close

Вход

Забыли?

вход по аккаунту

?

10934529.2017.1369813

код для вставкиСкачать
Journal of Environmental Science and Health, Part A
Toxic/Hazardous Substances and Environmental Engineering
ISSN: 1093-4529 (Print) 1532-4117 (Online) Journal homepage: http://www.tandfonline.com/loi/lesa20
Organophosphorus flame retardants (PFRs)
and phthalates in floor and road dust from a
manual e-waste dismantling facility and adjacent
communities in Thailand
Dudsadee Muenhor, Hyo-Bang Moon, Sunggyu Lee & Emma Goosey
To cite this article: Dudsadee Muenhor, Hyo-Bang Moon, Sunggyu Lee & Emma Goosey (2017):
Organophosphorus flame retardants (PFRs) and phthalates in floor and road dust from a manual ewaste dismantling facility and adjacent communities in Thailand, Journal of Environmental Science
and Health, Part A, DOI: 10.1080/10934529.2017.1369813
To link to this article: http://dx.doi.org/10.1080/10934529.2017.1369813
Published online: 24 Oct 2017.
Submit your article to this journal
Article views: 2
View related articles
View Crossmark data
Full Terms & Conditions of access and use can be found at
http://www.tandfonline.com/action/journalInformation?journalCode=lesa20
Download by: [University of Florida]
Date: 25 October 2017, At: 22:27
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
2017, VOL. 0, NO. 0, 1?12
https://doi.org/10.1080/10934529.2017.1369813
Organophosphorus ?ame retardants (PFRs) and phthalates in ?oor and road dust
from a manual e-waste dismantling facility and adjacent communities in Thailand
Dudsadee Muenhora,b,c,d, Hyo-Bang Moone, Sunggyu Leee, and Emma Gooseyf
a
Faculty of Environmental Management, Prince of Songkla University, Hat Yai, Songkhla, Thailand; bAir Pollution and Health Effect Research Center,
Prince of Songkla University, Hat Yai, Songkhla, Thailand; cHealth Impact Assessment Research Center, Prince of Songkla University, Hat Yai, Songkhla,
Thailand; dCenter of Excellence on Hazardous Substance Management (HSM), Bangkok, Thailand; eDepartment of Marine Science and Convergence
Engineering, Hanyang University, Ansan, Republic of Korea; fMTG Research Ltd, Wales, UK
Downloaded by [University of Florida] at 22:27 25 October 2017
ABSTRACT
This study was undertaken to investigate levels of organophosphorus ?ame retardants (PFRs) and phthalates
in ?oor and road dust from a manual e-waste dismantling facility and nearby communities in Thailand.
Concentrations of S10 PFRs and S6 phthalates in ?oor dust from the facility were approximately 36?1,700
and 86,000?790,000 ng g� whereas those from the communities were about 13?9,200 and 44,000?
2,700,000 ng g� respectively. The highest content of S10 PFRs (9,200 ng g� and S6 phthalates
(2,700,000 ng g� in indoor dust was both detected in the dust sampled from a house with no prevailing
winds located 350 m northeast of the facility. Levels of S10 PFRs and S6 phthalates in road dust from the
facility were around 1,100?2,100 and 40,000?670,000 ng g� while those from the residences were about
650?2,000 and 27,000?650,000 ng g� respectively. Concentrations of S10 PFRs (2,100 ng g� and S6
phthalates (670,000 ng g� in road dust were greatest in the dust collected from the facility. For the
distributional pattern, TBEP (tris (2-butoxyethyl) phosphate) was the main PFR in residential dust, whereas
TPP (triphenyl phosphate) was the major PFR in facility dust. TBEP was also found to be the most prominent
PFR in all road dust samples. Furthermore, DEHP (di-2-ethylhexyl phthalate) was the most abundant
phthalate congener in both ?oor and road dust samples. Under realistic high-end scenarios of environmental
exposure to DEHP, Thai toddlers (25.29 mg kg�bw day� in the adjacent communities were exposed above
the US EPA?s (United States Environmental Protection Agency) reference dose (RfD) for this congener (20 mg
kg�bw day�. Our data reveal that the PFR and phthalate-containing products at the residences are a likely
substantial source of PFRs and phthalates to the surrounding indoor environment, and humans can be
exposed to PFRs and phthalates in their dwellings via the settled ?oor dust.
Introduction
Organophosphorus ?ame retardants (PFRs) and phthalates are
polymer additives present in a diverse array of household and
industrial goods. They have become ubiquitous pollutants
observed in both indoor and outdoor environments especially
indoor dust around the world.[1,2] PFRs are considered to be
suitable alternatives to PBDE (polybrominated diphenyl ether)
formulations (deca-BDE, octa-BDE and penta-BDE) that have
been recently restricted or phased out. Therefore, the manufacture and application of these chemicals has been growing
remarkably during the recent decade.[3] PFRs have a large variety
of utilizations, with the predominant use of several as ?ame
retardants (FRs), plasticizers, stabilizers, lubricants, polyurethane
foams (PUFs) and ?oor polish.[1,4] For example, chlorinated
organophosphorus compounds tris (2-chloroethyl)-phosphate
(TCEP), tris (1-chloro-2-propyl)-phosphate (TCPP) and tris
(1,3-dichloro-2-propyl) phosphate (TDCPP) are penta-BDE
replacements utilized primarily as FRs in both ?exible and rigid
Received 31 March 2017
Accepted 16 August 2017
KEYWORDS
Organophosphorus ?ame
retardants (PFRs); phthalates;
?oor dust; road dust; ewaste; exposure
PUFs deployed in chairs, sofas, vehicle upholstery and relevant
products.[1,5?7] On the one hand, non-chlorinated organophosphates triphenyl phosphate (TPP) and tricresyl phosphate (TCP)
are extensively used as FRs in PVC (polyvinylchloride), tents,
electrical cables, synthetic leather and conveyor belts.[1,8,9] Moreover, tris (2-butoxyethyl) phosphate (TBEP) is typically utilized
as an additive in synthetic rubber, e.g. in soles of shoes, seals,
hoses and gaskets as well as a levelling agent in paints and paper
coating and ?oor waxes and polishes.[4,5,10]
Phthalates (otherwise known as phthalate diesters, phthalic
acid esters (PAEs) and dialkyl phthalate esters) are synthetic
diesters of phthalic acid that can be broadly categorized into
lighter molecular weight (dimethyl phthalate (DMP), diethyl
phthalate (DEP), and di-n-butyl phthalate (DBP)), and greater
molecular weight (benzyl butyl phthalate (BBP), di-n-octyl
phthalate (DOP), di-2-ethylhexyl phthalate (DEHP), diisononyl phthalate (DiNP) and diisodecyl phthalate (DiDP)).[11,12]
The lower molecular weight congeners (DMP, DEP and DBP)
CONTACT Dudsadee Muenhor
dudsadeem@hotmail.co.uk, mdudsadee@gmail.com, dudsadee.m@psu.ac.th
Songkla University, Hat Yai, Songkhla 90110, Thailand.
Color versions of one or more of the ?gures in the article can be found online at www.tandfonline.com/lesa.
� 2017 Taylor & Francis Group, LLC
ARTICLE HISTORY
Faculty of Environmental Management, Prince of
Downloaded by [University of Florida] at 22:27 25 October 2017
2
D. MUENHOR ET AL.
are utilized mostly in pharmaceuticals, cosmetics, adhesives,
solvents, inks, waxes and insecticides.[12] DBP is also applied to
the enteric coatings of some medications. Higher congeners
(DEHP, DiNP, DOP and DiDP) are utilized in clothing, building material and furnishings, but their greatest use is as plasticizers.[12?14]
PFRs and phthalates are not chemically bound to the
polymeric matrix; thus, they can relatively readily leach out,
evaporate, migrate or abrade from the treated products, and
then spread out into the surrounding air or adsorbed on airborne particulates and settled dust over time.[2,5] Levels of
PFRs and phthalates are substantially higher in indoor environments than in outdoor environments.[15,16] Human exposure to all these chemicals can occur via three primary
pathways including inhalation of air and airborne particles,
dietary ingestion and dermal contact.[16,17] Nonetheless,
ingestion of indoor dust has also been considered a predominant exposure pathway for humans particularly for infants
and toddlers.[18?20]
Limited data is available on the toxicity of PFRs. However, it
is known that TDCPP and TCEP are animal carcinogens, as
well as TBEP and TCPP are suspected carcinogens.[10,21] TCEP
also affects adversely foetal development.[22,23] Neurotoxic
effects have been documented for TCEP, TPP and TCP.[10,24,25]
TDCPP and TPP may be associated with reduced sperm quality, and TDCPP was signi?cantly inversely related to free thyroxin T4, one of the thyroid function indicator.[9]
Based on the toxicological and epidemiological research conducted to date, the health concerns of phthalates generally fall
into two major categories: cancer and reproductive effects.[26?28]
According to the International Agency for Research on Cancer
(IARC), these chemicals are not classi?able as to their carcinogenicity to humans (Group 3).[29] DEHP is a carcinogenic, endocrine and teratogenic toxicant in animals.[30,31] A study by Toft
et al.[32] shows the relationship between periconceptional urinary
level of MEHP (the principal urinary metabolite of DEHP) and
pregnancy loss. DBP, DEP, BBP and DEHP affect deleteriously
the mobility of human sperm.[33?36] DBP, BBP and DEHP may
also disturb the expression luteinizing hormone (LH) and therefore human testosterone levels.[34?37]
The application of PFRs and phthalates in Thailand is not
strictly regulated; hence, all these compounds may be found in
a wide range of consumer and commercial products as well as
wastes. Most importantly, Thai populations may be exposed to
PFRs and phthalates at houses, of?ces or workplaces via ingestion of contaminated ?oor dust. This study ?rstly reports concentrations of PFRs and phthalates in ?oor and road dust
samples collected from a manual e-waste dismantling facility
and adjacent communities in Thailand. PFRs (TEP, TBP,
TCEP, TCPP, TDCPP, TBEP, TPP, EHDPP, TEHP and TCP)
and phthalates (DMP, DEP, DBP, BBP, DEHP and DOP) were
determined in ?oor and road dust. The main objectives are (i)
to obtain comprehensive data on contamination of PFRs and
phthalates in the workplace (a manual e-waste dismantling
facility) and the residences (adjacent communities) in Thailand;
(ii) to compare levels of PFRs and phthalates in this study with
those published previously elsewhere in the world to elucidate
differences in contamination of indoor settled dust among
countries; and (iii) to estimate human exposure to all these
pollutants via ?oor dust ingestion within the workplace and
residences for both adults and children as appropriate.
