TY - JOUR
AU1 - Gravel,, Sabrina
AU2 - Aubin,, Simon
AU3 - Labrèche,, France
AB - Abstract Background Flame retardants (FRs) are widespread in common goods, and workers in some industries can be exposed to high concentrations. Numerous studies describe occupational exposure to FRs, but the diversity of methods and of reported results renders their interpretation difficult for researchers, occupational hygienists, and decision makers. Objectives The objectives of this paper are to compile and summarize the scientific knowledge on occupational exposure to FRs as well as to identify research gaps and to formulate recommendations. Methods Five databases were consulted for this systematic literature review (Embase, Medline [Pubmed], Global health, Web of Science, and Google Scholar), with terms related to occupational exposure and to FRs. Selected studies report quantitative measurements of exposure to organic FRs in a workplace, either in air, dust, or in workers’ biological fluids. The Preferred Reporting Items for Systematic reviews and Meta-Analyses statement guidelines were followed. Results The search yielded 1540 published articles, of which 58 were retained. The most frequently sampled FRs were polybrominated diphenyl ethers and novel brominated FRs. Offices and electronic waste recycling facilities were the most studied occupational settings, and the highest reported exposures were found in the latter, as well as in manufacturing of printed circuit boards, in aircrafts, and in firefighters. There were recurrent methodological issues, such as unstandardized and ill-described air and dust sampling, as well as deficient statistical analyses. Conclusions This review offers several recommendations. Workplaces such as electronic waste recycling or manufacturing of electronics as well as firefighters and aircraft personnel should be granted more attention from researchers and industrial hygienists. Methodical and standardized occupational exposure assessment approaches should be employed, and data analysis and reporting should be more systematic. Finally, more research is needed on newer chemical classes of FRs, on occupational exposure pathways, and on airborne FR particle distribution. brominated diphenyl ethers, electronic waste recycling, firefighters, flame retardants, occupational exposure, sampling methods, systematic review Introduction Organic flame retardants (FRs) are chemicals used to slow down or prevent the burning process of fabrics, plastics, and other materials to which they are added (Dishaw et al., 2014). Various FRs have been introduced in consumer goods at an increasing pace since the mid-twentieth century to meet fire safety standards. A non-negligible background exposure level can be detected in the serum and urine of the general population (Brasseur et al., 2014; Butt et al., 2014; Fromme et al., 2015; Gravel et al., 2018). Among the organic compounds introduced since the 1970s, polybrominated diphenyl ethers (PBDEs) have been shown to bioaccumulate and to present endocrine activity; consequently, some commercial formulations were banned and gradually removed from the market (Besis and Samara, 2012; Cowell et al., 2017). PBDEs have been superseded by novel brominated FRs (NBFRs), such as hexabromobenzene (HBB) and tetrabromobisphenol A (TBBPA) (Covaci et al., 2011), and more recently by polychlorinated (Dechlorane plus) and various organophosphate (OPs) compounds, such as tris (1-chloro-2-propyl) phosphate (TDCiPP) and triphenyl phosphate (TPhP) (Tao et al., 2016; Hoffman et al., 2017a). Despite the ban of specific formulations of FRs and the withdrawal of some commercial mixtures, those substances may still be found in common goods and can, for years on, off-gas or detach from the materials, adsorb to dust, and therefore be released in the environment (Takigami et al., 2008; Webster et al., 2009; Liagkouridis et al., 2014). Some of the novel formulations, albeit less bioaccumulative, are also suspected to have endocrine active properties or to induce oxidative stress in living organisms (Wu et al., 2012; Hoffman et al., 2017b; Preston et al., 2017; Hill et al., 2018). As for many contaminants, occupational exposure to FRs can be much higher than environmental exposure (Semple, 2005). Indeed, some of the highest concentrations in dust were measured in occupational settings such as offices, aircrafts and electronic waste (e-waste) recycling facilities, as opposed to levels found in house dust (Dodson et al., 2012; Deng et al., 2014; Strid et al., 2014; Li et al., 2015). To date, most evidence on health effects of FRs and risk assessments has been gathered on children, or in animal and in vitro studies (He et al., 2011; Lyche et al., 2015). As the dose–response evidence on adverse effects in exposed adults is still scarce, no occupational exposure limit values (OELs) have been proposed. As more and more researchers, industrial hygienists, and occupational physicians are striving to assess exposure to FRs in several environments and workplaces, our understanding of the actual importance of these compounds is contingent on thorough and reproducible exposure measurements. A small number of reviews on exposure to FRs in various environments have been published, but they focused on home or environmental exposure (Frederiksen et al., 2009; Mercier et al., 2011; Sverko et al., 2011; Besis and Samara, 2012; Ni et al., 2013; Coelho et al., 2014; Yu et al., 2016). The objectives of this systematic review are to compile and lay a critical eye on published quantitative assessments of occupational exposure to organic FRs in dust, air, or biological fluids in order to report the concentrations found in various formal workplaces and to identify exposure assessment gaps that would benefit from improvement. Methods This systematic review follows the Preferred Reporting Items for Systematic reviews and Meta-Analyses (PRISMA) statement guidelines (Moher et al., 2009). The PRISMA checklist for this systematic review is provided in Supplementary Table 1, available at Annals of Work Exposures and Health online. Search strategy description Five databases were searched for papers published from database inception until July 2018: Embase, Medline (PubMed), Global Health, Web of Science and Google Scholar (Bramer et al., 2017). The detailed search strategy is described in Supplementary Table 2, available at Annals of Work Exposures and Health online. The broad search terms ‘occupational exposure’ and ‘flame retardants’ were used and restricted to studies on humans. The search in Google Scholar produced more than 15 000 results, of which 1000 were consulted for identification of additional relevant publications. There were no restrictions of language or publication date. A consultation of the reference list of other review papers was also performed. Inclusion and exclusion criteria To be included in the review, a study had to report a quantitative assessment of occupational exposure to an organic FR, or an epidemiological study that included at least one group of workers and presented a quantitative exposure assessment to FRs. Based on recommendations for industrial hygiene assessments, sampling media included were air (personal or stationary active sampling), dust (collected by either surface wipe sampling or vacuuming), blood (serum or plasma), and urine (American Conference of Governmental Industrial Hygienists, 2015). In order to allow comparison of exposure measurement data to OELs, the American Industrial Hygienists Association (AIHA) recommends that at least six measurements per similar exposure group or task be taken in a given workplace (Waters et al., 2015). However, as very few studies in this review would have met this criterion, the number of required measurements for inclusion was set to at least three measurements per sampling medium (air, dust, blood or urine sample) per workplace in a given study, which still allows for some interpretation of levels of exposure, keeping in mind that the variability could be quite substantial. In the occurrence of a sample size smaller than three per workplace, a study with a total sample size of six per industrial group was deemed acceptable. Where the number of samples was not reported or if it was unclear whether the workplace was in a formal sector, the authors of the paper were contacted. We excluded studies on children’s exposure or on population living in the vicinity of contaminated sites, assessments in informal workplaces (such as in Leung et al. (2011), where makeshift workshops are part of the workers’ dwellings), case studies, ecological studies, studies that focused only on household exposure, toxicokinetics research, reviews, letters to the editor, and conference abstracts. Individual studies were not assessed for risk of exposure bias. Data collection After a preliminary assessment of the relevance of each study from the summary by one reviewer (SG), full texts of the selected publications were obtained. Eligibility was assessed independently by two reviewers (SG and FL), and disagreement was resolved by consensus. A data extraction sheet was developed, tested with the first 10 references, and then revised to finally include: publication year and country where the study was conducted, aim of the study, methodological characteristics (sample size and study design), media used for exposure assessment (air, dust, serum, urine), FRs assessed, reported exposure data, data analysis preparation (censored data imputation method, reporting of the percentage of values below the limit of detection, etc.), and statistical analyses. Results were extracted for the most commonly cited FRs by one reviewer (SG) and a sample of 10% of articles was checked by a second reviewer (FL). They comprised for PBDEs: congeners 2,2',4,4'-Tetrabromodiphenyl ether (BDE47), 2,2',3,4,4',5',6-Heptabromodiphenyl ether (BDE183), and decabromodiphenyl ether (BDE209); for NBFRs: hexabromocyclododecane and TBBPA; for chlorinated FRs: syn- and anti-Dechlorane Plus; and for OPs: Tris(1,3-dichloroisopropyl)phosphate (TDCiPP) and TPhP (or corresponding major urinary metabolites bis-(2-chloroisopropyl) phosphate and diphenyl phosphate. Statistical analyses For FRs with detailed data available in the articles, additional central tendency metrics (geometric mean, arithmetic mean, and standard deviation) were calculated when >50% of measures were above the limit of detection (otherwise, these metrics were not calculated and the FR was not reported), using either the substitution method for censored data mentioned in the paper or the value 0 if not specified (Thuresson et al., 2005; Thomsen et al., 2007; Batterman et al., 2010; Schecter et al., 2010; Schindler et al., 2014; Strid et al., 2014). When means were available for BDE47, BDE183, and BDE209 (respectively, the main congener in commercial formulations of penta, octa, and deca-BDEs), weighted means were compiled for similar workplace groups. PBDE congener profiles were also calculated as percentage of the sum of BDE47, BDE183, and BDE209 for blood and dust levels, for which sufficient data were available. Results Study selection The flow diagram of study selection is available in Fig. 1. Three hundred and nine articles were screened and 116 of those were obtained and read throughout to assess eligibility. Fifty-eight studies, published between 1999 and July 2018, reported exposure to FRs in workplaces, with a sampling approach that met our inclusion criteria. Thirteen studies took place in China, 12 in the USA, 10 in Sweden, 3 in Taiwan, 3 in the UK, 2 each in Finland, Germany, Norway, South Korea, and Thailand, and 1 each in Belgium, Canada, Denmark, India, Pakistan, and South Africa. One was not attributed to a specific country because it took place in aircrafts during flights (Allen et al., 2013b). The main reasons for exclusion of studies were that the workplace studied was informal (mostly rudimentary e-waste recycling; n = 24) or that the sampling method or the matrix sampled did not meet selection criteria (e.g. passive air sampling, bulk dust sampling in vacuum bags, hair samples, clothing samples; n = 14). All excluded studies are listed in Supplementary Table 3, available at Annals of Work Exposures and Health online, with the reason for their exclusion. Figure 1 View largeDownload slide Flow diagram of study selection. Figure 1 View largeDownload slide Flow diagram of study selection. Characteristics of selected studies References of the studies included in this review, as well as the countries, workplaces, sampling media, sample sizes, and the chemical class of FRs, are listed in Table 1. Some occupational settings were more studied than others, such as offices (16 studies) and electronic waste (e-waste) recycling (15 studies). Aircrafts, classrooms, and daycare centres were also the focus of several studies, as well as various manufacturing industries. PBDEs were the most commonly measured, followed by novel brominated, organophosphate, and polychlorinated FRs. The two favoured exposure matrices were blood, with results presented from serum or plasma in 20 studies (23 different occupational settings), and dust in 20 studies as well, in which 16 different occupational settings were sampled mainly by dust vacuuming. Stationary air sampling was used in 16 studies and personal air sampling in 6, representing altogether 14 occupational settings. Finally, urinary biomarkers were used in four studies, in six different occupational settings. Most studies analysed the different sampling media by gas chromatography coupled with mass spectrometry (GC-MS), operated in different modes, including electron impact ionization and selective ion monitoring, except Bello et al. (2018) and Harrad et al. (2010) who used liquid chromatography-electrospray ionization tandem mass spectrometry. Table 1. Workplaces sampled, country of assessment, number of samples per matrix and group of FRs sampled for all references included in the review. Workplace Country Number of samples per matrix Flame retardant Reference Dust Air(P) Air(A) Blood Urine PBDEs NBFRs OPFRs ClFRs Aircraft USA 40 ● ● ● ● Allen et al. (2013a) Several 59 ● Allen et al. (2013b) USA 30 ● Schecter et al. (2010) Germany 332 ● Schindler et al. (2013) Sweden 13 41 ● Strid et al. (2014) Aircraft maintenance Germany 10 ● Schindler et al. (2014) Sweden 6 9 27 ● Strid et al. (2014) Carpet layers USA 3 ●  a Stapleton et al. (2008) Catering China 61 ● Wang et al. (2012) Classrooms, daycare centres, universities UK 36 ● Ali et al. (2011) Pakistan 16 ●  a ● Ali et al. (2014) UK 28 ● Brommer and Harrad (2015) Sweden 10 20 ● Bergh et al. (2011) UK 43 ● ● Harrad et al. (2010) UK 17 ● Harrad et al. (2004) China 4 ● Kang et al. (2011) Denmark 151 ● Langer et al. (2016) Sweden 10 ● Strid et al. (2014) China 16 ● Wu et al. (2016) Clothing store, shopping mall Pakistan 15 ●  a ● Ali et al. (2014) China 5 ● Kang et al. (2011) Computer classroom Taiwan 4 ● Chang et al. (2009) Finland 3 ● Makinen et al. (2009) Computer technicians Sweden 19 ● ● Jakobsson et al. (2002) Construction USA 14 24 ● Bello et al. (2018) Electronic repair shop or store South Africa 3 ● Abafe and Martincigh (2015) Pakistan 30 ●  a ● Ali et al. (2014) E-waste recycling South Africa 12 ● Abafe and Martincigh (2015) China 30 ● ● Deng et al. (2014) India 25 ● Eguchi et al. (2012) Canada 7 ● Guo et al. (2018) China 15 ● Guo et al. (2015) Sweden 54 ●  a Julander et al. (2005a) Sweden 11 ● Julander et al. (2005b) Finland 12 6 ● Makinen et al. (2009) Thailand 10 ● Muenhor et al. (2017) Sweden 12 ● Pettersson-Julander et al. (2004) Finland 45 ● ● ● Rosenberg et al. (2011) Sweden 19 ● Sjödin et al. (1999) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) Sweden 25 ● Thuresson et al. (2006a) E-waste storage facilities Thailand 25 ● ● Muenhor et al. (2010) Firestation USA 101 ● Park et al. (2015) USA 12 ● ● Shaw et al. (2013) Foam recycling USA 12 ●  a Stapleton et al. (2008) Furniture workshop Finland 2 7 ● Makinen et al. (2009) Gymnastic training facility USA 12b ● ● ● Ceballos et al. (2018) Hospitals, medical clinics Taiwan 9 ● Chou et al. (2017) China 16 ● Kang et al. (2011) Sweden 20 ● Sjödin et al. (1999) Hotels China 26 ● Tao et al. (2018) Laboratory Norway 5 ●  a ● Thomsen et al. (2001) Leather factory China 49 ● Wang et al. (2012) Manufacturing of cables Sweden 19 ● Thuresson et al. (2005) Manufacturing of circuit board Finland 4 6 ● Makinen et al. (2009) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) China 36 36 ● Zhou et al. (2014) Manufacturing of Dechlorane plus China 35 ● Zhang et al. (2013) Manufacturing of electric appliances and electronics Taiwan 14 ● ● Chou et al. (2017) China 6 ● Kang et al. (2011) China 194 ● Wang et al. (2012) Manufacturing of expandable polystyrene Norway 30 20 ● Thomsen et al. (2007) Manufacturing of furniture, toys and textiles China 4 ● Kang et al. (2011) Manufacturing of rubber Sweden 11 ● Thuresson et al. (2005) Offices Belgium 6 ● Ali et al. (2011) USA 12 31 ● ● Batterman et al. (2010) Sweden 10 20 ● Bergh et al. (2011) UK 61 ● Brommer and Harrad (2015) USA 30 29 ● Carignan et al. (2013) China 6 ● Chen et al. (2008) China 20 ● Kang et al. (2011) China 92 ● Li et al. (2015) USA 137 ●  a Makey et al. (2016) China 18 ● ● Newton et al. (2016) Sweden 20 ● Sjödin et al. (1999) Sweden 4 ● ● ● Sjödin et al. (2001) Sweden 21 ● Strid et al. (2014) USA 31 31 ● Watkins et al. (2011) USA 31b,c 31 ● Watkins et al. (2013) China 23 ● Wu et al. (2016) China 10 Yang et al. (2014) Slaughterhouse Sweden 17 ● Thuresson et al. (2005) Vehicle-dismantling factories Taiwan 6 ● Gou et al. (2016) Vehicle parking China 27 ● ● Li et al. (2016) Vehicles UK 21 ● Brommer and Harrad (2015) USA 20 ● Carignan et al. (2013) Waste incinerator South Korea 13 ●  a Kim et al. (2005) South Korea 30 ●  a Lee et al. (2007) Workplace Country Number of samples per matrix Flame retardant Reference Dust Air(P) Air(A) Blood Urine PBDEs NBFRs OPFRs ClFRs Aircraft USA 40 ● ● ● ● Allen et al. (2013a) Several 59 ● Allen et al. (2013b) USA 30 ● Schecter et al. (2010) Germany 332 ● Schindler et al. (2013) Sweden 13 41 ● Strid et al. (2014) Aircraft maintenance Germany 10 ● Schindler et al. (2014) Sweden 6 9 27 ● Strid et al. (2014) Carpet layers USA 3 ●  a Stapleton et al. (2008) Catering China 61 ● Wang et al. (2012) Classrooms, daycare centres, universities UK 36 ● Ali et al. (2011) Pakistan 16 ●  a ● Ali et al. (2014) UK 28 ● Brommer and Harrad (2015) Sweden 10 20 ● Bergh et al. (2011) UK 43 ● ● Harrad et al. (2010) UK 17 ● Harrad et al. (2004) China 4 ● Kang et al. (2011) Denmark 151 ● Langer et al. (2016) Sweden 10 ● Strid et al. (2014) China 16 ● Wu et al. (2016) Clothing store, shopping mall Pakistan 15 ●  a ● Ali et al. (2014) China 5 ● Kang et al. (2011) Computer classroom Taiwan 4 ● Chang et al. (2009) Finland 3 ● Makinen et al. (2009) Computer technicians Sweden 19 ● ● Jakobsson et al. (2002) Construction USA 14 24 ● Bello et al. (2018) Electronic repair shop or store South Africa 3 ● Abafe and Martincigh (2015) Pakistan 30 ●  a ● Ali et al. (2014) E-waste recycling South Africa 12 ● Abafe and Martincigh (2015) China 30 ● ● Deng et al. (2014) India 25 ● Eguchi et al. (2012) Canada 7 ● Guo et al. (2018) China 15 ● Guo et al. (2015) Sweden 54 ●  a Julander et al. (2005a) Sweden 11 ● Julander et al. (2005b) Finland 12 6 ● Makinen et al. (2009) Thailand 10 ● Muenhor et al. (2017) Sweden 12 ● Pettersson-Julander et al. (2004) Finland 45 ● ● ● Rosenberg et al. (2011) Sweden 19 ● Sjödin et al. (1999) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) Sweden 25 ● Thuresson et al. (2006a) E-waste storage facilities Thailand 25 ● ● Muenhor et al. (2010) Firestation USA 101 ● Park et al. (2015) USA 12 ● ● Shaw et al. (2013) Foam recycling USA 12 ●  a Stapleton et al. (2008) Furniture workshop Finland 2 7 ● Makinen et al. (2009) Gymnastic training facility USA 12b ● ● ● Ceballos et al. (2018) Hospitals, medical clinics Taiwan 9 ● Chou et al. (2017) China 16 ● Kang et al. (2011) Sweden 20 ● Sjödin et al. (1999) Hotels China 26 ● Tao et al. (2018) Laboratory Norway 5 ●  a ● Thomsen et al. (2001) Leather factory China 49 ● Wang et al. (2012) Manufacturing of cables Sweden 19 ● Thuresson et al. (2005) Manufacturing of circuit board Finland 4 6 ● Makinen et al. (2009) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) China 36 36 ● Zhou et al. (2014) Manufacturing of Dechlorane plus China 35 ● Zhang et al. (2013) Manufacturing of electric appliances and electronics Taiwan 14 ● ● Chou et al. (2017) China 6 ● Kang et al. (2011) China 194 ● Wang et al. (2012) Manufacturing of expandable polystyrene Norway 30 20 ● Thomsen et al. (2007) Manufacturing of furniture, toys and textiles China 4 ● Kang et al. (2011) Manufacturing of rubber Sweden 11 ● Thuresson et al. (2005) Offices Belgium 6 ● Ali et al. (2011) USA 12 31 ● ● Batterman et al. (2010) Sweden 10 20 ● Bergh et al. (2011) UK 61 ● Brommer and Harrad (2015) USA 30 29 ● Carignan et al. (2013) China 6 ● Chen et al. (2008) China 20 ● Kang et al. (2011) China 92 ● Li et al. (2015) USA 137 ●  a Makey et al. (2016) China 18 ● ● Newton et al. (2016) Sweden 20 ● Sjödin et al. (1999) Sweden 4 ● ● ● Sjödin et al. (2001) Sweden 21 ● Strid et al. (2014) USA 31 31 ● Watkins et al. (2011) USA 31b,c 31 ● Watkins et al. (2013) China 23 ● Wu et al. (2016) China 10 Yang et al. (2014) Slaughterhouse Sweden 17 ● Thuresson et al. (2005) Vehicle-dismantling factories Taiwan 6 ● Gou et al. (2016) Vehicle parking China 27 ● ● Li et al. (2016) Vehicles UK 21 ● Brommer and Harrad (2015) USA 20 ● Carignan et al. (2013) Waste incinerator South Korea 13 ●  a Kim et al. (2005) South Korea 30 ●  a Lee et al. (2007) Air(P), personal sample; Air(A), ambient sample; PBDEs, polybrominated diphenyl ethers; NBFRs, novel brominated flame retardants; OPFRs, organophosphate flame retardants; ClFRs, chlorinated flame retardants aCongener BDE209 was not measured bSurface wipes cn = 14 for BDE209 View Large Table 1. Workplaces sampled, country of assessment, number of samples per matrix and group of FRs sampled for all references included in the review. Workplace Country Number of samples per matrix Flame retardant Reference Dust Air(P) Air(A) Blood Urine PBDEs NBFRs OPFRs ClFRs Aircraft USA 40 ● ● ● ● Allen et al. (2013a) Several 59 ● Allen et al. (2013b) USA 30 ● Schecter et al. (2010) Germany 332 ● Schindler et al. (2013) Sweden 13 41 ● Strid et al. (2014) Aircraft maintenance Germany 10 ● Schindler et al. (2014) Sweden 6 9 27 ● Strid et al. (2014) Carpet layers USA 3 ●  a Stapleton et al. (2008) Catering China 61 ● Wang et al. (2012) Classrooms, daycare centres, universities UK 36 ● Ali et al. (2011) Pakistan 16 ●  a ● Ali et al. (2014) UK 28 ● Brommer and Harrad (2015) Sweden 10 20 ● Bergh et al. (2011) UK 43 ● ● Harrad et al. (2010) UK 17 ● Harrad et al. (2004) China 4 ● Kang et al. (2011) Denmark 151 ● Langer et al. (2016) Sweden 10 ● Strid et al. (2014) China 16 ● Wu et al. (2016) Clothing store, shopping mall Pakistan 15 ●  a ● Ali et al. (2014) China 5 ● Kang et al. (2011) Computer classroom Taiwan 4 ● Chang et al. (2009) Finland 3 ● Makinen et al. (2009) Computer technicians Sweden 19 ● ● Jakobsson et al. (2002) Construction USA 14 24 ● Bello et al. (2018) Electronic repair shop or store South Africa 3 ● Abafe and Martincigh (2015) Pakistan 30 ●  a ● Ali et al. (2014) E-waste recycling South Africa 12 ● Abafe and Martincigh (2015) China 30 ● ● Deng et al. (2014) India 25 ● Eguchi et al. (2012) Canada 7 ● Guo et al. (2018) China 15 ● Guo et al. (2015) Sweden 54 ●  a Julander et al. (2005a) Sweden 11 ● Julander et al. (2005b) Finland 12 6 ● Makinen et al. (2009) Thailand 10 ● Muenhor et al. (2017) Sweden 12 ● Pettersson-Julander et al. (2004) Finland 45 ● ● ● Rosenberg et al. (2011) Sweden 19 ● Sjödin et al. (1999) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) Sweden 25 ● Thuresson et al. (2006a) E-waste