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English Abstracts㻌

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1S01

The forefront of diagnostic imaging

beam is mainly used for μSR in study of solid

and therapies in nuclear medicine

state physics as well as fundamental physics

KATO, K.

experiments in particle and atomic physics. A(Grad. Sch. Med., Nagoya Univ.)

new ultra slow muon beam line has been

Diagnostic nuclear medicine is as useful as

constructed in order to open a new research area

the other imaging modalities as CT, MRI andof μSR. The strong neutron beams are used for

ultrasonography. Particularly, its utilization has

developing

been expanded after the appearance of PET/CT

life-related materials. Overview of the present

and SPECT/CT. Although there are manystatus of J-PARC will be presented in order todiagnostic nuclear medicine procedures for all

encourage young and motivated people to join tothe organs, the diagnostic imaging for tumors,use the unique and useful facility.

newmaterials

and

also

for

brain and heart of actual clinical cases will bepresented in this lecture.

1A01 Neutron-induced nuclear reactions forRadionuclide therapies include

131

I internal

Cu and Nb target at 134 and 184 MeV

therapy for thyroid cancer and hyperthyroidism,

NINOMIYA, K.1, FUJIHARA, K.1, YASUI, R.1,

89

Sr (Metastron) internal therapy for pain fromOMOTO,

bone metastases, 90Y (Zevalin) internal therapy

KASAMATSU,

Y.1,

SHINOHARA,

A.1,

for

SEKIMITO,

S.2,

YASHIMA,

H.2,

brachytherapy using 125I-seeds (OncoSeed) for

MATSUMURA,

H.3,

HAGIWARA,

M.3,

prostate cancer. Besides, there are 131I-MIBG

IWAMOTO, Y.4, SATOH, D.4, SHIBATA, S.5,

internal therapy, boron neutron capture therapy

CAFFEE, M. W.6, NISHIIZUMU, K.7(BNCT) for brain tumors and malignant(1Grad. Sch. Sci,. Osaka Univ., 2Kyoto Univ.,

B-cellmelanoma,non-Hodgkin

177

neuroendocrine

lymphoma,

Lu-octreotate
tumors,153

therapy
therapy

Sm-EDTMP (Quadramet) or

223

and

for
with

T.1,

Res. Reactor Inst., 3KEK,
6

N.1,

TAKAHASHI,

4

JAEA,

5

RIKEN,

7

Purdue Univ., Univ. California, Berkeley)

Ra (Xofigo)Thedeterminationofcross-sections

byfor pain from metastatic bone tumors etc. These

neutron-induced

will be presented in this lecture.

important in the view point of space andnuclearreactionisveryplanetary sciences to investigate the history of
2S01

cosmic ray exposure. These data are alsoRadiochemistry at J-PARC

KUBO, M. K.

required for estimation of residual radioactivities(International Christian University)in accelerator facilities. However, cross section

J-PARC (Japan Proton Accelerator Researchmeasurements in the energy region > 100 MeV

Complex) is a high intensity proton beam facility,

have scarcely been undertaken because of theconsisting of three proton accelerators anddifficultylaboratories using the proton beam wheremonoenergetic

secondary particle beams of neutron, muon,

developed a method for determination of highK-meson, neutron are available. MLF (Materials

energy monoenergetic neutron cross-sections atand Life Science Experimental Facility) uses a 3

the Research Center for Nuclear Physics

GeV proton beam to produce intense muon

(RCNP), Osaka University. This method is based

beams and spallation neutron beams. The muonon two neutron irradiation experiments produced- 171 -

inobtainingneutrons.

high
Our

energygroup

has

by Li (p, n) reaction with two different angles

separator GARIS. This is the first study on

for the axis of the primary proton beam toproduction of the SHE with Z≥113 after wecorrect the contribution of the low energy

finished to study on the cold fusion reaction ofneutron reaction. In this study, high-energy

209

Bi(70Zn,n)278113 using GARIS. Although amonoenergetic neutron-induced reactions withtrigger rate of 75 cps at focal plane in the

134 MeV and 184 MeV have been studied for248

Cu and Nb targets. Excitation functions of

few cps in the 209Bi+70Zn reaction, we observed

short-lived radionuclides were determined by

5 decay chains by accumulating the beam dose

gamma-ray spectrometry. We also measuredof 4.3×1018 during a net irradiation time of 10

cross-sections by proton-induced reactions withdays. Decay characteristics of those events well

the same energy range and compared with eachagree with the precedent studies by bothother.

neutron-richDubna-Livermore collaboration and GSI SHIP

nuclides by neutron-induced reaction werecollaboration. It is rather difficult to identify thesystematicallybynuclides of the products only from the present

proton-induced reactions at the same projectile

experimental study because we measured at only

energy.

excitation energy. However, referring to theThecross-sections
larger

of

than

these

Cm+48Ca reaction was relatively higher than aassignments of the precedent studies, we could
1A02
248

Study on hot fusion reaction of48

296

Cm+ Ca→ Lv using GARISKAJI, D.1, MORIMOTO, K.1, HABA, H.1,
1

1,2

WAKABAYASHI, Y. , TAKEYAMA, M. ,
1,3

1,4

1

1

state that two of the events are attributed to the
decays of 293Lv (3n evaporation channel), and*three of them are attributed to the decays of292

Lv (4n).

1

In this report, we will give these details

HUANG, M. , KANAYA, J. , MURAKAMI,

including performance of background level and

YAMAKI, S. , TANAKA, K. , HASEBE, H. ,
1,5

M. ,

1

YONEDA,

A. ,YOSHIDA,

3

1

A. ,

transmission of GARIS for hot fusion reaction.

1,6

YAMGUCHI, T. , TOKANAI, F. , YOSHIDA,
T.1,6, GAN, Z.7, Ma, L.7, GEISSEL, H.8,
8

8

1,9

TANAKA,

T.1,9,

HOFMANN, S. , MAURER, Y. , FUJITA, K. ,Y.1,9,NARIKIYO,

1,9

10

1

1A03 Excitation functions for production of
Nb and Ta isotopes in the natZr(d,x) andnat

Hf(d,x) reactions

YAMAMOTO, S. , ASAI, M. , KATORI, K. ,MURAKAMI, M.1,2, HABA, H.2, HUANG, M.2,

MORITA, K.1,9

GOTO, S.1, KUDO, H.3(1Nishina Center, RIKEN, 2Grad. Sch. of Sci.

(1Grad. School of Sci. and Technol., Niigata

and Eng., Yamagata Univ, 3Grad. Sch. of Sci.

Univ., 2 RIKEN Nishina Center, 3Fac. of Sci.,and Eng., Saitama Univ., 4Grad. Sch. of Sci. andNiigata Univ.)

5Tech., Tokyo Univ. of Sci., Grad. Sch. of Sci.

The isotopes 95gNb (T1/2 = 35 d) and 179Ta (T1/2

and Tech., Niigata Univ., 7Fac. of Sci., Yamagata= 1.82 y) are useful radiotracers for the basic

7

8

9

Univ., IMP, GSI, Fac. of Sci., Kyushu Univ.,

chemical studies of the element 105, Db.

10

JAEA)

Previously, we investigated the production of

We searched for a superheavy element (SHE)these radiotracers by the activation of natZr andproduced
248

48

by

Cm+ CaÆ

hot296

fusionreactionof

Lv* using a gas-filled recoilnat

Hf with a 14-MeV proton beam supplied by

the RIKEN AVF cyclotron. In this work, we- 172 -

investigated the production of Nb and Ta

University Dresden)

isotopes in the deuteron-induced reactions onnat

Zr andnat

Hf.

Nuclear targets are frequently produced bymeans of the so-called molecular plating (MP)A stacked-foil technique was used for themeasurement of the excitation functions. The
nat

nat

nat

technique,whichallowsthequickelectrodeposition of the element of interest fromZr/ Ti/ Ta andan organic medium with quantitative yields. Yet

Hf/ Ti were irradiated for 30 min with

MP-produced targets are usually defective,

24-MeV deuterons supplied by the RIKEN AVF

characterized by surface cracks, and sometimes

cyclotron. After the irradiation and properwith poor structural rigidity. In order to improvecooling duration, γ- and X-rays of each foil were

the quality of the targets, constant current

measured by Ge detectors.

density MP experiments with lanthanides (i.e.,

stacks of the thin foils of
nat

nat

Nb,

mainly Nd and Sm) were carried out. Several

Y were measured in theplating parameters were varied and their effects

The cross sections of
95,97

87m,87g,88

nat

reactions,Zr, andZr(d,x)90g,91m,92m,95m,95g,96

ofon the properties of the produced deposits were

Hf wereinvestigated. It was found that by using very

Hf(d,x) reactions. The crosssmooth deposition substrates and low volatility

175,176,178,179,180g

Ta andmeasured in thenatsections of the

nat

while

those

175,179m2,180m,181

179

Hf(d,x) Ta reaction weresolvents smooth defect-free layers can bemeasured for the first time in this work, and the

produced. The performance of defect-free 147Sm

excitation function exhibits the maximum crosslayerssection of 489 ± 50 mb at 21.1 ± 0.4 MeV. For

spectroscopy experiments proved to be superior

the most of the observed nuclides, only theto that of conventional targets as shown by 15%

partial agreements were found between theincreases in relative detection efficiency. The

measured cross sections and the calculated ones

optimized MP procedure was applied also forby the TALYS-1.4 code, unlike our previous

the preparation of homogeneous large-area (i.e.,

studies of the proton-induced reactions.

42 cm2) 242Pu targets with minimum defectivity.

1A04

1A05

On the improvement of material

properties

andperformance

1,2,3

2,4

of

nuclearusedasα-particle

sourcesforInvestigation of p-process aroundmass number 140 (I) -147Sm(γ,p) reaction andits reverse process-targets
5, WIEHL N. , RUNKE J. ,KINOSHITA, N.1, SEKIMOTO, S.2, OHTSUKI,

DREBERT J.2, REICH T.2, TRAUTMANN N.2,

T.2, MASUMOTO, K.3, HAMAJIMA, Y.4,

CREMER B.6, KÖGLER T.3,7, BEYER R.3,

YOKOYAMA, A.5

VASCON A.

A.R.3,

JUNGHANSEBERHARDT

K.2,4,(1Inst. Tech., Shimizu Corp., 2Research ReactorDÜLLMANN CH.E.2,4,5

Institute, Kyoto Univ., 3Rad. Sci. Center, KEK,

(1Advanced Science Research Center, JAEA,

4

2

Kanazawa Univ.)

University

DresdenofMainz,

Institute Mainz,

Helmholtz-Zentrum
45Inst. Sci. Eng.,

Helmholtz

The p-nuclei, which are not produced by

GSI Helmholtzzentrum fürneutron capture process, exist in the present

Rossendorf,
5

3

LLRL, Kanazawa Univ.,

HZDR,
6

Schwerionenforschung, European Commission,
7

Institute for Transuranium Elements, Technicalsolar system with low abundance. Nuclear
reactions with a neutrino and charged particle- 173 -

are considered to be dominant process forsuch reactions. There are 35 stable p-nuclei

nucleosynthesis of the p-nuclei. We haveheavier than iron, located between 74Se andattempted to establish abundance of the p-nuclei

196

in mass number 130–150 using proton capture

processes of p-nuclei are proposed, for example

reactions.

nuclear(γ, n) , (p, γ) , and (νe, e−) reactions and so on,reactions on excited nuclei should be considered.

but these reactions failed to describe the present

In the present work, the (p,γ) reaction crossisotopic ratios of p-nuclei in the solar system,

Instellarenvironment,146

section on excited state of
from

147

Pm was deduced

146

Hg. Up to now, some nucleosynthesisyet. One of improvements to make is renewal
the cross section data which are necessary toSm(γ,p) Pm reaction.

Samarium samples were irradiated withperform model calculations of the p-process.
For that purpose, we measured (p, γ) and (p,bremsstrahlung with end point energies of 10–50
147

146

Sm(γ,p) Pm wasn) reaction cross sections on several p-nuclei

determined from 146Pm activity measured with aaround A = 140. Targets of 136Ce, 138Ce, andHPGe detector and bremsstrahlung spectrum

144

estimated with Geant4 code. Cross sections ofbeam at Research Center for Nuclear Physics,

MeV. Cross section of the146

Sm were irradiated with low-energy proton

Pm nuclei,

Osaka University. The experimental crossPm(p,γ) Sm reaction, were estimatedsection of 144Sm (p, γ) was determined to be awith a detailed balance theorem. The crossvalue 10 times larger than a theoreticalsections on the excited nucleus estimated from

calculation using NON-SMOKER code at thethe (γ,p) reaction agreed with those estimated bylowest energy. The deviation may make aa theoretical calculation using the TALYS code

notable difference of isotopic abundances of theat energies around 6 MeV for proton energy. We

relevant nuclei in the model calculation. We willconcluded that large correction was not required

show how the discrepancy with the calculation

due to deviation of cross sections on excitedaffects an evolution of isotopic abundance.

the reverse process on excitednamely146

147

nuclei from those on the ground state.
1A07
1A06

Investigation of p-process aroundmass number 140 (II)-(p,γ) cross section

mass number 140 (Ⅲ)-model calculation of

isotopic abundance based on proton capture
reaction-measurements on proton rich nuclei1

Investigation of p-process around

1

2

HAYASHI, K. , UENO, S. , KINOSHITA, N. ,UENO, S.1, KINOSHITA, N.2, HAYASHI, K.1,

TAKAHASHI, N.3, YOKOYAMA, A.4

YOKOYAMA, A.3(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,(1Grad. School Nat. Sci., Tech. Kanazawa Univ.,

2Inst. Tech., Shimizu Co., 3Grad. School Nat.

2

Sci., Osaka Univ., 4Inst. Sci. Eng., Kanazawa

Kanazawa Univ.)

Inst. Tech., Shimizu Co., 3Inst. Sci. Eng.,

Univ.)The p-nuclei which are unable to be produced

The majority of heavy elements which arepresent

in

the

solar

synthesizedbyneutronsystemnow

by neutron capture process exist in the present

weresolar system with low abundance. Nuclear

reaction.

reactions with neutrinos or charged particles are

However there is a group of neutron deficientconsidered to be dominant processes fornuclei, the p-nuclei, which cannot be created innucleosynthesis of the p-nuclei. We havecapture- 174 -

attempted to reproduce the current abundance of

104, Rf, we previously studied coprecipitation

the p-nuclei in mass number 130 – 150 using

behaviors of its homologous elements, Zr and Hf,

proton capture reactions. In the present work, we

and pseudo homologue, Th. In addition, we

performed a model simulation for the birth ofdeveloped an apparatus for rapid and repetitive

the p-nuclei present in the solar system.

preparation of precipitated samples. In this work,

First, we computed by using the reaction rate

we

performed

onlinecoprecipitation

isotopic abundances of Ba, Nd and Sm produced

experiments using the apparatus for the 85Zr andin s-process, which were not affected by the169

r-process. Then, we computed time variations of

AVF cyclotron at RIKEN and transported

abundances of the p-nuclei produced at (0.5 –continuously from the nuclear reaction chamber

98

Hf isotopes, which were produced with the3to the chemistry laboratory with a He/KCl

for neutron density assuming 10 – 10 g/cm forgas-jet system. Based on these results, theproton density. The NON-SMOKER code wasexperimental conditions for Rf were determined.

used for the reaction rate in the simulation.

Then, we produced 261Rf in the 248Cm(18O,2.0)×10 K for temperature and in 4×10 n/cm
2

A

long-term

6

nucleosynthesis
136

3

shows

a

138

5n)261Rf

reactionandinvestigatedits

Ce/ Ce ratio andcoprecipitation behavior with Sm hydroxide.

Ce/ Ba ratio in any temperature andCoprecipitation yields of Rf were determined as

discrepant trend between
136,138

134

proton density. In contrast, all the abundance

relativevaluestostandard

samples.

ratios of p-nuclei estimated in the work,

Coprecipitation behavior of Rf was not similar

136

138

to those of Zr and Hf but to that of Th.

144

142

136,138

Ce/ Ce,134

138

Ce/ Ba,Sm/ Nd,areexplained

well

134

La/ Ba,witha9

short-term nucleosynthesis at (1.2 – 1.5)×10 K

1A09

for temperature.

extraction apparatus for rutherfordium

1A08

Coprecipitation behavior of element

Development

a

rapid

solvent

NAKAMURA,

K.1,

YOKOKITA,

T.1,

KASAMATSU,

Y.1,

KUDOU,Y.2,

TAKAHASHI,

N.1,

YOSHIMURA,

104, Rf, with Sm hydroxide

of

T.3,

KASAMATSU,

Y.1,

TOYOMURA,

K.1,

SHINOHARA, A.1

YOKOKITA,

T.1,

SHIGEKAWA,

Y.1,(1Grad. Sch. of Sci., Osaka Univ., 2RIKEN, 3

TAKAHASHI, N.1, HABA, H.2, KOMORI, Y.2,
2

2

Radioisot. Res. Center, Osaka Univ.)

2

KANAYA, J. , HUANG, M. , MORITA, K. ,
2,3

M. ,

MURAKAMI,KIKUNAGA,

4OHTSUKI,T. ,SHINOHARA, A.

TAKAMIYA,

far,mainlysolid-liquid

extraction

H. ,experiments have been performed in solution

5chemistry on superheavy elements. It is difficult

6

to apply solvent extraction to short-lived

MITSUGASHIRA, T. , YOSHIMURA, T. ,
6

So

4

K. ,

1

superheavy elements because rapid equilibration

1

2

3

( Grad. Sch. Sci., Osaka Univ., RIKEN, Grad.
4

Sch. Sci., Niigata Univ., Res. Center Elec.
5and phase separation are needed to determine the
distribution ratios (D) of superheavy elements.

Radioisot. Res.

In this study, we developed a rapid extraction

Center, Osaka Univ., Res. Reactor Inst., Kyoto

apparatus named “Flow Injection Extractor

Univ.)(FIE)” and phase separator to accomplish the

Photon Sci., Tohoku Univ.,
6

For coprecipitation experiment on element

solvent extraction and phase separation within- 175 -

the lifetime of 261Rf (68 s).

by proton bombardments on natZr and natHf

FIE is a flow-type extraction apparatus andconsists of a Teflon tube filled with Teflon beads.
88

Solvent extraction of Zr and175

Hf (homologues

metallic foil targets, using the AVF cyclotron at
RIKEN

and

TohokuUniversity.

