Chemosphere 264 (2021) 128457

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Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

Deposition of Fukushima nuclear power plant accident-derived

radiocesium in the soils of Jeju Island, Korea, and evidence for long-
and short-lived radionuclides in rainwater
Tae-Woo Kang a, *, Young-Un Han a, Eun Hye Na a, Bon-Jun Koo b, Won-Pyo Park c, **
a
Yeongsan River Environment Research Center, National Institute of Environmental Research, Gwangju, 61011, Republic of Korea
b
Department of Biological Sciences, California Baptist University, Riverside, CA, 92504-3297, USA
c
Major of Plant Resources and Environment, Jeju National University, Jeju, 63243, Republic of Korea

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

Post-Fukushima soil and wet/dry

deposition samples were collected
from Jeju Island.

Fukushima-derived radionuclides
were detected in the collected
samples.

Total radiocesium inventories were
affected by a plume that covered the
Jeju Island.

FNPPA-derived 134Cs present in trace
amounts in only the topsoil. .

Short-lived radionuclides in rain-
water indicate direct inflow from
Fukushima.

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

Article history: In this study, we investigated the concentrations of Fukushima nuclear power plant accident (FNPPA)-
Received 10 July 2020 derived radiocesium (134Cs, 137Cs) deposited in the topsoil of Jeju Island, Korea. We also evaluated the soil
Received in revised form inventories of radionuclides and compared the concentrations deposited by rainwater and fallout. We
24 September 2020
present the first evidence of FNPPA-derived radionuclides directly entering the environment of Jeju Is-
Accepted 27 September 2020
land. In the case of FNPPA-derived 134Cs in soil, only a trace amount was identified in the surface layer
Available online 30 September 2020
(1 cm depth), whereas 137Cs derived from past atmospheric deposition of nuclear testing were detected
Handling Editor: Martine Leermakers along with those derived from the nuclear power plant accident. The total measured radiocesium
(134Cs þ 137Cs) indicates that although the value obtained from soils was slightly lower, both values were
Keywords: within the same order of magnitude. Of the FNPPA-derived radiocesium deposited in the soil, the impact
Fukushima nuclear power plant accident from April 2011 was the largest at most sampling sites indicating that the radioactive plume directly
Radiocesium covered Jeju Island. Furthermore, a variety of long- and short-lived gamma-emitting radionuclides were
134
Cs detected in the rainwater samples collected on April 7, 2011. Among them, short-lived radionuclides such
Short-lived radionuclides
as 140La, 110mAg, 95Nb, 125Sb, 113Sn, 129Te, 129mTe, 132Te, 132I, and 136Cs, were observed. The findings of this
Surface soil
study provide evidence for the direct effects of FNPPA-derived radionuclides in Jeju Island. This is the first
Jeju island

Abbreviations: ACS, acrylic cylinder sampler; CS, core sampling; DSS, direct surface sampling; FNPPA, Fukushima nuclear power plant accident; HPGe, high purity
Germanium; KINS, Korea Institute of Nuclear Safety; MDA, minimum detectable activity; MP, Nationwide Environmental Radioactivity Monitoring Post; SSS, stainless-steel
sampler; NISA, Nuclear and Industrial Safety Agency.
* Corresponding author.
** Corresponding author.
E-mail addresses: kangtw@korea.kr (T.-W. Kang), oneticket@jejunu.ac.kr (W.-P. Park).

