Science of the Total Environment 788 (2021) 147831

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Science of the Total Environment

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Profiles of phthalic acid esters (PAEs) in bottled water, tap water, lake
water, and wastewater samples collected from Hanoi, Vietnam
Thuy Minh Le a,b, Ha My Nu Nguyen a,c, Vy Khanh Nguyen d, Anh Viet Nguyen a, Nam Duc Vu b,
Nguyen Thi Hong Yen e, Anh Quoc Hoang a,f, Tu Binh Minh a, Kurunthachalam Kannan g, Tri Manh Tran a,⁎
a
Faculty of Chemistry, University of Science, Vietnam National University, 19 Le Thanh Tong, Hanoi 10000, Viet Nam
b
Center for Research and Technology Transfer, Vietnam Academy of Science and Technology, 18 Hoang Quoc Viet, Hanoi 10000, Vietnam
c
Ha Tinh University, Cam Vinh Commune, Cam Xuyen District, Ha Tinh 45000, Viet Nam
d
Chemistry Department, The College of Wooster, 1189 Beall Avenue, Wooster, OH 44691, USA
e
National Institute of Hygiene and Epidemiology, 1 Yersin streat, Ha Ba Trung, Hanoi 10000, Viet Nam
f
Center of Advanced Technology for the Environment (CATE), Graduate School of Agriculture, Ehime University, 3-5-7 Tarumi, Matsuyama 790-8566, Japan
g
Department of Pediatrics and Department of Environmental Medicine, New York University School of Medicine, New York, NY 10016, USA

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

• Elevated concentrations of PAEs were

measured in wastewater samples from
Vietnam.
• DEHP was a major compound found in
tap water, lake water and wastewater
samples.
• DiBP and DBP were the dominant PAEs
in bottled water.
• PAE concentrations in drinking water
and associated exposure doses were
below the reference values.

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

Article history: Contamination levels and distribution patterns of ten typical phthalic acid esters (PAEs) were investigated in var-
Received 26 March 2021 ious types of water samples collected from Hanoi metropolitan area in Vietnam. Concentrations of 10 PAEs in bot-
Received in revised form 10 May 2021 tled water, tap water, lake water, and wastewater samples were measured in the ranges of 1640–15,700 ng/L
Accepted 12 May 2021
(mean/median: 6400/5820 ng/L), 2100–18,000 ng/L (mean/median: 11,200/9270 ng/L), 19,600–127,000 ng/L
Available online 19 May 2021
(mean/median: 51,800/49,300 ng/L), and 20,700–405,000 ng/L (mean/median: 121,000/115,000 ng/L), respec-
Editor: Jay Gan tively. Among PAEs, di-(2-ethylhexyl) phthalate (DEHP) accounted for a major proportion of total concentrations
(45%) in wastewater, followed by diisobutyl phthalate (DiBP, 10.3%), and dibutyl phthalate (DBP, 9.53%). Concen-
trations of PAEs in wastewater decreased significantly with distance from the wastewater treatment plants
Keywords: (WWTPs). Concentrations of PAEs in surface water samples did not vary greatly between locations. PAEs were
PAEs found in bottled water in the following order: DBP (22.4%), DiBP (22.3%), benzylbutyl phthalate (BzBP, 20.1%),
Bottled water and DEHP (15.5%). The estimated mean exposure doses of 10 PAEs through consumption of drinking water for
Tap water adults and children in Vietnam were 254 and 256 ng/kg-bw/day, respectively.
Lake water
Capsule: Highest concentrations of PAEs were measured in wastewater, followed by lake water, tap water, and
Wastewater
bottled water.
Human exposure
© 2021 Elsevier B.V. All rights reserved.

⁎ Corresponding author.
E-mail address: manhtri0908@gmail.com (T.M. Tran).

