+!%0 ) ( !%...* v ) îd z# :Ã ! d@kgq5 rtf kd s9q5cq3 å . e2.3-1 ra kÓ Ì Å Ì Ö..... 31 e2.3-2...

i

1 .......................................................................................................... 1

TF Kd

......................................................................................................................... 3

................................................................................................................. 3

.............................................. 5

2.2.1. TF ......................................... 5

2.2.1.1 .......................................... 5

2.2.1.2 ................................................................... 5

2.2.2. .................................................................. 6

TF

.......................................................................................................... 7

2.3.1. TF .................. 7

2.3.1.1. .............................................................................. 7

2.3.1.2. ..................................................................................... 7

2.3.1.3. ................................................................................. 7

2.3.1.4. ..................................................................................... 8

2.3.1.5. ................................................................................. 9

2.3.1.6. ............................................................................ 10

2.3.1.7. ....................................................................................... 11

2.3.1.8. 28 ....................................................... 12

2.3.2. 27 .......................................................... 12

2.3.3. TF

.................................................................................................... 12

................................................................... 14

2.4.1. ................................................................ 14

2.4.2. ............................................................................................. 14

2.4.3. .......................................................................................... 14

Kd ............................... 16

2.5.1. 30 .............................. 16

2.5.2. 30 ......................................... 17

2.5.3. 30˚C Kd-137Cs .................................................................... 17

2.5.4. 30˚C Kd-137Cs ..................................................... 17

.................. 18

ii

2.6.1. Cs ................................................................. 18

2.6.1.1. ..................................................................................... 18

2.6.1.2. Cs ..................................................... 18

2.6.2. Cs ...................................................................................... 19

2.6.2.1. ........................................................................................................ 19

2.6.2.2. .................................................................................................... 20

2.6.2.3. ................................................................................................ 20

2.6.2.4. Tag ............................................................................... 20

2.6.3. 137Cs ........................................................................................... 21

2.6.3.1. ....................................................... 21

2.6.3.2. 137Cs ..................................................... 21

2.6.3.3. .................................................................. 23

............................................................................................................... 25

2.7.1. TF ........................................................ 25

2.7.2. TF 25

2.7.3. TF .................................................. 26

2.7.4. ......................................... 26

2.7.5. Cs ...................... 26

.......................................................................................................................... 27

2- 1. ...................................................................................... 30

.......................... 59

............................................................................................................... 59

.......................................................................................................................... 60 14C ............................................................................... 61

3.2.1. 14CO214C .......................................... 61

3.2.1.1. 14C 14C .............................................. 61

3.2.1.2. 14C ........................................................... 62

3.2.2. .................................................................................................................. 63

.......................................................................................................................... 63

............................................................... 65

3.3.1. .......................................................... 65

3.3.2. ..................................................................... 66

3.3.3. ..................................................................... 67

3.3.4. .................................................................................................................. 67

.......................................................................................................................... 68

..................................................................................... 70

3.4.1. ................................................................. 70

3.4.1.1. .................................................................. 70

3.4.1.2. ......................................................................................... 71

iii

3.4.1.3. 14C ........... 71

3.4.2. .................................... 72

3.4.2.1. ............................................................................. 72

3.4.2.2. CO2 .................................................................. 75

3.4.3. ............................................... 75

3.4.3.1. ................................................................................. 76

3.4.3.2. .................................... 77

3.4.3.3. ................................................ 77

3.4.3.4. 14C ........................................................ 78

3.4.4. .................................................................................................................. 79

.......................................................................................................................... 79

............................................................................................................... 81

4 Pu, Am, Th Cl

.................................................................................................... 119

............................................................................................................. 119

Am ................................................................. 120

4.2.1. Am ........................................................ 120

4.2.1.1. ...................................................................................................... 121

4.2.1.2. Aridus-SF-ICP-MS ........................................................ 121

4.2.1.3. ...................................................................................................... 122

4.2.1.4. ............................................................................................................. 122

4.2.1.5. ....................................................................................... 122

4.2.1.6. .............................................................................................. 124

4.2.2. 241Am ................................................................................ 125

4.2.2.1. ...................................................................................................... 125

4.2.2.2. ...................................................................................................... 125

4.2.2.3. .......................................................................................... 125

........................................................................................................................ 127

Th ............................................................................................ 130

4.3.1. ............................................................................................................ 130

4.3.2. ............................................................................................................ 130

4.3.3. ............................................................................................................ 130

4.3.4. ................................................................................................. 131

........................................................................................................................ 132

.................................................................... 133

4.4.1. ............................................................................................................. 133

4.4.2. TMAH ...................................................... 133

4.4.3. TMAH ICP-MS ....................................................... 134

4.4.4. TF .............................................. 134

iv

4.4.5. ........................................................... 135

........................................................................................................................ 135

Pu - .............................................................. 136

4.5.1. ............................................................................................................ 136

4.5.2. ..................................................................................................... 136

4.5.2.1. ....................................................................................................... 136

4.5.2.2. ............................................................................................................... 136

4.5.2.3. Pu .................................................................................... 136

4.5.3. ................................................................................................. 137

4.5.3.1. Pu ................................................. 137

4.5.3.2. Pu ................................................................................................ 138

4.5.3.3. Pu - ............................................................................... 138

..................................................................................................................... 139

Pu, Am, Th Cl - .................... 141

4.6.1. ............................................................................................................ 141

4.6.2. .............................................................................. 141

4.6.3. IAEA TRS-472 .................................................................................... 142

........................................................................................................................ 143

................................................................................................................. 147

4.7.1. Am Cl .......................................................................... 147

4.7.1.1. Am ......................................................... 147

4.7.1.2. ................................................................................... 147

4.7.2. Th ............................................................................................... 147

4.7.3. Pu - ....................................................................... 148

5 ................................................................................................................. 171

............................................................................................................. 171

TF Kd

................................................................................................................. 172

5.2.1. TF ...................................................... 172

5.2.2. TF 172

5.2.3. TF ................................................ 173

5.2.4. Kd ............................ 173

5.2.5 Cs .................................... 173

........................ 175

5.3.1. 14C .......................................................................... 175

5.3.2. .......................................................... 175

5.3.3. ................................................................................ 175

Pu, Am, Th Cl

.......................................................................................................... 177

v

5.4.1 Am Cl ........................................................................... 177

5.4.1.1. Am ..................................................... 177

5.4.1.2. ........................................................................ 177

5.4.2. - ............................................................................... 177

.................................................. 179

..................................................... 181

28 .................. 182

.................................................................................................................................... 183

vii

TF Kd

2.3-1 ........................................................................... 31

2.3-2 ....................................................... 31

2.3-3 ................................................................................... 32

2.3-4 ........................................................... 32

2.3-5 ....................................................................... 33

2.3-6 ........................................................... 35

2.3-7 28 ......................................... 37

2.3-8 14-18 26-28 ................................................................................................................ 37

2.3-9 28 ..................................................... 38

2.3-10 28 ............................................... 39

2.3-11 28 ....................................................... 40

2.3-12 27 ....................................... 41

2.3-13 27 ................................... 42

2.3-14 27 ........................... 43

2.4-1 - 2016 .............. 44

2.4-2 ........... 44

2.4-3 ................... 45

2.4-4 ....................... 45

2.5-1 ............................................................................... 46

2.5-2 Cs Kd 30˚C Kd ....................................... 46

2.6-1 137Cs ..... 47

2.6-2 Cs Tag: m2 kg-1 ................. 47

2.6-3 ................................................................................................... 47

2.6-4 ....................................................................................... 47

2.6-5 137Cs ..................................... 48

2.6-6 δ13C δ15N ......................................................................... 48

2s-1 2015 2016 .......................................... 48

2.2-1 Ni, Sr, Mo Pb .......................................... 49

2.4-1 .................................................................................................................... 50

2.4-2 Fe, Co, Ni, Cu, Zn Sr ........................................................................................................................ 50

2.5-1 1 30 Cs 3 7 30

viii

Kd pH ......................................................................................................... 51

2.5-2 10 23 30˚C Kd-137Cs .............................................. 52

2.5-3 10 23 30˚C Kd-137Cs ........... 52

2.6-1 137Cs ................................................................................................ 53

2.6-2 2012-2016 137CsTag, m2 kg-1 ...................................................................... 54

2.6-3 2011 11 2016 9 ...... 55

2.6-4 ............................................................................................... 55

2.6-5 137Cs ............................................................................................. 56

2.6-6 ........................................................................................................... 56

2.6-7 13C 15N .......................................................................... 57

2.6-8 ................................................... 57

2s-1 2015 2016 Air Soil 20cm ......... 58

2s-2 2015 2016 ........................................ 58

3.3-1 ............................................................... 83

3.3-2 .............................................................................. 83

3.4-1

.......................................................................................................... 84

3.4-2 14C ......................... 84

3.4-3 ....................................................... 85

3.4-4 1 ................................................ 86

3.4-5 1 ........................................ 86

3.4-6 2 ................................................ 87

3.4-7 2 ........................................ 87

3.4-8 3 ................................................ 88

3.4-9 3 ........................................ 88

3.4-10 4 .............................................. 89

3.4-11 4 ...................................... 89

3.4-12 5 ................................................................. 90

3.4-13 5 ......................................................... 90

3.4-14 6 ................................................................. 91

3.4-15 6 ......................................................... 91

3.4-16 7 ................................................................. 92

3.4-17 7 ......................................................... 92

3.4-18 8 ................................................................. 93

ix

3.4-19 8 ......................................................... 93

3.4-20 ................................................................. 94

3.2-1 14C 14C .......................................... 95

3.2-2 14CO2 ............................................................................... 95

3.2-3 14CO2 ......................................... 95

3.2-4 14CO2 ............................................................................... 96

3.2-5 14CO2 ......................................... 96

3.3-1 P2 ................................................. 97

3.3-2 P11 ............................................... 97

3.3-3 14C DGGE ......................................... 98

3.3-4 DGGE DNA ......................................................... 98

3.4-1 ............................................................................................. 99

3.4-2 ....................... 100

3.4-3 14C .......................................... 101

3.4-4 14C .............................................. 101

3.4-5 14C ....................................... 102

3.4-6 -> 14C .......................................................... 103

3.4-7 -> 14C .......................................................... 103

3.4-8 -> 14C ...................................................... 104

3.4-9 4 14C . 105

3.4-10 ................................ 106

3.4-11 1 ............................................................................................. 106

3.4-12 2 ............................................................................................. 106

3.4-13 3 ............................................................................................. 106

3.4-14 4 ............................................................................................. 107

3.4-15 5 ............................................................................................. 107

3.4-16 6 ............................................................................................. 107

3.4-17 7 ............................................................................................. 108

3.4-18 8 ............................................................................................. 108

3.4-19 .................................................................................. 108

3.4-20 CO2 . 109

3.4-21 14C ......................... 110

3.4-22 14C ............................................ 111

3.4-2314C .......................................................................................................... 112

3.4-2414C .......................................................................................................... 112

3.4-2514C ............................................................................................................ 113

x

3.4-2614C ............................................................................................................ 113

3.4-27 14C ............................................................ 114

3.4-28 - ................................... 114

3.4-29 .................................... 115

3.4-30 14C

..................................................................................... 116

3.4-3114C ................................................................................................. 117

3.4-3214C .............................................................................................. 117

4 Pu, Am, Th Cl

4.2-1 CaC2O4 UTEVA + DGA-N Am 5g JSAC-0471

SF-ICP-MS 1mL ............... 149

4.2-2 241Am ...................................... 149

4.2-3 Pu 241Am/239+240Pu activity ............................... 150

4.3-1 Th ................................................................................. 150

4.3-2 Th .............................................................................. 151

4.4-1 TMAH RSD(%) ....... 152

4.4-2 RSD(%) ...................... 152

4.4-3 TF ............................... 153

4.4-4. ................................... 153

4.5-1 Pu 240Pu/239Pu .................................................. 154

4.5-2 239Pu Pu - ................................................ 155

4.5-3 Pu - .......................................................................... 155

4.6-1 2008-2016 Th − ........................ 156

4.6-2 2008-2016 Am − ................. 157

4.6-3 2008-2016 Pu − ................... 158

4.2-1 Aridus II SF-ICP-MS (Element XR)

....................................................................................................................... 159

4.2-2 DGA-N . 159

4.2-3 Fe(OH)3 CaC2O4 CaF2 n = 3

........................................................................................................................... 160

4.2-4 DGN 0.05M HNO3 Am REE (a) TEVA

Am REE (b) ................................................. 160

4.2-5 SF-ICP-MS Am ................................................. 161

xi

4.2-6 DGA-N 0.5M HCl TEVA 4M HCl

Am ......................................................................................................... 161

4.2-7 IAEA-soil-6 and IAEA-375

NIST-4357, IAEA-385 and IAEA-384 (NIST-4354)

241Am .............................................................................. 162

4.2-8 241Am 239+240Pu 137Cs ...... 163

4.2-9 241Am/239+240Pu 241Am

241Am/239+240Pu ................................................................. 164

4.4-1 NAA TMAH -ICP-MS

................................................................................................................ 165

4.4-2 TMAH ..................... 165

4.4-3 1 TMAH 100

............................................................................................................ 166

4.4-4 1 TMAH 100

................................................................................................................ 166

4.5-1 (1-6, 27 ;

7-10, ) ................................................................................... 167

4.5-2 Pu HNO3 - ........................ 168

4.5-3 Pu - IAEA TRS-472

.............................................................. 169

4.6-1 2008 2016 Th - IAEA

TRS-472 .................................................................. 169

4.6-2 2008 2016 Am - IAEA

TRS-472 .................................................................. 170

4.6-3 2008 2016 Pu - IAEA

TRS-472 .................................................................. 172

14C

Pu

Am Th Cl

TF Kd

Pu Am Th Cl

TF Kd -Kd -Kd TF

28

TF

• TF • 5

20

• 20

• TF 27

Kd • TF

• 20 30 137Cs

Kd

• TF

TF TF

1

28

• 14C 14C • 14C • 14C

• 14C

• CO2

•

Pu Am Th Cl

Pu Am Th (Cl)

-

28

27

• 241Am ICP-MS -

• Pu Th Am Cl

• Pu Th Cl

• Pu Th Cl TF

• 25 28 TF

2

TF Kd

Kautsky et al., 2013; Staudt et al., 2013,

Becker et al., 2014

NUMO

Geosphere-Biosphere InterfaceNUMO 2011

Walke et al., 2015

FAO 2017

IAEA 2010

− Transfer Factor, TF

5

- 20

28

3 15

20 TF

TF Kd

Cs Kd Cs Kd

Kd

20 10 23 30

3

Cs 135Cs 2.3×106 y

4

2.2.1. TF

2.2.1.1

Staudt et al., 2013 Kautsky et al., 2013 Becker et al., 2014

Dowdall 2008

Gesellschaft für Anlagen- und Reaktorsicherheit 2008

90Sr 137Cs

TF

TF

2017

csv

web doi

Ref.

Single exponential

p

web doi

2.2.1.2

5

2.2.1.1

2.2.2.

Tagami and Uchida, 2010

FAO

Ni, Sr, Mo Pb 2.2-1 Ni

Zn, Cu, As, Cd Co

Pinson 2015 1763

P, Mg, K, S, Ca, As, Cd, Co, Cu, Fe, Mn, Mo,

Ni, Rb, Sr Zn

TF

6

TF

2.3.1. − TF

5 5

TF

26

15

2.3.1.1.

2.3-1 2.3-2

0-15cm 0-20cm

2.5 kg 0.5kg

100cc

5 kg 5 kg

2.3-22.3-3 2.3-4

2.3-5 2.3-6

2.3.1.2.

100 g

40

2mm

50 g

7

2.3.1.3.

RO Milli-Q

EYELA

FD-550

2.5 kg 0.5 kg 2.3-3

MC-90A

2.3.1.4.

1 pH(H2O)

10 g 25 mL 1pH pH

2 CEC Schollenberger

1M 100 mL

13 mm 120 mm 1M 2/3

8 cm1M 4 20

80 %

80 % 50 mL

10 % 100 mL

200 mL

3 Ca K

2 200 mL

1000 mg/L

< >

SpectrAA240FS

: 766.5 nm 422.7 nm

8

: 2.00 L/min 13.50 L/min

4 Al Fe

1.0 g 250 mL 0.2 M pH3.0 100 mL

4 25 mL 50 mL Superfloc ( ) 1 10 3000 rpm

ICP

<ICP >

ICPE-9000

1100 W 15 L/min

1.2 L/min

0.80 L/min

396.153 nm 238.204 nm

5 Al, Fe 0.05 g HNO3 3 mL HCl 3 mL

HNO3 1 mL HF 1 mL

PTFE HNO3 2 mL 4 mL

HNO3(1+2) 50 mL

ICP

<ICP >

Optima 8300

1300 W

12 L/min

0.2 L/min

0.55 L/min 396.153 nm 238.204 nm( ) 343.489 nm ;

RSD 10

2.3-7

2.3.1.5.

(1)

0.1 0.2 g 500˚C 5 g 900˚C 20

(1+1) (1+1) 20 mL

(1+1) 20 mL 10 No.5C[ ]

900 ˚C20 (W1) 2 3 10

9

mL (W2) 2

(W1-W2)

(2)

0.2 g 550 ˚C 2 1 g900 ˚C 20 155˚C 5 %HNO3

50 mL No.5C[ ] 100 mL

ICP

<ICP >

Optima 8300 1300 W

15 L/min

0.2 L/min

0.55 L/min

208.957 nm

451.131 nm ;

(3)

0.1 g

< > MA-3000

253.7 nm

(4) Cr, P, Co, Ni, Cu, Zn, Sr. Cd

2.3.1.4. (5) 213.617 nm ICP

Cr Co Ni Cu Zn Cd ICP

<ICP >

Agilent 8800

1550 W

15 L/min

1.0 L/min 5 mL/min

m/z 52( ) 59( ) 60( ) 63( ) 66( ) 111( )

103( ; )

2.3.1.6.

(1)

10

0.2 3 g 500 ˚C 5 g 900˚C

20 No.5B[ ]

2.3.1.4. 5 ICP

<ICP >

SPECTRO BLUE

1400 W

( ) 13 L/min

( ) 0.8 L/min

( ) 0.8 L/min 251.612 nm( ) 417.206 nm( ; )

(2) P, Fe, Ni, Cu, Zn, Cd

0.5 0.6 g 5 mL HNO3

50 mL

ICPICP

<ICP >

Optima 8300

1300 W ( ) 12 L/min

( ) 0.2 L/min

( ) 0.55 L/min

213.617 nm( ) 238.204 nm( ) 213.857 nm( )

371.029 nm( ; )

<ICP >

Agilent 8800

1550 W

( ) 15 L/min

( ) 1.0 L/min ( ) 5 mL/min

m/z 59( ) 60( ) 63( ) 111( ),

103( ; )

2.3.1.7.

(1) 100 mg HNO 7 mL HF 7 mL

11

AA-100 CEM MARS5

15 HClO 1 mL

1 mL HNO 0.5 mL H2O2

40%HNO 2.5 mL 50 mL Milli-Q >18MΩ

50mL HNO3 2%1 500

JB-1a JB-3 ICP Horiba Activa-M

ICP Agilent, 7500c

(2)

80˚C 3 500mg HNO3 10mLHF 4 mL 80˚C 10

10

1 mL HNO 0.5 mL H2O2

40%HNO 1 mL 20 mL 20 mL

HNO3 2% 1/40

GBW-07603 NISTSRM-1573a ICP Horiba Activa-M

ICP Agilent, 7500c

2.3.1.8. 28

2.3-8 26 28 14-18

CEC 26-28

t , p<0.05

2.3-9 2.3-10

21 20

TF 2.3-11

2.3.2. 27 2.3.1.7 27 20

TF

2.3-12 2.3-13

TF

2.3-14

12

2.3.3. − TF

28 10 5 5

10 5 5

20 2.3-7 2.3-9 2.3-10

TF 2.3-11

27

2.3-12 2.3-13 TF 2.3-14

13

14-18

5

5-9 2016 2.4-1

1981 2010 30

10.1 19.0

9 5-9 18.4 25.3 7

2.4.1.

26

21

Na, Mg, Al, Si, P, K, Ca, Cr, M, Fe, Co, Ni, Cu, Zn, Sr,

Cd, Ba Ca, K, Al, Fe pHKaleidaGraph ver. 4.1.4 t

2.4-2 2.4-3

p>0.01 Fe pH GM

Reinmann and Caritat, 2012

2.4-1 Fe, Cu, Zn Ba p<0.01

GM 2

2.4.2.

TF Ca, K, Al, Fe mg/kg

2.4-4 TFp<0.01 Fe, Zn Fe TF 2.4-2

p<0.05 Na, Si, K, Co, Ba K TF

TF

TF GM 2 TF

GSD Ca F

p<0.01 GSD TFTF

Na, Mg, Al, Si, P, K, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni,

Cu, Zn, Se, Rb, Sr, Y, Zr, Nb, Mo, Cd, Sn, Sb, Cs, Ba, La, Ce, Sm, Eu, Gd, Pb, Th, U 37

TF TF

14

2.4.3.

Na, Mg, Al, Si, P, K, Ca, Cr, M, Fe, Co, Ni, Cu, Zn, Sr, Cd, Ba

TF Fe, Zn

TFTF Pinson 2015

Ca,

Mg, K

Pinson TF

7

TF

15

10 Cs Kd 23 10

20 20 Kd 23

30 Kd

10 23 30 Wagai et

al., 2013 Cs Kd

Kd

Cs Kd

2.5.1. 30

Kd RI

Kd 30

1 3

1 7 1 30

30 7

- Cs 30

Kd

Kd

2.5-1 1 10 137Cs 120rpmHIMAC CT5L 3000 rpm 10

=0.45 µm PTFE 3mL NaI (Tl)

ARC-380 20

Kd

di l

Ci (Bq/L) 137Cs Cl (Bq/L) RI 137Cs

Wl L Ws Ci (Bq/L) Cl (Bq/L)cpm/mL

2.5-1 30

3 7, 30 Kd

1 30

Kd EP-SD-50Kd 2.5-1

30

16

Kd RI

3 7 30 EP-SD-50 Kd 30

10 23 1 7

2.5.2. 30

30 Kd

20 <2 mm

g 30 mL Milli-Q 10 mL 30˚C

120 rpm 24 137Cs CsCl 14 kBq 30˚C 120 rpm

2.5.1

2.5.3. 30˚C Kd-137Cs

30 Kd 2.5-2 10 23 10

23 30 10 30Kd Kd t-test p=0.0075 2.5-2 Kd

10 30 0.49 Kd 10 3.88×103

20 2.34×103 30 1.91×103

Cs Cs

Cs e.g. Bellenger and Staunton, 2008

Kd 2.5-3R=0.99 10 Kd 1000 Cs

Cs Kd

Sr Başçetin and Atun 2006 Kd

Kd

Cs Cs

2.5.4. 30˚C Kd-137Cs

10 23 30 Kd Kd

10 Kd 1000

30

17

135Cs

2.3 106 y

Cs

2.6.1. 137Cs

137Cs 2011 2013Tagami and Uchida, 2015 Smith et al., 2000

Cs

2.6.1.1.