Theseradiotracers were chemically isolated by anof Rf) was performed using 7.8-11.3 M

ion-exchange

method.

hydrochloric acid as aqueous phase and 0.01 M

dissolved in 600 μL of 0.01-27 M HF solution

Aliquat 336 benzene or carbon tetrachloride

and then mixed with the same volume of 10-4 M

solution as organic phase. Two phases passed

Aliquat 336 in 1,2-dichloroethane solutions in athrough FIE and then the mixture was collected

tube. After shaking the solutions for 5 min, andin a test tube. The two phases were separately

centrifuging for 5 min, the two phases were

pipetted in tubes after centrifugation and wereseparately pipetted into sample tubes. The

subjected to gamma ray measurement. The D

radioactivities

values were determined from the gamma ray

measured with a Ge detector. Distribution ratios

counts. The D values determined with FIE were(D) were obtained from the ratio of theconsistent with those in equilibrium. This means

radioactivities in the two phases.

of

The

the

tracerstwosamples

were

were

that extraction equilibrium was achieved within

As the result, while the maximum D value of

1 min by using FIE. In addition, we developed a

Ta was obtained in 0.27 M HF, that of Nb

flow-type phase separator using a PTFE filter.

decreased

We found that separation with the purity of eachconcentration from 0.01 M to 27 M. This

phase of higher than 95% was achieved with asuggests that there were clear differences

1-step separator.

between the chemical form species of Nb andgraduallywithincreasing

HF

Ta.
1A10

Extraction behavior of Nb and Ta
1A11 On-linewith Aliquat 336 in HF solution
1

reversed-phase

2

SATO, D. , MURAKAMI, M. , HABA, H. ,chromatography of group-5 elements, Nb and

KIKUNAGA, H.3, OOE, K.1, GOTO, S.1,

Ta, for the chemical experiment of dubnium

KUDO, H.

1,2

4

(Db)

1

( Graduate School of Science and Tecnology,

TSUTO, S.1, MURAKAMI, M.1,2, OOE, K.1,

Niigata Univ., 2Nishina Center for Accelerator

GOTO,

Based Science, RIKEN., 3Research Center for

KOYAMA, T.1, NAGAOKA, T.1, MOTOYAMA,

Electron

R.1, HABA, H.2, KOMORI, Y.2, TOYOSHIMA,

PhotonScience,TohokuUniv.,

4

S.1,

SATO,

D.1,

GOTO,

N.1,

Department of Chemistry, Niigata Univ.)

A.3, KITAYAMA, Y.4, FUKUDA, Y.4, KUDO,

We are planning to investigate the chemical

H.1

properties of Db. In this experiment, ion-pair(1Niigata Univ., 2RIKEN, 3JAEA, 4Kanazawa

extraction of Nb and Ta, which are the lighter

Univ.)

homologs of Db, with quaternary ammonium

We have studied the solvent extraction andsalt (Aliquat 336) from HF solutions is carried

reversed-phase extraction behaviors of Nb andout to study complex formations of theseTaelements with fluoride ions.

hydrofluoric acid solutions for the chemicalRadiotracers,

95g

Nb and179

Ta, were produced

withtributylphosphate

(TBP)

from

experiment of dubnium (Db). Since these results- 176 -

showed that the extraction behavior of Ta is

cyclotron. Nuclear reaction products werequite different from that of Nb, it is interesting torapidly transported with a KCl/He gas-jet system

carry out chemical experiment of Db in thistoexperimental condition. In this study, we

TTA-chromatographic behavior of Rf in acidic

performed

reversed-phase

HF/HNO3 solution was investigated with anchromatography of Nb and Ta with Automatedon-line automated chemistry-apparatus (ARCA)

Rapid Chemistry Apparatus (ARCA), using

andon-line90g

Nb and178

thechemistryalpha-particle

laboratory,andmeasurement

thensystemTa produced(RIDER). As a preliminary result, 17 counts

at the RIKEN AVF cyclotron. The reaction(7.82-8.38 MeV) and 10 counts (7.82-8.38

products transported by a He/KCl gas-jet system

MeV) of 261Rf and its daughter 257No were

were dissolved in 1 M HF at a flow rate of 1

observed in the 1st and 2nd effluent samples,mL/min. The solution was fed into the extraction

respectively, under an elution condition ofcolumn of ARCA filled with 62-wt. % TBP resin,

6×10-4 M HF/0.01 M HNO3. This demonstrates

and the effluents were collected in plastic tubes.

that a cationic complex of Rf is formed in the

These samples were then subjected to γ-ray

solution and is extracted into the TTA-resin

spectrometry using a Ge detector. Niobium wasunder the present conditions. In the symposium,

not adsorbed on the TBP resin, while Ta wasadsorption probability of Rf onto the resin willretained. The present results are consistent withbe discussed in detail by comparing with those

those obtained in our prior batch experiments.

of Zr and Hf.

short-lived isotopes of

We will carry out the on-line experiment of Db.
1A13
1A12

Adsorption behavior of a superheavy

element

Rfbya

TTA-reversed-phasetheStudy of mass asymmetric fission of

193

Ir

TAMURA, N.1, HIROSE, K.2, NISHIO, K.2,

chromatography method

NISHINAKA, I.2, MAKII, H.2, ORLANDI, R.2,

KITAYAMA, Y.1, FUKUDA, Y.1, TSUKADA,LÉGUILLON,

R.2,

SMALLCOMBE,

J.2,

K.2,

A.3,

OHTSUKI,

T.4,

TOYOSHIMA,
H.4,

KIKUNAGA,

A.2,

HABA,

H.3,

ANDREYEV,MURAKAMI,

M.3,5,TSEKHANOVICH, T.5, OOE, K.1, GOTO, S.1,

HUANG, M, H.2, TANIGUCHI, T.1, UENO, S.1,

KUDO, H.6

HAYASHI, K.1, YOKOYAMA, A.6(1Grad. Natural Science Niigata Univ., 2 Japan(1Grad. School Nat. Sci. Tech, Kanazawa Univ.,

Atomic Energy Agency, 3York Univ., 4Kyoto

2

Univ., 5CENBG, 6Niigata Univ.)

3

JAEA,

RIKEN,

4

Reserch Center for Elec.

Photon Sci., Tohoku Univ., 5Grad. School Sci.,
6

Niigata Univ., Inst. Sci. Eng., Kanazawa Univ.)
We

study

In the nuclear fission, mass distribution offission fragments changes with the fissioning

reversed-phase-chromatographic

nucleus systematically, that is, an asymmetricelement,

mass distribution appears in many actinide

Rutherfordium (Rf) with TTA as an extractant tonuclides while lighter nuclides lead to aclarify chemical properties of its cationicsymmetric fission. The cause of the asymmetricbehaviorofasuperheavy

261

Rf with ais that one fragment can easily become the248

Cm( O,

nucleus in the neighborhood of 132Sn which is5n)261Rf reaction at the RIKEN K70 AVF

the doubly closed shell nuclide. On the otherfluoride-complex. A nuclide ofhalf-life of 68 s was produced in the18- 177 -

hand, in the case of a fission of a lighter nucleus,

Tc-99m were precisely measured with various

the nuclear fission such as liquid drop comeschemical state to investigate the effects ofdominant.

chemical states on the decay constants of

It is expected that the mass distribution for the

nuclides. As a results, the difference of the decay

fission of 180Hg is symmetric because 90Zr hasconstants between the two chemical forms,

the neutron magic (N = 50) and the proton

pertechnetate(VII) and hexachlorotechnetate(IV),semimagic (Z = 40). In the beta-delayed fission

is obtained on the order of magnitude of 0.1%.

180

Tl,

mass

This indicates that the variation of the decay

distribution was observed by Andreev et al. This

constants of Tc-99m is affected by the difference

phenomenon is a new type of asymmetric fissionof the ligands rather than that of the oxidationand may not be caused by strong shell effects ofstate of Tc.

ofhowever,anasymmetric

the fragment, as observed in the actinide region.
Much theoretical investigation has been

1A15

Performance test of a gas-filled recoil

performed since this discovery. According to one

separator GARIS-II for asymmetric fusion

result, existence of a unique asymmetry fission

reactionsmode was predicted in the region of neutron-rich

KAJI, D.1, MORIMOTO, K.1, HABA, H.1,

nuclei around iridium and tungsten. We took

WAKABAYASHI, Y.1, TAKEYAMA, M.1,2,

note of this prediction and carried out the

YAMAKI, S.1,3, TANAKA, K.1,4, HUANG, M.1,

experiments to find out a new asymmetric

KANAYA, J.1, MURAKAMI, M.1,5, ASAI, M.6,

fission mode. In the presentation, we would like

MORITA, K.1,7

to talk about the results of the experiment in the(1Nishina Center, RIKEN, 2Grad. Sch. of Sci.

reaction of 7Li + W.

and Eng., Yamagata Univ, 3Grad. Sch. of Sci.
and Eng., Saitama Univ., 4Grad. Sch. of Sci. and

1A14

Variation measurements of decay

Tech., Tokyo Univ. of Sci., 5Grad. Sch. of Sci.

constants of Tc-99m as a chemical tracer

and Tech., Niigata Univ., 6JAEA, 7Fac. of Sci.,

KIKUNAGA, H.1, TAKAMIYA, K.2, OHTSUKI,

Kyushu Univ.)T.

2

We have developed a new gas-filled recoil ion

1( Res. Center for Elec. Photon Sci., Tohoku

separator GARIS-II to study on asymmetric

Univ., 2 Res. Reactor Inst., Kyoto Univ.)

actinide-target based fusion reactions (hotThe decay constants of some nuclides which

fusion). It will be used as a powerful tool for a

decay via the internal conversion process are

new superheavy element (SHE) search withchanged with changing environmental factors

Z≥119, SHE chemistry, studies on nuclear

such as its chemical states. Example of this typereaction and nuclear structure of SHE nuclide,of nuclides is metastable state of Tc-99 (Tc-99m).

and a direct mass measurement of SHE nuclide.

Therevariation

The first quadrupole magnet of GARIS-II for

measurement of the decay constants withvertical focusing is important role to increase aradiation detection is able to use a chemicalsolid angle of the separator. Therefore, thetracer. In this study, an apparatus for precise

separator is expected to have a high transmission

measurement of the decay constants wasfor a hot fusion. We have already tested thedeveloped at first. The decay constants ofseparator using a standard α-source of 241Am andispossibility

that

the

- 178 -

40

Ar-induced fusion reactions to evaluate theefficiency of an atom depends on its IP. To

separationfromobtain a relationship between IP and ionization

background particle and its transmission. These

efficiency in present system, we measured

reaction products were properly collected onto

ionization efficiencies of short-lived isotopes,

the focal plane detection system with high80

efficiency under extremely low background

153,154

capabilityof

GARIS-IIRb, 157Er, 162Tm, 168Lu, 142,143Eu, 143mSm, 148Tb,
Ho,

165

Yb, andnat

11

Ge+ B,

49

Cr produced in the151

Eu/156Gd/162Dy+11B,

condition. As a next step, on-line operating test

reaction ofof GARIS-II was performed using more136

asymmetric 22Ne-induced fusion reactions of

Ionization efficiency of 257No produced in the

197

248

He-H2 mixture as a filled gas of the separator for

Measured ionization efficiency of 257No was

the first time. In this report, we will talk about

0.8 %, which yields IP value of No to be 6.6 eV.

status of GARIS-II R&D and give the results

This value is in a good agreement with the value

Au and 208Pb. In this work, we tried to use

obtained from studies on

22

Ne-induced fusion

Ce/141Pr/159Tb/141Nd/147Sm+11B, and 45Sc+11B.
Cm(13C, 4n) reaction was also measured.

which has been evaluated by extrapolation fromreaction in detail.

those of the lighter actinide elements, 6.65 eV.

1A16

1A17

Measurement of the first ionization

potential of nobelium (No, Z=102)
1

Electrolytic reduction of Mo and W aslighter homologues of seaborgium (Sg)
1,2

SATO, T. K. , ASAI, M. , KANEYA, Y. ,TOYOSHIMA, A.1, MIYASHITA, S.2, OOE, K.3,

TSUKADA, K.1, TOYOSHIMA, A.1, VASCON,KITAYAMA, Y.4, LERUM, H. V.5, GOTO, N.3,

A.1,

A.1,2,

KANEYA, Y.1,6, KOMORI, Y.7,8, MITSUKAI,

NAGAME, Y.1, ICHIKAWA, S.1,4, MAKII, H.1,

A.1,6, VASCON, A.1, ASAI, M.1, SATO, T. K.1,

OSA, A.1, SAKAMA, M.3, OOE, K.5, SATO, D.5,

TSUKADA, K.1, KITATSUJI Y.1, NAGAME,

SCÄDEL, M.1, KRATZ, J. V.1,6, STORA, T.7

Y.1, SCHÄDEL, M.1, ATTALLH, M. F.5,

(1JAEA,

2

Ibaraki Univ.,

3

Tokushima Univ.,

GUPTA, N. S.5, OMTVEDT, J. P.5, TSUTO, S.3,

4

5

6

OSHIMI, Y.3, KOYAMA, T.3, TANAKA, A.3,

TAKEDA,

RIKEN,

1

S.1,3,

Niigata Univ.,

MITSUKAI,

Univ. of Mainz,

7

CERN)

SATO, D.3, KASAMATSU, Y.8, YOKOKITA,

The first ionization potentials (IPs) of heavy

T.8, SHIGEKAWA, Y.8, SHINOHARA, A.8,

elements with atomic number Z > 100 have not

KOGA, K.2, KANEKO, M.2, YOKOYAMA, A.4,

been measured due to the short half-life and the

HABA, H.7, HUANG, M.1,7, KRATZ, J. V.9,

low production rate of the isotopes. In order to

PERSHINA, V.10

determine the IP of the heavy elements, we have

(1JAEA,developed a novel measurement method based4

on a surface ionization technique by using a

7

2

Hiroshima Univ.,

3

Niigata Univ.,

5

Kanazawa Univ., Oslo Univ., 6Ibaraki Univ.,
RIKEN, 8Osaka Univ., 9Mainz Univ., 10GSI)

surface ionization ion source coupled to a

We have been studying extraction and

He/CdI2 gas-jet transport system for an Isotope

reduction behavior of Mo and W as preparatory

Separator On-Line (ISOL) at the JAEA tandem

experiments of a reduction of their heavier

accelerator facility. In this work, we havehomolog, seaborgium (Sg). In this study, we

determined IP value of No by using the method.

searched for the reduction conditions from 6+ toIn a surface ionization process, an ionization

4+ ions of Mo and W and the separation ones

- 179 -

between the 4+ and 6+ ions which are required

because the pyrite ratios were higher in thefor our future on-line experiment of Sg. In

seabed.

experiments,

wereduction of

93m

carriedelectrolytic

The values of Th/U and Ce/U ratios obtained

W radiotracers

from INAA were larger in the upper layers at

produced at the JAEA tandem accelerator inboth sites. Therefore, we concluded that thesuch as H2SO4/HClO4 solution. This was thensedimentary environment of the upper layers isfollowed by solvent extraction with TOA to

more oxidative than that of the lower layers.

identify the reduction of these elements on a

Since the U(VI)/U(IV) ratio was lower in the

tracer scale. Results showed that Mo is reduced

seabed, it is thought that the sedimentaryin H2SO4/HClO4 at around < -0.4 V while W isenvironment was more reductive there, which is

not reduced between 0.4 V and -1.4 V. In theconsistent with the results of the Mössbauer

presentation, details of the reduction andmeasurements.

Mo andout
176extraction of Mo and W are reported.

Results

obtained

spectroscopy

of

from

pyriteMössbauer

content

proved1B01 Evaluation of Redox Conditions atcomparable to those obtained by INAA.

DredgedbyHowever, using both in conjunction allows for

Neutronincreased precision in estimation of redox

Trenches

Mössbauer

in

Tokyo

Spectroscopy

and

Bay

potential in sediment.

Activation Analysis
1

T. ,YAMAGATA,SHOZUGAWA,

2

1

K. ,

2

OKUMURA, R. , TAKAMIYA, K. , MATSUO,
M.

1assembled1( Graduate School of Arts and Sciences, Univ. ofTokyo,

1B02 Difference of spin state in anion-mixed2

Research Reactor Institute, Kyoto

crystalsbridgedby

1,2-bis(4-pyridyl)ethane
DOTE, H.1, NAKASIMA, S.2(1Grad. Sch. Sci., Hiroshima Univ., 2N-BARD.,

Univ.)In this study, the redox conditions at two

Hiroshima Univ.)

dredged trenches in Tokyo Bay were evaluated

New anion-mixed complexes using KNCS

for severe hypoxia, which has been observedand NaNCBH3 having iron as metal andevery summer. The concentrations of U, Th, Ce,

1,2-bis(4-pyridyl)ethane as bridging ligand wereFe, and Mn in Tokyo Bay sediments weresynthesized. These complexes have a trend tomeasured by instrumental neutron activation

have more NCS than the fraction as synthesized.

analysis (INAA). The chemical states of iron

Powder X-ray diffraction pattern shows ( 2 0 -2 )57

were analyzed by Fe Mössbauer spectroscopy.

and ( 1 1 -2 ) diffraction, shifting to higher

In the Mössbauer spectra of the sediments,

degree with increasing fraction of NCS. All the

pyrite was detected in middle and lower layers

Mössbauer spectra basically consist of twoof a dredged trench and in all layers below the

doublets, outer and inner doublets. Q.S. value of

surface of the non-dredged seabed. Therefore,

outer doublet changes depending on the anion

both sites can be considered reductive, thereby

fraction. The values are relatively similar to thefostering pyrite generation. The sedimentary

original pure anion complexes. On the otherenvironment

more

hand, Q.S. value of inner doublet is independent

reductive in the seabed than in the trenchesof anion fraction, but the origin is unknown.

wasconcludedtobe- 180 -

There is a possibility of mixed complex having

observation. Very recently, new-type crystals

one NCS and one NCBH3 as counter anion,

havingalthough Q.S. of the iron with one NCS and one

Fe3O(C6F5COO)6(C5H5N)3·CH2Cl2 was obtained

NCBH3 is expected to have larger value. While

by a very slow recrystallization from a

the

by

dichloromethane solution. A powder X-ray

1,3-bis(4-pyridyl)propane did not show thediffraction showed a different diffraction pattern

spectrum having one NCS and one NCBH3. The

to that of the hexagonal crystals, suggesting a

difference

1,2-bis(4-pyridyl)ethane

polymorph. The new polymorph could becomplex and 1,3-bis(4-pyridyl)propane is also

assigned to orthorhombic from the XRD pattern.

unknown.

anion-mixed

complexes

betweenMixed

bridgedthesamechemicalformulacomplexes

includingTemperature-dependent Mössbauer spectra of

wereobtained.

the new-type complex showed that the iron

Mössbauer spectra revealed more low-spin state

valences were in the trapped state in a widecompared with the sum of low-spin state in eachtemperature range from 78 to 300 K, inpure complex.

remarkable contrast to the hexagonal one.