https://doi.org/10.1016/j.scitotenv.2021.147831
0048-9697/© 2021 Elsevier B.V. All rights reserved.
T.M. Le, H.M.N. Nguyen, V.K. Nguyen et al.
1. Introduction
Phthalic acid esters (PAEs) have been widely used as plasticizers in
building materials, pharmaceuticals, household products, toys, electrical
devices, and personal care products (PCPs) (Navarro et al., 2010; Guo
and Kannan, 2013; Gao and Wen, 2016). PAEs accounted for 65% of
the global consumption of plasticizers in 2017 (IHS Market, 2018).
Diethylhexyl phthalate (DEHP) was still the most frequently used
plasticizer in 2016, with a global consumption at 3.1 million tons
(Caresana Research, 2017). PAEs were found in plastic products and
PCPs at concentrations of up to a few percent by volume (Guo and
Kannan, 2013; Guo et al., 2014). The sum concentrations of dimethyl
phthalate (DMP), diethyl phthalate (DEP), and dibutyl phthalate
(DBP) measured in polyethylene terephthalate (PET) bottles in Beijing
ranged from 102 to 710 μg/kg (Xu et al., 2020).
Owing to the widespread use, PAEs have been found in various envi-
ronmental matrices (e.g., air, dust, sediment, sewage sludge) and food-
stuffs (Schecter et al., 2013; Shi et al., 2016; Tran et al., 2017; Giuliani
et al., 2020). Total mean concentration of six selected PAEs in 225 drink-
ing water samples collected from seven geographical zones in China
was 1280 ng/L (Liu et al., 2015). Moreover, metabolites of PAEs were
also found frequently in human urine (Guo et al., 2011a, 2011b;
Dewalque et al., 2015; Chen et al., 2019; Santos et al., 2021), and
mother's milk (Lin et al., 2011). In Vietnam, several recent studies re-
ported the occurrence of notable levels of PAEs in air (Tran et al.,
2017; Anh et al., 2021) and dust (Tran et al., 2016). Quynh and Toan
(2019) reported the distribution of PAEs in wastewater samples col-
lected in a sewage canal in Hanoi. Very high concentrations (μg/L
level) of DEHP, benzylbutyl phthalate (BzBP), DEP, and DBP were de-
tected in surface waters from the Red River, Hanoi, Hue, Danang, and
Ho Chi Minh City (Chau et al., 2018). Nevertheless, no earlier studies
have reported the occurrence of PAEs in drinking water in Vietnam.
Toxicity of PAEs has been widely studied in laboratory animals (Gray
et al., 2006; Boberg et al., 2008; Clewell et al., 2013). Based on the ad-
verse effects in laboratory animals, the U.S. EPA recommended an oral
reference dose (RfD) for DBP and DEHP at 100 and 20 μg/kg/d (US
FDA, 2012). In addition, data are available on the toxicity of PAEs in
humans (Chen and Chien, 2014; Benjamin et al., 2017; Radke et al.,
2018, 2019, 2020; Bolling et al., 2020). Zhang et al. (2021) summarized
that exposure to PAEs can lead to activation of cytochrome P450
(CYP450) and endocrine systems, which could result in oxidative stress,
metabolic disorders, endocrine disorders, and immunosuppression.
Radke et al. (2019) reported association between PAE exposure and ad-
verse female reproductive and developmental outcomes. PAE exposure
in pregnant women was linked to fetal growth restriction and adverse
birth outcomes (Santos et al., 2021) as well as behavioral changes in
children (Lin et al., 2011; Jia et al., 2019; Yao et al., 2020).
Regulations have been imposed on permissible levels of PAEs in
commercial products (US EPA, 2008; US CPSC, 2011; US FDA, 2012;
Commission regulation (EU) 2018/2005, 2018). DBP, DiBP, BzBP, and
DEHP should not be used as substances or in mixture, individually or
in any combination, at concentrations equal to or higher than 0.1% by
weight of the plasticized material, toys and childcare articles
(Commission regulation (EU) 2018/2005, 2018). Several industrially
developed countries have enacted regulations on permissible limits of
PAEs in the environment (US EPA, 2015; Environment Climate
Change, Canada, 2017). The maximum contaminant level of DEHP in
drinking water was set at 6.0 μg/L by the US EPA (US EPA, 2009) and
8.0 μg/L by the World Health Organization (WHO, 2000) and National
Standard of the People's Republic of China (2006). In Vietnam, the Min-
istry of Health issued a provisional limit for DEHP in food at 1.5 mg/kg
for solid food or 1.5 mg/L for liquid food (Vietnam Ministry of Health,
2011). Despite this, little is known on environmental occurrence of
PAEs in drinking water in Vietnam.
This study aims to investigate the occurrence and distribution levels
of ten typical PAEs in bottled water, tap water, surface water, and
2
Science of the Total Environment 788 (2021) 147831
wastewater samples collected in Hanoi metropolitan area, the capital
of Vietnam. Human exposure to PAEs through the consumption of
drinking water was assessed. To our knowledge, this is the first survey
on PAEs in various types of water samples collected from Vietnam.
2. Material and methods
2.1. Chemicals
Ten PAEs including dimethyl phthalate (DMP), diethyl phthalate
(DEP), di-n-propyl phthalate (DPP), di-n-butyl phthalate (DBP),
diisobutyl phthalate (DiBP), di-n-hexyl phthalate (DnHP), benzylbutyl
phthalate (BzBP), dicyclohexyl phthalate (DCHP), di(2-ethylhexyl)
phthalate (DEHP), and di-n-octyl phthalate (DnOP) were analyzed in
this study. Seven deuterated-PAEs including d4-DMP, d4-DEP, d4-DPP,
d4-DiBP, d4-BzBP, d4-DnHP, and d4-DEHP were used as surrogate
standards in the quantification of corresponding native compounds.
DnHP, DCHP, and DnOP concentrations were calculated based on the
