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Removal of radioactive iodine and cesium in water

purification processes after an explosion at a nuclear power
plant due to the Great East Japan Earthquake
Koji Kosaka a,*, Mari Asami a, Naoya Kobashigawa a, Keiko Ohkubo a, Hiroshi Terada a,
Naohiro Kishida a, Michihiro Akiba b
a
b

Department of Environmental Health, National Institute of Public Health, 2-3-6 Minami, Wako, Saitama 351-0197, Japan
National Institute of Public Health, 2-3-6 Minami, Wako, Saitama 351-0197, Japan

article info

abstract

Article history:

The presence of radionuclides at five water purification plants was investigated after an

Received 7 February 2012

explosion at a nuclear power plant hit by the Great East Japan Earthquake on 11 March

Received in revised form

2011. Radioactive iodine (131I) and cesium (134Cs and

6 May 2012

Fukushima and neighboring prefectures. 131I was not removed by coagulationeflocculation

Accepted 27 May 2012

esedimentation.

Available online 7 June 2012

activated carbon (PAC) at a level of about 30%e40%, although 131I was not removed in some

137

Cs) were detected in raw water in

131

I was removed by granular activated carbon (GAC) and powdered

cases. This was also confirmed by laboratory-scale experiments using PAC. The removal
131

I in river and pond waters by 25 mg dry/L of PAC increased from 36% to

Keywords:

percentages of

Radioactive iodine

59% and from 41% to 48%, respectively, with chlorine dosing before PAC.

Radioactive cesium

were effectively removed by coagulation at both a water purification plant and in

134

Cs and

Powdered activated carbon

laboratory-scale experiments when turbidity was relatively high. In contrast,

Chlorination

137

Coagulation

134

Water purification process

137

Cs

134

Cs and

Cs in pond water with low turbidity were not removed by coagulation. This was because
Cs and 137Cs in river water were present mainly in particulate form, while in pond water

they were present mainly as cesium ions (134Cs and 137Cs). However, the removal of 134Cs
and

137

Cs in pond water by coagulation increased markedly when

134

Cs and

137

Cs were

mixed with sediment 24 h before coagulation.

2012 Elsevier Ltd. All rights reserved.

1.

Introduction

Several groups have investigated the occurrence of 131I,

Cs, and 137Cs at water purification plants (Goossens et al.,
1989; Esumi et al., 1986; Gafvert et al., 2002; Kamata et al.,
1973) although data after nuclear accidents were limited. It
was considered that radionuclides existed in particulate and
dissolved forms in environmental water considering their
forms in the air released after nuclear power plant accidents
(Noguchi and Murata, 1988). They may also exist in colloidal
form. Dissolved 131I is separated into various forms, such as
radioactive iodide ion (131I), iodine molecule (131I2), hypo131
I. The
iodous acid (HO131I), iodate ion (131 IO
3 ), and organic
134

The Great East Japan Earthquake occurred on 11 March 2011,

and caused an explosion at the Tokyo Electric Power Company
(TEPCO) Fukushima Daiichi Nuclear Power Plant, which
resulted in the release of large amounts of radionuclides into
the environment (Water Supply Division (WSD), Health
Service Bureau (HSB), Ministry of Health, Labour, and Welfare
(MHLW), 2011). Radioactive iodine (131I) and cesium (134Cs and
137
Cs) were detected in drinking water after the explosion
(WSD, HSB, MHLW, 2011; Ikemoto and Magara, 2011).

* Corresponding author. Tel.: 81 48 458 6306; fax: 81 48 458 6305.

E-mail address: kosaka@niph.go.jp (K. Kosaka).
0043-1354/$ e see front matter 2012 Elsevier Ltd. All rights reserved.
10.1016/j.watres.2012.05.055