Materials and methods
Site and samples description
This study was performed at a manual e-waste dismantling
facility and adjacent communities (a house 1, a house 2 and
a Buddhist temple) ranged over a distance of 350 m in
Phatthalung Province, Southern Thailand, between May 3
and 15, 2014. Floor and road dust samples were taken from
each studied microenvironment (Table 1; Fig. 1S), and were
later analyzed for PFRs and phthalates at Hanyang University, Republic of Korea, between November 1 and December
31, 2014.
Dust sampling
In total, 60 samples of ?oor (n D 40) and road dust (n D 20)
were collected from a manual e-waste dismantling facility and
adjacent communities in Phatthalung Province, Southern Thailand (Fig. 2S) on 3, 6, 9, 12 and 15 May 2014 using the previously described standardized protocol.[38,39] Brie?y, ?oor and
road dust samples were collected from a manual e-waste dismantling facility and adjacent communities (Table 1; Fig. 1S)
using Hitachi CV-BM16 RE 1600 W vacuum cleaners. The vacuum cleaners were modi?ed to sample dust into a 25 mm pore
size nylon sock and were cleaned between sample collections to
avoid cross-contamination. In each sampling area, four m2 of
bare ?oor/road surface or one m2 of carpeted ?oor were thoroughly and evenly vacuumed for exactly 4 or 2 min, respectively. After collection, dust samples were stored at � C. All
dust samples were passed through a pre-cleaned and hexane
rinsed 500 mm mesh sieve, homogenized thoroughly, weighed,
immediately transferred to hexane rinsed glass vials and
Table 1. Studied microenvironments for dust sampling.
No. of dust
samples
Microenvironments
1) A manual e-waste dismantling facility
2) Communities sampled ranged over a
distance of 350 m of the facility (Facility)
2.1) A house predominantly downwind of the
facility located 10 m west of the facility
(House 1)
2.1.1) Living room
2.1.2) Bedroom
2.2) A Buddhist temple predominantly
downwind of the facility located 300 m
east of the facility (Temple)
2.3) A house with no prevailing winds located
350 m northeast of the facility (House 2)
2.3.1) Living room
2.3.2) Bedroom
Total
Floor
dust
10
Road
dust Sampling dates
5
5
5
5
10
3, 6, 9, 12 and
15 May 2014
5
5
5
5
40
20
Note: The study area was situated in rural Southern Thailand. There were only
three dwellings (House 1 and 2 as well as a Buddhist temple) close to the facility
and road, and dust samples for this study were collected from all three
dwellings.
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
refrigerated at � C until analysis for PFRs and phthalates.
Moreover, ?oor dust sampling questionnaires were used to collect basic information about the studied microenvironments,
i.e., room ventilation.
3
with selected ion monitoring (SIM) mode for PFRs, while
the MS/MS was employed in multiple reactions monitoring
(MRM) mode for phthalates. Target ions and con?rmation
ions for the determination of selected PFRs and phthalates
are available as supporting information (Table 1S).
Downloaded by [University of Florida] at 22:27 25 October 2017
Target compounds
In this study, 10 PFRs and 6 phthalates were measured in ?oor
and road dust samples. We de?ned S10 PFRs and S6 phthalates as the sum of TEP (triethyl phosphate), TBP (tributyl
phosphate), TCEP (tris (2-chloroethyl)-phosphate), TCPP (tris
(1-chloro-2-propyl)-phosphate), TDCPP (tris (1,3-dichloro-2propyl) phosphate), TBEP (tris (2-butoxyethyl) phosphate),
TPP (triphenyl phosphate), EHDPP (2-ethylhexyl diphenyl
phosphate), TEHP (tris (2-ethylhexyl) phosphate) and TCP
(tricresyl phosphate); and DMP (dimethyl phthalate), DEP
(diethyl phthalate), DBP (di-n-butyl phthalate), BBP (benzyl
butyl phthalate), DEHP (di-2-ethylhexyl phthalate) and DOP
(di-n-octyl phthalate), respectively.
Analysis of PFRs and phthalates in dust samples
At the Department of Marine Science and Convergence Engineering, Hanyang University, Ansan, Republic of Korea, concentrations of PFRs and phthalates were quanti?ed in each
dust sample using methods published previously,[2,40,41] with
modi?cations. In summary, accurately weighed 50?100 mg aliquots of each sample were spiked with 100 ng of each surrogate
standard (TCEP-d12, TCPP-d18, TDCPP-d15, TPP-d15,
DMP-d4, DEP-d4, DBP-d4, DEHP-d4 and DOP-d4), and
extracted in a Soxhlet apparatus using 200 mL of 50% dichloromethane (DCM; Ultra residue analysis, J.T. Baker, Phillipsburg,
NJ, USA): hexane (Ultra residue analysis, J.T. Baker) (3:1, v:v)
for 16?18 h. Following extraction, the crude extracts were concentrated using a rotary evaporator and made up to 5 mL in
hexane. A 100 mL aliquot of concentrate was transferred to a
tube and re-dissolved in 400 mL of acetone for the instrumental
analysis of PFRs and phthalates. Identi?cation and measurement of ten PFRs and six phthalates was conducted by GC/
MSD and GC/MS/MS, respectively.
GC analysis
The identi?cation and quanti?cation of PFRs and phthalates
in dust samples were carried out using an Agilent 7890 gas
chromatograph coupled to a 5975 mass spectrometer (GC/
MSD; Agilent Technologies, Wilmington, DE, USA) and
7000C tandem mass spectrometer (GC/MS/MS; Agilent
Technologies), respectively. A capillary column (DB-5MS,
30 m length, 0.25 mm inner diameter, 0.25 mL ?lm thickness; J&W Scienti?c, Palo Alto, CA, USA) was used for the
separation of PFRs and phthalates. Inlet and ion source temperatures were maintained at 250 C and 300 C for PFRs,
and 240 C and 300 C for phthalates, respectively. Helium
was used as a carrier gas with a constant ?ow rate of
1.0 mL/min. The oven temperature was programmed from
50 C (held for 3 min) to 230 C at 20 C/min, and ?nally
increased to 300 C at 10 C/min (held for 5 min). The MSD
was operated in positive electron impact ionization (EIC)
Quality assurance and quality control
To prevent contamination during quanti?cation of phthalates, only cleaned glass was used for sample storage, extraction, cleanup and analysis.[42] For each batch of ten
samples, a procedural blank comprising 0.2 g of preextracted sodium sulphate (treated in the same way as the
samples)[41] and only the solvent used in the extraction[40]
was processed to assess contamination occurred during PFR
and phthalate analysis, respectively. These procedural blanks
contained <5% of the target compounds in dust samples
and the data presented here are thus not blank-corrected.
Average � standard deviation percent recoveries of surrogate standards in all samples are: 105 � 14, 103 � 18, 94
� 18, 102 � 10, 92 � 14, 110 � 14, 112 � 15, 107 � 18
and 110 � 11% for TCEP-d12, TCPP-d18, TDCPP-d15,
TPP-d15, DMP-d4, DEP-d4, DBP-d4, DEHP-d4 and DOPd4, respectively. Additionally, accuracy for the PFR detection method was evaluated by replicate (n D 7) analysis of
NIST SRM 2585 (organics in indoor dust). The results of
these analyses are available as supporting information
(Table 2S) and indicate both excellent reproducibility (relative standard deviations ranging between 4.5% and 12.5%),
and agreement with the indicative values. For the purposes
of calculating descriptive statistics, concentrations below the
limits of quantitation (LOQs; S/N D 10) were assumed to
equal half the LOQ. LOQs for all target compounds are
given in Tables 2 and 3.
Results and discussion
Concentrations of PFRs and phthalates in dust samples
Concentrations of S10 PFRs and S6 phthalates in ?oor dust
from an e-waste dismantling facility were around 36?1,700 and
86,000?790,000 ng g� while those from nearby communities
were approximately 13?9,200 and 44,000?2,700,000 ng g�
respectively (Tables 2 and 3). The prominent PFR and phthalate in all forty ?oor dust samples was TBEP and DEHP,
respectively.
