Science of the Total Environment 760 (2021) 143862

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Science of the Total Environment

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Inhalation bioaccessibility and health risk assessment of flame retardants

in indoor dust from Vietnamese e-waste-dismantling workshops
Tatiya Wannomai a,⁎, Hidenori Matsukami b, Natsuyo Uchida b, Fumitake Takahashi a, Le Huu Tuyen c,d,
Pham Hung Viet c, Shin Takahashi e, Tatsuya Kunisue d, Go Suzuki b
a
Department of Transdisciplinary Science and Engineering, School of Environment and Society, Tokyo Institute of Technology, 4259, Nagatsuta, Midori-ku, Yokohama 226-8503, Japan
b
Center for Material Cycles and Waste Management Research, National Institute for Environmental Studies, 16-2 Onogawa, Tsukuba 305-8506, Japan
c
Centre for Environmental Technology and Sustainable Development, VNU Hanoi University of Science, 334 Nguyen Trai, Hanoi, Viet Nam
d
Center for Marine Environmental Studies, Ehime University, 2-5 Bunkyo-cho, Matsuyama 790-8577, Japan
e
Center of Advanced Technology for the Environment, Faculty of Agriculture, Ehime University, 3-5-7 Tarumi, Matsuyama 790-8566, Japan

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Inhalation bioaccessibility of FRs in dust

from e-waste dismantling was assessed.
• Bioaccessible concentrations of FRs
were markedly lower than their mass
concentrations.
• TCEP, TCIPP, and TDCIPP all showed
high inhalation bioaccessibility.
• Inhalation bioaccessibility of FRs was re-
lated to their log KOW and water solubil-
ity.
• Dismantling e-waste indoors poses neg-
ligible inhalation health risk from FRs.

a r t i c l e i n f o a b s t r a c t

Article history: Although bioaccessibility testing is applied worldwide for appropriate chemical risk assessment, few studies have
Received 21 July 2020 focused on the bioaccessibility of flame retardants (FRs), especially inhalation exposure. This study assessed in-
Received in revised form 16 October 2020 halation exposure to FRs in indoor dust by workers at e-waste-dismantling workshops in northern Vietnam, by
Accepted 10 November 2020
using modified simulated epithelial lung fluid (SELF) and artificial lysosomal fluid (ALF). The average mass con-
Available online 9 December 2020
centrations of FRs were 130,000 ng/g for workplace dust (n = 3), 140,000 ng/g for floor dust (n = 3), and
Editor: Adrian Covaci 74,000 ng/g for settled dust (n = 2), whereas the average bioaccessible concentrations of FRs were 1900,
1400, and 270 ng/g in the SELF condition and 2600, 770, and 490 ng/g in the ALF condition, respectively. Results
Keywords: clearly indicate that the bioaccessible concentrations of FRs are markedly lower than their mass concentra-
Bioaccessibility tions. Tris(2-chloroethyl) phosphate (TCEP, ~19%), tris(2-chloroisopropyl) phosphate (TCIPP, ~35%), and
Inhalation exposure tris(1,3-dichloroisopropyl) phosphate (TDCIPP, ~22%) showed comparably high bioaccessibility in both SELF
Flame retardants and ALF conditions. In contrast, the bioaccessibility of tetrabromobisphenol A (TBBPA, ~20%) was high in the
E-waste SELF condition, but not in the ALF condition. With regard to the test compounds' physicochemical properties,
Health risk assessment
the inhalation bioaccessibility of FRs in both conditions increased as molecular weight or octanol–water partition
Indoor dust
coefficient decreased, and it decreased as water solubility decreased. Health risk assessment clearly indicated
that the hazard quotient of FRs via inhalation exposure for workers in the e-waste-dismantling workshops
was less than 1, suggesting that the inhalation exposure to FRs during indoor dismantling of e-waste at this
site was negligible based on the current methodology of non-cancer health risk assessment used in this study.
© 2020 Elsevier B.V. All rights reserved.

⁎ Corresponding author.
E-mail address: [email protected] (T. Wannomai).

https://doi.org/10.1016/j.scitotenv.2020.143862
0048-9697/© 2020 Elsevier B.V. All rights reserved.
T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