4398

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

proportions of the forms of 131I were considered to be different

among environmental waters and to change due to reactions
in the environmental water. For example, 131I slowly transforms into 131 IO
3 in environmental water under the action of
sunlight (Lettinga, 1972). 131I2 and HO131I react with natural
organic matter (NOM) in the environmental water. Thus, it
was assumed that 131I removal at water purification plants
would depend on the environmental water. Information
regarding the occurrence of radionuclides at water purification plants is valuable. However, their levels in the environmental water are usually very low, and thus such data are
limited.
There have also been experimental investigations of 131I,
134
Cs, and 137Cs removal by water purification processes, such
as coagulation and powdered activated carbon (PAC) (Morton
and Straub, 1955; Lettinga, 1972; Brown et al., 2008a, b).
Brown et al. (2008a and 2008b) evaluated the treatability of
radionuclides by each unit process applied to water purification plants based on data obtained from the literature. These
data are useful, but in many cases the experiments were
performed using only certain forms of radionuclide; e.g., 131I
and radioactive cesium ion (134Cs and 137Cs). As described
above, radionuclides seem to exist in particulate and dissolved forms in environmental water. Thus, the removal of
131
I, 134Cs, and 137Cs from environmental water may occasionally be different from those of 131I, 134Cs, and 137Cs,
respectively. It was reported that 131I removal by PAC was
low (Lettinga, 1972); however, some other forms of 131I (e.g.,
organic 131I) were removed by PAC (Summers et al., 1988). In
addition, it was reported that ionic forms of 137Cs-radioactive
barium (137Ba) were not removed by coagulation (Morton and
Straub, 1955). However, Cs is known to be sorbed by soils
and minerals (Cornell, 1993; Staunton, 1994). Thus, it was
considered that particles of 134Cs and 137Cs could be removed
by coagulation. In fact, it was reported that removal of ionic
forms of 137Cse137Ba by coagulation was increased in the
presence of clay (Morton and Straub, 1955). As in the case
regarding the occurrence of radionuclides at water purification plants, only limited experimental data obtained using
environmental water containing radionuclides are available.
In the present study, we investigated the removal of 131I,
134
Cs, and 137Cs at water purification plants after the explosion
at a nuclear power plant caused by the Great East Japan
Earthquake. We also investigated 131I removal by PAC and
removal of 134Cs and 137Cs by coagulation taking their forms in
environmental water into consideration.

2.

Material and methods

2.1.

Reagents and solutions

The reagents and solutions used are described in Supplementary Materials. Three types of PAC (PAC-1 to PAC-3) were
used in the present study.

2.2.

Sampling

Raw, process, and finished water samples at five water purification plants (WPP-1 to WPP-5) were collected in April 2011.

The details of these water purification plants and sampling

procedures are described in Supplementary Materials. In
cases where levels of 131I, 134Cs, and 137Cs levels in raw water
were higher than 1 Bq/L, the data were used for analysis. Pond
water was also collected from Iitate Village in Fukushima
Prefecture on 7 May 2011. Water quality data of raw waters of
WPP-1 to WPP-5 and pond water are listed in Table S1. Granular activated carbon (GAC) and sand from the rapid sand filter
at WPP-1 were collected from April to September 2011. The
GAC was that at depths of up to 5 cm from the surface.
Moreover, sediments were collected from the Yodo and Ara
Rivers, and were designated as sediments A and B,
respectively.

2.3.

Removal test of radioactive iodine and cesium

Removal of 131I in river and pond waters by PACs was investigated. To investigate the form of 131I, its removal by silver ion
(Ag) was also performed. Removal of 134Cs and 137Cs in river
and pond waters by coagulation with polyaluminum chloride
(PACl) was investigated. Removal of 134Cs and 137Cs in pond
waters by PAC (PAC-1) and cation exchange resin was also
investigated. The procedures of the removal tests of 131I, 134Cs,
and 137Cs are described in Supplementary Materials.

2.4.

Analytical methods

Gamma-emitting radionuclides (131I, 134Cs, and 137Cs) in the

samples were determined using high-purity germanium
semiconductor detectors (GX2518; Canberra Co., Meriden, CT
and EGPC20-190-R; EURYSIS Co., Cedex, France). In the case of
occurrence of radionuclides at water purification plants, their
levels were expressed as those on sampling days and time
using their half-lives. In the radionuclide removal experiments, their levels on each experimental day were used. Other
analytical methods are described in Supplementary Materials.

3.

