, changing concns. of these and other FR have not been evaluated following the 2004 US phase-out of PentaBDE and OctaBDE. This work analyzed dust collected in 16 California homes in 2006 and again in 2011 for 62 FR and organohalogens; this represents the broadest in-home FR investigation. A total of 55 compds. were detected in at least one sample; 41 in at least 50% of samples. Chlorinated organophosphate flame retardants concns., including 2 (TCEP, TDCIPP) listed as carcinogens under California Proposition 65, were obsd. up to 0.01% in dust, higher than previously reported in the US. In 75% of homes, TDBPP (brominated Tris) was detected; this compd. was banned in sleep-wear for children due to carcinogenicity. This is the first report on TDBPP in house dust. Concns. of Firemaster 550 components (EH-TBB, BEH-TEBP, TPHP) were higher in 2011 than 2006, consistent with its use as a PentaBDE replacement. Results highlighted the evolving nature of FR exposure and suggested manufacturers continue to use hazardous chems. and replace chems. of concern with chems. with uncharacterized toxicity.
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    Stapleton, H. M.; Sharma, S.; Getzinger, G.; Ferguson, P. L.; Gabriel, M.; Webster, T. F.; Blum, A. Novel and high volume use flame retardants in US couches reflective of the 2005 PentaBDE phase out. Environ. Sci. Technol. 2012, 46 (24), 13432– 9,  DOI: 10.1021/es303471d
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    Novel and High Volume Use Flame Retardants in US Couches Reflective of the 2005 PentaBDE Phase Out
    Stapleton, Heather M.; Sharma, Smriti; Getzinger, Gordon; Ferguson, P. Lee; Gabriel, Michelle; Webster, Thomas F.; Blum, Arlene
    Environmental Science & Technology (2012), 46 (24), 13432-13439CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    The California furniture flammability std., Tech. Bulletin 117 (TB 117), is believed to be a major driver of chem. flame retardant (FR) use in residential furniture in the US. With the phase-out of the polybrominated di-Ph ether (PBDE) FR mixt., PentaBDE, in 2005, alternative FR are increasingly being used to meet TB 117; however, it is unclear which chems. were being used and how frequently. To address this data gap, this work collected and analyzed 102 samples of polyurethane foam from residential couches purchased in the US from 1985 to 2010. Overall, chem. FR were detected in 85% of the couches. In samples purchased prior to 2005 (n = 41), PBDE assocd. with the PentaBDE mixt. (including BDE 47, 99, 100; PentaBDE) were the most common FR detected (39%), followed by tris(1,3-dichloroisopropyl) phosphate (TDCPP; 24%), a suspected human carcinogen. In samples purchased in 2005 or later (n = 61)m the most common FR detected were TDCPP (52%) and components assocd. with the Firemaster550 (FM 550) mixt. (18%). Since the 2005 phase-out of PentaBDE, use of TDCPP significantly increased. Also, a mixt. of non-halogenated organophosphate FR, including tri-Ph phosphate (TPP), tris(4-butylphenyl) phosphate (TBPP), and a mix of butylphenyl phosphate isomers, were obsd. in 13% of couch samples purchased in 2005 or later. Overall, the prevalence of FR (and PentaBDE) was higher in couches bought in California vs. elsewhere, although the difference was not quite significant (p = 0.054 for PentaBDE). The difference was greater before 2005 than after, suggesting TB 117 is becoming a de-facto std. across the US. This work detd. the presence of a TB 117 label predicted the presence of a FR; however, lack of a label did not predict the absence of a FR. Following the PentaBDE phase-out, an increased no. of flame retardants was obsd. on the market. With these results and the potential for human exposure to FR, health studies should be conducted on the types of FR identified here.
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    Decabromodiphenylether: An Investigation of Non-Halogen Substitutes in Electronic Enclosure and Textile Applications; Lowell Center for Sustainable Production, University of Massachusetts Lowell: Lowell, MA, 2005.
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    Ghanem, R.; Delmani, F.-A. Kinetics of thermal and photolytic degradation of decabromodiphenyl ether (BDE 209) in backcoated textile samples. J. Anal. Appl. Pyrolysis 2012, 98, 79– 85,  DOI: 10.1016/j.jaap.2012.09.001
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    25
    Kinetics of thermal and photolytic degradation of decabromodiphenyl ether (BDE 209) in backcoated textile samples
    Ghanem, Raed; Delmani, Fatima-Azzahra
    Journal of Analytical and Applied Pyrolysis (2012), 98 (), 79-85CODEN: JAAPDD; ISSN:0165-2370. (Elsevier B.V.)
    Kinetics of the thermal and photolytic degrdn. of decabromodiphenyl ether (DBE 209) was studied using HPLC. Samples lost an amt. of ∼8.4% (wt./wt.), 24% (wt./wt.), 39.4% (wt./wt.) and 28.5% of the amt. of DBE 209 originally present in the samples due to ageing at 25, 60, 90° C and UV exposure, resp. The thermal and photolytic release was found to follow the first order kinetics with rate consts. estd. to be 3.6 × 10-3, 1.03 × 10-2, 3.6 × 10-2 and 3.94 × 10-2 day-1, resp. Ageing of the textile samples enhanced the release of the DBE 209 from the backcoated textile. Photodegrdn. of BDE 209 into lower congeners of brominated flame retardants was also obsd. for the UV-aged samples.Migration of DBE 209 from the backcoated textile into biol. fluids was studied using Head-over-Heels and contact-Blotting test for unaged, thermally and UV aged samples. The presence of biol. fluids (sweat, saliva and juice) was found to enhance the migration of DBE 209 compared to water. Migration of BDE 209 into artificial biol. fluids is significantly increased for samples previously exposed to UV radiation or thermally aged. An increase from 0.6% (wt./wt.) to a max. of 2% (wt./wt.) of the amt. of BDE 209 migrated into artificial biol. fluids due to ageing conditions in the presence of biol. fluid was recorded.
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    Abbasi, G.; Buser, A. M.; Soehl, A.; Murray, M. W.; Diamond, M. L. Stocks and flows of PBDEs in products from use to waste in the U.S. and Canada from 1970 to 2020. Environ. Sci. Technol. 2015, 49 (3), 1521– 8,  DOI: 10.1021/es504007v
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    Stocks and Flows of PBDEs in Products from Use to Waste in the U.S. and Canada from 1970 to 2020
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    The time-dependent stock of PBDEs contained in in-use products (excluding building materials and large vehicles) was estd. for the U.S. and Canada from 1970 to 2020 based on product consumption patterns, PBDE contents, and product lifespan. The stocks of penta- and octaBDE peaked in in-use products at 17,000 (95% confidence interval: 6000-70 000) and 4000 (1000-50 000) tonnes in 2004, resp., and for decaBDE at 140,000 (40,000-300,000) tonnes in 2008. Products dominating PBDE usage were polyurethane foam used in furniture (65% of pentaBDE), casings of elec. and electronic equipment or EEE (80% of octaBDE), and EEE and automotive seating (35% of decaBDE for each category). The largest flow of PBDEs in products, excluding automotive sector, to the waste phase occurred between 2005 and 2008 at ∼10,000 tonnes per yr. Total consumption of penta-, octa-, and decaBDE from 1970 to 2020 in products considered was estd. at ∼46,000, ∼25,000, and ∼380,000 tonnes, resp. Per capita usage was estd. at 10-250, 10-150, and 200-2000 g/capita y for penta-, octa-, and decaBDE, resp., over the time span. Considering only the first use (no reuse and/or storage) of PBDE-contg. products, approx. 60% of the stock of PBDEs in 2014 or ∼70,000 tonnes, of which 95% is decaBDE, will remain in the use phase in 2020. Total emissions to air of all PBDEs from the in-use product stock was estd. at 70-700 tonnes between 1970 and 2020, with annual emissions of 0.4-4 tonnes/y for each of penta- and octaBDE and 0.35-3.5 tonnes/y for decaBDE in 2014.
