Journal of Environmental Radioactivity 174 (2017) 30e37

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Journal of Environmental Radioactivity

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210
Po in the marine biota of Korean coastal waters and the effective
dose from seafood consumption
S.H. Kim a, b, *, G.H. Hong a, b, H.M. Lee a, B.E. Cho a, b
a
Korea Institute of Ocean Science & Technology, Ansan, 15627, Republic of Korea
b
Graduate School of Ocean Science and Technology, Korea Maritime and Ocean University, Busan, 49112, Republic of Korea

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

Article history: The activity concentrations of 210Po were determined in plankton and selected species of macroalgae,
Received 11 May 2016 crustaceans, molluscs, and sh from Korean coastal waters to understand 210Po distribution in these
Received in revised form trophic levels and to assess the effective dose of 210Po from seafood ingested by the average Korean. The
31 October 2016
activity concentration of 210Po in macroalgae, mixed plankton, anchovy (whole body), abalone muscle,
Accepted 1 November 2016
Available online 28 November 2016
and abalone viscera was 0.97e1.43, 32e137, 59e392, 2.93 0.86, and 1495 484 Bq kg
1 (w.w.),
respectively. Polonium-210 concentration in the whole esh of mussel and oyster were 47.8 5.9 and
45.3 7.1 Bq kg
1 (w.w.), respectively. Polonium-210 concentration in the muscle of the ve tested
Keywords:
Dose
species of sh other than anchovy ranged from 0.51 to 5.56 Bq kg
1 (w.w.), with the lowest amount in a
Ingestion demersal species. In sh, 210Po activity concentration was as much as three orders of magnitude higher in
Marine organism viscera than in muscle. The average annual effective 210Po dose per average Korean adult, who consumes
210
Po 42.8 kg of seafood a year (excluding anchovy), was estimated to be 94 mSv y
1, with 42e71% of this
attributed to shellsh. Further studies are required to assess the dose of 210Po from anchovy owing to its
high activity concentration and the manner in which anchovy is consumed.
2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction much higher than those of articial radionuclides such as 137Cs

Polonium-210 (210Po) is a natural radionuclide in the 238U decay
series that accumulates in marine biota (Beasley et al., 1969, 1973;
Bustamante et al., 2002; Carvalho, 2011; Cherry and Heyraud,
1982; Cherry and Shannon, 1974; Folsom et al., 1972; Folsom and
Beasley, 1973; McDonald et al., 1986; Rodriguez y Baena et al.,
2007; Ryan et al., 1999; Schell et al., 1973; Shannon, 1973;
Skwarzec, 1988; Suh et al., 1995; Waska et al., 2008). Polonium-
210 activity concentrations in marine organisms vary widely
among taxonomic groups and among different tissues of a given
species, with concentration factors varying from 103 to 106 (Fowler,
2011). The reference value of 210Po concentration in sh is 2.0 Bq
kg
1 (w.w.), but actual amounts vary widely, from 0.08 to 12 Bq
kg
1 (w.w.) (UNSCEAR, 2000).
Polonium-210 is highly radioactive as an alpha emitter, and has
a characteristic energy of 5.3 MeV. The committed effective dose
coefcient for ingestion of 210Po for an adult (1.2  10
6 Sv Bq
1) is
* Corresponding author.Korea Institute of Ocean Science & Technology, Ansan,
15627, Republic of Korea
E-mail address: shkim@kiost.ac.kr (S.H. Kim).
(1.3  10
8 Sv Bq
1), 90Sr (2.8  10
8 Sv Bq
1), and 239240Pu
(2.5  10
7 Sv Bq
1), which have been dispersed widely in the
environment since nuclear weapon tests began in the 1940s (ICRP,
2012). The median lethal dose (LD50) for acute radiation exposure is
generally about 4.5 Sv (Strom, 2003). A fatal dose from ingestion of
210
Po corresponds to 3.75 MBq, which is equivalent to about 21 ng
of 210Po with a committed effective dose coefcient of 1.2  10
6 Sv
Bq
1. The death of Russian dissident Alexander Litvinenko in 2006
was due to 210Po poisoning (Maguire et al., 2010).
Given its high concentration in marine biota and high
committed effective dose for ingestion, radiation doses of 210Po
from seafood consumption have been assessed in various regions
(Aoun et al., 2015; Carvalho and Fowler, 1993; IAEA, 1995; Smith
and Towler, 1993; Suriyanarayanan et al., 2010; Yamamoto et al.,
1994). The radiation exposure of adult populations from ingestion
of natural radionuclides is 0.11 mSv y
1, and a large portion of that
is contributed by 210Pb/210Po (UNSCEAR, 2000). Marine sh prod-
ucts are consumed around the world, but seafood consumption is
relatively high in eastern Asia and northern and western Europe,
with an average per capita rate of 30e60 kg yr
1 in these regions
(FAO, 2014). In the Republic of Korea, the 15-year average per capita

http://dx.doi.org/10.1016/j.jenvrad.2016.11.001
0265-931X/ 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37 31

consumption of seafood is 47.6 kg yr
1, or 42.8 kg yr
1 excluding

anchovy (KREI, 2012). The objectives of this study were to inves-
tigate the concentrations and distribution of 210Po in selected ma-
rine organisms that constitute the primary seafood items in Korea,
and to estimate the effective dose of 210Po from seafood
consumption.