Results and discussion

3.1.
Levels of radioactive iodine and cesium in drinking
water after explosion at a nuclear power plant
After the explosion at a nuclear power plant, the levels of 131I,
134
Cs, and 137Cs in drinking water have been investigated at
Fukushima Prefecture and its 10 neighboring prefectures
(Fig. S1) (Ikemoto and Magara, 2011). Figure S3 shows the
results of monitoring of 131I in drinking water at Fukushima
Prefecture and its 10 neighboring prefectures in March to May
2011 (WSD, HSB, MHLW, 2011; Asami and Akiba, 2011). During
the monitoring, results indicating > 100 Bq/kg of 131I in
drinking water were only reported in March 2011. 131I in
drinking water exceeded 300 Bq/kg and drinking water for the
general public was restricted at 1 water utility in Iitate Village,
Fukushima Prefecture (maximum, 965 Bq/kg). 131I in drinking
water exceeded 100 Bq/kg and drinking water for infants was
restricted at 20 water utilities in 5 prefectures (Fukushima,
Ibaragi, Tochigi, and Chiba Prefectures, and Tokyo Metropolitan Government) (WSD, HSB, MHLW, 2011). Figure S4 shows
the profiles of 131I in tap water in Iitate Village, Fukushima

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

Prefecture, and in finished water at a water purification plant

in Tokyo Metropolitan Government (WSD, HSB, MHLW, 2011).
The initially high levels of 131I in drinking water were shown to
have dropped considerably.
Figure S5 shows the results of monitoring of the sum of
134
Cs and 137Cs in drinking water in Fukushima Prefecture and
its 10 neighboring prefectures from March 2011 to January
2012 (WSD, HSB, MHLW, 2012). The maximum of the sum of
134
Cs and 137Cs was 180.5 Bq/kg in tap water in Tamura City,
Fukushima Prefecture, which was lower than 200 Bq/kg, an
index of restriction of drinking water for the general public.
Figure S6 shows the profiles of the sum of 134Cs and 137Cs in
tap water in Iitate Village, Fukushima Prefecture (WSD, HSB,
MHLW, 2011). The trend of the sum of 134Cs and 137Cs was
different from that of 131I.
Compared to the data of radionuclides in drinking water,
those in raw water were limited and therefore their introduction is not described here. One reason for this was that the
number of inspection institutes with monitoring instruments
was small just after the nuclear power plant accident and it
was difficult to monitor the levels of radionuclides in samples
other than drinking water. Similarly, in the present study,
samples with high levels of radionuclides could not be
collected because of the confusion immediately following the
accident.

3.2.
Removal of radioactive iodine at water purification
plants
Fig. 1 and Fig. S7 show the profiles of 131I at WPP-1 and WPP-2
to WPP-5, respectively. As shown in Fig. S2 and Table S1, their
treatment flows and sampling days were different. 131I
removal by unit purification processes was evaluated based
on the results of WPP-1 to WPP-5.

3.2.1.

Coagulation

Fig. 1 shows the profiles of 131I at WPP-1. 131I level in raw water
was 2.9 Bq/L and that in rapid sand filtration was 2.8 Bq/L. At
WPP-2, 131I levels in raw water and sand filtration on 20 April
were 5.4 and 5.7 Bq/L, respectively (Fig. S7(a)). Thus, 131I was
not removed by coagulationeflocculationesedimentation. A
similar tendency was also seen at WPP-2 on 28 April. In

6.0

131I

(Bq/L)

4.0

4399

addition, 131I in raw water at WPP-1 and WPP-2 was considered to be present not in particulate form but in dissolved
form.

3.2.2.