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    Davis, E. F.; Stapleton, H. M. Photodegradation pathways of nonabrominated diphenyl ethers, 2-ethylhexyltetrabromobenzoate and di(2-ethylhexyl)tetrabromophthalate: identifying potential markers of photodegradation. Environ. Sci. Technol. 2009, 43 (15), 5739– 46,  DOI: 10.1021/es901019w
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    Photodegrdn. kinetics of several polybrominated di-Ph ethers (PBDEs), particularly decabromodiphenyl ether (PBDE 209), have been reported in various matrixes, demonstrating that it photodegrades primarily via debromination. However, it has been difficult to det. the primary pathways by which Br is cleaved from PBDE 209 to form nona- and octabrominated congeners. The photodegrdn. of 3 nonaBDE congeners (i.e., PBDE 206, 207, and 208) was examd. individually in 3 different solvents exposed to natural sunlight and then analyzed to identify the primary degrdn. products. Rapid degrdn. of nonaBDEs (half-lives 4.25-12.78 min) was obsd. coincident with formation of octa- and heptabrominated PBDEs. PBDE 207 photodegraded most rapidly while PBDE 206 photodegraded the slowest. The photodegrdn. pathways of each nonaBDE congener were consistent among the different solvent matrixes tested; however, mass balances varied with the type of solvent used in the expt. (recovery 76-95%). The octabrominated congener, PBDE 202, and the ratio of PBDE 197 to PBDE 201, were identified as congeners that may serve as environmental markers of photolytic debromination of decaBDE. Addnl. photodegrdn. studies were conducted with 2 new brominated flame retardants used in replacements for pentaBDE mixts.: 2-ethylhexyltetrabromobenzoate (TBB) and di(2-ethylhexyl)-tetrabromophthalate (TBPH). Both TBB and TBPH underwent photolysis more slowly than nonaBDEs (half-lives 85.70-220.17 min) and primarily formed debrominated products.
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    Covaci, A.; Gerecke, A. C.; Law, R. J.; Voorspoels, S.; Kohler, M.; Heeb, N. V.; Leslie, H.; Allchin, C. R.; De Boer, J. Hexabromocyclododecanes (HBCDs) in the environment and humans: a review. Environ. Sci. Technol. 2006, 40 (12), 3679– 88,  DOI: 10.1021/es0602492
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    Bello, A.; Carignan, C. C.; Xue, Y.; Stapleton, H. M.; Bello, D. Exposure to organophosphate flame retardants in spray polyurethane foam applicators: Role of dermal exposure. Environ. Int. 2018, 113, 55– 65,  DOI: 10.1016/j.envint.2018.01.020
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    Exposure to organophosphate flame retardants in spray polyurethane foam applicators: Role of dermal exposure
    Bello, Anila; Carignan, Courtney C.; Xue, Yalong; Stapleton, Heather M.; Bello, Dhimiter
    Environment International (2018), 113 (), 55-65CODEN: ENVIDV; ISSN:0160-4120. (Elsevier Ltd.)
    Spray polyurethane foam (SPF) is a highly effective thermal insulation material that has seen considerable market growth in the past decade. Organophosphate flame retardants (PFRs) are added to SPF formulations to meet fire code requirements. A common flame retardant used in SPF formulations is tris 1-chloro 2-Pr phosphate (TCIPP), a suspected endocrine disruptor. Exposure monitoring efforts during SPF applications have focused primarily on the isocyanate component, a potent respiratory and dermal sensitizer. However, to our knowledge, there is no monitoring data for TCIPP. To characterize occupational exposures to TCIPP and other flame retardants during SPF insulation. Workers at four SPF insulation sites and one foam removal site (total n = 14) were recruited as part of this pilot study. Personal inhalation exposure to TCIPP was monitored with a CIP-10MI inhalable sampler and potential dermal exposure was assessed through the use of a glove dosimeter. Biomarkers of TCIPP and three other PFRs were measured in urine collected from workers pre-and post-shift. Linear mixed effect models were used to analyze assocns. of urinary biomarkers with inhalation and dermal exposures and paired t-tests were used to examine the difference on the means of urinary biomarkers pre-and post-shift. Chem. anal. of all species was performed with liq. chromatog.-electrospray ionization tandem mass spectrometry. Geometric mean (GM) concns. of TCIPP in personal air monitors and glove dosimeters collected from SPF applicators, 294.7 μg/m3 and 18.8 mg/pair resp. Overall, GM concns. of the two TCIPP urinary biomarkers BCIPP and BCIPHIPP and (6.2 and 88.8 μg/mL) were 26-35 times higher than reported in the general population. Post-shift levels of TCIPP biomarkers were higher than pre-shift even though workers at insulation sites wore supplied air respirators, gloves and coveralls. The urinary biomarkers for the other PFRs were not elevated post shift. Concns. of TCIPP on glove dosimeters were pos. assocd. with post-shift urinary TCIPP biomarkers (p < 0.05) whereas concns. in personal air samples were not. High levels of urinary biomarkers for TCIPP among SPF applicators, including post-shift, points to absorption of TCIPP during the work shift, in spite of the use of best industry exposure control practices. Dermal exposure appears to be an important, if not the primary exposure pathway for TCIPP, although inhalation or incidental ingestion of foam particles post-SPF application cannot be ruled out in this pilot study.
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  • Abstract

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    Figure 1

    Figure 1. FR concentrations (ng/g) in spaces (n = 86) adhering to different furniture flammability standards. Estimated marginal means plotted as diamonds with color indicating statistically significant differences compared to TB117-2013 (baseline model). Nondetects are unfilled circles.

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    Figure 2

    Figure 2. FR composition in spaces adhering to different furniture flammability standards. Proportions are GM of each chemical to sum of GMs for all chemicals (top bar graph).

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  • References

    This article references 31 other publications.

    1. 1
      State of California Technical Bulletin 117-2013: Requirements, Test Procedure, and Apparatus for Testing the Smolder Resistance of Materials Used in Upholstered Furniture; State of California, Department of Consumer Affairs, Bureau of Electronic & Appliance Repair Home Furnishings & Thermal Insulation: Sacramento, CA, 2013.
      There is no corresponding record for this reference.