2. Materials and methods

2.1. Study area

The study area is located between the East China Sea and the
southern coast of the Korean peninsula. The East China Sea is one of
the largest continental shelves in the world. This area is inuenced
by the warm Thushima current and is subject to the inuence of the
Changjiang Diluted Water inow from the west. Thus, this area has
rich grounds for capture sheries. The species diversity of shes in
the Korea Strait is impressively high. A total of 301 marine sh
species are known from off the southern coast of the Korean
peninsula, and 612 species are known from the waters off Jeju Is-
land (Kim, 2009). The southern coast of the Korean peninsula has a
heavily indented coastline and provides many suitable habitats for
aquaculture. More than 90% of aquaculture and 70% of coastal and
offshore capture sheries in the Republic of Korea are located in
Fig. 1. Location of the sampling sites off the Korean coast. Samples were collected
this area (MOF, 2015).
within the open circles. Numbers in map indicate coastal shery area codes of Republic
of Korea.
2.2. Sampling

Marine biota from selected trophic levels were collected in
Korean coastal waters throughout 2013e2015. Sample species
included mixed plankton, two species of macroalgae, one crusta-
cean, four molluscs (one gastropod, two bivalves, and one cepha-
lopod), one planktivorous sh, and ve carnivorous sh. Plankton
samples were collected with plankton nets with mesh sizes of
20 mm or 300 mm towed behind a small boat at 1e1.5 m s
1.
Plankton were classied according to the size fractions of
20e300 mm and >300 mm. After collection, plankton samples were
sieved immediately with a same-sized mesh lter, stored in acid-
cleaned plastic petri dishes, and frozen. The two kinds of macro-
algae, laver (Porphyra tenera) and sea mustard (Undaria pinnatida),
were collected from a macroalgae farm along the southwestern
Korean coast in February, the typical harvest month. Mussels
(Mytilus coruscus) and oysters (Crassostrea gigas) were collected
from farms on the southern coast. Abalone (Nordotis discus) were
collected from the coast of Jeju Island. Samples of other popular
Korean shery products were purchased from a commercial shery
market, and their harvest dates and collection localities were noted.
Sampling locations and dates are shown in Fig. 1 and Table 1.
Samples were stored in cold storage boxes and transported to the
laboratory. Samples (except plankton) were washed with distilled
water to remove any material attached to the surface. The edible
tissue, skin, and internal organs of individual sh and shellsh were
separated as much as possible before being pooled, freeze-dried,
and homogenized by species. Samples were weighed twice: wet
weight immediately after separation and dry weight after freeze-
drying, homogenization, and oven drying. All results were
expressed as Bq kg
1 wet weight (w.w) or Bq kg
1 dry weight
(d.w.). The wet sample weight for the pooled parts was more than
10 kg. For plankton, dry weight was not determined and the anal-
ysis of 210Po concentration was performed with a fresh wet sample.
2.3. Determination of the 210
Po activity concentration
Analysis of 210Po was done using aliquots of freeze-dried and
homogenized samples that had equivalent wet weights (w.w.) of 10
g for shery samples, and 2 g of fresh samples for plankton. Sam-
ples, with the addition of a209Po tracer, were completely digested
with concentrated nitric acid and hydrogen peroxide on a hot plate.
The resulting solution was gently evaporated to dryness. The res-
idue was repeatedly dissolved in 6 N hydrochloric acid, which was
then evaporated off to remove residual nitric acid. The nal residue
was dissolved with 100 mL 0.5 N hydrochloric acid. Polonium iso-
topes were spontaneously deposited onto a silver planchet while
being stirred continuously at room temperature overnight (Lee
et al., 2014). The activity of deposited polonium isotopes was
counted using a spectrometry (PIPS detector: Canberra Model 7404
MCA; Canberra Industries, Meriden, CT, USA). Analysis was per-
formed for three aliquots of each sample. Sample preparation and
analysis was done within a month of sample collection to reduce
the inuence of 210Po in-growth from the decay of 210Pb. 210Po
activity concentrations were corrected to the time of collection.
To verify the accuracy of 210Po analyses in this study, reference
material IAEA-414 (Pham et al., 2004), made from Irish and North
Sea sh, was analysed simultaneously (Table 2). The activity con-
centration of 210Po determined in this study reected the estab-
lished value of IAEA-414 (99.5 8.5% accuracy).
3. Results and discussion
Tables 3e5 include the activity concentrations and concentra-
tion factors (CFs) of 210Po in the marine organisms investigated in
this study. CFs were calculated from the dissolved 210Po concen-
tration of 0.75 0.06 mBq kg
1 in the seawater around Jeju Island
(Cho and Kim, 2016).
3.1. Plankton and macroalgae
The activity concentration of 210Po was 32e137 Bq kg
1 (w.w.) in
the 20e300 mm plankton fraction and 46.8e113 Bq kg
1 (w.w.) in
the >300 mm plankton fraction (Table 3). The activity concentra-
tions of 210Po in both plankton fractions were several times higher
in winter than in summer. This seasonal variation may be attributed
32 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37