responses of d4-DiBP, d4-DnHP, and d4-DEHP, respectively. The target
and surrogate standards were purchased from Sigma-Aldrich
(St. Louis, MO, USA). Dichloromethane (DCM), n-hexane and acetone
(analytical grade) were obtained from Merck KGaA (Darmstadt,
Germany). All native and surrogate standard solutions, and final sample
extracts were prepared in n-hexane.
Analysis was performed using a gas chromatograph (GC 7890B)
interfaced with a mass spectrometer (MS 5977A). A fused silica capillary
column (DB-5 ms, 30 m × 0.25 mm × 0.25 μm; Agilent Technologies;
Santa Clara, CA, USA) was used for chromatographic separation of
analytes. Detailed instrumental parameters for PAE analysis were re-
ported in our previous studies (Tran and Kannan, 2015; Tran et al.,
2017; Anh et al., 2021) and are provided in Table S1 (Supplementary
data).
2.2. Sampling
All water samples were collected from Hanoi metropolitan area
during August to December 2020 (Table S2). Samples were categorized
as tap water, bottled water, lake water and wastewater. Tap water
samples (n = 7) were collected directly from domestic water supplies
distributed to residents living in Hanoi. Plastic bottled water including
non-carbonated (n = 11) and carbonated (n = 10) water samples
(21 brands) were purchased in Hanoi supermarkets and stores. Tap
water and bottled water were extracted immediately following the
procedure for PAEs analysis or kept at 5 °C for no more than 7 days
(tap water) and expiry date (bottled water).
Lake water (n = 33) and wastewater samples (n = 35) were col-
lected by pooling of samples from five sampling trips at 2 h intervals.
There was no rainfall event for over 3 days prior to sampling. Lake
water samples were obtained from six lakes in Hanoi metropolitan
area including Thien Quang Lake (TQL, n = 7), Ba Mau Lake (BML, n
= 6), Hoan Kiem Lake (HKL, n = 7), Yen So Lake (YSL, n = 5), Truc
Bach Lake (TBL, n = 4), and West Lake (WL, n = 4). Wastewater sam-
ples were grouped into influents (n = 27) and effluents (n =
8) (Fig. S1, Supplementary data). For influent wastewater, samples
were collected along the lengths (15 and 20 km) of two sewage canals
which receive domestic discharges from central Hanoi. Wastewater
from one canal is directed into a wastewater treatment plant (WWTP)
whereas that from the other canal is pre-treated with sand before enter-
ing the WWTP. NaN3 was spiked into lake and wastewater samples at a
concentration of 0.25 g/L to inhibit microbial activity and ensure stabil-
ity of analytes. Samples were collected in amber glass bottles and
transported to the laboratory, and filtered through a Whatman filter
paper (pore size of 11 μm) to remove suspended particles. BOD (biolog-
ical oxygen demand) and COD (chemical oxygen demand) were deter-
mined for lake water and wastewater samples immediately after
collection (Table S2). Samples were extracted immediately as described
T.M. Le, H.M.N. Nguyen, V.K. Nguyen et al.
below or kept at 5 °C for no more than 7 days. Before storage, water
samples were filled-up in amber glass containers to avoid evaporation
of the target compounds.
2.3. Sample preparation
Two hundred nanograms of each surrogate standards were spiked
into 1500 mL of bottled water and tap water and 150 mL samples of
lake water and wastewater. Spiked samples were thoroughly mixed
for 5 min and allowed to equilibrate at room temperature for 30 min.
Each sample was passed through a C18 solid phase extraction (SPE) car-
tridge (500 mg/6 mL, Macherey-Nagel, Thermo Fisher Scientific Inc.,
Waltham, MA, USA) which was conditioned by 5 mL of n-hexane.
Then, the cartridge was dried under a gentle stream of nitrogen. Target
compounds were eluted with 20 mL mixture of DCM and n-hexane (1:1,
v/v). The eluted solution was concentrated under a gentle stream of ni-
trogen to 1 mL and transferred into a GC vial for analysis.
2.4. Quality assurance and quality control (QA/QC)
In order to reduce blank levels of PAEs, several precautions were
taken in the laboratory (Guo and Kannan, 2012). All glassware was
washed with a detergent and tap water, rinsed with double-distilled de-
ionized water and solvents (i.e., acetone, DCM and n-hexane), baked at
400 °C for 24 h, and kept in an oven at 100 °C until use. Before analysis,
pure hexane was injected into GC–MS until the background is stabilized.
Hexane was also injected simultaneously with every batch of real sam-
ples to check for any contamination from the instrument. Procedural
blanks were analyzed with real samples. Trace levels of PAEs were
found in procedural blanks (Table S4). The reported concentrations of
PAEs were corrected for the recoveries of surrogate standards and
subtracted from the mean value found in procedural blanks. Recoveries
of surrogate standards spiked in all samples ranged from 79% to 116%
with a relative standard deviation (RSD) of <15%. The method quantita-
tion limits (MQLs) were calculated based on the instrument detection
limits (a quantifiable peak must have a signal-to-noise ratio > 10),
water volume used in extraction (1500 mL for bottled water and tap
water and 150 mL for lake water and wastewater), and a final extract
volume (1 mL). Concentrations of the target compounds were calcu-
lated from an external standard method with a linear calibration
range from 0.5 to 1000 ng/mL and regression coefficients of (R2) >
0.995 for all compounds. The dilution factors were included in the calcu-
lation of PAEs concentrations.