1,4-dichlorobenzene

also

1B03 Synthesis

andMössbauer

Spectroscopic

Observation

of

1B04

Determination of Formation Energyof Oxygen Vacancies in Zinc Oxide Doped

Valence-trapping and Detrapping of two

with Al and In Impurities

Polymorphs of Mixed-valence Trinuclear Iron

KOMATSUDA, S.1,SATO, W.1,2, OHKUBO, Y.3

Pentafluorobenzoate complex(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,

OGISO, R.1, SAKAI, Y.1, ONAKA, S.1,

2

T.2,1,NAKAMOTO,

M.3,

TAKAHASHI,

1

Inst. Sci. Eng., Kanazawa Univ., 3Res. Reactor

Inst. Kyoto Univ.)

4

TAKAYAMA, T. , OZEKI, T. , KOBAYASHI,
Y.

5

The

time-differential

perturbed

angularcorrelation method was applied to a study of

1

2

3

111

In(→111Cd) probe in( Daido Univ., Toray Res. Cent., Toho Univ.,

local fields at the

4

Nihon Univ., 5Tokyo Inst. Tech.)Al-doped ZnO. In one of our previous TDPAC

We have studied behaviors of iron-valence

studies, we observed contrasting atmospheretrapping

anddetrapping

phenomenon

mixed-valence

trinuclear

ironcomplexes.

incarboxylate

dependence of the stability of aggregations of111

In and Al impurities doped in 100 ppm

In our previous Mössbauer work,

Al-doped ZnO: (i) Al and In impurities associate

it was revealed that three iron ions inwith each other by their thermal diffusion in air,

3+

3+

Fe Fe Fe O(C6F5COO)6(C5H5N)3·CH2Cl2 areand (ii) the 111In probe is detrapped from the Al

inaggregations

the

2+

valence-trapped

state

in

lower

in

high-temperature

vacuum,temperatures, while in the valence-detrapped

resulting in substitution at defect-free Zn sites.

state in higher temperatures, the transition

Furthermore, it is suggested from anothertemperature being around 80 K. A single-crystal

TDPAC measurement for 100 ppm Al-doped

X-ray diffraction analysis at 123 K revealed that

ZnO annealed in Ar gas that the local association

this mixed-valence complex crystallized in aof Al and 111In becomes unstable in anaerobic

hexagonal system and three iron atoms were

atmosphere due to the formation of oxygen

equivalent in consistent to the Mössbauer

vacancies in the sample. In order to provide- 181 -

further insight into the dissociation mechanism,

then performed at various temperatures down toin the present work, we analyzed TDPAC

room temperature.

spectra for 100 ppm Al-doped ZnO prepared on

All the TDPAC spectra show exponential

various heat-treatment conditions, and foundrelaxationthat the relevant atmosphere dependence of theascribable to hopping motion of Ag+ ions. It is

impurity behaviors provides a helpful clue to theconsidered that the PVP-coating has made it

dissociation

possible for the α phase to survive even at roommechanism

triggeredbythereflecting

temperature.

formation of oxygen vacancies.

We

dynamic

herereportperturbation

successful

atomic-level observation of room-temperature
Dynamics of 111Ag in a superionic

1B05

activation energy of the local dynamics.

conductor AgI
1, 2, 3

SATO, W.

dynamic motion of Ag+ ions, and discuss the23, MIZUUCHI, R. , IRIOKA, N. ,KOMATSUDA, S.2, KAWATA, S.4, TAOKA,
1,2

A. , OHKUBO, Y.

5

1B06 Medical Radioisotope Production withAccelerator Neutrons by 40 MeV Deuterons

1

2( Inst. Sci. Eng., Kanazawa Univ., Grad. School

TSUKADA, K.1, SATO, N.1, WATANABE, S.1,

Nat. Sci. Tech., Kanazawa Univ., 3School Chem.,

ISHIOKA,

Kanazawa Univ., 4Dep. Chem., Fukuoka Univ.,

HASHIMOTO, K.1, KIN, T.1, KAWABATA, M.1,

5

SAEKI, H. 1, NAGAI, Y. 1

Res. Reactor Inst., Kyoto Univ.)
Silveriodide(AgI)

offerssuperionic

conductivity expected for future technological

N.

S.1,

HATSUKAWA.

Y.1,(1JAEA, 2Dep. of Engineering Sci., Kyushu
Univ.)

This conducting phenomenon,

A new system has been proposed for the

however, emerges only in its high-temperature α

generation of radioisotopes with accelerator

phase (≥ 420 K), which has long been a barrier

neutrons by deuterons, especially the production

to practical applications of this compound.

of 99Mo (T1/2 = 66 h), 90Y (T1/2 = 64 h),

Recently, an epoch-making technique overcame

67

this

Enriched

applications.

situation:

AgI

powdercoatedbyCu (T1/2 = 61.8 h), and 64Cu (T1/2 = 12.7 h).
100

Mo,

90

Zr,

68

Zn and64

Zn oxidepoly-N-vinyl-2-pyrrolidone (PVP) can partiallysamples were irradiated with neutrons, which

preserve the conducting α phase even at room

were obtained by the natC(d,n) and Be(d,n) using

temperature. For detailed understanding of the

40 MeV deuterons provided from the TIARA

low temperature conductivity, in the present

cyclotron.

+

work, local dynamics of Ag

99

Mo,

90

Y,

67

Cu, and64

Cu wereions wassuccessfully produced via the (n, x) reactions,investigated by means of the time-differential

and we clearly observed the γ-rays. Particularly,

perturbed

yields of impurity radionuclides were muchangulartechnique using theThecorrelation(TDPAC)111

smaller than that of 99Mo and 67Cu, and therefore

Ag(→ Cd) probe.
anradioactive waste produced during chemicalanion-exchange chromatography from Pd matrix

processing would be reduced compared with

irradiated with thermal neutrons in KUR. The

other proposed reaction systems. The present

isolated

probe

111

was

separatedby111

Ag was then incorporated in AgI

results demonstrate that the radioisotopes, 99Mo,

powder when it was synthesized by precipitation

90

Y, 67Cu, and 64Cu, can be produced by usingwith PVP powder. TDPAC measurements were

fast neutrons, and strongly suggest that the- 182 -

reaction system is one of the most promising

S.1, NAGAI, Y.1, WATANABE, S.2, ISHIOKA,

routesS. N.2

toproducehighquality

medical(1Nuclear Engineering Research Collaboration

radioisotope.

Center,
1B07 Production and utilization of astatine
7

AtomicEnergyAgency,2

Quantum Beam Science Center, Japan Atomic

Energy Agency)

and iodine radioisotopes using Li ion beams
1

Japan

2

A. ,

Copper-67 is an attractive radionuclide for

WASHIYAMA, K. , AMANO, R. , MAEDA,

cancer therapy, because of emissions of medium

NISHINAKA,

I. ,YOKOYAMA,

3

3

4

4

4

energy beta particle (a mean energy of 141 keV)

WATANABE, S. , SUZUKI, H. , ISHIOKA, N.

and gamma rays (91, 93, 185 keV) suitable for

E. , TANIGUCHI, T. , MURAKAMI, K. ,
1

1

1

1

S. , HASHIMOTO, K. , MAKII, H.

imaging, and its appropriate half-life (62 hours).

Inst. Sci. Eng. ， Kanazawa Univ.,

However, the use of 67Cu for clinical researches

College Med. Pharmaceutical and Health Sci.,

has been limited due to the difficulty in

1( JAEA,
3

1

2

4

Kanazawa Univ., Grad. School Nat. Sci. Tech.,obtaining sufficient quantities. In this study, weKanazawa Univ.)

have investigated the production of 67Cu by the

In general, an α-emitter 211At which is a68

Zn(n,x)67Cu reaction (x=n’p, d) using fast

prospective candidate for utilization in targeted

neutrons from natC(d,n) reaction. The highly

alpha radiotherapy is produced through thepurified 67Cu was obtained by the two columns

209

In contrast, ourseparation method (chelate resin chelex-100 andproject is focusing on the production in theanion exchange resin AG1-X8). Furthermore,209

the labelling of DOTA and TETA which are

Bi(4He,2n)211At reaction.
7211

Bi( Li,5n) Rn reaction. This enables us to211

supplyAt in aThe daughter
from

the

211

211

211

Rn/ At generator system.

useful bifunctional ligands for the labelling

At (7.2 h half-life) is extracted

monoclonal antibodies was succeeded in more211

parentRn(14h),

expanding
211

time-frame for transportation and use ofthan 97% yield.

At.

To use astatine and iodine radioisotopes in our

1B09

Preparation ofproject,

theexcitation

functionsoftreatment

209

216-x

nat

nat-x

and

HAYASHI,

7

Bi( Li,xn)

Rn,

7

Pb( Li,xn)

At

Sn(7Li,xn)nat-xI reactions have been measured.

Y.1,

191

Pt for cancer

TAKAHASHI,

N.1,

nat

YOSHIMURA, T.2, IKEDA, H.3, WATABE, T.3,

In addition to that, separation techniques have

KANAI,

been developed. We report not only on the

SAKABAYASHI, K.4, OGAWA, K.5, ODANI,

production and separation of astatine and iodine

A.5, SHINOHARA, A.1

radioisotopes in the reactions but also on the(1Grad. Sch. Sci., Osaka Univ., 2Radioisotope

utilization of those radioisotopes.

Res. center, Osaka Univ., 3Grad. Sch. Med.,Y.3,

HATAZAWA,

J.3,

Osaka Univ., 4Sch. Pha., Kanazawa Univ., 5Grad.
1B08 Production

of

67

Cu

for

Therapy Using Fast Neutrons from

Cancer

The platinum-based anticancer agent likeC(d,n)

cisplatin

Reaction
1,2

1

HASHIMOTO, K. , KAWABATA, M. , SAEKI,
1

Sch. Pha., Kanazawa Univ.,)

nat

1

1

H. , TSUKADA, K. , SATO, N. , MOTOISHI,

is

one

of

the

most

importantcarcinostatic, because of its broad spectrum
anticancer activity. However, it is difficult to- 183 -

produce RI-tracer of Pt, and the biodistribution

211

of these drugs are still unknown. Then we aim towith 8M HCl (99%), but decreased when using

191

make the establishment of preparation of

At on AG 1x8 was high when loading 211At

Pt

boric buffer. Low capture efficiency wasand visualize the uptakes of platinum-based

observed when AG MP-50 was used. High

anticancer drug. In this work, we investigate thecapture efficiencies (96-99%) were obtained

191

nat

Pt(p, xn) reaction with

with PEG-coated resin. Low recovery efficiency

46 - 60 MeV proton beam from AVF cyclotron(~6%) from AG 1x8 was obtained using strongat Research Center for Nuclear Physics.

base solution. On the other hand, 211At was

Furthermore, several method to purify 191Pt withrecovered from PEG-coated resin in goodliquid-liquid extraction was tested, and we

efficiency

production of

Pt viaobtained high radio specific activity

191

contained

impurities.

littleradioactive

Additionally, we synthesized

191

Pt whichPt-cisplatin, and(60-79%)

when

using

NH4OH

solution as eluent. These studies demonstrated
that PEG-coated resin could be used to isolate
211

At from a Bi target.

observed the biodistribution of it in mice at the 1
and 24 h time point (each n = 4). This work
indicates that our preparation method of

191

Pt is

available for medical use.

1B11 Evaluation of radon trapping anddaughter recovery in organic solvent based
system
MAEDA, E.1, WASHIYAMA, K.2, YAMADA,

1B10 Isolation of 211At from an irradiated Bi

N.1, TANIGUCHI, T.1, MURAKAMI, K.3,

target using a wet chemistry approach

AMANO, R.2, NISHINAKA, I.4, YOKOYAMA,WATANABE, S.1, BALKIN, E.R.2, HAMLIN,

A.3

D.K.2,(1Grad. School Nat. Sci., Tech. Kanazawa Univ.,

GAGNON,

K.3,

CHYAN,

M.-K.2,2WILBUR D.S.2
1

2

3( JAEA, Univ. of Washington, Univ. of Albata)211

At (Half-life: 7.21 h) is one of thepromising radionuclides for targeted alphaSch. of Health Sci., College of Med., Pharma.

Health Sci., Kanazawa Univ., 3Inst. Sci. Eng.,
Kanazawa Univ., 4ASRC, Japan Atomic Energy
Agency)Radon-211(211Rn), a noble gas radionuclide istherapy. Dry distillation has been widely used toisolate

211

At

from

a

Bi

Poor

a promising for supply an alpha emitting

reproducibility of recovery yield in the dry

radionuclide astatine-211(211At), which has been

distillation led us to employ a wet chemistry

used for targeted alpha therapy in nuclear

approach. High and stable recovery yield

medicine, as a 211Rn/211At generator system. To(~78±11%) was accomplished by the approach.

make a suitable design of generator system, we

However, the use of diisopropylether (DIPE) inchoose wet chemistry and solvent extraction

the isolation process has made it difficult tomethods to collect 211Rn and retain it in an

automatetheprocess

appropriate solvent to ingrowth of 211At. In this

Therefore,

we

have

due

target.

tomiscibility.
columnstudy, we evaluate trapping yield of 211Rn in

methods to simplify the isolation of 211At. Anion

several organic solvents (such as DIPE, MIBK,

exchange resin (AG1x8), cation exchange resin

toluene, hexane, decane, dodecane), and also

(AG MP-50), and polyethylene glycol (PEG)

evaluated back extraction yield of211

methanol. The trapping yields of211

investigatedcoated resin were used. The capture efficiency of- 184 -

At in

Rn in

organic solvents were ca 70-90% and there

the U(V) complex was obtained. In the case of

seems no correlation in each selected solvent.

U(V),The back extraction yields of

211

two

geometricalisomers,a

At in methanol

square-antiprismatic (2a) and a dodecahedral

15 hour after ingrowth in hexane, decane,(2b) structures, tautomerized. The equilibrium

dodecane were ca 20-30%.

constant defined as [2b]/[2a] was 6.5 in CH2Cl2.
This indicates that the more stable structure of

1B12 Conversion of Stable Geometrical

U(V) complex is the dodecahedral structure,

Isomers between Pentavalent and Tetravalent

unlike in the case of the isomorphic U(IV)

Uranium

complexes.

Complexes

with

Salophen-type

LigandMORIMOTO,

K.1,

NAKATSUKA,

1

K. ,

YOSHIMURA, T.

MATSUDA,

K.1,

SHINOHARA,

1

A. ,

2

1B13 Complexation

177

Lu

of

with

bifunctional chelators in the presence ofcompeting metals

1( Graduate School of Science, Osaka Univ.,

WATANABE, S., HASHIMOTO, K., ISHIOKA,

2

Radioisotope Research Center, Osaka Univ.)

N. S.

Our

group

recentlysynthesized

the(JAEA)
As part of basic studies for the production ofeight-coordinated dodecahedral U(V) complex
ligands

177(N,N’-(1,2-phenylene)bis(5-methyl-2-hydroxybe

177

nzylidenimine)) by the one-electron oxidation ofN´´´-tetraacetic acid (DOTA)-antibody, 177Lu

the eight-coordinated square-antiprismatic U(IV)complexation

complex.

diethylenetriamine-N,N,N´,N´´,N´´-pentaacetic

withsalophen-type

In the present study, we investigatedLu

capableoflabelingof

Lu-1,4,7,10-tetraazacyclododecan-N,N´,N´´,
of

DOTA

and

in detail about the structural transformation byacid (DTPA) was investigated in the presence ofoxidation of the uranium center.

competing metals: Mg, Cu, and Yb in addition to

A brown precipitate of the U(IV) complex

Ca, Fe, and Zn. The inhibition of

177

Lu

was obtained by the reaction of UCl4 with 2 eq.

complexation by the competing metals was inof salophen-type ligand. When the precipitate

the order of Mg, Ca < Fe < Yb < Cu, Zn and Mg,

was recrystallized from THF, platelet (1a) andCa < Zn < Fe < Cu < Yb with DOTA and DTPA,

block

respectively. Consequently, the elimination of(1b)

crystalswereobtained.

The

177

Lu final solution

single-crystal X-ray structure analysis revealed

Mg and Ca from the

that

a

produced was not found to be necessary, whilesquare-antiprismatic structure, and that in 1b is athe elimination of Cu, Fe, Zn and Yb fromdodecahedral

the177Lu final solution was found to betheuraniumiongeometry.

in
These

1a

is

structures

tautomerized in solution, which was studied bynecessary.

the change in redox waves of 1a and 1b. The
equilibrium constant defined as [1b]/[1a] was
0.082

in

CH2Cl2.

Therefore,

a

2A01

Determination of antistatic properties

of non-woven fabrics of protective clothingsquare-antiprismatic structure was more stable inwith

the U(IV) isomers.

radioactive radon daughters

When 1a was chemically oxidized in CH2Cl2,- 185 -

measurementof

α-particles

fromICHIHARA, C.1, MISAWA, T.2, SATO, K.3,
NAKATA, K.3, AOYAMA, M.3 , KONISHI, T.4(1Aichi Medical Univ., 2Kyoto Univ., 3Du
Pont-Mitsui Polychemicals Co. Ltd., 4Meditec
Japan Co. Ltd.)
Most tasks for restoring Fukusima Daiichi
nuclear disaster force personnel to put protective
cloths on. The radioactive contamination of
those cloths increases radioactive dose of
personnel and also makes difficulty in the waste
disposal. As the contamination might mainly becaused from electrostatic adsorption, it isimportant to reduce the electrification of theprotective cloths.
The

Entira®

film

developedbyDu

Pont-Mitsui Polychemicals is not just anti-static
but waterproof and breathable. By backing
Entira film with suitable unwoven fabric,
adequate material for protective cloths can be
fabricated. However, as the contamination canbe caused even by very weak electrification,
unwoven fabric layer could destroy anti-static
propertyofEntira

film.