https://doi.org/10.1016/j.chemosphere.2020.128457
0045-6535/© 2020 Elsevier Ltd. All rights reserved.
T.-W. Kang, Y.-U. Han, E.H. Na et al.
location in Korea and the first in the entire East Asian region, excluding Japan that is confirmed to have
been directly affected FNPP accident.
1. Introduction
The Fukushima nuclear power plant accident (FNPPA) occurred
in the northeastern region of Japan on March 11, 2011, when a
magnitude 9.0 earthquake caused a massive tsunami that affected
the adjacent Fukushima Dai-ichi nuclear power plant. This led to
the release of a large amount of radionuclides into the environment
and their subsequent spread worldwide. According to the Nuclear
and Industrial Safety Agency (NISA) of Japan, from March 11e16,
2011, 131I (half-life of 8.02 days), 134Cs (half-life of 2.07 years), and
137
Cs (half-life of 30.2 years) radionuclides were released into the
atmosphere in amounts of approximately 1.6  1017 Bq, 1.8  1016
Bq, and 1.5  1016 Bq, respectively (NISA, 2011). Prior studies have
reported that this level of exposure is ~10e15% of that released
during the Chernobyl nuclear accident (Hamada et al., 2012;
Steinhauser et al., 2014; Ten Hoeve and Jacobson, 2012; Winiarek
et al., 2012).
Radionuclides released into the atmosphere by the FNPPA were
transported across the Pacific, over the North American continent,
and as far as Europe and Asia, despite dispersion or washout
throughout the course of their transport by the prevailing west-
erlies. As a result, radionuclides such as 131I, 134Cs, and 137Cs were
first detected and reported after mid-March 2011 in aerosol sam-
ples from (in order) the United States, Europe, and Asia
(Bolsunovsky and Dementyev, 2011; Bowyer et al., 2011; Diaz et al.,
2011; Huh et al., 2012; Kim et al., 2012; Long et al., 2012; Lozano
et al., 2011; Manolopoulou et al., 2011; Masson et al., 2011;
Pittauerova
et al., 2011; Thakur et al., 2013; Tuo et al., 2013). In the
case of Korea (Kim et al., 2012), the FNPPA-derived 131I radionu-
clides were first detected in aerosol samples throughout the entire
country on March 28, 2011 during the nationwide environmental
radiation monitoring conducted by the Korea Institute of Nuclear
Safety (KINS). The activity concentrations of 131I, 134Cs, and 137Cs in
the aerosol samples were the highest in Gunsan (131I ¼ 3.12 mBq
m3) and Busan (134Cs ¼ 1.19 mBq m3; 137Cs ¼ 1.25 mBq m3) on
April 7, but were no longer detected after May 2011. Among the
aerosol samples collected in the Jeju region, the activity concen-
trations of 131I, 134Cs, and 137Cs were the highest on April 6
(131I ¼ 0.887 mBq m3) and April 7 (134Cs ¼ 0.541 mBq m3;
137
Cs ¼ 0.550 mBq m3). In particular, rainwater samples exhibited
their highest concentrations on April 7 (131I ¼ 2.81 Bq L1) and April
11 (134Cs ¼ 1.67 Bq L1; 137Cs ¼ 2.02 Bq L1). These activity con-
centrations were reported to be ~5 times higher than the detection
level for the entire Korean region (excluding the Busan region) (Kim
et al., 2012).
Korea, Taiwan, and the Fukuoka region of Japan, which are
located west of the Fukushima nuclear power plant, were subjected
to further exposure to 131I, 134Cs, and 137Cs radionuclides as the
radioactive plume was directly transported by monsoon winds
produced by the high pressure system that develops in the north-
east during early April. Modeling results from previous studies have
estimated that these radionuclides should be detected (Hong et al.,
2012; Huh et al., 2012; Lee et al., 2015, 2017; Momoshima et al.,
2012). For these reasons, it is estimated that Jeju Island has
received more radioactive materials than other regions due to
rainfall. However, apart from a few studies (Hao et al., 2013; Park
et al., 2013; Tsuboi et al., 2012), there have been no reports on
2
Chemosphere 264 (2021) 128457
© 2020 Elsevier Ltd. All rights reserved.
the presence of FNPPA-derived radiocesium in soils from the re-
gions located west of the Fukushima nuclear power plant. FNPPA-
derived radiocesium was measured in soils (10 cm depth) in the
northeastern region of Beijing, China; however, the results indi-
cated no detection of such radionuclides (Tuo et al., 2013). So far,
there has been no report on the detection of radionuclides from
environmental samples that serve as direct evidence of an FNPPA-
derived radioactive plume affecting the relevant regions.
Therefore, this study is the first to investigate FNPPA-derived
radionuclides in Jeju Island, located to the southwest of the
FNPPA site, by measuring the activity concentration of radiocesium
(134Cs, 137Cs) in soils. The amount of FNPPA-derived radiocesium
was assessed using comparative evaluations of wet and dry depo-
sition by rainwater and fallout, respectively, by calculating the
deposited inventories at the ground surface from these activity
concentrations. In this study, the first evidence for an FNPPA-
derived radioactive plume that flowed directly over Korea is pre-
sented using various long- and short-lived gamma-emitting ra-
dionuclides detected in rainwater samples from the Jeju region.
2. Materials and methods
2.1. Study area
Jeju Island (33 060 e34 000 N, 126 080 e126 580 E) is a volcanic
island located 1350 km southwest of the FNPPA site. The island
forms an elliptical shape with an area of 1847 km2, centered at Halla
mountain (1950 m a.s.l.) (Fig. 1a). The climate of the island is humid
and sub-tropical but mild in winter, with elevated precipitation
levels and a mean annual temperature of 15  C. The mean annual
precipitation on the island differs by region (east ¼ 1967 mm,
west ¼ 1143 mm, south ¼ 1923 mm, and north ¼ 1498 mm). The
soils of Jeju Island are volcanically derived, with basalt as the base
material, while some originated from trachytes and trachytic an-
desites (Shin and George, 1988; Song and Kang, 2019). Andisols,
which are volcanic ash soils, comprise 80% of the soils in Jeju island.
The western region, northern coastal region, and mid-mountain
region, as well as areas with less precipitation, contain non-
Andisol soils (Song and Kang, 2019).
2.2. Soil sampling and pre-treatment
Preliminary surveys were conducted at three sites (S1eS3) in
November 2011 to identify FNPPA-derived radiocesium (134Cs,
137
Cs) in the soil (Fig. 1a). During these surveys, the activity con-
centrations of radiocesium were comparatively assessed according
to the sampling method used at each sampling site. The sampling
methods used were core sampling (CS), which is used in bulk
density analyses of soils (Blake and Hartge, 1986), and direct surface
sampling (DSS) that is constrained to a certain area. In addition, at
site S2, the behavior of radiocesium according to soil depth was
investigated using an acrylic cylinder sampler (ACS). Following
these preliminary surveys, the FNPPA-derived radiocesium depos-
ited in the surface soil of Jeju Island was assessed using a stainless-
steel sampler (SSS) at five sites (S4eS8) in November 2012 (Fig. 1a).
Table 1 lists the geographic locations and sampling details for the
sampling sites used to assess radiocesium in the soil after the
T.-W. Kang, Y.-U. Han, E.H. Na et al. Chemosphere 264 (2021) 128457

Fig. 1. (a) Map showing the sampling sites for radiocesium measurements on Jeju Island, Korea after the FNPPA (B: soil samples, -: dry and wet deposition samples). MP:
nationwide environmental radiation monitoring post on Jeju Island. An asterisk in the box indicates the FNPPA located ~1350 km northeast of the study area. (b) Photographs of the
soil sampling methods used to measure radiocesium derived from the FNPPA (CS: core sampling, depth 5 cm, volume 100 cm3; DSS: direct surface sampling, depth 1 cm, area
50  50 cm; ACS: acrylic cylinder sampling, depth 25 cm; SSS: stainless-steel sampling, depth 2 cm, area 10  10 cm).

