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Article history:
Received 3 February 2016
Received in revised form 21 April 2016
Accepted 27 April 2016
Available online xxxx
Editor: D. Barcelo
Keywords:
Phthalates
Indoor dust
a b s t r a c t
Phthalates are widely used chemicals in household products, which severely affect human health. However,
there were limited studies emphasized on young adults' exposure to phthalates in dormitories. In this study,
seven phthalates were extracted from indoor dust that collected in university dormitories in Harbin, Shenyang,
and Baoding, in the north of China. Dust samples were also collected in houses in Harbin for comparison. The
total concentrations of phthalates in dormitory dust in Harbin and Shenyang samples were signicantly higher
than those in Baoding samples. The total geometric mean concentration of phthalates in dormitory dust in Harbin
was lower than in house dust. Di-(2-ethylhexyl) phthalate (DEHP) was the most abundant phthalate in both dormitory and house dust. The daily intakes of the total phthalates, carcinogenic risk (CR) of DEHP, hazard index (HI)
of di-isobutyl phthalate (DiBP), dibutyl phthalate (DBP), and DEHP were estimated, the median values for all students in dormitories were lower than adults who live in the houses. Monte Carlo simulation was applied to
Corresponding author.
Correspondence to: Y.F. Li, International Joint Research Center for Persistent Toxic Substances (IJRC-PTS), State Key Laboratory of Urban Water Resource and Environment, School of
Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090, China.
E-mail address: ijrc_pts_paper@yahoo.com (Y.-F. Li).
http://dx.doi.org/10.1016/j.scitotenv.2016.04.187
0048-9697/ 2016 Elsevier B.V. All rights reserved.
497
predict the human exposure risk of phthalates. HI of DiBP, DBP, and DEHP was predicted according to the reference doses (RfD) provided by the United States Environmental Protection Agency (U.S.EPA) and the reference
doses for anti-androgenicity (RfD AA) developed by Kortenkamp and Faust. The results indicated that the risks
of some students had exceeded the limitation, however, the measured results were not exceeded the limitation.
Risk quotients (RQ) of DEHP were predicted based on China specic No Signicant Risk Level (NSRL) and Maximum Allowable Dose Level (MADL). The predicted results of CR and RQ of DEHP suggested that DEHP could
pose a health risk through intake of indoor dust.
2016 Elsevier B.V. All rights reserved.
1. Introduction
Phthalate esters are a group of chemicals, which are widely used as
plasticizers in various household products. Properties and usages of
phthalates are different, due to their molecular weight. Phthalates
with high molecular weight phthalates, including di-(2-ethylhexyl)
phthalate (DEHP), di-isodecyl phthalate (DiDP), di-isononyl phthalate
(DiNP), and di-n-octyl phthalate (DOP) are generally used as plasticizers in building materials, furniture, and plastic toys (Schettler,
2006). Phthalates with low molecular weight, such as dimethyl phthalate (DMP), diethyl phthalate (DEP), and dibutyl phthalate (DBP) are
widely used in personal care products, lacquers, coatings, and varnishes
(Guo and Kannan, 2013; Schettler, 2006).
Phthalates severely risk on human health. Previous studies found
that the increased exposure to phthalates in humans was associated
with reproductive system variations, such as DNA damage in human
sperm, human semen parameters, and altered reproductive hormones
levels (Duty et al., 2003a, b, 2005). DEHP has been identied as a possible carcinogen to humans (group 2B) by the International Agency for
Research on Cancer (IARC) (IARC, 1982). DEHP is also announced as a
reasonably anticipated carcinogen to humans by the U.S. National Toxicology Program (NTP) (NTP, 1983).
Widespread usages of phthalates lead to continuous human exposure in various environmental media, such as indoor dust, air, water,
and soil (Gaspar et al., 2014; Ma et al., 2014a, b; Ranjbari and
Hadjmohammadi, 2012; Tran and Kannan, 2015; Tran et al., 2016;
Wang et al., 2013; Zhang et al., 2013). Human exposure to phthalates
occurs via inhalation, ingestion, and dermal absorption (Guo et al.,
2012; Wormuth et al., 2006). Moreover, previous studies had found
phthalate metabolites in body uids, such as breast milk, serum, and
urine (Gao et al., 2016; Guo et al., 2011; Hogberg et al., 2008), and
phthalates can be metabolized to more toxic compounds in human
body (Preuss et al., 2005).