Such

weak

electrification cannot be evaluated with theconventional method such as measuring thesurface charge.
We tried to evaluate electrification by utilizing
alpha measurement of Radon daughters. The
materials are left in the Kyoto University
Critical Assembly (KUCA) for a several weeks.
Fine particles containing Radon daughters
emitted from thick concrete walls of KUCA
accumulate on the surfaces of those materials.
The alpha emission was counted with the alphasurvey meters. Large difference in alphacounting among different material was clearlyobserved. It can be considered that this method
is effective for evaluating weak electrification.
2A02

Considerationofmonitoring method by measuring isotope
ratio of FP rare gas −Focusing on collection ofradioactive rare gas from the fuel debris−
USUDA, S., NAITO, Y.
(NAIS Co., Inc.)For Fukushima Daiichi nuclear power station,
it is important to establish a sub-criticality
monitoring

method

in

order

to

prevent

re-criticality of the fuel debris. The conventional
technique is the neutron method, but it isdifficult for the damaged reactor cores to detect
neutrons

due

to

high

backgroundandcomplicated structure. In such situations, thesub-criticality monitoring method by measuring
FP rare gas is effective. As an example, theauthors pay attention to the fission yield ratio of
Kr-88 and Xe-135 which are produced bythermal neutron induced fission of U-235 andspontaneous fission of Cm-244. The ratio varies
in approximately one digit: 1.86 for U-235 and17.6 for Cm-244. Therefore it will be easy toestimate ratio of the number of U-235 neutron
fission and the number of Cm-244 spontaneous
fission by taking isotope correlation between
Kr-88 and the Xe-135. In this presentation,collection of the radioactive rare gas areespecially considered for the sub-criticality
monitoring method by measuring isotope ratioof short lived rare gas nuclides, such as Kr-88
and Xe-135, from the fuel debris.
2A03

Isotopic composition of Uranium andTransuranium in the environment derived
from Fukushima Dai-ichi Nuclear Power
Plant accident
SAKAGUCHI, A.1, YAMAMOTO, M2, STEIER,
P.3, TAKAHASHI, Y.4(1Univ. of Tsukuba, 2Kanazawa Univ., 3Univ. of

sub-criticality

Vienna, 4The Univ. of Tokyo)- 186 -

Dust samples from the sides of roads (blacksubstances) have been collected together with

It is well known that radioactive Cs is easy tolitter and soil samples at more than 100 sites

adsorption to clay with study of macro

contaminated heavily in the 20-km exclusion

autoradiography (ARG). But, discussion iszones around Fukushima Dai-ichi Nuclear

difficult for the relevance of adsorption andPower Plant (Minamisoma City, and Namie,

micro structure, because Imaging Plate method

Futaba and Okuma Towns), in Iitate Village

is low resolution. We tried to observed thelocated from 25 to 45 km northwest of the plantmicroscopic distribution of radioactive Cs in

and in southern areas from the plant. Isotopes ofphlogopite by Scanning Electron MicroscopeU, Pu, Am and Cm have been measured in the(SEM)-ARG. SEM-ARG is using the emulsion

samples to evaluate their total releases into theand observe by SEM.

environment from the FDNPP and to get theExperimental results shows to observe theisotopic compositions among these nuclides.

microscopic distribution of radioactive Cs on

The results provided a coherent data set on

phlogopite at tens of micrometers. The form of

239+240

the Ag that was exposed is different by

among these uranium and transuranic nuclides.

development

When these activity ratios were compared with

Observed Ag grain size is 5 to 20 μm.

those for fuel core inventories in the FDNPPThis method may be applicable to phlogopite asaccident estimated by a group at JAEA, except

well as other materials. This method could be239+240

useful to elucidate the adsorption state of

Pu inventories and isotopic composition

137

Pu/ Csactivityratios,fairlygood

agreements were found, indicating that uranium

time

and

the

radioactivity.

radionuclide.

and transuranic nuclides were released into theenvironment without their large fractionations.

2A05 Analysis of 93Zr in the contaminated

The obtained data may lead to more accurate

water generated at the Fukushima Daiichi

information about the on-site situation (e.g.,

Nuclear Power Station

burn-up, conditions of fuel during the release

SIMADA, A., KAMEO, Y.

phase, etc.), which would be difficult to get(Japan Atomic Energy Agency)
Recently, the separation method of Zr, Nb,

otherwise, and more detailed information on theofand Mo from major elements of contaminatedtransuranic nuclides and the behavior of thesewater, followed by mutual separation of Zr, Nb,

nuclides in the environment.

and Mo using single solid phase extractant

dispersion

anddeposition

processes

column, TEtra VAlent actinide (TEVA) resinofcolumn, has been developed to analyze 93Zr. In

radioactive Cs in the phlogopite, using

this work, the separation method was applied toelectron microscope autoradiography

the analysis of

2A04

Microscopic

1

distribution

2

SASAKI, M. ,TAKASE, T. , YAMAGUCHI, K.
1

1

2( Fukushima Univ., IER., Fukushima Univ.)93

Zr in contaminated water

generated at the Fukushima Daiichi Nuclear
Power Station. Zirconium in the contaminatedRadioactive material of a large amount has

water sample and in 90Zr spiked contaminatedbeen released to the environment by the accident

water sample was separated with the method andat the Fukushima Daiichi nuclear power plant.

then measured by inductively coupled plasma

As a result, radioactive Cs adsorbed in the soil.

mass spectrometry (ICP-MS). Recovery of Zr- 187 -

90

determined by spiked

Zr was 100±2%.

Calibration curve of 93Zr was induced from theslope and intercept of92

Zr and94

same place point, moreover, the river water
sampledforbiweekly

andobtainedtheZr. The countradioactive cesium concentration of the moment

rate of mass number 93 of the Zr fraction wasfrom May, 2012. It is thought which these timebackground level. Consequently, 93Zr in thevariations make it possible to evaluate thecontaminated water was determined < 0.1 ng/mL

external factors over river such as rain. We(9 mBq/mL).

obtained that [137Cs]SS/[137Cs]DM ratio is 4.0×104
in the Ohori River. And it correlated well

2A06

Behavior of Cesium-134, 137 andbetween the variation of the radioactive cesium
concentration and its iodine-129 concentration in

Iodine-129 in River
1

2

2

SUEKI, K. , SHIBAYAMA, N. , SATOU, Y. ,1

dissolved matter.

3

SASA, K. , TAKAHASHI, T. , MATSUNAKA,
T.3, MATSUMURA, M.3, MATSUZAKI, H.4,

2A07

MURAKAMI, M.5, YAMASHITA, R.6, SAHA ,ratios of SPM collected at automated SPM

6

6

7

M. , TAKADA, H. , KOIBUCHI, Y. , LAMXAY,
775S. , O, H. , MOURI, G. , OKI, T.

5

Autoradiography

and

134

Cs/137Cs

monitoring stations at the FDNPP accident
OURA, Y.1, TSURUTA, H.2, EBIHARA, M.1,

(1Faculty of Pure Applied Sci., Univ. Tsukuba,

OHARA, T.3, NAKAJIMA, T.2

2

Graduate School of Pure Applied Sci., Univ.

(1Tokyo Metropolitan Univ., 2Univ. of Tokyo,

Tsukuba, 3TAC, Univ. Tsukuba, 4MALT, the3

National Institute of Environmental Sci.)

5

Univ. of Tokyo, Institute of Indust. Sci., theRadioactivity ratios of 134Cs/137Cs of SPM

Univ. of Tokyo, 6Tokyo Univ. of Agri. & Tech.,collected SPM monitoring stations operated by

7

Graduate School of Frontier Sci., the Univ. of

local governments in eastern Japan on 11 to 23

Tokyo)

Mar. 2011 were determined precisely andRadioactive cesium and iodine which emitted

autoradiographs using an imaging plate werefrom the Fukushima Daiichi nuclear power planttaken for the SPM samples to evaluate awere detected from water in environment. In the

distribution of radionuclides

within SPM.

metropolitan area, higher concentration of

Although most of SPM samples had 1.03 ofradioactive cesium was detected from sediment

134of the Ohori River, Chiba Prefecture. In this

0.921 and 1.01. The ratio of 0.921 was found in

work,

the

only SPM collected at stations located on

concentrations of the radioactive cesium in thenorthern area to FDNPP on 12 Mar. 2011.

suspended substance (SS) and dissolved matter

Radiocesium having low 134Cs/137Cs ratio was(DM) were observed for the Ohori River, andexpected to be released along with an accident at

the elucidation of the actual condition was tried.

Fukushima Daiichi Unit 1 reactor on 12 Mar.

thelong-term

variations

134

of

Cs

and determined ratio, 0.921, in this work was

I in the SS and DM in the river. The

close to evaluated ratio, 0.941, in the core ofconcentration change of the average of theUnit 1 obtained by ORIGEN2 code by Nishihara

radioactive cesium contained in the SS waset al. Ratio of 1.03 was observed in SPM

obtained by the SS sampler of the Ohori River

collected on only 16 Mar. In autoradiography of

installed at the mostly median center. In the

SPM

It was observed concentrations of
and

Cs,

137

Cs/137Cs ratio, some SPM had different ratios,

129- 188 -

samples,fineparticles

with

high

radioactivity were found in SPM collected on 15

be compared with that of 90Sr by considering

Mar. at most of monitoring stations in eastern

total inventory in the core.

Japan. On the contrary, on 21 Mar., a few
particles with high radioactivity were observed

2A09

in each SPM smaples.

Characteristics of Radio-Cs Emitted during

PhysicalandChemicalthe Early Stage of the Fukushima Nuclear
2A08

Radioactive measurement of

140

Ba in

Power Plant Accident

air-dust samples collected in the early phase

IGARASHI, Y.1, ADACHI, K.1, KAJINO, M.1,

of FDNPPZAIZEN, Y.1, NAKAI, I.2, ABE, Y.2, IIZAWA,ZHANG, Z.1, NINOMIYA, K.1, KITA, K.2,

Y.2, SATOU, Y.3, SUEKI, K.3

TSURUTA, H.3, IGARASHI, Y.4, SHINOHARA,(1Meteorolo. Res. Inst., 2Tokyo Univ. Sci., 3Univ.

A.1

Tsukuba)

1

2

3( Osaka Univ., Ibaraki Univ., AORI., Tokyo
4

Univ. Meteorologica Res Ins.)

We have investigated chemical and physicalproperties of the radioactive aerosol, from theBarium-140 was one of radioactive nuclide

Fukushima

Dai-ichiNuclear

Power

Plant

discharged to the atmosphere by the Fukushima(FDNPP) accident occurred in March 2011, by

Dai-ichi nuclear power plant accident. The

using imaging plate technique, scanning electron

discharge behavior ofthat of140

Ba was different from137

Cs due to non-volatility property of

microscopy

energydispersive

X-ray

spectroscopy, etc. (Adachi et al., 2013).

barium. Also Barium-140 is the same chemical
90

with

We have found more than 10 sphericalfamily with Sr and have the similar behavior in

Cs-bearing particles (Cs-ball) from HV filter

fuels when the nuclear reactor normal operation.

samples collected during Mar. 14-15, 2011,

140

90

Ba has more volatility thanSr inwhen the first radioactive plume arrived fromthe severe accident phase. Therefore, comparing

the FDNPP accident at the MeteorologicalHowever,the discharge amount of
bring

us

137

information

90

Cs, Sr and140

Ba canResearch Institute as well as Univ. Tsukuba,

about

accident

Japan. While the second plume gave no suchthecircumstances.
We measured

Cs-ball.
137

Cs and

140

They

have

basically

spherical

Ba activity in the airmorphology, characterized composition of Fe,

dust samples collected in the early phase of theZn, Mn, O, etc. with an appreciable amount of

FDNPP accident with germanium semiconductor

Cs. They are a few microns in diameter with adetector. The sampling spots were Tsukuba,

few Bq of radio-Cs activity but as high specific

Hitachi and Mito cities, Ibaraki Prefecture andactivity as sub-terra Bq/g. They were found to be

KawasakiPrefecture.

insoluble; even refractory to conc. nitric acid

Strontium-90 was isolated from each sample

and soluble only to sodium hydroxide solution

with solid-phase extraction and ion-exchange(Sueki et al., 2013). Also, the bulk extraction

separation and its activity was measured byexperiments showed that the Cs-ball could

Cherenkov light counting.

occupy major part in the first plume.

City,

140

Kanagawa

137

Ba/ Cs activity ratio was 0.07 at

The synchrotron X-ray microbeam analyses

2011/03/15 and it rose about 0.15 in April. In theby using SPring-8 facility suggested that theThe

presentation, the discharge amount of

140

Ba willCs-ball contains many possible fission products- 189 -

in glass matrix (Abe et al., 2014). Therefore,

H2+CO2 mixtures in low pressure gaseous

they would persist for a long time in theconditions

environment, and we need to consider the

YOSHIDA, G.1, NINOMIYA, K.1, INAGAKI,

impacts of the Cs-ball.

M.1,

ITO,

T.U.2,

HIGEMOTO,

W.2,

Aerosol model simulation gave the results that

NAGATOMO,

T.3,

STRASSER,

P.3,

non-hygroscopic super-micron Cs-ball could be

KAWAMURA,

N.3,

SHIMOMURA,

K.3,

removed more by the dry deposition and

MIYAKE, Y.3, MIURA, T.3, KUBO, M.K.4,

below-cloud

SHINOHARA, A.1

scavenging

than

conventional(1Grad. sch. Sci., Osaka Univ., 2JAEA, 3KEK,

sulfate-hosted particles.

4

2A10 ClassificationofInternational Christian Univ.)
A negative muon is one of the elementary

radioactive
110m

137

Ag/ Csparticles that has charge and approximately two

ratios in the northwest area of the Fukushimahundred times heavier mass than an electron. A

Daiichi NPP

negative muon can be captured by the Coulomb

contamination

SATOU,

1

Y. ,according

SUEKI,
1

T. ,MATSUNAKA,

to

1

SASA,

1

K. ,

field of a nucleus, and then a muonic atom is

SHIBAYAMA,

1

formed. When the muon is captured by a

K. ,

1

TAKAHASHI, T. , KINOSHITA, N.
1

N. ,

2

( AMS Group Univ. of Tsukuba,hydrogen atom, muonic hydrogen atom which
2

Shimizu

Corp.,)

can be regarded as a pseudo neutron is formed.
Muonic hydrogen atom can penetrate theActivity ratio and isotopic ratio are one ofelectron cloud of heavier atom and gives theessential information to determine a source ofmuon to the deeper atomic levels in the heavier

110m

137

Ag/ Cs was

nucleus. This process is called muon transfer.

varied at the northwestern area from the

The muon capture processes by muon transfer

Fukushima

Plantprosess and direct capture process (negative(FDNPP) by the MEXT survey. Three groups

muon is captured by heavier atom directly) are

were recognized from the activity ratio at thedifferent each other, however, the difference on

northwestern area. The ratio of the one group,

initial muon capture levels and muon capture

which located in the vicinity of the FDNPP

probabilities by these processes still not beencorresponded to that of the unit 1 estimated withwell examined. In this study, we performed

the ORIGEN 2 code. In contrast, the ratios ofmuon irradiation experiments at J-PARC, Ibaraki,

another two groups were lower than thefor low pressure CO, CO2, H2+CO and H2+CO2

estimation by one order because the area was

mixture gases, and measured muonic X-rays

contaminated after the nuclear core was cooled

which are emitted after muonic atom formation.

down. These groups would be affected from the

From these experiments, the initial muon capture

unit 2 or 3. The present work indicates that threelevels and muon capture ratios were determinedkinds of local contamination are observed fromquantitatively for CO and CO2 molecules by two

the activity ratio at the northwestern area frommuonic atom formation processes.

radionuclides. Activity ratio of
Dai-ichiNuclearPower

the FDNPP.
2A12 Muon transfer process from muonic
2A11

Muon transfer process for H2+CO andhydrogen in gaseous benzene and cyclohexane- 190 -

INAGAKI, M.1, YOSHIDA, G.1, NINOMIYA,MIYAKE, Y.2, NAKAMOTO, T.4,1, ONAKA, S.1,

K.1,

OGISO, R.1, TAKAHASHI, M.5, TAKAYAMA,

KUBO,

M.

K.2,

HIGEMOTO,

W.3,

KAWAMURA, N.4, MIYAKE, Y.4, MIURA, T.4,

T.1

SHINOHARA, A.1(1Daido Univ., 2KEK(J-Parc), 3Intern. Christ.

(1Grad. Sch. Sci., Osaka Univ., 2International

Univ., 4Toray Res. Cent., 5Toho Univ.)

Christian Univ., 3JAEA, 4KEK)Both

The formation processes of muonic and pionic

by

muon

technique andspinrelaxation

(μSR)

57

Fe Mössbauer spectroscopy,

atoms are affected by the chemical environmentiron-valence fluctuation behaviors were probedof the muon- or pion-capturing atoms. Such ain polycrystalline mixed-valence trinuclear ironphenomenon is called chemical effect. Such acarboxylate complexes. A Mössbauer study ofchemical effect was also reported in pion

Fe3O(CH3COO)6(H2O)3·2H2Otransfer process, but it has never been founded in

the valence states of the three iron atoms were

muon transfer process. To examine the chemicalchanged from the trapped one (Fe3+Fe3+Fe2+) at

effect on muon transfer process, we selected the78 K to the detrapped one (Fe2.7+Fe2.7+Fe2.7+)

gas mixture of C6H6 (0.2 kPa) + Ne (3.0 kPa) +with increase in temperature, and the transition

H2 (96.8 kPa) and C6H12 (0.2 kPa) + Ne

temperature was estimated to be around 200 K.

(3.0 kPa) + H2 (96.8 kPa) as the muon

Above this temperature, valence fluctuation via

irradiation samples. The

irradiationelectron-hopping was assumed to occur. μSR

experiments were performed at the MLF/MUSE

experiments were carried out at D1 muon-beam

D1 beam line of the Japan Proton Accelerator

port in MLF of J-Parc and the muon spin

Research Complex (J-PARC), Ibaraki, Japan.

relaxation rates (i.e., the decay constant of

Muonic X-rays emitted after muon-capture formuon-spin polarization) were determined at 100,carbon or neon atoms were measured using high170, 240, and 300 K under a transverse magnetic

purity germanium detectors.

field of 20 G. A maximum value in the relaxation

muon

indicatedthat

Muon transfer rates were determined fromrates was observed at 170 K. A slow electronic

delayed component of the muonic X-rays.

fluctuation would occur around 170 K in

Delayed muonic X-ray intensity ratio of μC/μNe

Fe3O(CH3COO)6(H2O)3·2H2O,

corresponds to the ratio of muon transfer rates

consistentfor carbon atoms to that for neon atoms. The

spectroscopic observation. The Mössbauer andratios of μC/μNe were 6.4±0.7 in C6H6+Ne+H2µSR

sample and 5.7±0.5 in C6H12+Ne+H2 sample.

