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1 Current Knowledge Concerning the Impacts of the Fukushima Daiichi Nuclear Power Plant accident on the environment *Abubakar Sadiq Aliyu a,b , Junwen Wu c , Timothy Alexander Mousseau d Ahmad Termizi Ramli a a Department of Physics, Universiti Teknologi Malaysia, 81310 Johor Baru, Malaysia b Department of Physics, Nasarawa State University Keffi, P.M.B 1022, Keffi, Nigeria. c State Key Laboratory of Marine Environmental Science, Xiamen University, Xiamen 361005, China d Department of Biological Sciences and the Environment and Sustainability Program, University of South Carolina, Columbia, SC 29208 *Corresponding author E-mail: [email protected] or [email protected]. HP: +601116167589 (A.A Sadiq). Abstract It is now more than four years since the Fukushima nuclear accident; how it affects the environment will continue to be an issue of great concern to the public and energy policy makers. Thus, scientists around the world have been investigating the impacts of the accident and the question of how the Fukushima nuclear accident has affected man and his environment will remain one of great interest for centuries. Here, we review the current understanding of the Fukushima nuclear accident’s interactions with the environment, which includes studies on the source term assessment, radioactive contamination of the atmosphere, soil and the marine environment. This review addresses some fundamental scientific questions concerning the environmental impacts of Fukushima nuclear accident with the aim of stimulating further discussion on the topic. Finally, the paper presents a concise discussion of how the released radionuclides from the Fukushima nuclear accident could be used as tracers for studying environmental processes. Keywords: Fukushima nuclear accident, environmental effect, radioactive contamination, 137 Cs

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Page 1: Current Knowledge Concerning the Impacts of the Fukushima ...cricket.biol.sc.edu/chernobyl/papers/Energy & Env. Sci Manuscript (Aliyu, Wu, Mousseau...1 Current Knowledge Concerning

1

Current Knowledge Concerning the Impacts of the Fukushima Daiichi

Nuclear Power Plant accident on the environment

*Abubakar Sadiq Aliyu a,b

, Junwen Wu c, Timothy Alexander Mousseau

d Ahmad Termizi Ramli

a

a Department of Physics, Universiti Teknologi Malaysia, 81310 Johor Baru, Malaysia

b Department of Physics, Nasarawa State University Keffi, P.M.B 1022, Keffi, Nigeria.

c State Key Laboratory of Marine Environmental Science, Xiamen University, Xiamen 361005, China

d Department of Biological Sciences and the Environment and Sustainability Program, University of South Carolina,

Columbia, SC 29208

*Corresponding author E-mail: [email protected] or [email protected]. HP:

+601116167589 (A.A Sadiq).

Abstract

It is now more than four years since the Fukushima nuclear accident; how it affects

the environment will continue to be an issue of great concern to the public and energy

policy makers. Thus, scientists around the world have been investigating the impacts

of the accident and the question of how the Fukushima nuclear accident has affected

man and his environment will remain one of great interest for centuries. Here, we

review the current understanding of the Fukushima nuclear accident’s interactions

with the environment, which includes studies on the source term assessment,

radioactive contamination of the atmosphere, soil and the marine environment. This

review addresses some fundamental scientific questions concerning the environmental

impacts of Fukushima nuclear accident with the aim of stimulating further discussion

on the topic. Finally, the paper presents a concise discussion of how the released

radionuclides from the Fukushima nuclear accident could be used as tracers for

studying environmental processes.

Keywords: Fukushima nuclear accident, environmental effect, radioactive

contamination, 137

Cs

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1. Introduction

The confluence of a magnitude 9.0 earthquake, a subsequent gigantic tsunami,

and design flaws related to the plant site and emergency cooling systems resulted in

the Fukushima Dai-ichi nuclear power plant accident (FDNPP) on March 11, 2011. As

a result, enormous quantities of radionuclides were released into the atmosphere and

the ocean 1-3

. Major radionuclides released to the atmosphere included 131

I (t1/2=8.02

d), 134

Cs (t1/2=2.06 y), 137

Cs (t1/2=30.07 y) and 90

Sr (t1/2=28.78 y), which were then

distributed globally 4 leading to the contamination of both terrestrial and marine

environments. Additionally, large amounts of radionuclides were directly released into

the ocean as liquid wastes via discharge from the FDNPP, which widely contaminated

seawater in areas offshore of Japan. The total amounts of 137

Cs and 90

Sr directly

released to the sea have been estimated to be 1~42 PBq (1PBq=1015

Bq) 5-7

and

0.1~2.2 PBq 8, respectively. Obviously, there has been considerable uncertainty

concerning the total amounts released from the FDNPP 1, 9-11

. It is clear that currently

there is a poor understanding about some fundamental questions of the FDNPP (for

example, the release amounts and rate of radionuclides); hence, we cannot derive

reliable conclusions concerning the impacts of FDNPP on the environment.