Fallopia japonica Artemisia indica var.

maximowiczii Petasites japonicus

80˚C U8 Ge

Seiko EG&G Ortec 80,000 150,000

t

Yt

Yt = A*exp(-λa*t)+ B*exp(-λb*t) ….(1)

: A

B

λa Teff=ln(2)/λa

λb Teff=ln(2)/λb

KaleidaGraph ver. 4.1.4

2.6.1.2. Cs 137Cs 2.6-1

R=0.99, R=0.90, R=0.892.7-10.5 10.5

18

137Cs

13-21 2016

2015-2016

Tag m2 kg-1 137Cs

TF

Tag

Tag= 137Cs Bq kg-1 137Cs Bq m-2 ….(2)

Bq m-2 0-5cm

5 cm 137Cs 5% 2011-2016

(2) Tag 5.3×10-5 1.6×10-4 m2 kg-1 Tag

2.5×10-3 1.2×10-2 m2 kg-1 IAEA, 2010 1-2

Cs

2.6.2. Cs

Cs

2017 Cs

2.6.1137Cs

Tag

2017

2017 in-situ

Bq m-2

2016 12

2.6.2.1. Tag 325 1177 183 968 205

2.6-2 Tag=10-5

N.D. 2015-2016

R=-0.51, p<0.001 Tag 0.2

19

137Cs

1.8y 9.3 2016

Cs 134+137Cs134Cs

Cs134Cs

137Cs137Cs

Tag Tag

Tag 3.4×10-3 m2 kg-1 2.6-2 IAEA 2010 5×10-4

3.4×10-1 m2 kg-1 Tag

2016

2.6.2.2. Tag 97 78 44 83 359

2.6-2

p

3.6- Tag Tag

Tag 5.5×10-3 m2 kg-1 2.6-2 t

p<0.01 Red deer

Roe deer 1×10-2 5×10-2 m2 kg-1 5×10-3 5×10-2 m2 kg-1 IAEA, 2010

Tag Red deer Roe deer

2.6.2.3.

Tag 50 56 346 200

Tag 2.6-2

Tag

Tag

Tag 3.8×10-3 m2 kg-1 2.6-2IAEA TRS472

2010

2.6.2.4. Tag 137Cs Tag

Tag Tag

3.4×10-3 m2 kg-1 5.5×10-3 m2 kg-1 3.8×10-3 m2 kg-1

20

Cs Tag

2017aHohmann & Huckschlag, 2005

Cs

2.6.3. 137Cs

Cs Cs

Cs

Tsuji et al. 2014

Cs

Kurita et al. (2015) Cs 2011

3 Cs

Tagami and Uchida, 2016 6

Cs2015 9

137Cs 2016 3

2.6.3.1.

2.6-3

134+137Cs

, on line 2011 11 5 30k Bq/m2

, 2017b 2011 11 2016 92.6-3 28 12 6 9 2

348 Bq/kg-dry 357 Bq/kg-dry

2011 11 2016

9 20 1 Bq/L

2.6.3.2. 137Cs

21

2016 3 2 12 8 51

2.6-4 - - 2.6-4

37 15 2 1

80

U U8,

JSAC0473, 137Cs 2.6-5 137Cs

137Cs 32-49%

21-43% 137Cs4-8%

Yankovich, 2009

137Cs

Cs137Cs 137Cs

100 Bq/kg

137Cs

137Cs

2.6-5 2 2

7 3 2 2 2137Cs 2

6 3

37 22137Cs 18

5 10

10 137Cs 86 Bq/kg-dry137Cs

137Cs 137Cs 137Cs

22

137Cs

2.6.3.3.

Rybczynski et al. 2008, Perkins et al. 2014

2010, 2013

, 2:1

Logan and Lutcavage 2008

10 mg

2.6-6 2015 12 14

10-20 mg 2 mL

=2:1 1.5 mL

5,500

× g 5 1.5 mL1

2 2 3

50 24

DELTA V Advantage, Thermo Fisher

Scientific Inc. 3 SI Science Reference Material; Amino Standard13C 15N

13C 15N 2.6-7 1 13C -42.8 -26.6

2 1 13C

3 13C13C

13C 13C15N

23

Eliot and Eliot (2016) 15N

3 3

2015 9 13C 15N

2.6-6 2.6-8

15N 15N

Minagawa and Wada, 1984 15N 13C

, 2013 2 13C

137Cs

15N 13.2 15.9 2.715N 3-4 2013

15N 16.1

15N 16.813C 15N

137Cs

24

TF Kd

—TF Cs Kd

135Cs

Cs

2.7.1. TF

90Sr 137Cs

Ni, Sr, Mo Pb

Ni

5 Co, Zn, Cu, As, Cd

2.7.2. − TF 28 10

10

26

15 20

TF

TF26 28

14-18

26-28

TF

2.420

25

2.7.3 TF

Na, Mg, Al, Si, P, K, Ca, Cr, M, Fe, Co, Ni, Cu, Zn, Sr, Cd, Ba 14-18

TF

18.4 25.3 7

TF Fe, Zn, p<0.01

Pinson 2015

TF 7

TF37 Na, Mg, Al, Si, P, K, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Se, Rb, Sr,

Y, Zr, Nb, Mo, Cd, Sn, Sb, Cs, Ba, La, Ce, Sm, Eu, Gd, Pb, Th, U TF

2.7.4.

20 30 Kd

10 23 Kd Kd 10 3.88×103

20 2.34×103 30 1.91×103 Kd

10 Kd 1000

30

2.7.5 Cs

27-28

Tag 5.3×10-5 1.6×10-4 m2 kg-1

137Cs

Tag 3.4×10-3 m2 kg-1

5.5×10-3 m2 kg-1 3.8×10-3 m2 kg-1 Cs Tag

26

137Cs

137Cs137Cs 137Cs

137Cs13C 15N

TF Tag Kd

Başçetin, E., & Atun, G. (2006). Adsorption behavior of strontium on binary mineral mixtures of Montmorillonite

and Kaolinite. Applied radiation and isotopes, 64(8), 957-964.

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Bellenger J.-P., Staunton, S. (2008) Adsorption and desorption of 85Sr and 137Cs on reference minerals, withi and without inorganic and organic surface coatings. J. Environ. Radioactiv. 99, 831-840.

Dowdall, M., Standring, W., Shaw, G., & Strand, P. (2008). Will global warming affect soil-to-plant transfer of

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Elliott, K. H., & Elliott, J. E. (2016). Lipid extraction techniques for stable isotope analysis of bird eggs:

Chloroform–methanol leads to more enriched 13C values than extraction via petroleum ether. Journal of

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27

Kurita, Y., Shigenobu, Y., Sakuma, T., & Ito, S.-i. (2015). Radiocesium contamination histories of Japanese

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28

microbial physiology. Global Change Biology, 19(4), 1114-1125. Walke, R. C., Kirchner, G., Xu, S., & Dverstorp, B. (2015). Post-closure biosphere assessment modelling:

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fish tissues using stable analogues. J Environ Radioact, 100(9), 795-801. 2017a

https://www.env.go.jp/nature/choju/plan/plan3-2a/ 2017/1/17

2017b . .

http://www.env.go.jp/jishin/monitoring/results_r-pw.html 2017/1/6

2017 http://www.data.jma.go.jp/gmd/risk/obsdl/ 2017.1.10

2017

http://www.mhlw.go.jp/stf/kinkyu/0000045250.html 2017/1/17

2016 29 90 .

, , , , , & . (2013).

. Journal of Fisheries

Technology, 6(1), 57-68. , & . (2010). / (TCEA/IRMS)

. Researches in organic

geochemistry, 26, 31-37.

2017 -137 http://ramap.jmc.or.jp/map/

2017/1/17

2017http://www.pref.fukushima.lg.jp/site/portal/wildlife-radiationmonitoring1.html 2017/1/17

, 2016. 27

, .

29

- 1. 2014 11 2015 11

2015 1 1 2015

12 31 2016 1 2016 12 31

(1)

20 cm 0.5 m

20 cm 1.5 mSK-L210T

TR-71wf 5

6 0-4 4-8 8-12 12-16 16-20 20-24

2 6 10 14 18 22

2017 2015 20161 1 12 31

(2) 2s-1 2015 2016

2015

2016 2s-2 2015 2016

0.996 p<0.001

2s-1 2015 2016 1

R>0.90,

p<0.001

30

2.3-1

Sample code EPII-CF- 21 2016/7/28 EPII-CF- 22 2016/7/28 EPII-CF- 23 2016/8/13 EPII-CF- 24 2016/6/10 EPII-CF- 25 2016/9/17 EPII-CF- 26 2016/9/21 EPII-CF- 27 2016/9/17 EPII-CF- 28 2016/10/11 EPII-CF- 29 2016/9/25 EPII-CF- 30 2016/10/20 EFII-CF- 41 2016/5/29 EFII-CF- 42 2016/5/31 EFII-CF- 43 2016/6/1 EFII-CF- 44 2016/6/2 EFII-CF- 45 2016/6/9 EFII-CF- 46 2016/7/4 EFII-CF- 47 2016/7/12 EFII-CF- 48 2016/8/6 EFII-CF- 49 2016/8/9 EFII-CF- 50 2016/8/10

2.3-2

Sample code EPII-SD- 21 2016/7/30 0.82 EPII-SD- 22 2016/8/2 1.06 EPII-SD- 23 2016/8/17 0.15 EPII-SD- 24 2016/9/5 1.49 EPII-SD- 25 2016/9/20 0.9 EPII-SD- 26 2016/9/27 0.66 EPII-SD- 27 2016/10/14 1.05 EPII-SD- 28 2016/10/20 1.15 EPII-SD- 29 2016/10/22 0.74 EPII-SD- 30 2016/10/20 0.1 EFII-SD- 41 2016/5/29 0.87 EFII-SD- 42 2016/5/31 0.9 EFII-SD- 43 2016/6/1 0.8 EFII-SD- 44 2016/6/2 0.92 EFII-SD- 45 2016/6/9 0.81 EFII-SD- 46 2016/7/4 0.72 EFII-SD- 47 2016/7/12 0.65 EFII-SD- 48 2016/8/6 0.73 EFII-SD- 49 2016/8/9 0.86 EFII-SD- 50 2016/8/10 0.92

31

2.3-3

2.3-4

(g)

EPII-CF- 21 9.3 % 480.02 435.40 90.7 %

EPII-CF- 22 9.5 % 480.04 436.99 91.0 %

EPII-CF- 23 9.6 % 480.05 438.25 91.3 %

EPII-CF- 24 10.1 % 480.07 440.74 91.8 %

EPII-CF- 25 9.2 % 480.03 439.69 91.6 % EPII-CF- 26 10.9 % 480.06 437.74 91.2 % EPII-CF- 27 10.4 % 480.08 439.11 91.5 %

EPII-CF- 28 9.5 % 480.05 438.38 91.3 %

EPII-CF- 29 8.3 % 480.01 437.74 91.2 %

EPII-CF- 30 9.7 % 480.09 441.01 91.9 %

EFII-CF- 41 2.3 % 81.2 % EFII-CF- 42 8.0 % 79.0 % EFII-CF- 43 4.7 % 82.6 % EFII-CF- 44 8.8 % 79.6 % EFII-CF- 45 2.4 % 79.8 % EFII-CF- 46 7.9 % 78.4 % EFII-CF- 47 4.5 % 81.8 % EFII-CF- 48 7.2 % 81.3 % EFII-CF- 49 5.7 % 78.9 % EFII-CF- 50 2.1 % 76.5 %

32

2.3-5

21

2016.8.2 2016.8.2

22

2016.8.5 2016.8.5

23

2016.8.18 2016.8.18

24

2016.9.14 2015.9.14

25

2016.9.23 2016.9.23

33

2.3-5

26

2016.9.29 2016.9.29

27

2016.10.17 2016.10.17

28

2016.10.24 2016.10.24

29

2016.10.24 2016.10.24

30

2016.10.28 2016.10.28

34

2.3-6

41

2016.5.31 2016.5.31

42

2016.6.2 2016.6.2

43

2016.6.2 2016.6.2

44

2016.6.6 2016.6.6

45

2016.6.10 2016.6.10

35

2.3-6

46

2016.7.6 2016.7.6

47

2016.7.13 2016.7.13

48

2016.8.8 2016.8.8

49 1

2016.8.11 2016.8.11

50 2

2016.8.12 2016.8.12

36

2.3-7 28

pH CEC Ca K Al Fe

No. (H2O) meq/100g mg/100g mg/100g g/kg g/kg

EPII-SD- 21 5.7 15 156 10 2.3 4.7 EPII-SD- 22 5.5 10 96 13 2.2 3.9 EPII-SD- 23 4.7 10 49 12 1.2 2.1 EPII-SD- 24 6.6 8 137 9 3.2 3.7 EPII-SD- 25 5.5 20 186 15 3.0 10.4 EPII-SD- 26 5.5 24 169 61 4.8 3.0 EPII-SD- 27 5.8 19 141 27 9.6 9.7 EPII-SD- 28 5.6 18 165 17 2.1 11.5 EPII-SD- 29 5.3 37 329 29 3.2 10.9 EPII-SD- 30 5.2 39 246 18 14.5 16.5 EFII-SD- 41 3.9 20 30 41 5.0 6.0 EFII-SD- 42 5.4 10 64 25 3.2 3.8 EFII-SD- 43 5 19 158 29 4.1 5.9 EFII-SD- 44 7 16 354 25 2.2 4.7 EFII-SD- 45 6.9 21 461 39 3.6 3.6 EFII-SD- 46 6 26 354 56 12.4 3.7 EFII-SD- 47 5.6 26 268 71 28.6 10.6 EFII-SD- 48 4.5 36 28 30 10.7 14.5 EFII-SD- 49 6.1 31 435 47 3.3 7.1 EFII-SD- 50 5 13 85 10 2.7 6.1

2.3-8 14-18 26-28

p<0.05

pH CEC Ca K Al Fe

Sample (H2O) meq/100g mg/100g mg/100g g/kg g/kg

Paddy field H14−18 5.7 13.3 171 19 3.5 6.6 H26-28 5.7 15.2 140 18 3.9 6.0

Upland field H14−18 6.3 14.1 252 44 6.2 7.6 H26-28 5.9 20.4* 192 33 9.6 7.2

37

2.3-9 28

B Na Mg Al Si P K Ca Cr Mn Fe Sample code mg/kg mg/kg mg/kg g/kg g/kg g/kg mg/kg mg/kg mg/kg mg/kg g/kg EPII-SD- 21 4.1E+1 1.4E+4 3.8E+3 6.7E+1 3.0E+2 1.7E+0 1.3E+4 4.8E+3 4.7E+1 2.7E+2 2.6E+1 EPII-SD- 22 3.0E+1 1.5E+4 4.7E+3 8.5E+1 2.8E+2 8.3E-1 1.6E+4 6.8E+3 2.6E+1 3.8E+2 2.8E+1 EPII-SD- 23 4.3E+1 8.2E+3 2.0E+3 5.9E+1 3.3E+2 7.4E-1 2.1E+4 9.3E+2 4.6E+1 1.3E+2 1.3E+1 EPII-SD- 24 2.1E+1 5.4E+3 3.4E+3 5.1E+1 3.5E+2 7.5E-1 1.3E+4 3.3E+3 5.4E+1 5.6E+2 2.7E+1 EPII-SD- 25 1.7E+1 1.2E+4 6.1E+3 8.4E+1 2.6E+2 1.3E+0 9.6E+3 1.1E+4 2.7E+1 6.1E+2 4.7E+1 EPII-SD- 26 1.6E+1 1.5E+4 6.5E+3 7.7E+1 2.6E+2 2.0E+0 9.9E+3 1.0E+4 1.8E+1 4.3E+2 2.8E+1 EPII-SD- 27 2.2E+1 1.3E+4 8.1E+3 8.0E+1 2.5E+2 2.1E+0 1.2E+4 1.4E+4 4.7E+1 7.5E+2 4.1E+1 EPII-SD- 28 7.0E+0 1.1E+4 2.4E+4 9.1E+1 2.1E+2 1.2E+0 4.1E+3 2.3E+4 4.2E+2 1.4E+3 6.2E+1 EPII-SD- 29 3.2E+1 1.0E+4 1.1E+4 7.2E+1 2.6E+2 1.1E+0 1.3E+4 1.2E+4 6.4E+1 4.3E+2 3.6E+1 EPII-SD- 30 1.4E+1 7.0E+3 5.0E+3 7.8E+1 2.1E+2 5.2E+0 4.2E+3 9.7E+3 5.5E+1 5.8E+2 5.7E+1 EFII-SD- 41 1.8E+1 1.3E+3 6.5E+2 4.5E+1 1.8E+2 2.7E+0 4.3E+3 7.3E+2 1.7E+2 9.8E+2 8.9E+1 EFII-SD- 42 5.1E+1 1.4E+4 1.1E+4 6.4E+1 3.0E+2 1.8E+0 2.1E+4 1.1E+4 8.4E+1 1.0E+3 4.0E+1 EFII-SD- 43 1.7E+1 8.7E+2 4.6E+2 4.1E+1 1.8E+2 1.6E+0 2.4E+3 7.3E+2 5.7E+1 1.3E+3 8.1E+1 EFII-SD- 44 2.7E+1 1.5E+4 9.8E+3 7.0E+1 2.7E+2 2.2E+0 1.5E+4 1.4E+4 8.8E+1 8.8E+2 4.2E+1 EFII-SD- 45 6.9E+1 5.3E+3 3.2E+3 6.4E+1 2.8E+2 3.8E+0 1.9E+4 8.7E+3 6.6E+1 6.1E+2 2.7E+1 EFII-SD- 46 1.0E+1 1.5E+4 8.5E+3 6.8E+1 2.6E+2 3.0E+0 8.1E+3 1.9E+4 2.2E+1 7.9E+2 3.1E+1 EFII-SD- 47 2.4E+1 1.1E+4 6.5E+3 7.2E+1 2.1E+2 2.2E+0 9.7E+3 8.7E+3 4.6E+1 9.0E+2 4.9E+1 EFII-SD- 48 4.6E+1 6.2E+3 3.1E+3 6.1E+1 2.3E+2 1.8E+0 1.4E+4 2.4E+3 7.1E+1 6.9E+2 3.8E+1 EFII-SD- 49 2.9E+1 8.4E+3 3.9E+3 6.0E+1 2.4E+2 2.0E+0 9.0E+3 7.6E+3 9.9E+1 4.2E+2 3.3E+1 EFII-SD- 50 2.7E+1 1.4E+4 2.3E+4 7.2E+1 2.4E+2 1.9E+0 7.3E+3 4.1E+4 4.7E+1 1.5E+3 6.9E+1

Co Ni Cu Zn Rb Sr Mo Cd Ba Hg Sample code mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg EPII-SD- 21 8.2E+0 1.7E+1 2.1E+1 9.7E+1 5.7E+1 5.8E+1 3.2E-1 2.1E-1 2.6E+2 9.0E-2 EPII-SD- 22 8.5E+0 1.0E+1 1.4E+1 7.2E+1 8.3E+1 7.9E+1 4.5E-1 1.4E-1 3.5E+2 7.0E-2 EPII-SD- 23 4.2E+0 1.5E+1 1.7E+1 6.1E+1 4.2E+1 4.3E+1 1.9E-1 2.2E-1 3.9E+2 1.8E-1 EPII-SD- 24 1.1E+1 2.2E+1 2.3E+1 6.8E+1 3.6E+1 3.4E+1 5.0E-1 1.4E-1 2.0E+2 3.0E-2 EPII-SD- 25 1.2E+1 1.1E+1 1.7E+1 8.9E+1 9.5E+1 8.8E+1 8.3E-1 2.0E-1 3.9E+2 9.0E-2 EPII-SD- 26 7.3E+0 8.9E+0 3.3E+1 1.2E+2 8.9E+1 8.1E+1 9.2E-1 4.7E-1 3.1E+2 2.0E-1 EPII-SD- 27 1.3E+1 2.2E+1 3.5E+1 1.5E+2 1.2E+2 1.1E+2 1.4E+0 4.9E-1 3.6E+2 1.7E-1 EPII-SD- 28 3.1E+1 7.6E+1 6.2E+1 1.1E+2 2.5E+2 2.3E+2 5.9E-1 3.1E-1 2.8E+2 4.0E-2 EPII-SD- 29 1.1E+1 2.3E+1 2.4E+1 1.1E+2 1.2E+2 1.2E+2 2.1E+0 4.1E-1 4.0E+2 1.4E-1 EPII-SD- 30 1.8E+1 1.9E+1 3.9E+1 1.2E+2 6.1E+1 5.6E+1 1.6E+0 7.6E-1 2.0E+2 2.1E-1 EFII-SD- 41 3.2E+1 4.2E+1 3.6E+1 1.4E+2 8.0E+0 8.2E+0 1.4E+0 7.2E-2 3.1E+2 7.0E-2 EFII-SD- 42 1.4E+1 3.4E+1 4.3E+1 1.7E+2 1.8E+2 1.8E+2 6.1E-1 3.5E-1 4.2E+2 4.0E-2 EFII-SD- 43 3.3E+1 2.9E+1 3.0E+1 1.5E+2 5.9E+0 6.2E+0 1.1E+0 1.5E-1 3.6E+2 3.0E-2 EFII-SD- 44 1.5E+1 3.5E+1 1.8E+2 5.4E+2 1.6E+2 1.6E+2 9.6E-1 1.0E+0 3.7E+2 3.5E-1 EFII-SD- 45 9.5E+0 2.1E+1 4.1E+1 2.2E+2 4.4E+1 4.4E+1 6.8E-1 3.2E-1 3.4E+2 2.0E-1 EFII-SD- 46 1.1E+1 1.2E+1 2.0E+1 9.1E+1 1.9E+2 1.9E+2 2.9E-1 2.4E-1 2.1E+2 6.0E-2 EFII-SD- 47 1.4E+1 1.7E+1 1.5E+1 1.1E+2 7.6E+1 7.5E+1 1.8E+0 2.0E-1 2.6E+2 1.0E-1 EFII-SD- 48 9.6E+0 2.4E+1 2.5E+1 1.2E+2 3.7E+1 3.7E+1 2.2E+0 4.2E-1 2.1E+2 1.4E-1 EFII-SD- 49 1.4E+1 3.0E+1 2.6E+1 8.3E+1 5.2E+1 5.1E+1 7.3E-1 2.7E-1 3.0E+2 2.1E-1 EFII-SD- 50 2.4E+1 1.8E+1 3.8E+1 1.1E+2 2.2E+2 2.1E+2 7.2E-1 1.9E-1 2.7E+2 5.0E-2