Human exposure to phthalates from indoor dust is an important
pathway of hazardous intake. To date, phthalates have been measured
in indoor dust in different microenvironments, including homes,
daycare centers, and workplaces (Bamai et al., 2014; Bergh et al.,
2011; Fromme et al., 2013; Fromme et al., 2004; Gaspar et al., 2014;
Guo and Kannan, 2011; Kang et al., 2012; Kolarik et al., 2008; Lan et
al., 2012; Langer et al., 2010; Ma et al., 2014b; Tran et al., 2016; Zhang
et al., 2013). However, there are few studies mention phthalates in university dormitories (Bi et al., 2015; He et al., 2016; Shen, 2009), which
considered the importance of indoor exposure for young adults, especially in developing countries. In China, there are approximately 15 million undergraduate students and 1.8 million graduate students residing
in dormitories (NBSC, 2014). Dormitories in China are furnished simpler
than homes, and less numbers of electric appliances (computers). And
students have limited private space in dormitories. All students have
to live in the dormitories for four or more years. The specic indoor environment of university dormitories may result to varying exposures to
phthalates, and lead to signicant risks on students' health status. And
the effects may last for years, which may affect the health of their next
generation.
In this study, 34 indoor dust samples were collected in dormitories
in Harbin, Baoding, and Shenyang, the north of China. For comparison,
35 house dust samples were also collected in Harbin. The objectives of
498
499
second step, phthalates with high exposure levels and high toxicities
were selected. Further exposure risk assessment was carried out, including carcinogenic risk assessment of DEHP, cumulative risk assessment of DiBP, DBP, and DEHP, and risk assessment of DEHP according
to China specic NSRL and MADL. Individual estimation of exposure
risk cannot demonstrate the overall trend, hence the predicted probability density functions were applied by using Monte Carlo simulation.
Moreover, sensitivities and uncertainties of exposure risk assessment
were concerned. The human health risk assessment was based on the
data of university dormitories and houses in Harbin.
3.3.1. Estimation of human exposure
To estimate students' daily intakes of phthalates from dormitory
dust, the EDIs of phthalates via ingestion and dermal absorption were
calculated (Table 1). The EDIs of phthalates for male students (119 ng/
kgday) were lower than those for female students (160 ng/kgday),
which were both lower than predicted values (148 ng/kgday for
male students and 189 ng/kgday for female students, Fig. S3). The median EDIs of DEHP for male and female students from dormitory dust
were 69.8 ng/kgday and 93.7 ng/kgday, respectively. DBP and DiBP
were also major phthalates of daily intake. The median EDI values of
DBP and DiBP for male students were 11.7 ng/kgday and 5.53 ng/
kgday, respectively, and 15.8 ng/kgday and 7.42 ng/kgday for female
students, respectively. The comparisons between EDI values of DEHP
and DBP and RfD recommended by the U.S.EPA (USEPA, 1990, 1997)
and RfD AA developed by Kortenkamp and Faust (Kortenkamp and
Faust, 2010) were shown in Fig. 1. The EDIs of DEHP and DBP from dormitory dust were all below the recommended levels.
The EDIs of phthalates for adults in houses were higher than those
for students in dormitories (Table 1). Compared to predictions, the calculated EDI of the total phthalates for adults was lower than predicted
value (265 ng/kgday, Fig. S3). DEHP and DBP, were the major
phthalates contributing to EDIs with the median values of 167 ng/
kgday and 23.1 ng/kgday, respectively. Compared to the RfD and
RfD AA, the EDIs of DEHP and DBP for adults in houses were all below
the recommended levels (Kortenkamp and Faust, 2010; USEPA, 1990,
1997) (Fig. 1). Compared to adults in houses in other countries or
other cities in China (Fig. S4), the measured EDIs of DEHP in this study
were generally lower. For DiBP and DBP, the median EDI values were
higher than those reported elsewhere, except for the EDI values measured in Xi'an in China, which were approximately one order of magnitude higher. The median EDI value of DEP was lower than that reported
from other countries, but similar to other Chinese cities. Furthermore,
the median EDI value of DMP found in this study was higher than
those measured in other countries and other cities of China, while an
opposite trend was found for BBP and DOP.