Answering some of these fundamental questions will lead to a better understanding of

how the uncontrolled release of radioactive fission products from the FDNPP has and

will continue to affect both human and non-human biota 12

.

This article will summarize the current state of understanding about the major

radionuclides derived from the FDNPP, including the amounts released and isotopic

composition, the effects on environment (seawater, sediment, terrestrial and marine

biota), and their application as tracers for environmental processes. This paper also

aims to present the results of global field measurements of radionuclides stemming

from Fukushima, which were obtained from the literature. This field measurement

data may be used in the investigation of environmental process as well as the basis for

conducting country-wise comparative impacts assessment of the FDNPP accident.

2. Source term assessment

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Following the Fukushima nuclear accident, there was tremendous public

concern about the release of radionuclides into the environment (i.e. atmosphere

and ocean). Several research institutes and scientists conducted many studies in an

attempt to estimate the total release amounts as a measure of the source term. For

instance, the Japanese government estimated the source term for 131

I and 137

Cs to be

160 PBq and 15 PBq ,respectively as the total atmospheric releases of radioactivity

from the FDNPP 13

. The Nuclear Safety Commission of Japan (NSCJ) 2 estimated

that the total amounts of 131

I and 137

Cs discharged into the atmosphere were 150

PBq and 12 PBq, respectively. Masson, et al. 4 estimated that

131I (153 PBq) and

137Cs (13 PBq) were released to the atmosphere. Other researchers have reported the

total emission of 137

Cs as high as 13~35.8 PBq 1, 14

. To estimate the source terms

of radioactive cesium (137

Cs) and iodine (131

I), Chino, et al. 1 adopted an

estimation method to compute the source terms using an atmospheric dispersion

model. Their results were comparable to that of the Ministry of Education,

Culture, Sports, Science and Technology, Japan 15

. The authors verified the

validity of this technique in later studies 16, 17

. In a most recent study18

, the group

improved its computational methodology to account for limitations in their earlier

studies. The new study18

considered a new scheme of parameterizations for wet,

dry, and fog-water depositions of both gaseous and particulate radionuclides.

Environmental data that are coupled into the new model include those from other

part of Japan and the Pacific Ocean. The new study18

methodology estimated the

total release amount of total

131I and

137Cs to be 151.0 and 14.5 PBq, respectively

considering environmental data from both land and sea (New-landsea). For the new

land data, the total release amount for total 131

I and 137

Cs are ~ 27% and ~32% ,

respectively less than the results of the WINSPEEDI-II simulation that considered

New-landsea data. The reported total release amount of 131

I is in good agreement

with the estimate of the NSCJ 2 and lies within the range estimate for total release

amount of 131

I by this review ~ (150 – 160) PBq (See Table 1).

Additionally, the important source of ocean radioactive contamination was

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derived from direct discharge into the cooling waters at the NPP. Accurate estimation

of radioactive pollutants directly discharged into the sea is the basis for assessment of

the impact to the marine habitat. There have been many studies concerning this

question. Using a regional ocean model, Tsumune, et al. 6 estimated that the total

137Cs directly released to the ocean was 3.5 ± 0.7 PBq from March 26 to the end of

May, 2011. The total amounts of 137

Cs directly released into the ocean have been

estimated to range from 1 to 42 PBq 5-7

. We have summarized the total release

amounts of major radionuclides derived from the FDNPP and compared them with

global fallout and the source term from the Chernobyl accident (Table 1)8, 19, 20

.

Despite the uncertainty associated with the total release of fission products from

Fukushima, Table 1 depicts that the Chernobyl accident resulted in the largest

discharge of 137

Cs into the environment (85 PBq), and Fukushima resulted in the

largest accidental source term release to the ocean. Ten months later, in the winter of

2012, the mean value for water column inventories of Fukushima-derived

radiocesium (137

Cs) and bomb-derived 134

Cs were nearly equal. These values were

1020 ± 80 and 820 ± 120 Bq m-2

, respectively 21

.This suggests that the accident and

nuclear bomb testing had almost the same impacts on the Pacific Ocean during this

period.

Table1 Source terms of anthropogenic radionuclides in the atmosphere and the ocean

(PBq).

Radionuclide Global fallout Chernobyl Fukushima

atmosphere Ocean Atmosphere Ocean Atmosphere Ocean 131

I 1760 160

153

150 137

Cs 950 600 85 16 15 3.5±0.7

13 4

12 27±15 90

Sr 600 380 1 0.14 0.1

0.01 2.2 239,240

Pu 10.87 6.6 0.087 (1-2.4)×10-6

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3. Environmental effect

3.1 Atmosphere transportation

Vast amounts of radioactivity were emitted into the atmosphere by the accident

at the FDNPP, and the radioactive plume spread over the globe in the free troposphere

by the prevailing westerly winds 22-26

. Table 2 shows the results of measurements and

detection of Fukushima-derived radioactive fission products in receptor locations

(sampling points) around the globe. The readings are for air concentrations (in Bq m-

3), soil deposition (in Bq m

-3) and concentration in both fresh water and marine

environments (in Bq l-1

). The data in Table 2 may be used in the investigation of

environmental processes as well as basis for conducting country wise comparative

impacts assessment of the FDNPP accident.