1. Introduction PBDEs, AHFRs, and PFRs, with the SELF condition representing intersti-
tial fluid in the deep lung and with the ALF condition representing the
Flame retardants (FRs) have been added to various products, partic- more acidic intracellular conditions found in the lysosomes of alveolar
ularly electrical and electronic devices (e-devices), since the 1970s in macrophages. First, we evaluated the inhalation bioaccessible concen-
accordance with fire safety standards (Agency for Toxic Substances tration and bioaccessibility of FRs in indoor dust generated by e-waste
and Disease Registry, 2004; Rauert and Harrad, 2015). These chemicals dismantling in the SELF and ALF conditions. We then investigated the
are added into several polymeric materials of e-devices, including relationships between the measured bioaccessibility values and physi-
printed circuit boards and plastic casings (Kajiwara et al., 2011; cochemical properties to identify the key factors affecting the inhalation
Robinson, 2009; Stubbings et al., 2019; van der Veen and de Boer, bioaccessibility of FRs contained in indoor dust. Finally, we estimated
2012). After FRs had been in use for decades, adverse effects on endo- the daily intake of FRs via inhalation exposure for workers in the e-
crine function and the nervous system were found for polybrominated waste-dismantling workshops for subsequent assessment of non-
diphenyl ethers (PBDEs) (Ikonomou et al., 2002). Use of these com- cancer health risk.
pounds has been prohibited by the Restriction of Hazardous Substances
in the European Union since 2006, and hence alternative halogenated 2. Materials and methods
flame retardants (AHFRs) and phosphorus-containing flame retardants
(PFRs) are now widely used as replacements for PBDEs (Stapleton et al., 2.1. Sample collection and preparation
2009; US EPA, 2005; van den Eede et al., 2011). These alternative FRs are
slowly released from the materials into the environment by volatiliza- Indoor dust samples were collected from three e-waste-dismantling
tion and abrasion (Suzuki et al., 2009; van den Eede et al., 2011; workshops in Bui Dau, Hung Yen Province, northern Vietnam, in 2015.
Webster et al., 2009; Wensing et al., 2005). Based on studies of indoor Detailed information about this e-waste processing area and method
dust, compounds including FRs can be detected at high concentrations, of indoor dust collection and preparation was given in our previous re-
and these reports indicate that most of the additive compounds are re- ports (Matsukami et al., 2015, 2017; Someya et al., 2016; Suzuki et al.,
leased to the environment by volatilization, abrasion, and direct contact 2016; Wannomai et al., 2020). Briefly, the three workshops where the
between source and dust (Rauert and Harrad, 2015; Takigami et al., dust samples were collected were chosen as typical e-waste-
2008). Therefore, indoor dust appears to be one of the main exposure dismantling workshops from approximately 50 households doing e-
sources of FRs (Fang and Stapleton, 2014; Johnson et al., 2010; Jones- waste processing in the area. Samples of workplace dust (i.e., dust gen-
Otazo et al., 2005). erated by e-waste dismantling onto a tarpaulin; n = 3), floor dust
E-devices become obvious contamination sources of FRs after their (i.e., indoor dust deposited on the floor surface of the workshop; n =
dismantling and disposal, and FRs are easily released into the environ- 3), and settled dust (i.e., dust accumulated on the workshop shelves
ment when e-devices are stored or dismantled improperly. Therefore, and window frames after floating in the working environment; n = 3)
electrical and electronic waste (e-waste) recycling sites with manual were collected; a total of eight samples were used because there was
dismantling processes are important research targets for investigating not enough settled dust-1 for use in this study. Collected dust samples
the fate of chemicals such as FRs in products. Our study area is Bui were sieved into three fractions according to particle size (<250 μm,
Dau, Hun Yen Province, northern Vietnam, which is a good representa- 250 μm to 2 mm, and >2 mm). To compare with the reported ingestion
tive of manual e-waste disposal and dismantling sites throughout the bioaccessibility (Wannomai et al., 2020), the same fraction (<250 μm)
world. Moreover, our previous studies in the area indicated that was used for the inhalation bioaccessibility tests. The sieved dust sam-
PBDEs and related compounds were present in dust and soil samples ples were kept at −20 °C until analysis.
at high concentrations, which were one to two orders of magnitude
higher than in the Hanoi urban area (Anh et al., 2018; Matsukami 2.2. Inhalation bioaccessibility test
et al., 2015, 2016, 2017; Suzuki et al., 2013, 2016; Takahashi et al.,
2017; Tue et al., 2010, 2013; Wannomai et al., 2020). SELF (Boisa et al., 2014) and ALF (Colombo et al., 2008; Midander
While considering human exposure to FRs via indoor dust, several et al., 2007) were used to assess inhalation bioaccessibility of FRs in
studies have assumed 100% intake of FRs in the matrices, but this likely dust samples. SELF (pH 7.4) represents fluid in the deep lung and
overestimates the exposure risk. In vitro methods that simulate the di- mimics the in vivo condition of a healthy non-smoking human (Boisa
gestive and respiratory systems are commonly used in such assess- et al., 2014), whereas ALF (pH 4.5) mimics the more acidic intracellular
ments to avoid overestimating risk. Some studies focused on FR conditions found in the lysosomes of alveolar macrophages (Colombo
ingestion bioaccessibility, and several methods were modified to appro- et al., 2008; Midander et al., 2007). The composition and concentrations
priately simulate the digestive and respiratory systems (Ruby et al., of components of SELF and ALF is given in Table S1, and the schematic
1996; Turner and Hefzi, 2010; Turner and Ip, 2007). In addition, inhala- representation of inhalation bioaccessibility tests with SELF and ALF
tion bioaccessibility, especially for metals and metalloids, has been for FRs in dust samples are shown in Fig. S1. Briefly, 0.2 g of the dust
widely studied using materials based on the original Gamble's solution sample was added to 20 mL of SELF or ALF at a fixed solid-to-liquid
(Moss, 1979), such as Hatch's solution (Berlinger et al., 2008), simulated ratio of 1:100; this ratio was chosen based on the lower limit of quanti-
lung fluid (Twining et al., 2005), simulated epithelial lung fluid (SELF) fication during analysis and for ease of comparison with previous stud-
(Boisa et al., 2014), and artificial lysosomal fluid (ALF) (Midander ies. The sample was then shaken by an end-over-end shaking machine
et al., 2007). However, few studies have examined the inhalation bioac- for 24 h at 37 °C in the dark. The pH values of SELF and ALF solutions
cessibility of hydrophobic organic contaminants such as FRs, which may were controlled at 7.4 and 4.5, respectively, during experiments. The
have adverse human health effects via inhalation exposure (Kademoglou sample solutions were centrifuged at 3000 rpm for 15 min and then fil-
et al., 2018; Li et al., 2019; Xie et al., 2018; Zeng et al., 2019). tered through a 0.5-μm glass fiber filter (Toyo Roshi Kaisha, Ltd., Tokyo,
Our previous study investigated oral ingestion bioaccessibility by Japan). Supernatant without dust particles was transferred to a new
using a modified version of a physiologically based extraction test de- glass tube. This procedure was repeated over 4 consecutive days. Pooled
scribed by Huang et al. (2014). We found that the bioaccessible concen- supernatant was stored at −20 °C until extraction.
trations of several FRs were high in indoor dust collected from e-waste-
dismantling workshops and that the ingestion bioaccessible concentra- 2.3. Chemical analysis
tions of several FRs were also high (290, 380, and 5900 ng/g for PBDEs,
AHFRs, and PFRs, respectively; Wannomai et al., 2020). In the present In this study, 36 FRs (12 PBDEs, 8 AHFRs, and 16 PFRs; Table S2)
study, we used two inhalation bioaccessibility tests for 36 FRs including were measured as described previously (Matsukami et al., 2015,

2
T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

2017). Briefly, an aliquot of the supernatants of SELF and ALF was where HQ is the non-cancer hazard quotient of FR via daily inhalation
liquid-liquid extracted with dichloromethane and used as a crude exposure for workers in an e-waste-dismantling workshop, DI is calcu-
extract. For PBDE and AHFR measurements, a portion of the crude ex- lated by using Eq. (2), and RfD represents the reference doses (ng/kg
tract was spiked with 13C12-labeled PBDE congeners, 13C6 -labeled BW/d) associated with adverse effects for four PBDEs (US EPA, 1987,
hexabromobenzene (HBB), and 13 C 12 -labeled 1,2-bis(2,4,6- 2008, 2017), five AHFRs (Hardy et al., 2008; Wikoff et al., 2015), and
tribromophenoxy) ethane (BTBPE), applied to a column packed six PFRs (Ali et al., 2012; Kamata et al., 1989; Matthews et al., 1990;
with florisil and eluted with 50% (v/v) dichloromethane/n-hexane. Stauffer, 1981), as shown in Table S3.
The eluate was evaporated and redissolved in nonane. For
tetrabromobisphenol A (TBBPA) and PFRs analysis, D 12-tris(2- 2.6. Statistical analysis
chloroethyl) phosphate (TCEP), D9-tris(dimethylphenyl) phosphate
(TDMPP), D 51-tris(2-ethylhexyl) phosphate (TEHP), D21 - tris The associations between obtained bioaccessibility values and phys-
(methylphenyl) phosphate (TMPP), D 27-tri-n-butyl phosphate icochemical properties such as molecular weight, octanol–water parti-
(TNBP), and D15-triphenyl phosphate (TPHP) were added to a por- tion coefficient (log KOW), and water solubility were investigated by
tion of crude extract. The mixture was passed through an Isolute Spearman's rank order correlation analysis (SigmaPlot version 14.0;
C18 (EC) column, followed by 10 mL of methanol. The methanol elu- Systat Software, Inc., San Jose, CA, USA).
ate was evaporated until small volume. We used GC-EI-MS/MS to
determine concentrations of PBDEs and AHFRs without TBBPA and 2.7. Quality assurance and quality control
LC-ESI-MS/MS to determine TBBPA and PFRs concentrations. The
GC-EI-MS/MS and LC-ESI-MS/MS measurement conditions are Samples were analyzed in accordance with the established
described in the Supplementary data. laboratory quality assurance and quality control procedures. Chemical
analysis was conducted under UV-cutoff conditions to prevent
2.4. Inhalation bioaccessibility of FRs photodegradation of the brominated FRs. Precision and accuracy were
promoted via replicate analyses (n = 3) for all tested samples. The av-
The inhalation bioaccessibility value of each FR in the indoor dust erage recovery rates of internal standards of nine PBDE congeners
samples in the SELF or ALF condition (%Bio) was determined as: ( 13 C 12 -BDE-28, -47, -99, -153, -154, -183, -197, -207, and -209),
two AHFRs (13C 6 -HBB and 13 C 12 -BTBPE), and six PFR compounds
C bio (D12-TCEP, D15-TPHP, D21-TMPP, D9-TDMPP, D27-TNBP, and D51-TEHP)
%Bio ¼  100 ð1Þ
C mass for all samples were 85%, 77%, and 91%, respectively. The external
standards D18-HBCD (for LC analysis) and 13C12-BDE138 (for GC analysis)
where Cbio is the cumulative bioaccessible concentration of FR in super- were spiked in all tested samples. Detailed information is presented in
natant for 4 days, and Cmass represents the mass concentration of FR in Tables S4–S6. The limit of quantification values of PBDEs, AHFRs, and
the indoor dust (Wannomai et al., 2020). Those FRs having no bioacces- PFRs are listed in Table 1. The concentrations of PBDEs, AHFRs, and most
sible concentration because of their low mass concentration were PFRs in procedural blanks for the bioaccessibility test with SELF or ALF
excluded from the calculation of bioaccessibility to appropriately com- solution were below the limit of quantification, whereas the blank values
pare FR bioaccessibility among indoor dust samples in this study. were subtracted from the samples for TCEP, TCIPP, and TNBP.