FNPPA.
Soil sampling was conducted as follows: Level sites without
artificial disturbance were selected and foreign matter, such as non-
decomposed leaves and gravels, were removed from the specified
areas. The soils were sampled using the DSS or CS method, and with
the ACS and SSS. For the DSS method, a 50  50 cm (2500 cm2) area
was specified and the uppermost 1 cm of topsoil was directly
sampled. For the CS method, a core sampler with a diameter of 5 cm
and a length of 5 cm (100 cm3) was used. Soil samples were
collected with five core samplers at each site and mixed in the field
(IAEA, 2019; Khomutinin et al., 2020). The ACS was 5 cm in diam-
eter and 25 cm in length, and the rectangular SSS was 10 cm in
width, 10 cm in length, and 2 cm in depth. All the samplers were
made by the authors of the study (Fig. 1b). The collected soil
samples were immediately sealed in plastic bags and transferred to
the laboratory, and were dried in a 105  C oven to calculate the bulk
density of each soil sample. The dried soil samples were passed
through a 2 mm sieve, crushed, and placed (approximately
50e80 g) into sample containers (U8 vial, 50 mm width, 70 mm
height, Japan, Mizuho Chemical Co.) for the radiocesium (134Cs,
137
Cs) analyses. To investigate the behavior of radiocesium ac-
cording to soil depth, the soil at each site was sampled with the four
acrylic cylinder samplers and then transferred to a laboratory. The
collected soil samples were carefully scraped and separated
sequentially from the upper layer at constant intervals (soil depth
0e5 cm, 1 cm interval; soil depth 5e25 cm, 2.5 cm interval). Then,
multiple core sample sections obtained at the same depth interval
were mixed to make a composite sample. These samples were pre-
treated as above and used for the analyses.
2.3. Sampling and pre-treatment of wet (rainwater) and dry
deposition
Samples of daily wet deposition (rainwater) and monthly wet
(rainwater) and dry deposition (fallout) were collected at the
Nationwide Environmental Radioactivity Monitoring Post (MP)
located on Jeju Island after the FNPPA (Fig. 1a). Daily wet deposition
samples were collected for two months from March to May 2011
following each occasion of rainfall. Monthly wet (rainwater) and
dry deposition samples were collected at monthly intervals for 10

Table 1
Geographical and sampling information for the sampling sites used to measure radiocesium in the soils of Jeju Island after the FNPPA.

Site Name Coordinates Altitude (m) Sampling date Sampling method

Latitude Longitude

S1 N 33 250 2300 E 126 370 2800 605 Nov 11, 2011 CSa, DSSb
S2 N 33 270 0100 E 126 460 0200 250 Nov 23, 2011 CS, DSS, ACSc
S3 N 33 230 5500 E 126 430 1300 352 Nov 11, 2011 CS, DSS
S4 N 33 260 0800 E 126 410 3200 402 Nov 15, 2012 SSSd
S5 N 33 210 4900 E 126 200 4300 382 Nov 14, 2012 SSS
S6 N 33 140 1300 E 126 180 4500 52 Nov 14, 2012 SSS
S7 N 33 250 2700 E 126 330 2300 570 Nov 16, 2012 SSS
S8 N 33 180 5100 E 126 340 3300 495 Nov 16, 2012 SSS
a
Core sampling (depth 2 cm, volume 100 cm3).
b
Direct surface sampling (depth 1 cm, area 50  50 cm).
c
Acrylic cylinder sampling (depth 25 cm).
d
Stainless-steel sampling (depth 2 cm, area 10  10 cm).

3
T.-W. Kang, Y.-U. Han, E.H. Na et al. Chemosphere 264 (2021) 128457

months from March to December 2011. The sampling device can

simultaneously collect both wet and dry deposition samples and is
composed of 2 sampling basins, each with an area of 1 m2
(1 m  1 m). A basin cover and a rainfall sensor are connected such
that the basin cover is automatically opened for each rainfall event.
The basin covers are designed so that only fallout samples are
collected from the dry deposition basin on days without rain, as the
fallout is usually located on top of the wet deposition basin. During
rainfall, the basin cover is automatically moved by a rain sensor, so
that only rainwater samples in the wet deposition basin are
collected. To keep the dry deposition basin from drying out,
distilled water was added to the basin and maintained at a 1 cm
depth.
For the daily wet deposition samples, 1 L or, if less than 1 L
accumulated, the total amount of the collected sample was trans-
ferred to a sample container (Marinelli beaker, 1 L) for direct ana-
lyses. The monthly dry deposition samples were collected by
rinsing the basin with distilled water to collect the fallout, the
whole volume was collected, and any foreign matter (leaves, in-
sects, etc.) was removed. The samples were then transferred to
Teflon-coated 100 L stainless steel bottles, underwent slow evap- Fig. 2. A typical gamma-ray spectrum of the soil samples collected from Jeju Island
oration and drying processes, and the resulting materials were after the FNPPA. The spectrum in the box indicates the radiocesium (134Cs, 604.7 keV
and 795.8 keV; 137Cs, 661.66 keV) measured from the soil sample.
pulverized to a powder state and placed into sample containers for
measurement (U8 vial, 50 mm width, 70 mm height). For the
monthly wet deposition samples, the whole volume of rainwater
with a gamma spectrometer. This was followed by software ana-
collected in the sampling basin after each rainfall event was
lyses (Aptec, Gennie, 2000) for energy calibration and to calculate
collected. These samples then underwent the same pre-treatment
the measurement efficiency.
process as the dry deposition samples.