The highest level of S10 PFRs (9,200 ng g� and S6
phthalates (2,700,000 ng g� were both observed in ?oor dust
sampled from house 2 (no prevailing winds) located 350 m
northeast of the facility, revealing that the treated consumer
and commercial items present at the home represent a potential source of PFRs and phthalates to the indoor environment.
The Kolmogorov?Smirnov (KS) statistical analysis indicated that the concentrations of S10 PFRs, S6 phthalates as
well as the ten individual PFRs and the six individual phthalates in settled indoor dust samples taken in the present study
deviate signi?cantly from a normal distribution. Thus, a
t-test was performed on log-transformed concentrations to
elucidate any differences in average concentrations of PFRs
4
D. MUENHOR ET AL.
Table 2. Mean concentrations (ng g� range in parentheses) of PFRs in ?oor and road dust samples from a manual e-waste dismantling facility, houses and a Buddhist
temple in Thailand.
Downloaded by [University of Florida] at 22:27 25 October 2017
Compound
Floor dust
TEP
TBP
TCEP
TCPP
TDCPP
TBEP
TPP
EHDPP
TEHP
TCP total
S10 PFRs
Road dust
TEP
TBP
TCEP
TCPP
TDCPP
TBEP
TPP
EHDPP
TEHP
TCP total
S10 PFRs
LOQ
Facility (n D 10)
House 1 Downwind
(n D 10)
Temple Downwind
(n D 10)
House 2 No winds
(n D 10)
All studied residences (House 1 C
Temple C House 2) (n D 30)
2.5
2.5
2.5
2.5
2.5
25
0.5
0.5
0.5
0.1
?
<2.5 (<2.5?<2.5)
<2.5 (<2.5?<2.5)
3.8 (<2.5?14)
30 (<2.5?100)
20 (6.8?55)
140 (<25?1,200)
150 (19?480)
1.5 (<0.5?2.4)
1.1 (<0.5?8.4)
26 (10?48)
380 (54?1,700)
<2.5 (<2.5?<2.5)
3.7 (<2.5?9.0)
2.5 (<2.5?5.8)
30 (<2.5?60)
12 (6.0?51)
240 (<25?720)
1.3 (<0.5?9.0)
0.58 (<0.5?1.3)
<0.5 (<0.5?<0.5)
7.7 (6.4?11)
300 (45?760)
<2.5 (<2.5?<2.5)
<2.5 (<2.5?<2.5)
1.8 (<2.5?3.1)
28 (<2.5?58)
5.9 (4.0?7.7)
2,200 (<25?4,500)
<0.5 (<0.5?<0.5)
1.1 (<0.5?3.0)
<0.5 (<0.5?<0.5)
6.4 (5.0?9.2)
2,300 (31?4,500)
2.1 (<2.5?5.5)
<2.5 (<2.5?<2.5)
1.6 (<2.5?3.3)
50 (8.1?76)
6.3 (5.2?7.8)
4,400 (1,500?9,100)
0.37 (<0.5?1.5)
0.81 (<0.5?1.5)
<0.5 (<0.5?<0.5)
5.1 (1.3?10)
4,500 (1,500?9,200)
1.5 (<2.5?5.5)
2.1 (<2.5?9.0)
2.0 (<2.5?5.8)
36 (<2.5?76)
8.0 (4.0?51)
2,300 (<25?9,100)
0.65 (<0.5?9.0)
0.83 (<0.5?3.0)
<0.5 (<0.5?<0.5)
6.4 (1.3?11)
2,400 (13?9,200)
2.5
2.5
2.5
2.5
2.5
25
0.5
0.5
0.5
0.1
?
<2.5 (<2.5?<2.5)
<2.5 (<2.5?<2.5)
5.6 (3.5?12)
48 (12?170)
12 (5.3?33)
1,300 (1,100?1,600)
110 (<0.5?300)
<0.5 (<0.5?<0.5)
<0.5 (<0.5?<0.5)
10 (1.6?42)
1,500 (1,100?2,100)
<2.5 (<2.5?<2.5)
<2.5 (<2.5?<2.5)
4.4 (3.1?5.0)
28 (11?43)
5.9 (5.4?6.4)
1,200 (920?1,300)
<0.5 (<0.5?<0.5)
<0.5 (<0.5?<0.5)
<0.5 (<0.5?<0.5)
2.8 (1.2?6.4)
1,200 (970?1,300)
<2.5 (<2.5?<2.5)
<2.5 (<2.5?<2.5)
3.9 (3.3?4.5)
2.6 (<2.5?6.6)
5.8 (5.4?6.1)
1,200 (900?2,000)
<0.5 (<0.5?<0.5)
0.76 (<0.5?2.8)
<0.5 (<0.5?<0.5)
0.58 (0.49?0.74)
1,200 (920?2,000)
<2.5 (<2.5?2.5)
<2.5 (<2.5?<2.5)
4.2 (3.2?5.0)
2.6 (<2.5?6.3)
5.7 (5.2?5.9)
870 (640?1,100)
<0.5 (<0.5?<0.5)
<0.5 (<0.5?<0.5)
<0.5 (<0.5?<0.5)
0.47 (0.44?0.51)
890 (650?1,100)
<2.5 (<2.5?2.5)
<2.5 (<2.5?<2.5)
4.1 (3.1?5.0)
11 (<2.5?43)
5.8 (5.2?6.4)
1,100 (640?2,000)
<0.5 (<0.5?<0.5)
0.42 (<0.5?2.8)
<0.5 (<0.5?<0.5)
1.3 (0.44?6.4)
1,100 (650?2,000)
Note: For the purposes of calculating descriptive statistics, values <LOQ assumed to equal half the LOQ.
and phthalates between the facility and domestic dust. The
results suggested that the levels of S10 PFRs in indoor dust
collected from house 2 (no prevailing winds) were signi?cantly greater than those taken from the facility and house 1
(predominantly downwind of the facility) located 10 m west
of the facility (P D <0.05), indicating that the newest wall
coverings and painted walls at home 2 could be the possible
indoor sources of PFRs.[4,5,10] However, levels of TPP and
TCP were signi?cantly higher in facility dust than in residential dust (House 1, Temple and House 2) (P D <0.05). A ttest also demonstrated that the DOP concentrations detected
in dust sampled from the facility, the temple (predominantly
downwind of the facility) located 300 m east of the facility
and house 2 (no prevailing winds) were signi?cantly lower
than those detected in the dust collected from house 1 (predominantly downwind of the facility) (P D <0.05). These
?ndings implied that some old blood storage bags unintentionally left in house 1 previously owned by a veterinarian
may possibly be the local emission sources of DOP to the surrounding environment.[14] In Thailand, the same type of a
blood storage bag is used for both humans and animals.
Levels of S10 PFRs and S6 phthalates in road dust from the
facility were approximately 1,100?2,100 and 40,000?670,000
ng g� whereas those from the adjacent residences were
about 650?2,000 and 27,000?650,000 ng g� respectively
(Tables 2 and 3). The main PFR and phthalate in both road
Table 3. Mean concentrations (ng g� range in parentheses) of phthalates in ?oor and road dust samples from a manual e-waste dismantling facility, houses and a Buddhist temple
in Thailand.
Compound
Floor dust
DMP
DEP
DBP
BBP
DEHP
DOP
Road dust
DMP
DEP
DBP
BBP
DEHP
DOP
S6 phthalates
LOQ
Facility
(n D 10)
House 1 Downwind
(n D 10)
Temple Downwind
(n D 10)
House 2 No winds
(n D 10)
5
5
5
2
50
10
1,200 (400?3,600)
1,600 (850?4,300)
2,300 (830?4,000)
2,400 (1,400?5,000)
620 (<5?770)
1,100 (540?2,100)
1,300 (730?3,600)
990 (840?1,300)
5,400 (<5?8,000)
14,000 (4,300?40,000)
6,900 (4,100?17,000)
4,900 (3,400?6,300)
430 (<2?1,100)
690 (410?940)
220 (10?620)
170 (100?280)
550,000 (79,000?780,000) 900,000 (460,000?1,900,000) 380,000 (39,000?590,000) 580,000 (200,000?2,700,000)
480 (180?890)
3,800 (1,100?15,000)
360 (110?770)
910 (220?2,200)
5
5
5
2
50
10
620 (270?830)
680 (640?800)
3,200 (2,700?4,100)
80 (20?270)
170,000 (36,000?670,000)
190 (50?540)
170,000 (40,000?670,000)
?
810 (670?890)
790 (630?1,000)
4,600 (3,200?6,600)
30 (20?50)
26,000 (22,000?32,000)
70 (50?130)
32,000 (27,000?40,000)
1,200 (550?3,200)
830 (720?940)
4,200 (2,700?6,300)
60 (30?170)
160,000 (31,000?640,000)
250 (90?520)
170,000 (36,000?650,000)
Note: For the purposes of calculating descriptive statistics, values <LOQ assumed to equal half the LOQ.