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Table 2 Fukushima-derived anthropogenic radioisotopes detected in locations around

the world

Location,

Country

Media (Soil Air or Water): Activity concentrations of

radionuclide, ( r e f )

Japan

Air (Bq m-3

): 132

Te: 9.9, 131

I: 16.2, 134

Cs: 10.13, 137

Cs: 10.27, 129m

Te: 4.0, 136

Cs: 123 27

Soil(Bq m

-2):

137Cs: 9 0 0

28, 29

South Korea

Air (Bq m-3

): 131

I: 3.12 x 10-3

, 134

Cs: 1.19 x10-3

, 137

Cs: .25 x 10-3

30

Soil(Bq m

-2):

137Cs:649,

134Cs: 802

31

United States Air (Bq m-3

): 134

Cs: 1.11x 10-3

, 137

Cs: 1.18 x 10-3

, 131

I: 3.85 x 10-3

32

Krasnoyarsk (Russia) Water (Bql-1

): 131

I: 0.62, 137

Cs: 0.075, 134

Cs: 0.095 23

Thessaloniki (Greece)

Air (Bq m-3

): 131

I: 497 x 10-6

, 137

Cs: 145 x 10-6

, 134

Cs: 126 x 10-6

24

Water (Bql

-1):

131I: 0.7

23, 24

Ibaraki (Japan) Soil (Bqm-2

): 137

Cs: 1.4 x 104 33

China

Air (Bq m-3

): 131

I: 1720 x 10-3

, 134

Cs: 247 x 10-3

, 137

Cs: 289 x 10-3

, 136

Cs:

23 x 10-3

34

Soil(Bq kg-1

): 131

I: 2.68 34

Milan (Italy) Air (Bq m

-3):

131I: ~4.2 x 10

-4,

137Cs: ~9.4 x 10

-5,

134Cs: 8 x 10

-5

35

Czech Republic Air (Bq m-3

): 131

I: 5.6 x 10-3

, 137

Cs: 0.72 x 10-3

, 134

Cs: 0.64 x10-3

36

Lithuania Air (Bq m-3

): 131

I: 3700 x 10-6

, 137

Cs : 1040 x 10-6

37, 38

France Air (Bq m-3

): 131

I: 2.4 x 10-3

, 134

Cs: 0.2 x 10-3

, 137

Cs: 0.7 x 10-3

39, 40

Bratislava (Slovakia) Air (Bq m-3

): 131

I: 0.5 x 10-3

, 137

Cs: 0.07 x 10-3

41

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Spain Air (Bq m

-3):

131I: 3080 x 10

-6,

137Cs: 690 x 10

-6,

134Cs: 620 x 10

-6,

132Te:

330 x 10-3

42

Serbia Air (Bq m-3

): 131

I: 2.8 x 10-3

, 137

Cs: 0.21 x 10-3

43

Vietnam Air (Bq m-3

): 131

I: 193 x 10-6

, 134

Cs: 33 x 10-6

, 137

Cs: 37 x 10-6

44

UK Grass (Bq kg-1

): dry matter for 131

I: 55, dry matter for 137

Cs: 8 45

Romania Water (Bq l-1

): 131

I: 1.61 46

Svalbard (Norway) Air (Bq m-3

): 131

I: 810 x 10-6

, 134

Cs: 659 x 10-6

, 137

Cs: 675 x 10-6

47

Lisbon (Portugal)

Air (Bq m-3

): 131

I: 1.47 x 10-3

, 137

Cs: 134 x 10-3

48

Soil (Bq m23

): 131

I: 1.03, 134

Cs: 0.65, 137

Cs: 0.74 48

Vancouver Island

(Canada)

Air (Bq m-3

): 133

Xe: 70 49

Finland Air (Bq m

-3):

131I: 11 x 10

-3,

134Cs: 0.39 x 10

-3,

137Cs: 0.47 x 10

-3,

136Cs: 30

x 10-3

, 129

Te: 148 x 10-3

, 129m

Te: 254 x 10-3

, 132

Te: 54 x10-3 50

Iberian Peninsula

Air (Bq m-3

): 131

I: 3.88 x10-3

, 132

I: 0.175 x 10-3

, 134

Cs: 0.193 x10-3

, 137

Cs:

1.0 x 10-3

51

Istanbul (Turkey) Air (Bq m-3

): 131

I: 1.11 x 10-3

, 134

Cs: 0.28 x 10-3

, 137

Cs: 0.26 x 10-3

52

Taiwan

Air (Bq m-3

): 131

I: 0.1 x 10-3

, 134

Cs: 1.13 x 10-3

, 137

Cs: 1.45 x 10-3

26

N:B Only maximum detected values were considered for all sampling

points.