2.5. Health risk assessment 3. Results and discussion

To assess inhalation exposure, we must consider groups of exposed 3.1. Bioaccessible concentration
population, condition and pathways of exposure, and the amount of
chemical consumed (US EPA, 2003). To assess the non-cancer risk The mass concentrations (Wannomai et al., 2020) and bioaccessible
from inhalation exposure to FRs for workers in an e-waste- concentrations of 12 PBDEs, 8 AHFRs, and 16 PFRs in the SELF and ALF
dismantling workshop, the daily intake of FRs via inhalation exposure conditions are listed in Table 1. The average mass concentrations of FRs
(DI; ng/kg BW/d) was calculated as: were 130,000, 140,000, and 74,000 ng/g for workplace dust (n = 3),
floor dust (n = 3), and settled dust (n = 2), respectively. The average
C bio  IR  ET
DI ¼ ð2Þ bioaccessible concentrations of FRs were 1900, 1400, and 270 ng/g in
BW
the SELF condition and 2600, 770, and 490 ng/g in the ALF condition, re-
where Cbio is the bioaccessible concentration of FR for inhalation expo- spectively. Thus, our results clearly indicate that the bioaccessible con-
sure (ng/m3), IR is the rate of inhalation (m3/h), ET is the exposure time centrations of FRs investigated in this study are much lower than their
(h/d), and BW is body weight (kg). Because we tried to compare bioac- mass concentrations. The average mass concentrations of FRs obtained
cessible concentrations and bioaccessibility values of FRs upon inhala- for the indoor dust samples decreased in the order floor dust > work-
tion exposure (this study) and ingestion exposure (Wannomai et al., place dust > settled dust, and the average bioaccessible concentrations
2020) with the same dust matrices, the FR concentration in indoor dust of FRs in both the SELF and ALF conditions decreased in the order work-
(ng/g dust) was converted to FR concentration in the working environ- place dust > floor dust > settled dust. These results indicated that the
ment air (ng/m3) by using the average (0.747 mg dust/m3) and bioaccessible concentrations of FRs in settled dust tended to be lower
maximum (4.183 mg dust/m3) dust concentrations in working environ- than those of workplace dust and floor dust, reflecting the order of
ment air of e-waste-dismantling facilities in Japan (Suzuki et al., 2019). mass concentration of FRs detected in dust. As noted by Xie et al.
The IR value used here was 1.67 m3/h (Wang et al., 2009). ET was 8 h/d (2018), this result might be due to finer particulates having greater sur-
based on interviews with workers, and BW was 55 kg of the average for face area for subsequent sorption of hydrophobic chemicals. In fact, the
Vietnamese adults (Wannomai et al., 2020). mass percentage for the fine particle size fraction (<250 μm) in the set-
The hazard quotient (HQ) was obtained by dividing DI by reference tled dust (average 76%, n = 2) was higher than those in the floor dust
doses: (average 60%, n = 3) and workplace dust (average 7.7%, n = 3)
(Wannomai et al., 2020), suggesting that the settled dust tends to have
more fine particles compared to the other dust samples, especially the
DI workplace dust. However, workplace dust was dust generated from e-
HQ ¼ ð3Þ
RfD waste dismantling collected onto a tarpaulin, meaning that workplace

3
 T. Wannomai, H. Matsukami, N. Uchida et al.
Table 1
Mass concentrations and inhalation bioaccessible concentrations (ng/g) in the simulated epithelial lung fluid (SELF) or artificial lysosomal fluid (ALF) for indoor dust samples.

Compounds LOQ Workplace dust Floor dust Settled dust

Mass concc Bioaccessible conc Mass concc Bioaccessible conc Mass concc Bioaccessible conc

SELF ALF SELF ALF SELF ALF

a b
Mass Bio 1 2 3 1 2 3 1 2 3 1 2 3 1 2 3 1 2 3 2 3 2 3 2 3

PBDEs
BDE-28 1 0.5 360 720 34 <LOQ 1 <LOQ <LOQ <LOQ <LOQ 16 800 130 <LOQ 15 <LOQ <LOQ <LOQ <LOQ 160 120 <LOQ <LOQ <LOQ <LOQ
BDE-47 1 0.5 1100 2800 170 <LOQ 5 <LOQ <LOQ 2 <LOQ 50 4100 570 1 71 1 <LOQ 3 <LOQ 820 640 <LOQ <LOQ <LOQ 1
BDE-99 1 0.5 670 2500 220 <LOQ 2 <LOQ <LOQ 1 <LOQ 63 4200 670 <LOQ 51 <LOQ <LOQ 2 <LOQ 980 730 <LOQ <LOQ <LOQ 2
BDE-100 1 0.5 41 130 13 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 21 350 45 <LOQ 3 <LOQ <LOQ <LOQ <LOQ 68 50 <LOQ <LOQ <LOQ <LOQ
BDE-153 1 1 430 660 47 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 57 890 170 <LOQ 12 1 <LOQ <LOQ <LOQ 290 230 <LOQ 1 <LOQ <LOQ
BDE-154 1 1 100 180 19 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 12 280 44 <LOQ 1 <LOQ <LOQ <LOQ <LOQ 79 45 <LOQ <LOQ <LOQ <LOQ
BDE-183 2 1 750 230 40 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 190 660 120 <LOQ 8 <LOQ <LOQ <LOQ <LOQ 360 330 <LOQ <LOQ <LOQ <LOQ
BDE-196 5 1 390 100 57 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 53 520 79 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 170 200 <LOQ <LOQ <LOQ <LOQ
BDE-197 5 1 480 130 34 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 87 390 45 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 200 160 <LOQ <LOQ <LOQ <LOQ
BDE-206 10 3 2400 1400 1000 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 180 5600 1500 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 1600 1900 <LOQ <LOQ <LOQ <LOQ
BDE-207 10 3 1600 720 490 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 180 2800 660 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 960 970 <LOQ <LOQ <LOQ <LOQ
BDE-209 20 5 48,000 31,000 28,000 <LOQ <LOQ <LOQ <LOQ <LOQ 31 4000 130,000 36,000 <LOQ 73 <LOQ <LOQ <LOQ <LOQ 33,000 41,000 <LOQ <LOQ 13 25
Total PBDEs 56,321 40,570 30,124 <LOQ 8 <LOQ <LOQ 3 31 4909 150,590 40,033 1 234 2 <LOQ 5 <LOQ 38,687 46,375 <LOQ 1 13 28
AHFRs
TBBPA 20 30 9100 4900 8500 37 200 72 <LOQ <LOQ <LOQ 780 13,000 6200 <LOQ 2600 180 <LOQ 23 <LOQ 19,000 9700 150 190 <LOQ <LOQ
DBDPE 25 10 22,000 4700 4800 <LOQ <LOQ <LOQ <LOQ <LOQ 100 1300 37,000 7900 <LOQ <LOQ <LOQ <LOQ 49 <LOQ 14,000 8200 <LOQ <LOQ <LOQ 180
BTBPE 10 2 2000 1800 110 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 950 2100 420 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 960 890 <LOQ <LOQ <LOQ <LOQ
HBB 5 2 920 640 3000 <LOQ <LOQ 8 <LOQ <LOQ <LOQ 650 4300 320 <LOQ 26 <LOQ <LOQ <LOQ <LOQ 460 1200 <LOQ <LOQ <LOQ 4
4