2.5. Statistical analysis
Statistical analysis was performed using Microsoft Excel (Microsoft
Office 2010) and Minitab® 16 (Minitab LLC., State College, PA, USA).
The relationship between PAE concentrations and water sample types
was evaluated using Spearman's rank correlation analysis and hierar-
chical cluster analysis (HCA). The level of statistical significance was
set at p < 0.05. For concentrations below the MQLs, a value of one-half
the MQL was used in statistical analysis.
3. Results and discussion
3.1. Concentrations of PAEs in bottled water and human exposure to PAEs
through consumption of drinking water
The sum concentration of 10 PAEs measured in 21 plastic bottled
water samples ranged from 1640 to 15,700 ng/L (mean/median: 6400/
5820 ng/L). PAE concentrations in carbonated bottled water samples
were 1.2–1.5 times higher than those in non‑carbonated bottled water
samples. Our results are similar to those previously reported from Tehran,
Iran (Moazzen et al., 2018; Abtahi et al., 2019) and Portugal (Santana
et al., 2013) (Table 2). High concentrations of five target PAEs (DMP,
3
Science of the Total Environment 788 (2021) 147831
DEP, DBP, BzBP, and DEHP) were measured in bottled waters from 21
countries worldwide with a maximum value of 520,000 ng/L (mean:
14,900 ng/L) (Luo et al., 2018). The concentrations of PAEs (range:
190–980 ng/L; mean: 390 ng/L) in bottled water collected in Beijing,
China were lower than those found in our study (Xu et al., 2020).
In general, the profiles of individual PAEs in carbonated and
non‑carbonated bottled water were similar. Among PAEs, DBP was
found at the highest concentration at a range of 93–4710 ng/L (mean/
median: 1430/1120 ng/L), followed by DiBP (1420/1040 ng/L), BzBP
(1290/931 ng/L), and DEHP (993/902 ng/L). DMP, DPP, and DCHP
were found at lower frequencies (Table 1). These results were similar
to those reported earlier at 60–6500 ng/L for DBP, 100–1890 ng/L for
DiBP, and 20–160 ng/L for DEHP (Santana et al., 2013). In contrast,
Keresztes et al. (2013) showed that DEHP was the most abundant PAE
found in polyethylene terephthalate (PET) bottles packaged mineral
water. This suggests that the sources of PAEs in bottled waters may be
from leaching of plastic containers, water source, or/and during produc-
tion and bottling.
Overall, PAE levels found in bottled drinking water were signifi-
cantly below the permissible levels suggested by the US EPA. The no ob-
served adverse effect level (NOAEL) of BzBP, DEHP, DBP, DEP, and DMP
in water were 0.10; 0.32; 20; 600; and 2000 μg/L, respectively (US EPA,
2015). The Vietnamese Ministry of Health only regulates DEHP in drink-
ing water with a maximum permissible limit of 1500 μg/L (Vietnam
Ministry of Health, 2011).
Human exposure doses of PAEs were estimated based on the mean
concentrations of PAEs measured in bottled water, the body weight
(bw) of Vietnamese [adults (63 kg-bw) and children (25 kg-bw)] (Do
et al., 2017; Truong et al., 2020), and the amount of water consumed
by individuals (2.5 and 1.0 L/day for adults and children, respectively)
(WHO, 2005). The mean/median exposure doses of 10 PAEs calculated
for adults and children through the consumption of bottled drinking
water were 254/231 and 256/233 ng/kg-bw/day, respectively. The ex-
posure doses of PAEs through the consumption of drinking water for
adults and children were not significantly different. The exposure
doses to individual PAEs through water consumption were also esti-
mated for adults and children (Table 2). Among PAEs, the mean expo-
sure doses of DBP were the highest (56.9/57.3 ng/kg-bw/day for
adults/children, respectively), followed by DiBP (65.5/57 ng/kg-bw/
day), BzBP (51.5/51.6 ng/kg-bw/day), and DEHP (39.4/39.7 ng/kg-bw/
day). The estimated exposure doses of PAEs for Vietnamese were simi-
lar to those reported for Iranians at values ranging from 21 ng/kg-bw/
day (for BzBP) to 70 ng/kg-bw/day (for DEHP) (Jeddi et al., 2016).
Human exposure doses of PAEs through drinking water consump-
tion were much lower than the oral RfDs (100 and 20 μg/kg/day for
DBP and DEHP, respectively) recommended by the US FDA (US FDA,
2012). Humans are exposed to PAEs via multiple pathways including in-
halation, ingestion, and dermal absorption. In general, the exposure
doses of PAEs through the consumption of drinking water were
1.5–2.5 times lower than those estimated for inhalation (Tran et al.,
2017; Anh et al., 2021) but still higher than the values for dust ingestion
(Tran et al., 2016). An earlier study reported exposure doses to PAEs
through inhalation, at a range of 213 ng/kg-bw/day (for adults) to 780
ng/kg-bw/day (for infants) in Vietnam (Tran et al., 2017). Based on
male developmental toxicity (anti-androgenicity), a new reference
dose for PAEs was suggested for use in mixture risk assessment: DBP
(6.7 μg/kg-bw/day), BzBP (10 μg/kg-bw/day), DEHP (10 μg/kg-bw/
day), DINP (diisononyl phthalate: 59 μg/kg-bw/day), and DiBP (100
μg/kg-bw/day) (Kortenkamp and Koch, 2020). The calculated exposure
doses of PAEs through drinking water in Vietnam were below the max-
imum allowable limits (US FDA, 2012; Kortenkamp and Koch, 2020).
3.2. Concentrations of PAEs in tap water
PAEs were found in tap water samples collected from several house-
holds in mid Hanoi. Total concentrations of PAEs in tap water samples
 T.M. Le, H.M.N. Nguyen, V.K. Nguyen et al. Science of the Total Environment 788 (2021) 147831