storage facilities Thailand 25 ● ● Muenhor et al. (2010) Firestation USA 101 ● Park et al. (2015) USA 12 ● ● Shaw et al. (2013) Foam recycling USA 12 ●  a Stapleton et al. (2008) Furniture workshop Finland 2 7 ● Makinen et al. (2009) Gymnastic training facility USA 12b ● ● ● Ceballos et al. (2018) Hospitals, medical clinics Taiwan 9 ● Chou et al. (2017) China 16 ● Kang et al. (2011) Sweden 20 ● Sjödin et al. (1999) Hotels China 26 ● Tao et al. (2018) Laboratory Norway 5 ●  a ● Thomsen et al. (2001) Leather factory China 49 ● Wang et al. (2012) Manufacturing of cables Sweden 19 ● Thuresson et al. (2005) Manufacturing of circuit board Finland 4 6 ● Makinen et al. (2009) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) China 36 36 ● Zhou et al. (2014) Manufacturing of Dechlorane plus China 35 ● Zhang et al. (2013) Manufacturing of electric appliances and electronics Taiwan 14 ● ● Chou et al. (2017) China 6 ● Kang et al. (2011) China 194 ● Wang et al. (2012) Manufacturing of expandable polystyrene Norway 30 20 ● Thomsen et al. (2007) Manufacturing of furniture, toys and textiles China 4 ● Kang et al. (2011) Manufacturing of rubber Sweden 11 ● Thuresson et al. (2005) Offices Belgium 6 ● Ali et al. (2011) USA 12 31 ● ● Batterman et al. (2010) Sweden 10 20 ● Bergh et al. (2011) UK 61 ● Brommer and Harrad (2015) USA 30 29 ● Carignan et al. (2013) China 6 ● Chen et al. (2008) China 20 ● Kang et al. (2011) China 92 ● Li et al. (2015) USA 137 ●  a Makey et al. (2016) China 18 ● ● Newton et al. (2016) Sweden 20 ● Sjödin et al. (1999) Sweden 4 ● ● ● Sjödin et al. (2001) Sweden 21 ● Strid et al. (2014) USA 31 31 ● Watkins et al. (2011) USA 31b,c 31 ● Watkins et al. (2013) China 23 ● Wu et al. (2016) China 10 Yang et al. (2014) Slaughterhouse Sweden 17 ● Thuresson et al. (2005) Vehicle-dismantling factories Taiwan 6 ● Gou et al. (2016) Vehicle parking China 27 ● ● Li et al. (2016) Vehicles UK 21 ● Brommer and Harrad (2015) USA 20 ● Carignan et al. (2013) Waste incinerator South Korea 13 ●  a Kim et al. (2005) South Korea 30 ●  a Lee et al. (2007) Workplace Country Number of samples per matrix Flame retardant Reference Dust Air(P) Air(A) Blood Urine PBDEs NBFRs OPFRs ClFRs Aircraft USA 40 ● ● ● ● Allen et al. (2013a) Several 59 ● Allen et al. (2013b) USA 30 ● Schecter et al. (2010) Germany 332 ● Schindler et al. (2013) Sweden 13 41 ● Strid et al. (2014) Aircraft maintenance Germany 10 ● Schindler et al. (2014) Sweden 6 9 27 ● Strid et al. (2014) Carpet layers USA 3 ●  a Stapleton et al. (2008) Catering China 61 ● Wang et al. (2012) Classrooms, daycare centres, universities UK 36 ● Ali et al. (2011) Pakistan 16 ●  a ● Ali et al. (2014) UK 28 ● Brommer and Harrad (2015) Sweden 10 20 ● Bergh et al. (2011) UK 43 ● ● Harrad et al. (2010) UK 17 ● Harrad et al. (2004) China 4 ● Kang et al. (2011) Denmark 151 ● Langer et al. (2016) Sweden 10 ● Strid et al. (2014) China 16 ● Wu et al. (2016) Clothing store, shopping mall Pakistan 15 ●  a ● Ali et al. (2014) China 5 ● Kang et al. (2011) Computer classroom Taiwan 4 ● Chang et al. (2009) Finland 3 ● Makinen et al. (2009) Computer technicians Sweden 19 ● ● Jakobsson et al. (2002) Construction USA 14 24 ● Bello et al. (2018) Electronic repair shop or store South Africa 3 ● Abafe and Martincigh (2015) Pakistan 30 ●  a ● Ali et al. (2014) E-waste recycling South Africa 12 ● Abafe and Martincigh (2015) China 30 ● ● Deng et al. (2014) India 25 ● Eguchi et al. (2012) Canada 7 ● Guo et al. (2018) China 15 ● Guo et al. (2015) Sweden 54 ●  a Julander et al. (2005a) Sweden 11 ● Julander et al. (2005b) Finland 12 6 ● Makinen et al. (2009) Thailand 10 ● Muenhor et al. (2017) Sweden 12 ● Pettersson-Julander et al. (2004) Finland 45 ● ● ● Rosenberg et al. (2011) Sweden 19 ● Sjödin et al. (1999) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) Sweden 25 ● Thuresson et al. (2006a) E-waste storage facilities Thailand 25 ● ● Muenhor et al. (2010) Firestation USA 101 ● Park et al. (2015) USA 12 ● ● Shaw et al. (2013) Foam recycling USA 12 ●  a Stapleton et al. (2008) Furniture workshop Finland 2 7 ● Makinen et al. (2009) Gymnastic training facility USA 12b ● ● ● Ceballos et al. (2018) Hospitals, medical clinics Taiwan 9 ● Chou et al. (2017) China 16 ● Kang et al. (2011) Sweden 20 ● Sjödin et al. (1999) Hotels China 26 ● Tao et al. (2018) Laboratory Norway 5 ●  a ● Thomsen et al. (2001) Leather factory China 49 ● Wang et al. (2012) Manufacturing of cables Sweden 19 ● Thuresson et al. (2005) Manufacturing of circuit board Finland 4 6 ● Makinen et al. (2009) Sweden 6 ● ● ● Sjödin et al. (2001) Norway 5 ●  a ● Thomsen et al. (2001) China 36 36 ● Zhou et al. (2014) Manufacturing of Dechlorane plus China 35 ● Zhang et al. (2013) Manufacturing of electric appliances and electronics Taiwan 14 ● ● Chou et al. (2017) China 6 ● Kang et al. (2011) China 194 ● Wang et al. (2012) Manufacturing of expandable polystyrene Norway 30 20 ● Thomsen et al. (2007) Manufacturing of furniture, toys and textiles China 4 ● Kang et al. (2011) Manufacturing of rubber Sweden 11 ● Thuresson et al. (2005) Offices Belgium 6 ● Ali et al. (2011) USA 12 31 ● ● Batterman et al. (2010) Sweden 10 20 ● Bergh et al. (2011) UK 61 ● Brommer and Harrad (2015) USA 30 29 ● Carignan et al. (2013) China 6 ● Chen et al. (2008) China 20 ● Kang et al. (2011) China 92 ● Li et al. (2015) USA 137 ●  a Makey et al. (2016) China 18 ● ● Newton et al. (2016) Sweden 20 ● Sjödin et al. (1999) Sweden 4 ● ● ● Sjödin et al. (2001) Sweden 21 ● Strid et al. (2014) USA 31 31 ● Watkins et al. (2011) USA 31b,c 31 ● Watkins et al. (2013) China 23 ● Wu et al. (2016) China 10 Yang et al. (2014) Slaughterhouse Sweden 17 ● Thuresson et al. (2005) Vehicle-dismantling factories Taiwan 6 ● Gou et al. (2016) Vehicle parking China 27 ● ● Li et al. (2016) Vehicles UK 21 ● Brommer and Harrad (2015) USA 20 ● Carignan et al. (2013) Waste incinerator South Korea 13 ●  a Kim et al. (2005) South Korea 30 ●  a Lee et al. (2007) Air(P), personal sample; Air(A), ambient sample; PBDEs, polybrominated diphenyl ethers; NBFRs, novel brominated flame retardants; OPFRs, organophosphate flame retardants; ClFRs, chlorinated flame retardants aCongener BDE209 was not measured bSurface wipes cn = 14 for BDE209 View Large Sampling approach Stationary air samples were collected on 9 different types of substrates among 22 studies, the most common being a cartridge containing polyurethane foam and a glass fibre filter in 8 of them. XAD-2, a hydrophobic copolymer of styrene-divinylbenzene resin, was used as the absorbent in six of the studies, either using home-made sampling tubes (n = 2 studies) or Occupational Health and Safety Administration (OSHA) versatile samplers (OVS) (n = 4). Air sampling parameters of the selected studies are listed in Table 2. Table 2. Air sampling methods used in all references included in the review. Reference Substrate Pump Flow Sampling time Allen et al. (2013b) Sorbent tube (SKC No. 226-143) and in-house-prepared glass cartridges; XAD-2 and polyurethane foam Not mentioned 1.5–8.6 l min−1 Not mentioned Batterman et al. (2010) Polytetrafluoroethylene filters (47-mm diameter, 1-µm pore size) (SKC Inc., Eighty Four, PA), followed by pre-cleaned polyurethane foam (22 × 76 mm, SKC, Inc.), in custom glass cartridges. Not mentioned (‘Medium-flow sampling systems’) 15 l min−1 1 week Bello et al. (2018) • Aerosol dust: IOM inhalable sampler (25-mm quartz filter) • CIP 10-M rotating cup bioaerosol sampler with solution of butyl benzoate containing 5-mM 1-(9-anthracenylmethyl) piperazine • GilAir 3 (Sensidyne) • CIP-10MI sampler (Arelco, Fontenay-Sous-Bios Cedex, France) 2 l min−1 10 l min−1 15–176 min Bergh et al. (2011) Solid-phase extraction cartridges (IST, Hengoed, UK); aminopropyl silica AC-powered pump (N026.1.2AN.18; KNF Neuberger, Germany) Not mentioned (max. of ~2m3 h−1 according to manufacturer) 8 h Chang et al. (2009) Modified total suspended particulate inlet; polyurethane foam and glass fibre filter PS-1 high volume air sampler (General Metal Works, USA) 250 l min−1 24 h Chen et al. (2008) Polyurethane foam and glass fibre filter High-volume sampler 400–700 l min−1 8–10 h Gou et al. (2016) Glass cartridge; polyurethane foam and quartz fibre filter PS-1 sampler (Graseby Andersen, GA, USA) 225 l min−1 40 h Guo et al. (2015) Polyurethane foam plugs (60-cm diameter × 51-mm length, SKC Inc.) and glass fibre filter (90-mm diameter, pore size 0.1 µm, SKC Inc.) High-volume sampler model (TE-100, Tisch, NY, USA) 3 middle volume samplers (Lao Ying 2030, Qingdao Laoshan electronic instrument factory Co. Ltd., China) 220–280 l min−1 100 l min−1 8 h Guo et al. (2018) ORBO sampler: glass fibre filter (pore size 0.7 μm) with polyurethane foam (PUF/XAD/PUF, Sigma-Aldrich) Low-volume air samplers 5.5–10 l min−1 8–30 h Harrad et al. (2004) Total suspended particulate inlet modified to hold a teflon-coated glass fibre filter (pore size 0.6 µm) and precleaned polyurethane foam plugs (0.016 g cm-3, 827 cm3) High-volume sampler (Graseby Andersen, GA, USA) 600–800 l min−1 Depending on room volume (max. 24 h) Julander et al. (2005b) Open-face 25-mm cassette; SKC 2 aluminium cyclone, 25-mm cassette; IOM inhalable dust sampler, 25-mm cassette. All used with cellulose acetate filters Not mentioned 2 l min−1 16 h Li et al. (2016) Glass fibre filter (20.3× 25.4 cm, Whatman) and polyurethane foam (90× 65 mm id.) plug High-volume sampler Not mentioned 4.5–24 h Makinen et al. (2009) OVS (filter + XAD resin and polyurethane foam) IOM sampler (glass fibre filters) Personal pumps (SKC 224, SKC Ltd.) 0.98–1.05 l min−1 (OVS) 1.95–2.08 l min−1 (IOM) 119–663 min Newton et al. (2016) Glass fibre filters from Pall Corp., MI, USA (binder-free A/E borosilicate, 25-mm diameter) and polyurethane foam plugs from Specialplast AB, Gillinge, Sweden (diameter 15 mm, thickness 15 mm) Low volume pump 5 l min−1 •2.5 h day−1 for 28 days •2.5 days cont. Pettersson-Julander et al. (2004) Modified version of NIOSH method 0500 ‘’Particulates, not otherwise regulated’’, sampler with pre-washed XAD-2 adsorbent, and a cellulose pad onto which a glass fibre filter was placed Personal sampling pumps 2 l min−1 8 h Rosenberg et al. (2011) OVS (no. 226-30-16, SKC Ltd): glass fibre filter + 2 XAD-2 resin layers (270 and 140 mg), separated by PUF plugs Not mentioned 2.5 l min−1 191–408 min Sjödin et al. (2001) Anodized aluminum sampler, 25-mm, binder-free A/E borosilicate glass fibre filter (Gelman Sciences Inc.), 2 polyurethane foam plugs (15-mm diameter and thickness (special last AB) Personal pump (224-PCXR7, SKC Inc.) 3 l min−1 500 min Strid et al. (2014) OVS: glass fibre filter, two XAD-2 adsorbent layers (separated by polyurethane foam) Not mentioned 3 l min−1 8 h Thomsen et al. (2007) Total dust: 25-mm black Gelman cassettes (no. 4376, Pall) and 25-mm glass fibre microfibre filters (1.6-µm pore size, no. 1820025, Whatman), Millipore absorbent pads (no. AP1002500, Billerica). In-house-made pumps 2 l min−1 8 h Watkins et al. (2013) Glass tube casing; glass fibre filter (pore size 1 μm) with polyurethane foam plug (76 gm). Sampling pump 4 l min−1 48 h Yang et al. (2014) Cascade impactor; glass fibre filters Anderson eight-stage nonviable cascade impactor with a back-up filter (Tisch Environmental, Cleves, USA) 28.3 l min−1 48 h Zhou et al. (2014) Pre-baked glass fibre filters (11-cm diameter) Median-volume samplers 100 l min−1 8 h Reference Substrate Pump Flow Sampling time Allen et al. (2013b) Sorbent tube (SKC No. 226-143) and in-house-prepared glass cartridges; XAD-2 and polyurethane foam Not mentioned 1.5–8.6 l min−1 Not mentioned Batterman et al. (2010) Polytetrafluoroethylene filters (47-mm diameter, 1-µm pore size) (SKC Inc., Eighty Four, PA), followed by pre-cleaned polyurethane foam (22 × 76 mm, SKC, Inc.), in custom glass cartridges. Not mentioned (‘Medium-flow sampling systems’) 15 l min−1 1 week Bello et al. (2018) • Aerosol dust: IOM inhalable sampler (25-mm quartz filter) • CIP 10-M rotating