650 (470?910)
790 (710?960)
4,400 (2,900?6,200)
40 (30?90)
70,000 (42,000?110,000)
420 (270?770)
76,000 (50,000?120,000)
All studied residences (House 1 C
Temple C House 2) (n D 30)
2,100 (830?5,000)
1,100 (540?3,600)
8,400 (3,400?40,000)
360 (10?940)
620,000 (39,000?2,700,000)
1,700 (110?15,000)
880 (470?3,200)
800 (630?1,000)
4,400 (2,700?6,600)
40 (20?170)
85,000 (22,000?640,000)
250 (50?770)
91,000 (27,000?650,000)
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
5
Table 4. Summary of concentrations (ng g-1) of selected PFRs in indoor dust samples from this and selected other studies.
Location[reference]
Thailand, This study,
A manual e-waste dismantling facility, n D 10
Thailand, This study,
Three residences, n D 30
Malate, The Philippines,
Homes, n D 17 [43]
Payatas, The Philippines,
Homes, n D 20 [43]
Downloaded by [University of Florida] at 22:27 25 October 2017
Japan, Homes, Floor dust,
n D 148 [44]
Jeddah, Kingdom of Saudi
Arabia, House ?oor,
n D 15 [45]
Assiut, Egypt, Homes, n D 20[46]
New Zealand, Homes,
Living room ?oors, n D 34 [47]
The Netherlands, Around electronics, n D 8 [48]
Germany, Homes, n D 6 [49]
Stockholm, Sweden,
Homes, Settled dust, n D 10 [50]
Stockholm, Sweden,
Workplaces, Settled dust, n D 10 [50]
California, USA, House dust, 2011 samples, n D 16 [6]
USA, Homes, n D 30 [51]
Statistical parameter/
compound
TCEP
TCPP
TDCPP
Average
Median
Minimum
Maximum
Average
Median
Minimum
Maximum
GM
Minimum
Maximum
GM
Minimum
Maximum
Median
Minimum
Maximum
Mean
Median
Minimum
Maximum
Average
Median
Minimum
Maximum
Median
Median
Minimum
Maximum
Average
Minimum
Maximum
Mean
Median
Minimum
Maximum
Mean
Median
Minimum
Maximum
Median
Minimum
Maximum
GM
Minimum
Maximum
30
20
<2.5
100
36
38
<2.5
76
8,700
<MDLb
430,000
1,600
1,700
200
3,700
53
28
<LOQ
123
350
1,300
480
3,800
740
370
960
3,100
1,600
700
11,000
32,000
19,000
3,400
120,000
2,200
490
140,000
3,440
217
67,810
20
140
150
1.5
1.1
15
<25
160
1.7
<0.5
6.8
<25
19
<0.5 <0.5
55
1,200
480
2.4
8.4
8.0
2,300
0.65
0.83
<0.5
6.4
2,300
<0.5
0.68
<0.5
4.0
<25
<0.5
<0.5 <0.5
51
9,100
9.0
3.0
<0.5
110
110
130
8.5
8.0
4.1
2,100
770
970
73
45
30
13
7.7
<0.17
440
560
370
2,800
510,000
4,500
2,100
6,200
<MDLb
860,000 5,890,000 250,000
51,000
1,800
580
310
220
100
500
200
230
220
70
150
LOQ
65
55
LOQ
8,700
2,800
1,200
520
270
147
86
101
52
72
18
67
42
<LOQ
<LOQ
8
<LOQ
557
305
289
102
230
4,020
600
280
22,000
820
350
70
4,600
680
300
3,200
159,000 11,000 2,000
<80
730
380
<80
<60
180
110
2,800
1,300
12,000
8,500
1,600
10,000
4,000
1,200
n.d.
2,200
600
100
n.d.
27,000
30,000
4,200
200
30,000 250,000
8,800
100
17,000
87,000
5,300
n.d.
3,300
4,500
900
n.d.
91,000 960,000 32,000
300
2,100
11,000
560
<200
920
790
140
<200
44,000 170,000
1,500
340
2,730
621
13,110
-
3.8
3.3
<2.5
14
2.0
<2.5
<2.5
5.8
32
<0.44
1,200
6.4
<0.44
140
5,800
<MDLb
340,000
560
410
130
1,700
49
22
<LOQ
132
110
1,300
220
6,900
200
140
280
7,600
2,100
n.d.
33,000
36,000
6,700
1,300
260,000
2,700
330
110,000
348
20
6,920
TBEP
TPP
EHDPP TEHP
TCP total SPFRsa
26
25
10
48
6.4
6.3
1.3
11
13
<0.27
25
7.5
<0.27
140
120
110
<50
180
94
<40
240
680
180
10,000
-
380
250
54
1,700
2,400
2,300
13
9,200
550
21
4,300
253
55
880
580,000
34,000
6,000,000
5,200
3,800
1,000
14,000
310
189
38
962
27,000
7,400
167,000
3,000
800
6,000
37,000
21,000
4,000
120,000
370,000
140,000
14,000
1,600,000
-
a
Sum of PFRs TEP, TBP, TCEP, TCPP, TDCPP, TBEP, TPP, EHDPP, TEHP and TCP (this study only).
MDLD Method detection limit.
b
dust from the facility and residences was TBEP and DEHP,
respectively. Concentrations of S10 PFRs (2,100 ng g�
and S6 phthalates (670,000 ng g� were highest in road
dust taken at the facility.
Comparison with literature
The contents of SPFRs observed in indoor dust in this study
were lower than the contents reported in the Philippines, Japan,
Kingdom of Saudi Arabia, Egypt, New Zealand, the Netherlands, Germany, Sweden and the United States (Table 4).[6,43?51]
Nevertheless, the levels of residential TBEP reported here
exceeded those detected in houses in Kingdom of Saudi Arabia,
Egypt and Germany,[45,46,49] presumably due to the higher quantity of TBEP-treated materials including wall coverings as well
as levelling agents for paints and coatings in the studied Thai
residences. The low concentrations of SPFRs in dust samples in
this study could possibly be ascribed to the differences in application of PFR-containing products, a substantial air ventilation
and exchange between indoor and outdoor owing to the investigated facility consisting of open barns with no walls and open
windows/doors all year-round in the investigated residences
and the lower use in rural Thai homes and the Buddhist temple
of the PFR containing products compared to other dwellings
across the world.
Phthalate concentrations found in settled ?oor dust in the
present study were lower than the levels reported in Japan,
Kingdom of Saudi Arabia, Kuwait, Bulgary, Italy, Germany,
Denmark, Sweden and Canada (Table 5),[40,52?61] but were
greater than the contents reported in Vietnam.[62] Nonetheless,
the contents of DMP, DEP, BBP, DEHP and DOP presented
here were greater than those measured in Chinese houses.[42]
Furthermore, the DMP, DEHP and DOP concentrations
detected in this study were higher than those seen in American
6
D. MUENHOR ET AL.
Table 5. Summary of concentrations (ng g-1) of selected phthalates in indoor dust samples from this and selected other studies.
Statistical parameter/compound
DMP
DEP
DBP
BBP
DEHP
DOP
Thailand, This study, A manual
e-waste dismantling facility,
n D 10
Average
Median
Minimum
Maximum
Average
Median
Minimum
Maximum
Mean
Median
Minimum
Maximum
Median
Minimum
Maximum
Median
Minimum
Maximum
Median
Minimum
Maximum
Mean
Median
Minimum
Maximum
GM
Median
Minimum
Maximum
GM
Median
Minimum
Maximum
Mean
Mean
Median
Maximum
Mean
Median
Minimum
Maximum
GM
Median
Average
Median
Minimum
Maximum
Median
Minimum
Maximum
Median
Minimum
Maximum
1,200
770
400
3,600
2,100
1,800
830
5,000
91
20
n.d.
690
200
n.d.
8,200
<LOD
<LOD
4,600
<MDLb
<MDLb
61,000
1,400
600
170
5,200
10
30
<d.l.
100
260,000
280,000
210,000
320,000
15,000
11,000
1,500
160,000
700
300
<40
11,000
80
n.d.
3,300
120
<MDLb
22,000
620
680
<5
770
1,100
950
540
3,600
77
21
9
360
400
n.d.
46,000
<LOD
<LOD
59,000
280
<MDLb
2,900
4,200
1,400
290
23,400
1,500
1,800
100
16,000
350,000
340,000
290,000
420,000
31,000
45,000
6,100
630,000
3,400
1,400
400
100,000
3,100
1,700
31,000
0
0
2,400,000
2,000
700
12,000
2,000
<MDLb
190,000
5,400
5,700
<0
8,000
8,400
5,700
3,400
40,000
1,100
470
74
4,900
20,000
1,500
1,200,000
17,000
<LOD
1,700,000
19,000
<MDLb
2,100,000
80,200
33,300
5,200
375,000
51,000
45,000
8,300
160,000
7,990,000
9,990,000
6,600,000
9,400,000
800,000
56,000
47,000
140,000
30,000
21,000
2,000
270,000
8,100
15,000
230,000
150,000
0
5,400,000
13,000
45,000
95,000
17,000
<MDLb
1,400,000
430
330
<2
1,100
360
230
10
940
970
220
28
4,600
200
n.d.
12,000
2,000
<LOD
140,000
1,900
<MDLb
61,000
1,500
800
370
3,800
6,400
8,600
<d.l.