ranged from 2100 to 18,000 ng/L (mean/median: 11,200/9270 ng/L).

19,600–127,000

20,700–405,000

26,800–79,800
1790–10,700

1640–15,700

2100–18,000
The concentrations of PAEs in tap water collected from Hanoi were sim-
ilar to those reported from Tianjin, China (Wang et al., 2021) but signif-

121,000
115,000
11,200

51,800
49,300

46,900
41,800
ƩPAEs

icantly higher than those from Tehran, Iran (Abtahi et al., 2019). In
5590
5300

7290
5900

9270
general, PAE levels in tap water were slightly higher than those found
in bottled water (Fig. 1). Among PAEs, DEHP accounted for the highest

1030–37,300
proportion of up to 47.6% of the total concentrations, followed by BzBP
n.d. – 1110

n.d. – 1930

n.d. – 7310

539–2730
n.d. – 945

(12.5%), and DEP (9.75%). These results suggest different profiles of

10,300
DnOP

2440
2260

7180

1630
1610
PAEs in tap water (normally used in daily activities) compared with bot-
81.8

90.0

97.0
71.4

97.0
315
191

505
535

450

100

100
tled water (used directly for drinking).
To our knowledge, no earlier study has reported the distribution of

8580–150,000
1010–14,500

1040–48,700

2840–42,400
PAEs in tap water in Vietnam. Our results suggest widespread occur-
227–1950

103–2710

18,000 rence of PAEs in tap water. Sources of PAEs include water sources,
14,000

54,600
44,700

16,500
11,500
DEHP

1120

5340
4300

water treatment processes and distribution pipes. Polyvinyl chloride

873
615
100

920
100

100

100

100

100
(PVC) pipes are widely used to distribute water in households in
Vietnam. Previous studies showed that PAEs, especially DEHP, are
1280–29,700

widely used as plasticizers in PVC (Navarro et al., 2010; Xu et al.,

101–8500

218–3570
n.d. – 732

n.d. – 915

5.0–1290

2012; Chong et al., 2019). Release of DEHP from PVC plastic has been re-
DCHP

2780
1770

6420
4430

1380
81.8

60.0
347
365

339
205

542
533
100

100

100

927
100
ported (Clausen et al., 2012; Rose et al., 2012), which can explain the oc-
currence of PAEs in tap water.
182–21,100

425–39,200
256–4370

132–2520

197–4210

380–8970

3.3. Concentrations of PAEs in lake water

1420

1140
1100

1400

2920
1600

8830
4830

4680
5960
BzBP

873
100

100

731
100

100

100

100

Ten PAEs were found in 33 surface water samples collected from 6

lakes in Hanoi metropolitan area. Most PAEs were found in lake water
n.d. – 1060

n.d. – 2720

n.d. – 3200
104–8020
n.d. – 641

37.5–900

samples with frequencies of 100%, except DnHP (90.9%) and DnOP

DnHP

(97.0%). DEHP was measured at the highest levels in the range of

2360
1370

1630
1630
65.0
81.8

91.0
80.0

90.9

87.5
172

182

417
369
100

357
192

100

1040–48,700 ng/L (mean/median: 18,000/14,000 ng/L), followed by

DBP (12,300/11,800 ng/L), and DiBP (8070/6860 ng/L) (Fig. 2). Total con-
1740–44,900
783–34,000

centrations of PAEs in lake water ranged from 19,600 to 127,000 ng/L

1580–9450
93.0–4710

14.0–2560
145–3070

(mean/median: 51,800/49,300 ng/L). Generally, the concentrations of

12,300
11,800

11,500
1150

1740
1340

7420

5820
5810

PAEs in lake water were significantly higher than those in plastic bottled
DBP

823
100

100

796
406
100

100

100

100

water and tap water.

The similar levels of PAEs in water samples collected from various
1170–73,900

5500–11,900
605–26,600
94.0–3930

27.0–1390

lakes located in Hanoi metropolitan area suggest ubiquitous distribu-

123–5190

12,500

tion of these chemicals. All these lakes receive storm water from
1100

1790
1400

8070
6860

7560

7860
7770
DiBP

233
100

100

456
131
100

100

100

100

crowded residential areas. High levels of PAEs measured in water sam-

ples from lakes can be explained by urban runoff and storm water dis-
320–11,600

charges. PAE levels in lake water in our study were significantly

167–4820
n.d. – 423

n.d. – 493

n.d. – 940

62–2990

higher than those reported for river water in China (Li et al., 2016,
Concentrations (ng/L) of PAEs in different types of water samples collected from Hanoi, Vietnam.