2.4. Radioactivity measurements 3. Results and discussion

Radioactivity analyses were performed using a gamma spec- 3.1. Fukushima-derived radiocesium in soils
trometer comprised of a high purity germanium (HPGe) detector
(GEM-30185, Ortec, USA; GC 3020, Canberra, USA) and a multi- Table 2 shows the results of the preliminary surveys used to
channel analyzer (92X, Ortec, USA; DSA-1000, Canberra, USA). All identify FNPPA-derived radiocesium in Jeju Island soils. Table 2 also
samples, as well as the background radioactivity, were measured compares the activity concentrations of 134Cs and 137Cs in the soils
for 80,000 s each. The relative efficiencies, energy resolutions, and according to the collection method used. The preliminary survey
peak/Compton ratios were 31% and 34%, 1.69 keV and 1.74 keV, and findings indicate that the activity concentrations of 134Cs and 137Cs
65.0:1 and 62.1:1, respectively, for 60Co (1332 keV) for the two in the soils sampled using the CS method were below the MDA and
HPGe detectors used in the analyses. The measured spectrum was in a range of 25.7e128 Bq kg1, respectively. For the soils sampled
analyzed using the gamma-ray energies for 134Cs (604.7 keV) and using the DSS method, the activity concentrations were in the range
137
Cs (661.66 keV) by Aptec (Aptec Co.) and Gennie 2000 software of 2.04e11.8 Bq kg1 and 26.2e99.3 Bq kg1, respectively, indi-
(Canberra Co.) packages, respectively. Fig. 2 shows a typical cating that this sampling method produced samples in which both
gamma-ray spectrum for a soil sample, which confirms the pres- radionuclides were detected. Radionuclides of 134Cs (half-life of
ence of FNPPA-derived radiocesium (134Cs, 137Cs). The activity 2.06 y) and 137Cs (half-life of 30.17 y) are well-known fission
concentrations of all samples were determined by considering the products that are representative of artificial radionuclides released
radioactive decay according to the sampling and measurement by past atmospheric nuclear testing and nuclear power plant ac-
times. They were also corrected for coincidence summing and self- cidents (ICRP, 1978; UNSCEAR, 2000). Among these types of radi-
absorption from the 134Cs gamma-ray energy and the soil sample ocesium, 134Cs with its short half-life cannot be detected after an
density. The minimum detectable activity (MDA) values for 134Cs extended period due to the effect of radioactive decay, whereas
and 137Cs were 0.759 and 1.00 Bq kg1 (soil), 0.0687 and 0.0919 Bq 137
Cs can still be detected in Jeju soil due to its longer half-life,
L1 (daily wet deposition), 0.0209 and 0.0231 Bq m2 (monthly dry according to a number of previous studies (Cha et al., 2006; Kang
deposition), and 0.0744 and 0.108 Bq L1 (monthly wet deposition),
respectively. The activity concentrations of the soil (Bq kg1) and
monthly wet deposition (Bq L1) samples were converted to Table 2
deposited activity concentrations (Bq m2) using the soil bulk Comparison of the sampling methods for measuring radiocesium in soil from Jeju
Island after the FNPPA.
density (g cm3) and sampled amount (L m2), respectively.
Standard samples were used to calibrate the energy and effi- Site CSa DSSb
ciency of the gamma spectrometer. Standard volumetric sources 134
Cs (Bq kg 1
) 137
Cs (Bq kg 1
) 134
Cs (Bq kg1) 137
Cs (Bq kg1)
(Analytics Co.) containing a mixture of gamma radionuclides c
S1 <1.91 25.7 ± 0.99 11.8 ± 0.72 26.2 ± 1.09
(241Am, 109Cd, 57Co, 139Ce, 203Hg, 113Sn, 85Sr, 137Cs, 88Y, and 60Co) that S2 <1.50 128 ± 2.46 2.04 ± 0.30 96.2 ± 1.84
emit gamma-ray energies between 50 keV and 2 MeV were used. S3 <1.55 111 ± 2.23 4.51 ± 0.47 99.3 ± 2.10
The standard samples were prepared by diluting standard volu- a
Core sampling (depth 5 cm, volume 100 cm3).
metric sources with 1 M HCl solution in sample containers b
Direct surface sampling (depth 1 cm, area 50  50 cm).
c
(Marinelli beaker, U8 vial), which were then measured for 30,000 s Less than minimum detectable activity (<MDA).