38

2.3-10 28

Sample code Li mg/kg

Na mg/kg

Mg mg/kg

Al mg/kg

Si mg/kg

P mg/kg

K mg/kg

Ca mg/kg

Cr mg/kg

Mn mg/kg

EPII-CF- 21 4.7E-3 2.3E+1 1.4E+3 4.9E+0 1.7E+2 4.3E+3 3.1E+3 8.5E+1 1.4E-1 2.4E+1 EPII-CF- 22 4.4E-3 3.2E+1 1.3E+3 2.9E-1 2.2E+2 3.8E+3 3.2E+3 9.1E+1 1.2E-1 3.1E+1 EPII-CF- 23 5.6E-3 1.6E+1 1.1E+3 1.2E+0 4.5E+2 3.6E+3 3.3E+3 8.0E+1 1.2E-1 3.8E+1 EPII-CF- 24 7.3E-3 2.8E+1 1.1E+3 8.9E+0 3.1E+2 3.5E+3 3.3E+3 7.7E+1 2.5E-1 2.8E+1 EPII-CF- 25 2.5E-3 1.8E+1 1.2E+3 1.4E+0 1.2E+2 4.0E+3 3.4E+3 8.0E+1 1.3E-1 2.8E+1 EPII-CF- 26 5.7E-3 1.0E+1 1.2E+3 1.1E+0 3.0E+2 3.3E+3 2.9E+3 1.0E+2 1.4E-1 2.9E+1 EPII-CF- 27 1.8E-3 2.2E+1 1.2E+3 2.8E-1 3.3E+2 3.8E+3 3.2E+3 9.2E+1 1.3E-1 4.3E+1 EPII-CF- 28 1.8E-3 8.5E+0 1.2E+3 4.2E-1 6.9E+1 3.2E+3 2.7E+3 8.8E+1 1.6E-1 3.3E+1 EPII-CF- 29 3.6E-3 1.8E+1 1.3E+3 3.5E+0 1.6E+2 3.1E+3 2.9E+3 8.3E+1 1.6E-1 4.4E+1 EPII-CF- 30 1.4E-3 1.0E+1 1.4E+3 1.6E-1 2.0E+2 3.3E+3 2.9E+3 8.7E+1 1.5E-1 3.3E+1 EFII-CF- 41 1.2E-2 3.5E+1 1.0E+3 5.9E+1 5.7E+1 2.5E+3 1.9E+4 1.4E+2 9.4E-2 5.2E+1 EFII-CF- 42 3.6E-3 2.7E+1 1.0E+3 7.4E+0 1.7E+1 3.9E+3 2.5E+4 1.6E+2 6.2E-2 9.7E+0 EFII-CF- 43 2.8E-3 3.3E+1 1.0E+3 1.4E+1 1.7E+1 2.9E+3 2.3E+4 3.8E+2 4.1E-2 1.2E+1 EFII-CF- 44 1.6E-3 1.6E+1 8.7E+2 3.5E+0 9.9E+0 3.4E+3 2.1E+4 5.1E+2 5.8E-2 5.3E+0 EFII-CF- 45 9.3E-4 1.4E+1 1.0E+3 3.9E+0 7.8E+0 3.5E+3 2.4E+4 3.5E+2 5.6E-2 7.3E+0 EFII-CF- 46 1.5E-3 2.1E+1 1.2E+3 6.2E+0 1.0E+1 3.1E+3 2.3E+4 1.7E+2 4.7E-2 7.3E+0 EFII-CF- 47 3.6E-3 2.1E+1 9.9E+2 3.4E+0 6.8E+0 2.4E+3 2.3E+4 1.8E+2 5.0E-2 6.7E+0 EFII-CF- 48 1.2E-3 2.4E+1 9.1E+2 1.6E+0 4.2E+0 2.1E+3 2.2E+4 1.4E+2 4.7E-2 9.6E+0 EFII-CF- 49 1.4E-3 1.2E+1 1.0E+3 3.4E+0 9.2E+0 3.5E+3 2.2E+4 2.9E+2 4.8E-2 5.7E+0 EFII-CF- 50 1.8E-3 1.7E+1 8.7E+2 5.1E+0 1.1E+1 2.6E+3 1.7E+4 1.6E+2 3.5E-2 6.5E+0

Sample code Fe mg/kg

Co mg/kg

Ni mg/kg

Cu mg/kg

Zn mg/kg

Rb mg/kg

Sr mg/kg

Mo mg/kg

Cd mg/kg

Ba mg/kg

EPII-CF- 21 1.6E+1 1.1E-2 9.1E-2 2.0E+0 2.4E+1 3.7E+0 2.0E-1 7.4E-1 8.5E-3 3.6E-1 EPII-CF- 22 1.0E+1 1.2E-2 8.6E-2 2.9E+0 2.6E+1 2.8E+0 2.8E-1 1.2E+0 1.3E-2 1.6E+0 EPII-CF- 23 1.1E+1 6.0E-3 8.0E-1 3.9E+0 3.0E+1 3.2E+0 2.0E-1 2.1E+0 1.8E-1 8.0E-1 EPII-CF- 24 3.4E+1 2.2E-2 1.5E-1 3.1E+0 3.8E+1 2.7E+0 3.5E-1 1.3E+0 2.0E-3 4.3E-1 EPII-CF- 25 8.5E+0 1.4E-2 7.2E-2 9.9E-1 2.3E+1 7.4E+0 1.6E-1 1.2E+0 1.7E-2 1.4E-1 EPII-CF- 26 1.2E+1 4.0E-3 1.6E-1 3.9E+0 2.4E+1 1.5E+0 1.9E-1 8.5E-1 1.1E-1 4.6E-1 EPII-CF- 27 8.3E+0 8.5E-3 9.2E-2 3.3E+0 2.4E+1 4.2E+0 1.7E-1 9.9E-1 6.3E-2 4.2E-1 EPII-CF- 28 1.1E+1 1.1E-2 1.4E-1 2.5E+0 2.5E+1 8.8E+0 2.8E-1 5.9E-1 2.1E-2 5.9E-1 EPII-CF- 29 1.1E+1 9.0E-3 8.9E-1 3.0E+0 2.5E+1 8.5E+0 2.0E-1 1.5E+0 3.1E-1 6.1E-1 EPII-CF- 30 1.0E+1 7.5E-3 9.4E-2 2.1E+0 2.3E+1 2.2E+0 1.1E-1 5.1E-1 8.5E-3 1.3E-1 EFII-CF- 41 4.0E+1 2.0E+0 4.1E-1 4.5E+0 2.1E+1 1.6E+1 5.4E-1 7.5E-2 4.0E-2 2.5E+0 EFII-CF- 42 1.4E+1 5.8E-2 2.1E-1 4.8E+0 1.4E+1 1.2E+1 4.4E-1 2.7E-1 5.0E-2 1.1E+0 EFII-CF- 43 2.6E+1 1.3E-1 1.2E-1 4.1E+0 1.8E+1 1.8E+1 1.9E+0 3.8E-2 1.6E-1 8.5E+0 EFII-CF- 44 1.5E+1 2.1E-2 8.2E-2 5.7E+0 1.8E+1 6.6E+0 1.4E+0 6.2E-1 1.1E-1 9.8E-1 EFII-CF- 45 1.8E+1 2.3E-2 6.1E-2 4.0E+0 1.7E+1 9.8E+0 7.0E-1 3.1E-1 3.0E-2 4.4E-1 EFII-CF- 46 2.1E+1 4.1E-2 5.6E-2 2.1E+0 1.5E+1 9.3E+0 5.9E-1 6.8E-1 5.0E-2 2.7E-1 EFII-CF- 47 1.9E+1 3.5E-2 2.0E-1 2.5E+0 1.5E+1 7.3E+0 1.0E+0 2.3E-1 1.1E-1 4.9E-1 EFII-CF- 48 1.5E+1 8.3E-2 3.0E-1 5.2E+0 2.0E+1 1.7E+1 4.8E-1 7.5E-2 1.2E-1 1.7E+0 EFII-CF- 49 1.6E+1 8.7E-2 2.1E-1 4.8E+0 1.3E+1 4.7E+0 9.4E-1 1.6E-1 1.5E-1 1.5E+0 EFII-CF- 50 1.4E+1 6.8E-2 6.0E-1 4.5E+0 1.1E+1 4.9E+0 6.9E-1 1.3E-1 7.0E-2 1.1E+0

39

2.3-11 28

Sample code Na Mg Al Si P K ex. K* Ca ex. Ca* EPII-CF-21 1.6E-3 3.6E-1 7.3E-5 5.6E-4 2.5E+0 2.4E-1 3.0E+1 1.8E-2 5.4E-2 EPII-CF-22 2.1E-3 2.8E-1 3.4E-6 7.9E-4 4.5E+0 2.0E-1 2.5E+1 1.3E-2 9.5E-2 EPII-CF-23 2.0E-3 5.5E-1 1.9E-5 1.3E-3 4.8E+0 1.6E-1 2.9E+1 8.6E-2 1.7E-1 EPII-CF-24 5.1E-3 3.4E-1 1.8E-4 9.0E-4 4.7E+0 2.6E-1 3.7E+1 2.3E-2 5.6E-2 EPII-CF-25 1.5E-3 2.0E-1 1.7E-5 4.8E-4 3.0E+0 3.5E-1 2.4E+1 7.3E-3 4.3E-2 EPII-CF-26 6.6E-4 1.9E-1 1.4E-5 1.2E-3 1.6E+0 2.9E-1 4.7E+0 1.0E-2 6.0E-2 EPII-CF-27 1.7E-3 1.5E-1 3.5E-6 1.3E-3 1.8E+0 2.7E-1 1.2E+1 6.8E-3 6.5E-2 EPII-CF-28 7.4E-4 5.0E-2 4.7E-6 3.2E-4 2.6E+0 6.6E-1 1.6E+1 3.8E-3 5.3E-2 EPII-CF-29 1.7E-3 1.2E-1 4.9E-5 6.0E-4 2.9E+0 2.3E-1 1.0E+1 7.1E-3 2.5E-2 EPII-CF-30 1.5E-3 2.9E-1 2.0E-6 9.6E-4 6.4E-1 6.9E-1 1.6E+1 9.0E-3 3.6E-2 EFII-CF-41 2.6E-2 1.6E+0 1.3E-3 3.2E-4 9.4E-1 4.4E+0 4.6E+1 1.9E-1 4.6E-1 EFII-CF-42 2.0E-3 9.7E-2 1.2E-4 5.9E-5 2.1E+0 1.2E+0 9.9E+1 1.4E-2 2.5E-1 EFII-CF-43 3.8E-2 2.2E+0 3.4E-4 9.6E-5 1.8E+0 9.7E+0 7.8E+1 5.2E-1 2.4E-1 EFII-CF-44 1.1E-3 8.8E-2 5.0E-5 3.6E-5 1.5E+0 1.4E+0 8.4E+1 3.6E-2 1.5E-1 EFII-CF-45 2.7E-3 3.1E-1 6.0E-5 2.8E-5 9.4E-1 1.2E+0 6.1E+1 4.0E-2 7.6E-2 EFII-CF-46 1.4E-3 1.4E-1 9.1E-5 4.1E-5 1.1E+0 2.9E+0 4.2E+1 8.7E-3 4.8E-2 EFII-CF-47 2.0E-3 1.5E-1 4.7E-5 3.2E-5 1.1E+0 2.4E+0 3.2E+1 2.0E-2 6.6E-2 EFII-CF-48 3.8E-3 2.9E-1 2.7E-5 1.8E-5 1.2E+0 1.6E+0 7.4E+1 5.7E-2 5.0E-1 EFII-CF-49 1.5E-3 2.6E-1 5.6E-5 3.9E-5 1.8E+0 2.5E+0 4.8E+1 3.9E-2 6.8E-2 EFII-CF-50 1.2E-3 3.8E-2 7.0E-5 4.4E-5 1.3E+0 2.4E+0 1.7E+2 3.8E-3 1.8E-1

Cr Mn Fe Co Ni Cu Zn Rb Sr Cd Ba

EPII-CF-21 3.1E-3 8.7E-2 6.3E-4 1.3E-3 5.5E-3 9.5E-2 2.5E-1 6.5E-2 3.4E-3 4.1E-2 1.4E-3 EPII-CF-22 4.7E-3 8.1E-2 3.6E-4 1.4E-3 8.3E-3 2.0E-1 3.7E-1 3.4E-2 3.6E-3 9.2E-2 4.6E-3 EPII-CF-23 2.7E-3 2.9E-1 8.7E-4 1.4E-3 5.3E-2 2.3E-1 5.0E-1 7.6E-2 4.6E-3 7.9E-1 2.0E-3 EPII-CF-24 4.6E-3 5.0E-2 1.3E-3 2.1E-3 6.6E-3 1.4E-1 5.6E-1 7.3E-2 1.0E-2 1.4E-2 2.2E-3 EPII-CF-25 4.9E-3 4.7E-2 1.8E-4 1.1E-3 6.4E-3 5.9E-2 2.6E-1 7.7E-2 1.8E-3 8.3E-2 3.6E-4 EPII-CF-26 7.7E-3 6.7E-2 4.2E-4 5.5E-4 1.7E-2 1.2E-1 2.0E-1 1.7E-2 2.3E-3 2.3E-1 1.5E-3 EPII-CF-27 2.8E-3 5.7E-2 2.0E-4 6.5E-4 4.1E-3 9.5E-2 1.6E-1 3.4E-2 1.5E-3 1.3E-1 1.2E-3 EPII-CF-28 3.9E-4 2.4E-2 1.7E-4 3.4E-4 1.8E-3 4.1E-2 2.4E-1 3.6E-2 1.2E-3 6.8E-2 2.1E-3 EPII-CF-29 2.4E-3 1.0E-1 3.1E-4 8.5E-4 3.9E-2 1.3E-1 2.3E-1 6.8E-2 1.7E-3 7.6E-1 1.5E-3 EPII-CF-30 2.7E-3 5.6E-2 1.8E-4 4.2E-4 4.9E-3 5.4E-2 1.8E-1 3.5E-2 2.1E-3 1.1E-2 6.7E-4 EFII-CF-41 5.6E-4 5.3E-2 4.6E-4 6.3E-2 9.9E-3 1.2E-1 1.5E-1 2.0E+0 6.6E-2 4.9E-1 8.1E-3 EFII-CF-42 7.4E-4 9.4E-3 3.6E-4 4.2E-3 6.0E-3 1.1E-1 8.1E-2 6.6E-2 2.5E-3 1.4E-1 2.6E-3 EFII-CF-43 7.2E-4 9.1E-3 3.3E-4 4.1E-3 4.2E-3 1.4E-1 1.3E-1 3.0E+0 3.1E-1 1.1E+0 2.4E-2 EFII-CF-44 6.6E-4 6.0E-3 3.6E-4 1.4E-3 2.3E-3 3.2E-2 3.4E-2 4.1E-2 8.9E-3 1.1E-1 2.7E-3 EFII-CF-45 8.5E-4 1.2E-2 6.6E-4 2.4E-3 2.9E-3 9.9E-2 7.7E-2 2.2E-1 1.6E-2 1.0E-1 1.3E-3 EFII-CF-46 2.1E-3 9.2E-3 6.6E-4 3.8E-3 4.8E-3 1.1E-1 1.6E-1 4.8E-2 3.1E-3 2.2E-1 1.3E-3 EFII-CF-47 1.1E-3 7.5E-3 3.8E-4 2.6E-3 1.2E-2 1.6E-1 1.3E-1 9.6E-2 1.3E-2 5.5E-1 1.9E-3 EFII-CF-48 6.6E-4 1.4E-2 4.0E-4 8.6E-3 1.3E-2 2.1E-1 1.7E-1 4.7E-1 1.3E-2 2.9E-1 8.1E-3 EFII-CF-49 4.8E-4 1.4E-2 4.8E-4 6.2E-3 7.1E-3 1.9E-1 1.5E-1 9.1E-2 1.9E-2 5.5E-1 5.1E-3 EFII-CF-50 7.6E-4 4.3E-3 2.0E-4 2.9E-3 3.4E-2 1.2E-1 9.8E-2 2.3E-2 3.2E-3 3.9E-1 3.9E-3

* K Ca TF.

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Sample code Li Be V Ga As Mo Cd Cs Ba La Ce Pr Nd

mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg EPII-SD-11 2.8E+1 1.2E+0 1.2E+2 5.1E+0 1.3E+1 2.9E-1 1.6E-1 3.5E+0 2.5E+2 1.5E+1 4.0E+1 3.9E+0 1.5E+1 EPII-SD-12 5.0E+1 1.9E+0 8.9E+1 5.6E+0 7.4E+0 4.0E-1 3.6E-1 6.6E+0 2.7E+2 2.5E+1 6.0E+1 6.2E+0 2.3E+1 EPII-SD-13 4.3E+1 1.9E+0 8.1E+1 4.8E+0 7.5E+0 4.7E-1 2.7E-1 6.5E+0 1.6E+2 1.1E+1 3.2E+1 2.8E+0 1.1E+1 EPII-SD-14 3.1E+1 1.5E+0 6.0E+1 6.5E+0 5.5E+0 7.6E-1 3.3E-1 6.3E+0 4.0E+2 2.2E+1 4.5E+1 5.1E+0 1.9E+1 EPII-SD-15 2.1E+1 9.0E-1 1.2E+2 5.0E+0 6.1E+0 7.3E-1 4.2E-1 1.7E+0 2.9E+2 1.0E+1 2.5E+1 2.7E+0 1.1E+1 EPII-SD-16 1.3E+1 1.1E+0 1.2E+2 5.6E+0 7.2E+0 7.7E-1 4.7E-1 2.0E+0 3.0E+2 1.6E+1 3.3E+1 4.0E+0 1.7E+1 EPII-SD-17 2.2E+1 1.1E+0 9.4E+1 5.1E+0 1.2E+1 9.1E-1 5.8E-1 3.5E+0 2.6E+2 1.0E+1 2.6E+1 3.0E+0 1.2E+1 EPII-SD-18 2.9E+1 1.3E+0 1.9E+2 5.1E+0 1.3E+1 9.1E-1 5.3E-1 2.5E+0 2.0E+2 2.0E+1 3.4E+1 6.1E+0 2.5E+1 EPII-SD-19 2.1E+1 8.0E-1 8.1E+1 5.5E+0 1.6E+1 1.2E+0 3.9E-1 4.5E+0 4.1E+2 1.4E+1 3.2E+1 3.8E+0 1.5E+1 EPII-SD-20 2.5E+1 1.2E+0 1.3E+2 6.8E+0 1.8E+1 8.5E-1 2.8E-1 5.4E+0 5.0E+2 1.7E+1 4.0E+1 4.3E+0 1.7E+1 EFII-SD-31 3.6E+1 8.1E-1 7.5E+1 4.6E+0 1.2E+1 1.5E+0 3.8E-1 4.4E+0 2.3E+2 1.4E+1 3.9E+1 3.6E+0 1.4E+1 EFII-SD-32 1.5E+1 1.1E+0 1.2E+2 4.5E+0 6.9E+0 1.6E+0 4.4E-1 2.4E+0 1.5E+2 1.4E+1 2.6E+1 3.9E+0 1.6E+1 EFII-SD-33 3.4E+1 1.4E+0 1.2E+2 4.7E+0 8.1E+0 8.4E-1 2.4E-1 4.5E+0 1.9E+2 1.6E+1 3.6E+1 4.5E+0 1.7E+1 EFII-SD-34 2.9E+1 1.2E+0 9.5E+1 4.6E+0 1.9E+1 8.5E-1 6.6E-1 4.9E+0 2.1E+2 1.7E+1 3.8E+1 4.4E+0 1.7E+1 EFII-SD-35 3.2E+1 1.5E+0 8.2E+1 4.9E+0 1.8E+1 1.7E+0 4.5E-1 4.8E+0 1.6E+2 1.3E+1 2.4E+1 3.6E+0 1.5E+1 EFII-SD-36 4.1E+1 9.0E-1 1.4E+2 4.8E+0 2.3E+1 1.0E+0 6.2E-1 1.7E+0 1.6E+2 9.7E+0 2.4E+1 2.9E+0 1.3E+1 EFII-SD-37 2.8E+1 9.5E-1 7.4E+1 5.4E+0 1.3E+1 1.5E+0 3.2E-1 3.4E+0 3.6E+2 1.5E+1 3.4E+1 3.6E+0 1.4E+1 EFII-SD-38 3.9E+1 1.8E+0 1.4E+2 6.3E+0 2.0E+1 2.4E+0 5.2E-1 6.9E+0 2.7E+2 2.3E+1 5.3E+1 5.4E+0 2.1E+1 EFII-SD-39 2.6E+1 1.2E+0 1.5E+2 6.1E+0 1.7E+1 1.4E+0 4.1E-1 5.9E+0 3.3E+2 1.6E+1 4.0E+1 4.5E+0 1.8E+1 EFII-SD-40 9.0E+0 4.8E-1 9.3E+1 4.5E+0 6.6E+0 1.3E+0 4.1E-1 1.3E+0 2.0E+2 7.6E+0 1.7E+1 2.5E+0 1.2E+1

Sample code Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Pb Th U

mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg EPII-SD-11 3.1E+0 7.6E-1 3.3E+0 3.4E-1 2.5E+0 5.2E-1 1.5E+0 2.2E-1 1.5E+0 2.1E-1 1.2E+1 6.1E+0 2.0E+0

EPII-SD-12 4.2E+0 8.3E-1 3.8E+0 3.7E-1 2.4E+0 4.8E-1 1.4E+0 2.1E-1 1.5E+0 2.1E-1 2.4E+1 5.7E+0 3.3E+0 EPII-SD-13 2.0E+0 4.2E-1 2.1E+0 1.9E-1 1.6E+0 3.5E-1 1.1E+0 1.7E-1 1.2E+0 1.8E-1 2.5E+1 3.8E+0 2.7E+0

EPII-SD-14 4.1E+0 9.8E-1 4.5E+0 5.9E-1 4.2E+0 8.9E-1 2.7E+0 4.0E-1 2.8E+0 4.2E-1 2.3E+1 1.0E+1 3.7E+0

EPII-SD-15 2.5E+0 8.4E-1 2.8E+0 3.5E-1 2.8E+0 6.0E-1 1.9E+0 2.8E-1 2.0E+0 2.9E-1 1.5E+1 3.2E+0 2.3E+0 EPII-SD-16 4.1E+0 1.2E+0 4.8E+0 6.7E-1 4.8E+0 1.0E+0 3.0E+0 4.3E-1 2.9E+0 4.4E-1 1.6E+1 5.0E+0 2.2E+0


EPII-SD-18 5.5E+0 1.4E+0 5.8E+0 7.6E-1 4.9E+0 1.0E+0 3.0E+0 4.2E-1 2.8E+0 4.1E-1 2.0E+1 7.1E+0 3.0E+0


EPII-SD-20 3.7E+0 1.0E+0 4.1E+0 5.3E-1 3.7E+0 7.6E-1 2.3E+0 3.3E-1 2.3E+0 3.4E-1 2.1E+1 6.8E+0 2.5E+0

EFII-SD-31 2.8E+0 5.9E-1 2.9E+0 3.7E-1 2.6E+0 5.4E-1 1.7E+0 2.6E-1 1.8E+0 2.7E-1 2.8E+1 8.5E+0 3.1E+0

EFII-SD-32 3.8E+0 1.0E+0 4.1E+0 5.9E-1 4.0E+0 8.4E-1 2.6E+0 3.7E-1 2.6E+0 3.8E-1 1.6E+1 5.5E+0 2.2E+0







EFII-SD-39 4.2E+0 1.1E+0 4.6E+0 6.9E-1 4.5E+0 9.4E-1 2.9E+0 4.2E-1 2.9E+0 4.3E-1 2.6E+1 7.1E+0 3.0E+0

EFII-SD-40 3.5E+0 1.1E+0 4.5E+0 7.3E-1 5.1E+0 1.1E+0 3.4E+0 5.0E-1 3.4E+0 5.2E-1 8.5E+0 1.8E+0 2.5E+0

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Sample code Li Be V Ga As Mo Cd Cs Ba La Ce Pr Nd mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg

EPII-CF-11 2.8E-3 1.2E-3 1.8E-2 3.5E-3 1.8E-1 4.6E-1 2.4E-2 5.4E-3 5.5E-1 3.3E-4 2.2E-3 n.d. 1.4E-4 EPII-CF-12 7.2E-3 1.7E-3 3.0E-2 4.9E-3 9.1E-2 7.8E-1 2.7E-2 3.0E-3 7.1E-1 1.5E-3 4.6E-3 n.d. 1.3E-3


EPII-CF-15 5.2E-3 1.1E-3 1.4E-2 3.4E-3 5.0E-2 1.1E+0 5.5E-2 3.2E-3 4.8E-1 3.4E-4 1.5E-3 n.d. 4.1E-4


EPII-CF-18 3.2E-3 9.0E-4 6.9E-3 1.6E-3 3.0E-1 3.8E-1 2.2E-2 7.5E-3 1.6E-1 3.2E-4 5.2E-4 n.d. 1.5E-4

EPII-CF-19 3.0E-3 2.8E-4 1.6E-2 8.4E-4 9.5E-2 4.8E-1 2.1E-2 1.7E-3 1.0E-1 2.9E-4 1.0E-3 n.d. 2.9E-4 EPII-CF-20 2.4E-3 4.0E-4 1.2E-2 1.3E-3 1.4E-1 7.7E-1 2.2E-2 6.0E-3 9.7E-2 2.0E-4 6.7E-4 n.d. 3.5E-4 EFII-CF-31 7.9E-3 2.7E-3 5.8E-2 1.4E-2 3.4E-2 7.4E-1 3.1E-2 1.0E-2 9.6E-1 7.3E-3 6.2E-3 1.4E-3 5.6E-3