3180
1870

1820
1310

2017; Wen et al., 2017) (Table 3). No previous study reported the occur-
66.0
36.5
63.6

68.5
70.0

85.7
DPP

158

372
219

702
439
100

100

100

rence of PAEs in water samples collected from lakes in Hanoi metropol-

itan area. Therefore, further assessment of the PAEs distribution in lake
639–14,000

931–29,400

1260–7040
n.d. – 2570
n.d. – 988

n.d. – 626

water as well as surface water from Vietnam should be conducted.

1090

3310
1910

7760
5700

4390
4950
16.0
81.8

90.0

85.7
DEP

109

234
171

736

100

100

100

3.4. Concentrations of PAEs in wastewater

115–2950

241–8390

220–1870
n.d. – 174

n.d. – 312

n.d. – 545

All ten PAEs were found in wastewater samples collected from two
main sewage canals flowing across the Hanoi metropolitan area. The
3630
3360

1120
1020
DMP

30.0
10.0
72.7

87.0
42.0
80.0

85.7
351
369

924
830
100

100

100

sum concentrations of PAEs in 27 wastewater samples collected along

the transection of two canals (Kim Nguu and To Lich) ranged from
Statistics

Median

Median

Median

Median

Median

Median

20,700 to 405,000 ng/L (mean/median: 121,000/115,000 ng/L)

Freq.%

Freq.%

Freq.%

Freq.%

Freq.%

Freq.%
Range

Range

Range

Range

Range

Range
Mean

Mean

Mean

Mean

Mean

Mean

(Table 1). DEHP was found at the highest levels in wastewater at a

concentration range of 8580–150,000 ng/L (mean/median: 54,600/
n.d.: not detection; Freq.%: detection rate (%);
Non‑carbonated bottled water (n = 11)

44,700 ng/L). The concentrations of PAEs in wastewater in these two ca-

nals were much higher than those reported in previous studies in
Carbonated bottled water (n = 10)

Vietnam (Quynh and Toan, 2019; Toan et al., 2019). A recent study re-
Wastewater (Influent) (n = 27)

Wastewater (Effluent) (n = 8)

ported six PAEs in wastewater samples from the Kim Nguu canal at a
concentration range of 2.78–412 ng/L. In comparison, PAEs concentra-
tions in wastewater in our study were similar to those reported in
Lake water (n = 33)
Tap water (n = 7)

Lithuania, Poland, and Denmark (Anne and Paulauskiene, 2021). Very

high levels of PAEs were reported in wastewater from Austria (Clara
et al., 2010) and China (Wu et al., 2018).
Categories

The spatial distributions of PAEs in wastewater samples (both two

Table 1

canals) were not significantly different (Table S6). Total concentrations

of PAEs in 8 effluents from WWTPs ranged from 26,800 to 79,800 ng/L

4
T.M. Le, H.M.N. Nguyen, V.K. Nguyen et al. Science of the Total Environment 788 (2021) 147831

Table 2
The exposure doses (ng/kg-bw/day) of PAEs through the consumption of drinking water estimated for Vietnamese adults and children.

Age DMP DEP DPP DiBP DBP DnHP BzBP DCHP DEHP DnOP ƩPAEs

Adults Mean 2.28 6.68 4.36 56.5 56.9 7.01 51.5 13.6 39.4 16.1 254
Median 0.859 1.89 2.09 41.2 44.4 2.57 36.9 12.0 35.8 11.0 231
Children Mean 2.30 6.74 4.39 57.0 57.3 7.07 51.6 13.7 39.7 16.2 256
Median 0.866 1.91 2.11 41.5 44.7 2.59 37.2 12.0 36.1 11.1 233