4
T.-W. Kang, Y.-U. Han, E.H. Na et al.
et al., 2020; Kim et al., 1995, 1998; Yun et al., 2005). As mentioned
above, the differences in the results depend on the soil sampling
method because the concentration distribution profile according to
the soil depth is not constant for past or FNPPA-derived radio-
cesium. Since the FNPPA-derived 134Cs was deposited only in trace
amounts in the topsoil (1 cm depth) only, it was not detected (less
than MDA) when sampled using the CS method (5 cm depth) as it
was diluted by ~5 times. However, the 137Cs exhibited no significant
differences depending on the sampling method because it exhibits
a uniform distribution profile in surface soils (5 cm depth), most of
which are derived from past events. This is illustrated by the con-
centration distribution profile of radiocesium according to soil
depth at site S2, shown in Fig. 3. Therefore, this indicates that the
soil depth selection is important when analyzing radioactivity in
trace amounts.
From the preliminary survey, we confirmed that the FNPPA-
derived radiocesium was mostly present in the surface soil and
the deposited radiocesium on the surface of Jeju Island was
assessed by collecting samples up to 2 cm in depth using the SSS
method. Table 3 shows the bulk densities, activity concentrations of
radiocesium, and the radiocesium inventories calculated from
these values, from soils sampled at 5 sites in November 2012. The
radiocesium inventories were calculated as follows (Cochran et al.,
1998; Lee et al., 2013):
X lization of radiocesium.
I¼ ri hi Ai ,
i higher values than those of 134Cs radionuclides because they
where I represents the radiocesium inventory (Bq m2), ri is the
bulk density of the soil at depth i (g cm3), and Ai is the activity
concentration in the soil at depth i (Bq kg1).
The bulk density of the soil ranged from 0.167 to 0.359 g cm3
(mean ¼ 0.277 ± 0.079 g cm3), which is lower than that observed
by previous studies of Jeju Island soil (Kang et al., 2020; Song and
Yoo, 1991). This is because the analyses were performed using
soil samples collected only to a depth of 2 cm, and the results were
affected by the litter layers present at the surface. The same trend
was also reported in the forest soils of the study by Hao et al. (2013)
and Takahashi et al. (2015). Additionally, these studies reported
that the litter layers were initially very closely related to the
Fig. 3. Depth distribution profiles of radiocesium activity concentrations in soil samples collected at site S2 on Jeju Island after the FNPPA.
Chemosphere 264 (2021) 128457
presence of the FNPPA-derived radiocesium. The 134Cs and 137Cs
activity concentrations in the soil ranged from <1.15 to 3.57 Bq kg1
(mean ¼ 2.51 ± 1.01 Bq kg1) and 11.1e105 Bq kg1
(mean ¼ 57.1 ± 37.4 Bq kg1), respectively, and were the highest at
sites S4 and S8, respectively. For the radiocesium inventories
calculated from these activity concentrations, the 134Cs and 137Cs
radionuclides in the soil ranged from 9.85 to 14.5 Bq m2
(mean ¼ 11.8 ± 2.0 Bq m2) and 79.7e493 Bq m2
(mean ¼ 293 ± 187 Bq m2), respectively, and in both cases the
values were the highest at site S8. Apart from site S6 that showed
no detection, the 137Cs radionuclide inventory was ~25 times larger
than that of the 134Cs radionuclides. It is believed that site S8, where
the highest inventory was observed, is closely related to rainfall
events (Apr 6e11, 132.5 mm) that occurred when the FNPPA-
derived materials that extended over Jeju Island were most
concentrated, or to the physicochemical characteristics of the soil at
the site. In general, radiocesium is known to strongly adsorb onto
soil particles after a plume of radioactive materials is released, or
can be dispersed or transported according to meteorological con-
ditions, washed out by rainfall, or deposited in the soil in the form
of fallout (ICRP, 1978; UNSCEAR, 2000). The FNPPA-derived radio-
cesium in soils investigated in this study was found to be correlated
with the rainfall at each site presented in Table 3. This implied that
being washed out by rainfall had the greatest effect on the mobi-
(1) As described above, the activity concentrations of 137Cs have
include components derived from past atmospheric nuclear tests
and nuclear power plant accidents; due to their influence, the
134
Cs/137Cs ratio is very different from the FNPPA-derived results
obtained after the accident. These results are consistent with the
results from the Jeju Island soil and moss samples obtained after
the FNPPA (Park et al., 2013), and exhibit the same trend as the
results reported by prior studies of the soils in other countries that
were not directly affected by FNPPA-derived radionuclides (Hao
et al., 2013; Ioannidou et al., 2012; Mckenzie and Dulai, 2017;
Ramzaev et al., 2013). Therefore, the 137Cs radionuclide inventory
was assessed after calculating the value of the 134Cs/137Cs ratio
(0.87) in aerosol samples from Jeju Island, which were collected in
5
T.-W. Kang, Y.-U. Han, E.H. Na et al. Chemosphere 264 (2021) 128457

Table 3
Activity concentrations of radiocesium in soil samples collected from Jeju Island after the FNPPA and inventories calculated from the activity concentrations.

Site Bulk density (g cm3) Rainfalla (mm) Activity concentration (Bq Inventory (Bq m2)
kg1)
134 137 134 137
Apr 6e11 ApreDec Cs Cs Cs Cs

Total Post-FNPPAb Pre-FNPPAc

d
S4 0.167 49.5 2145 3.57 ± 0.37 48.4 ± 1.23 11.9 ± 1.2 162 ± 4 13.7 (8.5%) 148
S5 0.337 56.5 1318 1.46 ± 0.25 37.1 ± 0.9 9.85 ± 1.69 250 ± 6 11.3 (4.5%) 239
S6 0.359 28.5 1148 <1.15e 11.1 ± 0.5 e 79.7 ± 3.6 e 79.7
S7 0.294 30.5 2096 1.86 ± 0.28 83.9 ± 1.63 10.9 ± 1.6 493 ± 10 12.6 (2.6%) 480
S8 0.229 132.5 2431 3.16 ± 0.31 105 ± 2 14.5 ± 1.4 480 ± 9 16.6 (3.5%) 463
Range 0.167e0.359 28.5e132.5 1148e2431 <1.15e3.57 11.1e105 9.85e14.5 79.7e493 11.3e16.6 79.7e480
Mean 0.277 ± 0.079 59.5 ± 42.5 1828 ± 561 2.51 ± 1.01 57.1 ± 37.4 11.8 ± 2.0 293 ± 187 13.6 ± 2.3 282 ± 182
a
Rainfall data were obtained from the Korea Meteorological Administration during 2011 (http://www.kma.go.kr).
b
FNPPA Origin. These values were estimated by calculating the134Cs/137Cs ratio (0.87) in aerosol samples from Jeju Island reported by KINS (Korea Institute of Nuclear
Safety) after the FNPPA (Kim et al., 2012).
c
Origin from past atmospheric nuclear testing and nuclear power plant accidents before the FNPPA.
d
Percentage of post-FNPPA137Cs in the total137Cs.
e
Less than minimum detectable activity.