·CH2Cl2 were also discussed.

withstudies

of

the

above

which

was

Mössbauer

Fe3O(C6F5COO)6(C5H5N)3

We concluded that the significant difference inmuon transfer rate for carbon atoms in two

2B01 A study on pretreatment of tritium

samples was not detected in this work.

analysis in environmental samples using
microwave heating method

2A13 Research of Fluctuating Valence-state

AKATA, N.1, TAKAYAMA, S.1, TANAKA, M.1,

in

Iron

TAMARI, T.2, KAKIUCHI, H.3, SANO, S.4

Spin(1National Institute for Fusion Science, 2Kyushu

Mixed-valence

Carboxylate

Complexes

Trinuclear
by

Muon

Relaxation and Mössbauer Spectroscopy

Environmental Evaluation Association, 3Institute

SAKAI, Y.1, KODA, A.2, KUBO, M. K.3,

for

- 191 -

Environmental

Sciences,

4

AdvancedIndustrial Science and Technology)

integration test under the practical condition

Tritium in environmental organic samples

using room air was conducted at Isotope

usually consists of free water tritium (FWT) and

Separation Laboratory as tritium handlingorganically-bound tritium (OBT). The FWT is

facility in Nagoya University. The system

tritiated water existed as HTO form, and its

mainly consists of proton conductor ceramic

behavior is similar to natural water. On the othermembrane, metal bellows pump, commercial

hand, OBT is bound tritium to organic tissue.

proportional

The OBT has a longer biological half-life andTechnology) and data logger LB5320. The

higher incorporation to organic materials thanestimated tritium concentration by the proposal

the FWT. The standard method of FWT andsystem

OBT analysis is a liquid scintillation counting

introduced tritium concentration. The result of

method after freeze-drying and combustion ofthis work is that the measurement of the tritium

the sample as summarized in MEXT report.

concentration via the proposed tritium monitor

However, pretreatment / analytical method ofsystem

FWT and OBT are complicated and take a long

Technically, the proposal system has reached atime over a week. In this paper, to simplify thelevel at which it can be put into practical use.

shows

was

counter

good

LB110

(Bertholdagreement

successfully

with

the

demonstrated.

analytical method for FWT and OBT, we report
basic study of TG/DTA analysis of pine needle

2B03 Dynamics of tritium recovery systems

samples and the preliminary result of effective

using water bubbler and CuO catalyst

pretreatment for pine needle samples using

SATO, M.1, YUYAMA, K.1, HARA, M.2,

microwave heating method.

HATANO, Y.2, MATSUYAMA, M.2, CHIKADA,
T.1, OYA, Y.1

2B02 Developmentof

tritium

detector(1Graduate School of Sci., Shizuoka Univ.,

system combined with proton conductor

2

ceramic membrane

Toyama)Hydrogen Isotope Res. Center, University of

TANAKA, M.1, SUGIYAMA, T.2
1

Tritium is used as a tracer of hydrogen

2( NIFS, Grad. Sch. Eng., Nagoya Univ.)

isotopes. However, the recovery of a small

The detection of low level tritium withoutamount of tritium at radiation facility is usually

radioactive waste such as liquid scintillation

unreasonable

due

to

higherbasic

safetycocktail is one of the key issues for tritium

standards of tritium. To enhance the social

management in tritium handling facilities. In

acceptance, tritium should be recovered as muchorder to detect a low level gaseous tritium, theas possible without complex procedure. In thisenrichment of tritium by a membrane separator

study, elucidation of reaction mechanism fromis an effective measure. The application of antritium gas to tritiated water by CuO catalyst andelectrochemical hydrogen pump using a proton

evaluation of reaction rate constant wereconducting oxide that transports protons in

performed.

oxides at high temperatures have been proposed

Tritium gas was recovered from a tritium ion

as a membrane separator. We have reported theirradiation device via a scroll pump. It was

results of the system integration test under themixed with PR gas and introduced into the first

conditions without oxygen gas. In this study, theproportional counter to measure over all tritium.

- 192 -

Thereafter, CuO was used to oxidize the gas

was different from those in lower acidity.

including HT. The oxidized gas was completely
recovered by a water bubbler. Finally, the gas

2B05 Systematic difference in the stabilities

was introduced into the second proportionalof complexes of hard cations with various

counter to measure unreacted HT.

oxygen-donor ligands

It was found that the conversion ratio of HTO
from HT was clearly controlled by temperature

TAKAHASHI, Y.1, MIYAJI, A.2, TANAKA, M.1(1The Univ. of Tokyo, 2Hiroshima Univ.)
Complexation of metal cations by ligands

and almost all HT was oxidized at 550 K. In
addition, the gas flow rate clearly controls thesuchconversion rate, too. The reaction rate constantcarboxylate ion, and phosphate ion is one of theabove 473 K could be expressed by themost important factors to control behavior of-1

following equation, k [s ] = 5.4 × 10 exp (-0.65

metal ions in natural environment, especially foreV / kBT), indicating the oxidation of tritium

hard ions such as actinide and lanthanide ions.

was governed by one elementary process.

Previous studies showed that these ligands were2ashydroxideion,

carbonateion,classified as intermediate hard ligands having
2B04 Aggregation of actinide ion associatedoxygen donor, which favors to form ionicwith electrode reduction

bonding. However, it was found that the

KITATSUJI, Y., OTOBE, H., WATANABE, M.,

reactivity of each ligand greatly depends on

KIMURA, T.

ionic radius and that there is a great difference of(Japan Atomic Energy Agency)

the reactivity between hydroxide ion and other

Reduction of uranyl(VI) ion in weakly acidic
solution
reductionandaggregation

were

electrochemical

associatedinvestigatedmeasurements.

based

with
on

Stripping

ligand such as carbonate and carboxylate.
However,quantitative

discussion

on

the

selectivity of metal cations is not quantitatively
performed

including

discussiononvoltammetry with a gold micro-electrode wasthermodynamic parameters (ΔG, ΔH, ΔS) andperformed after preelectrolysis. In the case ofquantum chemical calculation. As a result, weconcentrated U solution of pH 3, decrease of thefound that the entropic contribution to the free

reduction current of U(VI) to U(V) wasenergy was large in the case of hydroxide

observed. This phenomena was explained by thecomplex of small radius cation. In the aqueous

deposition of reduction species of U(VI).

complexation

Current peak due to oxidation of deposits wascontrolled by the number of water molecules

observed at +0.2 V vs SSE. These results show

replacedthat deposition of reduced U on the electrodehydroxide complex for large cation was notsurface was very severe. In the case of pH 2,

stable due to the small effect of dehydration.

byreaction,theentropyligand,changesuggesting

is
that

small oxidation current peak was observed at+0.2 V, but inhibition of reduction of U(VI) was

2B06 Synthesis and spectroscopic properties

not observed. On the other hand, the currentof uranium-containing ionic liquids

peak due to deposits was appeared at -0.05 V in

AOYAGI, N.1,WATANABE, M.1, KIMURA, T.1,

the case of pH 1. This fact indicates that the

KIRISHIMA, A.2, SATO, N.2

chemical species formed in the solution of pH 1

(1NSED, JAEA, 2Tohoku univ.)- 193 -

Photophysical properties such as UV-Vis-NIR

relativistic density functional calculation. For

spectroscopy and time-resolved laser-induced

the comparison of the difference of thefluorescence spectroscopy of uranium(IV) andseparation between MAs and lanthanides, we

uranium(VI) complexes in ionic liquids arefocused on the extraction behavior of MAs andstudied as well as synthesis and purification oflanthanides employing Cyanex-272 and -301

uranium tetrahalides and related materials. For

ligands which were phosphinic acid andexample, the powder of U3O8 was put on thedithiophosphinic acid respectively. All geometry

glass boat under Ar atmosphere in an open

optimization

glassware. To this was added CCl4 vapor atwithout any constrains for ML3 (M = SmIII, EuIII,

420 °C for two hours affording the dark green

AmIII and CmIII; L- = [(Me2PO2)2H]- andproduct of crude UCl4 crystals contaminated[Me2PS2]-) complexes. All equilibrium structureswith other uranium chlorides. Purification by

at ZORA-BP86 / def2-SVP level reproduced thesublimation was subsequently performed in aexperimental

closed quartz tube at 542 °C for six hours,

Complexation

affording green crystals of UCl4. These halides

single-point calculations at ZORA-B2PLYP /were reacted with a proper amount of KSCN anddef2-TZVP level, which gave the excellent

1,3-dimethylimidazolium

givecorrelation with experimental Mössbauer isomer[C1mim]4[U(NCS)8], a target compound. There

shifts for 151Eu and 237Np complexes, showed theis a definitive difference in UV-Vis-NIR spectra

reproducibility of experimental Gibbs energy

of UX4 dissolved in organic solvents and ionicdifferences. This result indicated that the origin

liquids presumably due to the coordinationof selective separation of minor actinides ischlorideto4+

environment around U center. White-to-yellow
4-luminescence of U(NCS)8 has a very short

attributed

calculations

weremetal-ligand

toenergythelengths.

resultsstability

performed

obtainedofbyextraction

complexes by the complex formation reaction.

lifetime around 10 ns, which is far shorter thanthat of UO2(NCS)53- species reported in our

2B08 Relations

previous work with different spectral shape.

cross-section

betweenmeasurement

captureandpromptgamma-ray analysis
2B07

Computational approach to theselective separation of minor actinides by

KIMURA, A.1(1Japan Atomic Energy Agency)
Accurate neutron capture cross section datameans of density functional theory
KANEKO,

1M. ,NAKASHIMA, S.
1MIYASHITA,

1

S. ,

2

for minor actinides (MAs) and long-lived fission
products (LLFPs) are required to estimate the2( Grad. Sch. Sci., Hiroshima Univ., N-BARD,

production

andHiroshima Univ.)

developing

innovative

The selective separation of minor actinides

transmutation
nuclear

rates

for

systems.

However, accurate measurements of these cross(MAs) from high-level liquid waste and thesections

disposal by the transmutation of MAs have beenradioactivity of these samples. To overcome thechallenging tasks because of the difficulty ofdifficulty, “Accurate Neutron-Nucleus Reaction

their separation. We investigated the separation

measurement Instrument (ANNRI)” has been

behavior of MAs from lanthanides by means ofconstructed in the Materials and Life science- 194 -

arevery

difficult

due

to

high

experimental Facility at the Japan Proton

developed

Accelerator

The

gamma-ray analysis (PGA) combined withenergy-integrated neutron intensities at the flight

gamma-ray coincidence technique. We have

Research

Complex.
72

atime-of-flight(TOF)

promptlength of 21.5 m are 1.2×10 n/s/cm in the

conducted several experiments of standard

neutron energy range of 1.5-25 meV, andsamples to assess the feasibility of the method.

62

1.8×10 n/s/cm in 0.9-1.1 keV at a beam power

Neutron capture resonance peaks are clearlyof 300 kW. In the epithermal energy region, theobserved in the TOF spectra of the standard

energy-integrated neutron intensity is more thansamples. This presentation will describe the17 times as high as the values of the otherdetail of the experiments and the current status

instruments. A series of neutron captureof the development of the method.

cross-section measurements with high intensity
pulsed neutrons have been started.

2B10 Elemental Analysis using Time of

On the other hand, not only neutron capture

Flight–Multiple

PromptGamma

Raycross-section measurement but also prompt

Analysis Method on J-PARC BL04 ANNRI–

gamma-ray analysis with time-of-flight has been

MIURA, T.1, EBIHARA, M.2, TOH Y.3,

performed using the ANNRI.

MATSUO, M.4, CHIBA, K.1, KIMURA, A.3,

In this presentation, relations between capture
cross-section

measurementandpromptOURA, Y.3, SHOZUGAWA, K. 4
(1National Metrology Institute of Japan-AIST.,
2Tokyo Metropolitan Univ.,

gamma-ray analysis are presented.

3Japan Atomic

4

Energy Agency, Tokyo Univ.)
2B09 Current status of development of

We are developing the new analytical method

multiple prompt gamma-ray analysis withfor precious metals in solid sample using thetime-of-flight method

time of flight–multiple prompt gamma ray

TOH, Y.

analysis method on J-PARC/MLF BL04 ANNRI(Japan Atomic Energy Agency)(Accurate

Neutron-Nucleus

Measurement

Reaction

Instrument). The Pd-Ag alloy foil (Pd:Ag; 75:25,

Measurement Instrument (ANNRI) has beensample mass; 21.6 mg, thickness; 0.025 mm,

designed and developed for the measurement of

9.28 mm×9.28 mm) was selected for test sample.

prompt gamma-ray analysis (PGA), nuclear

We presented the results and the possibility ofcross-section data and nuclear astrophysics atdeveloped analytical method.

The

Accurate

Neutron-Nucleus

BL04 of the Material and Life Science
Experimental Facility (MLF) of the Japan

3A01

Proton Accelerator Research Complex (J-PARC).

radioactive Sr isotopes in seawater using

The germanium detector-array, which consists ofliquid scintillation counting

two cluster-Ge detectors and eight coaxial-Ge

WATANABE, R.1, UESUGI, M.2, SAKAI, H.2,

detectors

YOKOYAMA, A.2

with

BGO

Compton-suppression

Examination of the rapid analysis ofshields, was installed at the flight length of(1 Grad. School Nat. Sci. Tech., Kanazawa Univ.,

21.5m in ANNRI. The detector-array is designed

2Strontium 90 is one of the nuclides that haveto provide high gamma ray energy resolution
and

high

detection

efficiency.

We

have

Inst. Sci. Eng., Kanazawa Univ.)

been released to the environment by the- 195 -

Fukushima Daiichi nuclear power plant accident.

35ml solution of 2 or 3M HNO3. The solution

The radio isotopes have been leaking to thewas through an Analig Sr-1 column or anunderground and released into the ocean with

EmporeTM RadDisk to absorb the strontium.

contaminatedits

Activity of 90Sr and 90Y of the column wasradioactivity measurement fuming nitric acidmeasured directly by well-type NaI (Horiba

water.

Currently,for90

method has been used for the analysis of Sr inLtd.). After that, Sr was eluted from the column

seawater. However, it is necessary to improvewith 0.03% EDTA solution. Eluate and disks

the method because of its time-consuming

were determined using a liquid scintillation

hazardous procedures. A rapid determination ofcounter LSC-6100 (Hitachi Aloka Medical Ltd.).

radioactive Sr isotopes requires separation andBy the quantified measurements of strontium

purification of either of

90

Y and

90

Sr. In thisafter about three weeks

at the90

Sr-90Y

study, we examined the precipitation method ofradiochemical equilibrium, the elution rates and

90

Y and the concentration method of Sr using Sr

the absorption rate to the column or disks were

Rad-Disk. For the measurement, we examined

estimated. The time required for chemical

the two techniques of the Cherenkov light

separation procedure by this method was 2 days

measurement and the measurement using withalthough it took about 2 weeks in a conventional

an extraction scintillator.

manner. In the range of the amount of calcium
1-5g (0.1-0.5% relative to 1L) in the sample,ofstrontium absorption rate to the Analig Sr-1

radiostrontium in water by solid extraction

column was 77%. This method is applicable totechnique: part 1

the screening analysis of seawater samples. The

3A02

Rapid

determination

1

2

MINOWA, H. , KATO, Y. , OGATA, Y.
1( Radioisotope

Res.

2

Facility.,

3

Jikei

column used was confirmed to be reused.
Univ.,

3

Hitachi Aloka Medical, Grad. Sch. Med.,

Simple determination of radioactive strontium
became possible by this method.

Nagoya Univ.)
The conventional standard method used fortheanalysisofradioactive

strontium

in

3A03

Rapid

determinationofradiostrontium in water by solid extraction

environmental samples is required complicatedtechnique: part 2time-consuming procedure with toxic chemical.

KATO, Y.1, MINOWA, H.2, OGATA, Y.3

For the purpose of development of simple and(1Hitachi Aloka Medical ､ Ltd., 2Radioisotope

quickRes. Facility., Jikei Univ., 3Grad. Sch. Med.,andsafetyanalyticalmethods

ofradioactive strontium, we used an Analig Sr-01

Nagoya Univ.)column (IBC Advanced Technologies, Inc.) of

The standard methods used for the analysis ofusing a solid extraction separating agent. This

radiostrontium in environmental samples requireTM

Srcomplicated time-consuming procedure with

RadDisk (Sumitomo 3M Ltd.) of using similar

toxic chemical. To explore a simple, rapid andagent. We applied the water samples spiked withsafety radiostrontium analysis, we tried to use a

90

Sr and addition of calcium and strontium

column with a solid extraction separating agent

carrier. After the precipitation of calcium(Analig Sr-01, IBC Advanced Technologies,

carbonate, the precipitate was dissolved in aboutInc.).

method was compared with an Empore- 196 -

This method was compared with one

with a solid disk (EmporeTM Sr RadDisk,

the most important long-lived fission products.

Sumitomo 3M Ltd.) with similar agent. The

In order to remove these nuclides from the90

measurement method is described here. Sr wascontaminated water, two systems had been

spikedinstalledinthewater samples.

After theincludingthecesiumabsorption

precipitating, the precipitate was dissolved in

filtration system and the Advanced Liquid

about 35 ml solution of 2 or 3M HNO3. The

Processing System (ALPS). However, due to thesolution was through the column or the disk todifficulties in the operation of such column

absorb strontium. The activity of90

Sr and90

Ysystems, their operations have not been proved

absorbed on the column was measured directlytoby a well-type NaI(Tl) detector (Horiba Ltd.).

decontamination.

be

very

effective

for

the

intendedThen, strontium was eluted from the column

Solvent extractions are one of the most usefulwith EDTA solution. The activity of the elated

separation methods of metal ions. Using

solution was determined with the well-type

1,2-dichloroethane, 1-octanol or chloroform as a

NaI(Tl) detector and a liquid scintillation

diluent and crown ethers can functions as

counter

Aloka

extractants of cesium and strontium from acid

Medical Ltd.). RadDisk was put in an LSC

solutions[1][2]. The diluents has inevitable risks

standard vial containing liquid scintillator, andof

was measured with the LSC. The time required

soundness. In our previous works, the solvent

for chemical separation procedure by thisextraction of uranium from nitric acid solution

method was two days although it would takewas conducted by HFC-43-10mee (DuPont;

about two weeks by the conventional manner.