Activated carbon treatment

GAC treatment is applied at WPP-1. 131I levels before and after

GAC treatment were 2.8 and 1.9 Bq/L, respectively, and
therefore 34% of 131I was removed (Fig. 1). 131I was detected in
GAC at 1500 Bq/kg on 22 April and at 94 Bq/kg wet weight on 30
May (Table S2). These results supported the removal of 131I by
GAC. Biological activated carbon (BAC) treatment followed by
rapid sand filtration is applied at WPP-2 (Fig. S2). The removal
percentages of 131I on 20 and 28 April were 4% and >39%,
respectively, and were different between sampling days. The
results on 20 April may be more reliable because 131I levels on
28 April were lower. However, on 28 April, 131I was not
detected either after BAC treatment or rapid sand filtration
although 131I levels were similar in other samples. Thus, the
treatability of 131I by BAC was not clarified in the present
study. If 131I was removed by BAC to some degree, some 131I
was considered to exist in forms that could be better adsorbed
by AC or biologically removed, such as organic 131I.
PAC treatment was applied at WPP-3 to WPP-5 during the
study (Fig. S2). 131I levels in raw water at WPP-3 to WPP-5 were
1.0e2.9, 1.5, and 1.5 Bq/L, respectively (Fig. S7). PAC concentrations at WPP-3 to WPP-5 were 5, 20, and 30 mg dry/L,
respectively. From the results between raw water and rapid
sand filtration, the removal percentages of 131I at WPP-3 to
WPP-5 were 0% e >27%, 13%, and 39%, respectively. It was
notable that the removal percentage of 131I at WPP-3 on 5 April
was regarded as 0%. From the results at WPP-1 to WPP-5, it
was considered that 131I was removed by GAC and PAC
ranging from about 30% to 40%, although 131I was not removed
in some cases.
It was reported that 131I removal by PAC was low and
increased by a combination of chlorination and PAC (Lettinga,
1972). On the other hand, in the case of 131I-containing water,
it was reported that the removal percentages of 131I in raw
water and process water after sand filtration by PAC (30 mg/L)
were 100% and 39%, respectively, and that in rain water by
PAC (50 mg/L) was 37% (Honma et al., 1988). Prechlorination
was applied at the water purification plant. It was notable that
in this report reference data were used as the results for raw
water because 131I level in raw water was below the limit of
quantification. In the present study, prechlorination was
applied at WPP-1 and WPP-4 on the sampling days. Therefore,
similar to the previous study by Honma et al. (1988), it was
considered that 131I was partially removed by AC (i.e., PAC or
BAC) without prechlorination at WPP-2, WPP-3, and WPP-5.
This was presumed to be because not only 131I but also
other forms of 131I were present in raw water. No clear effects
of prechlorination were observed in the present study.

2.0

3.2.3.

0.0
Raw water

Sedimentation

Fig. 1 e Profiles of

131

Rapid sand
f iltration

I at WPP-1.

GAC

Slow sand filtration

Slow sand filtration is applied at WPP-2 (Fig. S2). The removal

percentages of 131I by slow sand filtration on 20 and 28 April
were 67% and 3%, respectively. The removal efficiencies of 131I
were significantly different between sampling days. On 20
April, 131I level dropped after slow sand filtration. Therefore,
131
I may be removed by slow sand filtration; however, the

4400

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

results were not conclusive in the present study. If 131I was

removed by slow sand filtration, it was considered that some
131
I existed in forms that could be biologically removed, such
as organic 131I.

3.3.

Removal test of radioactive iodine

Fig. 2 shows removal percentages of 131I in river and pond

waters by PAC (PAC-1 was used). 131I levels in river and pond
waters before treatment were 3.4e3.5 and 7.4e9.5 Bq/L,
respectively. Reaction time was 30 min. Removal percentages
of 131I in river water at 2.5, 5, 10, 25, and 50 mg dry/L of PAC
were 11%, 11%, 9%, 36%, and 71%, respectively. Those in pond
water at 10 and 25 mg dry/L of PAC were 13% and 41%,
respectively. It was reported that the removal percentages of
131 
I by 1000 mg/L of PAC were 4.1%e6.1% at pH 8.5 (contact
time, 30 min) (Lettinga, 1972). Thus, the removal efficiency of
131
I by PAC in the present study was higher than that of 131I in
previous studies.
The environmental water associated with the explosion at
a nuclear power plant was considered to contain various
forms of 131I, including 131I and various types of organic 131I. It
was reported that the removal percentage of radioactive
131
I forms detected in
iodomethane (CH131
3 I), one of the organic
air after the accident at the Chernobyl nuclear power plant
(Noguchi and Murata, 1988), in humic substance solution
(5.98 mg C/L, pH 6.5) by 100 mg/L of AC with a reaction time of
2 days was 92% (Summers et al., 1988). Thus, the differences in
results between the present study and that of Lettinga (1972)
were considered to be at least partly due to differences in
the form of 131I. This agreed with the results presented in the
previous section.
To estimate the proportions of 131I to total 131I, the
removal of 131I in pond waters by Ag was investigated after
acidification of the samples (Fig. S8). The removal percentages
of 131I by 0.5 and 1.0 g/L were 34% and 28%, respectively. Ag is
known to react with halide ions, such as chloride, bromide,
and iodide ions, with resultant deposition of silver halides.