Table 1
Sampling locations and dates for marine organisms caught in Korean coastal waters.

Name of samples Locationa Date

Plankton 223 Feb-2014; June-2015

Macroalgae
Laver (Porphyra tenera) 213 Feb-2014
Sea mustard (Undaria pinnatida) 213 Feb-2014
Crustaceans
Red-banded lobster (Metanephrops thomsoni) 230, 231 Feb-2015
Molluscs
Abalone (Nordotis discus) 232 Feb-2014
Far eastern Mussel (Mytilus coruscus) 98 Nov-2013
Giant Pacic Oyster (Crassostrea gigas) 98 Nov-2013
Japanese common Squid (Todarodes pacicus) 222, 232, 242 Feb-2015
Fish
Anchovy (Engraulis japonicus) 232; 98 May-14; June-15
Chub mackerel (Scomber japonicus) 222, 232, 242 Feb-15
Largehead hairtail (Trichiurus lepturus) 241 June-15
Japanese Horse mackerel (Trachurus japonicus) 241 June-15
Red tilesh (Branchiostegus japonicus) 241 June-15
Olive ounder (Paralichthys olivaceus) 230, 231 Feb-14
a
Numbers are the coastal shery area codes of Republic of Korea.

Table 2 to differences in phytoplankton communities. Diatoms dominate in

Determination of 210
Pb(210Po)a concentration in Sea Fish Reference Material IAEA- late winter and dinoagellates in summer along the coast of Jeju
414. Island (Affan and Lee, 2004), where samples were collected.
Information value Condence interval This study (N 3) Polonium-210 accumulates more in diatom species than in di-
noagellates (Stewart and Fisher, 2003). The activity concentration
(unit: Bg kg
1 d.w)
of 210Po in the small-sized plankton fraction was somewhat higher
2.1 1.8e2.5 2.21 0.19 than that in the large-sized plankton fraction in winter, but this
a 210
Po is in equilibrium with 210
Pb at the time of measurement. relationship was reversed in summer. In the 20e300 mm and
>300 mm plankton fractions, the 210Po CFs were 4.0e18  104 and

Table 3
The 210Po activity concentrations and concentration factors in plankton and macroalgae from Korean coastal waters.

Name of samples Activity (Bq kg
1 w.w) Weight ratio Concentration Factor (104)
Mean SD dry/wet Mean SD

Plankton [20e300 mm] 137 51a e 17 9a

32 3b e 4 2b
Plankton [>300 mm] 113 2a e 14 5a
47 9b e 6 2b
Macroalgae
Laver 1.43 0.21 0.099 0.18 0.07
Sea mustard 0.97 0.13 0.080 0.12 0.05
a
Sampling in February 2014.
b
Sampling in June 2015.

Table 4
The 210Po activity concentrations and concentration factors in crustaceans and molluscs from Korean coastal waters.

Name of samples Activity (Bq kg
1 w.w) Weight ratio Concentration Factor (104)
Mean SD dry/wet Mean SD

Crustaceans
Red-banded lobster
Muscle 2.84 0.23 0.20 0.35 0.13
Exoskeleton 46 10 0.36 5.7 2.4
Viscera 906 226 0.29 112 49
Molluscs
Abalone
Muscle 2.93 0.86 0.20 0.36 0.17
Viscera 1500 484 0.20 185 89
Far eastern mussel
Whole esh 47.8 5.9 0.24 5.9 2.2
Giant Pacic oyster
Whole esh 46.3 7.1 0.21 5.7 2.2
Japanese common squid
Muscle 8.61 2.01 0.21 1.1 0.5
Skin 948 77 0.21 117 43
Viscera 1940 93 0.30 239 86
 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37 33

Table 5
The 210Po activity concentrations and concentration factors in sh from Korean coastal waters.