Vertrel XF) - TBP system. With the strong C-F

Furthermore, the Analig column was confirmed

bonds the dilents show excellence in theto be reusable. Measurements by the liquid

noninflammability, the low toxicity, and thescintillation counting can be determined rapidly

chemical stability.

(LSC,

LSC-6100,

Hitachifires,

explosions,andenvironmental

without waiting the radiochemical equilibrium.

In this study, we investigated the use of theThis method is applicable to the screening of

HFC-43-10mee and its azeotropes as diluents.

seawater samples. A feasibility of simple

We will present the results obtained bydetermination method of radiostrontium was

extractions of alkali metals and alkaline earth

presented.

metalsfrom

aqueoussolutionsbydicyclohexano-18-crown-6-ether as an extractant
3A04

Investigation of selective extraction ofin these diluents.

cesium and strontium by solvent extraction[1] R. A. Sachleben, et al., Sep. Sci. Technol.,NAGAI, M., SHIRASAKI, K., SAKAMOTO,

32(1997)275.

K., YAMAMURA, T.

[2] K. K. Gupta, et al., Solvent Extr. Ion Exch,(Tohoku Univ.)

21(2003)53.

As a serious result of the damaged vessel ofthe Fukushima Daiichi Nuclear Power Plant due

3A05

to the 2011 Tohoku earthquake, the extensive

the atmosphere observed in Tsukuba andleakage of the contaminated water has occurred

Iitatewhich includes137

Cs and90

Sr, both are one of

Fukushima-derived radionuclides in

DOI, T.1, TAKAGI, M.1, TANAKA, A.1,

- 197 -KANNO,

2M.

,

DOKIYA,

2

Y.

,(Japan Atomic Energy Agency)

MASUMOTO, K.3

Due to the accident of Fukushima Daiichi

1( National Institute for Environmental Studies,

NPS, TEPCO, wide area was contaminated.

2

TEPCO analyzed radioactivities of the soil

Resurrection of Fukushima,

3

High Energy

Accelerator Research Organization)

within the NPS site and reported activity
Cs

concentrations during 2011. Based on the data

Cs in aerosols were observed to be in thedisclosed, transport behavior of the detected

Since March 2012, the concentrations of
and

137

134

-5

-3

level of 10 Bq m at Tsukuba, about 170 km

radionuclides from the fuel of damaged reactors

from the Fukushima Dai-ichi Nuclear Powerto the soil was investigated. The concentration of

Plant (FDNPP). Since March 20, 2012, weradionuclide in the soil was normalized with themeasured radiocesium in surface air at two

fuel composition after correcting decay andpoints of Iitate (Sasu and Itamisawa), aboutobtained relative value to that of 137Cs as the

30km from FDNPP. The concentrations of 137Cs

transport ratio. The transport ratio calculated

and

134

Cs in aerosols were observed to be in the-4-3

was almost constant for time of sampling andlevel of 10 Bq m . Aerosols at Sasu showed athe ratios of isotopes correspond with each other.

higher concentration of radiocesium during 31

It was found that the transport ratio to the soil

March-8 to April 2012, which could have been

was in the order of followings:

caused by the re-suspension of soil particles

I > Te > Cs > Ag~Sb > Mo~Ru > Ba > Sr > Nb

including radiocesium for a strong wind. During> Pu~Am~Cm

March 10-21, 2013, a higher concentration of

And the transport ratios for I, Sr and alpharadiocecium was also observed in the Itamisawa

emitters would be dependent on the location ofaerosols, but in this case it was supposed to besampling soil. Uranium was dominated by that

due to the re-suspension of soil particles

of naturally occurred.

including radiocesium because

anofficial

decontamination activity took place at the site.

3A07 Properties

The higher aerosol mass and concentration ofRadioactive Caesium of the Surface Soil ofsoluble calcium ion in the aerosol supports thisJapanese Cedar Forest in Fukushima

hypothesis. Aerosols at Sasu and Itamisawa

ISHII,

showed a higher concentration of radiocesium

WATANABE, T., ODA, Y., NIIZATO, T.

during August 6-28 2013, which could have

(Japan Atomic Energy Agency)

Y.,

and

SASAKI,

DistributionY.,

KIKUCHI,ofN.,

been caused by a radioactive plume of FDNPP

As part of "Long-Term Assessment of

which passed through this area from the backTransport of Radioactive Contaminant in the

trajectory analysis and other information. The

Environment of Fukushima" (F-TRACE project),activity

JAEA

medianaerodynamic

diameterofhave

researchedtopredicttheradiocesium -bearing particles were larger thantransportation of radioactive caesium from

1.2 µm.

contaminated mountain forests to estuary andcoast through dam, pond, river etc. based on

3A06

Transport of radionuclides to soil atsurvey data in Fukushima prefecture, and to

Fukushima Daiichi NPS, TEPCO

implement technical information and remedial

KOMA, Y.

measures- 198 -

toprevent

contaminationofdecontaminated areas and domestic water supply.

semiconductor detectors. The discharge ratio of

In the forest area, it is considered thatparticulate radiocesium increased in summer

radioactive caesium existed in the tree canopies

during the rainy and typhoon seasons. The

move to the surface of the ground through litter

dissolved

fall, through fall and stem flow. In this study, we

maximum of 46% in winter, with a decrease inreport properties and distribution of radioactive

the flow rate. The largest discharge of particulate

caesium of the surface soils at stem base ofradiocesium

Japanesecomponent (F4) and, as a consequence, the F4

cedar

in

the

Ogi

districtofKawauchi-mura to know the influence of theradiocesium

occurred

ratio

in

reachedthefinestthesize

had the highest radiocesium load.

stem flow on soil.
3A09
3A08

Fluvial discharges of particulate anddissolved

radiocesium

from

a

forestInfluenceofpotassiumandammonium ion in filtering the environmental
radiocesium

catchment

HIGAKI, S.1,HIROTA, M.2, ITO, S.3

TAKEUCHI, E., ATARASHI-ANDOH, M.,(1RIC Univ. of Tokyo, 2Res. Center Human and

NISHIMURA, S., NAKANISHI, T., TSUDUKI,

Env. Sci., Shinshu Univ., 3Grad. Sch. Life Sci.,

K., KOARASHI, J., MATSUNAGA, T.

Kumamoto Univ.)
The potassium fertilizer is encouraged to(Japan Atomic Energy Agency)
A large amount of radiocesium emitted fromapply for paddy fields for contamination control

the Fukushima Daiichi nuclear power plantof radiocesium, because potassium is effective to(FDNPP) was deposited in mountainous areas. It

reduce the migration of radiocesium fromis therefore important to determine the quantity

radiocesium-soil to crops. Prussian blue isofeffective

radiocesiumtransported

from

these

to

collectofcesium.

The

mountainous areas by hydrological processes tononwoven-fabric filter containing Prussian blue

predict the future contamination status of(PB-filter) is able to reducing the volume bydownstream areas. We developed an efficientburnout. Therefore, the local government unit issystem for the collection of radiocesium in bothconsidering to use PB-filter for decontaminating

the dissolved and suspended solid (SS) forms inwater which generated by decontamination of

stream water, which comprised sequentiallyresidential district. In our previous study, we

connected

have reported that NH4+ and K+ ion promoted tofiltervessels,

containing

long

depth-type filters (pore size: 100 and 0.5 µm),

extract

and columns filled with an absorbent to collectradiocesium-contaminated soil to water phasedissolved radiocesium. The system was applied

while these ion interfere the collection by

to a small stream located about 65 km southwest

PB-filter.

from FDNPP, and the filters and columns wereapplicability to the colleting environmental

collected monthly. The SS samples were

contamination of radiocesium, the collecting

collected separated into four particle sizes

effect of radiocesium which extracted fromfractions (F1: > 2000 µm, F2: 500-2000 µm, F3:

wood humus (Quercus serrata) under the

75-500 µm, F4: < 75 µm) and the radiocesium

conditions presence of NH4+ and K+ ion bycontent

PB-filter were evaluated. Almost of radiocesium

wasmeasured

using

the

Ge

- 199 -

radiocesium

In

this

study,

fromtoclarifythetheextracted from wood was collected by twice offungi and algae. A number of studies were

filtering as with Cs+ ion in 137CsCl standard

carried out after the nuclear weapons tests andsolution.

Chernobyl accident, and demonstrated thatlichens were useful for indicator of radioactive

Elucidation of migration behavior of

fallout because they could take up large amountradioactive cesium and tritium in the teaof radionuclides directly from their thallus due

plantsto lack of root system and retain them. It is

3A10

1

1

YUYAMA, K. , SATO, M. , KAMOSHIDA,
2

2

2

1

M. , IKKA, T. , MORITA, A. , CHIKADA, T. ,1essential to evaluate retention characteristics ofradiocaesium in lichens for the purpose of

OYA, Y.

prediction of the initial concentration brought by

1( Graduate School of Sci., Shizuoka Univ.,

fall-out. Especially, the retention behavior of2

Graduate School of Agr., Shizuoka Univ.)

radiocaesium in lichens in Japan has not been

Various radionuclides could be released by theinvestigated so far.

severe accident of nuclear power plants. In
137

3

The objective of this study is to investigate

particular, radiocesium ( Cs) and tritium ( H)thethat have long half-lives will have a large impact

concentration in individual lichen. Lichen

on environment for a longer time. Green tea issamples were parmelioid lichens grown on tree

one of special products in Shizuoka, and it istrunkimportanttounderstand

137

Cs

and

3

H

distribution behavior in the tea plants from theviewpoint of safety. In this study,

137

of

changePrunusspp.

ofradiocaesium

withinFukushima

prefecture. The counting rate of surface of lichen
wasperiodicallymeasured

by

means

of

3

Geiger-Mueller (GM) survey meter (ALOKA,

Cs or

TGS-146B) with a lead collimator to evaluate

Cs and H

distributions in the tea plants grown bytemporal137

3

H contaminated water were evaluated by

the evolution of radiocaesium concentration.

Imaging Plate and NaI (Tl) scintillation detector.
137

The counting rate of lichens increased with

Cs dissolution behavior by brewing tea leaves

the elapse of time for one year. It can be

was also estimated. 137Cs in the tea plants grownconsidered that lichen may take up radiocaesium

by

137

Cs solution was localized at stems andsprouts that cell division is usually done. Thesefrom stem flow including radiocaesium desorbed
from canopy or stem.

results indicate that 137Cs is chemically trapped
and locally accumulated in the tea plants. In this3

3A12

Distribution of radiocesium and its

presentation, H migration behavior will be also

relationship with the other elements in tree

discussed.

body
WANG, W.1, KANASASHI, T.1, SUGIURA, Y.1,

3A11 Retention

characteristics

radiocaesiumlichens

in

and

of
their

2

(1Graduate School of Bioagricultural Sciences,
Nagoya University)

applicability as fall-out indicator
1

TAKENAKA, C.1

1

DOHI, T. , OHMURA, Y. , FUJIWARA, K. ,IIJIMA, K.
1

1

In the present work, we investigated the
distribution of radiocesium and its relationship2( JAEA, TNS)

with the other elements in different parts of tree

Lichens are symbiotic organisms consisted ofbody. The primary purposes are to clarify the- 200 -

uptake pathway of 137Cs and to predict its

thebehavior and accumulation within tree body.

contaminated by radiocesium collected in

Two tree species were selected for study: Sugi

Fukushima. Absorption of radiocesium was also

(Cryptomeria

Koshiaburahighly related to exchangeable potassium in soil.

(Eleutherococcus sciadophyllodides). Trees were

Vegetables happened to be contaminatedcollected from forests located about 30 km away

through the use of contaminated cultivationfrom the Nuclear Power Plant. Stem disks frommaterials, such as plastic film. Application ofseveral vertical positions, branches and leaves

contaminated leaf litters or hums to the soil waswere sampled. Disks were separated into bark,also influenced to the absorption of radiocesium

sapwood and heartwood. In the case of E.

in vegetables.

japonica)

and

137

cultivation

experiments

using

soil

Cs

These results indicated that high radiocesium

and the other elements varied among different

values in vegetables were mainly caused by the

sciadophyllodides, the correlation between
tree components, the correlation between
and

K,

Rb

was

in

the

order

137

Cs

direct contamination due to the dissolvedofradiocesium from the contaminated cultivationwood>leaves>bark, the same tendency was also
observed for133

Cs which had the highest

correlation with137

Cs compared to otherelements, indicates that
with

137

Cs was well mixed133

Cs within the biological cycle in theforest ecosystems. High correlation between Mn
andmaterials.

137

Cs was only found in leaves. The
137

3A14

Concentration Differences between

Radiocesium and Potassium in Tissues of
Herbaceous Plants
TAGAMI, K., UCHIDA, S.
(Natl. Inst. Radiol. Sci.)

Cs and K lead

The fate of cesium (Cs) in plant body isto the high correlation between them whereas

known as similar to that of potassium (K).

the difference in wood and leaves may be

However, due to their different chemical

attributable to their different physiological role.

characteristics,

chemical similarities between

their

fates

would

not

be

completely the same, although their major
Transfer of radiocesium in vegetables

chemical forms in plants are Cs+ and K+. In this

KOBAYASHI, T.1, SAITO, S.1, HARA, Y.1,

study, we used four herbaceous plants (giant

MURAMATSU, Y.2, OHNO, T.2

butterbur, Japanese knotweed, tall goldenrod,

1( Fukushima Agricultural Technology Centre.,and field horsetail) to see whether 137Cs and 40K

2

Gakushuin Univ.)

concentrations were different among plant parts,

The accident occurred at Fukushima Daiichi

that is, leaf blades and petioles, or leaves andNuclear Power Plant, brought the serious

stems. All samples were grown on the NIRS

radioactive material pollution to the farmland.

campus in Chiba City; after their collection,

Immediately after the accident, some vegetables

samples

3A13

were

separated

into

each

137

Cs

and

parts,
40

K

exceeded the regulation value of radiocesium byoven-dried

direct contamination. However, quite a few

concentrations with a Ge detecting systems

vegetables grown after the accident exceeded the(Seiko EG&G). Giant butterbur samples havereregulation value of radiocesium. Absorption ofbeen collected regularly since October 2011 (17radiocesium in vegetables was extremely low intimes in total), and every time we found that- 201 -

andmeasured

137

Cs concentration in leaf blades was higher

the knowledge of the total count rate as well asthan that in petioles, while 40K concentration in

the peak count rates and the sum peak count rate.

leaf blades were lower than that in petioles. The

However

results indicated that distribution patterns of Cs

radionuclides, it is fraught with difficulty toand K were different in different plant parts.

evaluate the total count rate of the corresponding

Similar tendency was also found in leaves andradionuclide. To solve the problem, we modified

stems of other plant samples.

the formula of the method by removing the total

when

a

samplecontains

othercount rate and tried to evaluate the activity. The
3A15

Correction of Sum coincidence effectmodified sum-peak method was theoreticallyusing total efficiency

investigated and experimentally verified with- Sum Coincidence effect correction for

two HP-Ge detectors using 60Co, 22Na, and was

Ag110m -successfully confirmed. Although the accuracy

HAMAJIMA, Y.

is limited, it was proved that the modified(Kanazawa Univ., LLRL)

sum-peak method was effective to measure

The correction of sum coincidence effectwouldrequirefor

nuclidewithcascadesamples containing multiple radionuclides andwas quite simple and practical.

gamma-ray emission, such as Cs134, Al26,
Ag110m, Na22 and Co60. The correction factors

3A17of these nuclides have not been estimated from

to

134

peak to total ratio, but from total efficiency as a

OGATA, Y.1, MIYAHARA, H.2, ISHIHARA,

function of gamma-ray energy. The total

M.3, ISHIGURE, N.1, YAMAMOTO, S.1,

efficiency curve as a function of energy leads to

KOJIMA, S.4

correction of sum coincidence effect of all of(1Grad. Sch. Med., Nagoya Univ., 2Gifu Univ.

nuclidesMed. Sci., 3Nagoya City Univ., 4Aichi Med.

including

those

with

extremely

Application of the sum-peak method

Cs activity measurement

complicate decay scheme, such as Ag110m.

Univ.)

Correction of sum coincidence effect by total

134

Cs emits more than ten gamma-rays per asingle decay, so the decay scheme is quite

efficiency is practical.

complex. Therefore, there are few reports about
3A16

Development

of

the

modifiedsum-peek

sum-peak method
1

2

OGATA, Y. , MIYAHARA, H. , ISHIHARA,
3

1

M. , ISHIGURE, N. ,KOJIMA, S.

1

YAMAMOTO, S. ,4method.

2( Grad. Sch. Med., Nagoya Univ., Gifu Univ.
4

In

this

134

Cs by thestudy,

theconventional sum-peak method and the modified
sum-peak method developed by us are applied todetermination

1

3

the activity determination of

of

134

Cs

activity.

It

wassuccessfully proved that both the methods wereMed. Sci., Nagoya City Univ., Aichi Med.

applicable to determination of the activity.

Univ.)

Especially, the modified sum-peak method was

The sum-peak method is one of the absolute

useful to determine the activity of the sample

radioactivity measurement methods, which iscontaining other radionuclides; such as 137Cs.

applicable to radionuclides emitting more than

Furthermore, the modified sum-peak method

one photon in coincidence. The method requires

potentially has an ability to determine the- 202 -

activity of a volume sample with nonuniform

3B02 The indirect radiocarbon dating using

distribution of activity. Consequently, it was

microscope observation and bibliographicalproved that the modified sum-peak methods

consideration of kohitsugire

were quite effective to measure samples

ODA, H.1, SAKAMOTO, S.2, YASU, H.3,

extracted from Fukushima.

IKEDA, K.4(1Cen. Chronological Res., Nagoya Univ.,
correction

2

models in quantitative EPMA for accurate

3

Chemical U-Th-total Pb Isochron Method

Univ.)

3B01 ValidationofmatrixDegital Archives Res. Cen., Ryukoku Univ.,
Taga High School, 4Faculty of Letters, Chuo
Ganjin brought Japan many Buddhist sutra,(CHIME) dating
KATO, T.