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      Dodson, R. E.; Rodgers, K. M.; Carey, G.; Cedeno Laurent, J. G.; Covaci, A.; Poma, G.; Malarvannan, G.; Spengler, J. D.; Rudel, R. A.; Allen, J. G. Flame Retardant Chemicals in College Dormitories: Flammability Standards Influence Dust Concentrations. Environ. Sci. Technol. 2017, 51 (9), 4860– 4869,  DOI: 10.1021/acs.est.7b00429
      2
      Flame Retardant Chemicals in College Dormitories: Flammability Standards Influence Dust Concentrations
      Dodson, Robin E.; Rodgers, Kathryn M.; Carey, Gale; Cedeno Laurent, Jose Guillermo; Covaci, Adrian; Poma, Giulia; Malarvannan, Govindan; Spengler, John D.; Rudel, Ruthann A.; Allen, Joseph G.
      Environmental Science & Technology (2017), 51 (9), 4860-4869CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Furniture flammability stds. are typically met using chem. flame retardants (FR). FR can migrate from products into dust and are linked to cancer, neurol. impairment, and endocrine disruption. This work collected 95 dust samples from dormitory common areas and student rooms at two US college campuses adhering to two different furniture flammability stds.: Tech. Bulletin 117 (TB117) and Tech. Bulletin 133 (TB133). Since TB133 requires furniture to withstand a much more demanding test flame than TB117, it was hypothesized that spaces with TB133 furniture would have higher FR concns. in dust. In total, 47 targeted FR (12 polybrominated di-Ph ether [PBDE] congeners, 19 other brominated FR, 11 P FR (PFR), 2 Dechlorane-Plus [DP] isomers, 3 hexabromocyclododecane [HBCDD] isomers) were obsd. in the 95 dust samples. The highest reported US concns. for several FR (BDE 209 [up to 990 000 ng/g]) were measured, which may have been used to meet the TB133 std. Sixteen FR were prioritized and concn. were analyzed in relation to flammability stds. and the presence and age of furniture and electronics. Adherence to TB133 was assocd. with higher BDE 209, decabromodiphenylethane (DBDPE), DP, and HBCDD concns. vs. adherence to TB117 in univariate models (p <0.05). Student dormitory rooms tended to have higher concns. of some FR vs. common rooms, likely a result of furniture and electronics d. As flammability stds. are updated, it is crit. to understand their impact on exposure and health risks.
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      Zota, A. R.; Rudel, R. A.; Morello-Frosch, R. A.; Brody, J. G. Elevated house dust and serum concentrations of PBDEs in California: Unintended consequences of furniture flammability standards?. Environ. Sci. Technol. 2008, 42 (21), 8158– 8164,  DOI: 10.1021/es801792z
      3
      Elevated House Dust and Serum Concentrations of PBDEs in California: Unintended Consequences of Furniture Flammability Standards?
      Zota, Ami R.; Rudel, Ruthann A.; Morello-Frosch, Rachel A.; Brody, Julia Green
      Environmental Science & Technology (2008), 42 (21), 8158-8164CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Studies showed higher house dust and body burden concns. of polybrominated di-Ph ether (PBDE) flame retardants in North America vs. Europe; but little is known about exposure variation within North America, where the California furniture flammability std. affects PBDE use. Dust samples from 49 homes in 2 California communities were compared with 120 Massachusetts homes and other published studies. Dust concns. [median (range) ng/g] in California homes of BDE-47, -99, and -100 were 2700 (112-107,000), 3800 (102-170,000), and 684 (less than min. reporting level to 30,900), resp., and were 4-10 times higher than previously reported in North America; max. concns. were the highest ever reported in indoor dust. Then, whether human serum PBDE concns. were also higher in California vs. other North American regions was assessed by analyzing the 2003-2004 National Health and Nutrition Examn. Survey, the only data set available with serum from a representative sample of the US population (n = 2040). California residence was significantly assocd. with nearly 2-fold higher ΣPBDE serum concns. (least square geometric mean, ng/g lipid: 73.0 vs. 38.5 [p = 0.002]). Elevated PBDE exposure in California may result from state furniture flammability stds.; results suggested the need for further research with a larger representative sample.
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    4. 4
      State of California Technical Bulletin 117: Requirements, Test Procedure, and Apparatus for Testing the Flame Retardance of Resilient Filling Materials Used in Upholstered Furniture; State of California, Department of Consumer Affairs, Bureau of Electronic & Appliance Repair Home Furnishings & Thermal Insulation: North Highlands, CA, 2000.
      There is no corresponding record for this reference.
    5. 5
      Massachusetts Comprehensive Fire Safety Code: 527 CMR 1.00; Massachusetts Department of Fire Services: Board of Fire Prevention Regulations, 2015.
      There is no corresponding record for this reference.
    6. 6
      Regulation of Upholstered Furniture: BFD IX-10; Boston Fire Department, 2016.
      There is no corresponding record for this reference.
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      Division 3 of Title 4 of the California Code of Regulation, Bureau of Electronic and Appliance Repair Home Furnishings; State of California, Office of Administrative Law, Bureau of Electronic and Appliance Repair Home Furnishings, and Thermal Insulation, 2019.
      There is no corresponding record for this reference.
    8. 8
      Initial Statement of Reasons: Subject Matter of Proposed Regulations: Amendment of Flammability Standards; State of California, Bureau of Electronic and Appliance Repair, 2018.
      There is no corresponding record for this reference.
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      Babrauskas, V.; Blum, A.; Daley, R.; Birnbaum, L. Flame Retardants in Furniture Foam: Benefits and Risks. Fire Saf. Sci. 2011, 10, 265– 278,  DOI: 10.3801/IAFSS.FSS.10-265
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      Rodgers, K. M.; Swetschinski, L. R.; Dodson, R. E.; Alpert, H. R.; Fleming, J. M.; Rudel, R. A. Health Toll From Open Flame and Cigarette-Started Fires on Flame-Retardant Furniture in Massachusetts, 2003–2016. Am. J. Public Health 2019, 109 (9), 1205– 1211,  DOI: 10.2105/AJPH.2019.305157
      10
      Health Toll From Open Flame and Cigarette-Started Fires on Flame-Retardant Furniture in Massachusetts, 2003-2016
      Rodgers Kathryn M; Swetschinski Lucien R; Dodson Robin E; Alpert Hillel R; Fleming Joseph M; Rudel Ruthann A
      American journal of public health (2019), 109 (9), 1205-1211 ISSN:.
      Objectives. To evaluate the risk of death and injury in residential fires started on upholstered furniture, with a focus on open flame and cigarette-related heat sources.Methods. We used civilian death and injury data from 34 081 residential fires in the Massachusetts Fire Incident Reporting System from 2003 to 2016. We compared outcomes associated with fires that started on upholstered furniture ignited by smoking materials versus open flames.Results. Although fires starting on upholstered furniture were not common (2.2% of total fires), odds of death and injury were significantly higher in these fires than in fires started on other substrates. Among furniture fires, odds of death were 3 times greater when those fires were ignited by smoking materials than when ignited by open flames (odds ratio = 3.4; 95% confidence interval = 1.3, 10.9).Conclusions. Furniture fires started by smoking materials were associated with more deaths than were furniture fires started by open flames.Public Health Implications. Historically, furniture flammability regulations have focused on open flame heat sources, resulting in the addition of toxic flame retardants to furniture. Interventions to reduce deaths should instead focus on smoking materials.