2011 to distinguish the origins of pre- and post-FNPPA materials
(Kim et al., 2012). From these results, the 137Cs inventory origi-
nating from the FNPPA was calculated to be in the range of
11.3e16.6 Bq m2 (mean ¼ 13.6 ± 2.3 Bq m2), which is less than
10% of the total 137Cs inventory. We estimate that most of this in-
ventory was introduced by past events. According to previous
studies conducted before the FNPPA occurred, the soil in Jeju Island
contained a high concentration of 137Cs radionuclides with a long
half-life (derived from past nuclear tests and accidents) due to the
high cation exchange capacity and the organic matter content of
the soil (Cha et al., 2006; Kang et al., 2020; Kim et al., 1995, 1998;
Yun et al., 2005).
According to the data collected after the FNPPA occurred, 134Cs
and 137Cs activity concentrations in the soil (wet weight, 5 cm
depth) surveyed in Fukushima and Miyagi Prefectures in Japan near
the nuclear power plant were in the range of 0.26e28.35 kBq kg1
and 0.30e29.43 kBq kg1, respectively, which are ~103 times higher
than the results of this study due to the direct effects of the
radioactive plume released by the FNPPA (Hosoda et al., 2013). In
other regions of Japan and the surrounding countries that were not
directly affected, the 134Cs and 137Cs activity concentrations were
0.75e11.9 Bq kg1 and 10.1e105 Bq kg1 in the soil (5 cm depth) in
Hokkaido in northern Japan (Hao et al., 2013), while the soil (1 cm
depth) in Jeju Island had activity concentrations in the ranges of
<MDAe16.7 Bq kg1 and 12.1e109 Bq kg1, respectively (Park et al.,
2013). In addition, for soils (1 cm depth) in the regions of Sakhalin,
Kunashir, and Shikotan Island in Russia (close to northern Japan),
the activity concentrations were in the ranges of 0.75e4.27 Bq kg1
(134Cs) and 2.42e32.2 Bq kg1 (137Cs) for Sakhalin Island, 6.26e28.0
Bq kg1 and 8.46e124 Bq kg1 for Kunashir Island, and 1.15e24.6
Bq kg1 and 4.27e170 Bq kg1 for Shikotan Island (Ramzaev et al.,
2013). These 134Cs and 137Cs activity concentrations detected in
parts of Japan, Korea, and Russia exhibited similar magnitudes as
the results of this study. In particular, the distribution profile results
according to soil depth in Russia showed the presence of 134Cs ra-
dionuclides only in the topsoil (1 cm depth), which is consistent
with the results of this study. In contrast, 134Cs radionuclides were
not detected in the soil (wet weight, 10 cm depth) from the
northeastern region of Beijing, China (Tuo et al., 2013). In other
countries, such as the United States and Europe, FNPPA-derived
radiocesium (134Cs) was detected in soils from Hawaii in the US,
from Milano in Italy, and from Athens in Greece in similar magni-
tudes as the results of this study (Ioannidou et al., 2012; Kritidis)
et al., 2012; Mckenzie and Dulai (2017). However, soils from Vienna,
Austria, from Bremen, Germany, and from the Seine River basin in
6
France did not contain detectable levels of radiocesium (134Cs)
(Evrard et al., 2012; Pittauerova
et al., 2011; Steinhauser et al.,
2013).
The results of these previous studies indicate that 134Cs detected
in soils was derived from the FNPPA, whereas 137Cs included not
only inputs derived from the FNPPA but also those derived from
past atmospheric nuclear testing and the Chernobyl nuclear acci-
dent (Hao et al., 2013; Ioannidou et al., 2012; Kritidis et al., 2012;
Mckenzie and Dulai, 2017; Park et al., 2013; Ramzaev et al., 2013;
Steinhauser et al., 2013).
3.2. Fukushima-derived radiocesium in wet and dry deposition
Table 4 shows the monthly radiocesium inventories analyzed by
collecting rainwater and fallout samples from Jeju Island between
March and December 2011 after the FNPPA. The deposition of
radiocesium in these rainwater and fallout samples is represented
as wet and dry deposition, respectively. The monthly wet deposi-
tion was calculated from the sample amount (L m2) collected in a
1 m2 area for a month and the analyzed rainwater activity con-
centration (Bq L1) from Table S1 (Ioannidou et al., 2012).
In the case of monthly wet and dry deposition, 134Cs and 137Cs
radionuclides were not detected in March immediately following
the FNPPA; however, both had their highest values in April. 134Cs
and 137Cs activity concentrations in April were 10.8 Bq m2 and 12.7
Bq m2 in wet deposition samples, and 4.04 Bq m2 and 4.64 Bq
m2 in dry deposition samples, respectively. The activity concen-
trations in wet deposition samples were ~2.7 times larger than
those of dry deposition samples, reflecting the scavenging effect of
radionuclides in the atmosphere by rainfall (Ioannidou et al., 2012;
Leppa €nen et al., 2013). Wet þ dry deposition values in April were
14.8 Bq m2 for 134Cs and 17.3 Bq m2 for 137Cs, accounting for most
of the total deposition (134Cs ¼ 16.0 Bq m2; 137Cs ¼ 18.8 Bq m2)
for the ten months from March to December. This can be attributed
to the highest inventories that were observed in daily rainwater
samples from April 7 and April 11 after the FNPPA (Fig. S1). After
April, the monthly radiocesium inventory declined sharply, then
became undetectable after September (except for 137Cs in wet
deposition in October). In daily rainwater samples, both 134Cs and
137
Cs radionuclides were not detected after May (Fig. S1). The
134
Cs/137Cs ratio of wet þ dry deposition ranged from 0.70 to 0.86,
which is consistent with the results of a previous study
(134Cs/137Cs ¼ 0.86) reported in aerosol samples from Jeju Island
(Kim et al., 2012). In particular, the wet þ dry deposition of 134Cs
and 137Cs measured in April was ~15 times larger for both
T.-W. Kang, Y.-U. Han, E.H. Na et al. Chemosphere 264 (2021) 128457

Table 4
Activity concentrations of radiocesium in monthly wet (rainwater) and dry deposition samples collected from Jeju Island from March to December 2011 after the FNPPA.