anti-DP 5 2 710 1000 1600 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 200 2900 250 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 870 1600 <LOQ <LOQ <LOQ 3
syn-DP 5 2 220 870 480 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 74 1200 130 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 580 660 <LOQ <LOQ <LOQ 3
BEH-TEBP 20 2 520 810 92 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 410 160 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 200 310 <LOQ <LOQ <LOQ <LOQ
EH-TBB 5 2 21 140 170 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 9 160 230 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 19 160 <LOQ <LOQ <LOQ <LOQ
Total AHFRs 35,491 14,860 18,752 37 200 80 <LOQ <LOQ 100 3963 61,070 15,610 <LOQ 2626 180 <LOQ 72 <LOQ 36,089 22,720 150 190 <LOQ 190
PFRs
TCEP 20 10 390 3300 12,000 21 240 1500 57 310 1800 120 2200 410 <LOQ 130 69 19 210 78 450 550 26 53 49 61
TCIPP 20 10 890 18,000 1100 111 2700 330 240 3900 390 280 11,000 2100 <LOQ 670 260 41 930 220 2400 1100 110 91 240 96
TDCIPP 20 10 250 380 2100 <LOQ 19 150 33 21 250 210 1300 350 47 41 52 <LOQ 130 70 350 630 22 38 24 39
TPHP 20 10 23,000 28,000 30,000 <LOQ <LOQ 97 75 160 280 1700 37,000 17,000 <LOQ 22 <LOQ 12 390 100 27,000 14,000 81 52 130 100
MPDPP 20 10 2400 6600 11,000 <LOQ <LOQ 42 <LOQ <LOQ 82 390 12,000 3100 <LOQ <LOQ <LOQ <LOQ 42 <LOQ 4300 2400 <LOQ <LOQ 11 10
BMPPP 20 10 1700 5300 8400 <LOQ <LOQ 18 <LOQ <LOQ 23 270 10,000 2700 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 3200 2000 <LOQ <LOQ <LOQ <LOQ
EHDPP 20 10 48 52 78 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 50 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 66 <LOQ <LOQ <LOQ <LOQ <LOQ

Science of the Total Environment 760 (2021) 143862

TMPP 20 10 1500 2600 3600 <LOQ <LOQ 25 <LOQ <LOQ <LOQ 170 6900 1300 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 2400 1700 <LOQ <LOQ <LOQ <LOQ
TDMPP 20 10 130 360 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 200 780 77 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 160 66 <LOQ <LOQ <LOQ <LOQ
TIPPP 20 10 1600 1400 260 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 100 4100 1200 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 1200 880 <LOQ <LOQ <LOQ <LOQ
PBDPP 20 10 6000 1000 130 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 1400 5600 2700 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 3300 1100 <LOQ <LOQ <LOQ <LOQ
BPA-BDPP 20 10 10,000 3100 960 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 1300 12,000 2600 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 6300 2200 <LOQ <LOQ <LOQ <LOQ
PBDMPP 20 10 1400 860 89 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 86 1100 240 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 700 320 <LOQ <LOQ <LOQ <LOQ
TNBP 20 10 82 170 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 150 250 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ
TBOEP 20 10 180 45 <LOQ 25 <LOQ <LOQ 24 <LOQ <LOQ 57 50 67 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ
TEHP 20 10 200 150 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 74 <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ <LOQ 90 <LOQ <LOQ <LOQ <LOQ <LOQ
Total PFRs 49,770 71,317 69,717 157 2959 2162 429 4391 2825 6433 104,404 33,844 47 863 381 72 1702 468 51,916 26,946 239 234 454 306

LOQ, limit of quantification; SELF, simulated epithelial lung fluid; ALF, artificial lysosomal fluid.
a
LOQ for mass concentration cited from Wannomai et al. (2020).
b
LOQ for bioaccessible concentration in this study.
c
Cited from Wannomai et al. (2020).
T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