cup bioaerosol sampler with solution of butyl benzoate containing 5-mM 1-(9-anthracenylmethyl) piperazine • GilAir 3 (Sensidyne) • CIP-10MI sampler (Arelco, Fontenay-Sous-Bios Cedex, France) 2 l min−1 10 l min−1 15–176 min Bergh et al. (2011) Solid-phase extraction cartridges (IST, Hengoed, UK); aminopropyl silica AC-powered pump (N026.1.2AN.18; KNF Neuberger, Germany) Not mentioned (max. of ~2m3 h−1 according to manufacturer) 8 h Chang et al. (2009) Modified total suspended particulate inlet; polyurethane foam and glass fibre filter PS-1 high volume air sampler (General Metal Works, USA) 250 l min−1 24 h Chen et al. (2008) Polyurethane foam and glass fibre filter High-volume sampler 400–700 l min−1 8–10 h Gou et al. (2016) Glass cartridge; polyurethane foam and quartz fibre filter PS-1 sampler (Graseby Andersen, GA, USA) 225 l min−1 40 h Guo et al. (2015) Polyurethane foam plugs (60-cm diameter × 51-mm length, SKC Inc.) and glass fibre filter (90-mm diameter, pore size 0.1 µm, SKC Inc.) High-volume sampler model (TE-100, Tisch, NY, USA) 3 middle volume samplers (Lao Ying 2030, Qingdao Laoshan electronic instrument factory Co. Ltd., China) 220–280 l min−1 100 l min−1 8 h Guo et al. (2018) ORBO sampler: glass fibre filter (pore size 0.7 μm) with polyurethane foam (PUF/XAD/PUF, Sigma-Aldrich) Low-volume air samplers 5.5–10 l min−1 8–30 h Harrad et al. (2004) Total suspended particulate inlet modified to hold a teflon-coated glass fibre filter (pore size 0.6 µm) and precleaned polyurethane foam plugs (0.016 g cm-3, 827 cm3) High-volume sampler (Graseby Andersen, GA, USA) 600–800 l min−1 Depending on room volume (max. 24 h) Julander et al. (2005b) Open-face 25-mm cassette; SKC 2 aluminium cyclone, 25-mm cassette; IOM inhalable dust sampler, 25-mm cassette. All used with cellulose acetate filters Not mentioned 2 l min−1 16 h Li et al. (2016) Glass fibre filter (20.3× 25.4 cm, Whatman) and polyurethane foam (90× 65 mm id.) plug High-volume sampler Not mentioned 4.5–24 h Makinen et al. (2009) OVS (filter + XAD resin and polyurethane foam) IOM sampler (glass fibre filters) Personal pumps (SKC 224, SKC Ltd.) 0.98–1.05 l min−1 (OVS) 1.95–2.08 l min−1 (IOM) 119–663 min Newton et al. (2016) Glass fibre filters from Pall Corp., MI, USA (binder-free A/E borosilicate, 25-mm diameter) and polyurethane foam plugs from Specialplast AB, Gillinge, Sweden (diameter 15 mm, thickness 15 mm) Low volume pump 5 l min−1 •2.5 h day−1 for 28 days •2.5 days cont. Pettersson-Julander et al. (2004) Modified version of NIOSH method 0500 ‘’Particulates, not otherwise regulated’’, sampler with pre-washed XAD-2 adsorbent, and a cellulose pad onto which a glass fibre filter was placed Personal sampling pumps 2 l min−1 8 h Rosenberg et al. (2011) OVS (no. 226-30-16, SKC Ltd): glass fibre filter + 2 XAD-2 resin layers (270 and 140 mg), separated by PUF plugs Not mentioned 2.5 l min−1 191–408 min Sjödin et al. (2001) Anodized aluminum sampler, 25-mm, binder-free A/E borosilicate glass fibre filter (Gelman Sciences Inc.), 2 polyurethane foam plugs (15-mm diameter and thickness (special last AB) Personal pump (224-PCXR7, SKC Inc.) 3 l min−1 500 min Strid et al. (2014) OVS: glass fibre filter, two XAD-2 adsorbent layers (separated by polyurethane foam) Not mentioned 3 l min−1 8 h Thomsen et al. (2007) Total dust: 25-mm black Gelman cassettes (no. 4376, Pall) and 25-mm glass fibre microfibre filters (1.6-µm pore size, no. 1820025, Whatman), Millipore absorbent pads (no. AP1002500, Billerica). In-house-made pumps 2 l min−1 8 h Watkins et al. (2013) Glass tube casing; glass fibre filter (pore size 1 μm) with polyurethane foam plug (76 gm). Sampling pump 4 l min−1 48 h Yang et al. (2014) Cascade impactor; glass fibre filters Anderson eight-stage nonviable cascade impactor with a back-up filter (Tisch Environmental, Cleves, USA) 28.3 l min−1 48 h Zhou et al. (2014) Pre-baked glass fibre filters (11-cm diameter) Median-volume samplers 100 l min−1 8 h View Large Table 2. Air sampling methods used in all references included in the review. Reference Substrate Pump Flow Sampling time Allen et al. (2013b) Sorbent tube (SKC No. 226-143) and in-house-prepared glass cartridges; XAD-2 and polyurethane foam Not mentioned 1.5–8.6 l min−1 Not mentioned Batterman et al. (2010) Polytetrafluoroethylene filters (47-mm diameter, 1-µm pore size) (SKC Inc., Eighty Four, PA), followed by pre-cleaned polyurethane foam (22 × 76 mm, SKC, Inc.), in custom glass cartridges. Not mentioned (‘Medium-flow sampling systems’) 15 l min−1 1 week Bello et al. (2018) • Aerosol dust: IOM inhalable sampler (25-mm quartz filter) • CIP 10-M rotating cup bioaerosol sampler with solution of butyl benzoate containing 5-mM 1-(9-anthracenylmethyl) piperazine • GilAir 3 (Sensidyne) • CIP-10MI sampler (Arelco, Fontenay-Sous-Bios Cedex, France) 2 l min−1 10 l min−1 15–176 min Bergh et al. (2011) Solid-phase extraction cartridges (IST, Hengoed, UK); aminopropyl silica AC-powered pump (N026.1.2AN.18; KNF Neuberger, Germany) Not mentioned (max. of ~2m3 h−1 according to manufacturer) 8 h Chang et al. (2009) Modified total suspended particulate inlet; polyurethane foam and glass fibre filter PS-1 high volume air sampler (General Metal Works, USA) 250 l min−1 24 h Chen et al. (2008) Polyurethane foam and glass fibre filter High-volume sampler 400–700 l min−1 8–10 h Gou et al. (2016) Glass cartridge; polyurethane foam and quartz fibre filter PS-1 sampler (Graseby Andersen, GA, USA) 225 l min−1 40 h Guo et al. (2015) Polyurethane foam plugs (60-cm diameter × 51-mm length, SKC Inc.) and glass fibre filter (90-mm diameter, pore size 0.1 µm, SKC Inc.) High-volume sampler model (TE-100, Tisch, NY, USA) 3 middle volume samplers (Lao Ying 2030, Qingdao Laoshan electronic instrument factory Co. Ltd., China) 220–280 l min−1 100 l min−1 8 h Guo et al. (2018) ORBO sampler: glass fibre filter (pore size 0.7 μm) with polyurethane foam (PUF/XAD/PUF, Sigma-Aldrich) Low-volume air samplers 5.5–10 l min−1 8–30 h Harrad et al. (2004) Total suspended particulate inlet modified to hold a teflon-coated glass fibre filter (pore size 0.6 µm) and precleaned polyurethane foam plugs (0.016 g cm-3, 827 cm3) High-volume sampler (Graseby Andersen, GA, USA) 600–800 l min−1 Depending on room volume (max. 24 h) Julander et al. (2005b) Open-face 25-mm cassette; SKC 2 aluminium cyclone, 25-mm cassette; IOM inhalable dust sampler, 25-mm cassette. All used with cellulose acetate filters Not mentioned 2 l min−1 16 h Li et al. (2016) Glass fibre filter (20.3× 25.4 cm, Whatman) and polyurethane foam (90× 65 mm id.) plug High-volume sampler Not mentioned 4.5–24 h Makinen et al. (2009) OVS (filter + XAD resin and polyurethane foam) IOM sampler (glass fibre filters) Personal pumps (SKC 224, SKC Ltd.) 0.98–1.05 l min−1 (OVS) 1.95–2.08 l min−1 (IOM) 119–663 min Newton et al. (2016) Glass fibre filters from Pall Corp., MI, USA (binder-free A/E borosilicate, 25-mm diameter) and polyurethane foam plugs from Specialplast AB, Gillinge, Sweden (diameter 15 mm, thickness 15 mm) Low volume pump 5 l min−1 •2.5 h day−1 for 28 days •2.5 days cont. Pettersson-Julander et al. (2004) Modified version of NIOSH method 0500 ‘’Particulates, not otherwise regulated’’, sampler with pre-washed XAD-2 adsorbent, and a cellulose pad onto which a glass fibre filter was placed Personal sampling pumps 2 l min−1 8 h Rosenberg et al. (2011) OVS (no. 226-30-16, SKC Ltd): glass fibre filter + 2 XAD-2 resin layers (270 and 140 mg), separated by PUF plugs Not mentioned 2.5 l min−1 191–408 min Sjödin et al. (2001) Anodized aluminum sampler, 25-mm, binder-free A/E borosilicate glass fibre filter (Gelman Sciences Inc.), 2 polyurethane foam plugs (15-mm diameter and thickness (special last AB) Personal pump (224-PCXR7, SKC Inc.) 3 l min−1 500 min Strid et al. (2014) OVS: glass fibre filter, two XAD-2 adsorbent layers (separated by polyurethane foam) Not mentioned 3 l min−1 8 h Thomsen et al. (2007) Total dust: 25-mm black Gelman cassettes (no. 4376, Pall) and 25-mm glass fibre microfibre filters (1.6-µm pore size, no. 1820025, Whatman), Millipore absorbent pads (no. AP1002500, Billerica). In-house-made pumps 2 l min−1 8 h Watkins et al. (2013) Glass tube casing; glass fibre filter (pore size 1 μm) with polyurethane foam plug (76 gm). Sampling pump 4 l min−1 48 h Yang et al. (2014) Cascade impactor; glass fibre filters Anderson eight-stage nonviable cascade impactor with a back-up filter (Tisch Environmental, Cleves, USA) 28.3 l min−1 48 h Zhou et al. (2014) Pre-baked glass fibre filters (11-cm diameter) Median-volume samplers 100 l min−1 8 h Reference Substrate Pump Flow Sampling time Allen et al. (2013b) Sorbent tube (SKC No. 226-143) and in-house-prepared glass cartridges; XAD-2 and polyurethane foam Not mentioned 1.5–8.6 l min−1 Not mentioned Batterman et al. (2010) Polytetrafluoroethylene filters (47-mm diameter, 1-µm pore size) (SKC Inc., Eighty Four, PA), followed by pre-cleaned polyurethane foam (22 × 76 mm, SKC, Inc.), in custom glass cartridges. Not mentioned (‘Medium-flow sampling systems’) 15 l min−1 1 week Bello et al. (2018) • Aerosol dust: IOM inhalable sampler (25-mm quartz filter) • CIP 10-M rotating cup bioaerosol sampler with solution of butyl benzoate containing 5-mM 1-(9-anthracenylmethyl) piperazine • GilAir 3 (Sensidyne) • CIP-10MI sampler (Arelco, Fontenay-Sous-Bios Cedex, France) 2 l min−1 10 l min−1 15–176 min Bergh et al. (2011) Solid-phase extraction cartridges (IST, Hengoed, UK); aminopropyl silica AC-powered pump (N026.1.2AN.18; KNF Neuberger, Germany) Not mentioned (max. of ~2m3 h−1 according to manufacturer) 8 h Chang et al. (2009) Modified total suspended particulate inlet; polyurethane foam and glass fibre filter PS-1 high volume air sampler (General Metal Works, USA) 250 l min−1 24 h Chen et al. (2008) Polyurethane foam and glass fibre filter High-volume sampler 400–700 l min−1 8–10 h Gou et al. (2016) Glass cartridge; polyurethane foam and quartz fibre filter PS-1 sampler (Graseby Andersen, GA, USA) 225 l min−1 40 h Guo et al. (2015) Polyurethane foam plugs (60-cm diameter × 51-mm length, SKC Inc.) and glass fibre filter (90-mm diameter, pore size 0.1 µm, SKC Inc.) High-volume sampler model (TE-100, Tisch, NY, USA) 3 middle volume samplers (Lao Ying 2030, Qingdao Laoshan electronic instrument factory Co. Ltd., China) 220–280 l min−1 100 l min−1 8 h Guo et al. (2018) ORBO sampler: glass fibre filter (pore size 0.7 μm) with polyurethane foam (PUF/XAD/PUF, Sigma-Aldrich) Low-volume air samplers 5.5–10 l min−1 8–30 h Harrad et al. (2004) Total suspended particulate inlet modified to hold a teflon-coated glass fibre filter (pore size 0.6 µm) and precleaned polyurethane foam plugs (0.016 g cm-3, 827 cm3) High-volume sampler (Graseby Andersen, GA, USA) 600–800 l min−1 Depending on room volume (max. 24 h) Julander et al. (2005b) Open-face 25-mm cassette; SKC 2 aluminium cyclone, 25-mm cassette; IOM inhalable dust sampler, 25-mm cassette. All used with cellulose acetate filters Not mentioned 2 l min−1 16 h Li et al. (2016) Glass fibre filter (20.3× 25.4 cm, Whatman) and polyurethane foam (90× 65 mm id.) plug High-volume sampler Not mentioned 4.5–24 h Makinen et al. (2009) OVS (filter + XAD resin and polyurethane foam) IOM sampler (glass fibre filters) Personal pumps (SKC 224, SKC Ltd.) 0.98–1.05 l min−1 (OVS) 1.95–2.08 l min−1 (IOM) 119–663 min Newton et al. (2016) Glass fibre filters from Pall Corp., MI, USA (binder-free A/E borosilicate, 25-mm diameter) and polyurethane foam plugs from Specialplast AB, Gillinge, Sweden (diameter 15 mm, thickness 15 mm) Low volume pump 5 l min−1 •2.5 h day−1 for 28 days •2.5 days cont. Pettersson-Julander et al. (2004) Modified version of NIOSH method 0500 ‘’Particulates, not otherwise regulated’’, sampler with pre-washed XAD-2 adsorbent, and a cellulose pad onto which a glass fibre filter was placed Personal sampling pumps 2 l min−1 8 h Rosenberg et al. (2011) OVS (no. 226-30-16, SKC Ltd): glass fibre filter + 2 XAD-2 resin layers (270 and 140 mg), separated by PUF plugs Not mentioned 2.5 l min−1 191–408 min Sjödin et al. (2001) Anodized aluminum sampler, 25-mm, binder-free A/E borosilicate glass fibre filter (Gelman Sciences Inc.), 2 polyurethane foam plugs (15-mm diameter and thickness (special last AB) Personal pump (224-PCXR7, SKC Inc.) 3 l min−1 500 min Strid et al. (2014) OVS: glass fibre filter, two XAD-2 adsorbent layers (separated by polyurethane foam) Not mentioned 3 l min−1 8 h Thomsen et al. (2007) Total dust: 25-mm black Gelman cassettes (no. 4376, Pall) and 25-mm glass fibre microfibre filters (1.6-µm pore size, no. 1820025, Whatman), Millipore absorbent pads (no. AP1002500, Billerica). In-house-made pumps 2 l min−1 8 h Watkins et al. (2013) Glass tube casing; glass fibre filter (pore size 1 μm) with polyurethane foam plug (76 gm). Sampling pump 4 l min−1 48 h Yang et al. (2014) Cascade impactor; glass fibre filters Anderson eight-stage nonviable cascade impactor with a back-up filter (Tisch Environmental, Cleves, USA) 28.3 l min−1 48 h Zhou et al. (2014) Pre-baked glass fibre filters (11-cm diameter) Median-volume samplers 100 l min−1 8 h View Large Environmental sampling methods were very diverse, and this was especially true for settled dust. Dust was almost exclusively collected via vacuum sampling, except for two studies that used surface wiping as well (Watkins et al., 2013; Ceballos et al., 2018). Some characteristics of the methods employed for dust vacuuming are listed in Supplementary Table 4, available at Annals of Work Exposures and Health online. Of the 19 studies that sampled settled dust, only 5 detailed their method, with the type of vacuum cleaner used, the collection apparatus fitted to the vacuum nozzle (or the use of the vacuum bag itself), and a description of the surface and area being sampled (Muenhor et al., 2010; Bergh et al., 2011; Kang et al., 2011; Li et al., 2015; Muenhor et al., 2017). Biological monitoring of FRs was performed in either blood or urine, depending on the chemicals. Brominated and chlorinated FRs are thought to undergo minimal metabolic transformation and therefore the parent compounds are measured directly in serum or plasma (Genuis et al., 2017; Sales et al., 2017). Most blood concentrations were adjusted on total blood lipids, but Wang et al. (2012) presented results as ng ml−1 of serum and Eguchi et al. (2012) in pg g−1 wet weight of serum. Organophosphate molecules are, on the other hand, rapidly metabolized and their metabolites can be measured in urine within a few hours (Hou et al., 2016). Carignan et al. (2013) and Tao et al. (2018) presented urinary concentrations adjusted on urine’s specific gravity, whereas Schindler et al. (2013) reported unadjusted results (but still showed the creatinine content of urine) and Schindler et al. (2014) presented both unadjusted results and results adjusted on creatinine. Summary of study findings The majority of selected studies (n = 46/58) had an exposure assessment primary endeavor. The others focused mostly on other objectives (e.g. methodological developments or health-risk assessment) but still presented exposure data. The lowest and highest detected means and the highest maxima for each sampling matrix are presented in Table 3. The metrics presented and their level of detail varied greatly between studies, which complicated their comparison: some studies presented medians with detailed quartiles, means with or without standard deviation, with or without a range, or geometric means and geometric standard deviations. Moreover, of the 52 studies that reported some values below the detection limit, 39 specified their imputation approach used in statistical analyses of the data, and only 29 presented the percentage of censored data for each FR. Table 3. Summary of the reported highest means and maxima for brominated and organophosphate esters FRs in dust, air, and blood. Substance Reported concentrationa Workplace (process or task) Country Reference Lowest detected mean Highest mean Highest max Air (ng m−3) BDE47 0.014 Vehicle-dismantling factories (daytime) Taiwan Gou et al. (2016) 343 E-waste recycling (printed wiring board heating) China Guo et al. (2015) 2 895 Office USA Watkins et al. (2013) BDE183 0.001 Computer classroom Taiwan Chang et al. (2009) 19.5 E-waste recycling Finland Rosenberg et al. (2011) 98.0 Aircraft International Allen et al. (2013b) BDE209 0.0023 Computer classroom Taiwan Chang et al. (2009) 2 170 E-waste recycling (crushing) China Guo et al. (2015) 2100 Aircraft USA Allen et al. (2013a) TPhP 0.1 Daycare Sweden Bergh et al. (2011) 850b 10 300 E-waste recycling Finland Makinen et al. (2009) TDCiPP 2.25 Offices China Yang et al. (2014) 90b 450 E-waste recycling Finland Makinen et al. (2009) TBBPA 0.0121 Offices (vapour phase) USA Batterman et al. (2010) 1150 Manufacturing of circuit boards (lamination) China Zhou, 2014 14 600 E-waste recycling Finland Makinen et al. (2009) ƩHBCDD 0.087 Office (low use) China Newton et al. (2016) 48 Aircraft Sweden Strid et al. (2014) 963 Aircraft maintenance Sweden Strid et al. (2014) Dust (ng g−1) BDE47 1.79 Office floor dust China Li et al. (2015) 6240 E-waste recycling (coarse crushing room) China Deng et al. (2014) 23 000 E-waste recycling (dismantling) Thailand Muenhor et al. (2017) BDE183 1.00 Clothing store Pakistan Ali et al. (2014) 22 100a E-waste recycling (shredding wires) China Deng et al. (2014) 12 970a Office floor dust USA Watkins et al. (2011) BDE209 65.0 Clothing store Pakistan Ali et al. (2014) 665 000 E-waste recycling (shredding wires) China Deng et al. (2014) 2 600 000 Aircraft (vent dust) USA Allen et al. (2013a) TPhP 88 Clothing store Pakistan Ali et al. (2014) 15 000 170 000 Vehicle UK Brommer and Harrad (2015) TDCiPP 11 Clothing store Pakistan Ali et al. (2014) 110 000 740 000 Vehicle UK Brommer and Harrad (2015) TBBPA 223 Office floor dust USA Batterman et al. (2010) 6940 9010 Office (dust in computer case) China Li et al. (2015) ƩHBCDD 8900 8900 Classrooms UK Harrad et al. (2010) 1 100 000 Aircraft (carpet) USA Allen et al. (2013a) Blood (ng g−1 lipids) BDE47 0.26 Catering China Wang et al. (2012) 52 Firestation USA Shaw et al. (2013) 540 Foam recyclers USA Stapleton et al. (2008) BDE183 0.148 Manufacturing of cable (measurements) Sweden Thuresson et al. (2005) 4.12 Waste incinerator South Korea Kim et al. (2005) 18.7 E-waste recycling Sweden Sjödin et al. (1999) BDE209 0.75 Leather factory China Wang et al. (2012) 52.4 268 Manufacturing of cables (miscellaneous) Sweden Thuresson et al. (2005) TBBPA 0.34 Laboratory Norway Thomsen et al. (2001) 27 88 Firestation USA Shaw et al. (2013) ƩHBCDD 162 218 Manufacturing of expandable polystyrene Norway Thomsen et al. (2007) Urine (µg l−1, adjusted on specific gravity) DPhP 0.24b Hotel China Tao et al. (2018) 2.96 Aircraft maintenance Germany Schindler et al. (2013) 302 Airline workers Germany Schindler et al. (2013) BDCPP 0.24b Hotel China Tao et al. (2018) 408 1760 Office USA Carignan et al. (2013) Substance Reported concentrationa Workplace (process or task) Country Reference Lowest detected mean Highest mean Highest max Air (ng m−3) BDE47 0.014 Vehicle-dismantling factories (daytime) Taiwan Gou et al. (2016) 343 E-waste recycling (printed wiring board heating) China Guo et al. (2015) 2 895 Office USA Watkins et al. (2013) BDE183 0.001 Computer classroom Taiwan Chang et al. (2009) 19.5 E-waste recycling Finland Rosenberg et al. (2011) 98.0 Aircraft International Allen et al. (2013b) BDE209 0.0023 Computer classroom Taiwan Chang et al. (2009) 2 170 E-waste recycling (crushing) China Guo et al. (2015) 2100 Aircraft USA Allen et al. (2013a) TPhP 0.1 Daycare Sweden Bergh et al. (2011) 850b 10 300 E-waste recycling Finland Makinen et al. (2009) TDCiPP 2.25 Offices China Yang et al. (2014) 90b 450 E-waste recycling Finland Makinen et al. (2009) TBBPA 0.0121 Offices (vapour phase) USA Batterman et al. (2010) 1150 Manufacturing of circuit boards (lamination) China Zhou, 2014 14 600 E-waste recycling Finland Makinen et al. (2009) ƩHBCDD 0.087 Office (low use) China Newton et al. (2016) 48 Aircraft Sweden Strid et al. (2014) 963 Aircraft maintenance Sweden Strid et al. (2014) Dust (ng g−1) BDE47 1.79 Office floor dust China Li et al. (2015) 6240 E-waste recycling (coarse crushing room) China Deng et al. (2014) 23 000 E-waste recycling (dismantling) Thailand Muenhor et al. (2017) BDE183 1.00 Clothing store Pakistan Ali et al. (2014) 22 100a E-waste recycling (shredding wires) China Deng et al. (2014) 12 970a Office floor dust USA Watkins et al. (2011) BDE209 65.0 Clothing store Pakistan Ali et al. (2014) 665 000 E-waste recycling (shredding wires) China Deng et al. (2014) 2 600 000 Aircraft (vent dust) USA Allen et al. (2013a) TPhP 88 Clothing store Pakistan Ali et al. (2014) 15 000 170 000 Vehicle UK Brommer and Harrad (2015) TDCiPP 11 Clothing store Pakistan Ali et al. (2014) 110 000 740 000 Vehicle UK Brommer and Harrad (2015) TBBPA 223 Office floor dust USA Batterman et al. (2010) 6940 9010 Office (dust in computer case) China Li et al. (2015) ƩHBCDD 8900 8900 Classrooms UK Harrad et al. (2010) 1 100 000 Aircraft (carpet) USA Allen et al. (2013a) Blood (ng g−1 lipids) BDE47 0.26 Catering China Wang et al. (2012) 52 Firestation USA Shaw et al. (2013) 540 Foam recyclers USA Stapleton et al. (2008) BDE183 0.148 Manufacturing of cable (measurements) Sweden Thuresson et al. (2005) 4.12 Waste incinerator South Korea Kim et al. (2005) 18.7 E-waste recycling Sweden Sjödin et al. (1999) BDE209 0.75 Leather factory China Wang et al. (2012) 52.4 268 Manufacturing of cables (miscellaneous) Sweden Thuresson et al. (2005) TBBPA 0.34 Laboratory Norway Thomsen et al. (2001) 27 88 Firestation USA Shaw et al. (2013) ƩHBCDD 162 218 Manufacturing of expandable polystyrene Norway Thomsen et al. (2007) Urine (µg l−1, adjusted on specific gravity) DPhP 0.24b Hotel China Tao et al. (2018) 2.96 Aircraft maintenance Germany Schindler et al. (2013) 302 Airline workers Germany Schindler et al. (2013) BDCPP 0.24b Hotel China Tao et al. (2018) 408 1760 Office USA Carignan et al. (2013) BDCPP, bis(1,3-dichloro-2-propyl) phosphate; aDeng et al. (2014) did not report the range of values, but they probably found a higher maximum value than Watkins et al. (2011). bGeometric mean. View Large Table 3. Summary of the reported highest means and maxima for brominated and organophosphate esters FRs in dust, air, and blood. Substance Reported concentrationa Workplace (process or task) Country Reference Lowest detected mean Highest mean Highest max Air (ng m−3) BDE47 0.014 Vehicle-dismantling factories (daytime) Taiwan Gou et al. (2016) 343 E-waste recycling (printed wiring board heating) China Guo et al. (2015) 2 895 Office USA Watkins et al. (2013) BDE183 0.001 Computer classroom Taiwan Chang et al. (2009) 19.5 E-waste recycling Finland Rosenberg et al. (2011) 98.0 Aircraft International Allen et al. (2013b) BDE209 0.0023 Computer classroom Taiwan Chang et al. (2009) 2 170 E-waste recycling (crushing) China Guo et al. (2015) 2100 Aircraft USA Allen et al. (2013a) TPhP 0.1 Daycare Sweden Bergh et al. (2011) 850b 10 300 E-waste recycling Finland Makinen et al. (2009) TDCiPP 2.25 Offices China Yang et al. (2014) 90b 450 E-waste recycling Finland Makinen et al. (2009) TBBPA 0.0121 Offices (vapour phase) USA Batterman et al. (2010) 1150 Manufacturing of circuit boards (lamination) China Zhou, 2014 14 600 E-waste recycling Finland Makinen et al. (2009) ƩHBCDD 0.087 Office (low use) China Newton et al. (2016) 48 Aircraft Sweden Strid et al. (2014) 963 Aircraft maintenance Sweden Strid et al. (2014) Dust (ng g−1) BDE47 1.79 Office floor dust China Li et al. (2015) 6240 E-waste recycling (coarse crushing room) China Deng et al. (2014) 23 000 E-waste recycling (dismantling) Thailand Muenhor et al. (2017) BDE183 1.00 Clothing store Pakistan Ali et al. (2014) 22 100a E-waste recycling (shredding wires) China Deng et al. (2014) 