Buddha statues, medicine and spice. Especially(Cntr. Chronological Res., Nagoya Univ.)

an important thing is the Shibunritsu sutra of 60

The CHIME dating is a chemical dating

volumes which described commandments andmethod using U-Th-Pb series. This methodorganizational operation of temple. At present,

provides micro-volume subgrain dating using

the Shibunritsu sutra of 16 volumes that are said

electron probe micro analysis. Accuracy of thefor Ganjin to have brought are stored in Shosoin.

CHIME dating depends of the quality of chosen

Radiocarbon dating is destructive analysis. It,

matrix model in addition to that of X-ray

therefore, cannot be applied to Sutra stored inmeasurement and standard materials because an

Shosoin directly. Kohitsugire is a fragment ofage is obtained from a set of chemicalancient calligraphy. They were cut from ancompositionsThe

ancient book or roll of sutras. We obtained asurface-center Gaussian model by Armstrong[1]kohitsugire considered to have been cut fromwith the atomic number correction by Love etShibunritsu stored in Shosoin. Microscopeal.[2] gives inaccurate chemical compositions ofobservation and bibliographical consideration

U, Th and Pb, while the double parabola modelclarified that the kohitsugire is rightly fragment

by Pouchou & Pichoir[3] gives accurateofchemical compositions. It is result of (1)Radiocarbon dating of the kohitsugire indicatedmathematical limitation in the surface-center

that it was written before the Ganjin visit toGaussian model and (2) inaccuracy of electronJapan. This result shows that possibility that thebackscattering correction by Love et al.[2]kohitsugire and Shibunritsu of Shosoin were

[1] Armstrong, J.T. (1991) In: Electron Probe

brought about by is very high. This study using

Quantitation, Heinrich, K.F.J. & Newbury, D.E.

microscope(eds), Plenum Press, New York, 261 – 315.

consideration and radiocarbon dating indicated[2] Love, G., Cox, M.G. & Scott, V.D. (1978), J.

that indirectly radiocarbon dating can be applied

Phys. D, 11, 7 – 21.

for samples to which destructive analysis could[3] Pouchou, J.L. & Pichoir, F. (1991) In:

not be originally applied.

of

U,

Th

and

Pb.

the

Shibunritsu

storedobservation,inShosoin.

bibliographicalElectron Probe Quantitation, Heinrich, K.F.J. &Newbury, D.E. (eds), Plenum Press, New York,

3B03 Radiocarbon dating of carbonized

31 – 75.

material attached to pottery: implications ofchemical component of inner and outer- 203 -

SGMB-4232b was similar to that of the innersurfaces on potsherds
MIYATA, Y.1, ONBE, S.2, HORIUCHI, A.3,
4

SAKAMOTO,IMAMURA, M.

M. ,MATSUZAKI,International

H. ,

4

ones. There was a possibility that some of “foodresidues” were attached to the outer surface on
pottery and burned out. The origin of “boiling(1LLRL, Kanazawa Univ.,
35Christian2

Hokkaido Univ.,over” in outer surface on pottery could be4

possibly explained by chemical compositions ofUniv.,

National

5

Museum of Japanese History, The University

SGMB-4232b.

Museum, The University of Tokyo)

In this paper, we also discuss the correlation

The difference of radiocarbon ages areof the radiocarbon ages found in inner and outerexamined for the charred materials between

surfaces on potsherds, with the change of

inner and outer surfaces on pottery from achemical compositions (C/N ratios) before andwetland archaeological site, and discussed inafter AAA treatment and the difference of lipid

light of chemical component on the carbonizedcomposition in inner and outer surfaces onmaterials. The samples consist of eight pieces ofpotshers, which may provide a scientificallypotsherds, which are excavated from Irienaiko

evidence to explain “boiling over” in outerarcheological site, around the lake Biwa, Shiga

surface on pottery.

prefecture, Japan and are found to be originated
from

the

same

pottery

of

the

3B04

Determination of V in geological“Kitashirakawa-kasou IIc type” in the Earlyreference samples by INAA and ICP-AES

Jomon era. The AMS radiocarbon dating for

TAKAHASHI, H., SHIRAI, N., EBIHARA, M.

these potsherds indicates that the inner surface(Tokyo Metropolitan University)(charred food residues) of the potsherds (5052 ±14

Vanadium is widely distributed in the Earth’s

12 BP; N = 5) are about 91 ± 25 C year older

crust and mantle. It is geochemically classified

than that of outer (soots) ones (4961 ± 22 BP; N

into lithophile elements. The determination of V

= 7; except for SGMB-4232b). There is nofor cosmochemical and geological rock samples

marine reservoir effect of the samples fromis important in unraveling early history of our13

Irienaiko site, because the δ C values of innersolar system and evolution of planetary bodies

charred matters after AAA treatment are lessrespectively.

than -26‰ notation, which means typical of(ICP-AES, ICP-MS, INAA, AAS, and XRF)

terrestrial origin. Therefore, the difference of

have been developed for the determination of Vages is likely to be caused by freshwaterat low concentration level. Among them,reservoir effect, the ages of outer surface (soots)

ICP-AES is the most frequently used nowadays.

were corresponded to the age of the site.

In ICP-AES, several wavelengths were used in

Severalanalyticalmethods

The chemical composition of outer surface

previous studies, but a suitable wavelength forsample SGMB-4232b, which was from the outerthe determination of V has not been examined.

surface, was similar to that of the other outerIn new study, we valuated three wavelengths

surface samples, but the radiocarbon age of this(292.402nm, 310.230nm and 311.071nm) bysample was similar to those of the inner surface

analyzing geological reference samples andsamples after AAA treatment. Before AAA

comparing ICP-AES data with INAA data. It

treatment,

was observed that 292.402nm and 311.071nm

thechemicalcompositionof- 204 -

have spectral interference from Ti and that

good agreement with certified and reference

interference at 311.071nm is 10 times higher

values. Although absolute REE abundances forthan that at 292.402nm. Argon gives spectral

NIST-1400

interferences for 310.230nm, increasing the

CI-normalized REE abundances patterns forbackgroundotherthese three reference materials are similar towavelengths. Considering detection limits andeach other and continental crustal materials.

spectral interferences, we concluded that V

Through this research, a new data set of twenty

could be accurately determined by using theseven, 28 and 39 elements for NIST-1400,

292.402nm emission line in ICP-AES.

IAEA-450 and IAEA-395, respectively, havehigher

than

those

for

and

IAEA-450aredifferent,

been proposed.
3B05 Multielemental analysis of NIST and
IAEA

referencematerials(NIST-1646a,

3B06 Neutron

activation

analysisof

NIST-1400, IAEA-450 and IAEA-395) byhousehold aluminum foils – Comparison

INAA, ICP-AES and ICP-MS

between comparative method and k0-IAEA

1

2

3

VU, C. D. , SUCGANG, R. , THIEN, T. Q. ,3

1

DOANH, H. V. , SHIRAI, N. , EBIHARA, M.
11method –MIURA, Y., OURA, Y.

2( Tokyo Metropolitan Univ., Philippine Nuclear(Tokyo Metropolitan Univ.)

3

Instrumental

Research Inst., Nuclear Research Inst.)

neutronactivation

analysis

Certified reference materials (CRMs) are(INAA) using the k0 method can determine all

greatly important in chemical analysis. They canelements that emit γ rays as it does not require abe used as reference standard or quality control

reference standard sample. However, somesamples. A survey of literatures reveals that theparameters, such as a neutron characteristics andnumber of published values for NIST-1400

an efficiency of a detector, should be determined(Bone Ash), supplied from the Institute ofprior to an elemental determination. In this study,

Science and Technology (NIST), and two ofhousehold Al foils were analyzed by k0-INAA to

IAEA-450 (Algae) and IAEA-395 (Urban Dust)evaluate impurity concentrations and their

supplied from International Atomic Energy

determination values were compared with those

Agency (IAEA), is very limited. In this study,

by a comparative method. Household Al foils

the multi-element abundances in these three

are often used in the cooking, and recently cheap

CRMs were determined. A combination of threeimported foils are marketed. Thus impurities instandardized

involving

Al foils are interesting. To evaluate theinstrumental neutron activation analysis (INAA),

determination values by the k0-INAA method,

inductively coupled plasma atomic emission

some reference materials were also analyzed.

spectroscopy (ICP-AES), and the inductively

Elemental compositions obtained by k0-INAA

coupled plasma mass spectrometry (ICP-MS)

method were fairly consistent within 10% withhas been applied to obtain a wide range of

those of literature values for most of elements.

elemental abundances in the mentioned samples.

For Al foil samples, V and Mn were determined

Our analytical data was evaluated by analyzing

from

NIST-1646a Estuarine Sediment. Our data for

determination

NIST-1400, IAEA-450 and IAEA-395 are insystematically about 10% smaller than those byanalyticalmethods- 205 -

irradiation

for

ten

seconds.

Thosevaluesbyk0-INAA

were

a comparative method. The concentrations of V

distributions of radioactive aerosols are an

and Mn in Al foils varied from 25 to 300 ppm

importantand from 14 to 220 ppm, respectively. It wasinternal dose. In this study, the number size

found that the amount of impurities vary greatly

distributions

according to the manufactures.

accelerator target room of KUR LINAC werefactoroftoestimate

aerosols

occupational

formedinthemeasured by a scanning mobility particle sizer(SMPS). Formed aerosols were also collected

3B07 INAA of Chinese medicine and herbs
1

2

3

FURUTA, E. , SATO, N. , OKUMURA, R. ,IINUMA, Y.

3

by a low-pressure cascade impactor and activityof aerosols collected on collection plates was

12( Ochanomizu Univ., IMRAM, Tohoku Univ.,

measured by a GM counter. In the target room, a3Res. Reactor Inst., Kyoto Univ.)

Ta target was irradiated with 30 MeV electron

At the APSORC13 in 2013, INAA results ofbeam and currents of 20-100μA for about two

Chinese medicine and herbs were reported. The

hours. The number of aerosols increased with

Niuhuang Jiedu Pian and the Liushen Wan,

beam current.

which were purchased with a doctor prescription

diameters of the number size distribution wasin China, added to As and Hg with extremely

approximately constant without depending onhigh concentration. Five kinds of the same

beam currents. Under the irradiation condition

named Chinese medicine were gotten by awith a current of 80μA, the median diameter of

personal import with the Internet and analyzed

activity size distribution of aerosols collected byby neutron activation and X-ray Diffraction

the impactor was about 1.3 times as large as that

(XRD) method. It was clear that both of the As

estimated from the number size distribution

and Hg were included in these samples by INAA

measured by the SMPS. This would be because

and their chemical forms were identified asthat small particles or gases attached tosulfide by the XRD analysis. It is considered thatcollection plates of the impactor.

However, the count medianthese minerals of realgar and cinnabar were90

added to some of these medicines named

3B09 Environmental

Niuhuang Jiedu Pian and Liushen Wan. Also it isconcentration in shallow well waterconsidered that these sulfides work to give a

KOU,

shock to the body without absorption of them.

OKAMURA, Y. 1, FUKAGAI, J.2

Other Chinese medicine and herbs were

(1Japan Nuclear Fuel Limited, 2Tokyo Power

analyzed and many kinds of elements wereTechnology Ltd.)

S.1,

OKA,

factors
M.1,

on

SASAKI,

Sr

K.1,

In the course of environmental radiation

detected in them, which were main elements ofmonitoring around RRP and related facilities,

the crust.

the concentration of 90Sr in water of one well
3B08 Factor Affecting Activity Distribution

gradually increased from 3mBq/L in 2003 andofreached 28mBq/L in 2011. Considering theRadioactive

Aerosols

FormedinAccelerator Target Room

specific activity of 90Sr and operation history of

YOKOYAMA, S.1, OKI, Y.2, SEKIMOTO, S.2

RRP, this phenomenon was attributed to fallout

1

from

2

( Fujita Health Univ., Kyoto Univ.)
In

accelerator

facilities,

particle

size

past

nucleartests.

For

furtherunderstanding, we studied from various aspects.

- 206 -

Results of the study were summarized as

field soil samples collected around Tokai

following. 1) Specific activity of 90Sr stayed

Reprocessing

constantof

inductively coupled plasma mass spectrometry

Sr(ICP-QQQ). At first, we found the bestnone

concentration of

the
90

less

of

increase

Sr. 2) Concentration of

90

Plant

by

triplequadrupole

correlated with electric conductivity (EC). 3) EC

measurement

value rapidly changed in short term. 4)

reducing the background intensity of m/z 129 byConcentrations of sodium and chloride showed129

better correlation with EC. 5) Small surface

ions such as 127IH2+. Iodine-129 concentrations

stream near the well connected with small sandin the field soils were then measured by thebasin, whose water level was influenced by

optimized ICP-QQQ protocol after isolatingsnow dumping.

iodine by combustion-solvent extraction method.

conditionof

ICP-QQQ

for

Xe included in plasma gas and polyatomic

Thus, following mechanisms were suggested.

The results of 129I concentrations agreed with the1) Concentration of 90Sr in the well water

values obtained by AMS. This suggested thechanged in accordance with non-radioactive

applicability of ICP-QQQ to determination ofsubstances. 2) The well water quality was a

129

mixturePlant.

ofsomecomponents.

3)

Land

I in field soil around Tokai Reprocessing

development and snow dumping might bereasons for gradual change of well water quality.

3B11

We concluded that the quality of the shallow

multi-elements including Pu

well water was easily affected by local condition

MIYAMOTO, Y., YASUDA, K., MAGARA, M.

and human activities.

(Research Group for Analytical Chemistry,

Sequential separation of ultra-trace

JAEA)
3B10 Application
determination of

129

to

Abundance and isotopic ratios of trace

I in field soil around Tokai

uranium, thorium, lead and lanthanides inof

ICP-MS

Reprocessing Plant

environmental samples play a key role to

NAGAOKA, M., YOKOYAMA, H., FUJITA,

investigate features of the samples. Plutonium isH.

an artificial element which originates from

(Japan Atomic Energy Agency)

nuclear bomb tests and accidental releases from

Iodine-129 (129I) has been discharged into the

nuclear power plants. The authors accomplishedenvironment from the nuclear weapons tests,

the development of technique for sequential

nuclear power plant accidents, and nuclear fuelseparation of U, Th, Pb, and the lanthanides

reprocessing plants. Therefore, the distribution

using a single anion-exchange column and

129

I in field soil around Tokai Reprocessing

mixed media consisting of hydrochloric acid,

Plant has been studied since 1982 by Japannitric acid, acetic acid, and hydrofluoric acid in

Atomic Energy Agency. Neutron activation

the previous work. The chemical composition ofanalysis and accelerator mass spectrometryeluents for separation of Pu and Th was(AMS) have been used for the determination of

optimized

129

I. However, both methods depend on theseparation of multi-elements including Pu. The

operation schedule of the facility. In this study,

mixture of 11 pg of Pu and 200 pg of Th wasofwe examined the possibility to determine

129

I in

to

accomplishthesequential

completely separated, and >95% of these- 207 -

elements were recovered by a single anion(JAEA)

exchange column with the mixed-media of 70

In the Mizunami Underground Research

vol.% acetic acid, 2 M HCl, and 0.1 M HF. By

Laboratory of Japan Atomic Energy Agency,

using this mixed-media for separating Th and Pu,

horizontal tunnels and vertical shafts aretheultra-trace

excavated, and many kinds of observation ofmulti-elements including Pu was accomplished.

underground environment are performed as

This work was supported by financial aids

geoscientific research related to the geologicalfrom the Ministry of Education, Culture, Sports,

disposal technology of high-level radioactive

Science and Technology (MEXT) of Japan

waste. Since the geological feature of this area

(Scientific Research (C): Grand No. 25340078).

mainly consists of granite, measurements of thesequential

separation

of

radon

equilibrium

equivalentconcentration

3B12 Alpha-ray measurement of dissolved(EECRn) in the underground research facilities

plutonium particle on the TIMS filamentand dose evaluation to workers were performed.

YASUDA, K., SUZUKI, D., KANAZAWA, K.,

EECRn was measured intermittently using an

MIYAMOTO, Y., ESAKA, F., MAGARA, M.

instrument WLM-Plus (Tracerlab Co., Ltd.) in(Japan Atomic Energy Agency)

2012 and 2013. The measurements wereIn order to detect of undeclared activities in

performed at two locations, where relatively

nuclear facilities, we develop to technique ofhigh EECRn values were observed before, at asafeguards environmental sample analysis indepth of 300m below the surface. Trends to

JAEA. As part of this effort, isotope ratio

increase EECRn during summer as a seasonal

analysis of individual MOX particle wasvariation were observed, because the natural

performed using by TIMS without chemicalventilation

treatment. It is possible to estimate an age

suppressed by high air temperature outside. The

determination of plutonium purification by amaximum value of 3,300 Bq/m was measured

combination of the plutonium isotope ratios andin July 2013. During the workers entrance time(Pu-238+Am-241)/(Pu-239+Pu-240)

alphazone, 10:00 to 15:00 when ventilation blowers

activity ratios were obtained by the alphawere operated, the maximum EECRn of 1,880

spectrometry. Since the plutonium particle size

Bq/m was observed in July 2013 and theis more than 1 µm due to the influence ofmonthly maximum average value was 765

self-absorption, exactly measurement of the

Bq/m in August 2013. Using the monthly

activity ratios has been difficult. Therefore, weaverage EECRn, the annual effective dose towere examining how to acid dissolution in theworkers was estimated to be about 0.35 mSv on

plutonium particles on the TIMS filament before

the assumption of 10 hours working time at thealpha spectrometry.

area per each month.

3B13 EEC radon in underground research

3B14 North-south

facilities

concentration in seawater in the Indian

FURUTA, S., IKEDA, K., MIKAKE, S.,

Ocean

IMAEDA, Y., NAGASAKI, Y., SUZUKI, H.,

YAMAGATA, T.1, INOUE, K.2, TAZOE, H.3,

NOMURA, Y.