dust may contain more small e-waste particles produced during disman- et al., 2019; Kademoglou et al., 2018; Li et al., 2019; Wannomai et al.,
tling activity than the other two types of dust. This would explain why 2020; Xie et al., 2018; Zeng et al., 2019), the bioaccessibility in an artifi-
the bioaccessible concentrations of FRs from workplace dust tended to cial fluid is likely to be influenced by the physicochemical properties of
be higher than those of settled dust and floor dust. The average mass con- the compounds. Therefore, correlations between the measured bioac-
centrations of FRs for workplace dust decreased in the order PFRs > cessibility of FR in the SELF or ALF condition and physicochemical prop-
PBDEs > AHFRs and those for floor dust and settled dust decreased in erties such as molecular weight, log KOW, and water solubility were
the order PBDEs > PFRs > AHFRs. The average bioaccessible concentra- investigated in this study. As shown in Fig. 3, we observed a negative
tions of FRs for indoor dust samples in the SELF and ALF conditions, ex- correlation with molecular weight (SELF: r = −0.397, P < 0.01, n =
cept those for floor dust-2 in the SELF condition, decreased in the order 53; ALF: r = −0.582, P < 0.01, n = 53), and log KOW (SELF: r =
PFRs > AHFRs > PBDEs. As shown in Table 1 for the bioaccessible concen- −0.604, P < 0.01, n = 53; ALF: r = −0.842, P < 0.01, n = 53), and a pos-
trations of indoor dust samples in the SELF and ALF conditions, some PFRs itive correlation with water solubility (SELF: r = 0.688, P < 0.01, n = 53;
and AHFRs tended to be easier to elute from dust matrices to the artificial ALF: r = 0.846, P < 0.01, n = 53).
fluids as compared to PBDEs. In terms of individual FRs, TCEP, TCIPP, Similar trends were observed in our previous study investigating the
TDCIPP, and TPHP among the 16 PFRs and TBBPA among the 8 AHFRs ingestion bioaccessibility of FRs in the same dust samples (Wannomai
showed relatively high inhalation bioaccessible concentrations. et al., 2020). Previous studies using the inhalation bioaccessibility test
with artificial fluid also noted that the bioaccessibility of organic pollut-
3.2. Inhalation bioaccessibility ants is governed by their physicochemical properties. Kademoglou et al.
(2018) reported that the inhalation bioaccessibility of phthalate esters
The inhalation bioaccessibility values of FRs in the SELF and ALF con- in indoor dust (<63 μm) significantly decreased with lower log KOW in
ditions for the indoor dust samples are shown in Figs. 1 and 2. Detailed Gamble's solution and ALF but increased with greater water solubility
inhalation bioaccessibility data are provided in Table S7. Our results in Gamble's solution. A negative correlation was observed between
tended to show a similar profile of the FR bioaccessibility among indoor the inhalation bioaccessibility of polyaromatic sahydrocarbons (PAHs)
dust samples. This means that TCEP (5.4–19%, Table S7), TCIPP in e-waste-burning particulate matter (<5.6 μm) and log KOW in modi-
(4.6–35%), and TDCIPP (3.2–22%) had comparably high bioaccessibility fied Gamble's solution and in ALF (Xie et al., 2018). The inhalation bio-
values in the SELF and ALF conditions as compared to other FRs detected accessibility of the PAHs in PM2.5 also had a negative relationship with
in the indoor dust samples. Note, however, that TCEP and TCIPP bioac- log KOW (Li et al., 2019). Thus, results of this and previous studies sug-
cessibility values in the SELF condition and bioaccessibility of TDCIPP gest that log KOW and water solubility are key factors for the bioaccessi-
in the ALF condition for floor dust-1 were not obtained because of bility of organic contaminants adsorbed on particulates.
their low mass concentrations (Table S7). Furthermore, some FRs con-
cern us based on bioaccessibility and/or detection frequency. Among 3.4. Daily intake of FRs via inhalation exposure
the FRs investigated, TBBPA (0.41–20%) also showed moderately high
bioaccessibility at medium frequency in the SELF condition, but not in The DI values of FRs via inhalation exposure for workers in the e-
the ALF condition. This suggests that slightly acidic phenolic com- waste-dismantling workshops are listed in Table S8. While considering
pounds, such as TBBPA, cannot be easily eluted from particulates of in- the daily intake for lower airway passages such as trachea, alveoli, and
door dust in ALF, which simulates the more acidic environment bronchioles in this pathway, it was expected that the particle size
following phagocytosis by alveolar and interstitial macrophages within which could potentially be inhaled and placed into SELF and ALF condi-
the lung (Kademoglou et al., 2018; Midander et al., 2007). TBOEP bioac- tions should be approximately 2.5–100 μm or smaller (Ogden, 1992).
cessibility for workplace dust-1 was high in not only the SELF but also This research, however, is subjected to the particle size limitation. So,
the ALF condition (14% and 13%, respectively), even though the mass the DI values of FRs via inhalation exposure was considered from the
concentration of TBOEP was lower than those of major FRs such as particle size under 0.25 mm. The ratios of median-based DI of FRs by
BDE-209, TBBPA, DBDPE, TCIPP, and TPHP (Table 1). This probably re- using mass concentration, bioaccessible concentration in the SELF con-
flects the fact that the water solubility of TBOEP (1100 mg/L at 25 °C) dition, or bioaccessible concentration in the ALF condition are shown
is much higher than that of other FRs (Table S2). Based on that, the in Fig. 4. In this study, FR concentration (ng/g dust) was converted to
mass concentrations of TBOEP in other dust samples must be quite FR concentration (ng/m3) by using the average (0.747 mg dust/m3)
low to detect its bioaccessibility in these kinds of experiments. and maximum (4.183 mg dust/m3) dust concentrations in the working
When we compared the inhalation bioaccessibility of FRs with the environment of e-waste-dismantling facilities in Japan (Suzuki et al.,
ingestion bioaccessibility of FRs determined using a physiologically 2019). The median concentrations of PBDEs and PFRs in the working en-
based extraction test for the same samples used in this study vironment were 30 (3.7–110) ng/m3 and 38 (4.8–78) ng/m3 for the
(Wannomai et al., 2020), the profile of the FR bioaccessibility was sim- normal-case scenario with the average dust concentration and 170
ilar but there were some differences. TCEP, TCIPP, and TDCIPP bioacces- (21–630) ng/m3 and 210 (27–440) ng/m3 for the worst-case scenario
sibility values were high in the ingestion condition. In addition, with the maximum dust concentration, respectively. Concentrations of
ingestion bioaccessibility values of TBOEP and TNBP, which have high PBDEs and PFRs in the normal-case scenario were ten times those of
water solubility (Table S2), were also high. Although TCEP, TNBP, and PBDEs (BDE-28, -47, -99, -100, -153, -154, -183, and -209) and equiva-
TBOEP bioaccessibility values were apparently higher in the ingestion lent to those of PFRs (TIBP, TNBP, TCEP, TCIPP, TDCIPP, TBOEP, TPHP,
condition than in the inhalation condition, those of TCIPP and TDCIPP EHDPP, TEHP, and TCPs) in indoor and outdoor environment samples
were similar in both conditions. These results indicate that profiles of (school, office, and residence) collected in three districts of a megacity
the FR bioaccessibility are basically similar in the artificial fluids, includ- in China (Hu et al., 2019). Based on this result, we concluded that FR
ing the small-intestine solution used for physiologically based extrac- concentrations (ng/m3) calculated for the working environment of e-
tion test, SELF, and ALF, although FR bioaccessibility is somewhat waste-dismantling workshops were reasonable for calculation of daily
different among the compounds tested and the chemical composition intake via inhalation exposure. As shown in Table S8, DI based on the
and pH of the artificial fluid does influence the bioaccessibility. mass concentration was hundreds of times those based on bioaccessible
concentrations in the SELF and ALF conditions. Reflecting the bioacces-
3.3. The influence of physicochemical properties on inhalation bioaccessibility sibility values obtained in this study, calculated DI values in the
normal- and worst-case scenarios clearly indicate that PBDE values
Based on previous studies using the bioaccessibility test of organic were highest when using mass concentrations and lowest when using
contaminants (Collins et al., 2015; Fang and Stapleton, 2014; Guo bioaccessible concentrations. The median-based DI values of FRs via

5
 6

FR bioacces s ibility (%)

10%
15%
20%
25%
30%
35%

0%
5%
10%
20%
30%

15%
25%
35%

0%
5%
BDE-28 BDE-28
BDE-47 BDE-47
BDE-99 BDE-99
BDE-100 BDE-100
BDE-153 BDE-153
BDE-154 BDE-154
BDE-183 BDE-183
BDE-196 BDE-196
BDE-197 BDE-197
BDE-206 BDE-206
BDE-207 BDE-207
BDE-209 BDE-209
TBBPA TBBPA
DBDPE DBDPE
BTBPE BTBPE
HBB HBB
an-DP an-DP
syn-DP syn-DP
BEH-TEBP BEH-TEBP
EH-TBB

Floor dust-1
EH-TBB
TCEP TCEP
Workplace dust-1

TCIPP TCIPP
TDCIPP TDCIPP
TPHP TPHP
MPDPP MPDPP
BMPPP BMPPP
EHDPP EHDPP
TMPP TMPP
TDMPP TDMPP
TIPPP TIPPP
PBDPP PBDPP
BPA-BDPP BPA-BDPP
PBDMPP PBDMPP
TNBP TNBP
TBOEP TBOEP
TEHP TEHP

20%
35%

10%
15%
25%
30%
35%
10%
15%
20%
25%
30%

0%

0%
5%
5%

10%
15%
20%
25%
30%
35%

5%
0%

BDE-28 BDE-28 BDE-28

BDE-47 BDE-47 BDE-47
BDE-99 BDE-99 BDE-99
BDE-100 BDE-100 BDE-100
BDE-153 BDE-153 BDE-153
BDE-154 BDE-154 BDE-154
BDE-183 BDE-183 BDE-183
BDE-196 BDE-196 BDE-196
BDE-197 BDE-197 BDE-197
BDE-206 BDE-206 BDE-206
BDE-207 BDE-207 BDE-207
BDE-209 BDE-209 BDE-209
TBBPA TBBPA TBBPA
DBDPE DBDPE DBDPE
BTBPE BTBPE BTBPE
HBB HBB HBB
an-DP an-DP an-DP
syn-DP syn-DP syn-DP
BEH-TEBP BEH-TEBP BEH-TEBP
EH-TBB EH-TBB EH-TBB
Floor dust-2