Month Wet deposition (Bq m2) Dry deposition (Bq m2) Wet þ Dry deposition (Bq m2)
134 137 134 137 134 137 134
Cs Cs Cs Cs Cs Cs Cs/137Cs
a
Mar <0.0230 <0.0289 <0.0567 <0.0277 e e e
Apr 10.8 ± 0.2 12.7 ± 0.2 4.04 ± 0.07 4.64 ± 0.08 14.8 17.3 0.86
May 0.242 ± 0.010 0.287 ± 0.012 0.442 ± 0.015 0.540 ± 0.018 0.684 0.827 0.83
Jun 0.0975 ± 0.0070 0.137 ± 0.008 0.123 ± 0.008 0.157 ± 0.009 0.221 0.294 0.75
July 0.0983 ± 0.0068 0.112 ± 0.008 <0.0263 0.0286 ± 0.0054 0.0983 0.141 0.70
Aug 0.0929 ± 0.0068 0.122 ± 0.008 0.0571 ± 0.0054 0.0631 ± 0.0060 0.150 0.185 0.81
Sep <0.0477 <0.0219 <0.0544 <0.0540 e e e
Oct <0.0462 0.0235 ± 0.0055 <0.0513 <0.0498 e 0.0235 e
Nov <0.0471 <0.0474 <0.0506 <0.0515 e e e
Dec <0.0450 <0.0448 <0.0497 <0.0509 e e e
Range (Total) <0.0230e10.8 (11.3) <0.0219e12.7 (13.4) <0.0263e4.04 (4.66) <0.0498e4.64 (5.43) 0.0983e14.8 (16.0) 0.0235e17.3 (18.8) 0.70e0.86
a
Less than minimum detectable activity.

radionuclide species than the results from Kim et al. (2012) in
Daejeon, Korea. The two radionuclide species exhibited similar
values to the results of Kim et al. (2012) in May, which indicates that
a highly radioactive plume was directly introduced to Jeju Island
during April. The results of this study were tens of times higher
than those obtained from Finland, Germany, Italy (Milano), and
Portugal as follows: Finland, 0.21e0.57 Bq m2 (134Cs), 0.28e0.62
Bq m2 (137Cs); Germany, 0.2 Bq m2 (137Cs); Italy Milano,
0.27e0.48 Bq m2 (137Cs); Portugal, 0.59e0.62 Bq m2 (137Cs)
(Carvalho et al., 2012; Ioannidou et al., 2012; Leppa€nen et al., 2013;
Pittauerova
et al., 2011). On the other hand, most of the 137Cs
deposition measured in April 2011 in Japan was higher than the
results obtained by this study but exhibited various concentration
distribution profiles that varied by region. Regions located closest
to Jeju Island, such as Fukuoka and Satsuma-Sendai, exhibited re-
sults similar to or lower than the values obtained by this study
(Hirose, 2012).
3.3. Comparison of Fukushima-derived radiocesium in soil and
deposition samples
The inventories of FNPPA-derived radiocesium assessed from
the soil and deposition (wet and dry) samples collected from Jeju
Island were compared. The 134Cs and 137Cs inventories calculated
from the mean concentrations of radiocesium in the soil from the
five sampling sites are 11.8 Bq m2 and 13.6 Bq m2, respectively
(Table 3). The 134Cs and 137Cs deposition values from the wet and
dry deposition samples are 16.0 Bq m2 and 18.8 Bq m2, respec-
tively (Table 4). The total radiocesium inventories (134Cs þ 137Cs)
are 25.4 Bq m2 (soil) and 34.8 Bq m2 (wet þ dry deposition);
although the values obtained from the soil are slightly lower, the
two sets of values are of a similar order (Fig. S2). The total radio-
cesium inventory deposited at site S8 was 31.1 Bq m2, which is
almost the same magnitude as the deposition from wet þ dry
samples. However, at some sampling sites, as noted above (section
3.1), the differing results may be due to different physicochemical
properties of the soil in the region and/or the meteorological con-
ditions (rainfall amount), which affected the adsorption behavior
and the loss of FNPPA-derived radiocesium in the soil. This may
have been caused by the plume of radionuclides released from the
FNPPA that had a non-uniform distribution in each region with
differing rainfall amounts, leading to changes in the radiocesium
inventory. This means that most of the radiocesium was absorbed
by the litter layer on top of the soil after deposition in April 2011
(92% of the total). The soil samples were collected after an extended
period (November 2012) elapsed, resulting in the loss of
radiocesium.
3.4. Evidence of Fukushima-derived radionuclides in rainwater
Fig. 4 (a) shows the sample and background gamma-ray spec-
trum (measured for 150,000 s) of the rainwater sample collected on
April 7, 2011 after the FNPPA. We collected 10.66 L of rainwater
from the rainfall that occurred from 9 p.m. on April 6e9 a.m. on
April 7. According to data from the Korea Meteorological Admin-
istration, the rainfall amount during this period was 17.5 mm. After
collection, the rainwater sample was removed from the foreign
matter (leaves, insects, etc.), transferred to a 20 L beaker (Duran
Co.), and slowly evaporated to concentrate to 100 mL or less. Then,
the sample was transferred to an evaporation dish, dried
completely, and pulverized to obtain a fine powder and placed into
sample container for measurement (U8 vial, 50 mm width, 70 mm
height). The collected rainwater sample was pre-treated with the
total amount and analyzed by gamma spectrometer. Fig. 4 (b)
shows the gamma-ray spectrum of long- and short-lived radionu-
clides derived from the FNPPA in the rainwater samples. The
detected gamma-emitting radionuclides are listed in Table S2. Ra-
dionuclides detected in the rainwater samples included 140La,
110m
Ag, 95Nb, 125Sb, 113Sn, 129Te, 129mTe, 132Te, 132I, and 136Cs radio-
nuclides, as well as the representative 131I, 134Cs, and 137Cs
radionuclides.
Activity concentrations of these gamma-emitting radionuclides
were mostly trace amounts, similar to the MDA threshold. Because
the values were assessed without taking correction factors such as
coincidence summing from gamma-ray emission into account, the
values are not presented here. Nevertheless, the highest activity
concentrations of 131I, 134Cs, and 137Cs radionuclides exhibited
similar activity concentrations as the daily rainwater samples
shown in Fig. S1. The total activity concentration of all gamma-
emitting radionuclides detected was at a level that can be dis-
regarded for considering radiation risk. Among the detected
gamma-emitting radionuclides, even very short half-life radionu-
clides (140La, 110mAg, 95Nb, 113Sn, 129Te, 129mTe, 132Te, 132I, and 136Cs)
were measured. On the other hand, other gamma-emitting radio-
nuclides, except for 131I, 134Cs, and 137Cs, were not detected in the
daily rainwater and monthly wet deposition samples. Since the
radionuclides introduced by the FNPPA were in trace amounts, only
a small quantity of sample was used (daily rainwater, 1 L) and the
effect of radioactive decay due to the long sampling period was also
present. In other countries, the short-lived gamma-emitting ra-
dionuclides detected by this study were reported in environmental
samples from the US and Europe (France, Lithuania), not only in
Japan, which was directly affected by the radioactive plume after
the FNPPA (Amano et al., 2012; Biegalski et al., 2012; de Vismes-Ott
et al., 2013; Endo et al., 2012; Gudelis et al., 2012; Hazama and
Matsushima, 2013; Hosoda et al., 2013; Kanai, 2012; Saegusa