Austria

Air (Bq m-3

): 131

I: 1.2 x 10-3

53

Rain water (Bq l-1

) : 131

I: 5.2 53

Hungary Air (Bq m-3

): 7Be: 10

-2,

131I: 3 x10

-3,

137Cs: 10

-4, 134

Cs: 10-4

54

Monaco Air (Bq m-3

): 131

I: 354 x 10-6

, 134

Cs: 30 x 10-6

, 137

Cs: 37 x 10-6

55

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Germany

Air (Bq m-3

): 131

I: 2.1 x10-3

25

Soil (Bq kg-1

): 131

I: 0.093, 137

Cs: 3.07, 134

Cs: 0.69 25

Darwin (Australia)

Air (Bq m-3

): 133

Xe: 12 x 10-3

No Fukushima-derived radio iodine and

cesium was detected in Australia 56

Krakow (Poland) Air (Bq m-3

): 131

I: 6.08 x 10-3

, 134

Cs: 0.50 x 10-3

, 137

Cs: 0.474 x 10-3

3 57

It has been estimated that it took radionuclides from FDNNP ~18 days to reach

locations around the globe 58

. This is much longer than the time (~10 days) it took for

the radiation clouds emitted from the Chernobyl accident to do the same 59

, and it is

longer than the time (~13 days) for Asian dust to go around the world 60

. It is known

that the largest portion of the radioactive plume from Fukushima was transported

through the atmosphere and deposited over the Pacific Ocean. This might have

resulted in the longer time for travel around the world as the space and temporal

variation of the boundary layer over the oceans is relatively slow. This is because the

surface temperature of the sea varies little during the diurnal cycle owing to large

mixing within the top layer of the ocean 61-63

.

Airborne radioactivity from FDNPP accident was detected at many laboratories

around the world and possible health effects from the radioactivity transported by the

radioactive plumes from Japan was of concern. In Japan, as of October 21 2011 (7

months after the accident), the air concentrations of 134

Cs and 137

Cs in Fukushima city

were still elevated to 613 µBq m-3

and 829 µBq m-3

, respectively 64

. Other prefectural

governments also conducted environmental radioactivity monitoring, which included

45 stations covering the Japanese Islands 65

. Outside Japan, as shown in Table 2,

radioactive materials were detected in Korea, Vietnam, Taiwan, U.S., Canada, and

Europe 4, 22, 26, 30, 66

. In Europe, the first signs of the radioactive cloud were detected on

March 19th, 2011 (slightly more than one week after the accident) while the first peak

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of activity level was observed between March 28th and 30th. Measurements have

shown that airborne activity levels are now of minimal concern for public health in

Europe 4. The activity concentrations of the radionuclides in the plume exponentially

decreased with downwind distance 58

due to deposition (dry and wet) and scavenging

67.

3.2 Soil deposition

Deposition of Fukushima-derived radionuclides on land mostly stemmed from

the release to the atmosphere of relatively volatile fission products, most importantly

137Cs,

134Cs and

131I and radioactive noble gases

68, which present a large risk for

internal radiation exposure via inhalation and ingestion of contaminated agricultural

crops, stock farming, and thus human life . The soils around the FDNPP and

neighboring prefectures have been extensively contaminated with 137

Cs and 134

Cs

depositions of more than 105 and 10

4 Bq m

-2, respectively

28, 68. Similarly,

Kinoshita, et al. 29

has also reported that the top soil deposition of 137

Cs in the

central-east Japan due to the Fukushima accident ranged from 0.4 to 900 kBq m-2

,

which are 0.06-130 times the cumulative deposition from the atmospheric nuclear test

(100-1000 Bq m-2

). It is estimated that a total of more than 5.6 PBq 137

Cs was

deposited over the Japanese Islands 28

. High activity concentrations of radionuclides

have been reported. For example, soil activities for 134

Cs and 137

Cs in the Iitate Village

area (located 25-45 km northwest of the Fukushima site) were 62400 and 72900 Bq

kg-1

, respectively 69

. As of March 2011, the top soil concentration of 137

Cs was

measured to be 80 kBq m-2

. The environmental external radiation dose rate before the

accident was approximately 0.05 µSv h-1

29

. Additionally, the radiation dose rate of

other prefectural areas due to the Fukushima accident have also been estimated, for

example, 1.14 µSv h-1

in Naka-Dori, 4.57 µSv h-1

in Iitate, 0.02 µSv h-1

in the region

between northern Ibaraki and eastern Saitama, and 0.23 µSv h-1

in southern Ibaraki

and northern Chiba prefectures 29

. This clearly demonstrates that large areas in eastern

and northern Japan were strongly contaminated by 137

Cs derived from Fukushima,

while in contrast, the western part of Japan was shielded by its mountainous terrain.