Seled dust-2

TCEP TCEP TCEP

Workplace dust-2

TCIPP TCIPP TCIPP

TDCIPP TDCIPP TDCIPP
TPHP TPHP TPHP
MPDPP MPDPP MPDPP
BMPPP BMPPP BMPPP
EHDPP EHDPP EHDPP
TMPP TMPP TMPP
TDMPP TDMPP TDMPP
TIPPP TIPPP TIPPP
PBDPP PBDPP PBDPP
BPA-BDPP BPA-BDPP BPA-BDPP
PBDMPP PBDMPP PBDMPP
TNBP TNBP TNBP
TBOEP TBOEP TBOEP
TEHP TEHP TEHP
35%

10%
15%
20%
25%
30%

0%
5%

25%
35%

10%
15%
20%
30%

0%
5%
10%
15%
20%
25%
30%
35%

5%
0%

BDE-28 BDE-28 BDE-28

BDE-47 BDE-47 BDE-47
BDE-99 BDE-99 BDE-99
BDE-100 BDE-100 BDE-100
BDE-153 BDE-153 BDE-153
BDE-154 BDE-154 BDE-154
BDE-183 BDE-183 BDE-183
BDE-196 BDE-196 BDE-196
BDE-197 BDE-197 BDE-197
BDE-206 BDE-206 BDE-206
BDE-207 BDE-207 BDE-207
BDE-209 BDE-209 BDE-209
TBBPA
Fig. 1. The inhalation bioaccessibility values of flame retardants (FRs) in the simulated epithelial lung fluid (SELF) condition for the indoor dust samples.

TBBPA TBBPA
DBDPE DBDPE DBDPE
BTBPE BTBPE BTBPE
HBB HBB HBB
an-DP an-DP an-DP
syn-DP syn-DP syn-DP
BEH-TEBP BEH-TEBP BEH-TEBP
EH-TBB EH-TBB EH-TBB
Floor dust-3

Seled dust-3

TCEP TCEP TCEP

Workplace dust-3

TCIPP TCIPP TCIPP

TDCIPP TDCIPP TDCIPP
TPHP TPHP TPHP
MPDPP MPDPP MPDPP
BMPPP BMPPP BMPPP
EHDPP EHDPP EHDPP
TMPP TMPP TMPP
TDMPP TDMPP TDMPP
TIPPP TIPPP TIPPP
PBDPP PBDPP PBDPP
BPA-BDPP BPA-BDPP BPA-BDPP
PBDMPP PBDMPP PBDMPP
TNBP TNBP TNBP
TBOEP TBOEP TBOEP
TEHP TEHP TEHP

Science of the Total Environment 760 (2021) 143862 T. Wannomai, H. Matsukami, N. Uchida et al.
 7

FR bioacces s ibility (%)

10%
15%
20%
25%
30%
35%

5%
0%
35%

10%
15%
20%
25%
30%

0%
5%
BDE-28 BDE-28
BDE-47 BDE-47
BDE-99 BDE-99
BDE-100 BDE-100
BDE-153 BDE-153
BDE-154 BDE-154
BDE-183 BDE-183
BDE-196 BDE-196
BDE-197 BDE-197
BDE-206 BDE-206
BDE-207 BDE-207
BDE-209 BDE-209
TBBPA TBBPA
DBDPE DBDPE
BTBPE BTBPE
HBB HBB
an-DP an-DP
syn-DP syn-DP
BEH-TEBP BEH-TEBP
EH-TBB

Floor dust-1
EH-TBB
TCEP TCEP
Workplace dust-1

TCIPP TCIPP
TDCIPP TDCIPP
TPHP TPHP
MPDPP MPDPP
BMPPP BMPPP
EHDPP EHDPP
TMPP TMPP
TDMPP TDMPP
TIPPP TIPPP
PBDPP PBDPP
BPA-BDPP BPA-BDPP
PBDMPP PBDMPP
TNBP TNBP
TBOEP TBOEP
TEHP TEHP

25%
35%

10%
15%
20%
30%

0%
5%
10%
20%
15%
25%
30%
35%

0%
5%
10%
15%
20%
25%
30%
35%

5%
0%

BDE-28 BDE-28 BDE-28

BDE-47 BDE-47 BDE-47
BDE-99 BDE-99 BDE-99
BDE-100 BDE-100 BDE-100
BDE-153 BDE-153 BDE-153
BDE-154 BDE-154 BDE-154
BDE-183 BDE-183 BDE-183
BDE-196 BDE-196 BDE-196
BDE-197 BDE-197 BDE-197
BDE-206 BDE-206 BDE-206
BDE-207 BDE-207 BDE-207
BDE-209 BDE-209 BDE-209
TBBPA TBBPA TBBPA
DBDPE DBDPE DBDPE
BTBPE BTBPE BTBPE
HBB HBB HBB
an-DP an-DP an-DP
syn-DP syn-DP syn-DP
BEH-TEBP BEH-TEBP BEH-TEBP
EH-TBB
Floor dust-2

EH-TBB EH-TBB
Seled dust-2

TCEP TCEP TCEP

TCIPP
Workplace dust-2

TCIPP TCIPP
TDCIPP TDCIPP TDCIPP
TPHP TPHP TPHP
MPDPP MPDPP MPDPP
BMPPP BMPPP BMPPP
EHDPP EHDPP EHDPP
TMPP TMPP TMPP
TDMPP TDMPP TDMPP
TIPPP TIPPP TIPPP
PBDPP PBDPP PBDPP
BPA-BDPP BPA-BDPP BPA-BDPP
PBDMPP PBDMPP PBDMPP
TNBP TNBP TNBP
TBOEP TBOEP TBOEP
TEHP TEHP TEHP
10%
20%
15%
25%
30%
35%

0%
5%
10%
15%
20%
25%
30%
35%

5%
0%

10%
20%
15%
25%
30%
35%

0%
5%

BDE-28 BDE-28 BDE-28

BDE-47 BDE-47 BDE-47
BDE-99 BDE-99 BDE-99
BDE-100 BDE-100 BDE-100
BDE-153 BDE-153 BDE-153
BDE-154 BDE-154 BDE-154
BDE-183 BDE-183 BDE-183
BDE-196 BDE-196 BDE-196
BDE-197 BDE-197 BDE-197
BDE-206 BDE-206 BDE-206
BDE-207 BDE-207 BDE-207
BDE-209 BDE-209 BDE-209
Fig. 2. The inhalation bioaccessibility values of flame retardants (FRs) in the artificial lysosomal fluid (ALF) condition for the indoor dust samples.