(mean/median: 46,900/41,800 ng/L). The decrease 10-fold reduction in
PAE levels was evident between influent and effluent wastewater.
These results suggest that PAEs may be lost (volatilization), degraded,
transferred into sludge and/or transformed in biological wastewater
treatment processes.
Several factors affect the distribution of PAEs in the aqueous phase
(Gani and Kazmi, 2016; Kashyap and Agarwal, 2018). Solubility of a
chemical in water is an important property that governs the biodegra-
dation. Zhang et al. (2015) suggested that the solubility of PAEs in
water decreases with increasing alkyl chain length. Like other volatile
organic compounds, water solubility of PAEs decreases with increasing
temperature (Thomsen et al., 2001; Santana et al., 2013; Zhang et al.,
2015) (Table S3).
3.5. Sources of PAEs
PAE concentrations measured in each sample category (i.e., bottled
water, tap water, lake water, wastewater influent and effluent) were
subjected to Spearman's rank correlation analysis to assess their relation-
ships (Fig. S2). In bottled water samples, moderate correlations
(Spearman's rho = 0.53–0.76; p < 0.05) were observed for several
pairs such as DMP and DEP, DBP, DnOP; DEP and DBP, DiBP, DnOP;
DEHP and BzBP; and DBP and DiBP. No significant correlation among
PAEs was found in tap water samples. DBP and DiBP were highly corre-
lated in lake water (Spearman's rho = 0.74; p < 0.01). In wastewater in-
fluent samples, the highest correlation was observed for DBP and DiBP
(Spearman's rho = 0.78; p < 0.01). BzBP/DnHP and DnOP/DEHP showed
high correlation (Spearman's rho = 0.83 and 0.86, respectively; p < 0.05)
in wastewater effluent samples. Our previous studies showed significant
correlation between DiBP and DBP in Vietnamese ambient air (Anh et al.,
2019a, 2021) and road dust (Anh et al., 2019b). These two compounds
have similar physicochemical properties (Net et al., 2015) and are used
as plasticizers and additives in personal care products and are probably
used in combination (He et al., 2018; Zhang et al., 2018). Similarly,
DEHP levels were correlated with DnOP which can be explained by sim-
ilar properties and applications (e.g., plasticizers in PVC resins and other
plastics) (ATSDR, 1997; ATSDR, 2019).
We analyzed the compositions of PAEs in different sample categories
by using hierarchical cluster analysis (Fig. 3). Bottled water samples
were characterized by elevated proportions of DBP, DiBP, and BzBP,
and moderate proportions of DEHP. DBP was the major compound de-
tected in polyethylene terephthalate (PET) bottles (Salazar-Beltrán
et al., 2018). The occurrence of PAEs in bottled water is likely attributed
to migration from plastic bottles (Otero et al., 2015; Salazar-Beltrán
et al., 2018; Wang et al., 2021). DBP, BzBP, and DEHP were also fre-
quently found in bottled water samples (Otero et al., 2015; Wang
et al., 2021). The PAE profiles in tap water, Hoan Kiem Lake water, and
influent wastewater samples were similar (i.e., dominated by DEHP),
reflecting domestic discharge as the principal source of PAEs in the
urban Hanoi. Water samples from West Lake, Ba Mau, Yen So, and
Thien Quang Lakes showed similar distribution patterns of PAEs
(i.e., comparable proportions of DEHP and DBP). The PAE profiles in ef-
fluent wastewater samples were somewhat different from influent
ones, suggesting varied removal efficiency of PAEs in WWTPs. Thus, sev-
eral factors including emission sources, degradation, removal efficiency,
meteorological and hydrological conditions, affect the profiles of PAEs in
the aquatic environment.
4. Conclusions
This study provides baseline information on the contamination sta-
tus and distribution profiles of ten typical PAEs in water samples in
Hanoi. High levels of PAEs were measured in wastewater samples.
PAE concentrations in wastewater decreased significantly following
treatment in WWTPs. The contamination pattern of PAEs was in the de-
creasing order: wastewater ≫ lake water > tap water > bottled water.
Among PAEs, DEHP was the major compound found in tap water, lake
water, and wastewater samples. In contrast, DiBP, and DBP were the

Fig. 1. Concentrations (median and range, ng/L) of total PAEs in water samples from Hanoi,
Vietnam (NCB: non-carbonated bottled water, CB: carbonated bottled water, TAP: tap
water, TQL: Thien Quang Lake water, HKL: Hoan Kiem Lake water, BML: Ba Mau Lake
water, TBL: Truc Bach Lake water, YSL: Yen So Lake water, WL: West Lake water, EFF: ef-
fluent wastewater, KNIN: influent wastewater from Kim Nguu canal, TLIN: influent waste-
water from To Lich canal).
Fig. 2. Compositions of total PAEs in water samples from Hanoi, Vietnam (NCB: non-car-
bonated bottled water, CB: carbonated bottled water, TAP: tap water, TQL: Thien Quang
Lake water, HKL: Hoan Kiem Lake water, BML: Ba Mau Lake water, TBL: Truc Bach Lake
water, YSL: Yen So Lake water, WL: West Lake water, EFF: effluent wastewater, KNIN: in-
fluent wastewater from Kim Nguu canal, TLIN: influent wastewater from To Lich canal).

5
T.M. Le, H.M.N. Nguyen, V.K. Nguyen et al. Science of the Total Environment 788 (2021) 147831

Table 3
Comparison of PAE concentrations (ng/L) in water samples from various studies.