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    11. 11
      Dorman, D. C.; Chiu, W.; Hales, B. F.; Hauser, R.; Johnson, K. J.; Mantus, E.; Martel, S.; Robinson, K. A.; Rooney, A. A.; Rudel, R.; Sathyanarayana, S.; Schantz, S. L.; Waters, K. M. Polybrominated diphenyl ether (PBDE) neurotoxicity: a systematic review and meta-analysis of animal evidence. J. Toxicol. Environ. Health, Part B 2018, 21 (4), 269– 289,  DOI: 10.1080/10937404.2018.1514829
      11
      Polybrominated diphenyl ether (PBDE) neurotoxicity: a systematic review and meta-analysis of animal evidence
      Dorman, David C.; Chiu, Weihsueh; Hales, Barbara F.; Hauser, Russ; Johnson, Kamin J.; Mantus, Ellen; Martel, Susan; Robinson, Karen A.; Rooney, Andrew A.; Rudel, Ruthann; Sathyanarayana, Sheela; Schantz, Susan L.; Waters, Katrina M.
      Journal of Toxicology and Environmental Health, Part B: Critical Reviews (2018), 21 (4), 269-289CODEN: JTECFR; ISSN:1093-7404. (Taylor & Francis, Inc.)
      A review. A recent systematic review (SR) and meta-anal. of human studies found an assocn. between prenatal serum polybrominated di-Ph ethers (PBDE) concns. and a decrease in the IQ of children. A SR of exptl. developmental animal PBDE-mediated neurotoxicity studies was performed in the present study. Outcomes assessed included measures related to learning, memory, and attention, which parallel the intelligence-related outcomes evaluated in the human studies SR. PubMed, Embase, and Toxline were searched for relevant exptl. non-human mammalian studies. Evaluation of risk of bias (RoB) and overall body of evidence followed guidance developed by the National Toxicol. Program. Animal studies using varying designs and outcomes were available for BDEs 47, 99, 153, 203, 206, and 209 and the tech. mixt. DE-71. Study reporting of methods and results was often incomplete leading to concerns regarding RoB. A meta-anal. of 6 Morris water maze studies showed evidence of a significant increase in last trial latency (effect size of 25.8 [CI, 20.3 to 31.2]) in PBDE-exposed animals with low heterogeneity. For most endpoints, there were unexplained inconsistencies across studies and no consistent evidence of a dose-response relationship. There is a "moderate" level of evidence that exposure to BDEs 47, 99, and 209 affects learning. For other PBDEs and other endpoints, the level of evidence was "low" or "very low". The meta-anal. led to stronger conclusions than that based upon a qual. review of the evidence. The SR also identified RoB concerns that might be remedied by better study reporting.
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    12. 12
      Lam, J.; Lanphear, B. P.; Bellinger, D.; Axelrad, D. A.; McPartland, J.; Sutton, P.; Davidson, L.; Daniels, N.; Sen, S.; Woodruff, T. J. Developmental PBDE Exposure and IQ/ADHD in Childhood: A Systematic Review and Meta-analysis. Environ. Health Perspect. 2017, 125 (8), 086001,  DOI: 10.1289/EHP1632
      12
      Developmental PBDE Exposure and IQ/ADHD in Childhood: A Systematic Review and Meta-analysis
      Lam Juleen; Sutton Patrice; Daniels Natalyn; Woodruff Tracey J; Lanphear Bruce P; Bellinger David; Axelrad Daniel A; McPartland Jennifer; Davidson Lisette; Sen Saunak
      Environmental health perspectives (2017), 125 (8), 086001 ISSN:.
      BACKGROUND: In the United States, one in six children are affected by neurodevelopmental disorders, and polybrominated diphenyl ethers (PBDEs) in flame-retardant chemicals are measured ubiquitously in children. OBJECTIVE: We conducted a systematic a systematic review regarding developmental exposure to PBDEs and intelligence or Attention Deficit/Hyperactivity Disorder (ADHD) and attention-related behavioral conditions in humans. METHODS: We searched articles published up to 26 September 2016, and included original studies that quantified exposures to PBDEs incurred any time in proximity to conception or during in utero, perinatal, or childhood time periods. We evaluated the risk of bias of individual studies and the overall quality and strength of the evidence according to the Navigation Guide systematic review methodology. We established criteria in advance to identify studies that could be combined using random effects meta-analyses (DerSimonian-Laird method). RESULTS: Fifteen studies met the inclusion criteria; 10 studies met the criteria for intelligence and nine for attention-related problems. We rated studies generally with "low" to "probably low" risk of bias and rated the overall body of evidence as "moderate" quality with "sufficient" evidence for an association between Intelligence Quotient (IQ) and PBDEs. Our meta-analysis of four studies estimated a 10-fold increase (in other words, times 10) in PBDE exposure associated with a decrement of 3.70 IQ points (95% confidence interval: 0.83, 6.56). We concluded the body of evidence was of "moderate" quality for ADHD with "limited" evidence for an association with PBDEs, based on the heterogeneity of association estimates reported by a small number of studies and the fact that chance, bias, and confounding could not be ruled out with reasonable confidence. CONCLUSION: We concluded there was sufficient evidence supporting an association between developmental PBDE exposure and reduced IQ. Preventing developmental exposure to PBDEs could help prevent loss of human intelligence. https://doi.org/10.1289/EHP1632.
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    13. 13
      Allen, J. G.; Gale, S.; Zoeller, R. T.; Spengler, J. D.; Birnbaum, L.; McNeely, E. PBDE flame retardants, thyroid disease, and menopausal status in U.S. women. Environ. Health 2016, 15 (1), 60,  DOI: 10.1186/s12940-016-0141-0
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      PBDE flame retardants, thyroid disease, and menopausal status in U.S. women
      Allen, Joseph G.; Gale, Sara; Zoeller, R. Thomas; Spengler, John D.; Birnbaum, Linda; McNeely, Eileen
      Environmental Health (London, United Kingdom) (2016), 15 (), 60/1-60/9CODEN: EHAGAB; ISSN:1476-069X. (BioMed Central Ltd.)
      Background: Women have elevated rates of thyroid disease compared to men. Environmental toxicants have been implicated as contributors to this dimorphism, including polybrominated di-Ph ethers (PBDEs), flame retardant chems. that disrupt thyroid hormone action. PBDEs have also been implicated in the disruption of estrogenic activity, and estrogen levels regulate thyroid hormones. Post-menopausal women may therefore be particularly vulnerable to PBDE induced thyroid effects, given low estrogen reserves. The objective of this study was to test for an assocn. between serum PBDE concns. and thyroid disease in women from the United States (U.S.), stratified by menopause status. Methods: Serum PBDE concns. (BDEs 47, 99, 100 and 153) from the National Health and Examn. Survey (NHANES) and reports on thyroid problems were available in the NHANES 2003-2004 cycle. Odds ratios (ORs) were calcd. using multivariate logistic regression models accounting for population-weighted survey techniques and controlling for age, body mass index (BMI), education, smoking, alc. consumption and thyroid medication. Menopause status was obtained by self-reported absence of menstruation in the previous 12 mo and declared menopause. Results: Women in the highest quartile of serum concns. for BDEs 47, 99, and 100 had increased odds of currently having thyroid disease (ORs: 1.5, 1.8, 1.5, resp.) compared to the ref. group (1st and 2nd quartiles combined); stronger assocns. were obsd. when the anal. was restricted to postmenopausal women (ORs: 2.2, 3.6, 2.0, resp.). Conclusion: Exposure to BDEs 47, 99, and 100 is assocd. with thyroid disease in a national sample of U.S. women, with greater effects obsd. post-menopause, suggesting that the disruption of thyroid signaling by PBDEs may be enhanced by the altered estrogen levels during menopause.