TBBPA TBBPA TBBPA

DBDPE DBDPE DBDPE
BTBPE BTBPE BTBPE
HBB HBB HBB
an-DP an-DP an-DP
syn-DP syn-DP syn-DP
BEH-TEBP BEH-TEBP BEH-TEBP
EH-TBB EH-TBB EH-TBB
Floor dust-3

Seled dust-3

TCEP TCEP TCEP

TCIPP
Workplace dust-3

TCIPP TCIPP
TDCIPP TDCIPP TDCIPP
TPHP TPHP TPHP
MPDPP MPDPP MPDPP
BMPPP BMPPP BMPPP
EHDPP EHDPP EHDPP
TMPP TMPP TMPP
TDMPP TDMPP TDMPP
TIPPP TIPPP TIPPP
PBDPP PBDPP PBDPP
BPA-BDPP BPA-BDPP BPA-BDPP
PBDMPP PBDMPP PBDMPP
TNBP TNBP TNBP
TBOEP TBOEP TBOEP
TEHP TEHP TEHP

Science of the Total Environment 760 (2021) 143862 T. Wannomai, H. Matsukami, N. Uchida et al.
T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

SELF condi on
100%
r = −0.397 r = −0.604 r = 0.688
P < 0.01 P < 0.01 P < 0.01
10%

1.0%
PBDEs
AHFRs
FR bioaccessibility (%)

0.10%
PFRs

0.010%

10

1.0E-8

1.0E-6

1.0E-4

1.0E-2
12

1.0E+0

1.0E+2

1.0E+4
200

300

400

500

600

700

800

900
1000
0

14
ALF condi on
100%
r = −0.582 r = −0.842 r = 0.846
P < 0.01 P < 0.01 P < 0.01
10%

1.0%

0.10%

0.010%
10

1.0E-8

1.0E-6

1.0E-4

1.0E-2
12

1.0E+4
1.0E+0

1.0E+2
200

300

400

500

600

700

800

900

8
1000

14

Molecular weight Log KOW Water solubility (25 oC)

Fig. 3. Correlations between flame retardant (FR) inhalation bioaccessibility in the simulated epithelial lung fluid (SELF) or artificial lysosomal fluid (ALF) condition and molecular weight,
log KOW, and water solubility.

Mass concentraon
50
40
30
20
Rati o of me di an-based dai l y i nhal ation for FRs (%)

10
0
BPA-BDPP
an-DP
syn-DP

PBDPP
TIPPP
BTBPE

BMPPP
TCIPP

PBDMPP
TDCIPP

MPDPP

TBOEP
TBBPA

EH-TBB

TNBP
DBDPE

TMPP
TPHP

EHDPP

TDMPP
HBB

TCEP

TEHP
BDE-47
BDE-99
BDE-28

BEH-TEBP
BDE-100
BDE-153
BDE-154

BDE-196
BDE-183

BDE-197
BDE-206
BDE-207
BDE-209

Bioaccessible concentraon on SELF

50
40
30
20
10
0
BPA-BDPP
an-DP
syn-DP

PBDPP
TIPPP
BTBPE

BMPPP
TCIPP

PBDMPP
TDCIPP

MPDPP

TBOEP
TBBPA
DBDPE

EH-TBB

TNBP
TMPP
TPHP

EHDPP

TDMPP
HBB

TCEP

TEHP
BDE-28
BDE-47
BDE-99

BEH-TEBP
BDE-100
BDE-153
BDE-154

BDE-196
BDE-197

BDE-207
BDE-209
BDE-183

BDE-206

Bioaccessible concentraon on ALF

60
50
40
30
20
10
0
BPA-BDPP
an-DP
syn-DP

PBDPP
TIPPP
BTBPE

BMPPP

PBDMPP
TCIPP
TDCIPP

MPDPP

TBOEP
TBBPA
DBDPE

EH-TBB

TNBP
TMPP
TPHP

EHDPP

TDMPP
HBB

TCEP

TEHP
BDE-47
BDE-99
BDE-28

BEH-TEBP
BDE-100
BDE-153
BDE-154

BDE-196
BDE-197

BDE-207
BDE-209
BDE-183

BDE-206

Fig. 4. Ratio of the median-based daily intake of flame retardants (FRs) via inhalation exposure on the basis of mass concentration, bioaccessible concentration in the simulated epithelial
lung fluid (SELF) condition, and bioaccessible concentration in the artificial lysosomal fluid (ALF) condition for workers in an e-waste-dismantling workshop.

8
T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

inhalation exposure on the basis of mass concentration decreased in the are the upper airway passages (nose, nasal passages, mouth, and phar-
order of BDE-209 > TPHP > TBBPA > DBDPE > MPDPP, whereas those ynx) and the lower airway passages (trachea, alveoli, and bronchioles)
based on bioaccessible concentrations decreased in the order of TCIPP that the particles can get into the respiratory system. Besides, particles
> TBBPA > TCEP > TDCIPP > TPHP in the SELF condition and TCIPP > can deeply get into the air passages depending on several factors such
TPHP > TCEP > TDCIPP > MPDPP in the ALF condition. Our results indi- as size, shape, and density of the particles, Moreover, it also depends
cate that actual intake of FRs via inhalation exposure is probably much on their chemical and toxic properties. To our knowledge, this is the
lower than when estimated without their bioaccessibility. first health risk assessment of FRs via inhalation exposure based on bio-
accessible concentration. Our results clearly indicate that the inhalation
3.5. Hazard quotient of FRs via inhalation exposure exposure to FRs during indoor dismantling of e-waste in this area is neg-
ligible based on the current methodology of non-cancer health risk as-
Base on the DI values of FRs via inhalation exposure for workers in sessment used in this study. However, the effect estimates in the
this study, the non-cancer HQ values for FRs via inhalation exposure current methodology are based on interventional and prospective ob-
for workers in the e-waste-dismantling workshops are reported in servational studies. In this study, the chronic oral RfD values were
Table S9 and Fig. 5. In the worst-case scenario, the highest HQ values ob- used to calculate HQ, but it was inhalation exposure to FRs, not ingestion
tained by using mass concentration, bioaccessible concentration in the exposure, that was assessed. Thus, further in vivo studies are needed to
SELF condition, and bioaccessible concentration in the ALF condition measure chronic inhalation RfD values of FRs so that health risk assess-
were 4.3E-02 for BDE-99, 7.2E-04 for BDE-47, and 8.3E-05 for TCEP, re- ment can be based on those values. In the near future, highly toxic FRs as
spectively. These findings clearly indicate that the HQ values of FRs via well as bioaccessible FRs detected in indoor dust also should be evalu-
inhalation exposure for workers in the e-waste-dismantling workshops ated through this kind of in vivo study. It is also necessary to assess
are surely less than 1, even if mass concentration (100% bioaccessibility) the influence of various physiological parameters and substances
is used for the calculation of HQ. Furthermore, the sum of the bioacces- coexisting with toxic compounds (e.g., food material for the ingestion
sible concentration–based HQ values of individual FRs via inhalation ex- exposure) on bioaccessibility of particulate-bound or -containing
posure obtained in this study (3.9E-08 to 7.2E-04) and those via chemicals such as FRs (Zeng et al., 2019). As noted by Hu et al. (2019),
ingestion exposure in our previous study (1E-04 to 2.7E-01) mixture effect, such as synergistic effect, of chemicals among FRs as
(Wannomai et al., 2020) was less than 1, suggesting that the potential well as other contaminant classes such as heavy metals are unclear
non-cancer health risk for workers of e-waste-dismantling workshops and should be further investigated. According to a report conducted at
in northern Vietnam via both ingestion and inhalation exposure to FRs United Nations University, in 2016 the world generated 44.7 million
is low. Nonetheless, these results must be interpreted with caution tonnes of e-waste containing considerable quantities of valuable and re-
and a number of this study's limitations should be borne in mind. usable metals and plastics, but only 20% was recycled (Baldé et al.,
2017). Therefore, e-waste recycling will likely be encouraged world-
3.6. Implications of our results wide. Because manual dismantling of e-waste is an essential first step
in appropriate recycling. There is a possibility that some of the larger
The primary limitation to the generalization of these results is the particles would be non-respirable and therefore the estimated bioacces-
particle's excretion. Notwithstanding, dust particles ranging from <1 sibility may be overestimated. By the same token, our findings contrib-
to 100 μm might become airborne, depending on their origin and phys- ute to the emerging overall sight of excretion in human lung estimated
ical characteristics and ambient conditions (IUPAC, 1990). However, under lower airway passages including SELF and ALF conditions of the
larger particles up to 250 μm may accidentally enter the body system basis for the future, more integrated health risk assessment studies.
of workers with a high respiration rate and could possibly be able to We must devise better chemical risk assessment methods to ensure
reach a deeper airway passage. Typically, there are two systems which the health and safety of workers in these facilities.