160,000
320,000
340,000
280,000
380,000
99,000
86,000
30,000
820,000
21,000
6,000
<1,000
350,000
4,200
3,700
320,000
140,000
0
46,000,000
21,000
36,000
390,000
42,000
570
940,000
550,000
590,000
79,000
780,000
620,000
490,000
39,000
2,700,000
24,000
19,000
2,100
77,000
230,000
9,900
8,400,000
1,100,000
210,000
7,100,000
760,000
98,000
12,000,000
1,140,000
1,020,000
71,500
2,401,000
1,700,000
2,300,000
380,000
7,800,000
960,000
1,000,000
790,000
1,200,000
300,000
780,000
700,000
1,800,000
2,000,000
890,000
99,000
10,000,000
220,000
210,000
1,300,000
770,000
0
40,000,000
300,000
37,000
9,700,000
460,000
36,000
3,800,000
480
420
180
890
1,700
740
110
15,000
310
190
18
1,500
200
n.d.
46,000
102,400
26,800
3,280
827,000
14,000
14,000
<d.l.
1,300,000
250,000
300,000
200,000
300,000
41,000
-
550,000
600,000
86,000
790,000
630,000
510,000
44,000
2,700,000
27,000
23,000
3,400
79,000
300,000
24,000
8,600,000
1,347,000
1,134,000
90,000
3,005,000
2,100,000
2,400,000
470,000
7,800,000
1,300,000
-
400
n.d
14,000
-
400,000
87,000
9,700,000
-
Thailand, This study,
Three residences, n D 30
Vietnam, Homes, n D 16 [62]
China, Homes, n D 75 [42]
Japan, Houses, Floor dust,
n D 128 [52]
Downloaded by [University of Florida] at 22:27 25 October 2017
Japan, Houses, Floor dust,
n D 148 [53]
Jeddah, Kingdom of Saudi
Arabia, Houses, Floor dust,
n D 15 [54]
Kuwait, Homes, n D 21 [40]
Bulgary, Homes, n D 177 [55]
Palermo, Italy,
Indoor environments,
Indoor settled dust, n D 13 [56]
Berlin, Germany, Apartments,
Household dust, nD30 [57]
Germany, Daycare centers,
House dust, n D 63 [58]
The island of Fyn, Denmark,
Bedrooms, Homes, n D 500 [59]
Sweden, Homes, n D 346 [60]
Albany, USA, Homes, n D 33
[42]
Canada, Homes, Household
vacuum dust (HD), n D 126 [61]
a
S Phthalatesa
Location[reference]
Sum of phthalates DMP, DEP, DBP, BBP, DEHP and DOP (this study only).
MDLD Method detection limit.
b
homes.[42] The low phthalate concentrations in ?oor dust samples in the current study may be due to sampling areas (rural
areas) and domestic characteristics such as bare cement (facility), ceramic tile (house 1 and house 2) and marble ?oor (temple). Floor dust from rural areas contains low levels of
phthalates, a trend noted by Tran et al. (2016).[62] Moreover,
PVC ?oor is infrequently used in Thai residences. The bare
cement, ceramic tile, marble and wooden ?oor are used primarily in Thai houses, particularly in rural areas, the low phthalate
contents in settled ?oor dust samples were observed in this
study.
Distributional pattern of PFRs in ?oor and road
dust samples
TBEP was the most abundant PFR in domestic ?oor dust,
whereas TPP was the main PFR in facility ?oor dust. Moreover,
TBEP was found to be the most dominant PFR in all road dust
samples.
Contents of TPP in ?oor dust sampled from a manual ewaste dismantling facility contributed to 67% of the S10
PFRs. Furthermore, TBEP in residential ?oor dust contributed to 64%, 98% and 98% of the S10 PFRs for house 1,
temple (both downwind) and house 2 (no prevailing winds),
Downloaded by [University of Florida] at 22:27 25 October 2017
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
7
Figure 1. Patterns of PFRs (median concentrations) in ?oor dust samples.
Figure 3. Patterns of phthalates (median concentrations) in ?oor dust samples.
respectively (Fig. 1). For road dust, TBEP in the samples
collected from the facility, house 1, temple and house 2
contributed to 98%, 96%, 99% and 98% of the S10 PFRs,
respectively (Fig. 2).
Our data on the distributional pattern of PFRs in dust samples demonstrate that TBEP containing products such as wall
coverings and painted walls at the studied residences are a likely
substantial source of PFRs in surrounding environments,[4,5,10]
but this requires more detailed studies to assess the signi?cant
sources and exposure pathways of PFRs.
of the S6 phthalates for temple; and 92% of the S6 phthalates
for house 2) (Fig. 4).
The distributional pattern results indicate that DEHPtreated goods such as blood storage bags at the monitored
dwellings may constitute an important source of phthalates to
indoor dust,[13] and justify more detailed investigations of
indoor phthalates with a focus on point sources and primary
routes of exposure.
Distributional pattern of phthalates in ?oor and road
dust samples
It has been reported that PFRs and phthalates pose a risk of
causing deleterious effects on human health. For example,
TBEP, TCPP and DEHP are carcinogenic toxicants[10,21,30,31] as
well as DEHP and DBP have been linked to the disruption of
LH and human testosterone.[34?37] Therefore, in order to estimate occupational exposure to PFRs and phthalates within a
manual e-waste dismantling facility, we have assumed 100%
absorption of intake. Assuming that indoor dust ingestion
occurs only during waking hours (average 16 h per day), we
have used average adult dust ingestion ?gures of 1.25 mg h�
and high dust ingestion ?gures for adults of 3.13 mg h�[63]
DEHP was the major phthalate congener in both ?oor and road
dust. Levels of DEHP in settled ?oor dust sampled from the
facility, house 1, temple and house 2 contributed to 99%, 98%,
98% and 98% of the S6 phthalates, respectively (Fig. 3). The
same pattern of distribution is also seen in all road dust samples, but the contribution from DEHP was lesser in all outdoor
samples compared to all indoor samples (90% of the S6 phthalates for the facility; 80% of the S6 phthalates for house 1; 87%
Figure 2. Patterns of PFRs (median concentrations) in road dust samples.
Human exposure to PFRs and phthalates via indoor
dust ingestion
Figure 4. Patterns of phthalates (median concentrations) in road dust samples.
95th %ile
2.17 � 10�2.17 � 10�1.64 � 10�1.39 � 10�8.26 � 10�0.12
5.95 � 10�3.67 � 10�8.17 � 10�7.58 � 10�0.19
5.52 � 10�1.3 � 10�1.30 � 10�1.77 � 10�0.13
1.52 � 10�0.13
Median
2.17 � 10�2.17 � 10�5.68 � 10�3.50 � 10�2.52 � 10�2.17 � 10�2.80 � 10�2.88 � 10�4.33 � 10�4.29 � 10�4.40 � 10�1.34 � 10�1.18 � 10�9.95 � 10�5.7 � 10�0.10
7.31 � 10�0.10
Compounds
TEP
TBP
TCEP
TCPP
TDCPP
TBEP
TPP
EHDPP
TEHP
TCP
S10 PFRs
DMP
DEP
DBP
BBP
DEHP
DOP
S6 phthalates
Average dust ingestion
5.42 � 10�5.42 � 10�1.42 � 10�8.77 � 10�6.31 � 10�5.43 � 10�7.02 � 10�7.21 � 10�1.09 � 10�1.07 � 10�0.11
3.36 � 10�2.96 � 10�2.49 � 10�1.43 � 10�0.25
1.83 � 10�0.26
Median
5.42 � 10�5.42 � 10�4.11 � 10�3.49 � 10�2.07 � 10�0.29
0.15
9.18 � 10�2.05 � 10�1.90 � 10�0.49
1.38 � 10�3.26 � 10�3.24 � 10�4.43 � 10�0.33
3.8 � 10�0.33
95th %ile
High-end dust ingestion
Occupational exposure: Adults
4.33 � 10�4.33 � 10�4.33 � 10�1.31 � 10�2.22 � 10�0.79
8.67 � 10�2.35 � 10�8.67 � 10�2.17 � 10�0.80
6.15 � 10�3.29 � 10�1.97 � 10�8.01 � 10�0.17
2.55 � 10�0.18
Median
1.25 � 10�2.49 � 10�1.23 � 10�2.25 � 10�3.24 � 10�2.10
6.80 � 10�7.36 � 10�8.67 � 10�3.44 � 10�2.11
1.45 � 10�7.54 � 10�6.53 � 10�3.13 � 10�0.53
1.71 � 10�0.538
95th %ile
Average dust ingestion
1.08 � 10�1.08 � 10�1.08 � 10�3.27 � 10�5.56 � 10�1.97
2.17 � 10�5.88 � 10�2.17 � 10�5.43 � 10�2.00
1.54 � 10�8.22 � 10�4.92 � 10�2.0 � 10�0.43
6.38 � 10�0.448
Median
3.13 � 10�6.23 � 10�3.08 � 10�5.63 � 10�8.09 � 10�5.24
1.70 � 10�1.84 � 10�2.17 � 10�8.60 � 10�5.28
3.63 � 10�1.89 � 10�0.02
7.84 � 10�1.31
4.28 � 10�1.33
95th %ile
High-end dust ingestion
Environmental exposure: Adults
5.21 � 10�5.21 � 10�5.21 � 10�0.16
2.67 � 10�9.48
1.04 � 10�2.83 � 10�1.04 � 10�2.61 � 10�9.62
7.39 � 10�3.95 � 10�0.02
9.63 � 10�2.05
3.07 � 10�2.12
Median
1.50 � 10�2.99 � 10�1.48 � 10�0.27
3.89 � 10�25.20
8.17 � 10�8.85 � 10�1.04 � 10�4.13 � 10�25.37
1.75 � 10�9.06 � 10�0.08
3.77 � 10�6.32
0.02
6.40
95th %ile
Average dust ingestion
2.08 � 10�2.08 � 10�2.08 � 10�0.63
0.11
37.91
4.17 � 10�1.13 � 10�4.17 � 10�0.10
38.47
0.03
0.02
0.09
3.85 � 10�8.21
0.01
8.46
Median
6.01 � 10�0.12
5.92 � 10�1.08
0.16
100.80
0.03
0.04
4.17 � 10�0.17
101.50
0.07
0.04
0.31
0.02
25.29
0.08
25.59
95th %ile
High-end dust ingestion
Environmental exposure: Toddlers
Table 6. Estimated exposures (ng kg�bw day�for PFRs; mg kg�bw day�for phthalates) of Thai populations within a manual e-waste dismantling facility and dwellings to PFRs and phthalates via indoor dust ingestion.