Table 1
The total EDIs of phthalates via ingestion and dermal absorption for male and female students from dormitory dust and adults from house dust in Harbin (ng/kgday).
Male studentsa
Female studentsa
Adultsb
a
b
c
5th%c
25th%c
Median
75th%c
95th%c
5th%
25th%
Median
75th%
95th%
5th%
25th%
Median
75th%
95th%
DMP
DEP
DiBP
DBP
BBP
DEHP
DOP
Total
0.067
0.12
0.16
0.22
0.74
0.090
0.17
0.22
0.29
1.00
0.13
0.27
0.41
0.99
4.69
0.10
0.14
0.18
0.33
0.60
0.14
0.19
0.24
0.45
0.81
0.093
0.17
0.34
0.66
1.82
2.54
4.35
5.53
7.58
54.3
3.41
5.84
7.42
10.2
72.9
0.44
8.07
14.7
22.3
45.5
4.29
8.68
11.7
23.3
183
5.76
11.6
15.8
31.2
246
6.63
14.5
23.1
41.2
155
0.00057
0.031
0.066
0.15
0.46
0.00077
0.042
0.089
0.20
0.61
0.00089
0.046
0.12
0.20
0.48
15.2
35.0
69.8
129
2090
20.5
47.0
93.7
173
2800
59.7
90.1
167
380
1110
0.069
0.17
0.26
0.38
2.84
0.092
0.23
0.35
0.51
3.81
0.00056
0.00056
0.00056
0.49
1.64
32.5
44.4
119
218
2220
43.6
59.6
160
293
2990
78.7
154
221
458
1230
The total EDIs for male and female students were estimated only based on phthalates concentrations in dormitory dust from Harbin.
The total EDIs for adults were estimated based on phthalate concentrations in house dust from Harbin.
5th%, 25th%, 75th%, and 95th% represent the 5th, 25th, 75th, and 95th percentile values, respectively.
500
Fig. 1. The EDI values of DEHP and DBP from two types of indoor dust in Harbin (g/kgday). (The purple line represents 20 g/kgday; the orange line represents 30 g/kgday; and the
pink line represents 100 g/kgday.) (For interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)
The EDIs of phthalates from dust in this study were compared with
those from foodstuffs, including beverages, cereals, soy, meat, seafood,
milk, cooking oil, eggs, and condiments, which were collected in Harbin
and Shanghai of China. (Guo et al., 2012). In this study, DEHP and DBP
were the most abundant phthalates in dust. The median EDIs for three
population groups (Table 1) accounted for 1127% and 510% of those
for adults from foodstuffs (620 ng/kgday for DEHP and 243 ng/kgday
for DBP), respectively. The EDIs of other phthalates (Table 1)
were approximately 24 orders of magnitude lower than those from
foodstuffs for adults (16.5 ng/kgday for DMP, 13.6 ng/kgday for DEP,
245 ng/kgday for DiBP, and 10.0 ng/kgday for BBP), respectively.
Hence, exposure to phthalates for adults from dust also could be an important route, which should be considered.