12 970a Office floor dust USA Watkins et al. (2011) BDE209 65.0 Clothing store Pakistan Ali et al. (2014) 665 000 E-waste recycling (shredding wires) China Deng et al. (2014) 2 600 000 Aircraft (vent dust) USA Allen et al. (2013a) TPhP 88 Clothing store Pakistan Ali et al. (2014) 15 000 170 000 Vehicle UK Brommer and Harrad (2015) TDCiPP 11 Clothing store Pakistan Ali et al. (2014) 110 000 740 000 Vehicle UK Brommer and Harrad (2015) TBBPA 223 Office floor dust USA Batterman et al. (2010) 6940 9010 Office (dust in computer case) China Li et al. (2015) ƩHBCDD 8900 8900 Classrooms UK Harrad et al. (2010) 1 100 000 Aircraft (carpet) USA Allen et al. (2013a) Blood (ng g−1 lipids) BDE47 0.26 Catering China Wang et al. (2012) 52 Firestation USA Shaw et al. (2013) 540 Foam recyclers USA Stapleton et al. (2008) BDE183 0.148 Manufacturing of cable (measurements) Sweden Thuresson et al. (2005) 4.12 Waste incinerator South Korea Kim et al. (2005) 18.7 E-waste recycling Sweden Sjödin et al. (1999) BDE209 0.75 Leather factory China Wang et al. (2012) 52.4 268 Manufacturing of cables (miscellaneous) Sweden Thuresson et al. (2005) TBBPA 0.34 Laboratory Norway Thomsen et al. (2001) 27 88 Firestation USA Shaw et al. (2013) ƩHBCDD 162 218 Manufacturing of expandable polystyrene Norway Thomsen et al. (2007) Urine (µg l−1, adjusted on specific gravity) DPhP 0.24b Hotel China Tao et al. (2018) 2.96 Aircraft maintenance Germany Schindler et al. (2013) 302 Airline workers Germany Schindler et al. (2013) BDCPP 0.24b Hotel China Tao et al. (2018) 408 1760 Office USA Carignan et al. (2013) Substance Reported concentrationa Workplace (process or task) Country Reference Lowest detected mean Highest mean Highest max Air (ng m−3) BDE47 0.014 Vehicle-dismantling factories (daytime) Taiwan Gou et al. (2016) 343 E-waste recycling (printed wiring board heating) China Guo et al. (2015) 2 895 Office USA Watkins et al. (2013) BDE183 0.001 Computer classroom Taiwan Chang et al. (2009) 19.5 E-waste recycling Finland Rosenberg et al. (2011) 98.0 Aircraft International Allen et al. (2013b) BDE209 0.0023 Computer classroom Taiwan Chang et al. (2009) 2 170 E-waste recycling (crushing) China Guo et al. (2015) 2100 Aircraft USA Allen et al. (2013a) TPhP 0.1 Daycare Sweden Bergh et al. (2011) 850b 10 300 E-waste recycling Finland Makinen et al. (2009) TDCiPP 2.25 Offices China Yang et al. (2014) 90b 450 E-waste recycling Finland Makinen et al. (2009) TBBPA 0.0121 Offices (vapour phase) USA Batterman et al. (2010) 1150 Manufacturing of circuit boards (lamination) China Zhou, 2014 14 600 E-waste recycling Finland Makinen et al. (2009) ƩHBCDD 0.087 Office (low use) China Newton et al. (2016) 48 Aircraft Sweden Strid et al. (2014) 963 Aircraft maintenance Sweden Strid et al. (2014) Dust (ng g−1) BDE47 1.79 Office floor dust China Li et al. (2015) 6240 E-waste recycling (coarse crushing room) China Deng et al. (2014) 23 000 E-waste recycling (dismantling) Thailand Muenhor et al. (2017) BDE183 1.00 Clothing store Pakistan Ali et al. (2014) 22 100a E-waste recycling (shredding wires) China Deng et al. (2014) 12 970a Office floor dust USA Watkins et al. (2011) BDE209 65.0 Clothing store Pakistan Ali et al. (2014) 665 000 E-waste recycling (shredding wires) China Deng et al. (2014) 2 600 000 Aircraft (vent dust) USA Allen et al. (2013a) TPhP 88 Clothing store Pakistan Ali et al. (2014) 15 000 170 000 Vehicle UK Brommer and Harrad (2015) TDCiPP 11 Clothing store Pakistan Ali et al. (2014) 110 000 740 000 Vehicle UK Brommer and Harrad (2015) TBBPA 223 Office floor dust USA Batterman et al. (2010) 6940 9010 Office (dust in computer case) China Li et al. (2015) ƩHBCDD 8900 8900 Classrooms UK Harrad et al. (2010) 1 100 000 Aircraft (carpet) USA Allen et al. (2013a) Blood (ng g−1 lipids) BDE47 0.26 Catering China Wang et al. (2012) 52 Firestation USA Shaw et al. (2013) 540 Foam recyclers USA Stapleton et al. (2008) BDE183 0.148 Manufacturing of cable (measurements) Sweden Thuresson et al. (2005) 4.12 Waste incinerator South Korea Kim et al. (2005) 18.7 E-waste recycling Sweden Sjödin et al. (1999) BDE209 0.75 Leather factory China Wang et al. (2012) 52.4 268 Manufacturing of cables (miscellaneous) Sweden Thuresson et al. (2005) TBBPA 0.34 Laboratory Norway Thomsen et al. (2001) 27 88 Firestation USA Shaw et al. (2013) ƩHBCDD 162 218 Manufacturing of expandable polystyrene Norway Thomsen et al. (2007) Urine (µg l−1, adjusted on specific gravity) DPhP 0.24b Hotel China Tao et al. (2018) 2.96 Aircraft maintenance Germany Schindler et al. (2013) 302 Airline workers Germany Schindler et al. (2013) BDCPP 0.24b Hotel China Tao et al. (2018) 408 1760 Office USA Carignan et al. (2013) BDCPP, bis(1,3-dichloro-2-propyl) phosphate; aDeng et al. (2014) did not report the range of values, but they probably found a higher maximum value than Watkins et al. (2011). bGeometric mean. View Large Both highest means and maxima for BDE209, TPhP, and TBBPA were reported in the e-waste recycling industry and in manufacturing of printed circuit boards (Table 3). Regarding dust concentrations, the highest mean dust concentrations were found in e-waste recycling facilities for BDE47, BDE183, and BDE209 and in automobiles for TPhP and TDCiPP, whereas the highest values were found in aircrafts for hexabromocyclododecane (HBCDD), and in the dust inside an office computer case for TBBPA. Finally, firefighters, waste incinerators and cable manufacturing workers had the highest means of blood BDE47, BDE183 and BDE209 levels, respectively. Firefighters also had the highest blood TBBPA mean. Proportions of BDE47, BDE183, and BDE209 over the sum of the three congeners are presented in Fig. 2a for blood levels and in Fig. 2b for dust levels by type of workplaces. Overall, BDE47 and BDE183 are found in higher proportions in blood than in dust, in which BDE209 predominates. Figure 2 View largeDownload slide Congener profiles in blood (a) and dust (b), presented as the proportion of the sum of congeners BDE47, BDE183 and BDE209 based on weighted means, by type of workplace. Figure 2 View largeDownload slide Congener profiles in blood (a) and dust (b), presented as the proportion of the sum of congeners BDE47, BDE183 and BDE209 based on weighted means, by type of workplace. Nine studies reported on more than one exposure medium, providing the possibility to compare concentrations measured in different media. Watkins et al. (2013) and Batterman et al. (2010) showed moderately to highly correlated dust and air PBDE concentrations (Spearman correlation; PentaBDE: r = 0.60, P = 0.0003; BDE-47, 99, and 100: r = 0.59–0.92), especially for the more volatile PBDEs that have a smaller number of bromine atoms. Positive correlations between dust and air concentrations of OPFRs were reported (F-test for goodness of fit statistically significant; linear model R2: tris(2-chloroethyl) phosphate (TCEP) = 0.5; tris(2-chloroisopropyl)phosphate (TCiPP) = 0.4; dibutyl phosphate (DBP) = 0.2), whereas TBBPA was found almost exclusively in dust and not in air [ratio of log(concentration in dust/conc. in PM10) ranging from 0.71 to 3.57] (Bergh et al., 2011; Zhou et al., 2014). Concentrations in biological matrices did not correlate well with those in dust or air samples, aside from a positive trend between urinary bis(1,3-dichloro-2-propyl) phosphate (BDCiPP) and its parent compound TDCiPP in office dust (Spearman r = 0.45, P = 0.02) (Carignan et al., 2013). Ali et al. (2014) also found significant correlations between lower brominated congeners in dust and plasma (Spearman r = 0.64, P < 0.01). Only one study presented results according to particle size. Yang et al. (2014) used an eight-stage cascade impactor to sample 10 OPFRs in the air of offices. They showed that TCEP, tri(chloropropyl) phosphate (TCPP), Tri-n-butyl phosphate (TnBP), and TPhP were adsorbed to particles with a mass median aerodynamic diameter >2.5 µm, that tri n-propyl phosphate (TnPP), tributoxyethyl phosphate (TBEP), and 2-ethylhexyl diphenyl phosphate (EHDPP) were in the 1.0−2.5 μm range, and that TDCiPP, tricresyl phosphate (TCrP), and tri(2-ethylhexyl) phosphate (TEHP) were mostly distributed in particles of diameters <1 µm. Julander et al. (2005b) used different air samplers to determine the concentrations of PBDEs according to three airborne dust fractions: total (open faced 25-mm cassette), inhalable (particles <100 µm), and respirable (particles <10 µm) in an e-waste recycling facility. All measured congeners were found in higher concentrations in the inhalable dust fraction, compared to the respirable fraction, demonstrating the association of PBDEs with the larger airborne particles (Julander et al., 2005b). Two additional studies that reported separately concentrations of the particle and gaseous phases of PBDEs, in offices and in a vehicle parking lot, showed that most congeners were found in the particulate phase, the less brominated congeners having the highest proportion measured in the gaseous phase (Guo et al., 2015; Li et al., 2016). Dechlorane plus was also found mostly in the particulate phase (Li et al., 2016). Discussion This review is, to our knowledge, the most extensive appraisal of occupational exposure to FRs. The 58 collected peer-reviewed studies attest a growing interest in exposure assessment of these substances in occupational settings throughout the last two decades. Studies focused more on older FRs (PBDEs and OPFRs) and much less on NBFRs and ClFRs, possibly reflecting less concern on the potential health effects of the latter, as well as developing analytical methods for these compounds. PBDEs are also the most commonly found FRs in home dust, even decades after a phase-out in response to health concerns that raised the interest of researchers to identify sub-populations that remain highly exposed (Coelho et al., 2014). As pertinent analytical aspects of PBDEs and NBFRs have been previously reviewed (Covaci et al., 2011; Fulara and Czaplicka, 2012), they are not discussed further here. Workplaces in a few industrial sectors had high values for several FRs. E-waste recycling, air transportation and manufacturing facilities are among workplaces with the highest levels of FRs. E-waste recycling exposes its workers especially during dismantling operations of old electric and electronic equipment, in which several kinds of FRs are found (Schluep et al., 2009; Ceballos et al., 2015). For example, the dust inside a TV cabinet has been found to contain up to 2–3 orders of magnitude more PBDEs than household dust (Takigami et al., 2008), partly explaining such high exposures in e-waste workers. As for the air transportation sector, aircraft constructors have to abide by some of the strictest fire safety standards, increasing the use of FRs (Federal Aviation Administration, 2009). Finally, firefighters’ protective equipment and vehicles are treated with FRs, adding to their background exposure (Alexander and Baxter, 2016). Many different workplaces were investigated, but the tasks/activities or specific workplace areas were not always described comprehensively, which hinders the identification of determinants of exposure. On the other hand, studies that presented a detailed description of tasks or sampled areas had a small sample size, which reduced their power to bring out specific determinants [e.g. in Deng et al. (2014) or Zhou et al. (2014)]. Sampling approach FRs are semi-volatile organic chemicals (SVOCs), defined by their vapour pressure typically between 10 and 10–6 pascals (Pa), allowing them to be airborne in both vapour and particle phases (Bidleman, 1988), which explains the selection of sampling methodologies that allowed collection of both phases. Numerous sampling methodologies exist for SVOCs and generally rely on filtration (e.g. Teflon and glass or quartz fibres) and sorption (e.g. XAD-2, polyurethane foam. and combination of the two) for particle and gaseous phase compounds, respectively (Król et al., 