Name of samples Activity (Bq kg
1 w.w) Weight ratio Concentration Factor (104)
Mean SD dry/wet Mean SD

Anchovy
Whole bodya 59 4.59 e 7.3 2.7
Musclea 38.9 11.4 e 4.8 2.2
Visceraa 323 85.3 e 41 4
Heada 96.3 8.65 e 12 18
Whole bodyb 392 2.2 0.24 48 17
Chub mackerel
Muscle 0.8 0.03 0.37 0.1 0.04
Skin 12.6 3.15 0.46 1.6 0.7
Viscera (except liver) 142 10.5 0.35 18 6
Liver 429 179 0.40 53 29
Largehead hairtail
Muscle 5.56 1.23 0.28 0.69 0.29
Viscera 157 96.8 0.24 19 14
Japanese horse mackerel
Muscle 5.26 0.13 0.25 0.65 0.23
Skin 50.8 8.22 0.40 6.3 2.5
Viscera 112 20 0.32 14 6
Red tilesh
Muscle 3.08 0.94 0.21 0.38 0.18
Skin 6.45 3.29 0.34 0.8 0.5
Viscera 49.6 15.5 0.24 6.1 2.9
Olive ounder
Muscle 0.51 0.12 0.25 0.06 0.03
Skin 25.1 10.4 0.34 3.1 1.7
Viscera (except liver and gall bladder) 2236 242 0.18 276 103
Liver 222 18.4 0.43 27 10
Gall bladder 1017 96.3 0.13 126 46.5
a
Sampling in 2015.
b
Sampling in 2014.