Removal percentage of 131I %

100
River (PAC)
River (Cl2 + PAC)
Pond (PAC)
Pond (Cl2 + PAC)

80

60

40

20

0
0

10

20
30
PAC (mg-dry/L

40

50

Fig. 2 e 131I removal in river and pond waters by PAC (131I

in river water, 3.4e3.5 Bq/L; 131I in pond water, 7.4e9.5 Bq/
L; PAC, PAC-1; reaction time of PAC, 30 min).

Thus, it was considered that the proportion of 131I was

around 30% under the assumption that among the 131I species
only 131I was removed by Ag. This result supported the
presence of various forms of 131I in environmental water.
The effects of chlorination on the removal percentages of
131
I by PAC were investigated (Fig. 2). The order of treatment
was chlorination for 10 min followed by PAC for 30 min. Free
chlorine concentration in river and pond waters after 10 min
of chlorination was around 0.10e0.15 mg/L. Removal
percentages of 131I in river water at 10, 25, and 50 mg dry/L of
PAC were 41%, 59%, and 71%, respectively. Those in pond
water at 5, 10, 25, and 50 mg dry/L of PAC were 20%, 33%, 48%,
and 62%, respectively. Fig. S9 also shows the effects of chlorination on the removal percentages of 131I in pond water by
PACs (PAC-1, PAC-2, and PAC-3). PAC concentration was 25 mg
dry/L and other reaction conditions were the same as those in
Fig. 2. Removal percentages of 131I by PAC-1, PAC-2, and PAC-3
without chlorination were 43%, 11%, and 21%, respectively.
Those with chlorination were 48%, 27%, and 36%, respectively.
These results indicated that 131I removal by PAC increased
with chlorination, while the effects of chlorination were
higher at lower PAC concentration or lower removal by PAC
only.
Lettinga (1972) reported that 131I removal by PAC
increased with chlorine dosing before PAC treatment. The
tendency in this previous study agreed with our results
presented here. In addition, Summers et al. (1988) reported
that the removal percentage of 131I in river water by 100 mg/L
AC at a reaction time of 2 days was 57% when 131I was used
as 131I and 1 mg/L of chlorine was initially added. Addition of
chlorine simulated prechlorination in the actual purification
process. I reacts rapidly with chlorine and transforms
mainly into HOI at neutral pH (Lettinga, 1972; Bichsel and von
Gunten, 1999). The sorption capacities of HO131I and 131I2
with AC were reported to be higher than that of 131I by 15 et al., 1996). In addition, it
and 60-fold, respectively (Mandic
was also reported that I or organic I was formed when HOI
reacted with NOM in environmental water (Bichsel and von
Gunten, 1999). It was presumed that removal of organic 131I
by PAC was higher than 131I as in the case of CH131
3 I
(Summers et al., 1988). Therefore, it was considered that
a combination of chlorination and PAC was effective for 131I
removal among 131I species because of the formation of
HO131I. 131I removal in river water by PAC only was lower
than that in pond water (Fig. 2). However, 131I removal in river
water by combination of chlorination and PAC was higher
than that in pond water. Thus, it was presumed that the
proportion of 131I in river water was greater than that in
pond water.
HOI transformed by chlorination of I is further transformed into IO
3 by reaction with chlorine (Lettinga, 1972;
Bichsel and von Gunten, 1999). The transformation yield of
IO
3 depends on chlorination conditions, such as pH, chlorine
concentration, and reaction time. It was reported that the
distribution coefficients of 131 IO
3 for active charcoal at pH 6e8
were lower than those of 131I by one or two orders of
magnitude (Ikeda and Tanaka, 1975). Lettinga (1972) reported
that 131I removal decreased by combination of chlorination
and PAC when chlorination reaction time was longer or
chlorine concentration was much higher. Fig. S10 shows the

4401

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

effects of chlorination conditions on 131I removal in pond

waters by PAC (PAC-1). In the case of chlorination followed by
PAC, the removal percentages of 131I at chlorination reaction
times of 30 s and 10 min were 32% and 33%, respectively. In the
case of PAC followed by chlorination, the value was 33%. That
is, 131I removal by the combination of chlorination and PAC
was unaffected by chlorination conditions. Therefore, it was
considered that in the present study, chlorine concentration
was not excessive and the transformation of 131I into 131 IO
3
was small.
Fig. S11 shows the effects of reaction time of PAC on the
removal of 131I in pond water by combination of chlorination
and PAC (PAC-1). The reaction times were 5, 10, and 30 min 131I
levels in pond water before treatment were 7.4e9.5 Bq/L. PAC
concentration was 25 mg dry/L and chlorination reaction time
was 10 min. The removal percentages of 131I at reaction times
of 5, 10, and 30 min with PAC were 36%, 48%, and 48%,
respectively. That is, the removal percentages at reaction
times of 10 and 30 min were similar under the conditions used
in the present study.

