Behavior of Chemicals Suspected of EDCs andOther Related Chemicals in Drinking Water Supply
水道における内分泌かく乱化学物質とその他関連化学物質の挙動

Shoichi Kunikane, National Institute of Public Health, MHLW,
Japan
国立保健医療科学院‑ 311 ‑

国包章一

BEHAVIOR OF CHEMICALS SUSPECTED OF EDCs AND OTHER
RELATED CHEMICALS IN DRINKING WATER SUPPLY
Shoichi Kunikane*, Koji Kosaka* and Tatsuo Yonezawa**
ABSTRACT
A study on the behavior of di-2-ethylhexyl phthalate(DEHP) and di-n-butyl
phthalate(DNBP) at eleven water treatment plants showed that both DEHP and
DNBP could be removed to some extent by water treatment with a rapid sandfiltration system. DEHP in raw water tended to be concentrated in sludge and scum
more than DNBP in raw water. Another study on their mass balance at three water
treatment plants showed that a considerable part of DEHP and DNBP contained in
raw water was accumulated in sludge at a water treatment plant, and that only alimited part of them was concentrated in scum. In addition, it was found as the resultof repeated chemical release tests using water pipes coated with tar-epoxy resin
paint, which had widely been used, that phthalates, phenols and polyaromatichydrocarbons(PAHs) were released at the beginning of their use, but that the releaseof those chemicals would not last for many months.
KEYWORDS
Endocrine disrupting chemicals(EDCs), drinking water treatment, water pipes,
di-2-ethylhexyl phthalate(DEHP), di-n-butyl phthalate(DNBP), polyaromatichydrocarbons(PAHs)
INTRODUCTION
Endocrine disrupting chemicals(EDCs) are of concern among researchers since
several years ago. We have been conducting a series of researches on chemicals
suspected of EDCs in drinking water. The scope of such researches mainly includes
their occurrence in raw and treated waters, their removal and behavior in water
treatment processes, their release from water supply materials, and estrogenic
activities of their chlorination by-products. At present, we are conducting studies on
the behavior of di-2-ethylhexyl phthalate(DEHP) and di-n-butyl phthalate(DNBP) in
drinking water treatment, and the release of phthalates, phenols and polyaromatic___________________________________________________________________________* Department of Water Supply Engineering, National Institute of Public Heath,
Shirokanedai 4-6-1, Minato-ku, Tokyo 108-8638, Japan** Department of Engineering, Japan Water Works Association, Kudan-minami 4-8-9,
Chiyoda-ku, Tokyo 102-0074, Japan1‑ 312 ‑

hydrocarbons(PAHs) from tar-based resin paints.
In this paper, the result of such studies on the behavior of EDCs in drinking watersupply is reported and discussed.
BEHAVIOR OF PHTHALATES IN DRINKING WATER TREATMENT

Background and objective
Since phthalates, such as DEHP and DNBP, are widely used as the plasticizer ofplastics, they often occur in raw water for drinking water supply. They are also
released from the materials used for water supply, e.g. water pipes, in contact withwater. In our previous study1), we found that DEHP existed at a very highconcentration of more than 10µg/l in treated water at the top layer of a treated water
reservoir of a certain treatment plant. Then, the DEHP and DMBP contents insludge and scum as well as their concentrations in raw and treated waters at elevenwater treatment plants in Japan were investigated for the purpose to know their
behavior in water treatment processes. In addition, a more detailed study was
conducted at three out of those ten water treatment plants for the purpose to know
their mass balance in water treatment processes.

Methods
Samples of water, sludge and scum were taken once at each of eleven water
treatment plants in January through February, 2003, and analyzed on DEHP, DNBP
and other parameters. Ten treatment plants adopt a rapid sand filtration system,
whereas the other one treatment plant adopts a slow sand filtration system. After
that, samples of water, sludge and scum were taken again at each of three out of
those ten water treatment plants, with a rapid sand filtration system, once a monthin January through March, 2004, and analyzed on the same parameters as theprevious study. Other data necessary for mass balance analysis such as water flowrate and sludge generation were obtained from each water supply.