5.8e14  104, respectively. These CFs were comparable with the CF
for phytoplankton (7  104) and several times higher than the CF
for zooplankton (3  104) reported by IAEA (2004).
Polonium-210 activity concentrations were determined for two
species of macroalgae, laver (Porphyra tenera) and sea mustard
(Undaria pinnatida). The 210Po CFs in the macroalgae were
1.3e1.9  103, and were comparable to the CF for macroalgae
(1.0  103) reported by IAEA (2004).
Annual consumption of these two macroalgae is as much as
11 kg per person in the Republic of Korea (KREI, 2012). Samples
were collected during the traditional harvest season. Polonium-210
activity concentration in laver (red alga) was higher than in sea
mustard (brown macroalga), with average values of 1.43 0.21 and
0.97 0.13 Bq kg
1 (w.w.), respectively (Table 3). These values were
two or three times lower than the 2.3e3.1 Bq kg
1 (w.w.) reported
for benthic Sargassum in the northern Arabian Gulf (Uddin et al.,
2015), several times lower than the 2.8e8.0 Bq kg
1 (w.w.) re-
ported for a brown macroalga (species not identied) along the
Japanese shoreline (Baumann et al., 2013). It is known that there are
several contributing factors for differences in metal accumulation
by different species of macroalgae, including life span, morphology,
contact surface area, growth rate, and selective afnity for specic
metals by particular species (Chakraborty et al., 2014). Brown algae
generally accumulate divalent metal species in considerable
amounts due to their high content of binding polysaccharides and
polyphenols (Hashim and Chu, 2004). There was a study on the
210
Po activity concentrations in several species of macroalgae in the
intertidal zone off the coast of Portugal (Carvalho, 2011). Regardless
of algae classes, Ploccamium cartilagineum, Gelidium sesquipedale,
and Fucus vesiculosus, all with relatively large surface areas, had
higher 210Po activity concentrations, at 5.2e9.1 Bq kg-1 (w.w.), than
the 1.6e2.7 Bq kg-1 (w.w.) in other species. An experiment on the
uptake of americium by three benthic algal species (Ulva rigida,
Fucus vesiculosus, and Gigartina stellata) showed that the uptake by
the green alga was 3e5 times greater than that by the brown and
red species. This experimental evidence indicated that Am accu-
mulation is a passive process and that adsorption takes place
mainly on the thin outer organic coating of seaweed (Carvalho and
Fowler, 1985). The reason why Porphyra tenera (red algae) showed
higher 210Po activity concentration than Undaria pinnatida (brown
algae) in this study may be associated with the difference in contact
surface area. However, there should be more investigation into the
reasons for the differences in 210Po activity concentration among
species of macroalgae.
3.2. Crustaceans and molluscs
Measurements of 210Po from crustaceans and molluscs were
conducted with muscle, skin, and viscera from red-banded lobster
(Metanephrops thomsoni) and squid, muscle and viscera from
abalone, and all soft tissues for mussel and oyster (Table 4). The
exoskeleton of red-banded lobster was considered its skin, and
viscera were all internal organs and stomach contents.
The concentration of 210Po in red-banded lobster was
2.84 0.23 Bq kg
1 (w.w.) in muscle, 46 10 Bq kg
1 (w.w.) in the
exoskeleton, and 906 226 Bq kg
1 (w.w.) in the viscera. High 210Po
concentration in the viscera of red-banded lobster may be attrib-
uted to a210Po-rich diet, which includes organic particulates and
copepods (Cherry and Heyraud, 1981). The percentages of 210Po in
each part relative to the total amount of 210Po in the whole body
were 0.6 (muscle), 12.2 (exoskeleton), and 87.2% (viscera). This in-
dicates that in red-banded lobster, 210Po accumulates primarily in
the viscera through diet. Polonium-210 concentrations from more
than 30 species of marine shrimp, collected from the Mediterra-
nean Sea, Kuwait, South Africa, USA, and Great Britain, spanned two
orders of magnitude, from 15.5 to 1670 Bq kg
1 (d.w.) in the whole
34 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37
shrimp (Cherry and Heyraud, 1981), depending on the species and
the local environment. The concentration of 210Po in the whole
body of Metanephrops thomsoni investigated in this study was
calculated as 612 134 Bq kg
1 (d.w.), based on the wet weight
analysis and the wet: dry ratio. This value was approximately two
times higher than the median 210Po concentration of 296 Bq kg
1
(d.w.) of more than 30 species of shrimp and similar to the con-
centration in penaeid shrimp from the Mediterranean and caridean
shrimp from the Natal, which live in pelagic and deep pelagic en-
vironments (Cherry and Heyraud, 1981). Metanephrops thomsoni is
distributed in the Indo-West Pacic region, including the Korea
Strait, Yellow Sea, and East China Sea, and is found at a depth of
50e500 m, on sandy mud bottoms (Bate, 1888).
Polonium-210 concentration in the muscle of abalone (Nordotis
discus) was 2.93 0.86 Bq kg
1 (w.w.), two or three times higher
than concentrations in the macroalgae that form its diet. Polonium-
210 concentrations in abalone viscera were 1495 484 Bq kg
1
(w.w.), approximately three orders of magnitude higher than in the
muscle. The dry weight (d.w.) 210Po concentration of 15.0 4.4 Bq
kg
1 (d.w) in the muscle of Nordotis discus in this study was several
times higher than the 2.3e3.5 Bq kg
1 (d.w.) in the muscle of
Haliotis tuberculata, another species of abalone, on the French coast
(Connan et al., 2007). The d.w. 210Po concentration of 7660 2480
Bq kg
1 (d.w) in the viscera of Nordotis discus was several to ten
times higher than the 134.3e135.2 Bq kg
1 (d.w.) in the viscera of
Haliotis tuberculata. Comparison of 210Po concentrations in abalone
species is difcult because few have been studied. However, Nor-
dotis discus had higher accumulations of 210Po than did Haliotis
tuberculata, especially in the viscera. Polonium-210 CFs in the
muscle and viscera of Nordotis discus were 3.9  103 and 1.99  106,