3.4.
Removal of radioactive cesium at water purification
plants
Among the five water purification plants, the levels of 134Cs
and 137Cs at WPP-2 were sufficiently high to investigate their
removal during water purification processes. Fig. 3 shows the
profiles of 134Cs and 137Cs at WPP-2. On 20 April, 134Cs and
137
Cs levels in raw water were 2.5 and 3.0 Bq/L, respectively.
Those on 28 April were 5.6 and 6.4 Bq/L, respectively. Although
low levels of 137Cs and 134Cs were detected after sand filtration
and BAC, respectively, on 20 April, 134Cs and 137Cs were not
detected in other process water samples on 20 or 28 April.
Turbidities in raw water on 20 and 28 April were 15 and
51 degrees, respectively. The proportions of 134Cs and 137Cs
particles in raw water on 28 April were 86% and 87%, respectively (details are presented in the next section). These results
suggested that 134Cs and 137Cs at WPP-2 existed mainly as
particles, and they were therefore effectively removed by
coagulationeflocculationesedimentation.

It was reported that 134Cs and 137Cs were detected in

sludge from water purification plants in Fukushima and its
neighboring prefectures after the explosion at the nuclear
power plant (WSD, HSB, MHLW, 2012). These observations
suggested that particles of 134Cs and 137Cs were removed
during coagulationeflocculationesedimentation. On the
other hand, 134Cs and 137Cs were occasionally detected in
drinking water after the explosion (WSD, HSB, MHLW, 2011).
As 134Cs and 137Cs (ionic form of 137Cse137Ba) were not
removed by coagulation in laboratory-scale experiments
(Morton and Straub, 1955), this was presumed to be because
particles were not sufficiently removed during water purification processes or the proportions of dissolved forms of
134
Cs and 137Cs (e.g., 134Cs and 137Cs) were high. It was
reported that removal efficiency of 137Cs was low during
coagulationeflocculationesedimentation followed by rapid
and slow sand filtration when the turbidity in raw water was
0.80 FNU (Gafvert et al., 2002). At a pilot-scale, the maximum
134
Cs
by
coagulationeremoval
percentages
of
flocculationesedimentation and filtration were 31% and 56%,
respectively (Goossens et al., 1989). These reports also suggested that the proportions of particulate and dissolved
forms of 134Cs and 137Cs were dependent on environmental
water.
Although 134Cs and 137Cs were not detected in raw or
process water at WPP-1 in the present study, they were
detected in some samples of GAC and sand (Table S2). In the
case of GAC, 134Cs and 137Cs on 22 April were 7.4 and 13 Bq/kg
wet, respectively. It was reported that removal of ionic forms
of 137Cse137Ba by AC was low (Rivera-Utrilla et al., 1984). Thus,
the reason for the detection of 134Cs and 137Cs in GAC was
presumed to be because flocks containing 134Cs and 137Cs
passing the sand filter were captured at GAC. In the case of
sand, 134Cs and 137Cs on 31 May were 40 and 51 Bq/kg wet,
respectively. Those on 25 August were 13 and 11 Bq/kg wet,
respectively. One reason for the detection of 134Cs and 137Cs in
sand was presumed to be because flocks containing 134Cs and
137
Cs passing the sedimentation tank were captured at the
rapid sand filters. It was reported that 137Cs in pure water was
removed by sand filters despite the low ion exchange

15
137Cs

137Cs and 137Cs

(Bq/L)

12

134Cs

< 0.83 < 0.59

< 0.76 < 0.67 < 0.58 < 0.65 < 0.63
< 0.57 < 0.60 < 0.69
< 0.50 < 1.0 < 0.47 < 0.58

0
20 Apr.