7
T.-W. Kang, Y.-U. Han, E.H. Na et al. Chemosphere 264 (2021) 128457

Fig. 4. (a) Background (blue line) and rainwater (red line) gamma-ray spectrum collected on April 7, 2011 on Jeju Island after the FNPPA. (b) Long- and short-lived radionuclides
derived from the FNPPA were detected in rainwater collected on April 7, 2011. (rainfall event, April 6 21:00eApril 7 09:00; amount of rainfall, 17.5 mm; sampling volume, 10.66 L).
(For interpretation of the references to colour in this figure legend, the reader is referred to the Web version of this article.)

et al., 2013; Saito et al., 2015; Tagami et al., 2011). 4. Conclusions

The results indicate that the radioactive plume released by the
FNPPA was directly introduced to Jeju Island during a specific
period, which is evidence that reflects the atmospheric modeling
results obtained by previous studies (Hong et al., 2012; Huh et al.,
2012; Lee et al., 2015, 2017; Momoshima et al., 2012).
This study was conducted to confirm the presence of FNPPA-
derived radiocesium (134Cs, 137Cs) deposited in the surface soil of
Jeju Island, Korea. In addition, radiocesium inventories were eval-
uated based on the activity concentrations measured in the soil and

8
T.-W. Kang, Y.-U. Han, E.H. Na et al.
wet and dry deposition from rainwater and fallout, respectively,
were compared and analyzed. This study presents the first evidence
of FNPPA-derived radionuclides directly entering Jeju Island.
From the preliminary surveys, FNPPA-derived radiocesium
(134Cs) was present in trace amounts in the topsoil (1 cm depth)
only, indicating that soil depth selection was very important in the
analysis of FNPPA-derived radiocesium. On the other hand, the 137Cs
radionuclides detected included those derived from past atmo-
spheric nuclear testing and nuclear power plant accidents. Ac-
cording to the results of investigations at 5 sampling sites on Jeju
Island, the mean inventories calculated for 134Cs and 137Cs activity
concentrations, excluding 137Cs radionuclides of past origins, were
11.8 ± 2.0 Bq m2 and 13.6 ± 2.3 Bq m2, respectively. The 134Cs and
137
Cs deposition from rainwater (wet) and fallout (dry) were
assessed at 16.0 Bq m2 and 18.8 Bq m2 in each case. The total
radiocesium inventories (134Cs þ137Cs) were 25.4 Bq m2 (soils) and
34.8 Bq m2 (wet þ dry), respectively, and although the value ob-
tained from soils was slightly lower, it was of a similar order of
magnitude. In addition, the FNPPA-derived radiocesium deposited
in the soil was found to be greatly affected by the plume of radio-
nuclides that was released from the FNPPA and directly introduced
into the region in April. In the rainwater samples collected on April
7, 2011, 140La, 110mAg, 95Nb, 125Sb, 113Sn, 129Te, 129mTe, 132Te, 132I, and
136
Cs, which are short-lived radionuclides, as well as 131I, 134Cs, and
137
Cs radionuclides were all detected, indicating the direct inflow of
these radionuclides to Jeju Island. These results correlate with the
atmospheric modeling results obtained by previous studies. The
methods and results of this study can be utilized as references to
analyze trace amounts of radioactivity from other nuclear accidents.
CrediT author statement
Tae-Woo Kang, Conceptualization, Data curation, Formal anal-
ysis, Investigation, Methodology, Visualization, Writing - original
draft, Writing - review & editing, Young-Un Han, Data curation,
Validation, Visualization, Eun Hye Na, Conceptualization, Re-
sources, Supervision, Writing - review & editing, Bon-Jun Koo,
Conceptualization, Writing - review & editing, Won-Pyo Park,
Conceptualization, Data curation, Visualization, 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 influence the work reported in this paper.
Acknowledgements
This study was a part of the emergency monitoring response of
the Korea Institute of Nuclear Safety (KINS) in Korea during the
Fukushima nuclear power plant accident in 2011. T.W. Kang ap-
preciates the assistance of the staff members of KINS, especially Dr
Jong-In Byun for his technical assistance. T.W. Kang also deeply
appreciates the assistance of the Institute for Nuclear Science &
Technology at Jeju National University who helped analyze the
samples. This research was partially supported by a grant from the
National Institute of Environmental Research (NIER), funded by the
Ministry of Environment (MOE) of the Republic of Korea (NIER-
2020-03-03-002).
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.chemosphere.2020.128457.
9
Chemosphere 264 (2021) 128457
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