respectively. Even though the 210Po concentration in Nordotis discus
muscle was several times higher than in Haliotis tuberculata, the CF
was several times lower than the recommended value of 2  104 in
molluscs reported by IAEA (2004).
Polonium-210 concentrations measured in the whole esh of
mussel (Mytilus coruscus) and oyster (Crassostrea gigas) were
similar to each other, at 47.8 5.9 and 45.3 7.1 Bq kg
1 (w.w.),
respectively. They were collected in the same location on the same
date, so their shared physicochemical habitat may have produced
similar 210Po concentrations. Polonium-210 concentrations
measured in these species along the French coast were similar
within locations, but showed great variation across sites (Connan
et al., 2007). Mytilus coruscus and Crassostrea gigas, as lter
feeders, may show different levels of 210Po based on the type and
concentration of suspended food. Crassostrea gigas demonstrated
little change with diet quality or concentration (Ward et al., 2003).
Mytilus trossulus is known to non-selectively transport particles
(Ward et al., 1998). The similar trends in 210Po concentration in
Mytilus coruscus and Crassostrea gigas may be attributed to their
feeding on similar diets.
Polonium-210 concentrations in the whole esh of mussels from
several other places differed greatly within species by location: in
Mytilus galloprovincialis, 210Po ranged from 18.5 0.7 Bq kg
1
(w.w.) along the Portuguese coast (Carvalho, 2011), to 22.1e207 Bq
kg
1 (w.w.) on the Croatian Adriatic coast (Ro
zmaric et al., 2012),
and 53e1960 Bq kg
1 (d.w.) on the Turkish coast (Ug ur et al., 2011).
In Mytilus edulis, 210Po was 156e275 Bq kg
1 (w.w.) along the
French coast (Connan et al., 2007), and in Perna perna, 210Po was
78e320 Bq kg
1 (w.w.) on the Kanyakumari coast in South India
(Macklin Rani et al., 2014).
Polonium-210 concentrations in the whole esh of oysters also
showed variation of one order of magnitude according to the
location and species: 23.4e126 Bq kg
1 (w.w.) (species not identi-
ed) from the coast of Taiwan (Lee and Wang, 2013), 10e24 Bq kg
1
(w.w.) in Crassostrea gigas from the coast of France (Connan et al.,
2007), and 12.7 Bq kg
1 (w.w.) in Crassostrea madrasensis from
the east coast of India (Satheeshkumar et al., 2016).
The recommended CF of 210Po in the edible part of crustaceans
and molluscs is 2  104 (IAEA, 2004). In this study, CFs of 210Po were
0.4  104 in crustacean muscle and in the muscle of the gastropod
and 6  104 in the edible soft body of lter-feeding molluscs.
Squid comprises the largest quantity of shellsh seafood in the
Republic of Korea (KREI, 2012). Polonium-210 concentrations
measured from the muscle, skin, and viscera of squid (Todarodes
pacicus) were 8.61 2.01, 948 77, and 1940 93 Bq kg
1 (w.w.),
respectively. 210Po concentrations in the muscle of squid ranged
from 0.42 to 5.5 Bq kg
1 (w.w.) in Loligo vulgaris from the Atlantic
Ocean (Heyraud and Cherry, 1979), 1.33e2.3 Bq kg
1 (w.w.) in
Nototodarus spp. from New Zealand (Pearson et al., 2016), 3.5 0.3
Bq kg
1 (w.w.) in Loligo spp. from Slovenia (Strok
and Smodi
s,
2011), and 12.9 0.69 Bq kg
1 (w.w.) in Loligo duvauceli from In-
dia (Satheeshkumar et al., 2016). Polonium-210 concentration in
squid muscle was three times higher than that in other crustaceans
and molluscs investigated in this study. The 210Po concentration in
squid viscera was also the highest, but the ratio of concentration in
viscera to that in muscle was 225 in squid, which was somewhat
lower than the 319 in red-banded lobster and 512 in abalone.
3.3. Fish
Polonium-210 was determined from six species, including one
planktivorous sh (anchovy, Engraulis japonicus), four pelagic
carnivorous sh (chub mackerel, Scomber japonicus; largehead
hairtail, Trichiurus lepturus; Japanese horse mackerel, Trachurus
japonicus; and red tilesh, Branchiostegus japonicus), and one
demersal sh (olive ounder, Paralichthys olivaceus). Results are
presented by tissue in Table 5.
Anchovy is one of the most commonly consumed sh in the
Republic of Korea (KREI, 2012). Polonium-210 concentration in the
whole body of anchovy (Engraulis japonicus) collected in May 2014
was 392 2 Bq kg
1 (w.w.), several times higher than in the
plankton that comprise their main diet. This value was the highest
among the sh in this study. In 2015, 210Po concentration in an-
chovy was determined for a sample collected in another location.
Polonium-210 concentration in the whole body in June 2015 was
59.0 4.6 Bq kg
1 (w.w.), slightly higher than the values from
plankton. The difference in 210Po concentrations in anchovy
collected in May 2014 and in June 2015 may be due to habitat
differences. In anchovy studied from a single region of the Black
Sea, the whole-body 210Po concentration differed by a factor of two
within the space of one month (Lazorenko et al., 2002). Assuming
sh obtain most or all of their 210Po burden from the plankton they
ingest, the higher 210Po concentrations in anchovy, compared to
those in plankton, suggest that 210Po is biomagnied up the food
web to anchovy. Polonium-210 concentrations measured in the
muscle, viscera, head, and whole body of anchovy in June 2015
were 38.9 11.4, 323 85, 96.3 8.7, and 59.0 4.6 Bq kg
1 (w.w.),
respectively, demonstrating that 210Po accumulated eight times
more in viscera than in muscle. Polonium-210 concentrations in
anchovy from other regions had a range of 26.1e638 Bq kg
1 (w.w.)
in the whole body, and were the highest among all species of sh
investigated in the same regions (Khan and Wesley, 2012;
Lazorenko et al., 2002; Strady et al., 2015; Strok
and Smodi
s,
2011). Ako zcan and Ugur (2013) reported that the mechanism of
uptake of 210Po and 210Pb by sh reects biological variables such as
feeding habits and location, based on their investigation of these
radionuclides from some sh species of the Izmir, showing that the
measured activities in the species that feed on plankton are much
higher than the average values (Ako zcan and Ug