Result and discussions
Figure 1 shows the result of analysis on DEHP and DNBP concentrations in raw andtreated waters of eleven water treatment plants. Both DEHP and DNBP
concentrations in raw water at all treatment plants were less than 1µg/l, and DEHP
concentrations in raw water were almost the same as or higher than DNBP
concentrations in raw water. Both of the distribution of DEHP and DNBP
2
‑ 313 ‑

concentrations in water shifted to lower ranges after treatment, which means that
DEHP and DNBP were removed to some extent.
11

12

Number of plants(-)

8
6

DEHP in raw water
DEHP in treated water
DNBP in raw water
DNBP in treated water

9

10

5

6

4

2

2

3
1

3
1

0

2

1

0

0 0 0

0
<0.05

0.05-0.1

0.1-0.5

Range of concentration(µg/l)

0.5-1.0

Figure 1 DEHP and DNBP concentrations in raw and treated waters
Figure 2 and 3 show the contents of DEHP and DNBP, respectively, in sludge andscum. Sludge samples were taken only at ten treatment plants with a rapid sandfiltration system. Scum samples were taken at the inlet of a sedimentation basin inmost plants, but scum was not formed at three of those ten treatment plants. It isclear from these results that both DEHP and DNBP were concentrated not only insludge but also in scum, and that they tended to be concentrated more in scum thanin sludge. The maximum contents of DEHP in sludge and scum were 14 and 52mg/kg
dry weight, respectively. The maximum contents of DNBP in sludge and scum were
2.2 and 2.3mg/kg dry weight, respectively. It was also found that DEHP tended to beconcentrated in sludge and scum more than DNBP. This might be due to thedifference in Kow between DEHP and DNBP.
Figure 4 to 6 show the result of a detailed study on the mass balance of DEHP atthree water treatment plants with a rapid sand filtration system. It was found fromthe result that a considerable part of DEHP contained in raw water was accumulated

Number of plants(-)

6
5
4

5 5

S ludge
S cum

3

3
2

2

2
1

0 0

0

0
< 0.1

0.1～1

1～10

10～100Range of content(mg/kg)

Figure 2 DEHP contents in sludge and scum3
‑ 314 ‑

Number of plants(-)

7

6

6
5

S ludge
S cum

5

4
3

2

2
1

2

1

1
0 0

0
< 0.1

0.1～1

1～10

10～100Range of content(mg/kg)

Figure 3 DNBP contents in sludge and scumin sludge at each treatment plant, and only a limited part of it was concentrated inscum. The result of DNBP mass balance also showed a similar result. One of thetreatment plants was typical because the water at a top layer of its treated water
reservoir exhibited a very high DEHP concentration at every sampling occasion as
was in a previous study1). Such a phenomenon could not be found in other treatment
plants.
RELEASE OF PAHs AND OTHER CHEMICALS FROM WATER PIPES

Background and objective
Tar-based resin paints such as tar-epoxy and coal tar enamel resin paints had widely
been used for painting the inner wall of water pipes and basins in Japan. Although
they are not used since more than ten years ago, it is of concern that they may have apotential of releasing hazardous chemicals, like EDCs, to drinking water2). It is also amatter of concern that the by-product of a reaction of chemicals, which are released
2.9(2.0-3.7)

26,000(11,000-44,000)
Raw
water

Receivingwell160(90-230)
Cooling water

37,000(10,000-69,000)

Coag./Sed.
basin

Rapid sandfilter

9,300(7,600-12,000)

2,300(0-6,900)
TreatedTreatedwater
wat. res.

890(350-1,700)

Sludgebasin

Thickener

Sewer

Figure 4 Mass balance of DEHP at “R” water treatment plant(unit: mg/d)
4‑ 315 ‑

0.14
(0-0.41)

4,100(0-7,100)
Raw
water

Receiving
well

1,400
(0-4,100)

Coag./Sed.
basin

4,300
(0-4,000)

Rapid sandfilter

2,300(900-4,100)

Treatedwater

Treatedwat. res.

5(0-15)
Sewer

Sludgebasin

Thickener

Dehydrator

3.7(2.1-4.6)
2,300
2,100
(1,600-3,500)(1,200-2,800)
Sludge cake

3,500
(3,300-3,600)

Figure 5 Mass balance of DEHP at “Q” water treatment plant(unit: mg/d)
8,200(0-15,000)
Raw
water

<3.3

2,600
(0-7,700)
Receiving
well

Coag./Sed.
basin

Rapid sandfilter

13,000(9,100-16,000)

1,300(1,200-1,500)

Treatedwat. res.

25(0.02-58)

Treated
water

5,500
(3,900-7,000)
11,000(5,700-17,000)

Sludgebasin

0Thickener

Dehydrator

9,700(1,800-17,000)
Sludgecake

3.7(2.3-4.9)

Figure 6 Mass balance of DEHP at “T” water treatment plant(unit: mg/d)
to water, with residual chlorine in water may have a health risk potential as EDCs.
Then, a study on the release of chemicals was conducted using samples of water
pipes, coated with tar-epoxy resin paint, which were newly produced for the study.