EFII-CF-32 8.6E-3 2.6E-3 5.3E-2 9.0E-3 3.1E-2 4.9E-1 4.6E-2 6.5E-2 3.7E-1 1.8E-3 3.3E-3 3.9E-4 1.8E-3

EFII-CF-33 1.6E-2 3.0E-3 1.4E-1 2.7E-2 3.0E-2 3.3E-1 4.6E-2 2.8E-2 2.6E+0 4.8E-3 6.8E-3 9.6E-4 3.5E-3 EFII-CF-34 1.5E-2 3.8E-3 1.5E-1 1.1E-2 3.4E-2 3.7E-1 9.0E-2 7.5E-3 6.6E-1 5.2E-3 1.1E-2 1.2E-3 5.0E-3

EFII-CF-35 1.5E-2 3.0E-3 4.7E-2 1.4E-2 2.1E-2 3.4E-1 7.3E-2 2.6E-2 1.2E+0 2.2E-3 3.9E-3 4.5E-4 1.7E-3



EFII-CF-38 1.2E-2 2.6E-3 5.5E-2 1.5E-2 2.3E-2 4.2E-1 7.8E-2 7.7E-3 1.3E+0 8.3E-3 1.4E-2 1.6E-3 6.2E-3



Sample code Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Pb Th U

mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg mg/kg EPII-CF-11 n.d. n.d. 4.2E-4 n.d. n.d. n.d. 2.9E-4 n.d. 1.7E-4 n.d. 7.5E-3 2.3E-3 5.4E-5 EPII-CF-12 n.d. n.d. 3.6E-4 n.d. n.d. n.d. 2.8E-4 n.d. 1.4E-4 n.d. 7.3E-3 1.2E-3 2.6E-4

EPII-CF-13 n.d. n.d. 4.3E-4 n.d. n.d. n.d. 2.5E-4 n.d. 2.5E-4 n.d. 6.0E-3 9.0E-4 1.8E-4

EPII-CF-14 n.d. n.d. 5.0E-5 n.d. n.d. n.d. 1.9E-4 n.d. 1.1E-4 n.d. 3.8E-3 5.5E-4 1.6E-4 EPII-CF-15 n.d. n.d. 1.1E-4 n.d. n.d. n.d. 1.1E-4 n.d. 6.3E-5 n.d. 1.8E-3 3.8E-4 1.1E-4

EPII-CF-16 n.d. n.d. 4.7E-4 n.d. n.d. n.d. 3.0E-4 n.d. 9.4E-5 n.d. 5.9E-3 2.7E-4 6.0E-5



EFII-CF-31 1.8E-3 2.5E-4 1.4E-3 n.d. 6.1E-4 2.5E-4 7.3E-4 1.2E-4 5.2E-4 7.2E-5 2.9E-2 5.7E-4 3.0E-4

EFII-CF-32 9.8E-4 5.1E-5 7.0E-4 n.d. 3.2E-5 8.7E-5 2.7E-4 3.5E-5 3.5E-4 5.5E-5 9.6E-3 4.5E-4 2.0E-4 EFII-CF-33 1.3E-3 5.5E-4 9.2E-4 n.d. 4.3E-4 1.7E-4 3.5E-4 9.3E-5 5.2E-4 6.6E-5 1.3E-2 7.9E-4 6.0E-4








42

2.3-14 27

Sample code Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Pb Th U EPII-CF-11 − − 1.3E-4 − − − 1.9E-4 − 1.2E-4 − 6.5E-4 3.7E-4 2.7E-5 EPII-CF-12 − − 9.5E-5 − − − 2.0E-4 − 9.6E-5 − 3.0E-4 2.1E-4 8.0E-5 EPII-CF-13 − − 2.0E-4 − − − 2.3E-4 − 2.0E-4 − 2.4E-4 2.4E-4 6.5E-5 EPII-CF-14 − − 1.1E-5 − − − 7.0E-5 − 4.0E-5 − 1.6E-4 5.4E-5 4.2E-5 EPII-CF-15 − − 3.9E-5 − − − 5.9E-5 − 3.2E-5 − 1.2E-4 1.2E-4 4.8E-5 EPII-CF-16 − − 9.9E-5 − − − 9.9E-5 − 3.2E-5 − 3.7E-4 5.3E-5 2.7E-5 EPII-CF-17 − − 5.1E-5 − − − 5.3E-5 − 4.4E-5 − 3.9E-5 9.0E-5 3.4E-5 EPII-CF-18 − − 6.7E-6 − − − 5.9E-5 − 2.6E-5 − 1.1E-4 2.9E-5 1.1E-5 EPII-CF-19 − − 7.2E-5 − − − 8.8E-5 − 3.8E-5 − 2.3E-5 4.5E-5 2.1E-5 EPII-CF-20 − − 9.5E-6 − − − 4.2E-5 − 4.8E-5 − 1.6E-5 2.1E-5 1.3E-5 EFII-CF-31 6.4E-4 4.2E-4 5.0E-4 − 2.3E-4 4.6E-4 4.2E-4 4.5E-4 2.8E-4 2.7E-4 1.1E-3 6.7E-5 9.9E-5 EFII-CF-32 2.6E-4 5.1E-5 1.7E-4 − 8.1E-6 1.0E-4 1.0E-4 9.5E-5 1.4E-4 1.5E-4 6.0E-4 8.3E-5 9.3E-5 EFII-CF-33 3.7E-4 7.1E-4 2.7E-4 − 1.5E-4 2.8E-4 1.8E-4 3.3E-4 2.6E-4 2.2E-4 6.6E-4 1.4E-4 2.2E-4 EFII-CF-34 4.2E-4 3.8E-4 4.0E-4 − 1.4E-4 5.5E-4 3.8E-4 7.0E-4 4.6E-4 1.2E-3 6.5E-4 2.7E-4 7.5E-4 EFII-CF-35 3.5E-4 5.1E-4 1.7E-4 − 1.1E-4 3.2E-4 1.8E-4 4.0E-4 1.5E-4 1.0E-3 3.4E-4 1.2E-4 8.8E-5 EFII-CF-36 3.8E-4 3.7E-4 2.7E-4 − 1.8E-4 2.3E-4 1.4E-4 3.5E-4 1.6E-4 8.1E-4 3.8E-4 1.1E-4 1.6E-4 EFII-CF-37 4.8E-4 4.1E-4 4.7E-4 − 4.2E-4 3.6E-4 3.1E-4 3.2E-4 3.0E-4 9.7E-4 6.8E-4 2.4E-4 3.5E-4 EFII-CF-38 4.3E-4 3.8E-4 3.0E-4 − 3.5E-4 2.8E-4 2.3E-4 3.0E-4 2.7E-4 7.9E-4 4.6E-4 2.4E-4 3.0E-4 EFII-CF-39 4.3E-4 3.6E-4 2.9E-4 − 2.3E-4 2.8E-4 2.4E-4 3.1E-4 3.0E-4 7.9E-4 1.4E-3 1.8E-4 2.8E-4 EFII-CF-40 1.8E-4 1.1E-4 1.0E-4 − 5.3E-5 1.1E-4 8.8E-5 1.4E-4 8.4E-5 4.2E-4 7.8E-4 1.0E-4 2.1E-4

Sample code Li Be V Ga As Mo Cd Cs Ba La Ce Pr Nd

EPII-CF-11 1.0E-4 9.9E-4 1.5E-4 7.0E-4 1.4E-2 1.6E+0 1.5E-1 1.6E-3 2.2E-3 2.2E-5 5.4E-5 9.2E-6



EPII-CF-14 2.2E-4 1.2E-3 4.1E-4 3.9E-4 1.2E-2 8.0E-1 7.6E-2 3.2E-3 1.0E-3 2.8E-5 4.9E-5 1.9E-5

















43

2.4-1 - 2016

, ˚C 5-9 , ˚C

7.5 (-3.7 – 20.2) 15.8

10.6 (-0.7 – 23.3) 18.8

11.7 (0.1 – 24.9) 20.4

10.4 (-0.8 – 22.8) 18.6

10.1 18.4

23.9 (7.5 – 27.0) 23.9

24.8 (5.7 – 28.2) 24.8

24.4 (7.5 – 27.3) 24.4

26.0 (11.7 – 28.5) 26.0 27.2 (17.0 – 28.9) 27.2

19.0 25.3

2.4-2

*1 mg/100g. *2 g/kg. *3 p<0.05, p<0.01.

(mg/kg)

GM t n GM (A) GSD n GM (B) GSD A/B p

Na 26 1.2E+4 1.3 21 1.1E+4 2.1 1.1 0.643 Mg 26 6.2E+3 1.6 21 5.5E+3 2.1 1.1 0.535 Al 26 7.3E+4 1.3 21 7.2E+4 1.5 1.0 0.939 Si 25 2.6E+5 1.1 21 2.7E+5 1.2 1.0 0.252 P 25 1.6E+3 1.6 21 1.7E+3 2.1 1.0 0.808 K 26 9.3E+3 1.5 21 1.2E+4 1.5 0.8 0.024 Ca 26 1.2E+4 1.6 21 9.4E+3 3.0 1.3 0.341 Cr 26 4.9E+1 1.7 21 6.1E+1 2.2 0.8 0.289 Mn 26 5.6E+2 1.9 21 5.4E+2 1.7 1.0 0.800 Fe 26 3.9E+4 1.3 21 3.3E+4 1.5 1.2 0.105 Co 26 1.2E+1 1.5 21 1.1E+1 1.7 1.1 0.619 Ni 26 2.0E+1 1.9 21 1.9E+1 2.1 1.1 0.706 Cu 26 2.5E+1 1.4 21 2.9E+1 2.0 0.9 0.430 Zn 26 1.0E+2 1.2 21 8.8E+1 1.4 1.2 0.031 Sr 26 9.0E+1 1.7 21 1.0E+2 1.9 0.9 0.458 Cd 26 3.5E-1 1.5 21 2.5E-1 1.6 1.4 0.017 Ba 26 2.6E+2 1.4 21 2.9E+2 1.3 0.9 0.290

Ca*1 25 1.7E+2 1.5 21 1.2E+2 1.8 1.5 0.015 *1 25 2.1E+1 1.6 21 1.6E+1 1.8 1.3 0.119

Al*2 25 4.2E+0 2.1 21 4.1E+0 2.7 1.0 0.896 Fe*2 25 9.0E+0 1.6 21 4.4E+0 1.9 2.1 0.000

pH*3 25 5.4 5.9 0.002

44

2.4-3

p<0.05, p<0.01.

2.4-4

*1 mg/kg TF . p<0.05, p<0.01.

(mg/kg)


Na 26 1.3E+1 2.9 21 2.4E+1 2.5 0.5 0.036 Mg 26 1.3E+3 1.1 21 1.4E+3 1.2 0.9 0.123 Al 21 1.7E+0 1.9 17 2.9E+0 2.2 0.6 0.032 Si 25 1.2E+2 1.9 21 2.1E+2 2.1 0.6 0.015 P 25 3.1E+3 1.1 21 3.3E+3 1.1 0.9 0.024 K 26 2.6E+3 1.1 21 2.6E+3 1.1 1.0 0.974 Ca 26 9.3E+1 1.3 21 9.8E+1 1.4 1.0 0.564 Cr 26 1.4E-1 3.0 21 1.8E-1 2.8 0.7 0.351 Mn 26 2.8E+1 1.4 21 2.7E+1 1.3 1.0 0.865 Fe 26 9.4E+0 1.3 21 1.3E+1 1.3 0.7 0.000 Co 26 9.4E-3 1.8 21 1.3E-2 1.5 0.7 0.031 Ni 26 2.2E-1 2.7 21 1.8E-1 2.3 1.2 0.477 Cu 26 2.2E+0 1.6 21 3.0E+0 1.4 0.7 0.008 Zn 26 2.1E+1 1.1 21 2.7E+1 1.1 0.8 < .0001 Sr 26 1.7E-1 1.6 21 2.2E-1 1.7 0.7 0.049 Cd 26 2.9E-2 3.3 21 1.7E-2 2.9 1.6 0.140 Ba 26 2.9E-1 2.2 21 5.4E-1 2.1 0.5 0.008


Na 26 1.0E-3 3.0 21 2.1E-3 2.9 0.5 0.031 Mg 26 2.1E-1 1.6 21 2.5E-1 2.1 0.8 0.333 Al 21 2.4E-5 2.4 17 4.0E-5 2.7 0.6 0.112 Si 25 4.7E-4 2.0 21 7.7E-4 2.1 0.6 0.025 P 25 2.0E+0 1.7 21 2.0E+0 2.2 1.0 0.888 K 26 2.8E-1 1.6 21 2.2E-1 1.4 1.3 0.024 Ca 26 7.7E-3 1.7 21 1.0E-2 3.0 0.7 0.266 Cr 26 2.8E-3 3.3 21 3.0E-3 3.2 0.9 0.839 Mn 26 4.9E-2 1.8 21 5.1E-2 1.8 1.0 0.856 Fe 26 2.4E-4 1.5 21 3.9E-4 1.7 0.6 0.002 Co 26 8.0E-4 1.6 21 1.2E-3 1.9 0.7 0.022 Ni 26 1.1E-2 2.6 21 9.8E-3 2.5 1.1 0.675 Cu 26 8.9E-2 1.6 21 1.1E-1 2.0 0.8 0.323 Zn 26 2.0E-1 1.2 21 3.0E-1 1.4 0.7 < .0001 Sr 26 1.8E-3 2.0 21 2.2E-3 2.5 0.8 0.457 Cd 26 8.2E-2 3.1 21 6.9E-2 2.9 1.2 0.614 Ba 26 1.1E-3 2.6 21 1.9E-3 2.0 0.6 0.032

Ca*1 25 5.5E-2 1.7 21 8.3E-2 2.0 0.7 0.027 *1 25 1.3E+1 1.7 21 1.7E+1 1.9 0.8 0.122

Al*1 21 4.5E-4 2.6 16 5.6E-4 3.0 0.8 0.530 Fe*1 25 1.3E-2 2.3 21 4.7E-2 3.4 0.3 0.000

45

2.5-1

2.5-2 Cs Kd 30˚C Kd RI

Code 10˚C 23˚C 30˚C

EP-SD-35 4810 1930 2550 ±130 EP-SD-36 3180 680 1310 ±30 EP-SD-37 1610 570 470 ±30 EP-SD-38 4580 2360 2530 ±130 EP-SD-39 7290 7800 8610 ±1170 EP-SD-40 7920 3560 3850 ±230 EP-SD-41 8490 5710 4810 ±80 EP-SD-42 8090 2950 3610 ±240 EP-SD-43 840 340 250 ±30 EP-SD-44 5160 2950 2660 ±280 EP-SD-45 5200 11700 2370 ±10 EP-SD-46 4960 4410 2250 ±40 EP-SD-47 4580 1640 780 ±40 EP-SD-48 6690 6710 3710 ±190 EP-SD-49 2040 880 850 ±50 EP-SD-50 1190 770 450 ±10 EP-SD-51 3900 5030 2070 ±100 EP-SD-52 3340 2340 3240 ±20 EP-SD-53 5370 4470 4810 ±40

EP-SD-54 2350 1500 1370 ±60

GM 3880 2340 1910

GSD 1.9 2.6 2.5

pH Sand Silt Clay EC (1:5) Code H2O (%) (%) (%) (µS/cm)

EP-SD-43 5.8 50 35 15 10.9 108 EP-SD-49 5.2 68 18 14 2.6 77 EP-SD-50 6.1 61 25 14 8.4 97 EP-SD-51 5.6 45 28 27 8.3 72 EP-SD-52 5.2 40 33 27 8.0 88

46

2.6-1 137Cs

2.6-2 Cs Tag: m2 kg-1

2.6-3

11.55 km2 ( : 6.26 km2, : 5.29 km2)

19.7 × 106 m3

26.4 km

1.7 m ( 2.5 m)

22

2.6-4

(cm) (g) 37 8.5-42.0 9-1238 6 45.0-72.0 1012-4777

3 32.5-36.5 584-894 2 14.0-14.5 56-62

2 54.0-55.0 1070-1738 1 40 526

A λa, d-1 Teff y B λb, d-1 Teff y 172 0.00482 0.39 28.5 0.000782 4.7

404 0.00675 0.28 14.9 0.000142 10.5 125 0.00675 0.63 8.3 0.000399 2.7

2016

144 0.00402 0.47 14.9 0.000142 13.4

N GM 95

2790 3.4E-3 4.0E-4 2.9E-2

630 5.5E-3 7.3E-4 4.1E-2

644 3.8E-3 5.6E-4 2.5E-2

47

2.6-5 137Cs

2.6-6 13C 15N

2s-1 2015 2016

*1 2017 *2 5

*1 *2 *2

2015 —

1/1 – 12/31

16.8 -0.6 – 36.8

16.7 (-2.8 – 38.8)

16.6 (0.8 – 28.7)

16.3 (-3.4 – 36.7)

15.4 (2.1 – 28.5)

2016 —

1/1 – 12/31

16.8 (-0.6 – 36.3)

16.6 (-2.4 – 40.0)

16.9 (6.3 – 27.0)

16.2 (-3.4 – 36.2)

15.4 (3.4 – 26.4)

48

2.2-1 Ni, Sr, Mo Pb

49

2.4-1

2.4-2 Fe, Co, Ni, Cu, Zn Sr

10-1

100

101

102

103

104

105

106

10-1 100 101 102 103 104 105 106

GM-ColdGM-Warm

Ele

men

tal c

once

ntra

tion,

mg/

kg

World Average, mg/kg

50

2.5-1 1 30 Cs 3 7 30 Kd pH

p<0.05

102

103

104

P43_1d-3dP43_1d-7dP43_1d-30dP43_30d-7d

Kd

1d-3d 1d-7d 1d-30d 30d-7d

5.0

5.5

6.0

6.5

7.0

P43_1d-3dP43_1d-7dP43_1d-30dP43_30d-7d

pH

1d-3d 1d-7d 1d-30d 30d-7d

102

103

104

P49_1d-3dP49_1d-7dP49_1d-30dP49_30d-7d

Kd

1d-3d 1d-7d 1d-30d 30d-7d

5.0

5.5

6.0

6.5

7.0

P49_1d-3dP49_1d-7dP49_1d-30dP49_30d-7d

pH

1d-3d 1d-7d 1d-30d 30d-7d

102

103

104

P50_1d-3dP50_1d-7dP50_1d-30dP50_30d-7d

Kd

1d-3d 1d-7d 1d-30d 30d-7d

5.0

5.5

6.0

6.5

7.0P50_1d-3dP50_1d-7dP50_1d-30dP50_30d-7d

pH

1d-3d 1d-7d 1d-30d 30d-7d

51

d d RI

2.5-1 1 30 Cs 3 7 30 Kd pHp<0.05

102

103

104

P51_1d-3dP51_1d-7dP51_1d-30dP51_30d-7d

Kd

1d-3d 1d-7d 1d-30d 30d-7d

102

103

104

P52_1d-3dP52_1d-7dP52_1d-30dP52_30d-7d

Kd

1d-3d 1d-7d 1d-30d 30d-7d

5.0

5.5

6.0

6.5

7.0P51_1d-3dP51_1d-7dP51_1d-30dP51_30d-7d

pH

1d-3d 1d-7d 1d-30d 30d-7d

5.0

5.5

6.0

6.5

7.0P52_1d-3dP52_1d-7dP52_1d-30dP52_30d-7d

pH

1d-3d 1d-7d 1d-30d 30d-7d

52

2.5-2 10 23 30˚C Kd-137Cs RI

2.5-3 10 23 30˚C Kd-137Cs

aab b

1500

2000

2500

3000

3500

4000

5 10 15 20 25 30 35

Kd-

Cs

Temperature, ˚C

53

2.6-1 137Cs

1

10

100

1000

0 500 1000 1500 2000

137 C

s co

ncen

tratio

n, B

q kg

-1-d

ry

Days after March 11, 2011

1

10

100

1000

0 500 1000 1500 2000

137 C

s co

ncen

tratio

n, B

q kg

-1-d

ry


1

10

100

1000

0 500 1000 1500 2000

137 C

s co

ncen

tratio

n, B

q kg

-1-d

ry


54

2.6-2 2012-2016 137Cs

Tag, m2 kg-1

55

2.6-3 2011 11 2016 9

2.6-4 1. 2 3 4 5 6

1

2

3

4

5

6

56

2.6-5 137Cs n % 137Cs

2.6-6

1) 20 mg 2 mL 2) 1.5 mL , 2 1 3) 4) 5,500 × g, 5 , 5) 6) 1.5 mL 7) 5,500 × g, 5 , 8) 9) 6 8 1-2 10) 50˚C 24 11) 12)

57

2.6-7 13C 15N

2.6-8

58

2015.1.1-12.31 2016.1.1-12.31

2015.1.1-12.31 2016.1.1-12.31

2s-1 2015 2016 Air Soil 20cm

2s-2 2015 2016

59

MOX

TRU14C 5730

TRU

JAEA and FEPC, 2007 14C

, 1999 14C

14C 14C

14C

Ishii et al., 2015 25 114C

- Kd -

TF 14C

14C

Ishii et al., 2015 14C 14C14C

14C

Frölicher et al., 2014

Castro et al., 2010; Schindlbacher et al., 201114C

pH14C

ATP14C

, 2015 14C14C-

95

, 201614C

61

14C

, 2016

14C 14C 14C 14C

14C

3.2 3.3

3.4

Castro, H. F., Classen, A. T., Austin, E. E., Norby, R. J., & Schadt, C. W. (2010). Soil microbial community

responses to multiple experimental climate change drivers. Appl Environ Microbiol, 76(4), 999-1007.

Frölicher, T. L., Winton, M., & Sarmiento, J. L. (2014). Continued global warming after CO2 emissions

stoppage. Nature Climate Change, 4, 40-44.

Ishii, N., Ogiyama, S., Sakurai, S., Tagami, K., & Uchida, S. (2015). Environmental transfer of carbon-14 in Japanese paddy fields. In K. Nakajima (Ed.), Nuclear Back-end and transmutation technology for waste

disposal (pp. 303-309). Tokyo: Springer.

Japan Atomic Energy Agency, & The Federation of Electric Power Companies of Japan. (2007). Second

Progress Report on Research and Development for TRU Waste Disposal in Japan Repository Design,

Safety Assessment and Means of Implementation in the Generic Phase . Ibaraki, Japan.

Schindlbacher, A., Rodler, A., Kuffner, M., Kitzler, B., Sessitsch, A., & Zechmeister-Boltenstern, S. (2011). Experimental warming effects on the microbial community of a temperate mountain forest soil. Soil Biol

Biochem, 43(7), 1417-1425.

. (1999). —

2 —.

. (2015). 26

. . . (2016). 27

. .

