Journal of Radloanalytical and Nuelear Chemistry, Articles, VoL 178, No.

1 (1994) 81-90

POLONIUM-210 AND LEAD-210 IN MARINE ORGANISMS:

INTAKE LEVELS FOR JAPANESE
M. YAMAMOTO,* T. ABE,** J. KUWABARA,* K. KOMURA,* K. UENO,* and Y. TAKIZAWA**

*Low Level Radioactivity Laboratory, Kanazawa University, Tatsunokuchi, lshikawa 923-12 (Japan)
**Akita University School of Medicine, 1-1-1, Hondo, Akita.shi 010 (Japan)

(Received June 15, 1993)

The concentrations of 210po and 210pb were detemained in about 30 species of marine organisms
collected mainly from the north-eastern region of Japan to know the levels and distributions of these
radionuclides and to estimate their intake levels from marine foods. 210po and 210pb showed a wide
range of concentration in species: 0.6-26 and 0.04-0.54 Bq/kg (wet wt) in fishes, 0.5-220 and
0.2-43 Bq/kg (wet wt) in molluscs, eehinodermsand chordatas, and 2.8--4.3 and 0.4--1.3 Bq/kg (wet
wt) in algae, respectively. Higher accumulation of 210po relative to 210pb was found in all of the samples
analyzed. The intake levels of 210po and 210pb by marine foods consumption were roughly estimated
to be 0.48-0.69 and 0.022--0.042 Bq/d per person, respectively, on the basis of the statistical data on
the consumption of seafood and/or production rates of marine foods.

The nuclides 21~ (138.38 d, tx) and 21~ (22.3 y, 13-) are the last radioactive
members of the 238Useries, and present widely in the environment mainly as a natural
fallout from the decay of 222Rn in the atmosphere. According to the 1988 UNSCEAR
Report, l this pair is estimated to contribute about 8% of natural internal radiation dose
to man. These radionuclides are transferred to the human body via inhalation and/or
ingestion of food and water. Ingestion of food is recognized to be the most important
route of these nuclides to man. In general, the concentrations of 21~ and 21~ are
relatively low in meat and milk products, medium in vegetables and cereals, and much
higher in most of the marine organisms. 2
It is well known that Japanese people take amimal protein mainly through marine
foods. Therefore, Japanese living on seafood may be expected to have high intake of
21~ and 21~ Data on dietary intake of 21~ and 21~ are, however, very scarce in
Japan and only a few other data are available. ~6 In this context, it seems indispensable
to estimate the intake levels of 2~~ and 21~ through marine foods consumption,
which is the traditional dietary habit for Japanese.
In the present paper, we report the results of measurements of 2WPo and 21~ in
about 30 species of marine organisms collected mainly from the north-eastern region of
Japan. The study is very important not only to evaluate the levels and distributions of
2WPo and 21~ in marine organisms in Japanese waters but also to estimate the intake
levels of these n~clides by the people consuming large amounts of seafood.

Elsevier Sequoia S. A., Lausanne

Akaddmiai Kiadd, Budapest

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M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

Materials and methods

Samples: Most of the samples were collected during the years 1988-t990 from the
north-eastern region of Japan. Some samples were obtained by purchase from
commercial suppliers, the sampling date and catch region being guaranteed. Fishes were
dissected into muscle and remainder, and only muscle was used to analysis. Shellfish
were, whenever possible, dissected into muscle and viscera. All samples were
oven-dried at 80-90 ~ or freeze-dried and then mixed homogeneously.
Analytical procedures: Aliquots of the homogenized samples, 1-20 g dry weight,
were subjected to radiochemical analysis of 21~ and 21~ using 2~ as a yield tracer
of polonium. The sample was carefully decomposed by wet-ashing with HNO3, H20 2
and HCIO4, followed by HCI. The residue was then dissolved in 100-200 ml of 0.5M
HCI with wanning, and several 10 rag's of ascorbic acid were added to the solution.
Polonium was spontaneously deposited on a polished silver disc (the backside of which
was coated with heat-resistant tape) put in this solution for more than 6 hours at
70-90 ~ (time : tl). After the first deposition of polonium, the 0.5M HCI solution was
gently evaporated to dryness with the addition of small amounts of HNO 3 and H202.
The residue was dissolved in about 50 ml of 10M HCI, and the solution was passed
through a Dowex l-X8 anion exchange column to remove completely the polonium
remaining after the first deposition of polonium. The column was washed thoroughly
with about 50 ml of 10M HCI (time : t2). Lead is not adsorbed on the column under
these conditions, while Po is strongly adsorbed. 2~ was spiked to the effluent
(usually about 100 ml) from the column, and the solution was stored for 3-6 months to
allow 21~ ingrowth from the 2t~ contained in the solution. The 21~ grown from
21~ was coprecipitated with Fe(OH) 3, and deposited on another silver disc by the
above mentioned procedures (time : ts).
Measurements: The activity of polonium (21~ and 2~ deposited on the silver
disc was measured by using a Si(Au) surface barrier detector with a 450 or 500 mm 2
active area, coupled with a 1K channel pulse-height analyzer.
The concentrations of 21~ (Do) and 21~ (F0) at the sampling date (to) were
calculated using the following equations:

Oo=fl F2

G =f2' (F1 -f3' Do)

were F 1 - activity of 21~ (mBq/g) at time t l,
F 2 - activity of ingrowth 2101)O(mBq/g) at time t3 for the measurement
of 210pb,

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 M. YAMAMOTOet al.: POLONIUM-210AND LEAD-210IN MARINE

f l - factor to correct the growth of 21~
to t 3,
f2 - factor to correct the decay of 21~
f3 - factor to correct the growth of 21~
to to q.
The factors fl a n d f 3 were calculated by using
growth of three radionuclides, that is, 21~ 21~
from 21~ in the period from t2
in the period from to to t 1,
from 2t~ in the period from
Beteman's equation for the decay and
and 2t~

Results and discussion

The analytical data obtained from the measurements of samples by several categories
are presented in Tables 1, 2, 3 and 4. All results are discussed on the basis of wet
weight.

Accumulation levels of 21Opoand 210pb

The 21~ concentrations in muscles of fishes, listed in Table l, range from 0.6 to
26.3 Bq/kg (a factor of 44), while the 21~ concentrations vary over a range of only
18, from 0.03 to 0.54 Bq/kg. 21~ concentration is much lower than its granddaughter
21~ and resultant 21~176 activity ratios range from 5 to 149. The data on
molluscs, echinoderms and chordatas given in Table 2 show a wide range of 21~
concentrations from 0.5 to 220 Bq/kg, the higher values being found in viscera of
shellfish, Batillus cornutus and Neptunea polycostata, and the lower values in Octopus
vulgaris and in muscle of Buccinum striatissimum. The 2t~ values range from 0.21
Bq/kg in total soft tissues of Meretrix lusoria to 42.6 Bq/kg in viscera of Batillus
cormutus. The 21~176 ratios ranging from 1 to 57 as a whole seem to be lower than
those for fishes given in Table 1. Since higher concentrations of 21~ and 21~ were
found in viscera of shellfish (Batillus cornutus and Neptunea polycostata) analyzed
here, 21~ and 2t~ distributions between soft tissues with Patinopecten yessoensis
were studied. The results are presented in Table 3. The 21~ concentration in
hepatopancreas is as high as 479 Bq/kg, which corresponds to 86% of the total 21~
content of the organism. Similarly, 2t~ concentration reaches 6.1 Bq/kg in
hepatopancreas, and its content contributes 54% of the total 2t~ Both 21~ and 2Z~
concentrations in the organs analyzed decrease as follows: hepatopancreas > gonads >
gills > mantle -- adductor. The results that 21~ is concentrated highly in
hepatopancreas, accompanied by a lower accumulation of 21~ are consistent with the
results found already in several marine organisms by FOLLSOM et al.,7 HEYRAUD et
al. 8 and CHERRY et al.9-12 The concentrations of 2t~ and 21~ in algae shown in
Table 4 lie in the relatively narrow ranges of 2.8-4.3 and 0.43-1.32 Bq/kg, respectively.

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M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

=]

~ (',,I
~ ~ ~ ~ + l ~ + f ~

~o

[-,~

l.

[
8
s

.=

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 M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

e~
- ~ ~ ' ' ~ B- ~ _ - - N

,0
r
+1
o.
t~

d
-H-,I-I-H-H-H-H-H-H-I-I-I-I-H-H-I-I-H-I-I 44 44

v
'-o

~=~

44

=o ('4
r
44

t-q

e,
G !
td
~ ~i~ ~
.E ~ I
.~
[
r~
to

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M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

Table 3
Distribution of 210po and 210pb in Hotate Patinopecten yessoensis
% of total content
Tissue % of total 210po-+ lff*, 210pb_+la*,
o r organ weight Bq/kg (wet wt) Bq/kg (wet wt) 210po 210pb

Adductor 41 3.5 + 0.2 0.21 + 0.03 2.7 7.8

Mantle 14.3 3.5 + 0.2 0.27 + 0.04 0.9 3.5
Gills 13.5 14.6 + 0.9 0.48 + 0.05 3.7 6.0
Gonards 21.5 16.9 + 1.4 1.45 :l: 0.13 6.7 28.4
Hepatopancreas 9.7 479 + 27 6.14 + 0.41 86.0 54.3

Total 100 54.0 + 2.6 0.56 + 0.05 100 100

*Propagated counting error.