Categories Location n Concentration Phthalates Referrences

Bottled water Hanoi, Vietnam 21 1640–15,700 (6400) DMP, DEP, DPP, DiBP, DBP, DnHP, BzBP, DCHP, DEHP, DnOP This study
Bottled water Tianjin, China n.a. 1960 ± 160 DBP, BzBP, DEHP Wang et al., 2021
Bottled water global countries n.a. n.a. – 520,000 (14,900) DMP, DEP, DBP, BzBP, DEHP Luo et al., 2018
Bottled water Beijing, China 10 190–980 (390) DMP, DEP, DBP, BzBP, DEHP, DnOP Xu et al., 2020
Bottled water Beijing, China 60 155–5200 (519) DMP, DEP, DPP, DBP, BzBP, DEHP, DnOP Li et al., 2019
Bottled water Tehran, Iran 45 960 ± 100 DMP, DEP, DBP, BzBP, DEHP, DnOP Abtahi et al., 2019
Bottled water Tehran, Iran 6 547 ± 260 DBP, BzBP, DEHP Jeddi et al., 2016
Carbonated soft drinks Tehran, Iran 3 599–14,200 (3450) DMP, DEP, DBP, BzBP, DEHP, DnOP Moazzen et al., 2018
Drinking water Geographical zones, China 225 n.a. (1280) DMP, DEP, DBP, BzBP, DEHP, DnOP Liu et al., 2015
Drinking water Portugal 11 20–6500 DBP, BzBP, DEHP Santana et al., 2013
Tap water Hanoi, Vietnam 7 2090–18,000 (11,200) DMP, DEP, DPP, DiBP, DBP, DnHP, BzBP, DCHP, DEHP, DnOP This study
Tap water Tianjin, China n.a. 2410 ± 391 DBP, BzBP, DEHP Wang et al., 2021
Tap water Tehran, Iran 40 760 ± 190 DMP, DEP, DBP, BzBP, DEHP, DnOP Abtahi et al., 2019
Lake water Hanoi, Vietnam 33 19,600–127,000 (51,800) DMP, DEP, DPP, DiBP, DBP, DnHP, BzBP, DCHP, DEHP, DnOP This study
River water Songhua River, China 28 1150–7870 (3200) DMP, DEP, DBP, DEHP, DnOP, DINO, DIDP Wen et al., 2017
River water Pearl River Delta, China 18 500–28,100 DMP, DEP, DBP, BzBP, DEHP, DnOP Li et al., 2016
River water Jiulong River, China 25 3480–17,700 DMP, DEP, DIBP, DBP, DEHP, DINP Li et al., 2017
Influent Hanoi, Vietnam 27 20,700–405,000 (121,000) DMP, DEP, DPP, DiBP, DBP, DnHP, BzBP, DCHP, DEHP, DnOP This study
Effluent Hanoi, Vietnam 8 26,800–79,800 (46,900) DMP, DEP, DPP, DiBP, DBP, DnHP, BzBP, DCHP, DEHP, DnOP This study
Wastewater Hanoi, Vietnam 6 2.78–412 DMP, DEP, DBP, BzBP, DEHP, DnOP Quynh and Toan, 2019
Influent Vienna, Austria 15 4480–58,700 (26,700) DMP, DEP, DBP, BzBP, DEHP, DnOP Clara et al., 2010
Effluent Vienna, Austria 15 188–12,000 (3340) DMP, DEP, DBP, BzBP, DEHP, DnOP Clara et al., 2010
Influent Qingdao, China 57 114,000–180,000 DMP, DEP, DPP, DBP, BzBP, DCHP, DEHP, DnOP Wu et al., 2018
Effluent Qingdao, China 57 22,500–30,700 DMP, DEP, DPP, DBP, BzBP, DCHP, DEHP, DnOP Wu et al., 2018
Influent Alice, South Africa 6 n.a. (1,210,000) DMP, DEP, DBP, BzBP, DEHP, DnOP Salaudeen et al., 2018
Effluent Alice, South Africa 6 n.a. (22,500) DMP, DEP, DBP, BzBP, DEHP, DnOP Salaudeen et al., 2018

n: number of samples; n.a.: not available; values in parentheses refer to the mean concentrations.

major compounds in bottled water samples. The human exposure dose
to PAEs via drinking water was lower than that calculated for inhalation.
The measured PAE concentrations and exposure doses through drinking
water ingestion were below the permissible levels and reference doses.
CRediT authorship contribution statement
Thuy Minh Le: Conceptualization, Data curation, Formal analysis,
Funding acquisition, Writing – original draft. Ha My Nu Nguyen: Con-
ceptualization, Investigation, Methodology, Formal analysis. Vy Khanh
Nguyen: Formal analysis. Anh Viet Nguyen: Formal analysis. Nam
Duc Vu: Conceptualization, Resources. Nguyen Thi Hong Yen: Concep-
tualization, Resources. Anh Quoc Hoang: Writing – review & editing. Tu
Binh Minh: Writing – review & editing. Kurunthachalam Kannan:
Writing – review & editing. Tri Manh Tran: Supervision, Conceptualiza-
tion, Resources, Methodology, Writing – review & editing.

Declaration of competing interest

The authors declare that they have no known competing financial

interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.

Acknowledgements

Thuy Minh Le was funded by Vingroup Joint Stock Company and

supported by the Domestic Master/PhD Scholarship Programme of
Vingroup Innovation Foundation (VINIF), Vingroup Big Data Institute
(VINBIGDATA), code VINIF.2020.TS.58.

Appendix A. Supplementary data

Supplementary data to this article can be found online at https://doi.

org/10.1016/j.scitotenv.2021.147831.

Fig. 3. Hierarchical cluster analysis of PAEs in water samples from Hanoi, Vietnam (NCB:
non-carbonated bottled water, CB: carbonated bottled water, TAP: tap water, TQL: Thien
Quang Lake water, HKL: Hoan Kiem Lake water, BML: Ba Mau Lake water, TBL: Truc
Bach Lake water, YSL: Yen So Lake water, WL: West Lake water, EFF: effluent wastewater,
KNIN: influent wastewater from Kim Nguu canal, TLIN: influent wastewater from To Lich
canal).
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