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    14. 14
      Blum, A.; Behl, M.; Birnbaum, L. S.; Diamond, M. L.; Phillips, A.; Singla, V.; Sipes, N. S.; Stapleton, H. M.; Venier, M. Organophosphate Ester Flame Retardants: Are They a Regrettable Substitution for Polybrominated Diphenyl Ethers?. Environ. Sci. Technol. Lett. 2019, 6 (11), 638– 649,  DOI: 10.1021/acs.estlett.9b00582
      14
      Organophosphate Ester Flame Retardants: Are They a Regrettable Substitution for Polybrominated Diphenyl Ethers?
      Blum, Arlene; Behl, Mamta; Birnbaum, Linda S.; Diamond, Miriam L.; Phillips, Allison; Singla, Veena; Sipes, Nisha S.; Stapleton, Heather M.; Venier, Marta
      Environmental Science & Technology Letters (2019), 6 (11), 638-649CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
      A review to det. whether organophosphate ester flame retardants (OPFR) are a better choice (better alternative) than polybrominated di-Ph ether flame retardants (PBDE) by comparing the two over a range of properties is given. OPFR exposure is ubiquitous to humans and indoor/outdoor; they now often occur at higher concns. than PBDE peak exposure concns. Toxicity testing, epidemiol. study, and risk assessment data all suggest there are health concerns at current exposure levels for halogenated and non-halogenated OPFR. With the large no. of OPFR in use, producers can move toward healthier, safer products by developing innovative ways to reduce fire risks for electronics enclosures, upholstered furniture, building materials, and other consumer products with no added flame retardants. Topics discussed include: introduction; environmental behavior; indoor behavior and human exposure; toxicity and health effects; epidemiol. evidence; looking forward; supporting information (plasma bio-equiv. using high through-put toxicokinetic modeling).
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    15. 15
      Gold, M. D.; Blum, A.; Ames, B. N. Another flame retardant, tris-(1,3-dichloro-2-propyl)-phosphate, and its expected metabolites are mutagens. Science 1978, 200 (4343), 785– 7,  DOI: 10.1126/science.347576
      15
      Another flame retardant, tris-(1,3-dichloro-2-propyl)phosphate, and its expected metabolites are mutagens
      Gold, Marian Deborah; Blum, Arlene; Ames, Bruce N.
      Science (Washington, DC, United States) (1978), 200 (4343), 785-7CODEN: SCIEAS; ISSN:0036-8075.
      The flame retardant tris(1,3-dichloro-2-propyl) phosphate (Fyrol FR2) [13674-87-8] was a mutagen in the Salmonella-mammalian tissue homogenate tests after it was activated by mouse or rat liver homogenate. The expected enzymic hydrolysis product, 1,3-dichloro-2-propanol [96-23-1] was similarly a mutagen after activation by liver homogenate. A proposed metabolite of the flame retardant, 1,3-dichloro-2-propanone [534-07-6] was a potent mutagen in the absence of such activation. A flame retardant with a similar structure, tris(2,3-dibromopropyl) phosphate (tris-BP), was shown previously to be a mutagen, to cause sterility in animals, to be a carcinogen, and to be absorbed through human skin. These and other flame retardants have characteristic nuclear magnetic resonance spectra that can be used to det. which flame retardant is present in com. purchased sleepwear. Sleepwear treated with tris-BP, Fyrol FR2, and other chem. additives was being sold in late 1977.
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    16. 16
      Sanders, H. J. Flame Retardants: Government Regulations and Public Emphasis on Safety Provide the Impetus for an Expanding industry. Chem. Eng. News 1978, 56 (17), 22– 36,  DOI: 10.1021/cen-v056n017.p022
      There is no corresponding record for this reference.
    17. 17
      Chemicals Considered or Listed Under Proposition 65: Tris(2-chloroethyl) Phosphate. https://oehha.ca.gov/proposition-65/chemicals/tris2-chloroethyl-phosphate (accessed July 23, 2020).
      There is no corresponding record for this reference.
    18. 18
      The New POPs under the Stockholm Convention. http://chm.pops.int/TheConvention/ThePOPs/TheNewPOPs/tabid/2511/Default.aspx (accessed July 23, 2020),.
      There is no corresponding record for this reference.
    19. 19
      Stubbings, W. A.; Schreder, E. D.; Thomas, M. B.; Romanak, K.; Venier, M.; Salamova, A. Exposure to brominated and organophosphate ester flame retardants in U.S. childcare environments: Effect of removal of flame-retarded nap mats on indoor levels. Environ. Pollut. 2018, 238, 1056– 1068,  DOI: 10.1016/j.envpol.2018.03.083
      19
      Exposure to brominated and organophosphate ester flame retardants in U.S. childcare environments: Effect of removal of flame-retarded nap mats on indoor levels
      Stubbings, W. A.; Schreder, E. D.; Thomas, M. B.; Romanak, K.; Venier, M.; Salamova, A.
      Environmental Pollution (Oxford, United Kingdom) (2018), 238 (), 1056-1068CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
      We assessed exposure to 39 brominated and 16 organophosphate ester flame retardants (FRs) from both dust and indoor air at seven childcare centers in Seattle, USA, and investigated the importance of nap mats as a source of these chems. Many childcare centers serving young children use polyurethane foam mats for the childrens naptime. Until recently, the vast majority of these mats sold in the United States contained flame-retarded polyurethane foam to meet California Tech. Bulletin 117 (TB117) requirements. With the 2013 update of TB117, allowing manufacturers to meet flammability stds. without adding FRs to filling materials, FR-free nap mats have become widely available. We conducted an intervention study by actively switching out FR-treated nap mats with FR-free nap mats and measuring FR levels in indoor air and dust before and after the switch-out. The predominant FRs found in dust and indoor air were 2-ethylhexyl tetrabromobenzoate (EHTBB) and tris(1-chloro-2-propyl) phosphate (TCIPP), resp. Nap mat samples analyzed from four of the six centers contained a Firemaster mixt., while one mat was predominantly treated with tris(1,3-dichloroisopropyl) phosphate (TDCIPP) and the other contained no detectable target FRs. After replacement, there was a significant decrease (p = 0.03-0.09) in median dust concns. for bis(2-ethylhexyl) tetrabromophthalate (BEHTBP), EHTBB, tris(4-butylphenyl) phosphate (TBPP), and TDCIPP with redns. of 90%, 79%, 65%, and 42%, resp. These findings suggest that the nap mats were an important source of these FRs to dust in the investigated childcare environments and that a campaign of swapping out flame-retarded mats for FR-free ones would reduce exposure to these chems. While calcd. exposure ests. to the investigated FRs via inhalation, dust ingestion, and dermal absorption were below established ref. dose values, they are likely underestimated when considering the toddlers direct contact to the mats and personal cloud effects.