62

14C

TRU 14C

Kaneko et al.,

2003 14C2013 14C 14C

Ishii et al., 2015 14C

14C

2013

2016 14C 14C

14C [1,2-14C] 14C14C

3.2.1. 14CO214C

, 1990

TRU [1,2-14C] 14C14C 14C

3.2.1.1. 14C 14C

26

63

, 2015

3.2-1 0.5 g-dry < 2 mm 30 mL

5 mL [1,2-14C][1,2-14C] pH 14C 1.7 × 103 Bq/mL 4.2 × 103 Bq/mL

8.6 × 103 Bq/mL 1.7 × 104 Bq/mL 4.2 × 104 Bq/mL 8.4 × 104 Bq/mL 1 0.5 g

8.6 × 103 Bq 4.2 × 105 Bq 14C

0.2 µm

25 15 14CO2

20 mL/min 10 30 mL 14C

63

200 mL

16 g 1 mol/L 314CO2

14C Hionic-Fluor

PerkinElmer Tri-Carb-25WTR Liquid Scintilation Analyzer14C 0-156 KeV 3

dpm 14C 14CO2 3.2-2

4 14CO214CO2

Ishii et al., 2010 4 14CO214C 8.4 × 104 Bq/mL

[1,2-14C] 4.07 × 109 Bq/mmol Bq/mL mol/L

20.6 µmol/L 0.5 g 5 mL

1 kg 2.06 × 10-2 cmol/kg

, 1994 50 14CO2

14C 3.2-2 8.4 × 104 Bq/mL 14C

[1,2-14C] 1 2 5.8 × 104 Bq14C 14CO2 8.6 × 103 Bq/mL 14C [1,2-14C]

14C 4.2 × 104 Bq 14CO2

1 2

8.6 × 103 Bq/mL 14C [1,2-14C] 14CO2

[1,2-14C]14CO2

3.2-3

8.6 × 103 Bq/mL 14C [1,2-14C] 3 1514CO2

14C14CO2

14C [1,2-14C]8.6 × 103 Bq/mL 14C

1

3.2.1.2. 14C [1,2-14C] 3.2.1.1.

[1,2-14C] 14C 8.6 × 103 Bq/mL 15 20 25

30 4 14CO214C 3.2.1.1.

14CO2 3.2-4 4 14CO2

, 2016 4 14CO2

64

25

30

25 2514CO2

14CO2

3.2-5 14CO214C 3.2-4

25 30 4

25 30 14CO214C

14CO2

3.2.2. 14C [1,2-14C] 14C

14C

2 × 10-2 cmol/kg-soil 14CO2

[1,2-14C] 4.07 × 109 Bq/mmol14C 8.4 × 104 Bq/mL 14C

14C- 14C 14CO214CO2

14C

14CO2 25 30 2514CO2

Ishii, N., Koiso, H., Takeda, H., & Uchida, S. (2010). Partitioning of 14C into solid, liquid, and gas phases in

various paddy soils in Japan. Journal of Nuclear Science and Technology, 47(3), 238-243.

Ishii, N., Ogiyama, S., Sakurai, S., Tagami, K., & Uchida, S. (2015). Environmental transfer of carbon-14 in

Japanese paddy fields. In K. Nakajima (Ed.), Nuclear Back-end and transmutation technology for waste

disposal (pp. 303-309). Tokyo: Springer.

Kaneko, S., Tanabe, H., Sasoh, M., Takahashi, R., Shibano, T., & Tateyama, S. (2003). A study on the chemical forms and migration behavior of Carbon-14 leached from the simulated hull waste in the underground

condition. Materials Research Society Proceedings, 757, II3.8.1.

. (1994). . In (Ed.), 19

(pp. 91-118). : .

. (2013).

6 19 24 [ ]. . . (2015). 26

65

. .

. (2016). 27

. .

, , , & . (1990).

. , 61(6), 572-578.

66

14C Ishii et al., 2015

95

, 2016

14CO214CO2

3.3.1.

P2P11 P2

52% 31% 17%

84.7 g/kg 6.4 g/kg P11

36% 35% 29% 21.3 g/kg

2.2 g/kg P2 P11

, 2016

0.5 g-dry < 2 mm 50 mL

0.5 mL

15 20 25 30 7

3

DNA DNA ISOIL for Beads Beating

FastPrep 24 Instrument MP Biomedicals 6 m/sec 45

DNA 16S rRNA (PCR)

PCR 341f-GC 907R

3.3-1 PCR 50 µL 0.25 µL Takara Ex Taq polymerase

Hot Start Version (Takara Bio Inc) 0.5 µL 25 µM 341F-GC forward primer 0.5 µL 25 µM 907R reverse primer 1 µL 0.1% Bovine Serum Albumin (Takara Bio Inc.) 4 µL dNTP Mixture ( 2.5 mM)

5 µL 10 × Ex Taq Buffer 1 µL DNA 50 µL PCR

TProfessional 96 Gradient Thermocycler (Biometra GmbH) touch-down PCR

1) 95 , 60 sec, 2) 94 , 30 sec, 3) 65 , 30 sec, 4) 72 , 60 sec, 5) 94 , 30 sec,

6) 55 , 30 sec, 7) 72 , 60 sec, 8) 72 , 600 sec. 3), 4), 5) 20

3) 0.5 5) 5) 7) 98) PCR PCR QIAquick PCR Purification

67

Kit (QIAGEN) 2100 Bioanalyzer (Agilent) DNA Bp

(ng/µL)

DNA DGGE DGGE

D-code system (Bio-Rad Laboratories, Inc.) 120 ng DNA DGGE

61.5 50V 20 TAE buffer DGGE5.5% (w/v) 45% 60%

100% 7 M + 40% SYBR Gold

Nucleic Acid Gel Stain (ThermoFisher Scientific Inc.) Molecular Imager FX (Bio-Rad

Laboratories, Inc.)

P2 3.3-1

15

15

3.3-1

1 100% 15

P11 3.3-2 P2

P11

3.3.2.

14CO214CO2

P21 P33

P21 [1,2-14C] 7

75% 14C P33 47%, 2015 P21

47% 32% 21% 20.2 g/kg 2.2 g/kg

P33 50%

27% 22% 36.2 g/kg 4.2 g/kg

, 2016

3.3.1. DNA 0.5 g0.5 mL 7 ISOIL for Beads Beating

DNA 30 DNA QIAquick PCR Purification

Kit (QIAGEN) DGGE DGGE

200 ng DNA 62 50V 20

DGGE 6% (w/v)

40% 55% 3.3-3 P21 P33 P21

68

14C P33 , 2015P21 P33 14CO2

, 2006341f-GC/907R

PARCH 340f-GC PARCH 519R 3.3-1 PCR

3.3.3. 14CO2 16S rRNA

DGGE

3.3-3 5 CS0814C CS08

DGGE 40 µL 10mM Tris-Cl (pH8.5)

DNA TOPO TA Cloning Kits for Sequencing kit (ThermoFisher Scientific Inc.)

5 3

Ribosomal Database Project Release 11

3.3-2

MEGA: Molecular Evolutionary

Genetics Analysis Tamura et al. 2007

3.3-4 DNA

Clostridium carboxidivorans, Massilia aerilata, Bacillus niacini, Tumebacillus ginsengisoli, Ramlibacter solisilvae C. carboxidivorans

(Liou et al. 2005) 4M. aerilata Weon et al., 2008 B.

niacini (Nagel and

Andereesen, 1991) T. ginsengisoli (Baek et al, 2011) R. solisilvaeBiolog GN plate (Heulin et al, 2003)

3.3. 4. 14CO2

14CO2

15 30

14CO2

69

14C4

16S rRNA 4 31

14C14C

Baek, S.H., Cui, Y., Kim, S.C., Cui, C.H., Yin, C., Lee, S.T., Im, W.T., 2011. Tumebacillus ginsengisoli sp.

nov., isolated from soil of a ginseng field. International journal of systematic and evolutionary microbiology 61, 1715-1719.

Heulin, T., Barakat, M., Christen, R., Lesourd, M., Sutra, L., De Luca, G., Achouak, W., 2003. Ramlibacter

tataouinensis gen. nov., sp. nov., and Ramlibacter henchirensis sp. nov., cyst-producing bacteria isolated from

subdesert soil in Tunisia. International journal of systematic and evolutionary microbiology 53, 589-594.

Ishii, N., Ogiyama, S., Sakurai, S., Tagami, K., Uchida, S., 2015. Environmental transfer of carbon-14 in

Japanese paddy fields, in: Nakajima, K. (Ed.), Nuclear Back-end and transmutation technology for waste disposal. Springer, Tokyo, pp. 303-309.

Liou, J.S., Balkwill, D.L., Drake, G.R., Tanner, R.S., 2005. Clostridium carboxidivorans sp. nov., a

solvent-producing clostridium isolated from an agricultural settling lagoon, and reclassification of the

acetogen Clostridium scatologenes strain SL1 as Clostridium drakei sp. nov. International journal of

systematic and evolutionary microbiology 55, 2085-2091.

Muyzer, G., Brinkhoff, T., Nübel, U., Santegoeds, C., Schäfer, H., Wawer, C., 2004. Denaturing gradient gel electrophoresis (DGGE) in microbial ecology, in: Kowalchuk, G.A., de Bruijn, F., Head, I.M., Van der Zijpp,

A.J., van Elsas, J.D. (Eds.), Molecular Microbial Ecology Manual. Springer Netherlands, Netherlands.

Muyzer, G., de Waal, E., Uitterlinden, A., 1993. Profiling of complex microbial populations by denaturing

gradient gel electrophoresis analysis of polymerase chain reaction-amplified genes coding for 16S rRNA.

Applied and environmental microbiology 59, 695-700.

Nagel, M., Andreesen, J.R., 1991. Bacillus niacini sp. nov. a Nicotinate-Metabolizing Mesophile Isolated from Soil. International journal of systematic and evolutionary microbiology 41, 134-139.

Ovreås, L., Forney, L., Daae, F.L., Torsvik, V., 1997. Distribution of bacterioplankton in meromictic Lake

Saelenvannet, as determined by denaturing gradient gel electrophoresis of PCR-amplified gene fragments

coding for 16S rRNA. Applied and environmental microbiology 63, 3367-3373.

Tamura, K., Dudley, J., Nei, M., Kumar, S., 2007. MEGA4: Molecular Evolutionary Genetics Analysis

(MEGA) software version 4.0. Molecular biology and evolution 24, 1596-1599. Weon, H.Y., Kim, B.Y., Son, J.A., Jang, H.B., Hong, S.K., Go, S.J., Kwon, S.W., 2008. Massilia aerilata sp.

nov., isolated from an air sample. International journal of systematic and evolutionary microbiology 58,

1422-1425.

, , 2006. .

5, 81-89.

, 2015. 26 , .

70

, 2016. 27

, .

71

14C 14C

3.4-1 TRU14C

14C14C Ishii et al., 2015

14C

3.4.1.

3

3.4.1.1.

• • 3.4-1

72

• PREP (Homma and Saltelli, 1992)

• 100

• day

•

PREP

3.4-2

3.4.1.2.

14C

3.4-3 14C 3.4-414C 14C

1

3.4-5 14C 14C

1

2

14C

3.4-6 1 14C 3.4-7 14C14C 1 1

14C 2

3.4-8 14C 12

14C

14C 14C 114C

3.4.1.3. 14C

SPOP (Saltelli and Homma, 1992)

PCC Partial Correlation Coefficient

PRCC Partial Rank Correlation Coefficient PCC

squrious correlation

x,y,z x,y Rxy,x z Rxz y z

73

Ryz z Rxy.z 1 R 1

1

(3.4-1)

PRCC

PRCC 1 R 1 1

(3.4-2)

3.4-2 PCC PRCC

6

1

4 14C 3.4-9

2 1

14C14C

3.4.2.

Migration Of GRound Additions (MOGRA)

Amano, 2003 14C 3.4-1

3.4.2.1.

50 m × 20 m DS 2, Decagon Devices, Inc. 3.4-10

3 21 cm

18 cm 108 cm 94 cm

3.4-3

10 6 24

1 2018 6 15 9 7 8

74

1 6 15

3.4-11

3.4-4 3.4-5

0˚ 315˚ 0˚45˚ 135˚ 225˚

45˚ 135˚ 225˚ 315˚

1/2

0.7 m/s

0.92 0.30 m/s0.28 m/s (=0.92 × 0.30)

2 7 12

3.4-12

3.4-6 3.4-7

1 m/s

1

0.4 m/s

1 m/s

0.64 0.36

0.00

0.26 m/s

0.09 m/s (=0.36 × 0.26)

3 7 20 3.4-13

3.4-8 3.4-9

1/2

2 1 m/s

6:40 8:40

75

6:40 15 0.3 m/s

0.5 m/s 1/2

0.29 0.62 0.08

0.19 m/s 0.12 m/s (=0.62 ×

0.19)

4 7 28

3.4-14

3.4-10 3.4-11

1/3

19 27 5.89 m/s 21 33 5.85 m/s

0.58 0.41 0.02

0.20 m/s

0.08 m/s (=0.41 × 0.20)

4

5 8 4

3.4-15 1

3.4-12 3.4-13

1/3 1/2

6 8 23

3.4-16 1

3.4-14 3.4-15

0.1 0.4 m/s0.24

76

0.46 0.38

70cm 97cm 59cm

7 8 31

3.4-17 1

3.4-16 3.4-17

0.1 0.4m/s

0.20 0.40 0.42 6

70cm 92cm 74cm

8 9 6

3.4-18

3.4-18 3.4-19 6 7 0.1 0.4m/s

0.19 0.36 0.43

3.4.2.2. CO2 CO2 CO2

CO2 3.4-19 8 4 23

24 9 1 4

3.4-20 CO2

CO2

1.5 CO2

CO2

CO2

CO2 CO2

3.4.3.

77

3.4.3.1.

0.08 m/s 0.28 m/s

0.05 m/s 0.25 m/s

10 m 50 m

30 m 100 m 0.05 m/s 0.25 m/s

(10 m / 2) / 0.25 m/s 20 sec ( 2×10-4 day) (100 m / 2) / 0.05 m/s 1000 sec 0.28 hr ( 0.01 day)

0.01 day 1

day 0.1 day3 i) iii) 0.01 0.1 1 day

i)

ii)

iii)

3 i) 0.1 0.3 0.5 day ii) 0.5 2 4 dayiii) 4 20 40 day

78

3.4.3.2.

0.1 day 14C

3.4-21 271

14C 1 1

11

3.4-22 14C

14C 2 14C 114C

14C

14C

20 day 0.1day 1

3.4-23 0.01 day) 3.4-24 1 day)14C

3.4-25 14C

3.4-26 14C

14C 14C 14C

3.4-27 14C 3.4-2814C

2 2

- 14C

3.4.3.3.

79

3

50

0.01 4 day

0.5 2 day

1 1.9 24 day

3.4-29 3 50

3.4-30 3 14C

14C

3.4.1. 14C

3.4.1.3.4-31 2

3.4.3.4. 14C TF

TF

TF= 14C (Bq/g) 14C

(Bq/g) TF TF

1 14C 3.4-32 1 14C

14C 90 day 120 day14C 14C 14C

3.4-20

day 90 14C 4.63 × 10-5 Bq/g 5.35 × 10-5 Bq/g day 12014C 1.14 × 10-4 Bq/g 1.17 × 10-4 Bq/g day 150

14C 1.39 × 10-5 Bq/g 1.37 × 10-4 Bq/g

TF 0.12 2.56 14C

3.4-20 TF14C

14C -

TF - IAEA grain TF 0.1 IAEA, 2003 13C

80

TF 0.05 2.2 14C TF

, 2009 TF14C TF

3.4.4.

12

0.01 day 1 day

20 day

14C

3

TF0.05-2.2 , 2009

TF

Amano, H., Takahashi, T., Uchida, S., Matsuoka, S., Ikeda, H., Hayashi, H., Kurosawa, N., 2003. Development

of a code MOGRA for predicting the migration of ground additions and its application to various land

utilization areas. Journal of Nuclear Science and Technology 40, 975-979.

Homma, T., Saltelli, A., 1992. LISA package user guide, Part 1: PREP (Statistical PRE Processor) preparation of input sample for Monte Carlo simulations program description and user guide, 33 pp.

IAEA, 2003. Derivation of activity limits for the disposal of radioactive waste in near surface disposal facilities,

IAEA-TECDOC-1380, 145 pp.

Ishii, N., Ogiyama, S., Sakurai, S., Tagami, K., Uchida, S., 2015. Environmental transfer of carbon-14 in

Japanese paddy fields, in: Nakajima, K. (Ed.), Nuclear Back-end and transmutation technology for waste

disposal. Springer, Tokyo, pp. 303-309. Saltelli, A., Homma, T., 1992. LISA : Package user guide - Part III : SPOP (Statistical POst Processor) :

81

Uncertainty and sensitivity analysis for model output : Program description and user guide, 51 pp.

, , , 2009.

. Radioisotopes 58, 641-648.

82

14C14C 14C

14C14C

14C14C

14C 14C TRU

[1,2-14C] 0.5 g4.2 × 105 Bq 14C 14C

14C 4.2 × 103

Bq/mL 14C 14C14C

14C 25 3014C 14C

14C

77

14CO2

14C

4 3

14C

1

14C

14C

83

3.3-1

3.3-2

341F Bacteria 5′-CCTACGGGAGGCAGCAG Muyzer et al, 1993907R Bacteria 5′-CCGTCAATTCCTTT(A/G)AGTTT Muyzer et al, 2004PARCH340f Archae 5′-GCCTACGGGG(C/T)GCA(C/G)CAG Øvreås et al, 1997PARCH519r Archae 5′-TTACCGCGGC(T/G)GCTG Øvreås et al, 1997GC clamp 1 5′-CGCCCGCCGCGCCCCGCGCCCGTCCCGCCGCCCCCGCCCG Muyzer et al, 2004GC clamp 2 5′-CGCCCGCCGCGCGCGGCGGGCGGGGCGGGGGCACGGGGG Øvreås et al, 1997GC clamp 1 341F 5′GC clamp 2 PARCH340f 5′

Band ID Sequeice

CS07

CS08

CS09

CS10

CS11

85

3.4-1

3.4-2 14C

3.4-3

0-79day 0.3 0.1-0.5 day80-90day120-150day

2 0.5-4 day

91-119day 20 4-40 day2 0.5-2 day25 4-25 day

2.5 1.9-24 day

67 27-114 day

1 25 4-25 day6.1 1.9-24 day6.1 1.9-24 day

2 1.5 1.5-10 day2 0.5-2 day

10000 day1 10000 day

0.1 day730 730-2810 day73 73-168 day

PCC PRCC(R2) (R2)

( ) -0.06 10 0.04 11( ) -0.2 7 -0.02 12

) 0.87 1 0.92 10.02 12 -0.05 90.21 6 0.22 6-0.75 2 -0.75 2-0.12 8 -0.16 7

1 0.57 4 0.64 40.27 5 0.28 50.03 11 0.05 10

2 -0.62 3 -0.64 3-0.11 9 -0.08 8

PCCPRCC

cm)

1 2016.6.15 23 21 79 108 18 42 942 2016.7.12 67 21 50 108 18 42 943 2016.7.20 75 21 64 108 18 57 944 2016.7.28 83 21 64 108 18 73 945 2016.8.4 94 21 70 1086 2016.8.23 97 59 21 70 1087 2016.8.31 92 74 21 70 1088 2016.9.6 94 69 21 70 108

86

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0.06

0.13

0.16

0.09

0.16

0.33

0.03

3:30

4:29

0.40

0.50

0.30

0.11

0.24

0.05

0.39

0.79

0.11

0.07

0.10

0.04

0.13

0.17

0.09

0.25

0.58

0.03

4:30

5:29

0.48

0.50

0.46

0.11

0.16

0.07

0.15

0.61

0.00

0.08

0.13

0.02

0.12

0.16

0.10

0.11

0.41

0.01

5:30

6:29

0.50

0.53

0.46

0.10

0.16

0.05

0.26

0.50

0.02

0.10

0.12

0.07

0.14

0.19

0.10

0.17

0.40

0.01

6:30

7:29

0.49

0.53

0.45

0.17

0.36

0.05

0.46

1.02

0.04

0.08

0.15

0.02

0.16

0.23

0.11

0.20

0.58

0.01

7:30

8:29

0.48

0.54

0.37

0.14

0.31

0.04

0.63

1.23

0.21

0.18

0.36

0.04

0.17

0.24

0.10

0.34

0.84

0.08

8:30

9:29

0.18

0.40

0.11

0.10

0.27

0.02

0.54

1.14

0.07

0.26

0.35

0.12

0.10

0.22

0.02

0.27

0.78

0.01

9:30

10:2

90.

140.

190.

080.

080.

220.

010.

420.

770.

100.

340.

410.

290.

050.

160.

010.

290.

840.

0610

:30

11:2

90.

150.

210.

090.

060.

180.

010.

471.

210.

120.

370.

400.

340.

050.

090.

010.

250.

760.

0311

:30

12:2

90.

140.

200.

070.

060.

170.

000.

400.

770.

150.

350.

390.

280.

040.

100.

010.

220.

580.

0312

:30

13:2

90.

160.

230.

120.

080.

240.

020.

390.

810.

040.

280.

340.

240.

040.

090.

000.

170.

460.

0113

:30

14:2

90.

140.

200.

050.

080.

280.

010.

631.

370.

230.

280.

330.

230.

050.

130.

010.

411.

190.

0214

:30

15:0

00.

140.

210.

060.

080.

290.

010.

521.

150.

180.

300.

360.

260.

040.

100.

000.

261.

010.

02

-1.

0.E-

012.

9.E-

021.

7.E-

026.

4.E-

012.

0.E-

021.

1.E-

01-

2.1.

E-01

1.5.

E-01

1.4.

E-01

7.1.

E-04

2.9.

E-01

3.4.

E-02

-3.

7.E-

012.

5.E-

013.

9.E-

013.

6.E-

016.

9.E-

018.

6.E-

01-

3.1.

E-01

2.5.

E-01

3.2.

E-01

-5.

4.E-

031.

7.E-

018.

2.E-

02-

0.0.

E+00

7.4.

E-02

2.5.

E-02

-6.

8.E-

044.

6.E-

021.

2.E-

02-

0.0.

E+00

2.6.

E-02

3.4.

E-03

88

3.4-

8

3.4-

9

m/s

m/s

star

ten

d14

:40

15:3

90.

190.

380.

080.

480.

910.

181.

201.

860.

520.

090.

190.

030.

200.

450.

020.

661.

650.

0715

:40

16:3

90.

180.

310.

050.

470.

830.

111.

152.

240.

530.

090.

210.

000.

180.

410.

060.

601.

430.

1116

:40

17:3

90.

170.

260.

090.

390.

910.

090.

991.

580.

460.

080.

160.

040.

150.

360.

040.

531.

610.

0717

:40

18:3

90.

140.

340.

040.

350.

860.

071.

011.

940.

350.

080.

170.

030.

160.

550.

040.

782.

040.

2118

:40

19:3

90.

140.

320.

010.

370.

980.

060.

941.

560.

390.

060.

160.

000.

150.

320.

040.

751.

500.

2119

:40

20:3

90.

210.

360.

070.

350.

940.

010.

931.

690.

230.

050.

150.

000.

150.

330.

050.

842.

030.

1020

:40

21:3

90.

280.

380.

150.

210.

600.

010.

671.

280.

230.

030.

090.

000.

100.

260.

010.

501.

670.

0321

:40

22:3

90.

290.

400.

160.

260.

710.

020.

871.

610.

280.

040.

100.

000.

130.

340.

030.

671.

330.

0222

:40

23:3

90.

290.

430.

160.

260.

560.

080.

981.

780.

410.

040.

100.

000.

140.

380.

040.

711.

480.