Downloaded by [University of Florida] at 22:27 25 October 2017
8
D. MUENHOR ET AL.
Downloaded by [University of Florida] at 22:27 25 October 2017
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
We have also used an average adult weight for the Thai population of 57.7 kg[64], and assumed that occupational exposure
occurs for 8 h daily. Based on these assumptions, we have calculated different exposure scenarios. These estimate exposure
at average and high-end dust ingestion rates and where exposure is assumed to be because of dust contaminated at either
the median or 95th percentile concentrations measured within
this study. Table 6 provides these exposure assessments of
adults to PFRs (TEP, TBP, TCEP, TCPP, TDCPP, TBEP, TPP,
EHDPP, TEHP, TCP and S10 PFRs) and phthalates (DMP,
DEP, DBP, BBP, DEHP, DOP and S6 phthalates) via indoor
dust ingestion.
These values are compared with currently available reference doses (RfDs) for PFRs and phthalates. For TBP, TCEP,
TCPP, TDCPP, TBEP, TPP and TCP, a preliminary RfD of
24,000, 22,000, 80,000, 15,000, 15,000, 70,000 and 13,000 ng
kg�bw day�has been proposed by Ali et al.[45,47] Moreover,
for DBP and DEHP, the US EPA?s Integrated Risk Information
System (IRIS) Toxicological Evaluation recommends an RfD of
daily oral exposure to DBP and DEHP of 100 and 20 mg kg�bw day�that is considered to be without an appreciable risk
of harmful effects.[65] By comparison, all exposure estimates for
PFRs and phthalates were much lower than the RfDs (Table 6).
In order to assess environmental exposure to PFRs (TEP,
TBP, TCEP, TCPP, TDCPP, TBEP, TPP, EHDPP, TEHP, TCP
and S10 PFRs) and phthalates (DMP, DEP, DBP, BBP, DEHP,
DOP and S6 phthalates), average adult and toddler dust ingestion ?gures of 20 and 50 mg day� and high dust ingestion ?gures for adults and toddlers of 50 and 200 mg day�have been
utilized.[63] In addition, an average adult and toddler weight for
the Thai population of 57.7 and 12 kg have been applied.[64,66]
Assuming that 100% of PFRs and phthalates are absorbed and
the contents of PFRs and phthalates in all indoor environments
are identical to those in residences,[67] a variety of dust ingestion exposure scenarios have been computed using median and
95th percentile levels in the residential dust samples determined in this study. Table 6 shows these exposure assessments
of both adults and toddlers to PFRs and phthalates via domestic
dust ingestion. When compared with RfDs for TBP, TCEP,
TCPP, TDCPP, TBEP, TPP and TCP derived by Ali et al.[45,47]
and for DBP and DEHP proposed by the US EPA,[65] all exposure estimates for Thai adults were much lower than the RfDs
(Table 6). In contrast, for Thai toddlers, the high-end dust
ingestion estimates at 95th percentile concentrations of DEHP
(25.29 mg kg�bw day� exceeded the US EPA?s RfD (20 mg
kg�bw day� (Table 6).
Conclusion
The present study is the ?rst to examine contamination by
PFRs and phthalates in a manual e-waste dismantling facility,
residences and a Buddhist temple in Thailand. Settled ?oor
dust levels were lower than observed in various countries
throughout the world, but in some instances were greater than
those detected in other studies. TBEP was the most abundant
PFR in residential dust, whereas DEHP was the most dominant
phthalate congener in both ?oor and road dust. The ?ndings
presented here demonstrate that PFR and phthalate-containing
products at dwellings may constitute a substantial source of
9
PFRs and phthalates to surrounding indoor environments, and
humans are exposed to PFRs and phthalates in their residences
via the settled ?oor dust. Of signi?cant concern is that the
high-end dust ingestion estimates at 95th percentile concentrations of DEHP for Thai toddlers residing in the communities
exceeded the US EPA?s RfD. This study also justi?es further
research of these chemicals in both the domestic and workplace
environment with a focus on potential point sources and critical exposure pathways.
Acknowledgments
The authors would like to thank Miss Phiyachat Nookongbut for sample
processing. The authors also gratefully acknowledge the cooperation from
the owners and people at the manual e-waste dismantling facility as well as
the study participants for permitting us enter into the Buddhist temple
and their dwellings.
Funding
Dr. Dudsadee Muenhor is grateful to the Korean Association of Southeast
Asian Studies (KASEAS) and the ASEAN University Network (AUN) for
the ASEAN-ROK academic exchange fellowship funding.
References
[1] van der Veen, I.; de Boer, J. Phosphorus Flame Retardants: Properties, Production, Environmental Occurrence, Toxicity and Analysis.
Chemosphere 2012, 88, 1119?1153.
[2] Kang, Y.; Man, Y. B.; Cheung, K. C.; Wong, M. H. Risk Assessment
of Human Exposure to Bioaccessible Phthalate Esters via Indoor
Dust Around the Pearl River Delta. Environ. Sci. Technol. 2012, 46,
8422?8430.
[3] Morris, P. J.; Medina-Cleghorn, D.; Heslin, A.; King, S. M.; Orr, J.;
Mulvihill, M. M.; Krauss, R. M.; Nomura, D. K. Organophosphorus
Flame Retardants Inhibit Speci?c Liver Carboxylesterases and Cause
Serum Hypertriglyceridemia. ACS Chem. Biol. 2014, 9, 1097?1103.
[4] Marklund, A.; Andersson, B.; Haglund, P. Organophosphorus Flame
Retardants and Plasticizers in Air From Various Indoor Environments. J. Environ. Monit. 2005, 7, 814?819.
[5] Marklund, A.; Andersson, B.; Haglund, P. Screening of Organophosphorus Compounds and Their Distribution in Various Indoor Environments. Chemosphere 2003, 53, 1137?1146.
[6] Dodson, R. E.; Perovich, L. J.; Covaci, A.; Van den Eede, N.; Ionas, A.
C.; Dirtu, A. C.; Brody, J. G.; Rudel, R. A. After the PBDE Phase-Out:
A Broad Suite of Flame Retardants in Repeat House Dust Samples
from California. Environ. Sci. Technol. 2012, 46, 13056?13066.
[7] Stapleton, H. M.; Klosterhaus, S.; Eagle, S.; Fuh, J.; Meekers, J. D.;
Blum, A.; Webster, T. F. Detection of Organophosphate Flame
Retardants in Furniture Foam and U.S. House Dust. Environ. Sci.
Technol. 2009, 43, 7490?7495.
[8] Tina Organics (P) Ltd. (TOPL), Plasticizers & Allied Chemicals.
Phosphate Esters. 2015. Available at www.pac-india.com/organophosphate-esters.html (accessed 27 May 2015).
[9] Meeker, J. D.; Stapleton, H. M. House Dust Concentrations of
Organophosphate Flame Retardants in Relation to Hormone Levels
and Semen Quality Parameters. Environ. Health Perspect. 2010, 118,
318?323.
[10] WHO/IPCS. Flame Retardants: Tris (2-butoxyethyl) Phosphate, Tris
(2-ethylhexyl) Phosphate, Tetrakis (hydroxymethyl) Phosphonium
Salts. Environmental Health Criteria 218; World Health Organization: Geneva, Switzerland, 2000.
[11] North, M. L.; Takaro, T. K.; Diamond, M. L.; Ellis, A. K. Effects of
Phthalates on the Development and Expression of Allergic Disease
and Asthma. Ann. Allergy, Asthma Immunol. 2014, 112, 496?502.
Downloaded by [University of Florida] at 22:27 25 October 2017
10
D. MUENHOR ET AL.
[12] Takaro, T. K.; Diamond, M.; Gobas, F.; Otton, V.; Shu, H. Critical
Review of Phthalates in Canadian Indoor Environments; Health Canada, Safe Environments Program: Ottawa, Ontario, 31 March 2010;
1?128. Available at http://research.rem.sfu.ca/papers/gobas/FinalRe
portFIN-1.pdf (accessed 29 May 2015).