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    20. 20
      Rudel, R. A.; Brody, J. G.; Spengler, J. C.; Vallarino, J.; Geno, P. W.; Sun, G.; Yau, A. Identification of selected hormonally active agents and animal mammary carcinogens in commercial and residential air and dust samples. J. Air Waste Manage. Assoc. 2001, 51 (4), 499– 513,  DOI: 10.1080/10473289.2001.10464292
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      Identification of selected hormonally active agents and animal mammary carcinogens in commercial and residential air and dust samples
      Rudel, Ruthann A.; Brody, Julia G.; Spengler, John D.; Vallarino, Jose; Geno, Paul W.; Sun, Gang; Yau, Alice
      Journal of the Air & Waste Management Association (2001), 51 (4), 499-513CODEN: JAWAFC; ISSN:1096-2247. (Air & Waste Management Association)
      To characterize typical indoor exposure to chems. of interest for research on breast cancer and other hormonally-mediated health outcomes, methods were developed to analyze air and dust for target compds. identified as animal mammary carcinogens or hormonally-active agents and that are used in com. or consumer products or building materials. These methods were applied to a small no. of residential and com. environments to begin to characterize the extent of exposure to these classes of compds. Phenolic compds. (nonylphenol, octylphenol, bisphenol A, and the methoxychlor metabolite, 2,2-bis (p-hydroxyphenyl)-1,1,1-trichloroethane [HPTE]), were extd., derivatized, and analyzed by gas chromatog./mass spectrometry (GC/MS)-selective ion monitoring (SIM). Selected phthalates, pesticides, polycyclic arom. hydrocarbons (PAH), and polychlorinated biphenyls (PCB) were extd. and analyzed by GC/MS-SIM. Residential and workplace samples showed detectable concns. of 12 pesticides in dust and 7 in air samples. Phthalates were abundant in dust (0.3-524 μg/g) and air (0.005-2.8 μg/m3). Nonylphenol and its mono- and di-ethoxylates were prevalent in dust (0.82-14 μg/g) along with estrogenic phenols, such as bisphenol A and o-Ph phenol. In this 7-sample pilot study, 33 of 86 target compds. were detected in dust, and 24 of 57 target compds. were detected in air. In a single sample from 1 home, 27 target compds. were detected in dust and 15 in air, providing an indication of chem. mixts. to which humans are typically exposed.
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    21. 21
      Rudel, R. A.; Camann, D. E.; Spengler, J. D.; Korn, L. R.; Brody, J. G. Phthalates, alkylphenols, pesticides, polybrominated diphenyl ethers, and other endocrine-disrupting compounds in indoor air and dust. Environ. Sci. Technol. 2003, 37 (20), 4543– 53,  DOI: 10.1021/es0264596
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      Phthalates, Alkylphenols, Pesticides, Polybrominated Diphenyl Ethers, and Other Endocrine-Disrupting Compounds in Indoor Air and Dust
      Rudel, Ruthann A.; Camann, David E.; Spengler, John D.; Korn, Leo R.; Brody, Julia G.
      Environmental Science and Technology (2003), 37 (20), 4543-4553CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Endocrine-disrupting compds. (EDC) have widespread consumer uses, yet little is known about indoor exposure. Indoor air and dust was sampled in 120 homes and analyzed for 89 org. EDC: 52 compds. were detected in air and 66 were detected in dust. These are the first reported measurements in residential environments for >30 of these compds., including several detected at highest concns. The no. of compds. detected/home was 13-28 in air and 6-42 in dust. The most abundant compds. in air included phthalates (plasticizers, emulsifiers), o-phenylphenol (disinfectant), 4-nonylphenol (detergent metabolite), and 4-tert-butylphenol (adhesive), with typical concns. of 50-1500 ng/m3. Penta- and tetrabrominated di-Ph ethers (flame retardants) were frequently detected in dust, and 2,3-dibromo-1-propanol, the carcinogenic intermediate of a flame retardant banned in 1977, was detected in air and dust. A total of 23 pesticides were detected in air and 27 were detected in dust; the most abundant were permethrins and the synergist, piperonyl butoxide; banned pesticides (heptachlor, chlordane, methoxychlor, DDT) were also frequently detected, suggesting limited indoor degrdn. Detected concns. exceeded government health-based guidelines for 15 compds.; however, no guidelines are available for 28 compds. and existing guidelines do not consider endocrine effects. Results provided a basis to prioritize toxicol. and exposure research for individual EDC and mixts. and provided new tools for exposure assessment in health studies.
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    22. 22
      Dodson, R. E.; Perovich, L. J.; Covaci, A.; Van den Eede, N.; Ionas, A. C.; Dirtu, A. C.; Brody, J. G.; Rudel, R. A. After the PBDE phase-out: a broad suite of flame retardants in repeat house dust samples from California. Environ. Sci. Technol. 2012, 46 (24), 13056– 66,  DOI: 10.1021/es303879n
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      After the PBDE Phase-Out: A Broad Suite of Flame Retardants in Repeat House Dust Samples from California
      Dodson, Robin E.; Perovich, Laura J.; Covaci, Adrian; Van den Eede, Nele; Ionas, Alin C.; Dirtu, Alin C.; Brody, Julia Green; Rudel, Ruthann A.
      Environmental Science & Technology (2012), 46 (24), 13056-13066CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Higher house dust polybrominated di-Ph ether (PBDE) flame retardant (FR) concns. have been reported in California vs. other parts of the world due to the state furniture flammability std.; however, changing concns. of these and other FR have not been evaluated following the 2004 US phase-out of PentaBDE and OctaBDE. This work analyzed dust collected in 16 California homes in 2006 and again in 2011 for 62 FR and organohalogens; this represents the broadest in-home FR investigation. A total of 55 compds. were detected in at least one sample; 41 in at least 50% of samples. Chlorinated organophosphate flame retardants concns., including 2 (TCEP, TDCIPP) listed as carcinogens under California Proposition 65, were obsd. up to 0.01% in dust, higher than previously reported in the US. In 75% of homes, TDBPP (brominated Tris) was detected; this compd. was banned in sleep-wear for children due to carcinogenicity. This is the first report on TDBPP in house dust. Concns. of Firemaster 550 components (EH-TBB, BEH-TEBP, TPHP) were higher in 2011 than 2006, consistent with its use as a PentaBDE replacement. Results highlighted the evolving nature of FR exposure and suggested manufacturers continue to use hazardous chems. and replace chems. of concern with chems. with uncharacterized toxicity.