28 Apr. 20 Apr.

Raw water

28 Apr. 20 Apr.

Sedimentation

Fig. 3 e Profiles of

28 Apr.

BAC

134

Cs and

20 Apr.

28 Apr.

Rapid sand
f iltration
137

Cs at WPP-2.

20 Apr.

28 Apr.

Slow sand
f iltration

4402

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

capacities (Ohshio, 1960). The average removal percentages of

137
Cs by 13 types of sand filter were from 47.7% to 99.7% when
the ratio of passing water volume to sand filter volume was 15.
In this previous study, the sand was prepared for rapid/slow
sand filters at water purification plants or already used at
water purification plants. As shown in the next section, some
proportions of 134Cs and 137Cs existed as 134Cs and 137Cs,
respectively, in river and pond waters, although the proportions of 134Cs and 137Cs were very different between the
environmental waters. Thus, another possibility for the
detection of 134Cs and 137Cs in sand was that 134Cs and 137Cs
were removed by the ion exchange ability of sand and were
accumulated although their levels in process water were low.

3.5.

Removal test of radioactive cesium

Fig. 4 shows the removal percentages of 134Cs and 137Cs in river

and pond waters by coagulation. 134Cs and 137Cs levels in river
water were 5.6 and 6.4 Bq/L, respectively. 134Cs and 137Cs levels
in pond water were 9.8 and 11 Bq/L, respectively. Turbidities in
river and pond waters were 51 and 0.3 degrees, respectively. In
the case of river water, removal percentages of 134Cs and 137Cs
were 94% and 95%, respectively. In the case of pond water,
removal percentages of 134Cs and 137Cs were 5% and 6%,
respectively. In addition, the removal percentages of 134Cs and
137
Cs in river waters by filtration only were 86% and 87%,
respectively, and those in pond waters were 0%. These results
showed that 134Cs and 137Cs in river water were present mainly
in particulate form, and were therefore effectively removed by
coagulation. These results supported those shown in Fig. 3. On
the other hand, 134Cs and 137Cs in pond water were present
mainly in dissolved form, and therefore were not removed by
coagulation. In addition, the removal percentages of 134Cs by
coagulation in both river and pond waters were similar to those
of 137Cs. Thus, it was considered that the proportions of the
forms of 134Cs and 137Cs in both river and pond waters were
similar. Moreover, in both the river and pond waters, the
removal percentages of 134Cs and 137Cs by coagulation were
slightly higher than those by filtration. In the present study, it

was operationally defined that components passing 0.5-mm

filters were in the dissolved form. Thus, it was presumed that
some percentages of 134Cs and 137Cs may be sorbed onto small
particles <0.5 mm in diameter, and such 134Cs and 137Cs were
removed by coagulation with these small particles. Alternatively, some percentages of 134Cs and 137Cs may have been
present in dissolved form, which could be removed by coagulation (e.g., colloids).
To investigate the types of dissolved forms of 134Cs and
137
Cs in pond water, we examined their removal by PAC and
cation exchange resin (Fig. S12). Removal percentages of 134Cs
and 137Cs by cation exchange resin were 95% and 92%,
respectively. On the other hand, removal percentages of 134Cs
and 137Cs by PAC were 7% and 0%, respectively. It was reported
that cation exchange resin showed strong activity for removal
of the ionic form of 137Cse137Ba (Morton and Straub, 1955). It
was also reported that the removal levels of the ionic form of
137
Cse137Ba by AC (Rivera-Utrilla et al., 1984) and coagulation
were low (Morton and Straub, 1955). These results showed
that 134Cs and 137Cs in pond water exist mainly as Cs.
Moreover, the sample of river water after coagulation was
further treated by cation-exchange resin. 134Cs and 137Cs were
not detected in the sample after cation-exchange (data not
shown). Thus, it was presumed that the forms of 134Cs and
137
Cs remaining after coagulation in the river water were
134
Cs and 137Cs, respectively.
The effects of suspended solids on the removal of 134Cs and
137
Cs in pond water by coagulation were investigated. As
suspended solids, sediment A or B was initially added to pond
water and mixed at 24 h. Subsequently, coagulation of the
sample was performed. When the amounts of sediment A
added were 0, 5, 10, and 30 degrees as turbidity, the removal
percentages of 134Cs were 5%, 56%, 67%, and 92%, respectively
(Fig. 5). Those of 137Cs were 6%, 60%, 73%, and 91%, respectively. When the amounts of sediment B added were 10
degrees as turbidity, the removal percentages of 134Cs and
137
Cs were 94% and 90%, respectively. These results indicated
that removal of 134Cs and 137Cs by coagulation increased with