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However, as with Chernobyl, deposition was highly heterogeneous even within the

most contaminated areas e.g. 70, 71

with ground level readings ranging from 0.5 to >30 µSv h-1

within Namie township. The information on soil contamination which was detected in

countries in Asia, Europe and in North America is presented in Table 2. The advantage

of the information in Table 2 is that it is based on empirical environmental data and

not computer models. The advantages of empirical data stem from the fact that

dependence solely on environmental models may result in over or under estimation of

the impacts of the accident as it has been observed in the study of Hoeve and

Jacobson 11

. The authors 11

, estimated that there would be an additional 130 (15-1100)

and 180 (24-1800) cancer related mortalities and morbidities related to the Fukushima

radiological disaster, respectively with over 90% of the projected impacts occurring in

Japan. However, Beyea, et al. 72

argued that the failure by Hoeve and Jacobson 11

to

consider the long-term dose estimate from radiocesium in their studies may lead to

under estimation of the global effects of the accident. By including a more realistic

population perspective, Beyea, et al. 72

suggested that the mid-range estimate for the

number of future cancer mortalities due to Fukushima accident is probably closer to

1000 than 125. Recently, Evangeliou, et al. 73

developed a pioneering environmental

modeling study that considered numerous fission products. This study estimated that

cancer fatalities are likely to be fewer than 2000.

3.3 Marine environment

Other than fallout from atomic bomb testing, contamination of the marine

environment following the FDNPP accident represents the most important

anthropogenic radioactive release into the sea ever known. The radioactive marine

pollution came from atmospheric fallout onto the ocean, direct release of

contaminated water from the plant, and the transport of radioactive pollution from

leaching through contaminated soil. For instance, the total amount of 137

Cs directly

released to the ocean has been estimated as 1~42 PBq 5-7

. In the immediate vicinity of

the plant, the Cs levels of surface ocean at the discharge point are up to 103 times

higher activities than it has been (~1-2 Bq m-3

) 74

, with a peak of 68 kBq L-1

on

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April 6, 2011 75

. Certainly, dilution of the primary contaminant signal occurs quite

rapidly due to ocean mixing, particularly in the energetic coastal waters off Japan

where the Oyashio waters move south and interact with the rapidly flowing and

offshore meandering of the Kuroshio Current. These currents, tidal forces and eddies

mix the waters quite rapidly offshore. As a consequence, one month after the accident

the 137

Cs level decreased by a factor of 103.

Honda, et al. 76

reported that the 137

Cs activity in surface seawater ranged from

0.004 to 0.284 Bq kg-1

in the western North Pacific on 14 April to 5 May. Tsumune, et

al. 6 argued that if no additional releases occur, the effect of the

137Cs might be

smaller than that of global fallout in the North Pacific. The timescale of transport to

other basins is several decades. Thus, the effect of the 137

Cs release on other oceanic

basins might be negligible. With respect to dose effects on humans, Buesseler, et al. 75

calculated the dose due to direct exposure during human indirect contact with the

water to be 0.1 µSv d-1

when the 137

Cs level approaches 102 kBq m

-3, which is lower

than the average dose from all sources to the Japanese population of about 0.17µSv d-

1. Thus there is unlikely to be any significant direct external dose effect on humans via

this pathway.

Cesium-137 concentration in suspended solids (SS) from surface and subsurface

waters off western North Pacific has been measured by Honda, et al. 76

; it ranged

from 5.92 to 32.42 Bq kg-1

on a dry weight basis (kg-dw-1

). The same is true for 134

Cs.

Thus, it is likely that SS were contaminated with radionuclides from the FDNPP 76

.

The SS-seawater distribution coefficient (Kds: Bq kg-dw-1

for SS/Bq kg-1

for

seawater) was further estimated to be 200~4400, with an average of 2100. This

average Kds is comparable to the recommended Kds for open ocean (2000) reported 19

.