Overall, the data here show that the concentrations of both nuclides range over two
orders of magnitude. Surprisingly, no data, except one data on 21~ has been reported
as yet for both of 21~ and 21~ in marine organisms in Japanese waters. SHIMIZU 13
has measured 21~ contents in about 40 species of marine organisms collected by
trawling during the years 1981-1983 mainly from the offshore in Choshi, Chiba
Prefecture, facing the Pacific Ocean. The reported 21~ concentrations ranged from
0.03 to 0.3 Bq/kg in muscle of fishes and from 0.3 to 1.5 Bq/kg in muscle of molluscs.
The 21~ measured here for fishes and molluscs has activities within the ranges found
by SHIMIZU. 13 On the other hand, since no data on 21~ in marine organisms in
Japanese waters have been reported, the present 21~ data are, believed to be very
important for the fact that these data begin to provide a baseline of 21~ concentrations
in marine organisms in Japanese waters.

Comparison with other radionuclides

Besides 21~ and 21~ naturally occuring and artificial radionuclides such as 238U,
232Th, 226Ra, 4~ 137Cs, etc., were measured to compare their accumulation levels with
those for 21~ and 2~~ Such studies are necessary not only in assessing the dose to
humans via the consumption of seafood but also in providing useful analogous
information on the behavior of transuranic nuclides. Analytical techniques used have
been described previously. 14 Briefly, "y-ray emitting nuclides were determined by
"y-spectrometry using Ge detector. Alpha-my emitting nuclides such as 238U, 232Th and
226Ra were determined by a-spectrometry after chemical separation. The contents of
radionuclides measured in some species are shown in Table 5. As is seen from this
table, 21~ in viscera of Batillus cornutus exhibits the highest activity among the

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 M. Y A M A M O T O et al.: P O L O N I U M - 2 1 0 A N D LEAD-210 IN M A R I N E

~ o . . o o . . .--

+l +1 +1 +t O 0

b
+l r~
J +I +I +I +I

~ . ~.
+I -H +I -hl

4-1 oo .oo~ , , .~o

~.r,I
O
0 0 0 ~ 0
i
e,z3
v

r
o o . ' o o ~o

@1 ~ ~ ~ @1 ~ ~ ~ ~ ~ ~

~oo " ~

dddd c~ ~ c ~ d d ~ d
-H -H -H -H -.H "H "H +1 -I-I +t §

d d

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M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

radionuclides detected, although 4~ is the most abundant radionuclide in most of the

samples. Concentrations of the nuclides such as 232Th and 226Raare significantly lower
than those of 4~ 21~ and 2~~ It is evident here that marine organisms have a great
ability to accumulate 21~ and 21~ Thus, assessment of internal radiation dose via
marine food consumption is subsequently dominated by the contribution of natural
radionuclides 21~ and 21~ in particular 21~

Intake levels from marine food consumption

According to the 1977 UNSCER Report,2 Japanese people are classified as an
example of high 21~ intake by marine foods consumption. It is, therefore, very
important to evaluate the daily intake levels of 21~ and 21~ by ingestion of marine
foods. In Japan, one data on estimation of 2~~ intake by marine food consumption has
been reported. SHIMIZU13 has measured 21~ contents in 18 processed marine products
other than the about 40 species of marine organisms mentioned above. Using these data,
daffy intake of 21~ by ingestion of marine foods was estimated to be around 0.037 Bq/d
per person based on statistical data on the annual production of seafood by categories
and/or annual supply of seafood calculated from an average food supply in Japan.
Similarly, 21~ and 21~ ingestions from marine foods were calculated using the
geometric mean values of 2~~ and ~~ concentrations in each categories of marine
organisms measured here and the statistical data on annual production of seafood15 in a
similar manner as SHIMIZU (Method-I) and also on consumption rates of individual
species of marine organisms 16 (Method-II). The results thus obtained are presented in
Table 6. As is seen from this table, intake levels are in the range from 0.022 to 0.042
Bq/d per person for 21~ and from 0.48 to 0.69 Bq/d per person for 21~ The present
values for 21~ are close to the value (about 0.037 Bq/d per person) estimated by
SHIMIZU. On the other hand, as for 2~~ the intake level is about 10 to 20 times
higher than those of 21~ The intake level for 2~~ by Method I may be considerably
overestimated because all of the freshly caught marine organisms are not always
consumed immediately, and a part of them are used as processed marine products.
During their processed and/or stored periods most of the excess 2~~ relative to 2~~
would decay to lower concentrations, although some 21~ is produced by the decay of
21~ In case of 21~ such considerations seem to be not necessary because the
half-life of this nuclide is relatively long. Contrary to Method I, the values for 21~ and
21~ calculated by Method II may be underestimated because of the lack of a
consideration on the ingestion of both nuclides from processed marine products. It
should be borne in mind that these figures were calculated by using only a few data for
2~~ and 21~ obtained here. It is, moreover, not sure whether the marine organisms
used in the present estimation were representative for both 21~ and 21~ because the