0723

:40

0:39

0.27

0.47

0.15

0.27

1.00

0.06

0.96

1.69

0.38

0.05

0.15

0.00

0.14

0.33

0.03

0.69

1.63

0.11

0:40

1:39

0.27

0.43

0.15

0.31

0.67

0.04

1.15

2.30

0.42

0.05

0.17

0.00

0.16

0.40

0.05

0.83

1.53

0.23

1:40

2:39

0.25

0.39

0.09

0.34

0.77

0.07

1.16

2.14

0.46

0.06

0.27

0.01

0.17

0.36

0.04

0.86

1.57

0.14

2:40

3:39

0.22

0.34

0.13

0.29

0.66

0.08

1.11

1.96

0.41

0.06

0.13

0.01

0.16

0.39

0.05

0.76

1.88

0.17

3:40

4:39

0.18

0.28

0.09

0.27

0.69

0.02

0.91

1.58

0.43

0.04

0.13

0.00

0.13

0.30

0.03

0.52

1.00

0.08

4:40

5:39

0.11

0.19

0.03

0.18

0.45

0.01

0.66

1.37

0.13

0.06

0.13

0.00

0.11

0.23

0.05

0.32

0.98

0.00

5:40

6:39

0.13

0.21

0.07

0.22

0.54

0.01

0.58

1.08

0.04

0.08

0.14

0.05

0.42

2.51

0.09

0.23

1.09

0.06

6:40

7:39

0.13

0.24

0.06

0.21

0.46

0.01

0.62

1.19

0.21

0.06

0.13

0.01

5.74

7.82

2.53

1.80

2.49

0.34

7:40

8:39

0.14

0.28

0.03

0.24

0.54

0.02

0.77

1.52

0.20

0.05

0.11

0.01

7.38

7.86

6.01

2.12

2.43

1.42

8:40

9:39

0.16

0.28

0.07

0.23

0.69

0.02

0.83

1.39

0.30

0.04

0.11

0.00

2.86

3.14

2.07

9:40

10:3

90.

190.

300.

080.

270.

650.

040.

991.

830.

450.

040.

120.

002.

833.

292.

5710

:40

11:3

90.

220.

330.

080.

230.

910.

020.

911.

650.

330.

040.

110.

012.

443.

311.

1211

:40

12:3

90.

160.

320.

050.

280.

670.

060.

921.

930.

250.

070.

150.

014.

406.

712.

8412

:40

13:3

90.

140.

270.

060.

190.

500.

010.

741.

460.

210.

110.

210.

058.

439.

556.

6113

:40

14:3

90.

130.

230.

040.

220.

520.

090.

791.

240.

450.

120.

220.

0410

.15

11.8

67.

7614

:40

14:4

90.

140.

220.

090.

200.

460.

020.

771.

370.

29

-2.

8.E-

032.

5.E-

011.

6.E-

012.

9.E-

012.

9.E-

023.

3.E-

01-

7.4.

E-02

2.7.

E-01

5.2.

E-01

8.4.

E-02

2.3.

E-01

3.0.

E-02

-5.

9.E-

012.

7.E-

012.

4.E-

016.

2.E-

017.

4.E-

016.

4.E-

01-

3.1.

E-01

1.3.

E-01

7.1.

E-02

-1.

9.E-

026.

2.E-

036.

9.E-

04-

0.0.

E+00

4.1.

E-03

0.0.

E+00

-7.

0.E-

046.

9.E-

030.

0.E+

00-

0.0.

E+00

6.6.

E-02

4.8.

E-03

89

3.4-

10

3.4-

11

m/s

m/s

star

ten

d14

:30

15:2

90.

150.

260.

060.

100.

260.

010.

551.

320.

030.

050.

160.

010.

210.

510.

050.

471.

340.

0215

:30

16:2

90.

150.

300.

060.

140.

440.

010.

841.

470.

470.

070.

170.

010.

360.

720.

140.

671.

570.

2416

:30

17:2

90.

140.

220.

070.

110.

310.

010.

591.

230.

110.

050.

120.

010.

230.

610.

060.

361.

200.

0417

:30

18:2

90.

180.

340.

110.

080.

220.

020.

381.

050.

030.

030.

100.

000.

090.

230.

010.

160.

630.

0218

:30

19:2

90.

280.

370.

190.

120.

320.

010.

290.

660.

030.

050.

120.

000.

885.

890.

040.

160.

420.

0219

:30

20:2

90.

220.

270.

170.

060.

140.

010.

280.

510.

010.

040.

110.

000.

193.

830.

010.

120.

290.

0420

:30

21:2

90.

140.

220.

100.

050.

130.

010.

220.

560.

020.

040.

060.

020.

090.

180.

010.

130.

370.

0321

:30

22:2

90.

130.

160.

110.

030.

060.

010.

140.

330.

040.

030.

060.

010.

435.

850.

060.

140.

360.

0622

:30

23:2

90.

120.

150.

110.

030.

070.

000.

100.

220.

030.

050.

090.

010.

130.

160.

080.

120.

170.

0723

:30

0:29

0.15

0.18

0.13

0.08

0.13

0.05

0.16

0.35

0.01

0.08

0.10

0.03

0.16

0.30

0.09

0.15

0.27

0.08

0:30

1:29

0.15

0.17

0.11

0.06

0.12

0.01

0.23

0.47

0.05

0.09

0.11

0.07

0.19

0.27

0.13

0.21

0.40

0.11

1:30

2:29

0.15

0.18

0.11

0.07

0.11

0.04

0.14

0.37

0.01

0.09

0.11

0.05

0.17

0.25

0.12

0.19

0.28

0.12

2:30

3:29

0.15

0.18

0.12

0.07

0.11

0.04

0.12

0.35

0.02

0.08

0.09

0.06

0.16

0.21

0.14

0.15

0.24

0.10

3:30

4:29

0.16

0.18

0.12

0.07

0.11

0.02

0.19

0.51

0.05

0.07

0.10

0.05

0.18

0.36

0.13

0.21

0.53

0.10

4:30

5:29

0.18

0.32

0.14

0.08

0.15

0.02

0.21

0.44

0.02

0.09

0.11

0.07

0.22

0.41

0.16

0.20

0.38

0.08

5:30

6:29

0.36

0.45

0.28

0.12

0.25

0.03

0.40

0.77

0.19

0.08

0.11

0.04

0.24

0.44

0.13

0.32

0.59

0.09

6:30

7:29

0.44

0.53

0.36

0.13

0.43

0.02

0.48

0.92

0.19

0.10

0.16

0.06

0.18

0.42

0.00

0.25

0.71

0.04

7:30

8:29

0.39

0.50

0.31

0.13

0.29

0.02

0.45

0.90

0.04

0.10

0.16

0.04

0.17

0.44

0.03

0.25

0.70

0.01

8:30

9:29

0.25

0.48

0.06

0.14

0.38

0.01

0.38

0.86

0.11

0.05

0.12

0.00

0.15

0.44

0.01

0.35

0.85

0.05

9:30

10:2

90.

160.

260.

090.

120.

200.

040.

360.

800.

020.

040.

100.

010.

130.

310.

030.

340.

990.

0710

:30

11:2

90.

190.

310.

120.

130.

380.

030.

480.

900.

050.

070.

130.

020.

140.

290.

020.

280.

760.

0411

:30

12:2

90.

180.

320.

050.

180.

390.

030.

771.

500.

270.

080.

160.

030.

200.

700.

030.

290.

720.

0512

:30

13:2

90.

180.

320.

080.

250.

600.

041.

111.

660.

500.

110.

200.

050.

310.

680.

050.

602.

230.

1113

:30

14:2

90.

180.

340.

050.

260.

630.

051.

101.

720.

350.

100.

190.

020.

421.

240.

130.

641.

390.

0914

:30

15:0

00.

150.

300.

040.

130.

340.

000.

831.

450.

400.

090.

140.

050.

330.

770.

110.

531.

030.

05

-6.

2.E-

037.

0.E-

024.

3.E-

025.

8.E-

013.

8.E-

013.

8.E-

01-

1.4.

E-01

1.7.

E-01

9.5.

E-02

1.6.

E-02

1.6.

E-01

1.7.

E-02

-4.

9.E-

011.

8.E-

012.

7.E-

014.

1.E-

014.

5.E-

016.

0.E-

01-

3.5.

E-01

1.7.

E-01

3.4.

E-01

-6.

2.E-

031.

6.E-

011.

2.E-

01-

0.0.

E+00

1.1.

E-01

4.0.

E-02

-0.

0.E+

009.

9.E-

025.

1.E-

02-

0.0.

E+00

3.3.

E-02

4.4.

E-02

90

3.4-12

3.4-13

m/s

start end14:30 15:29 0.22 0.33 0.16 0.07 0.21 0.01 0.25 0.65 0.0415:30 16:29 0.19 0.28 0.13 0.12 0.34 0.01 0.56 1.08 0.2116:30 17:29 0.22 0.34 0.09 0.13 0.31 0.02 0.77 1.41 0.3317:30 18:29 0.24 0.33 0.16 0.10 0.27 0.00 0.53 0.95 0.1518:30 19:29 0.27 0.31 0.24 0.09 0.20 0.01 0.33 0.59 0.0519:30 20:29 0.25 0.29 0.21 0.09 0.21 0.01 0.33 0.69 0.1320:30 21:29 0.24 0.29 0.21 0.09 0.19 0.04 0.31 0.49 0.1721:30 22:29 0.22 0.25 0.19 0.11 0.21 0.04 0.32 0.66 0.0322:30 23:29 0.23 0.26 0.19 0.10 0.17 0.07 0.23 0.47 0.0623:30 0:29 0.21 0.26 0.17 0.10 0.18 0.05 0.21 0.58 0.050:30 1:29 0.22 0.25 0.17 0.11 0.16 0.09 0.19 0.42 0.051:30 2:29 0.18 0.21 0.15 0.10 0.13 0.07 0.11 0.21 0.022:30 3:29 0.17 0.19 0.14 0.11 0.16 0.08 0.15 0.34 0.013:30 4:29 0.15 0.18 0.11 0.12 0.22 0.09 0.25 0.46 0.064:30 5:29 0.15 0.18 0.13 0.09 0.14 0.05 0.16 0.39 0.035:30 6:29 0.22 0.29 0.17 0.09 0.16 0.04 0.17 0.67 0.026:30 7:29 0.28 0.35 0.22 0.09 0.24 0.01 0.56 1.06 0.227:30 8:29 0.27 0.39 0.17 0.12 0.25 0.03 0.60 1.22 0.188:30 9:29 0.14 0.26 0.06 0.11 0.33 0.01 0.46 0.95 0.169:30 10:29 0.16 0.29 0.09 0.10 0.27 0.03 0.33 0.66 0.0610:30 11:29 0.23 0.35 0.15 0.10 0.25 0.01 0.41 0.96 0.1511:30 12:29 0.26 0.39 0.18 0.10 0.26 0.01 0.47 1.07 0.0612:30 13:29 0.20 0.31 0.09 0.10 0.27 0.00 0.55 1.09 0.1413:30 14:29 0.16 0.27 0.07 0.08 0.26 0.01 0.53 1.08 0.1314:30 15:00 0.14 0.26 0.05 0.08 0.20 0.01 0.49 0.96 0.20

- 6 48 46- 174 442 58

- 1141 209 220- 131 254 525

- 0 176 331- 0 150 144

- 0 139 94- 0 31 35

91

3.4-14

3.4-15

m/s

start end14:49 15:48 0.27 0.43 0.16 0.72 1.24 0.27 0.98 1.57 0.4315:49 16:48 0.29 0.41 0.17 0.60 1.22 0.23 0.90 1.77 0.3116:49 17:48 0.41 0.55 0.28 0.53 1.29 0.19 0.83 1.59 0.3817:49 18:48 0.34 0.44 0.29 0.21 0.64 0.02 0.34 0.96 0.0518:49 19:48 0.35 0.45 0.31 0.20 0.48 0.03 0.38 1.16 0.0519:49 20:48 0.35 0.44 0.30 0.25 0.56 0.03 0.55 0.90 0.1320:49 21:48 0.32 0.38 0.25 0.27 0.50 0.05 0.65 1.11 0.2321:49 22:48 0.31 0.49 0.11 0.51 0.96 0.01 1.21 2.16 0.4822:49 23:48 0.19 0.31 0.11 0.27 0.69 0.04 0.75 1.40 0.2423:49 0:48 0.17 0.26 0.13 0.15 0.35 0.03 0.38 0.96 0.070:49 1:48 0.17 0.21 0.12 0.14 0.58 0.01 0.31 1.23 0.031:49 2:48 0.20 0.35 0.15 0.20 0.58 0.03 0.47 1.19 0.112:49 3:48 0.18 0.26 0.10 0.24 0.48 0.08 0.62 1.31 0.213:49 4:48 0.25 0.39 0.08 0.45 1.02 0.09 0.69 1.47 0.224:49 5:48 0.23 0.34 0.17 0.35 0.68 0.05 0.47 1.21 0.025:49 6:48 0.21 0.29 0.16 0.23 0.58 0.01 0.37 0.74 0.056:49 7:48 0.29 0.46 0.17 0.32 0.80 0.06 0.71 1.53 0.067:49 8:48 0.23 0.36 0.12 0.25 0.53 0.04 0.51 0.94 0.068:49 9:48 0.30 0.48 0.19 0.48 0.94 0.10 0.84 1.61 0.359:49 10:48 0.31 0.45 0.19 0.65 1.04 0.32 1.21 1.82 0.7410:49 11:48 0.31 0.51 0.16 0.50 1.10 0.11 0.92 1.75 0.2411:49 12:48 0.31 0.59 0.05 0.44 1.55 0.05 0.74 2.24 0.2212:49 13:48 0.35 0.47 0.2813:49 14:52 0.37 0.53 0.25

- 0 166 223- 135 176 273

- 1178 231 223- 127 236 249

- 0 210 178- 0 90 60

- 0 54 20- 0 100 36

92

3.4-16 7

3.4-17

m/s

start end14:23 15:22 0.28 0.56 0.06 1.23 2.81 0.50 1.93 3.50 0.8915:23 16:22 0.32 0.66 0.11 1.45 2.47 0.73 2.10 3.54 1.0216:23 17:22 0.37 0.62 0.14 1.02 2.12 0.46 1.48 3.08 0.5417:23 18:22 0.32 0.62 0.09 1.11 1.79 0.26 1.54 2.34 0.7418:23 19:22 0.19 0.33 0.09 0.98 1.49 0.55 1.15 1.91 0.5719:23 20:22 0.17 0.26 0.09 0.62 1.55 0.20 1.00 1.85 0.6220:23 21:22 0.18 0.22 0.14 0.41 0.70 0.18 0.95 1.47 0.6021:23 22:22 0.21 0.27 0.16 0.50 0.84 0.29 1.07 1.51 0.7222:23 23:22 0.22 0.28 0.16 0.45 0.83 0.24 1.03 1.62 0.7523:23 0:22 0.23 0.30 0.14 0.66 1.39 0.26 1.19 1.72 0.720:23 1:22 0.25 0.40 0.10 0.62 1.22 0.24 0.95 1.69 0.491:23 2:22 0.23 0.33 0.15 0.54 0.96 0.22 0.89 1.37 0.432:23 3:22 0.22 0.33 0.17 0.57 0.93 0.23 0.88 1.46 0.483:23 4:22 0.22 0.27 0.17 0.42 0.82 0.15 0.66 1.29 0.094:23 5:22 0.22 0.29 0.15 0.51 0.83 0.20 0.77 1.42 0.205:23 6:22 0.20 0.24 0.15 0.33 0.46 0.19 0.34 0.88 0.036:23 7:22 0.24 0.37 0.17 0.55 0.85 0.28 0.58 1.11 0.097:23 8:22 0.28 0.43 0.18 0.60 1.01 0.26 0.80 1.82 0.348:23 9:22 0.35 0.48 0.19 0.67 1.30 0.38 0.85 1.82 0.319:23 10:22 0.26 0.42 0.15 0.71 1.55 0.37 0.80 1.50 0.2710:23 11:22 0.28 0.50 0.11 0.65 1.21 0.25 0.87 2.19 0.3911:23 12:22 0.25 0.41 0.15 0.62 1.07 0.36 0.83 2.00 0.3912:23 13:22 0.23 0.36 0.12 0.55 1.00 0.23 0.70 1.35 0.0513:23 14:22 0.22 0.32 0.15 0.45 0.76 0.20 0.49 1.27 0.0314:23 14:56 0.25 0.37 0.17 0.55 0.96 0.25 0.58 1.22 0.21

- 1 0 10- 6 0 4

- 1269 0 3- 190 20 183

- 3 780 708- 0 397 262

- 0 237 163- 0 29 109

93

3.5-18

3.4-19

m/s

start end14:04 15:03 0.27 0.42 0.16 1.16 2.17 0.72 1.30 2.48 0.6415:04 16:03 0.26 0.42 0.04 1.54 2.42 0.55 2.02 3.34 0.7816:04 17:03 0.27 0.47 0.06 1.19 1.89 0.70 1.49 2.57 0.5117:04 18:03 0.28 0.50 0.12 1.01 1.67 0.48 1.19 3.09 0.4718:04 19:03 0.43 0.65 0.31 1.02 1.74 0.48 1.28 2.41 0.2619:04 20:03 0.40 0.52 0.21 0.84 1.45 0.49 0.89 1.69 0.4120:04 21:03 0.33 0.48 0.21 0.86 1.25 0.44 1.02 1.78 0.3621:04 22:03 0.31 0.44 0.18 0.89 1.49 0.41 1.28 2.09 0.3222:04 23:03 0.17 0.21 0.14 0.34 0.51 0.10 0.28 0.61 0.0123:04 0:03 0.21 0.26 0.16 0.55 0.97 0.26 0.54 1.14 0.090:04 1:03 0.24 0.28 0.22 0.45 0.89 0.15 0.51 1.01 0.131:04 2:03 0.24 0.29 0.18 0.40 0.79 0.11 0.44 0.91 0.092:04 3:03 0.24 0.31 0.21 0.50 1.15 0.32 0.47 1.04 0.093:04 4:03 0.26 0.33 0.20 0.63 1.71 0.14 0.75 1.85 0.054:04 5:03 0.28 0.34 0.20 0.85 1.67 0.52 1.10 1.89 0.565:04 6:03 0.28 0.32 0.24 0.78 1.38 0.31 0.74 1.24 0.446:04 7:03 0.27 0.31 0.22 0.59 0.99 0.29 0.58 1.15 0.247:04 8:03 0.24 0.33 0.19 0.40 0.78 0.07 0.61 1.38 0.068:04 9:03 0.23 0.34 0.18 0.55 1.34 0.06 0.83 1.78 0.139:04 10:03 0.25 0.43 0.15 1.00 1.70 0.47 1.44 2.13 0.8610:04 11:03 0.29 0.45 0.20 1.07 1.69 0.47 1.55 2.11 1.0711:04 12:03 0.28 0.46 0.13 1.10 1.67 0.63 1.40 2.31 0.5412:04 13:03 0.30 0.47 0.17 0.86 1.47 0.51 1.10 2.40 0.5113:04 13:28 0.28 0.38 0.22 0.89 1.09 0.60 1.17 1.55 0.84

- 1 0 5- 2 1 12

- 1255 5 36- 146 158 376

- 0 745 655- 0 420 239

- 0 58 71- 0 0 2

94

3.4-20

day

14C 90 4.42 4.48 5.1

Bq) 1Bq 120 10.84 10.87 11.14

150 6.97E-04 1.26E-03 6.85E-03

14C 90 4.63E-05 4.70E-05 5.35E-05

Bq/g 120 1.14E-04 1.14E-04 1.17E-04

150 1.39E-05 2.51E-05 1.37E-04

TF 90 0.30 0.53 2.56

120 0.12 0.22 1.17

95

3.2-1 14C 14C

3.2-2 14CO2

3.2-3 14CO2

97

3.2-4 14CO2

3.2-5 14CO2

98

3.3-1 P2 15˚C

3.3-2 P11

99

3.3-3 14C DGGE

3.3-4 DGGE DNA

100

3.4-

1

101

3.4-

2

0.0

0.2

0.4

0.6

0.8

020

4060

8010

0

day)

()

0.0

1.0

2.0

3.0

4.0

5.0

6.0

020

4060

8010

0

day)

()

0 10

20

30

40

50

60

020

4060

8010

0

day)

)

0.0

0.5

1.0

1.5

2.0

2.5

3.0

020

4060

8010

0

day)

→

0 10

20

30

40

020

4060

8010

0

day)

→

0 10

20

30

40

020

4060

8010

0

day)

→

0 50

100

150

020

4060

8010

0

day)

→

0 10

20

30

40

020

4060

8010

0

day)

→1

0 10

20

30

40

020

4060

8010

0

day)

→

0 10

20

30

40

020

4060

8010

0

day)

→

0 2 4 6 8 10

12

14

020

4060

8010

0

day)

2→

0 1 2 3

020

4060

8010

0

day)

→

102

3.4-

314

C3.

4-4

14C

103

3.4-5 14C 80-90 day 120 day

104

3.4-

6->

14C

3.4-

7->

14C

80

-90

day

120

day

80-9

0 da

y12

0 da

y

105

3.4-8 -> 14C 80-90 day 120 day

106

3.4-9 4 14C

y = 0.0167e0.0365x

R² = 0.5652

1.E-03

1.E-02

1.E-01

1.E+00

0 10 20 30 40

14C

-1B

qB

q)

(day

)

y = 0.0547e-0.03x

R² = 0.1424

1.E-03

1.E-02

1.E-01

1.E+00

0 10 20 30

14C

-1B

qB

q)

1→ (day

→

y = 0.0512e-0.056x

R² = 0.0732

1.E-03

1.E-02

1.E-01

1.E+00

0 5 10 15

14C

-1B

qB

q)

2→ 1 (day

2→

y = 0.0266e0.0232x

R² = 0.0779

1.E-03

1.E-02

1.E-01

1.E+00

0 10 20 30

14C

-1B

qB

q)

→ 1 (day

→ 1

107

3.4-10

3.4-11 1

108

3.4-12

3.4-13

3.4-14

109

3.4-15

3.4-16

3.4-17

110

3.4-18

3.4-19

111

3.4-

20C

O2

(0.4

)

(0.3

)

(0.2

)

(0.1

)

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0

1000

2000

3000

4000

5000

6000

0

1200

2400

3600

(m/s)

CO2 (ppm)

sec

84

Dry

ice

CO

2C

O2

(0.4

)

(0.3

)

(0.2

)

(0.1

)

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0

500

1000

1500

2000

2500

500

1100

1700

2300

(m/s)

CO2 (ppm)

sec

823

Dry

iceC

O2

CO

2

(0.4

)

(0.3

)

(0.2

)

(0.1

)

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0

1000

2000

3000

4000

5000

6000

7000

0

600

1200

1800

(m/s)

CO2 (ppm)

sec

824

Dry

ice

CO

2C

O2

(0.4

)

(0.3

)

(0.2

)

(0.1

)

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0

500

1000

1500

2000

2500

0

600

1200

1800

(m/s)

CO2 (ppm)se

c

91

Dry

ice

CO

2

CO

2

112

3.4-21 14C

113

3.4-22 14C

114

3.4-23

14C

3.4-24

14C

115

3.4-25

14C

3.4-26

14C

116

3.4-27 14C

3.4-28 -

0

0.002

0.004

0.006

0.008

0.01

0.012

0

0.1

0.2

0.3

0.4

0.5

0.6

0 50 100 150 200

14C

1Bq

Bq)

14C

(1B

qB

q)

(day)

117

3.4-29

0

1

2

3

4

5

0 10 20 30 40 50

day)

0.0

0.5

1.0

1.5

2.0

2.5

3.0

0 10 20 30 40 50

day)

→

0

10

20

30

40

0 10 20 30 40 50

day)

→

118

3.4-30 14C

y = 0.0023e0.601x

R² = 0.8311

1.E-04

1.E-03

1.E-02

1.E-01

1.E+00

0.0 1.0 2.0 3.0 4.0 5.0

14C

1Bq

)

(day

y = 0.0073e0.026x

R² = 0.0002

1.E-04

1.E-03

1.E-02

1.E-01

1.E+00

0.0 0.5 1.0 1.5 2.0 2.5

14C

1Bq

)

→ (day

→

y = 0.0089e-0.013x

R² = 0.0113

1.E-04

1.E-03

1.E-02

1.E-01

1.E+00

0 5 10 15 20 25

14C

1Bq

)

1→ (day

1→ )

119

3.4-31 14C

3.4-32 14C

y = 0.0055x0.6577

R² = 0.9193

1.E-04

1.E-03

1.E-02

1.E-01

1.E+00

0 5 10 15 20 25 30 35 40 45

14C

1Bq

)

(day

0.1 4day

4 40day

0

0.002

0.004

0.006

0.008

0.01

0.012

0

5

10

15

20

25

30

0 50 100 150 200

14C

1Bq

Bq)

114

C(1

Bq

Bq)

(day)1

1 1 1

120

4 Pu, Am, Th Cl

14 18

− TF - Kd

Pu, Am, Th Cl

Pu, Am, ThTF

Am Am

Am

Am

-

− ICP-MSTh Th Pu

25 Pu

Pu - Pu

Pu −

Pu, Am, Th TF 2015 -2016

27Am

121

Am

4.2.1. Am 241Am 241Am

241Am

Bennett, 1978 241Pu241Pu 241Am 241Am Zheng et al. (2012)

FDNPP 241Am

Am

Am241Pu 241Am Zheng et al., 2013a

241Am Amoli and

Barker, 2012; Maxwell and Faison, 2008; Zheng and Yamada, 2008241Am 0.1 1 Bq/kg

Xiao et al., 2014241Am Zheng et al.,

2013b Varga 2007

3-10238Pu, 210Po, 228Th 232U

10 Vajda and

Kim, 2010 ICP-MSAMS 241Am Kazi et al., 2015; Li et al., 2010

ICP-MS 241Am Hang et al., 2004; Truscott et al.,

2001 ICP-MS 241Am

Varga, 2007; Zheng and Yamada, 2008

ICP-MS AMS241Am

241Am

2

122

(Prohaska et al., 2014) 241Am

27 4.2-1

, 2016 ICP-MS

ICP-MS

(m/ m=300) Pu Bi, Pb, Tl, Hg, Ir m/z = 241

241Am Yamamoto et al. 1983 0.032-0.263 mBq/g 241Am

DGA-N

Am

Am CaC2O4 DGA-N Am

Am

Am Am

SF-ICP-MS AmTEVA

Am

Am 6

4.2.1.1. 4.2-1 Aridus

Aspire PFA PFA

Aspire PFA

Aridus II 110 oC

PFAPTFE

PTFE

SF-ICP-MS Aridus II

PFA 50, 100 200 µL min-1

50 µL min-1 ICP-AES Activa-M

Na Mg K Fe Ca Al

Bi Pb Tl Hg Pt Hf REEs SF-ICP-MS Element

XR Thermo Scientific Bremen Germany Scott

4.2.1.2. Aridus-SF-ICP-MS Element XR

123

H27 Aridus

H27 4.2-6

Am H27 4.2.2.