In terms of potential biological impacts, radiation doses in marine organisms are

generally dominated by the naturally occurring radionuclides 210

Po ( an alpha emitter)

and 40

K, even when organisms are exposed to anthropogenic radioactivity discharged

to coastal waters 77

. Fukushima-derived radiocesium was detected in zooplankton and

mescopelagic fish 78

, with the 137

Cs concentration in zooplankton off western North

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Pacific at 13.46~71.46 Bq kg-dw-1

, which is significantly higher than that of the

southern Baltic Sea and the northern Adriatic Sea one month after the Chernobyl

accident (0.4~5 Bq kg-ww-1

) 79, 80

. In contrast, the 137

Cs concentration in zooplankton

around Japan was less than 0.1 Bq kg-ww-1

during the last decade 81, 82

. Thus, the

observed concentrations were two orders of magnitude higher than before the

accident. Meanwhile, the concentration factor (CF, i.e. the ratio of the Cs

concentration of zooplankton to that of ambient seawater (Bq kg-ww-1/Bq kg-1

) was

calculated to be 200~840, which is an order of magnitude higher than the 10~100 of

previous observations 19, 81, 82

.

Buesseler, et al. 78

suggested that radiation risks of 137

Cs derived from the

FDNPP to marine organisms and human consumers of seafood are well below those

from natural radionuclides. Meanwhile, the total cesium levels in demersal (bottom-

dwelling) fish off Fukushima were investigated 83

, where the cesium levels in 40% of

fish were above the new regulatory limit (100 Bq kg-1

wet) set by Japan Ministry of

Agriculture 84

. However, this is lower than the new regulatory limit of cesium in fish

products in four prefectures (Iwate, Miyagi, Ibaraki and Chiba).

The effect of the FDNNP accident on marine products in Fukushima was also

assessed by Wada, et al. 85

. The authors concluded that the total activity

concentrations of radiocesium in marine products have decreased significantly.

However, the authors noted that higher activity concentrations have been observed in

shallower waters south of the FDNPP. Long-term monitoring of marine products

around the FDNPP is important before restarting the coastal fisheries 85

. For other

prefectures that are adjacent to Fukushima, Chen 86

reported the radioactivity level in

the fish products from these prefectures based on monitoring data of July 2013. The

activity concentrations of 134

Cs, and 137

Cs varied from 0.1 to 338 Bq kg-1

(average: 11

Bq kg-1

) and from 0.1 to 699 Bq kg-1

(average: 18 Bq kg-1

), respectively 86

. Three

years later, the dose rate to the most impacted fish species near the FDNPP have

remained above baseline levels and a theoretical human consumer of 50 kg of fish,

gathered a short distance (3 km) from the FDNPP in 2013, would have received a

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total committed effective dose of approximately 0.95 mSv y-1

with FDNPP

contributing ~14% of total committed effective dose 87

.

Numerous studies have assessed the impacts of the Fukushima accidents on the

marine and environment in both Japan and other countries 30, 88-93

. For instance, Aliyu

and co-authors concluded that within Japanese Coastal areas, the accident had heavier

damage to marine bionts compared to terrestrial flora and fauna. Even though many of

the studies outside Japan have demonstrated that the levels radiocesium in seafood

were not likely of discernible health effects 88

, further investigations of the marine

environment have continued in order to address public concern about the impact of

the accident.

Buck 90

reported that the radiation in the ocean will be diluted along the Japanese

coast, however exposed marine organisms and contaminated tsunami debris will

likely reach the U.S. Time series measurement of 134

Cs and 137

Cs in seawater showed

that the first arrival of the Fukushima derived radio-cesium in North America in a

location was in June 2012, which is 1.3 y after the accident 94

. This was in a location

that is 1ocation that is 1500 km west of British Columbia, Canada.

An assessment of the impact of the accident on marine environments in China

Sea showed that the activity concentration of 137

Cs ranged from 0.75 ± 0.07 to 1.43 ±

0.08 Bq m-3

, which is below the regulatory standard in China 92

.

Strontium-90 is of significant health and environmental concerns given that it is

a calcium analog and thus may bioaccumulate in the bones and teeth of many

organisms. The activity concentrations of 90

Sr have been measured in selected hotspot

in Japan 95

. The author reported that the 90Sr activity concentration in soil and

vegetation samples from the hot spots is relatively lower than the Japanese regulatory

limit. The activity concentrations of 90

Sr were less than 10% of 137

Cs.

4. Effects of FDNPP accident on some terrestrial species

Hiyama, et al. 96

used the Pale Blue Grass butterfly, Zizeeria maha, as indicator

species to evaluate the environmental impact of ionizing radiation. Observed

morphological abnormalities were detected on some individuals of adult butterflies

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collected in May 2011 increased in number and with time. Genetic studies indicated

that some abnormalities were inherited in the F2 generation. These abnormalities may

be explained by random mutation in important genes or by epigenetic mechanisms.