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 M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

Table 6
Estimation of daily intake of 210po and 210pb from marine foods. Geometric mean was used
as average concentrations of 210po and 210pb for each category, respectively

Method I

210po 210pb
Rate of
Production*
Category (1000 ton) edible Content, Amount, Content, Amount,
part Bq/kg wet 108 Bq, % Bq/kg wet 108 Bq, %

Fish 9949 0.6 4.2 250.7 83.1 0.14 8.60 46.7

Cephalopad 712 0.8 1.0 5.7 1.8 0.68 3.87 21.0
Shellfish 832 0.2 11.1 18.5 6.1 0.60 1.00 5.4
Cmstacean 119 0.4 4.2** 2.0 0.7 0.14"* 0.07 0.4
Seaweeds 798 0.9 3.5 25.1 8.3 0.68 4.88 26.5
Total 302.0 100 18.42 100
Bq/d/p*** 0.69 0.042

*From 1988 annual report of production statistics on fishery and aquaculture 15

**Assumed to be equal to fish.
***Total population: one hundred and twenty million.

Method II

Category Daily intake,* 210po 210pb 210po 210pb

g/d/p Bq/kg wet Bq/kg wet Bq/d/p Bq/d/p

Fish
Tuna 6.3 25.3 0.22 0.159 0.0014
Porgy, Plaice 7.4 8.6 0.I0 0.064 0.0007
Saurel, Sardine I I.I 12.6 0.26 0.140 0.0029
Salmon, Trout** 3 1.5 0.18 0.004 0.0005
Others 11.7 3.0 0.13 0.035 0.0015
Squid, Octopus 13 1.0 0.68 0.013 0.0088
Shellfish 4.4 11.1 0.60 0.049 0.0026
Seaweeds 5.6 3.6 0.68 0.020 0.0038
Total 0.48 0.022

*Averge daily intake in Ja~aanese.16

**Contents of 210po and 21vpb in Madara (Godus macrocephalus)and Hotsuke (Pleurogrammusazonus)
were used as substitute of this category.

scunples were limited to the north-eastern region. Further data are needed to estimate
reliable intake levels of 2~~ and 2t~ for Japanese by marine foods consumption.
Nevertheless, it is worth pointing out that Japanese people may ingest excess of 21~

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M. YAMAMOTO et al.: POLONIUM-210 AND LEAD-210 IN MARINE

relative to its grandparent 21~ from marine foods. Such a situation may be similar to
the excess zl~ intake by inhabitants of the Arctic and Sub-arctic regions of Alaska,
Canada, Scandinavia, etc., who consume large amounts of the meat of reindeer.

References

1. United Nations Scientific Committee on the Effects of Atomic Radiation, Ionizing radiation: Sources and
Biological. Effects, 1988 report to the general assembly, with annexes, United Nations, New York, 1988.
2. United Nations Scientific Committee on the Effects of Atomic Radiation, Ionizing radiation: Sources and
Biological Effects, 1977 report to the general assembly, 1977.
3. N. TAKATA, H. WATANABE, R. ICHIKAWA, J. Radiat. Res., 9 (1968) 29.
4. H. OKABAYASHI, M. SUZUKI-YASUMOTO, S. HONGO, S. WATANABE, J. Radiat. Res., 16 (1975)
142.
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6. S. HISAMATSU, Y. TAKIZAWA, K. KOMURA, T. TADA, Radioisotopes, 41 (1992) 574.
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13. M. SHIMIZU, in: 1982 Report of the Project: Studies on the distribution and behaviour of natural and
artificial radionuclides, Nuclear Safety Research Association, 1983, p. 42.
14. M. YAMAMOTO, in: Approach to the Nuclear Safety for Environment and Members of Public: Ecological
Behavior, Metabolism, Dose Evaluation of Radiounclides, T. iwakura, T. Nakajima, (Eds), Proc 20th
National Institute of Radiological Sciences, Seminar on Environmental Research, Chiba Japan, 1993, p.
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15. Ministry of Agriculture, Forestry and Fisheries, 1988 Annual Report of Production Statistics on Fishery
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16. Ministry of Health and Welfare, Japan, 1982, Showa 57 Neuban Kokumin Eiyon No Genjo (Current Status
of National Nutrition, 1982), Dai-Ichi Shuppan, Tokyo, 1982.

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