4.2.1.3. IAEA-soil-6 and IAEA-375 NIST-4357, IAEA-385 and

IAEA-384 (NIST-4354) 241Am

JSAC-0471241Am

4.2.1.4. HCl, HNO3, HF, HCOOH, H2C2O4, NH4OH, NaNO2, Ca(NO3)2, , NH4SCN

HCl HNO3

Bi, Tl, Hg, Pb, U, Hf, Pt, In, Rh REEs Merck Millipore

Eichrom (DGA-N, UTEVA and TEVA,

50-100µm 2 mL ) 243Am Amersham International, UK

Milli-Q-Plus>18 MΩ cm-1

4.2.1.5.

(1) DGA-N

DGA-N HCl HNO3

Am U, Bi, Tl, Hg, Pb, Hf, Pt Dy 2 ng mL-1 HNO3 HCl 5mL DGA-N

REE Am Dy

Am DGA-N

HCl HNO3 5mL

HCl HNO3 5mL

U, Bi, Tl, Hg, Pb, Hf, Pt Dy SF-ICP-MSHNO3 0.01 8 M 0.01M 0.05M 0.1M 0.5M 1M 3M 5M 8M

HCl 0.01 M 9.5 M 0.01M 0.1M 0.25M 0.5M 1M 4M 9M 9.5 M

4.2-2 Am Dy

4.2-2 a b HNO3 c d HCl

yHNO3 HCl DGA-N

1

0 Tl HNO3

HCl DGA-N Hg HNO3

HCl DGA-N 8M HNO3 Bi

Horwitz 2005 0.01~4M HCl 0.01~8M HNO3 DGA-N Pb DGA-N 0.5 3M HNO3

124

Horwitz 2005 0.5-1M HNO3

0.25M HCl Pt DGA-N

Kd Pourmand and Dauphas, 2010 Hf HNO3 HCl

4M Hf DGA-N

HNO3<0.1M HCl<1.0M DGA-N :

Pu U UTEVA DGA-N

HNO 3 15mL 8M HNO 3 Pb Hg Pt ; 15mL 0.5M HNO3

Tl ; 15mL 0.1M HNO3 U Pt Hf

(3 HCl 10mL HCl Bi Tl Pb UTEVA DGA-N Am

(2)

Am

Qiao et al., 2009; Xu et al., 2014 Am Fe(OH)3 CaF2

CaC2O 4 3

JSAC-0471 5g

4.2-3 Mg Al Fe(OH)3 Mg

Al CaF2 Al Fe

30 CaC2O4

Na 10 Am

CaC2O4

(3) Am

UTEVA + DGA-N Am CaC2O4

SF-ICP-MS

JSAC-0471 5g

Na K Mg Ca Fe Al REEs

4.2-1 0.1 7.6 g mL-1

REEs 6 66 gmL-1 Am Am REEsREEs 90 CaC2O4

Dy DGA-N

REEs SF-ICP-MS

SF-ICP-MS REEs SF-ICP-MS

Maxwell (2010) DGA-N REEs 0.05M HNO3

4.2-4a REEs Am

125

DGA-N 0.05M HNO3 0.05M HNO3 La Ce

65 La 25 Ce 10mL 0.05M HNO3

REEs

TEVA 241Am

Thakur et al., 2011; Luisier et al., 2009REEs

4.2-4b Pr Nd Sm Eu 10

TEVA La Ce Pr Nd Sm Eu

DGA-N 0.05M HNO3 10mL TEVA

REEs 4.2-4b Am 95

Am REEs

4.2.1.6

(1)

Am 4.2-5

105ºC 24 802-20g 0.5 pg 243Am

450ºC 5

Am 120 mL

Savillex Corporation, Minnesota, USA 20-40 mL

160 C 4 Advantec filter100 mL 40mL 1M HNO3

Ca 100mg 2.5g

NH4OH pH 2.0 2.5 30

3000 rpm 20 1 5mL

15mL HNO3 8M

HNO3 20mL 0.2 g NaNO2 8M HNO3 UTEVAPu Pu IV

UTEVA + DGA-N Am 5mL 8M HNO3

UTEVA + DGA-N UTEVA

Am DGA-N DGA-N

(1)15mL 8M HNO 3 Pb Hg Pt

; (2)15mL 0.5M HNO3 Tl ; (3)15mL 0.1M HNO3 U Pt Hf(4)10 mL 0.05 M HNO3 La, Ce ; (5)10mL HCl Bi Tl

Pb

UTEVA + DGA-N Am DGA-N

Am 10mL 0.5M HCl 10mL 2M

NH4SCN-0.1M HCOOH TEVA Am REEs

5mL 2M NH4SCN-0.1M HCOOH TEVA Am10mL 2M NH4SCN-0.1M HCOOH 10mL 1M NH4SCN-0.1M

126

HCOOH TEVA REEs Am 10mL 4M HCl DGA-N

TEVA 4.2-6 Am TEVA

NH4SCN 8mL

SF-ICP-MS 1mL 4 HNO3

(2) Am Am

IAEA-soil-6 DF DF

Bi Tl Hg Pb U, Pu DF 3.5 10 4 2.4

10 4 1.5 10 4 1.2 105 3.6 106, 7 105

Am

IAEA-384 78 3 IAEA-385 77 1 IAEA-375 82 1 IAEA- -6 765 NIST- 4354 79 6 NIST-4357 79 7 80 3

LOD 3

1g 0.097 fg g-1 0.012 mBq g-1 LOD Pimpl and Higgy (2001)

0.03 mBq g-1 Jia (1997) 0.034 mBq g-1

LOD DF241Am

(3)

Am SF-ICP-MS

IAEA-soil-6 and IAEA-375 NIST-4357, IAEA-385 and IAEA-384

(NIST-4354)4.2-7

241Am

4.2.2. 241Am

4.2.2.1.

1620 241Am 241Am

Pu 239+240Pu 240Pu/239Pu

4.2.2.2

105ºC 24 80

5-10g 0.5 pg 243Am

450ºC 5 4.2.1.6241Am SF-ICP-MS 241Am

Pu 4.5.2.

4.2.2.3. Am Am

127

Am -

, Am 241Pu T1/2 = 14.4241Am T1/2 = 433 241Pu

241Am

16

20 241Am 239+240Pu240Pu/239Pu 4.2-2

241Am 241Am 239+240Pu0.136 0.219 mBq/g 0.219

mBq/g 20 241Am 0.100 ± 0.047 mBq/g241Am 241Am

Yamamoto 1983 1963 1976 15

30 15 2 1957

1980 15 241Am 241Am 0.030 0.337 mBq/g 1963

30 241Am 0.163 ± 0.085 mBq/g 1976

30 241Am 0.118 ± 0.078 mBq/g241Am

241Am 0.407 2.701 mBq/g

(Yamamoto et al., 1980) 239+240Pu 240Pu/239Pu 241Am/239+240Pu activity ratio 4.2-3

240Pu/239Pu 0.166 0.183

Kelley et al., 1999 Pu

20 3.6 20.2 4.2-2 Pu241Am (Ovsiannikova et al., 2010) 4.2-8A

241Am

4.2-8B C 241Am 239+240Pu 137Cs241Am 239+240Pu 137Cs 241Am

137Cs Pu 241Am/239+240Pu 0.34

0.43 ( 4.2-3)

(0.69 ± 0.08) Pu 241Am

241Am/239+240Pu 241Am

4.2-9 19 241Am/239+240Pu

0.39±0.02 4.2-9A 4.2-9B Yamamoto 1983241Am/239+240Pu (1955-1980) 4.2-9B

1957 1958 241Am / 239+240Pu 0.44 19610.30

128

241Pu

2

1952-1958 1961-1962

(Hisamatsu et al., 1978; Koide et al., 1981) 1 241Pu / 239+240Pu

2 4.2-9B 1957 1958241Am / 239+240Pu

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Th 4.3.1.

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TF Wang, et al., 2015ICP-MS

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mg kg-1 (2.3 – 11 mg kg-1) 5.0 mg kg-1 (1.2 – 12 mg kg-1) Uchida et al. 2007a; Uchida et al.

2007b ThICP-MS Th 100 232

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ng g-1 Uchida et al. 2007b

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4.4.1.

-36 36Cl 30.1 35Cl

75.78

TF

2014

NAA

ICP-MSTF

TF

TMAH

2016

TMAH ICP

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H26 TMAH

2015

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mg Savillex 6 mL 25 TMAH Tama pureAA-1002 mL Milli-Q 1 mL 80 16

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NAA TMAH4.4-2 Br I -ICP-MS 0.35±0.15 Br

135

0.97±0.13 I 0.83±0.09 3 1 TMAH

TMAH NAA

Yamada 1996

TMAH Takeda 2011Br I I

Tagami et al., 2010

4.4.3. TMAH ICP-MS

ICP-MS 8800 2

DL MS/MS + He 35 -> 35He MS/MS

2 35 Br I

ICP-MS

TMAH H2O2

1 TMAH Cl, Br, I5 mL PTFE , 30 mL H2O2 Tama pureAA-100

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80 RSDRSD 8

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Tsukada and Nakamura 1998 Yuita 1983 TFTF Tsukada and Nakamura (1998) IAEA 2010

136

Yuita 1983

TF TF Yuita 1983

TF

4.4.5.

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35

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80 8%

Cl TF Cl

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Bq / kg

TF ICRU, 2001 1994 IAEA TF

TRS-364 (IAEA TRS-364, 1994) IAEA TF

TRS 472 (IAEA TRS-472, 2010) TRS-472 Pu

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acid, TiCl3, Ca(NO3)2, La(NO3)3, NH2OHHCl, Iron (II) sulfamate

Bio-Rad 2 AG 1X8 100-200 mesh, Cl- form AG MP-1M 100-200 mesh, Cl- form Tama Chemicals

HNO3 SF-ICP-MS

Eichrom 3 TEVA UTEVA DGA 50 100 m

2mL 242Pu (CRM 130, plutonium spike

assay and isotopic standard, New Brunswick Laboratory, USA)

>18 MΩ cm-1 240Pu/239Pu 0.242 PuNBS-947

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Pu IV Pu III TEVA Pu III 3M HNO3 - 0.1M

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DGA U Tl Pb Pt Hf Fe DGA 30mL 0.1M

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26 4.2.3.5

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2012) Pu 240Pu/239Pu

3 Pu 240Pu/239PuPu 240Pu/239Pu

140

7 240Pu/239Pu

0.160 0.182

Kelley et al., 1999 Pu

239+240Pu 0.204 0.919 mBq/g 239Pu 0.12

0.56 mBq/g Pu Yamamoto

1983 1963 1976 15 30

15 2 1957 1980

15 239+240Pu 239+240Pu 0.078 1.03

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Muramatsu et al., 2003

4.5.3.2. Pu

Pu Pu Pu

Pu

PuPu

20 30 ICP-MS 239Pu 240Pu240Pu

239Pu 4.5-2

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4.5.3.3. Pu -

Pu - TF

27 239Pu

Pu-TF 4.5-2

Pu - TF 4.5×10-6 1.0×10-4

2.7×10-5 3.7×10-5

TF 1 2 Pu

4.5-3

239,240Pu Duffa 2002 Zhang 1989 238Pu

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TF - re-suspension(Wang et al., 2015a) Pu

TF re-suspension TF

Pu

Pu

Pu1 4 Baeza et al., 2006

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Pu-TF Pu-TF -

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TRS-472

TECDOC-1616 TRS-472

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Th Pu Cl

Cu Ag Na W 100 IAEA, 2009

TRS-472 2007

TF 20072006-2007

Wang 2007 2014 TRS-472

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TF

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Nie et al. (2010) Tuovinen et al. (2016) Matveyeva et al. (2015) Asaduzzaman et al. (2015) Hossen and

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Todorov Djingova (2015) Li et al. (1994) Guillen (2016)

Am TF Guillen (2016) Pu 2

TF Froehlich 2016 AMS239Pu Pu 2 TF

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GM AM GSD SD

N

GM

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Th U ICP-MS Th TFs

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TF IAEA 1.2 10-3 1TF IAEA

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6 241Am

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241Am 241Am

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IAEA 4.4 10-7 9.0 10-4 Froehlich

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TRS-472 1

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149

4.7.1. Am Cl

4.7.1.1. Am

DGA-N TEVA Am / REEs3

SF-ICP-MS 2 20g 241Am

HNO3 CaC2O4

Am Na K Mg Al Fe UTEVA + DGA-N

Am TEVA REEs Aridus (II)-SF-ICP-MS241Am DF

Pu 7 105 241Am241Am ICP-MS 241Am

6 241Am241Am Am

76 82 LOD 0.012 mBq/g 241Am

16

20 241Am241Am

241Am 239+240Pu 0.136 0.219 mBq/g

4.7.1.2. TMAH

TMAH H2O2

ICP-MS/MS TF

4.7.2. Th

26 27 20 27

10 Th 20 Th 1.4×10-5 6.7×10-4 mg/kg

/ 48 1.8×10-4

1.0×10-4 mg/kg 27 10 Th 7.7×10-5

4.7×10-4 mg/kg / 6

2.1×10-4 1.8×10-4 mg/kg Th Th

/ 8

Th Th

Th -

4.7.3. Pu -

150

8 Pu Pu 240Pu/239Pu Pu Pu

Pu Pu - TF TF

4.5×10-6 1.0×10-4 2.7×10-5 TF-Pu

Pu TF Pu TF TF TF-Pu

151

4.2-1 CaC2O4 UTEVA + DGA-N Am 5g JSAC-0471 SF-ICP-MS 1mL

Matrix Na K Mg Ca Fe Al

Concentration ( g/mL) 1.5±0.2 7.6±1.1 0.1±0.0 1.9±1.6 2.2±0.2 1.7±0.4 REEs La Ce Nd Sm Dy

Concentration ( g/mL) 6±2 16±5 66±14 24±2 8±1

4.2-2 241Am

Organic matter 241Am activitySample code FAO-UNESCO Prefecture (%) mBq/g std

EF-SD-01 Andosol 18.0 0.067 0.017EF-SD-06 Fluvisol 8.5 0.154 0.011EF-SD-07 Andosol 8.4 0.084 0.012EF-SD-08 Cambisol 3.6 0.036 0.011EF-SD-09 Cambisol 5.4 0.089 0.014EF-SD-10 Andosol 17.0 0.122 0.015EF-SD-11 Fluvisol 7.0 0.060 0.010EF-SD-13 Fluvisol 7.1 0.110 0.014EF-SD-17 Fluvisol 20.0 0.058 0.015EF-SD-18 Andosol 14.2 0.113 0.013EF-SD-21 Fluvisol 6.5 0.104 0.015EF-SD-22 Cambisol 6.9 0.064 0.012EF-SD-23 Cambisol 6.6 0.037 0.010EF-SD-24 Fluvisol 6.3 0.058 0.011EF-SD-25 Fluvisol 8.1 0.099 0.010EF-SD-29 Cambisol 10.8 0.085 0.014EF-SD-30 Andosol 20.2 0.219 0.027EF-SD-35 Fluvisol 10.2 0.118 0.013EF-SD-36 Andosol 12.4 0.179 0.019EF-SD-37 Fluvisol 6.8 0.139 0.009

153

4.2-3 Pu 241Am/239+240Pu activity

4.3-1 Th

Th (mg/kg) std GBW-1 0.075 0.002 GBW-2 0.079 0.001 certified value 0.070 0.008 NIST-1573a-1 0.120 0.001 NIST-1573a-2 0.136 0.002 NIST-1573a-3 0.099 0.001 information value 0.12

239+240Pu activitySample code FAO-UNESCOPrefecture mBq/g std 240Pu/239Pu std 241Am/239+240Pu std

EF-SD-01 Andosol 0.182 0.001 0.182 0.015 0.37 0.09EF-SD-06 Fluvisol 0.384 0.007 0.166 0.016 0.40 0.03EF-SD-07 Andosol 0.207 0.002 0.169 0.014 0.41 0.06EF-SD-08 Cambisol 0.105 0.001 0.173 0.018 0.34 0.10EF-SD-09 Cambisol 0.227 0.002 0.182 0.015 0.39 0.06EF-SD-10 Andosol 0.339 0.005 0.172 0.017 0.36 0.04EF-SD-11 Fluvisol 0.161 0.001 0.175 0.012 0.37 0.06EF-SD-13 Fluvisol 0.256 0.003 0.172 0.016 0.43 0.05EF-SD-17 Fluvisol 0.159 0.001 0.183 0.019 0.37 0.10EF-SD-18 Andosol 0.290 0.003 0.182 0.013 0.39 0.04EF-SD-21 Fluvisol 0.283 0.002 0.170 0.008 0.37 0.05EF-SD-22 Cambisol 0.169 0.001 0.179 0.013 0.38 0.07EF-SD-23 Cambisol 0.100 0.000 0.180 0.012 0.37 0.10EF-SD-24 Fluvisol 0.145 0.001 0.183 0.014 0.40 0.08EF-SD-25 Fluvisol 0.254 0.001 0.174 0.008 0.39 0.04EF-SD-29 Cambisol 0.218 0.001 0.180 0.008 0.39 0.06EF-SD-30 Andosol 0.595 0.016 0.178 0.018 0.37 0.05EF-SD-35 Fluvisol 0.171 0.001 0.177 0.012 0.69 0.08EF-SD-36 Andosol 0.434 0.008 0.166 0.015 0.41 0.04EF-SD-37 Fluvisol 0.325 0.007 0.171 0.022 0.43 0.03

154

4.3-2 Th

Th (mg/kg) stdEP II-CF-1 6.7E-04 4.5E-05EP II-CF-2 NDEP II-CF-3 1.9E-04 1.9E-05EP II-CF-4 4.3E-05 2.0E-05EP II-CF-5 3.0E-05 1.1E-05EP II-CF-6 3.7E-05 1.5E-05EP II-CF-7 3.1E-05 1.1E-05EP II-CF-8 3.6E-04 2.8E-05EP II-CF-9 9.6E-05 2.5E-05EP II-CF-10 NDEP II-CF-11 3.7E-04 1.4E-05EP II-CF-12 3.0E-04 1.7E-05EP II-CF-13 2.8E-04 2.6E-05EP II-CF-14 5.1E-05 1.2E-05EP II-CF-15 2.7E-04 2.0E-05EP II-CF-16 NDEP II-CF-17 1.0E-04 1.4E-05EP II-CF-18 2.9E-05 5.6E-06EP II-CF-19 1.2E-04 2.5E-05EP II-CF-20 1.4E-05 7.0E-06Minimum 1.4E-05Maximum 6.7E-04Max./Min. 48Median 9.9E-05Arithmetric mean 1.8E-04Geometric mean 1.0E-04EP II-CF-11 2.9E-04 6.0E-06EP II-CF-12 2.5E-04 4.1E-05EP II-CF-13 4.7E-04 9.5E-06EP II-CF-14 1.4E-04 5.8E-06EP II-CF-15 2.0E-04 1.4E-05EP II-CF-16 7.9E-05 5.6E-06EP II-CF-17 1.7E-04 5.8E-06EP II-CF-18 7.7E-05 5.4E-06EP II-CF-19 2.3E-04 1.1E-05EP II-CF-20 1.5E-04 8.2E-06Minimum 7.7E-05Maximum 4.7E-04Max./Min. 6Median 1.9E-04Arithmetric mean 2.1E-04Geometric mean 1.8E-04

155

4.4-1 TMAH RSD(%)

*H27

4.4-2 RSD(%)

*H27

Code Cl mg/kg Br mg/kg I mg/kg

EFII Run-1 RSD Run-2 RSD Run-1 RSD Run-2 RSD Run-1 RSD Run-2 RSD

SD-1 51 18 29 11 7.3 1 7.2 5 1.9 17 1.8 7

SD-2 62 16 85 1 7.9 1 8.7 5 1.5 11 1.6 9

SD-3 90 15 76 5 113 2 115 3 30 0 29 4

SD-4 106 11 92 2 132 2 132 3 32 1 32 4

SD-5 99 5 88 5 110 1 110 3 32 2 31 4

SD-6 174 3 189 6 41 1 44 3 10 2 11 5

SD-7 222 3 210 4 158 1 161 3 21 1 22 4

SD-8 194 1 192 5 125 1 126 3 18 3 19 4

SD-9 37 18 32 10 54 0 53 5 30 2 29 4

SD-10 136 4 123 7 47 1 47 5 11 3 11 6

H27* RSD 78 (37-130) 2 (0-5) 2 (1-4)

Code Cl mg/kg Br mg/kg I mg/kg

EFII Run-1 RSD Run-2 RSD Run-1 RSD Run-2 RSD Run-1 RSD Run-2 RSD

CF-1 2530 2 2760 4 8.2 5 8.9 7 - - 0.026 21

CF-2 6380 2 6310 5 9.1 4 9.0 8 0.033 45 0.026 37

CF-3 1110 5 1060 4 10.4 6 10.0 5 0.037 44 0.022 71

CF-4 4770 4 4530 5 113 6 108 6 0.137 17 0.124 10

CF-5 5180 4 4890 6 46 5 44 7 0.290 9 0.357 5

CF-6 11900 7 11300 5 15.3 7 15.0 6 0.098 22 0.070 41

CF-7 2630 7 2500 4 29 7 28 4 0.104 20 0.101 33

CF-8 2110 6 2030 3 9.3 6 9.3 3 0.128 15 0.189 14

CF-9 5050 10 4720 5 51 8 50 5 0.347 11 0.360 9

CF-10 4760 9 4320 5 12.7 7 13.6 5 0.140 15 0.160 14

H27* RSD 7 (1-35) 2 (1-10) 19 (4-33)

156

4.4-3 TF

4.4-4.