By comparing their data with that obtained from control populations, the authors

concluded that Fukushima-derived anthropogenic radionuclides likely caused the

morphological and genetic damage to the butterfly species. The study by Hiyama, et

al. 96

was significantly strengthened by laboratory experiments that used both internal

and external radiation sources, and these findings validated observations of the

elevated mutation rates and phenotypic effects observed in the field 97

. However, a

recent article by Copplestone and Beresford 98

has highlighted some major drawbacks

in the work of Hiyama and colleagues. Copplestone and Beresford 98

argued that

based on data reported by Hiyama, et al. 96

, the lethal dose required to kill 50% of

exposed individuals (LD50) is equivalent to the radiation levels that organisms receive

from exposure to background natural radiation sources. This disconnect between

empirical findings and predictions based on theoretical models highlights the many

uncertainties associated with accurate estimation of dose in wild populations 99

and

the likelihood that wild animals are significantly more sensitive to the effects of

radiation than predicted by conventional approaches 100

. In a later study 101

, the

authors clarified some of the questions raised concerning their earlier study and

presented some new data on the study.

Low blood cell counts were reported in wild monkeys from the forests of

Fukushima City compared with the counts in monkeys from Aomori prefecture which

is 400 km away 102

. The total radiocesium concentration in the muscle of Fukushima

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wild monkeys was measured to range from 78 to 1778 Bq kg-1

, while the cesium

concentration in the control population was reported to be below detection limits. A

negative correlation was observed between activity concentrations of Cs and low

blood counts in juvenile Fukushima monkeys. Ochiai, et al. 102

concluded that the

observed hematological aberration was due to exposure to Fukushima-derived

anthropogenic radionuclides. This study is based on ecological design that is rather

limited. Firstly, the population size of the monkeys (61 from Fukushima and 31 from

Shimokita) considered in the study is rather small and does not include individuals

from the more contaminated areas of the region. A similar result which showed

hematological variations in the Fukushima monkeys was presented by the same group

of authors in an earlier study 103

. The level of radiocesium in the Fukushima wild

monkeys was similar to that found in sheep in some parts of the UK following the

Chernobyl accident, i.e. extremely low in terms of damage to the animals themselves

104. The greatest strength of this study comes from comparisons to children living in

contaminated areas of northern Ukraine near Chernobyl where similar hematological

effects were also observed 105

.

A recent study of bull sperm and testis from the Fukushima region found no

evidence for significant histological changes in the testes or sperm morphology 106

although this study was very preliminary with only two bulls from a relatively

uncontaminated part of Fukushima represented for the analysis of sperm.

Conservation biologists are concerned with the effects of environmental

perturbances on population abundances and biodiversity as these are indicators of

overall ecosystem “health”. Initial studies of the Fukushima region in July 2011

surveyed abundance and diversity at 300 locations that varied from 0.5 usv/h to more

than 30 usv/h. It was found that several bird species as well butterflies and cicadas

showed significant reductions in numbers in the more radioactive areas even after

correcting for other environmental factors known to influence population sizes 107, 108

.

Following an additional three years of biotic inventories at 400 locations, it was found

that bird abundance and diversity had continued to fall at contaminated locations 70,

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71 . A more detailed analysis of barn swallow (Hirundo rustica) populations found

strong evidence of population declines although preliminary molecular analysis found

no evidence for significant increases in genetic damage 109

. Overall, these

investigations of population effects bear a striking resemblance to those found for

Chernobyl-affected regions of Ukraine and Belarus, providing some support for the

hypothesis that radioactive contaminants are the likely cause for the observed declines

e.g. 110, 111-116

.

The radioloecological consequence of the Fukushima accident has been assessed

using ERICA assessment tool for different biota in two known studies 69, 89

. The

exposure profile to 131

I, 134

Cs, and 137

Cs, one month after Fukushima was used by

Garnier-Laplace, et al. 69

for the dose rates (mGy d-1

) calculations. The dose rate to

selected reference species were 1.5 (mGy d-1

) for birds, 2.3 (mGy d-1

) for soil

invertebrates, and 3.9 (mGy d-1

) for forest. Such dose rates could be biologically

significant especially for longer-lived or radiosensitive organisms.

5. Application of isotopes as tracers for environmental processes

In the oceans, the behavior of cesium is thought to be conservative, i.e. it is

soluble (less than 1% adsorbed to marine particulates) and is carried primarily with

ocean waters and as such has been used as a tracer of water mass mixing and transport

117-119. Following the Fukushima nuclear accident, cesium activity and the

134Cs/

137Cs

activity ratio have been measured to assess its environment effect and to study

oceanographic processes. Studies have shown that the 134

Cs/137

Cs activity ratio in the

Fukushima derived radionuclides was nearly 1.0 65, 75

, which is based on the samples

of atmosphere, soil, seawater and marine biota off Fukushima. It is higher than that in

the Chernobyl fallout (134

Cs/137

Cs activity ratios:0.5) 120, 121

. This makes the tracking

of Fukushima derived radionuclides in the ocean quite straightforward, since given its

relatively short half-life (2 yr), the only source of 134

Cs in the North Pacific at this

time would be the Dai-ichi NPPs. Hence in addition to the elevated cesium activities,

the presence of 134

Cs is a unique isotopic signature for tracking these waters and

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providing a means to study the rates of vertical and horizontal mixing processes in the

Pacific Ocean.