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    23. 23
      Stapleton, H. M.; Sharma, S.; Getzinger, G.; Ferguson, P. L.; Gabriel, M.; Webster, T. F.; Blum, A. Novel and high volume use flame retardants in US couches reflective of the 2005 PentaBDE phase out. Environ. Sci. Technol. 2012, 46 (24), 13432– 9,  DOI: 10.1021/es303471d
      23
      Novel and High Volume Use Flame Retardants in US Couches Reflective of the 2005 PentaBDE Phase Out
      Stapleton, Heather M.; Sharma, Smriti; Getzinger, Gordon; Ferguson, P. Lee; Gabriel, Michelle; Webster, Thomas F.; Blum, Arlene
      Environmental Science & Technology (2012), 46 (24), 13432-13439CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The California furniture flammability std., Tech. Bulletin 117 (TB 117), is believed to be a major driver of chem. flame retardant (FR) use in residential furniture in the US. With the phase-out of the polybrominated di-Ph ether (PBDE) FR mixt., PentaBDE, in 2005, alternative FR are increasingly being used to meet TB 117; however, it is unclear which chems. were being used and how frequently. To address this data gap, this work collected and analyzed 102 samples of polyurethane foam from residential couches purchased in the US from 1985 to 2010. Overall, chem. FR were detected in 85% of the couches. In samples purchased prior to 2005 (n = 41), PBDE assocd. with the PentaBDE mixt. (including BDE 47, 99, 100; PentaBDE) were the most common FR detected (39%), followed by tris(1,3-dichloroisopropyl) phosphate (TDCPP; 24%), a suspected human carcinogen. In samples purchased in 2005 or later (n = 61)m the most common FR detected were TDCPP (52%) and components assocd. with the Firemaster550 (FM 550) mixt. (18%). Since the 2005 phase-out of PentaBDE, use of TDCPP significantly increased. Also, a mixt. of non-halogenated organophosphate FR, including tri-Ph phosphate (TPP), tris(4-butylphenyl) phosphate (TBPP), and a mix of butylphenyl phosphate isomers, were obsd. in 13% of couch samples purchased in 2005 or later. Overall, the prevalence of FR (and PentaBDE) was higher in couches bought in California vs. elsewhere, although the difference was not quite significant (p = 0.054 for PentaBDE). The difference was greater before 2005 than after, suggesting TB 117 is becoming a de-facto std. across the US. This work detd. the presence of a TB 117 label predicted the presence of a FR; however, lack of a label did not predict the absence of a FR. Following the PentaBDE phase-out, an increased no. of flame retardants was obsd. on the market. With these results and the potential for human exposure to FR, health studies should be conducted on the types of FR identified here.
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    24. 24
      Decabromodiphenylether: An Investigation of Non-Halogen Substitutes in Electronic Enclosure and Textile Applications; Lowell Center for Sustainable Production, University of Massachusetts Lowell: Lowell, MA, 2005.
      There is no corresponding record for this reference.
    25. 25
      Ghanem, R.; Delmani, F.-A. Kinetics of thermal and photolytic degradation of decabromodiphenyl ether (BDE 209) in backcoated textile samples. J. Anal. Appl. Pyrolysis 2012, 98, 79– 85,  DOI: 10.1016/j.jaap.2012.09.001
      25
      Kinetics of thermal and photolytic degradation of decabromodiphenyl ether (BDE 209) in backcoated textile samples
      Ghanem, Raed; Delmani, Fatima-Azzahra
      Journal of Analytical and Applied Pyrolysis (2012), 98 (), 79-85CODEN: JAAPDD; ISSN:0165-2370. (Elsevier B.V.)
      Kinetics of the thermal and photolytic degrdn. of decabromodiphenyl ether (DBE 209) was studied using HPLC. Samples lost an amt. of ∼8.4% (wt./wt.), 24% (wt./wt.), 39.4% (wt./wt.) and 28.5% of the amt. of DBE 209 originally present in the samples due to ageing at 25, 60, 90° C and UV exposure, resp. The thermal and photolytic release was found to follow the first order kinetics with rate consts. estd. to be 3.6 × 10-3, 1.03 × 10-2, 3.6 × 10-2 and 3.94 × 10-2 day-1, resp. Ageing of the textile samples enhanced the release of the DBE 209 from the backcoated textile. Photodegrdn. of BDE 209 into lower congeners of brominated flame retardants was also obsd. for the UV-aged samples.Migration of DBE 209 from the backcoated textile into biol. fluids was studied using Head-over-Heels and contact-Blotting test for unaged, thermally and UV aged samples. The presence of biol. fluids (sweat, saliva and juice) was found to enhance the migration of DBE 209 compared to water. Migration of BDE 209 into artificial biol. fluids is significantly increased for samples previously exposed to UV radiation or thermally aged. An increase from 0.6% (wt./wt.) to a max. of 2% (wt./wt.) of the amt. of BDE 209 migrated into artificial biol. fluids due to ageing conditions in the presence of biol. fluid was recorded.
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    26. 26
      Abbasi, G.; Buser, A. M.; Soehl, A.; Murray, M. W.; Diamond, M. L. Stocks and flows of PBDEs in products from use to waste in the U.S. and Canada from 1970 to 2020. Environ. Sci. Technol. 2015, 49 (3), 1521– 8,  DOI: 10.1021/es504007v
      26
      Stocks and Flows of PBDEs in Products from Use to Waste in the U.S. and Canada from 1970 to 2020
      Abbasi, Golnoush; Buser, Andreas M.; Soehl, Anna; Murray, Michael W.; Diamond, Miriam L.
      Environmental Science & Technology (2015), 49 (3), 1521-1528CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The time-dependent stock of PBDEs contained in in-use products (excluding building materials and large vehicles) was estd. for the U.S. and Canada from 1970 to 2020 based on product consumption patterns, PBDE contents, and product lifespan. The stocks of penta- and octaBDE peaked in in-use products at 17,000 (95% confidence interval: 6000-70 000) and 4000 (1000-50 000) tonnes in 2004, resp., and for decaBDE at 140,000 (40,000-300,000) tonnes in 2008. Products dominating PBDE usage were polyurethane foam used in furniture (65% of pentaBDE), casings of elec. and electronic equipment or EEE (80% of octaBDE), and EEE and automotive seating (35% of decaBDE for each category). The largest flow of PBDEs in products, excluding automotive sector, to the waste phase occurred between 2005 and 2008 at ∼10,000 tonnes per yr. Total consumption of penta-, octa-, and decaBDE from 1970 to 2020 in products considered was estd. at ∼46,000, ∼25,000, and ∼380,000 tonnes, resp. Per capita usage was estd. at 10-250, 10-150, and 200-2000 g/capita y for penta-, octa-, and decaBDE, resp., over the time span. Considering only the first use (no reuse and/or storage) of PBDE-contg. products, approx. 60% of the stock of PBDEs in 2014 or ∼70,000 tonnes, of which 95% is decaBDE, will remain in the use phase in 2020. Total emissions to air of all PBDEs from the in-use product stock was estd. at 70-700 tonnes between 1970 and 2020, with annual emissions of 0.4-4 tonnes/y for each of penta- and octaBDE and 0.35-3.5 tonnes/y for decaBDE in 2014.
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    27. 27
      Davis, E. F.; Stapleton, H. M. Photodegradation pathways of nonabrominated diphenyl ethers, 2-ethylhexyltetrabromobenzoate and di(2-ethylhexyl)tetrabromophthalate: identifying potential markers of photodegradation. Environ. Sci. Technol. 2009, 43 (15), 5739– 46,  DOI: 10.1021/es901019w
      27
      Photodegradation Pathways of Nonabrominated Diphenyl Ethers, 2-Ethylhexyltetrabromobenzoate and Di(2-ethylhexyl)tetrabromophthalate: Identifying Potential Markers of Photodegradation
      Davis, Elizabeth F.; Stapleton, Heather M.