Reference Cl Br I

58 (11 – 141) 0.54 (0.07 – 1.2) 0.010 (0.001 – 0.019)

2016 42 (9 – 138) 0.69 (0.05 – 3.2) 0.011 (0.002 – 0.038)

Tsukada and Nakamura, 1998

15 44 0.36 1.7 0.005, 0.015

Yuita, 1983 127 (10-265) 0.79 (0.36-1.8) 0.011 (0.005-0.028)

TRS-472 (IAEA, 2010)

26 (14 – 48) - 0.0065

Code Cl Br I

EFII- Crop Soil TF Crop Soil TF Crop Soil TF

CF-1 2640±120 40±10 66 8.6±0.7 7.3±0.4 1.2 0.026 1.8±0.3 0.014

CF-2 6340±330 73±10 87 9.0±0.8 8.3±0.4 1.1 0.029±0.018 1.6±0.2 0.019

CF-3 1090±70 83±14 13 10.2±0.9 114±4 0.09 0.029±0.022 29.4±1.1 0.001

CF-4 4650±280 99±11 47 110±9 132±5 0.83 0.130±0.026 31.8±1.3 0.004

CF-5 5030±350 94±7 54 45±4 110±3 0.41 0.324±0.033 31.4±1.4 0.010

CF-6 11600±980 181±12 64 15.1±1.4 43±2 0.35 0.084±0.036 10.6±0.5 0.008

CF-7 2560±200 216±11 12 28±3 160±5 0.18 0.103±0.040 21.3±1.0 0.005

CF-8 2070±150 193±11 11 9.3±0.6 125±4 0.07 0.159±0.032 18.7±0.9 0.009

CF-9 4880±550 35±7 141 50±5 54±3 0.93 0.353±0.049 29.3±1.4 0.012

CF-10 4540±490 129±10 35 13.1±1.1 47±3 0.28 0.150±0.031 10.7±0.7 0.014

157

4.5-1 Pu 240Pu/239Pu 1-6, 27 7-10, 28

Sample ID

Prefecture 239Pu activity (mBq/g)

239+240Pu activity(mBq/g)

240Pu/239Pu atom ratio

1 Akita 5.55 ± 0.15 × 10-1 8.85 ± 0.30 × 10-1 0.162 ± 0.008

2 Niigata 2.78 ± 0.09 × 10-1 4.48 ± 0.02 × 10-1 0.166 ± 0.010

3 Toyama 2.20 ± 0.09 × 10-1 3.57 ± 0.10 × 10-1 0.171 ± 0.008

4 Gifu 3.62 ± 0.15 × 10-1 6.04 ± 0.31 × 10-1 0.182 ± 0.013

5 Nagasaki 1.47 ± 0.06 × 10-1 2.34 ± 0.11 × 10-1 0.160 ± 0.011

6 Fukushima 2.36 ± 0.12 × 10-1 3.93 ± 0.30 × 10-1 0.167 ± 0.012

7 Chiba 2.32 ± 0.11 × 10-1 3.87 ± 0.29 × 10-1 0.181 ± 0.013

8 Toyama 2.44 ± 0.08 × 10-1 3.92 ± 0.73 × 10-1 0.165 ± 0.012

9 Gifu 5.52 ± 0.33 × 10-1 9.19 ± 0.07 × 10-1 0.180 ± 0.014

10 Nara 1.23 ± 0.03 × 10-1 2.04 ± 0.23 × 10-1 0.179 ± 0.006

158

4.5-2 239Pu Pu -

4.5-3 Pu -

Sample ID Sampling location 239Pu in rice (mBq/g) std 239Pu in soil (mBq/g) std TF7 (EF-SD-40) Chiba 5.3E-06 1.5E-06 2.3E-01 1.1E-02 2.3E-058 (EF-SD-42) Toyama 4.9E-06 1.7E-06 2.4E-01 8.4E-03 2.0E-059 (EF-SD-43) Gifu 2.5E-06 8.9E-07 5.5E-01 3.3E-02 4.5E-0610 (EF-SD-45) Nara 1.3E-05 1.1E-06 1.2E-01 2.9E-03 1.0E-041 (EP-SD-64) Akita 1.9E-05 1.7E-05 5.6E-01 1.5E-02 3.5E-052 (EP-SD-65) Niigata 8.0E-06 2.9E-06 2.8E-01 9.0E-03 2.9E-053 (EP-SD-66) Toyama 4.5E-06 1.7E-06 2.2E-01 9.0E-03 2.0E-054 (EP-SD-67) Gifu 9.0E-06 2.2E-06 3.6E-01 1.5E-02 2.5E-055 (EP-SD-68) Nagasaki 1.2E-05 6.5E-06 1.5E-01 6.0E-03 8.2E-05

6 (OK-K2) Fukushima 6.6E-06 2.5E-06 2.4E-01 1.2E-02 2.8E-05RemarksThe 240Pu/239Pu atom ratio of EF-SD-45 was determined to be 0.195 ± 0.049, indicating global fallout sourceRange of TF of Pu for rice 4.5E-06 - 1.0E-04Minimum 4.5E-06Maximum 1.0E-04Max./Min. 22.7Median 2.6E-05Arithmetric mean (AM) of TF 3.7E-05Geometric mean (GM) of TF 2.7E-05

159

4.6-

120

08-2

016

Th−

a:

Und

er n

atur

al fi

eld

cond

ition

s, TF

s wer

e ob

tain

ed b

y ex

amin

ing

232 Th

con

cent

ratio

ns in

the

plan

t and

cor

resp

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ng so

il sa

mpl

es.

b: In

an

aban

done

d ur

aniu

m m

ine,

TFs

wer

e ob

tain

ed b

y ex

amin

ing

230 Th

(or 23

2 Th) c

once

ntra

tions

in th

e pl

ant a

nd c

orre

spon

ding

soil

sam

ples

. c:

In U

-mill

taili

ng d

ispo

sal s

ites,

TFs w

ere

obta

ined

by

exam

inin

g 23

0 Th c

once

ntra

tions

in th

e pl

ant a

nd c

orre

spon

ding

soil

sam

ples

.

Plan

t Gro

up

N

AM

SD

G

M

GSD

M

in.

Max

. TR

S 47

2 G

M

Ref

. No.

R

emar

k

Gra

ss

183

1.3×

10-1

1.

4×10

-1

6.0×

10-2

4.

4 2.

0×10

-3

9.0×

10-1

4.

2×10

-2

e Ref

(Gra

ss)

Nat

ural

fiel

d TF

sa U

min

e ta

iling

TFs

c 20

16 d

ata

entri

es: 1

2 Le

afy

Veg

etab

le

25

1.1×

10-1

1.

5×10

-1

1.5×

10-2

22

5.

8×10

-4

3.4×

10-1

1.

2×10

-3

Hos

sen,

201

5 Pl

anin

sek,

201

6 N

atur

al fi

eld

TFsa

Ura

nium

min

e TF

sb 20

16 d

ata

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es: 1

5 Fr

uit

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le p

art

ined

ible

par

t

18

7

1.5×

10-1

1.2×

10-1

4.5×

10-1

7.7×

10-2

6.0×

10-2

9.2×

10-2

7.0

6.3

2.5×

10-4

1.0×

10-3

1.3

0.7

f R

ef (F

ruit)

N

atur

al fi

eld

TFsa

Nat

ural

fiel

d TF

sa N

on-le

afy

Veg

etab

le

edib

le p

art

ined

ible

par

t

43

11

2.3×

10-1

3.4×

10-1

3.7×

10-1

2.7×

10-1

2.6×

10-2

2.4×

10-1

13

3.7

1.9×

10-4

3.8×

10-2

1.7

9.1×

10-1

7.8×

10-4

2.2×

10-3

g Ref

(N

on-L

eafy

V

eget

able

)

Nat

ural

fiel

d TF

sa N

atur

al fi

eld

TFsa

Cer

eal

(e

xcep

t ric

e)

38

5.5×

10-1

3.

3×10

-1

3.5×

10-1

12

3.

6×10

-4

1.0×

100

2.1×

10-3

j Ref

(Cer

eal)

Nat

ural

fiel

d TF

sa U

rani

um m

ine

TFsb

2016

dat

a en

tries

: 30

Ric

e ed

ible

par

t in

edib

le p

art

44

3

5.1×

10-2

3.0×

10-3

1.0×

10-1

2.0×

10-3

1.5×

10-2

2.5×

10-3

7.7

2.0

3.1×

10-5

1.0×

10-3

4.8×

10-1

5.0×

10-3

1.6×

10-4

h R

ef (R

ice)

N

atur

al fi

eld

TFsa

Pot e

xper

imen

t TFs

i 20

16 d

ata

entri

es: 4

Tu

ber

edib

le p

art

ined

ible

par

t

14

10

1.1×

10-1

3.6×

10-2

2.5×

10-1

2.9×

10-2

1.4×

10-2

2.9×

10-2

47

14

1.4×

10-3

1.3×

10-2

1.9×

10-1

1.2×

10-1

2.0×

10-4

1.9×

10-2

Asa

duzz

aman

, 20

14,

Kha

n 20

10;

C

hauh

an, 2

015

Plan

inse

k, 2

016

Nat

ural

fiel

d TF

sa

Ura

nium

min

e TF

sb 20

16 d

ata

entri

es: 5

Roo

t cro

p 6

5.9×

10-1

5.

5×10

-1

4.6×

10-1

2.

4 2.

8×10

-1

1.7

8.0×

10-4

A

sadu

zzam

an, 2

014

Shan

thi,

2012

N

atur

al fi

eld

TFsa

Tree

17

1.

5×10

-2

2.5×

10-2

2.

8×10

-3

12

4.6×

10-5

1.

0×10

-1

R

odrig

uez,

20

10;

Popi

c, 2

011;

Zh

ang,

198

9

Ura

nium

min

e TF

sb C

onta

min

ated

ar

ea

TFsd

160

d: In

a w

etla

nd si

te c

onta

min

ated

by

radi

oact

ive

was

te d

isch

arge

d fr

om a

nuc

lear

rese

arch

faci

lity,

TFs

for 23

2 Th w

ere

dete

rmin

ed.

e R

ef (G

rass

): N

ie, e

t al.,

201

0; T

uovi

nen,

et a

l., 2

016;

Mat

veye

va, e

t al.,

201

5; IC

RP,

200

9; A

lhar

bi a

nd E

l-Tah

er.,

2013

; Kris

tsan

anuw

at e

t al.,

201

4; C

erne

et a

l.,

2010

; Dra

govi

c et

al.,

201

0; K

han

et a

l., 2

011;

Ouf

ni e

t al.,

201

1; P

alla

vici

ni, 2

011;

Sm

odis

et a

l., 2

012;

Cha

krab

orty

et a

l., 2

013;

Stro

k an

d S

mod

is 2

013.

Yan

, 20

16.

f Ref

(Fru

it): A

lhar

bi a

nd E

l-Tah

er, 2

013;

Kris

tsan

auw

at e

t al.,

201

4; K

umar

et a

l., 2

008;

Sha

nthi

et a

l., 2

012

g Ref

(Non

-Lea

fy v

eget

able

): K

rists

anau

wat

et a

l., 2

014;

Zha

ng e

t al.,

201

1; S

hant

hi e

t al.,

201

2; A

swoo

d et

al.,

201

3; M

heem

eed

et a

l., 2

014.

h R

ef (R

ice)

: Asa

duzz

aman

, et a

l., 2

015;

Als

affa

r, et

al.,

201

5; K

rists

anau

wat

et a

l., 2

014;

Sha

nthi

et a

l., 2

012;

Sae

ed e

t al.,

201

2. A

lsaf

far,

et a

l., 2

016.

i:

In a

pot

exp

erim

ent u

sing

nat

ural

soil,

TFs

wer

e ob

tain

ed b

y ex

amin

ing

232 Th

con

cent

ratio

ns in

gra

in a

nd so

il sa

mpl

es.

j Ref

(Cer

eal):

Kha

n 20

10; M

ihay

lova

, el a

l.,

2013

; Alh

arbi

, et a

l., 2

013;

Mos

tafa

, et a

., 20

16.

4.

6-2

2008

-201

6A

m−

a:

In a

dun

e ad

jace

nt to

Sel

lafie

ld a

nd a

low

leve

l was

te d

ispo

sal s

ite, T

Fs fo

r 241 A

m w

ere

dete

rmin

ed.

b: In

lysi

met

ers s

pike

d w

ith 24

1 Am

, TFs

for A

m w

ere

obta

ined

by

exam

inin

g th

e 24

1 Am

con

cent

ratio

n in

pla

nt a

nd so

il sa

mpl

es.

c: In

nat

ural

con

ditio

ns, a

ggre

gate

d TF

s wer

e ob

tain

ed b

y ex

amin

ing

241 A

m c

once

ntra

tions

in th

e pl

ant a

nd c

orre

spon

ding

soil

sam

ples

. d:

In n

atur

al c

ondi

tions

, TFs

wer

e ob

tain

ed b

y ex

amin

ing

241 A

m c

once

ntra

tions

in th

e pl

ant a

nd c

orre

spon

ding

soil

sam

ples

. Pl

ant G

roup

N

A

M

SD

GM

G

SD

Min

. M

ax.

TRS

472

GM

R

ef. N

o.

Rem

ark

Gra

ss

28

0.24

0.

57

2.6×

10-3

10

3 9.

0×10

-5

1.4

3.3×

10-2

IC

RP,

2009

To

doro

v, 2

015

Con

tam

inat

ed a

rea

TFsa

241 A

m sp

iked

stud

y TF

sb Le

afy

Veg

etab

le

4 1.

2×10

-3

2.4×

10-3

6.

3×10

-5

19

3.6×

10-6

4.

9×10

-3

2.7×

10-4

G

omez

, 20

13,

Li, 1

994

241 A

m

spik

ed

stud

y TF

sb N

atur

al fi

eld

TFsd

Non

-leaf

y V

eget

able

edib

le p

art

ined

ible

par

t

7 3

1.4×

10-3

3.7×

10-4

1.4×

10-3

1.5×

10-4

6.9×

10-4

3.4×

10-4

11

1.5

9.0×

10-5

2.0×

10-4

3.7×

10-3

5.0×

10-4

3.6×

10-4

Leht

o, 2

013,

Li

, 199

4

Nat

ural

fiel

d TF

sc

Nat

ural

fiel

d TF

sd

Tube

r 3

1.1×

10-5

2.

3×10

-6

1.0×

10-5

1.

2 8.

4×10

-6

1.3×

10-5

2.

1×10

-4

Gom

ez, 2

013,

24

1 Am

spik

ed st

udy

TFsb

Roo

t cro

p 4

1.3×

10-3

2.

5×10

-3

6.2×

10-5

22

6.

9×10

-6

5.1×

10-3

6.

7×10

-4

Gom

ez,

2013

, Li

, 199

4

241 A

m

spik

ed

stud

y TF

sb N

atur

al fi

eld

TFsd

Cer

eal

ined

ible

par

t 2

2.5×

100

3.3×

100

2.0×

10-1

4.

8×10

0 7.

9×10

–5

Gui

llen,

2016

241 A

m sp

iked

stud

y TF

sb 20

16 d

ata

entri

es: 2

161

4.

6-3

2008

-201

6Pu

−

a: In

a d

une

adja

cent

to S

ella

field

and

a lo

w le

vel w

aste

dis

posa

l site

, TFs

was

det

erm

ined

by

exam

inin

g th

e 23

9,24

0 Pu c

once

ntra

tions

in p

lant

and

soil

b:

In a

con

tam

inat

ed a

rea

near

a d

ecom

mis

sion

ed n

ucle

ar fa

cilit

y, P

u TF

s wer

e de

term

ined

. c:

In n

atur

al e

nviro

nmen

t, TF

s wer

e de

term

ined

by

exam

inin

g 23

9 Pu c

once

ntra

tions

in th

e pl

ant a

nd c

orre

spon

ding

soil

sam

ples

d:

In ly

sim

eter

s con

tam

inat

ed w

ith 23

9,24

0 Pu, T

Fs fo

r Pu

wer

e ob

tain

ed b

y ex

amin

ing

the

239,

240 Pu

con

cent

ratio

n in

pla

nt a

nd so

il sa

mpl

es.

e: In

nat

ural

con

ditio

ns, a

ggre

gate

d TF

s wer

e ob

tain

ed b

y ex

amin

ing

239,

240 Pu

con

cent

ratio

ns in

the

plan

t and

cor

resp

ondi

ng so

il sa

mpl

es.

f: In

lysi

met

ers c

onta

min

ated

with

239 Pu

, TFs

for P

u w

ere

obta

ined

by

exam

inin

g th

e 23

9 Pu c

once

ntra

tion

in p

lant

and

soil

sam

ples

. Pl

ant G

roup

N

A

M

SD

GM

G

SD

Min

. M

ax.

TRS

472

GM

R

ef. N

o.

Rem

ark

Gra

ss

20

2.5×

10-2

7.

8×10

-2

2.3×

10-4

44

1.

1×10

-6

3.3×

10-1

1.

6×10

-4

ICR

P,20

09 X

u,

2009

, Li,

2011

Fr

oehl

ich,

201

5

Con

tam

inat

ed a

rea

TFsa

Con

tam

inat

ed a

rea

TFsb

Nat

ural

fiel

d TF

sc

Leaf

y V

eget

able

3

1.9×

10-5

1.

7×10

-5

1.5×

10-5

2.

0 7.

9×10

-6

1.1×

10-5

8.

3×10

-5

Gom

eze,

201

3,

Lysi

met

er st

udy

TFsd

Non

-leaf

y V

eget

able

ed

ible

par

t in

edib

le p

art

1 3

3.0×

10-5

1.9×

10-4

1.2×

10-4

1.5×

10-4

2.0

6.0×

10-5

3.0×

10-4

6.5×

10-5

Leht

o, 2

013

Leht

o, 2

013

Nat

ural

fiel

d TF

se

Nat

ural

fiel

d TF

se Tu

ber

3 1.

4×10

-5

3.1×

10-6

1.

3×10

-5

1.2

1.1×

10-5

1.

7×10

-5

1.1×

10-4

G

omez

e, 2

013,

Ly

sim

eter

stud

y TF

sd R

oot c

rop

3 2.

2×10

-5

1.7×

10-5

1.

6×10

-5

2.4

5.1×

10-6

3.

9×10

-5

3.9×

10-4

G

omez

e, 2

013,

Ly

sim

eter

stud

y TF

sd C

erea

l

ined

ible

par

t 2

7.7×

10-1

1.

0×10

0

4.

6×10

-2

1.5×

100

4.4×

10–5

G

uille

n,20

16

Lysi

met

er st

udy

TFsf

2016

dat

a en

tries

: 2

162

4.2-1 Aridus II SF-ICP-MS (Element XR)

4.2-2 DGA-N

163

4.2-3 Fe(OH)3 CaC2O4 CaF2 n = 3

4.2-4 DGN 0.05M HNO3 Am REE (a) TEVA Am REE (b)

164

4.2-5 SF-ICP-MS Am

4.2-6 DGA-N 0.5M HCl TEVA 4M HCl Am

165

4.2-7 IAEA-soil-6 IAEA-375 NIST-4357, IAEA-385 IAEA-384 (NIST-4354) 241Am

166

4.2-8 241Am 239+240Pu 137Cs

167

4.2-9 241Am/239+240Pu 241Am 241Am/239+240Pu

168

4.4-1 NAA TMAH -ICP-MS

4.4-2 TMAH

169

4.4-3 1 TMAH 100

4.4-4 1 TMAH 100

170

4.5-1

(1-6, 27 7-10, )

171

4.5-2 Pu HNO3 -

172

4.5-3 Pu - IAEA TRS-472

4.6-1 2008 2016 Th - IAEA TRS-472 ( TF

2015-2016.2 2016.2-2016.12)

173

4.6-2 2008 2016 Am - IAEA TRS-472TF

2015-2016.2 2016.2-2016.12

4.6-3 2008 2016 Pu - IAEA TRS-472TF

2015-2016.2 2016.2-2016.12

174

14C

Pu, Am, Th Cl

TF Kd

Pu, Am, Th Cl

3

175

TF Kd

TF Kd

—TF Cs - Kd

135Cs

Cs

5.2.1. TF

TF

90Sr 137Cs

Ni, Sr, Mo Pb

Ni 3

5 Co, Zn, Cu, As, Cd

5.2.2. − TF

28 10 5 5

10 5 5

26 3

1520 TF

TF 26 28

14-18

26-28

176

5.2.3. TF

Na, Mg, Al, Si, P, K, Ca, Cr, M, Fe, Co, Ni, Cu, Zn, Sr, Cd, Ba 14-18

TF

18.4 25.3 7 TF Fe, Zn, p<0.01

Pinson 2015

TF

7 TF

37 Na, Mg, Al, Si, P, K, Ca, Sc, Ti, V, Cr, Mn, Fe,

Co, Ni, Cu, Zn, Se, Rb, Sr, Y, Zr, Nb, Mo, Cd, Sn, Sb, Cs, Ba, La, Ce, Sm, Eu, Gd, Pb, Th, UTF

20

5.2.4. Kd

20 30 Kd

10 23 Kd Kd 10 3.88×103

20 2.34×103 30 1.91×103 Kd

10 Kd 1000

30

5.2.5. Cs

27-28 Tag 5.3×10-5

1.6×10-4 m2 kg-1

137Cs

Tag 3.4×10-3 m2 kg-1 5.5×10-3 m2 kg-1 3.8×10-3 m2 kg-1 Cs

177

Tag 137Cs

137Cs 137Cs137Cs 137Cs

13C 15N

TF Tag Kd

178

14C14C 14C

14C14C

14C14C

5.3.1. 14C 14C 14C TRU

[1,2-14C] 0.5 g

4.2 × 105 Bq 14C 14C14C 4.2 × 103

Bq/mL 14C 14C14C

14C 25˚C 30˚C14C 14C

14C

5.3.2.

7

7

14CO2

14C

4 3

14C

1

5.3.3. 14C

179

14C

-

180

Pu, Am, Th Cl

14 18− TF - Kd

Pu, Am, Th Cl

Pu, Am, Th

TF

5.4.1. Am Cl 5.4.1.1. Am

DGA-N TEVA Am REEs

3SF-ICP-MS 2 20g 241Am

Am HNO3 CaC2O4 Am

Na K Mg Al Fe UTEVA + DGA-N Am

TEVA REEs Aridus (II)-SF-ICP-MS241Am Pu DF

7 105 241Am241Am ICP-MS 241Am

6241Am Am

76 82 LOD

0.012 mBq/g 241Am

16

20 241Am 241Am 239+240Pu 0.136

0.219 mBq/g

5.4.1.2. TF TMAH

TMAH H2O2 ICP-MS/MS

TF

5.4.2. -

181

26 27 20 27

10 Th 20 Th 1.4×10-5 6.7×10-4 mg/kg

/ 48 1.8×10-4

1.0×10-4 mg/kg 27 10 Th 7.7×10-5 4.7×10-4

mg/kg / 6 2.1×10-4

1.8×10-4 mg/kg Th Th /

8

Th Th Th

-

8 Pu Pu 240Pu/239Pu Pu Pu

Pu Pu - TF TF

7.0×10-6 1.1×10-4 3.1×10-5 TF-Pu

Pu TF TF-Pu

182

RI

Pu

187

+!%0 ) ( !%...* v ) îd z# :Ã ! d@kgq5 rtf kd s9q5cq3 å . e2.3-1 ra kÓ Ì Å Ì Ö..... 31 e2.3-2...

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