Compared with cesium, Pu has high particle affinity, which thus provides a tool

for studying a variety of processes in the marine environment such as particle fluxes

and scavenging, the validation of various biogeochemical ocean models. However, the

most useful aspect of Pu as an environmental tracer is its well-defined sources terms

122. This is because the composition of Pu isotopes from different sources in marine

environment varies significantly due to the characteristic isotopic composition

corresponding to the means of production, for example, reactor-grade Pu typically

contains more than 35% 239

Pu with a 240

Pu/239

Pu atom ratio of 0.2-1.0 after fuel burn-

up 123

. The 240

Pu/239

Pu atom ratio in weapon-grade Pu is much lower (0.02-0.06)

because burn-up is kept low to minimize the production of higher Pu isotopes 124

. The

current study shows the Fukushima derived 240

Pu/239

Pu ratio is 0.216~0.255, which

is higher than that of global fallout (0.18), but lower than that of Chernobyl. A

summary of the composition of Cs and Pu isotopes for Fukushima, Chernobyl and the

global fallout is presented in Table 3.

Table 3 Anthropogenic nuclide isotope ratio characteristic

Source Fukushima Chernobyl Global fallout

134Cs/

137Cs(activity ratio) ~1 0.5

137Cs

/239,240

Pu (activity ratio) 1.95×105~2.53×10

7 38.5

238Pu/

239,240Pu(activity ratio) 1.2 0.5 0.030

241Pu/

239,240Pu(activity ratio) 107.8 13~16

240Pu/

239Pu(atom ratio) 0.216~0.255 0.408 0.180

241Pu/

239Pu(atom ratio) 0.132 0.00194

In soil, Fukushima-derived 137

Cs has been deposited in Japan and other parts

of the globe. Atmospheric and soil measurements of Fukushima-derived 137

Cs

activity concentrations, revealed that the detection of 137

Cs in the ambient aerosol

ended 2–3 months after the initial emissions 4, 47, 125, 126

. This indicates that topsoil

activity concentrations of 137

Cs that are obtained after this period are reliable for

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monitoring soil processes as most of the Cs in the air has been deposited on the soil

and surface of water bodies. Cesium is absorbed on soil particles, thus restraining its

movement by either biological or chemical means. The movement of 137

Cs in the

environment is by physical processes hence it can be used as a tracer for studying the

processes of sedimentation and erosion 127

. By determining the spatial distribution

patterns of 137

Cs in vertical and horizontal planes across the landscape, the rates of

soil loss or deposition can be measured for different parts of a watershed. As for

sedimentation rate, it can be measured by matching the vertical distribution of 137

Cs in

sediments with the temporal deposition of fallout 137

Cs from the atmosphere to locate

sediment horizons 128, 129

. Highlights of some of the state-of- the-art methods for

using anthropogenic radionuclides as tracers in soil process are presented in Zapata

130. The soil retention mechanism of Cs derived from FDNPP was investigated by

Mishra, et al. 131

. The authors reported that Cs is sorbed on the surface of clay

particles; and analysis of the vertical profile of deposited Cs showed that the

radionuclide largely retained in the top 5cm of the soil.

Conclusions

In this paper we have reviewed the current state of knowledge concerning the

environmental impacts of the Fukushima nuclear accident. First, we assessed the

source term for the Fukushima nuclear accident and concluded that the FDNPP

released a total amount of 10~15 PBq of 137

Cs to the atmosphere and 1~42 PBq to the

ocean. Next, we analyzed the radioactive contamination of atmosphere, soil and

marine environments (seawater, suspended solid and biota), whereby global

contamination was mediated through atmospheric dispersion. High deposition rates of

fission products have been observed in Japan. The radionuclides directly released into

the ocean caused activity levels and total inventory to significantly increase. The

concentrations of radionuclides in SS and marine biota have also been discussed. We

also summarized recent studies concerning the hematological, morphological and

genetic impacts of the accident on Fukushima wild monkeys, cows, birds, and

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butterflies. Finally, we discussed the application of anthropogenic radionuclides (for

example, 134

Cs/137

Cs activity ratio and 240

Pu/239

Pu atom ratio) as a tracer to study

marine and soil processes and/or identify sources.

Could the atmospheric and oceanic dispersion of anthropogenic radionuclides

provide a basis for climate change monitoring? This question should be considered by

climate change scientists as data from the CTBTO global monitoring facilities may

provide clues concerning mechanisms of global climate change.

Acknowledgements

A.S. Aliyu wishes to acknowledge the support of the Research Management

Center of Universiti Teknologi Malaysia for its support through the Post Doc

fellowship scheme under the project number (Q.J130000.21A2.01E98).

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