ur, 2013). Strok and
Smodi
s stated that the pelagic environment and plankton feeding
 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37 35

contribute signicantly to 210Po accumulation. They also reported
that the larger the animal, the lower the 210Po activity concentra-
tion. This is due to the slower metabolism of the larger, older, and


heavier animals (Strok and Smodi
s, 2011). Laboratory experiments
involving foods containing various natural concentrations of 210Po
showed that the 210Po content of a marine organism reects the
210
Po concentration in the food it eats and the process of incorpo-
ration of 210Po from the food into the sh is faster for the anchovy
than for other species, proceeding on a time-scale of 2e4 days
(Cherry et al., 1989).
Polonium-210 concentrations in sh muscle (except anchovy)
ranged from 0.8 to 5.26 Bq kg
1 (w.w.) in the four species of pelagic
sh and 0.51 0.12 Bq kg
1 (w.w.) in the demersal sh. Polonium-
210 concentration was highest in the viscera, which included in-
ternal organs and stomach contents. Polonium-210 concentrations
in the viscera and skin of sh were 49.6e2236 and 6.45e50.8 Bq
kg
1 (w.w.), respectively. Olive ounder, the demersal sh species,
had the highest 210Po concentration in the internal organs,
excluding the liver and gall bladder. Polonium-210 concentration in
the viscera of olive ounder was 2236 242 Bq kg
1 (w.w.) and was
ten times and three orders of magnitude higher than that in liver
and that in muscle, respectively. This high 210Po concentration in
the viscera of olive ounder may come from their diet, which in-
cludes crustaceans, polychaetes, and other taxa that contain high
210
Po concentrations.
The 210Po CFs in sh muscle varied widely from 0.7 to 52  103.
The CFs in pelagic sh (except anchovy) were 1.1e7.4  103, com-
parable with the recommended value of 2  103 in the fraction of
sh intended for human consumption (IAEA, 2004).
3.4. Dose estimation from seafood consumption
The annual effective dose of 210Po from seafood consumption by
an adult was estimated from the 210Po concentrations measured in
edible parts of macroalgae, crustaceans, molluscs, and sh in this
study. The average daily supply of seafood per capita includes one
hundred species and is 64.8 8.5, 35.4 6.8, and 30.0 10.5 g
day
1 for sh, shellsh including crustaceans and molluscs, and
macroalgae, respectively, in the Republic of Korea (KREI, 2012).
Although few species of sh, shellsh, and macroalgae were
investigated in this study, they account for 37, 64, and 72% of the
total annual per capita supply of these groups. The minimum,
maximum, and average 210Po concentrations in the edible portions
were used to assess the effect of natural variations on the effective
dose. Anchovy was considered separately because it is consumed
primarily in a broth made from dried salted sh. To calculate dose,
the ingestion dose coefcient of 1.2 mSv Bq
1 for an adult was used
(UNSCEAR, 2000). A delay factor of 0.6 (Aarkrog et al., 1997) was
applied to account for time elapsed between catch and consump-
tion, owing to the 138 d half-life of 210Po.
The annual effective dose for an individual from seafood con-
sumption was calculated as follows:
X
AED MF  eT  Ai  Ii (1)
i
where AED is the annual committed effective dose (mSv y
1), MF is a
weighted factor to account for the delay between catch and con-
sumption, e(T) is an effective dose coefcient (1.2 mSv Bq
1), Ai is
the activity concentration of 210Po in the edible tissues of seafood
products (Bq kg
1 (w.w)), and Ii is the annual intake rate of mac-
roalgae, shellsh, and sh per individual in the Republic of Korea
(kg y
1). Intake rate was calculated from per capita consumption
and the rate of edible parts in each category (Yamamoto et al.,
1994).
The annual effective dose of 210Po per adult individual from the
ingestion of seafood (except anchovy) was estimated to be 94
(average), 19 (minimum), and 189 mSv y
1 (maximum) (Table 6).
The dose from shellsh accounted for 42e71% of the average total
dose owing to the relatively high 210Po activity concentration in
shellsh, even though they accounted for only 14% of the total
seafood consumption. The dose for 210Po from the ingestion of
seafood estimated in this study may be compared with results from
other studies: 19 mSv y
1 in Ireland (Pollard et al., 1998), 45.6 mSv