[13] ATSDR. Toxicological Pro?le for di (2-ethylhexyl) Phthalate (DEHP);
Agency for Toxic Substances and Disease Registry: Atlanta, GA, The
United States, 2002. September. Available at http://www.atsdr.cdc.
gov/toxpro?les/tp9.pdf (accessed 2 July 2015).
[14] ATSDR. Toxicological Pro?le for di-n-octyl Phthalate (DnOP);
Agency for Toxic Substances and Disease Registry: Atlanta, GA, The
United States, 1997. September. Available at http://www.atsdr.cdc.
gov/toxpro?les/tp95.pdf (accessed 2 July 2017).
[15] Carlsson, H.; Nilsson, U.; Becker, G.; Ostman, C. Organophosphate
Ester Flame Retardants and Plasticizers in the Indoor Environment:
Analytical Methodology and Occurrence. Environ. Sci. Technol.
1997, 31, 2931?2936.
[16] Wensing, M.; Uhde, E.; Salthammer, T. Plastics Additives in the
Indoor Environment-Flame Retardants and Plasticizers. Sci. Total
Environ. 2005, 339, 19?40.
[17] Abb, M.; Heinrich, T.; Sorkau, E.; Lorenz, W. Phthalates in house
dust. Environ. Int. 2009, 35, 965?970.
[18] Guo, Y.; Wu, Q.; Kannan, K. Phthalate Metabolites in Urine from
China, and Implications for Human Exposures. Environ. Int. 2011,
37, 893?898.
[19] Mercier, F.; Glorennec, P.; Thomas, O.; Le Bot, B. Organic Contamination of Settled House Dust, A Review for Exposure Assessment
Purposes. Environ. Sci. Technol. 2011, 45, 6716?6727.
[20] Lioy, P. J.; Freeman, N. C.; Millette, J. Dust.: A Metric for use in Residential and Building Exposure Assessment and Source Characterization. Environ. Health Perspect. 2002, 110, 969?983.
[21] World Health Organization/ International Programme on Chemical
Safety (WHO/IPCS). Flame Retardants: Tris (chloropropyl) Phosphate and Tris (2- chloroethyl) Phosphate. Environmental Health Criteria 209; World Health Organization: Geneva, Switzerland, 1998.
[22] Sato, T.; Watanabe, K.; Nagase, H.; Kito, H.; Niikawa, M.; Yoshioka,
Y. Investigation of the Hemolytic Effects of Various Organophosphoric Acid Triesters (OPEs) and Their Structure-Activity Relationship. Toxicological Environ. Chem. 1997, 59, 305?313.
[23] Chapin, R. E.; Sloane, R. A.; Haseman, J. K. The Relationships
Among Reproductive Endpoints in Swiss Mice, Using the Reproductive Assessment by Continuous Breeding Database. Fundam. Appl.
Toxicol. 1997, 38, 129?142.
[24] WHO/IPCS. Tri-n-butyl Phosphate. Environmental Health Criteria
112; World Health Organization: Geneva, Switzerland, 1991.
[25] WHO/IPCS. Tricresyl Phosphate. Environmental Health Criteria 110;
World Health Organization: Geneva, Switzerland, 1990.
[26] Meeker, J. D.; Calafat, A. M.; Hauser, R. Urinary Phthalate Metabolites and Their Biotransformation Products: Predictors and Temporal
Variability Among Men and Women. J. Expo. Sci. Environ. Epidemiol. 2012, 22, 376?385.
[27] Sathyanarayana, S. Phthalates and Children?s Health. Curr. Probl.
Pediatr. Adolesc. Health Care 2008, 38, 34?49.
[28] Swan, S. H.; Main, K. M.; Liu, F.; Stewart, S. L.; Kruse, R. L.; Calafat, A. M.;
Mao, C. S.; Redmon, J. B.; Ternand, C. L.; Sullivan, S.; Tague, J. L.
Decrease in Anogenital Distance Among Male Infants with Prenatal
Phthalate Exposure. Environ. Health Perspect. 2005, 113, 1056?1061.
[29] Grosse, Y.; Baan, R.; Secretan-Lauby, B.; El Ghissassi, F.; Bouvard, V.;
Benbrahim-Tallaa, L.; Guha, N.; Islami, F.; Galichet, L.; Straif, K. Carcinogenicity of Chemicals in Industrial and Consumer Products,
Food Contaminants and Flavourings, and Water Chlorination
Byproducts. Lancet Oncol. 2011, 12, 328?329.
[30] Morgenroth, V. III. Scienti?c Evaluation of the Data-Derived Safety
Factors for the Acceptable Daily Intake. Case Study: Diethylhexylphthalate. Food Addit. Contam. 1993, 10, 363?373.
[31] WHO/IPCS. Diethylhexyl Phthalate. Environmental Health Criteria
131; World Health Organization: Geneva, Switzerland, 1992.
[32] Toft, G.; Jonsson, B. A. G.; Lindh, C. H.; Jensen, T. K.; Hjollund, N.
H.; Vested, A.; Bonde, J. P. Association Between Pregnancy Loss and
[33]
[34]
[35]
[36]
[37]
[38]
[39]
[40]
[41]
[42]
[43]
[44]
[45]
[46]
[47]
[48]
[49]
Urinary Phthalate Levels Around the Time of Conception. Environ.
Health Perspect. 2012, 120, 458?463.
Liu, L.; Bao, H.; Liu, F.; Zhang, J.; Shen, H. Phthalates Exposure of
Chinese Reproductive Age Couples and Its Effect on Male Semen
Quality: A Primary Study. Environ. Int. 2012, 42, 78?83.
Main, K. M.; Mortensen, G. K.; Kaleva, M. M.; Boisen, K. A.; Damgaard, I. N.; Chellakooty, M.; Schmidt, I. M.; Suomi, A.; Virtanen, H.
E.; Petersen, J. H.; Andersson, A.; Toppari, J.; Skakkebaek, N. E.
Human Breast Milk Contamination with Phthalates and Alteration
of Endogenous Reproductive Hormones in Infants Three Months of
Age. Environ. Health Perspect. 2006, 114, 270?276.
Duty, S. M.; Silva, M. J.; Barr, D. B.; Brock, J. W.; Ryan, L.; Chen, Z.;
Herrick, R. F.; Christiani, D. C.; Hauser, R. Phthalate Exposure and
Human Semen Parameters. Epidemiology 2003, 14, 269?277.
Becker, K.; Seiwert, M.; Angerer, J.; Heger, W.; Koch, H. M.;
Nagorka, R.; Rosskamp, E.; Schluter, C.; Seifert, B.; Ullrich, D. DEHP
Metabolites in Urine of Children and DEHP in House Dust. Int. J.
Hygiene Environ. Health 2004, 207, 409?417.
Mendiola, J.; Jorgensen, N.; Andersson, A.-M.; Calafat, A. M.; Silva,
M. J.; Redmon, J. B.; Sparks, A.; Drobnis, E. Z.; Wang, C.; Liu, F.;
Swan, S. H. Associations Between Urinary Metabolites of di (2-ethylhexyl) Phthalate and Reproductive Hormones in Fertile Men. Int. J.
Androl. 2011, 34, 369?378.
Muenhor, D.; Harrad, S. Within-Room and Within-Building Temporal and Spatial Variations in Concentrations of Polybrominated
Diphenyl Ethers (PBDEs) in Indoor Dust. Environ. Int. 2012, 47,
23?27.
Muenhor, D.; Harrad, S.; Ali, N.; Covaci, A. Brominated Flame
Retardants (BFRs) in Air and Dust from Electronic Waste Storage
Facilities in Thailand. Environ. Int. 2010, 36, 690?698.
Gevao, B.; Al-Ghadban, A. N.; Bahloul, M.; Uddin, S.; Zafar, J. Phthalates in Indoor Dust in Kuwait: Implications for Non-Dietary
Human Exposure. Indoor Air 2013, 23, 126?133.
Van den Eede, N.; Dirtu, A. C.; Ali, N.; Neels, H.; Covaci, A.
Multi-Residue Method for the Determination of Brominated and
Organophosphate Flame Retardants in Indoor Dust. Talanta.
2012, 89, 292?300.
Guo, Y.; Kannan, K. Comparative Assessment of Human Exposure
to Phthalate Esters from House Dust in China and the United States.
Environ. Sci. Technol. 2011, 45, 3788?3794.
Kim, J.-W.; Isobe, T.; Sudaryanto, A.; Malarvannan, G.; Chang, K.H.; Muto, M.; Prudente, M.; Tanabe, S. Organophosphorus Flame
Retardants in House Dust From the Philippines: Occurrence and
Assessment of Human Exposure. Environ. Sci. Pollut. Res. 2013, 20,
812?822.
Araki, A.; Saito, I.; Kanazawa, A.; Morimoto, K.; Nakayama, K.;
Shibata, E.; Tanaka, M.; Takigawa, T.; Yoshimura, T.; Chikara, H.;
Saijo, Y.; Kishi, R. Phosphorus Flame Retardants in Indoor Dust and
Their Relation to Asthma and Allergies of Inhabitants. Indoor Air
2014, 24, 3?15.