3.3.2. Carcinogenic risk assessment of DEHP
Carcinogenic risk assessment of DEHP in both dormitory dust and
house dust in Harbin was conducted. The threshold of CR value is
1 105 that indicates potential adverse effects (De Miguel et al.,
2007; Wu et al., 2011). The CR values of DEHP from dormitory and
house dust are illustrated in Fig. 2. The median CR values of DEHP for
male and female students from dormitory dust were 5.53 107 and
7.48 107, respectively, which were one order of magnitude lower
than those for adults in houses (1.32 10 6). The predicted CR of
DEHP for three population groups showed higher values than calculated
CR (based on measured data). The median of predicted CR values were
7.59 107, 9.31 107, and 1.44 106 for male students, female
students, and adults, respectively (Fig. S5). Exceeding appeared in all
three groups, which could exceed approximately 1326 folds in the
worst cases. Therefore, the results suggest that people are in the risk
of exposure to DEHP.
3.3.3. Cumulative risk assessment of exposure to phthalates
Applications of cumulative risk assessment of exposure to
phthalates are based on an assumption that phthalates share a common
mechanism of action (Foster, 2006; Howdeshell et al., 2007, 2008). In
this study, cumulative risk was applied to estimate the exposure to
DiBP, DBP, and DEHP. A HI value lower than 1 is considered safe, the
value between 1 and 100 indicates a potential risk for adverse effect
might be observed, while the value of 100 or more indicates a high potential that adverse effects might be observed in humans at these exposures (Benson, 2009). Two types of reference doses were applied, one is
RfD recommended by the U.S.EPA (USEPA, 1990, 1997) and another one
Fig. 2. Carcinogenic risk (CR) values of DEHP from dormitory dust and house dust in
Harbin. (The purple line represents the 1 105 value.) (For interpretation of the
references to color in this gure legend, the reader is referred to the web version of this
article.)
501
Table 2
The hazard index (HI) values based on RfD and RfD AA for different population groups in Harbin.
Based on RfD
Based on RfD AA
a
b
c
d
Median
(5th%, 95th%)c
(HI N 1)%d
Median
(5th%, 95th%)
(HI N 1)%
Male studentsa
Female studentsa
Adultsb
0.0035
(0.00082, 0.10)
0
0.0027
(0.00060, 0.067)
0
0.0047
(0.0011, 0.13)
0
0.0036
(0.00081, 0.090)
0
0.0080
(0.0029, 0.053)
0
0.0055
(0.0020, 0.036)
0
HI values were estimated only based on phthalate concentrations in dormitory dust from Harbin.
HI values were estimated based on phthalate concentrations in house dust from Harbin.
5th% and 95th% represent the 5th and 95th percentile values, respectively.
The percentage of the numbers of values exceeding 1.
Shenyang were signicantly higher than those from Baoding. The total
concentration of phthalates in dormitory dust was slightly lower than
that in house dust. The EDI values of phthalates for both male and female students in dormitories were lower than those for adults in houses, and the EDI values of DEHP and DBP were below the reference doses
suggested by the USEPA, and Kortenkamp and Faust. The results of CR of
DEHP for students in dormitories and adults in houses in Harbin suggested that people are in a potential carcinogenic risk from DEHP exposure. The predicted HI values of DiBP, DBP, and DEHP for students based
on RfD exceed the threshold for adverse effects, however, it was not
shown in the calculated results (based on measured data). The predicted values of the total phthalate EDIs, CR of DEHP, HI of DiBP, DBP, and
DEHP were higher than the calculated values. The predicted results of
probability density functions of RQ of DEHP suggested that people are
at risk of DEHP based on China specic NSRL or MADL. DEHP concentration and DIR contributed most to the output of exposure risk assessment
through sensitivity analysis.
However, there were still some limitations in this study as different
sampling methods (brush, vacuum cleaner, etc) and particle size fraction were not concerned. Those may provide more information of
phthalate properties and new ndings. And inaccuracies were occurred
in comparing phthalate concentrations in this study with other studies.
Conict of interest statement
The authors declare that they have no competing nancial interests.
Acknowledgments
This work was supported by the Fundamental Research Funds for
the Central Universities (Grant No. HIT.NSRIF.2012084), the National
Natural Science Foundation of China (No. 21277038), and the Open Project of State Key Laboratory of Urban Water Resource and Environment
(Harbin Institute of Technology) (No. HCK201533).
Appendix A. Supplementary data
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.scitotenv.2016.04.187.
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