y
1 in Slovenia (Strok and Smodi
s, 2011), 129 mSv y
1 from the
ingestion of molluscs and sh in France (Connan et al., 2007),
700 mSv y
1 in countries around the Baltic Sea (Nielsen et al., 1999),
and 50e200 mSv y
1 in Venice (Jia et al., 2003).
Assuming that anchovy is consumed in the same manner as
other seafood, the dose from the ingestion of anchovy would be 307
(average), 80 (minimum), and 534 mSv y
1 (maximum). These
values are two or three times greater than the total dose from
seafood excluding anchovy, even though anchovies represent just
10% of the total seafood supply. Anchovy's high dose may reect the
fact that its 210Po concentration is several times higher than that of
shellsh, which have the highest concentration among seafood
excluding anchovy. Polonium-210 from anchovy consumption may
depend on when the sh are caught and the preparation and
storage methods before ingestion. Polonium-210 has a short half-
life, so it may be minimally present in anchovy broth as typically
prepared in Korean cuisine. The dose of 210Po from anchovy needs
to be more precisely assessed.
4. Conclusions
210
Po concentrations in plankton from Korean coastal waters
ranged from 32 to 137 Bq kg
1 (w.w.) and were higher in winter
than summer. 210Po concentration in a small plankton size fraction
(20e300 mm) was somewhat higher than that in a large plankton
size fraction (>300 mm) in winter when diatom species were

Table 6
210
Annual Effective dose for the adult consumer in Republic of Korea by the ingestion of Po from seafood.

1
1
Category Supply (kg p y ) Rate of edible part Activity concentration Annual effective dose (mSv y
1)
(Bq kg
1 (w.w))

Min. Avg. Max. Min. Avg. Max.

Macroalgae 11.0 0.9 0.97 1.20 1.43 7 9 10

Shellsh 12.9 0.3 2.84 21.7 47.8 8 61 133
Fisha 18.9 0.6 0.51 3.04 5.56 4 25 45
Anchovyb 4.8 0.6 38.9 149 258 80 307 534
Total seafoodc 42.8 19 94 189
a
Fish except anchovy.
b
Assumed the case anchovy is consumed by same ways with other seafood.
c
Total seafood except anchovy.
36 S.H. Kim et al. / Journal of Environmental Radioactivity 174 (2017) 30e37
dominant, but the opposite was observed in summer when di-
noagellates were dominant. 210Po concentration in the whole
body of anchovy varied from 59 to 392 Bq kg
1 (w.w.), which was
higher than that in plankton. 210Po concentrations in two species of
macroalgae, laver and sea mustard, were 1.43 0.21 and 0.97 0.13
Bq kg
1 (w.w.), respectively. 210Po concentration in the muscle and
viscera of abalone was 2.93 0.86 and 1495 484 Bq kg
1 (w.w.),
respectively, and was higher in both than in macroalgae, which is
the primary food source for abalone. 210Po concentration in red-
banded lobster was 2.84 0.23 Bq kg
1 (w.w.) in muscle, 46 10
Bq kg
1 (w.w.) in the exoskeleton, and 906 226 Bq kg
1 (w.w.) in
the viscera, respectively. The percentages of 210Po in each part
relative to the total amount of 210Po in the whole body were 0.6,
12.2, and 87.2% in muscle, exoskeleton, and viscera, respectively.
Most of the 210Po burden in the body of red-banded lobster was
contributed through diet to the viscera. 210Po concentrations in the
whole esh of mussel and oyster collected in same location on the
same date were similar to each other, 47.8 5.9 and 45.3 7.1 Bq
kg
1 (w.w.), respectively. 210Po concentration in the muscle of ve
species of sh (not including anchovy) ranged from 0.51 to 5.56 Bq
kg
1 (w.w.) and was the lowest in a demersal species. 210Po con-
centrations in the viscera and skin of sh were 49.6e2236 and
6.45e50.8 Bq kg
1 (w.w.), respectively. 210Po in sh was enriched
from one to three orders of magnitude higher in viscera than in
muscle. A biomagnication of 210Po between trophic levels from
plankton to anchovy and from macroalgae to abalone is strongly
suggested.
The annual effective dose of 210Po per adult individual from the
ingestion of seafood excluding anchovy in the Republic of Korea
was estimated to be 94, 19, and 189 mSv y
1 for the average, min-
imum, and maximum. Forty-two to seventy-one percent of the
total dose was contributed through shellsh consumption. The
dose effect from anchovy had to be considered separately owing to
its consumption as a broth prepared from dried sh. Although it
had a high 210Po concentration, the dose from anchovy needs to be
assessed more precisely.
Acknowledgments
An earlier version of this manuscript was greatly improved by
incorporating two anonymous reviewers' comments and sugges-
tions. This work was funded by grants from the Korea Institute of
Ocean Science & Technology (PE99403) and the Korean Ministry of
Food and Drug Safety (PG48320).
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