      Environmental Science & Technology (2009), 43 (15), 5739-5746CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Photodegrdn. kinetics of several polybrominated di-Ph ethers (PBDEs), particularly decabromodiphenyl ether (PBDE 209), have been reported in various matrixes, demonstrating that it photodegrades primarily via debromination. However, it has been difficult to det. the primary pathways by which Br is cleaved from PBDE 209 to form nona- and octabrominated congeners. The photodegrdn. of 3 nonaBDE congeners (i.e., PBDE 206, 207, and 208) was examd. individually in 3 different solvents exposed to natural sunlight and then analyzed to identify the primary degrdn. products. Rapid degrdn. of nonaBDEs (half-lives 4.25-12.78 min) was obsd. coincident with formation of octa- and heptabrominated PBDEs. PBDE 207 photodegraded most rapidly while PBDE 206 photodegraded the slowest. The photodegrdn. pathways of each nonaBDE congener were consistent among the different solvent matrixes tested; however, mass balances varied with the type of solvent used in the expt. (recovery 76-95%). The octabrominated congener, PBDE 202, and the ratio of PBDE 197 to PBDE 201, were identified as congeners that may serve as environmental markers of photolytic debromination of decaBDE. Addnl. photodegrdn. studies were conducted with 2 new brominated flame retardants used in replacements for pentaBDE mixts.: 2-ethylhexyltetrabromobenzoate (TBB) and di(2-ethylhexyl)-tetrabromophthalate (TBPH). Both TBB and TBPH underwent photolysis more slowly than nonaBDEs (half-lives 85.70-220.17 min) and primarily formed debrominated products.
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    28. 28
      Covaci, A.; Gerecke, A. C.; Law, R. J.; Voorspoels, S.; Kohler, M.; Heeb, N. V.; Leslie, H.; Allchin, C. R.; De Boer, J. Hexabromocyclododecanes (HBCDs) in the environment and humans: a review. Environ. Sci. Technol. 2006, 40 (12), 3679– 88,  DOI: 10.1021/es0602492
      28
      Hexabromocyclododecanes (HBCDs) in the environment and humans: A Review
      Covaci, Adrian; Gerecke, Andreas C.; Law, Robin J.; Voorspoels, Stefan; Kohler, Martin; Heeb, Norbert V.; Leslie, Heather; Allchin, Collin R.; De Boer, Jacob
      Environmental Science & Technology (2006), 40 (12), 3679-3688CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      A review. Hexabromocyclododecanes (HBCDs) are brominated aliph. cyclic hydrocarbons used as flame retardants in thermal insulation building materials, upholstery textiles, and electronics. As a result of their widespread use and their phys. and chem. properties, HBCDs are now ubiquitous contaminants in the environment and humans. This article summarizes HBCD concns. in several environmental compartments and analyzes these data in terms of point sources vs. diffuse sources, biomagnification potential, stereoisomer profiles, time trends, and global distribution. Generally, higher concns. were measured in samples (air, sediment, and fish) collected near point sources (plants producing or processing HBCDs), while lower concns. were recorded in samples from locations with no obvious sources of HBCDs. High concns. were measured in top predators, such as marine mammals and birds of prey (≤9600 and 19,200 ng/g lipid wt., resp.), suggesting a biomagnification potential for HBCDs. Relatively low HBCD concns. were reported in the few human studies conducted to date (median values varied 0.35-1.1 ng/g lipid wt.). HBCD levels in biota are increasing slowly and seem to reflect the local market demand. One important observation is the shift from the high percentage of the γ-HBCD stereoisomer in the tech. products to a dominance of the α-HBCD stereoisomer in biol. samples. A combination of factors such as variations in soly., partitioning behavior, uptake, and, possibly, selective metab. of individual isomers may explain the obsd. changes in stereoisomer patterns. Recommendations for further work include research on how HBCDs are transferred from products into the environment upon prodn., use, and disposal. Time trends need to be analyzed more in detail, including HBCD stereoisomers, and more data on terrestrial organisms are needed, esp. for humans. Whenever possible, HBCDs should be analyzed as individual stereoisomers to address their fate and effects.
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    29. 29
      Company Strategies ICL-IP closes HBCD flame retardant production line. Additives for Polymers 2015, 2015 (9), 7– 8,  DOI: 10.1016/S0306-3747(15)30122-6
      There is no corresponding record for this reference.
    30. 30
      Hess, G., Industry To Phase Out decaBDE. Chem. Eng. News. https://cen.acs.org/articles/87/web/2009/12/Industry-Phase-decaBDE.html (July 23, 2020).
      There is no corresponding record for this reference.
    31. 31
      Bello, A.; Carignan, C. C.; Xue, Y.; Stapleton, H. M.; Bello, D. Exposure to organophosphate flame retardants in spray polyurethane foam applicators: Role of dermal exposure. Environ. Int. 2018, 113, 55– 65,  DOI: 10.1016/j.envint.2018.01.020
      31
      Exposure to organophosphate flame retardants in spray polyurethane foam applicators: Role of dermal exposure
      Bello, Anila; Carignan, Courtney C.; Xue, Yalong; Stapleton, Heather M.; Bello, Dhimiter
      Environment International (2018), 113 (), 55-65CODEN: ENVIDV; ISSN:0160-4120. (Elsevier Ltd.)
      Spray polyurethane foam (SPF) is a highly effective thermal insulation material that has seen considerable market growth in the past decade. Organophosphate flame retardants (PFRs) are added to SPF formulations to meet fire code requirements. A common flame retardant used in SPF formulations is tris 1-chloro 2-Pr phosphate (TCIPP), a suspected endocrine disruptor. Exposure monitoring efforts during SPF applications have focused primarily on the isocyanate component, a potent respiratory and dermal sensitizer. However, to our knowledge, there is no monitoring data for TCIPP. To characterize occupational exposures to TCIPP and other flame retardants during SPF insulation. Workers at four SPF insulation sites and one foam removal site (total n = 14) were recruited as part of this pilot study. Personal inhalation exposure to TCIPP was monitored with a CIP-10MI inhalable sampler and potential dermal exposure was assessed through the use of a glove dosimeter. Biomarkers of TCIPP and three other PFRs were measured in urine collected from workers pre-and post-shift. Linear mixed effect models were used to analyze assocns. of urinary biomarkers with inhalation and dermal exposures and paired t-tests were used to examine the difference on the means of urinary biomarkers pre-and post-shift. Chem. anal. of all species was performed with liq. chromatog.-electrospray ionization tandem mass spectrometry. Geometric mean (GM) concns. of TCIPP in personal air monitors and glove dosimeters collected from SPF applicators, 294.7 μg/m3 and 18.8 mg/pair resp. Overall, GM concns. of the two TCIPP urinary biomarkers BCIPP and BCIPHIPP and (6.2 and 88.8 μg/mL) were 26-35 times higher than reported in the general population. Post-shift levels of TCIPP biomarkers were higher than pre-shift even though workers at insulation sites wore supplied air respirators, gloves and coveralls. The urinary biomarkers for the other PFRs were not elevated post shift. Concns. of TCIPP on glove dosimeters were pos. assocd. with post-shift urinary TCIPP biomarkers (p < 0.05) whereas concns. in personal air samples were not. High levels of urinary biomarkers for TCIPP among SPF applicators, including post-shift, points to absorption of TCIPP during the work shift, in spite of the use of best industry exposure control practices. Dermal exposure appears to be an important, if not the primary exposure pathway for TCIPP, although inhalation or incidental ingestion of foam particles post-SPF application cannot be ruled out in this pilot study.
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