Removal percentages of 134Cs and 137Cs (%)

80

134Cs
137Cs

60

40

20

0
Filtration (River)

Coagulation (River)
134

137

Filtration (Pond)

Coagulation (Pond)

Fig. 4 e Removal of
Cs and
Cs in river and pond
waters by filtration and coagulation (134Cs, 137Cs in river
water, 5.6 and 6.4 Bq/L; 134Cs, 137Cs in pond water, 9.8 and
11 Bq/L; turbidity in river and pond water, 51 and 0.3
degrees).

Removal percentages of 134Cs and 137Cs (%)

100
100

80

60

40
134Cs (Sediment A)
134Cs (Sediment B)
137Cs (Sediment A)
137Cs (Sediment B)

20

0
0

10

20

30

Turbidity

Fig. 5 e Effects of suspended solids on removal of 134Cs and

137
Cs in pond water by coagulation (134Cs and 137Cs, 9.8 and
11 Bq/L; turbidity in pond water, 0.3 degrees).

w a t e r r e s e a r c h 4 6 ( 2 0 1 2 ) 4 3 9 7 e4 4 0 4

the addition of sediment. Cs is known to be sorbed by soils

and minerals (Cornell, 1993; Staunton, 1994). Thus, in the
present study it was considered that 134Cs and 137Cs in pond
water were sorbed on the sediments within 24 h of contact and
were removed by coagulation with sediments. Results similar
to those of the experiments using 137Cs (or ionic forms of
137
Cse137Ba) were reported previously (Morton and Straub,
1955; Kobayashi et al., 1969). However, the degree of increase
in removal of 134Cs and 137Cs by addition of suspended solids
was higher in the present study than in these previous studies.
That is, in the study by Morton and Straub (1955), the removal
percentages of ionic forms of 137Cse137Ba by coagulation in the
absence and presence of clay (100 mg/L) were 0%e6% and
35%e65%, respectively. In the study of Kobayashi et al. (1969),
the removal percentages of 137Cs in river water (turbidity, 10
degrees) by coagulation were 10.9%e31.0% and those after
addition of sediments to 95 degrees as turbidity were 71%e
76%. The reaction times of 137Cs (or ionic forms of
137
Cse137Ba) with suspended solids before coagulation were
not described in either of these previous reports. Thus, it was
presumed that the degree of improvement in the removal of
134
Cs and 137Cs by addition of suspended solids was dependent
on the types of suspended solids and experimental conditions.

4.

Conclusions

From the occurrence of 131I at water purification plants, it was

shown that 131I was not removed by coagulationeflocculationesedimentation. The removal of 131I by GAC and
PAC ranged from 30% to 40%, although 131I was not removed in
some cases.
Laboratory-scale experiments indicated that the removal
percentages of 131I in river and pond waters by 25 mg dry/L of
PAC (PAC-1) were 36% and 41%, respectively. These levels
were increased by the combination of chlorination and PAC
(59% for river water and 48% for pond water).
The occurrence of 134Cs and 137Cs at water purification
plants indicated that they were effectively removed by coagulationeflocculationesedimentation when turbidity in raw
water was relatively high.
The results of laboratory-scale experiments showed that
134
Cs and 137Cs in river water with relatively high turbidity (51
degrees) were removed by coagulation, but those in pond
water with low turbidity (0.3 degrees) were not. The proportions of particulate and dissolved forms of 134Cs and 137Cs
were high in river and pond waters, respectively. The removal
of 134Cs and 137Cs in pond water by coagulation increased
markedly when 134Cs and 137Cs were mixed with sediment at
24 h before coagulation.

Acknowledgments
The authors thank Mr. Masami Oya, Mr. Yasuo Tanaka, Mr.
Nobuaki Munakata, and Mr. Yusei Kobayashi (Hanshin Water
Authority, Japan) for their help with the experiments. The
authors also thank the officials of water utilities for sample
collection.

4403

Appendix A. Supplementary material

Supplementary data related to this article can be found online
at doi:10.1016/j.watres.2012.05.055.

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