Mass conc Bioaccessible conc in SELF Bioaccessible conc in ALF

TBOEP TBOEP TBOEP
TNBP TNBP TNBP
TPHP TPHP TPHP
TDCIPP TDCIPP TDCIPP
TCIPP TCIPP TCIPP Med Max
TCEP TCEP TCEP

EH-TBB EH-TBB EH-TBB

BEH-TEBP BEH-TEBP BEH-TEBP
BTBPE BTBPE BTBPE
DBDPE DBDPE DBDPE
TBBPA TBBPA TBBPA

BDE-209 BDE-209 BDE-209

BDE-153 BDE-153 BDE-153
BDE-99 BDE-99 BDE-99
BDE-47 BDE-47 BDE-47
1

1
1E-08

1E-06

1E-04

1E-08

1E-06

1E-04

1E-08

1E-06

1E-04
1E-02

1E-02
1E-02

Hazard quoent

Fig. 5. The non-cancer hazard quotient values for flame retardants (FRs) via inhalation exposure on the basis of mass concentration, bioaccessible concentration in the simulated epithelial
lung fluid (SELF) condition, and bioaccessible concentration in the artificial lysosomal fluid (ALF) condition for workers in an e-waste-dismantling workshop.

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T. Wannomai, H. Matsukami, N. Uchida et al. Science of the Total Environment 760 (2021) 143862

CRediT authorship contribution statement Huang, M., Wang, W., Chan, C.Y., Cheung, K.C., Man, Y.B., Wang, X., Wong, M.H., 2014.
Contamination and risk assessment (based on bioaccessibility via ingestion and inha-
lation) of metal(loid)s in outdoor and indoor particles from urban centers of Guang-
Tatiya Wannomai: Conceptualization, Investigation, Writing – zhou, China. Sci. Total Environ. 479–480, 117–124.
original draft, Writing – review & editing. Hidenori Matsukami: Concep- Ikonomou, M.G., Rayne, S., Fischer, M., Fernandez, M.P., Cretney, W., 2002. Occurrence and
congener profiles of polybrominated diphenyl ethers (PBDEs) in environmental sam-
tualization, Investigation, Methodology, Formal analysis, Writing – review ples from coastal British Columbia, Canada. 46 (5), 649–663.
& editing, Funding acquisition. Natsuyo Uchida: Investigation, Validation, IUPAC, 1990. Glossary of atmospheric chemistry terms. International Union of Pure and
Methodology, Writing – review & editing. Fumitake Takahashi: Applied Chemistry, Applied Chemistry Division, Commission on Atmospheric Chem-
istry. Pure Appl. Chem. 62 (11), 2167–2219.
Writing – review & editing. Le Huu Tuyen: Resources. Pham Hung
Johnson, P.I., Stapleton, H.M., Sjodin, A., Meeker, J.D., 2010. Relationships between
Viet: Resources. Shin Takahashi: Resources. Tatsuya Kunisue: polybrominated diphenyl ether concentrations in house dust and serum. Environ.
Resources, Writing – review & editing. Go Suzuki: Conceptualization, Sci. Technol. 44, 5627–5632.
Project administration, Supervision, Writing – review & editing, Jones-Otazo, H.A., Clarke, J.P., Diamond, M.L., Archbold, J.A., Ferguson, G., Harner, T.,
Richardson, G.M., Ryan, J.J., Wilford, B., 2005. Is house dust the missing exposure
Funding acquisition. pathway for PBDEs? An analysis of the urban fate and human exposure to PBDEs. En-
viron. Sci. Technol. 39, 5121–5130.
Declaration of competing interest Kademoglou, K., Giovanoulis, G., Palm-Cousins, A., Padilla-Sanchez, J.A., Magnér, J., de Wit,
C.A., Collins, C.D., 2018. In vitro inhalation bioaccessibility of phthalate esters and al-
ternative plasticisers present in indoor dust using artificial lung fluids. Environ. Sci.
The authors declare that they have no known competing financial Technol. Let. 5 (6), 329–334.
interests or personal relationship that could have appeared to influence Kajiwara, N., Noma, Y., Takigami, H., 2011. Brominated and organophosphate flame retar-
dants in selected consumer products on the Japanese market in 2008. J. Hazard.
the work reported in this paper.
Mater. 192, 1250–1259.
Kamata, E., Naito, K., Nakaji, Y., Ogawa, Y., Suzuku, S., Kaneko, T., Takada, K., Kurokawa, Y.,
Acknowledgements Tobe, M., 1989. Acute and subacute toxicity studies of tris(1, 3-dichloro-2-propyl)
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Li, Y., Juhasz, A., Ma, L.Q., Cui, X., 2019. Inhalation bioaccessibility of PAHs in PM 2.5: im-
We gratefully acknowledge the experimental assistance of Ms. Mino plications for risk assessment and toxicity prediction. Sci. Total Environ. 650, 56–64.
Hasegawa, Mr. Humiaki Kato, Ms. Chieko Michinaka, and Ms. Kyoko Matsukami, H., Tue, N.M., Suzuki, G., Someya, M., Tuyen, L.H., Viet, P.H., Takahashi, S.,
Yoneoka of the National Institute for Environmental Studies and sam- Tanabe, S., Takigami, H., 2015. Flame retardant emission from e-waste recycling op-
eration in northern Vietnam: environmental occurrence of emerging organophos-
pling assistance from members of the Centre for Environmental Tech- phorus esters used as alternatives for PBDEs. Sci. Total Environ. 514, 492–499.
nology and Sustainable Development of VNU Hanoi University of Matsukami, H., Suzuki, G., Tue, N.M., Tuyen, L.H., Viet, P.H., Takahashi, S., Takigami, H.,
Science in Vietnam. This study was supported by a Grant-in-Aid for Sci- 2016. Analysis of monomeric and oligomeric organophosphorus flame retardants in
fish muscle tissues using liquid chromatography–electrospray ionization tandem
entific Research (C) (no. 17K00641) and the Fund for the Promotion of
mass spectrometry: application to Nile tilapia (Oreochromis niloticus) from an e-
Joint International Research (Fostering Joint International Research (B)) waste processing area in northern Vietnam. Emerg. Contam. 2, 89–97.
(no. 18KK0300) from the Japan Society for the Promotion of Science. Matsukami, H., Suzuki, G., Someya, M., Uchida, N., Tue, N.M., Tuyen, L.H., Viet, P.H.,
Takahashi, S., Tanabe, S., Takigami, H., 2017. Concentrations of polybrominated
diphenyl ethers and alternative flame retardants in surface soils and river sediments
Appendix A. Supplementary data from an electronic waste-processing area in northern Vietnam, 2012–2014.
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