2011). This combined sampling approach is considered a standard method for several SVOCs such as pesticides and polycyclic aromatic hydrocarbons (Kim and Soderholm, 2013). A European standard now establishes the requirements for SVOC method validations and an ISO standard is currently in development (European Committee for Standardization, 2014). Methods used to evaluate exposure to FRs in occupational settings should hence be developed in accordance to the published or coming international standards. Caution is advised when comparing results between studies in which methodologies were not optimized for SVOC sampling such as those using filtration only (Julander et al., 2005b; Yang et al., 2014; Zhou et al., 2014). Filtration-only methods may be associated with important underestimation due to particle-phase evaporation under certain circumstances (Kim, 2010; Melymuk et al., 2014), a phenomenon that may be exacerbated by the use of higher flow rates, such as the ones used in ambient air sampling by Harrad et al. (2004) (600–800 l min−1), and by long sampling durations. Due to these limitations, the gas–particle partition of an airborne contaminant cannot be calculated with exactitude by a sampling assembly consisting of a filter and sorbent. Nonetheless, the methods used by Guo et al. (2015) and Li et al. (2016) can still provide a reasonable estimate of the gas–particle partition of the FRs sampled. The concentration of FRs in settled dust is often considered to be a proxy for their internal dose, thereby assuming significant skin permeation, hand-to-mouth behaviour, or unintentional dust ingestion in workers (Frederiksen et al., 2009; American Conference of Governmental Industrial Hygienists, 2015; Gorman Ng et al., 2016). None of the settled dust exposure assessment methods followed a standard procedure across the studies; this was also mentioned in a systematic review on the associations between internal dose of PBDEs and indoor dust (Bramwell et al., 2016). Among major parameters to be taken into account when collecting dust, the sampling method itself, the sample storage, and its preparation (sieving) are critical for sample stability (Allen et al., 2008; Mercier et al., 2011). Vacuuming can be an efficient way to capture semi-volatile compounds associated with dust particles and can allow for gravimetric analyses as mentioned in the Standard practice for collection of floor dust for chemical analysis (ASTM international, 2017). This dust collection method, developed by the US Environmental Protection Agency, was widely used in home dust exposure assessments (Mercier et al., 2011), but none of the studies included in the present review referred to it. This is unfortunate as many factors can affect the efficiency of particles collection, such as the distance between the nozzle and the vacuumed surface, the flow rate, the characteristics of the sampled surface, and the collection apparatus itself (filter, nylon sock, cyclone, etc.) (Roberts et al., 1996; ASTM International, 2016). Many studies that were excluded for methodological reasons collected bulk dust by sweeping surfaces with a brush or sampling directly from vacuum bags, approaches that are hardly reproducible and reliable. As with air sampling methods, the use of a filter only to collect dusts may result in an underestimation of measurements. Surface wiping has been shown to be a reliable way to quantify the presence of a semi-volatile on a given surface, when carried out following a strict protocol (Jung, 2014). However, method validations have yet to demonstrate the quantitative transfer of FRs from the sampled surface to the final extract in the laboratory to obtain a reproducible yield without bias (due, for instance, to strong chemical bond between contaminants and sampled surface or intermediate containers during storage). Moreover, the sampling location also has an impact on the potential transfer to humans, be it floor dust or the inside of a computer case (Allen et al., 2008). Dust may remain a useful non-invasive matrix for exposure assessment in workplaces but standardized and reproducible methods should be used, such as utilizing a standard template for wipe sampling or following a standard protocol for vacuuming and thoroughly detailing sampled surfaces and locations. Study results The association between air and dust content of FRs in various settings has not been consistently established in the reviewed studies. Atmospheric conditions, the sampling flow rate and duration, as well as the molecule’s intrinsic properties, can influence the particle–gas partition and can partly explain the variability in the associations between the sampling matrices (Ward and Smith, 2004; Liagkouridis et al., 2014). For instance, some industrial sectors use heating processes or hot temperatures, such as smelters and ovens, where the particle–gas partition would differ greatly from the partition in industries with more temperate workplaces (Guo et al., 2015). Occupational exposure assessments have to be performed with a device that collects both the particle and vapour phases, rather than only using settled dust, to adequately assess the potential inhalation exposure to such semi-volatile FRs. More studies are needed to describe the particle-size distributions of FR particles, as it may assist in understanding exposure and guide prevention efforts. Biological monitoring of FRs in workers, although used frequently in the reviewed research studies, would generally not be recommended for occupational exposure surveillance, particularly because the biological half-life of most FRs is not well documented, limiting inferences from measured concentrations in blood or urine (Thuresson et al., 2006b; Szabo et al., 2010; Tao et al., 2018). However, it can provide valuable insight when compared to levels in the general population, especially as most FRs are not regulated. Biological monitoring also takes into account all routes of exposure, allowing validation of the hypothesis that ingestion is a non-negligible exposure pathway, when coupled with other exposure assessment matrices (Covaci et al., 2011; Watkins et al., 2011). As for previously mentioned exposure assessment methods, biomarker measurements were also not presented in a standardized way. Most results of blood concentrations were presented on a total blood lipid content basis, which is considered to reflect the body burden of lipophilic substances, and enables comparisons between populations (Rylander et al., 2006). One epidemiology study (Eguchi et al., 2012) appropriately presented results on a serum wet weight basis, which may be less prone to bias than lipid adjustment for use in an epidemiology study (Schisterman et al., 2005). One study did not present results adjusted on lipids or wet weight, which impedes comparison of concentrations in these workers with others’ (Wang et al., 2012). The same applies for urinary metabolites of OPFRs, generally adjusted on urinary specific gravity, which is minimally impacted by age, body composition, urine flow, physical activity, and other factors, as opposed to creatinine (Boeniger et al., 1993). This is especially true if the sampled population works in a warm environment and with limited access to restroom breaks, leading to more concentrated urine and hence, overestimated levels. All of the studies included in this review specified the time of the day at which urine samples were taken (after work), which is important for rapidly metabolized molecules such as OPFRs (Hou et al., 2016). Only about a third of the studies had sample sizes above 30, which explains that their statistical analyses are essentially descriptive. Nevertheless, it is fundamental to report the limits of detection and quantification, the proportion of data that falls below those limits, and the approach used to handle the non-detected data in analyses (imputation/substitution rules or exclusion) for the reader to grasp the overall distribution of the exposure (IT Environmental Programs Inc. and ICF Kaiser Incorporated, 1994). Several statistical approaches were proposed in recent years to adequately analyse censored data and they all recommend avoiding simple substitution methods to reduce bias (Lubin et al., 2004; Helsel, 2010; Dinse et al., 2014; Lavoue et al., 2018). Statistical comparisons of concentrations between studies were quite challenging, as some articles did not present standard deviations or sometimes no means at all (arithmetic or geometric). Few articles presented geometric means, while occupational exposure data is generally recognized to be log-normally distributed (Waters et al., 2015). Finally, some articles even lacked a ‘Statistics’ or a ‘data analysis’ section in their methodology. Among the FRs reported in our study, only TPhP has an occupational threshold limit value (TLV) that would allow identification of workplaces needing urgent intervention. The TLV for TPhP of 3 mg m−3, established to prevent skin irritation and neurotoxic effects (American Conference of Governmental Industrial Hygienists, 2018), is quite high and none of the workplaces surveyed presented such values. The highest maximum for TPhP was recorded in e-waste recycling, at 0.5% of the TLV (Makinen et al., 2009). In the absence of an exposure standard, Haines et al. (2017) derived a biomonitoring reference value for BDE47 of 67 ng g−1 lipids based on the 95th percentile of Canadian population serum values of PBDEs; several occupational groups show maximal values exceeding this level, such as office workers, airline workers, firefighters, carpet layers, and foam recyclers (Stapleton et al., 2008; Schecter et al., 2010; Shaw et al., 2013; Makey et al., 2016). Regarding median values, firefighters in the USA had median concentrations of BDE47 exceeding those of the general population workers from both the USA (19.4 ng g−1 lipids) and Canada (9.1 ng g−1 lipids) (Gravel et al., 2018). The distribution profiles of the three main PBDEs according to sampling media can provide insight on avenues for exposure prevention. Some workplaces show a greater exposure to less brominated FRs, attesting to the presence of the commercial formulation PentaBDE, which has been found to be bioaccumulative and toxic (Dishaw et al., 2014). Schools and offices showed high levels of lower brominated PBDEs and would benefit from adequate ventilation to decrease the exposure of workers to these more volatile substances. On the other hand, workplaces where BDE209 is more prevalent in dust would benefit from a thorough cleaning and dusting, as this congener is less volatile and adsorbed mainly to dust. The proportions of the same congeners in blood show that although BDE209 is thought to be less bioaccumulative (Frederiksen et al., 2009), it is still highly prevalent in workers of all studied occupations, meaning that exposure to the commercial formulation DecaBDE is widespread. Finally, Table 4 lists several gaps that were identified in the body of literature and offers some recommendations to overcome them in the conduct of comprehensive occupational exposure assessments. Table 4. Research gaps and recommendations on occupational assessment of exposure to FRs. Research gaps Recommendations There are fewer studies on more recently introduced FRs (novel brominated, organophosphorus, and chlorinated) than on polybrominated diphenyl ethers. Conduct more occupational exposure assessments on novel brominated, organophosphorus, and chlorinated FRs. Workplaces and tasks should be well defined to help identify determinants of exposure and ensure comparability between studies. Settled dust and air-sampling methods are not standardized and not sufficiently described to be reproducible. Limitations of dust vacuum sampling methods are not well documented. A reproducible and standardized vacuuming or wiping dust collection method should be employed. Air-sampling methods should be better described and should refer to