Ali, N.; Eqani, S. A. M. A. S.; Ismail, I. M. I.; Malarvannan, G.; Kadi,
M. W.; Albar, H. M. S.; Rehan, M.; Covaci, A. Brominated and
Organophosphate Flame Retardants in Indoor Dust of Jeddah, Kingdom of Saudi Arabia: Implications for Human Exposure. Sci. Total
Environ. 2016, 569?570, 269?277.
Abdallah, M. A.-E.; Covaci, A. Organophosphate Flame Retardants
in Indoor Dust from Egypt: Implications for Human Exposure. Environ. Sci. Technol. 2014, 48, 4782?4789.
Ali, N.; Dirtu, A. C.; Van den Eede, N.; Goosey, E.; Harrad, S.; Neels,
H.; Mannetje, A.; Coakley, J.; Douwes, J.; Covaci, A. Occurrence of
Alternative Flame Retardants in Indoor Dust From New Zealand:
Indoor Sources and Human Exposure Assessment. Chemosphere
2012, 88, 1276?1282.
Brandsma, S. H.; de Boer, J.; van Velzen, M. J. M.; Leonards, P. E. G.
Organophosphorus Flame Retardants (PFRs) and Plasticizers in
House and Car Dust and the In?uence of Electronic Equipment.
Chemosphere 2014, 116, 3?9.
Brommer, S.; Harrad, S.; Van den Eede, N.; Covaci, A. Concentrations of Organophosphate Esters and Brominated Flame
JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH, PART A
[50]
[51]
[52]
[53]
Downloaded by [University of Florida] at 22:27 25 October 2017
[54]
[55]
[56]
[57]
[58]
Retardants in German Indoor Dust Samples. J. Environ. Monit.
2012, 14, 2482?2487.
Bergh, C.; Torgrip, R.; Emenius, G.; Ostman, C. Organophosphate
and Phthalate Esters in Air and Settled Dust ? A Multi-Location
Indoor Study. Indoor Air 2011, 21, 67?76.
Stapleton, H. M.; Misenheimer, J.; Hoffman, K.; Webster, T. F. Flame
Retardant Associations Between Children?s Handwipes and House
Dust. Chemosphere 2014, 116, 54?60.
Bamai, Y. A.; Araki, A.; Kawai, T.; Tsuboi, T.; Saito, I.; Yoshioka, E.;
Kanazawa, A.; Tajima, S.; Shi, C.; Tamakoshi, A.; Kishi, R. Associations of Phthalate Concentrations in Floor Dust and Multi-Surface
Dust with the Interior Materials in Japanese Dwellings. Sci. Total
Environ. 2014, 468?469, 147?157.
Bamai, Y. A.; Shibata, E.; Saito, I.; Araki, A.; Kanazawa, A.; Morimoto, K.; Nakayama, K.; Tanaka, M.; Takigawa, T.; Yoshimura, T.;
Chikara, H.; Saijo, Y.; Kishi, R. Exposure to House Dust Phthalates
in Relation to Asthma and Allergies in Both Children and Adults.
Sci. Total Environ. 2014, 485?486, 153?163.
Albar, H. M. S. A.; Ali, N.; Shahzad, K.; Ismail, I. M. I.; Rashid, M. I.;
Wang, W.; Ali, L. N.; Eqani, S. A. M. A. S. Phthalate Esters in Settled
Dust of Different Indoor Microenvironments; Source of Non-Dietary
Human Exposure. Microchem. J. 2017, 132, 227?232.
Kolarik, B., Bornehag, C.-G.; Naydenov, K.; Sundell, J.; Stavova,
P.; Nielsen, O. F. The Concentrations of Phthalates in Settled
Dust in Bulgarian Homes in Relation to Building Characteristic
and Cleaning Habits in the Family. Atmos. Environ. 2008, 42,
8553?8559.
Orecchio, S.; Indelicato, R.; Barreca, S. The Distribution of Phthalate
Esters in Indoor Dust of Palermo (Italy). Environ. Geochem. Health
2013, 35, 613?624.
Fromme, H.; Lahrz, T.; Piloty, M.; Gebhart, H.; Oddoy, A.; Ruden, H.
Occurrence of Phthalates and Musk Fragrances in Indoor Air and
Dust From Apartments and Kindergartens in Berlin (Germany).
Indoor Air 2004, 14, 188?195.
Fromme, H.; Lahrz, T.; Kraft, M.; Fembacher, L.; Dietrich, S.; Sievering, S.; Burghardt, R.; Schuster, R.; Bolte, G.; V?
olkel, W. Phthalates in
German Daycare Centers: Occurrence in Air and Dust and the
[59]
[60]
[61]
[62]
[63]
[64]
[65]
[66]
[67]
11
Excretion of Their Metabolites by Children (LUPE 3). Environ. Int.
2013, 61, 64?72.
Langer, S.; Weschler, C. J.; Fischer, A.; Bek?
o, G.; Toftum, J.; Clausen, G.
Phthalate and PAH Concentrations in Dust Collected from Danish
Homes and Daycare Centers. Atmos. Environ. 2010, 44, 2294?2301.
Bornehag, C.-G.; Sundell, J.; Weschler, C. J.; Sigsgaard, T.; Lundgren,
B.; Hasselgren, M.; Hagerhed-Engman, L. The Association Between
Asthma and Allergic Symptoms in Children and Phthalates in House
Dust: A Nested Case-Control Study. Environ. Health Perspect. 2004,
112, 1393?1397.
Kubwabo, C.; Rasmussen, P. E.; Fan, X.; Kosarac, I.; Wu, F.; Zidek,
A.; Kuchta, S. L. Analysis of Selected Phthalates in Canadian Indoor
Dust Collected Using Household Vacuum and Standardized Sampling Techniques. Indoor Air 2013, 23, 506?514.
Tran, T. M.; Minh, T. B.; Kumosani, T. A.; Kannan, K. Occurrence of
Phthalate Diesters (phthalates), p-hydroxybenzoic acid esters (parabens), Bisphenol A Diglycidyl Ether (BADGE) and Their Derivatives
in Indoor Dust from Vietnam: Implications for Exposure. Chemosphere 2016, 144, 1553?1559.
Jones-Otazo, H.; Clarke, J. P.; Diamond, M. L.; Archbold, J. A.;
Ferguson, G.; Harner, T.; Richardson, G. M.; Ryan, J. J.; Wilford, B.
Is House Dust the Missing Exposure Pathway for PBDEs? An Analysis of the Urban Fate and Human Exposure to PBDEs. Environ. Sci.
Technol. 2005, 39, 5121?5130.
Walpole, S. C.; Prieto-Merino, D.; Edwards, P.; Cleland, J.; Stevens,
G.; Roberts, I. The Weight of Nations: An Estimation of Adult
Human Biomass. BMC Public Health 2012, 12(439), 1?6.
US EPA. Integrated Risk Information System (IRIS); United States
Environmental Protection Agency: Washington, DC, 2011.
Dirtu, A. C.; Ali, N.; Van den Eede, N.; Neels, H.; Covaci, A. Country
Speci?c Comparison for Pro?le of Chlorinated, Brominated and
Phosphate Organic Contaminants in Indoor Dust. Case study for
Eastern Romania, 2010. Environ. Int. 2012, 49, 1?8.
Harrad, S.; Ibarra, C.; Abdallah, M. A.-E.; Boon, R.; Neels, H.; Covaci, A.
Concentrations of Brominated Flame Retardants in Dust From United
Kingdom Cars, Homes, and Of?ces: Causes of Variability and Implications for Human Exposure. Environ. Int. 2008, 34, 1170?1175.
Supplementary Materials
Figure 1S. Studied microenvironments for dust sampling (the prevailing winds run from east to west and west to east, equally, making both the Buddhist temple and
house 1 downwind of the facility).
Downloaded by [University of Florida] at 22:27 25 October 2017
12
D. MUENHOR ET AL.
Figure 2S. Map of ?oor and road dust sampling locations in Thailand.
Table 1S. Target ions and con?rmation ions for the determination of selected PFRs
and phthalates.
Analyte
PFRs
TEP
TBP
TCEP
TCPP
TDCPP
TBEP
TPP
EHDPP
TEHP
TCP
Phthalates
DMP
DEP
DBP
BBP
DEHP
DOP
Quanti?cation ion/MRM (m/z)
Con?rmation ion/MRM (m/z)
99
99
249
99
75
57
326
251
99
368
155
155
251
125
99
85
325
250
113
367
194 > 77
177 > 149
223 > 149
206 > 149
279 > 149
279 > 149
163 > 77
149 > 65
149 > 65
206 > 65
279 > 65
149 > 65
Table 2S. Concentrations (mg g�dw) of PFRs in house dust reference materials.
PFRs were measured at Hanyang University in SRM 2585 (n D 7).
PFRs
Indicative value
TCEP
TCPP
TDCPP
TPP
Average � SD
0.7 � 0.17
0.82 � 0.1
2.02 � 0.26
0.99 � 0.07
Experimental value
Average � SD
1.01 � 0.06
0.8 � 0.1
3.3 � 0.17
1.12 � 0.05
%RSD
5.94
12.5
5.15
4.46
Документ
Категория
Без категории
Просмотров
3
Размер файла
1 111 Кб
Теги
2017, 10934529, 1369813
1/--страниц
Пожаловаться на содержимое документа