Methods
Two types of new steel water pipes, with an inner diameter of 32mm and 40mm,
coated with tar-epoxy resin paint on their inner wall were used for the study. The
grade of the paint was same as that used for water pipes in old days. Ten pipes of5‑ 316 ‑

each type were installed on a rack, connecting them with each other in line, in awater treatment plant, and continuously supplied with treated water containing
residual chlorine at a flow rate of one cubic meter per day in order to simulate a daily
use of drinking water. The pipes were removed from the rack and transported to alaboratory for a chemical release test at selected time intervals.
The conditions of chemical release test were as follows: temperature at 23±1ºC andcontact time for 16 hours. A bland of commercially available mineral watercontaining minimum concentrations of target chemicals was used for the test without
adding chlorine or any other chemicals. A blank test with a similar procedure, but
without contact with the pipes, was also done in parallel. Chemicals analyzed on an
extract obtained after contact with the pipes and a blank water sample were DEHP,
DNBP, nonylphenol, bisphenol A, and PAHs. If the difference in the concentrations ofeach chemical between an extract and a blank water sample after a similar
procedure was not less than the lower limit of release detection for each chemical, it
was considered that its release had occurred. The lower limit of release detection foreach chemical was determined through a statistical analysis of the result of blanktests separately done. After finishing the test, the pipes were transported back to thewater treatment plant, reinstalled on a rack, and continuously supplied with treatedwater.

Result and discussions
Table 1 shows the result of chemical release tests during six months from the start ofthis study. The release of many kinds of chemicals from both types of water pipes wasobserved at the beginning. The concentrations of DNBP and fluoranthene in a water
sample after contact with 32mm pipes were more than 1µg/l, whereas those of others
chemicals were less than 1µg/l. The concentrations of all chemicals in a water sample
after contact with 40mm pipes were also less than 1µg/l. The concentrations of all
selected chemicals in the extract obtained after contact with both types of pipes
uniformly decreased until six months after the start of this study. It is consideredfrom such a result that water pipes coated with tar-epoxy resin paint may releasechemicals, including phthalates, phenols and PAHs, but the release of thosechemicals will not last for many months. It is planned to continue the study until
about two years after its start even though significant release of selected chemicals
may not occur.
CONCLUSIONS
The main findings of this research on the behavior and mass balance of chemicals
6‑ 317 ‑

Table 1 Release of phthalates, phenols and PAHs from water pipes coatedwith tar-epoxy resin paintChemicalLowerlimit*(µg/l)

Di-2-ethylhexyl phthalate

0.4

Di-n-butyl phthalate

Released concentration**(µg/l)
At the beginning

After 1 month

After 6 months

32mm

40mm

32mm

40mm

32mm

40mm

ND

ND

ND

ND

ND

ND

0.4

1.4

ND

0.7

ND

ND

ND

Nonylphenol

0.08

0.09

0.10

ND

ND

ND

ND

Bisphenol A

0.01

0.39

0.12

0.04

ND

ND

ND

Benzo(a)pyrene

0.01

ND

0.01

ND

ND

ND

ND

Benzo(a)fluoranthene

0.01

0.02

0.02

0.02

0.01

ND

ND

Fluoranthene

0.01

1.2

0.58

0.60

0.18

0.08

0.04

Benzo(a)antracene

0.01

0.04

0.03

0.02

ND

ND

ND

Pyrene

0.01

0.67

0.38

0.20

0.05

0.01

ND

Chrysene
0.01
0.11
0.12
0.07
0.04
0.02
ND
*) The lower limit of release diction. If the difference in the concentrations of each chemical
between an extract and a blank water sample was not less than this value, it was consideredthat the release of a chemical had occurred.
**) The difference in the concentrations of each chemical between an extract and a blank water
sample.

suspected of EDCs are as follows:
1) Both DEHP and DNBP can be removed to some extent by water treatment with arapid sand filtration system.
2) DEHP in raw water tends to be concentrated in sludge and scum more than DNBP
in raw water.
3) A considerable part of DEHP and DNBP contained in raw water is accumulated insludge at a water treatment plant, and only a limited part of them is concentrated
in scum.
4) Water pipes coated with tar-epoxy resin paint, which were widely used, releasephthalates, phenols and PAHs, but the release of those chemicals will not last for
many months.
ACKNOWLEDGMENT
This study is supported by a Health and Labor Sciences Research Grant in
FY2002-2004. The authors express sincere gratitude to local water supplies forcontributing to the sampling of water, sludge and scum, and to steel water pipe
manufacturers for providing water pipe samples.
REFERENCES
7‑ 318 ‑

1) S. Kunikane, et al.(2002) A report on the behavior of EDCs in drinking water andthe measures against drinking water contamination with them(in Japanese).
2) World Health Organization(1996) Guidelines for Drinking-water Quality, 2ndedition, Vol.2: Health criteria and other supporting information.

8‑ 319 ‑

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