reference methods developed according to standards such as EN 13936. Adjustment of concentrations in biological matrices is not systematic (e.g. by lipid or wet weight in blood, specific gravity, or creatinine levels in urine). Standardization of analysis and reporting of biological monitoring methods is necessary to facilitate interpretation of results across studies. The associations between FR concentrations in the different matrices are understudied and poorly understood. More biomonitoring research is needed, coupled with environmental sampling to understand associations between matrices. The particle: gas partition of flame retardants is insufficiently documented. Particle: gas partition is subject to be inaccurate with commonly used sampling methods. A standard method capable to yield an exact partition should be developed. The role of the nature of the particle on which flame retardant is adsorbed is not known. Understand to which extent the nature of the particle has a role in exposure. Information on the particle-size distribution of the particle-phase FR is scarce. More research is needed to understand exposure pathways in workers. Statistical analyses and reporting of results is disparate among the different studies. Statistical analyses should be adequate for the distribution of the data, and the limits of detection should be taken into account when reporting and analysing the data. More research should be undertaken in firefighter and e-waste recycling workers to assess potential adverse health effects associated with higher exposures. Research gaps Recommendations There are fewer studies on more recently introduced FRs (novel brominated, organophosphorus, and chlorinated) than on polybrominated diphenyl ethers. Conduct more occupational exposure assessments on novel brominated, organophosphorus, and chlorinated FRs. Workplaces and tasks should be well defined to help identify determinants of exposure and ensure comparability between studies. Settled dust and air-sampling methods are not standardized and not sufficiently described to be reproducible. Limitations of dust vacuum sampling methods are not well documented. A reproducible and standardized vacuuming or wiping dust collection method should be employed. Air-sampling methods should be better described and should refer to reference methods developed according to standards such as EN 13936. Adjustment of concentrations in biological matrices is not systematic (e.g. by lipid or wet weight in blood, specific gravity, or creatinine levels in urine). Standardization of analysis and reporting of biological monitoring methods is necessary to facilitate interpretation of results across studies. The associations between FR concentrations in the different matrices are understudied and poorly understood. More biomonitoring research is needed, coupled with environmental sampling to understand associations between matrices. The particle: gas partition of flame retardants is insufficiently documented. Particle: gas partition is subject to be inaccurate with commonly used sampling methods. A standard method capable to yield an exact partition should be developed. The role of the nature of the particle on which flame retardant is adsorbed is not known. Understand to which extent the nature of the particle has a role in exposure. Information on the particle-size distribution of the particle-phase FR is scarce. More research is needed to understand exposure pathways in workers. Statistical analyses and reporting of results is disparate among the different studies. Statistical analyses should be adequate for the distribution of the data, and the limits of detection should be taken into account when reporting and analysing the data. More research should be undertaken in firefighter and e-waste recycling workers to assess potential adverse health effects associated with higher exposures. View Large Table 4. Research gaps and recommendations on occupational assessment of exposure to FRs. Research gaps Recommendations There are fewer studies on more recently introduced FRs (novel brominated, organophosphorus, and chlorinated) than on polybrominated diphenyl ethers. Conduct more occupational exposure assessments on novel brominated, organophosphorus, and chlorinated FRs. Workplaces and tasks should be well defined to help identify determinants of exposure and ensure comparability between studies. Settled dust and air-sampling methods are not standardized and not sufficiently described to be reproducible. Limitations of dust vacuum sampling methods are not well documented. A reproducible and standardized vacuuming or wiping dust collection method should be employed. Air-sampling methods should be better described and should refer to reference methods developed according to standards such as EN 13936. Adjustment of concentrations in biological matrices is not systematic (e.g. by lipid or wet weight in blood, specific gravity, or creatinine levels in urine). Standardization of analysis and reporting of biological monitoring methods is necessary to facilitate interpretation of results across studies. The associations between FR concentrations in the different matrices are understudied and poorly understood. More biomonitoring research is needed, coupled with environmental sampling to understand associations between matrices. The particle: gas partition of flame retardants is insufficiently documented. Particle: gas partition is subject to be inaccurate with commonly used sampling methods. A standard method capable to yield an exact partition should be developed. The role of the nature of the particle on which flame retardant is adsorbed is not known. Understand to which extent the nature of the particle has a role in exposure. Information on the particle-size distribution of the particle-phase FR is scarce. More research is needed to understand exposure pathways in workers. Statistical analyses and reporting of results is disparate among the different studies. Statistical analyses should be adequate for the distribution of the data, and the limits of detection should be taken into account when reporting and analysing the data. More research should be undertaken in firefighter and e-waste recycling workers to assess potential adverse health effects associated with higher exposures. Research gaps Recommendations There are fewer studies on more recently introduced FRs (novel brominated, organophosphorus, and chlorinated) than on polybrominated diphenyl ethers. Conduct more occupational exposure assessments on novel brominated, organophosphorus, and chlorinated FRs. Workplaces and tasks should be well defined to help identify determinants of exposure and ensure comparability between studies. Settled dust and air-sampling methods are not standardized and not sufficiently described to be reproducible. Limitations of dust vacuum sampling methods are not well documented. A reproducible and standardized vacuuming or wiping dust collection method should be employed. Air-sampling methods should be better described and should refer to reference methods developed according to standards such as EN 13936. Adjustment of concentrations in biological matrices is not systematic (e.g. by lipid or wet weight in blood, specific gravity, or creatinine levels in urine). Standardization of analysis and reporting of biological monitoring methods is necessary to facilitate interpretation of results across studies. The associations between FR concentrations in the different matrices are understudied and poorly understood. More biomonitoring research is needed, coupled with environmental sampling to understand associations between matrices. The particle: gas partition of flame retardants is insufficiently documented. Particle: gas partition is subject to be inaccurate with commonly used sampling methods. A standard method capable to yield an exact partition should be developed. The role of the nature of the particle on which flame retardant is adsorbed is not known. Understand to which extent the nature of the particle has a role in exposure. Information on the particle-size distribution of the particle-phase FR is scarce. More research is needed to understand exposure pathways in workers. Statistical analyses and reporting of results is disparate among the different studies. Statistical analyses should be adequate for the distribution of the data, and the limits of detection should be taken into account when reporting and analysing the data. More research should be undertaken in firefighter and e-waste recycling workers to assess potential adverse health effects associated with higher exposures. View Large Strengths and limitations of the systematic review This is the first systematic review on occupational exposure to FRs. The PRISMA protocol was followed to ensure the exhaustiveness and the reproducibility of our work. Moreover, the bibliographic databases searched for article selection are considered to be optimal for an adequate and efficient coverage of the literature (Bramer et al., 2017). This review succeeded in identifying industrial sectors that would benefit from further investigation of exposure to FRs and reduction measures. Gaps in the body of literature were also identified and recommendations were made to improve the strength of future studies on the matter. Some limitations of this review need to be mentioned. It is difficult to assess the representativeness of the occupational exposure data presented here, as companies that welcome a research team into their facilities are probably more likely to be proactive in exposure prevention, and hence exposure levels in their premises are possibly not the most problematic. In the reviewed body of literature, the variety of experimental approaches limits the inference to their respective industrial sectors. Additionally, a whole body of literature on informal occupational settings was excluded from this review; FR concentrations in such uncontrolled conditions are not comparable to those in formal settings and probably need more attention from a general public health perspective than an occupational health point of view. Non peer-reviewed papers and grey literature were excluded, which may have reduced the available data, although it ensured a minimal degree of confidence in the results. Finally, most of the extraction of data was done by one reviewer, although a second reviewer checked a small proportion of the extracted data, which may have introduced difficult to quantify errors. Conclusion Some workplaces clearly expose their workers to FRs. While methodological inconsistencies among the different reviewed studies rendered exposure assessment difficult, the highest concentrations found in e-waste recycling, air transportation, and firefighting warrant more investigation into these workplaces using standard protocols and validated methods. Thorough and reproducible occupational exposure assessments will complement the body of knowledge and support occupational health decision-making for protective and preventive interventions. Conflict of Interest The authors declare no conflict of interest relating to the material presented in this article. References Abafe OA , Martincigh BS . ( 2015 ) An assessment of polybrominated diphenyl ethers and polychlorinated biphenyls in the indoor dust of e-waste recycling facilities in South Africa: implications for occupational exposure . Environ Sci Pollut Res Int ; 22 : 14078 – 86 . Google Scholar Crossref Search ADS PubMed Alexander BM , Baxter CS . 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TI - Assessment of Occupational Exposure to Organic Flame Retardants: A Systematic Review
JF - Annals of Work Exposures and Health (formerly Annals Of Occupational Hygiene)
DO - 10.1093/annweh/wxz012
DA - 2019-04-19
UR - https://www.deepdyve.com/lp/oxford-university-press/assessment-of-occupational-exposure-to-organic-flame-retardants-a-btQd0qDpDQ
SP - 386
VL - 63
IS - 4
DP - DeepDyve
ER -