MATSUZAKI, H.4, NAGAI, H.1- 208 -

ofundergroundfacilities

transection

of

was

Be-10

(1Nihon Univ., Grad. Sch. of IBS, 2Nihon Univ.,from natural quartz and feldspar has been used

Inst. of REM, 3Hirosaki univ., 4MALT, Univ. ofin retrospective dosimetry, dating of sediment,

Tokyo)

etc. In the application target minerals must be

Cosmogenic nuclide Be-10 (half-life 1.36 Ma)

extracted

with chemical

separation

which

is produced by nuclear interaction between

requires cumbersome work. Nowadays, pulsed

secondary cosmic ray and atmospheric nitrogen

optically stimulated luminescence (P-OSL) was

and oxygen. Because of Be-10 widely spread indeveloped to separate luminescence signal fromthe ocean and the residence time is shorter thanbetween quartz and feldspar as instrumental

ocean-mixing time, the Be-10 concentrations inseparation. The purpose of this study is to try

seawater could be a useful tracer for the ocean

apply the P-OSL to Japanese surface soil ascirculation. It is necessary accumulation ofretrospective dosimetry with easy physicaloceanic Be-10 to assess Be-10 as a tracer for

separation.

water mass. In this presentation, the north-south

In this study, a P-OSL instrument wastransection of Be-10 concentration shows indeveloped by the author. Performance of the

Indian Ocean during R/V Hakuho-maru in the

instrument was tested using natural quartz

KH09-5 cruise, and discuss a migration of

extracted from Japanese surface soil and

Be-10.

feldspar in mineral specimens. By using a

The concentration of Be-10 is high in 20-40˚Smixture of the quartz and feldspar, the P-OSL

and low in the south area of 40˚S, which is the

protocol was improved to determine theAntarctic Ocean, and between 20˚S and 20˚N inirradiation dose. Following irradiation using

surface. According to hydrological data, Be-10

X-rays, dose recovery test was conducted andconcentration in Antarctic intermediate waterthe(AAIW) is relatively low concentration. The

reconstructed by the P-OSL protocol. Moreover,

AAIW come from the low concentration surface

as-received surface soils were irradiated withwater of the Antarctic Ocean. In deep-sea, theCo-60 source of the Research Reactor Institute,

water mass, which named Common deep water,

Kyoto University and used in the dose recovery

has high concentration. The Common deep

test.

water is originated from Atlantic deep sea, butreconstructing the irradiated dose. From these

the concentration of Be-10 in the Atlantic Ocean

results, it was concluded that the P-OSL

is lower than Common deep water. It is consider

dosimetry is suitable for accident evaluationthat the Be-10 in the surface Antarctic Ocean isalthough further research is required to improvetransported down to the Antarctic deep sea by

the protocol using various kinds of Japanesebiogenic particles in Antarctic Ocean.

surface soils.

3B15 Application
stimulatedofluminescence

irradiatedThe

pulsedoptically

3B16

using

naturalresistance

test

dose

was

was

also

successfully

successfulinStudy on tardigrades with radiation

mineral to retrospective dosimetry

MIYAZAWA, T.1, OYA, Y.2

FUJITA, H.1(1Shizuoka Univ. Divi. of Tech. Serv., 2Shizuoka(1Japan Atomic Energy Agency)

Univ. Grad. Sch. of Sci. )Optically stimulated luminescence (OSL)- 209 -The tardigrades belong to a group which havea close relationship to an arthropoda and aresuch as halide ions. However, little has beenaquatic animal with a length of 1mm or less.

reported on chemical experiments of Rf with

Many tardigrades live in terrestrial mosses andorganic ligands. In this study, we carried out thelichens. The bodies of tardigrades are short,solvent extraction of zirconium (Zr) andplump, and ventrally there are four pairs ofhafnium (Hf) as lighter homologs of Rf using

stubby legs and each leg have four to eight

2-thenoyltrifluoroacetone (TTA) as a chelateclaws.

extractant toward the Rf experiment. In thisTardigrades exhibit remarkable ability toexperiment, radiotracers 88Zr and 175Hf werewithstand for extreme environment. When theused. These radiotracers were produced in themosses become desiccated the tardigrades

89

contracted and shriveled, and pass into an

using the AVF cyclotron at Tohoku University.

anabiotic state. An animal in such a condition is

Aqueous solution of 1 M HNO3 containing thecalled a tun. When water is again present, theradiotracers was mixed with an equal volume ofanimal swells and becomes active within a few

TTA in toluene solution, and the mixture wasminutes. Tardigrades recover after immersion

then shaken for 5 hours. The radioactivity offrom tun.

each phase was measured by a Ge detector. The

Y (p, 2n) and 175Lu (p, n) reaction, respectively,

We investigated the effects of environmental

results showed that the distribution ratio (D) ofstress on tardigrades (Milnesium tardigradum) ,Zr is approximately 10 times greater than that ofsuch as examined the effects of high or low

Hf. The log D vs. log [TTA] plot indicated thattemperature, and gamma-rays. Especially wethe extracted TTA complexes of Zr and Hf

examined the effects of gamma-ray irradiation

presumably contained OH- or NO3- ion as

equipment in Radioscience Research Laboratory,

ligands in this experimental condition. In the

Faculty of Science, Shizuoka University.

symposium, we will also report on the results of

We found that tardigrades withstand high orsolvent extraction from perchloric acid solution.

low temperature, and 4000 Gy gamma-rays. This
result suggests that tardigrades have a great

P02

abilityusing

towithstandradiation

than

other

organism.

Solid-liquid extraction of Zr and Hf
automated

solid-liquid

extraction

apparatus for element 104, Rf, experiment
YOKOKITA, T.1, KINO, A.1, SHIGEKAWA, Y.1,

P01 Study on solvent extraction behavior of

TOYOMURA,

K.1,

NAKAMURA,

K.1,

zirconium and hafnium as homologs of

KASAMATSU,

Y.1,

TAKAHASHI,

N.1,

rutherfordium (element 104) with chelate

YASUDA, Y.2, YOSHIMURA, T.3, KOMORI,

extractant

Y.1, HABA, H.4, KANAYA, J.4, HUANG, M.4,

TANAKA, A.1, OOE, K.1, KIKUNAGA, H.2,

MURAKAMI, M.4, SHINOHARA, A.1

GOTO, S.1, KUDO, H.3(1Grad. School of Sci., Osaka Univ., 2School of(1Grad. School of Sci. and Technol., Niigata

Sci., Osaka Univ., 3Radioisot. Res. Center,

Univ.,

2

Research Center Elec. Photon Sci.,

Osaka Univ., 4RIKEN Nishina Center)

Tohoku Univ., 3Fac. Sci., Niigata Univ.)

Solid-liquid

extraction

of

Zr

and

Hf,

Chemical studies on rutherfordium (Rf) havehomologues of Rf (Z = 104), by Aliquat 336

been carried out mainly with inorganic ligands

resin from hydrochloric acid (HCl) were

- 210 -

batch-type

Prevention Research Inst., Kyoto Univ., 3School

solid-liquid extraction apparatus for repetitiveof Eng., Univ. of Tokyo., 4KEK., 5Shimizu

extraction experiment on Rf. The Zr and Hf

Corporation.,

species adsorbed on the resin in 10 M HCl were9

stripped by washing the resin several times with

California Berkeley, 13RIKEN)

performed

using

automated

6

JAEA., 7ATOX., 8Fermi Lab.,

Osaka Univ., 10RCNP., 11Purdue Univ., 12Univ.

~0.25 mL of 4 M HCl. The back extraction

By accelerator mass spectrometry (AMS), we

yields of Zr were higher than those of Hf. The

have measured the 10Be and 26Al production

back extraction yields of Zr and Hf decreased

cross sections from Y, Tb produced by 120 GeV

with

336

and 400 MeV protons. The proton irradiation atconcentration. Under these conditions, constant

120 GeV and 400 MeV were performed at Fermi

distribution coefficients (Kd) were obtained in

National Accelerator Laboratory (FNAL) andrepetitive ~100 times extraction experiments of

the Research Center for Nuclear Physics

Zr and Hf without renewing the resin. Using this(RCNP), Osaka University, respectively. The

apparatus, we performed solid-liquid extraction

AMS measurements were performed at MALT

anincrease

89m,g

of

the

Aliquat169,173

Hf produced by(University of Tokyo). We will present thenuclear reactions and transported continuously

correlation between the cross section data offrom the nuclear reaction chamber by the10

He/KCl gas-jet system at RCNP and RIKEN.

discuss the taget mass dependence in those crossThe dependences of the Kd values of Zr and Hf

sections.

employing

Zr andBe and 26Al and the target mass number andon the shaking time were obtained in the online
experiment in 9 M HCl. The Kd values in online

P04

experiment were in agreement with those in theof BiCl3

offline experiment.

ASAI, T.1, GOTO, S.1, OOE, K.1, KUDO, H.2

Isothermal chromatographic behavior(1Grad. Sch. Sci., Niigata Univ., 2Fac. Sci.,
P03 Measurements of cross sections for

Niigata Univ.)
In the study of super heavy elements, aproduction of light nuclides by 120 GeV andtechnique of an isothermal chromatography has

400 MeV proton bombardment of Y
1

1

OKUMURA, S. , SEKIMOTO, S. , YASHIMA,

been often used to determine adsorption

H.1, MATSUSHI, Y.2, MATSUZAKI, H.3,

enthalpies of volatile compounds. The results of

4

4

MATSUMURA, H. , TOYODA, A. , OISHI,
5such experiments have been analyzed mostly

KASUGAI,

6

Y. ,using Monte Carlo method. In this simulation,

NAKASHIMA,

6

H. ,

experimental parameters such as a column

BOEHNLEIN, D. , COLEMAN, R. , LAUTEN,

length and radius are necessary but they have

K. ,

6

MATSUDA,

N. ,
7

Y. ,

SAKAMOTO,

8

8

8

8

N. ,

more or less uncertainty. Therefore it is8

necessary to ascertain an accuracy of adsorption

NINOMIYA, K. , SHIMA, T. , TAKAHASHI,

enthalpy for a typical material. In this study, we

G. ,LEVELING,

8A. ,MOKHOV,

8

8

9

10

RAMBERG, E. , SOHA, A. , VAZIRI, K. ,
9

9

11

N. , SHINOHARA, A. , CAFFEE, M, W. ,12

13

NISHIIZUMI, K. , SHIBATA, S. , OHTSUKI,
1( Res. Reactor Inst., Kyoto Univ.,

typical material, because we can easily handle
212

T.
1

consider whether volatile BiCl3 can be used as a
Bi as a tracer from the naturally occurring

2

Disasterradioactive series. First of all, we have

- 211 -

investigatedisothermal

chromatographic

266

Bh. The identification was based on a

behavior of BiCl3 in macro-scale. BiCl3 is

genetic link to the known daughter nucleus 262Db

deliquescent and changes to nonvolatile BiOClby α-decay. Thus, the decay chains from 266Bh

when rapidly heated. So, it needs to dehydrate

were well established. Therefore, we concluded

BiCl3 by gradual heating at 100°C while flushingthe 3 decay chains from 278113 are clearlyIn this experiment, BiCl3 was heated atconnected to the anchor nuclides and the

He gas.

100 °C for 1 hour with He flow (0.8 L/min) at
atmospheric

innerpressure.

Then,productions of 278113 are clearly confirmed.

thetemperature was raised at 500 °C and volatile

P06 Excitation functions for the natHf(α,x)

compound was transported to a collection

reactions

position. The amount of collected Bi was

MURAKAMI, M.1,2, HABA, H.2, SHIBATA, S.2,

determined

KUDO, H.3

withspectrophotometryusing

thiourea. The result was that the quantity of(1Grad. School of Sci. and Technol., Niigata

collected BiCl3 reached maximum at between 1

Univ., 2RIKEN Nishina Center, 3Fac. of Sci.,

and 3 min. It was found that BiCl3 started to

Niigata Univ.)
We previously investigated the production of

evaporate from ~250 °C immediately.

a long-lived Ta isotope, 179Ta (T1/2 = 1.82 y), in
P05 Summary on the 113th element search

the natHf(p,x) and natHf(d,x) reactions for theusing GARIS

basic chemical studies of 105th element, Db.

KAJI, D.1, MORIMOTO, K.1, HABA, H.1,

However, 179Ta emits no γ rays in its EC decay

MORITA, K.1,2

and therefore it is assayed by measuring the1( Nishina Center, RIKEN,

2

Faculty of Sci.,

characteristic X rays of Hf. The isotope 182Ta(T1/2 = 114.74 d) is a more useful radiotracer

Kyushu Univ.)
During ten years from 2003 to 2012, we havebecause it emits characteristic γ rays. In thisstudied on a production and decay properties ofwork, we investigated the production of 182Ta bya new superheavy nuclide 278113 produced by

the α-induced reaction on natHf.

209

Bi(70Zn,n)278113 using a gas-filled recoil

A stack of the thin foils of natHf and natCu wasseparator GARIS. Totally 3 decay chains due toirradiated by the 50-MeV α beam for 31 min.

the 278113 were observed during net irradiation

The average beam current of 0.23 μA wastime of 576 days. The 1st and 2nd decay chains

determinedconsist of four alpha decays from

278

Md.

reaction. After the irradiation and proper coolingDb.

duration, γ rays of each foil were measured by afrom 3 decay chains were consistent each other.
produced by248

Ge detector.

Observed decay properties

In 2009, we also tried to search for the23

monitorBh,

The 3 chain was consist of 6 alpha decays andconnected toCu(α,x)67Ga

262

rd

254

nat

266

113 toand then ended by spontaneous fission ofby the

266

Bh

266

Cm( Na,5n) Bh to establish

In this work, the cross sections of thenat

Hf(α,x)176,177,178W,

175,179m2

Hfreactions

measured

excitation

175,176,177,178,182,183

Ta,

were

measured.

function

for

The
the

the connection to known nuclides and the

nat

182

cross-bombardment. As a result, totally 14

cross section of 8.3 ± 0.3 mb at 41.5 ± 1.2 MeV.

events were assigned to decay chains from

Based on the measured cross sections, theHf(α,x) Ta reaction exhibits the maximum- 212 -

thick-target yield of 182Ta was deduced to be 5.2(1Grad. Sch. Sci., Niigata Univ., 2Fac. Sci.,

kBq/μAh.

Niigata Univ.)
To clarify chemical property of element 104,

P07 Measurement

of

cross

Rf, gas chromatographic behaviors of chlorides

Mo(d,x)of Rf and its homologs, Zr and Hf, have been

production

sections of Tc isotopes in thenatstudied in a single-atom scale. The reported

reactions
1

1,2

1

KOMORI, Y. , MURAKAMI, M. , HABA, H. ,SHIBATA, S.

1sequence of volatility was Zr ≳ Rf > Hf. But thisvolatile relation between Zr and Hf chlorides

1

2( RIKEN Nishina Center, Grad. School of Sci.

differs from sequence of sublimation expected

and Technol., Niigata Univ.)from their vapor pressure curves in the

We plan to conduct model experiments for

macro-scale. Appropriate explanation about thischemical studies of element 107, bohrium using

difference has not been given until now. In thisits homologues, Tc and Re radioisotopes. In thisstudy, we investigated gas chromatographic

work,

of

behaviors of Zr and Hf chlorides at off-line todeuteron-induced nuclear reactions on natural

clarify this contradiction. In macro-scale, wemolybdenum have been measured up to 24 MeV

obtained isothermal chromatographic data of Zr

for the quantitative production of the Tc isotopes.

and Hf chlorides. With analyzing these retention

The target stack of Mo/Ti/Ta foils was irradiatedcurves, it was found that HfCl4 is more volatilefor 1 h with the 24-MeV deuteron beam supplied

than ZrCl4, which agrees with the volatility

from the RIKEN AVF cyclotron. After the

deducedirradiation, each foil was subjected to γ-ray

investigate

spectrometry. The beam current of 0.17 μA wasbehavior follows the model of mobile adsorption,

production

cross

sections

determined by the monitor reaction

nat

48

Ti(d,x) V.

from

the

vapor

pressure.

To

whetherthischromatographic

we are going to perform the experiment of the

The excitation functions were measured for theisothermalnatusing radioactive tracer. In the symposium, theMo(d,x)93m,99,101

93m,93g,94m,94g,95m,95g,96m,96g,97m,99m,101

Tc,

Mo, 90g,92m,95m,95g,96gNb, 89gZr reactions.

They were discussed by referring to previously

gaschromatography experimentexperimental conditions and the results will bepresented in more detail.

reported data and to the theoretical model code
TALYS. Most of our results are in good

P09 Solvent extraction behavior of Mo andagreement with the previously reported data,

W from oxalic acid solution by Aliquat 336

though there is little agreement between the

GOTO, N.1, OOE, K.1, MURAKAMI, M.1, 6,

experimental values and the theoretical ones.

GOTO, S.1, TSUKADA, K.2, TOYOSHIMA, A.2,

Thick-target yields for the investigated isotopes

ASAI, M.2, SATO, T. K.2, MIYASHITA, S.3,

were deduced from the measured production

KANEYA, Y.2, 4, KITAYAMA, Y.5, HABA, H.6,

cross sections.

KOMORI, Y.6, KUDO, H.7(1Grad. School Sci., Niigata Univ., 2JAEA, 3Grad.
chromatographic

School Chem., Hiroshima Univ., 4Grad. School

behavior of Zr and Hf chlorides at off-line

Sci. Tech., Ibaraki Univ., 5Grad. School Nat. Sci.

experimentTech., Kanazawa Univ.,

P08

Isothermal

1

gas

1

1

OSHIMI, Y. , GOTO, S. , OOE, K. , KUDO, H.

2

Univ.)- 213 -

6

RIKEN,

7

Niigata

In this work, ion-pair extraction behavior of
molybdenum (Mo)homologsofand tungsten

seaborgium

(Sg)

(W)
has

clarify the deexcitation process of 235mU byasmeasuring the decay constants and the energy

been

spectra of the internal-conversion electrons forinvestigated with Aliquat 336. Radiotracers

235m

93m

we developed an apparatus for collecting 235mU

H2C2O4 (oxalic acid)/0.1 M HCl/0.9 M LiCl

recoiling out ofsolution, and the solution was shaken withperformance of the apparatus by using 224Ra

Aliquat 336/toluene solution. After separation ofrecoiling out of 228Th. The collection yields ofthe aqueous and organic phases, distribution

224

ratios (D) of Mo and W were calculated from thevoltages, air pressures, and 228Th source shapes.

radioactivity in each phase measured by γ-ray

Based on these results, we determined suitable

Mo, 176W and 181W were dissolved in 10-2 M

U with various chemical forms. In this work,
239

Pu. We evaluated the

Ra were determined in various applied

spectrometry with a Ge detector. In theexperimental conditions for the collection ofexperiment of extraction kinetics, D values of235m

Mo and W were constant in shaking time longer

apparatus for the low-energy internal-conversion

than 30 s. This result shows that the extraction

electrons are under development.

U from 239Pu. In addition, the detection

kinetics of Mo and W with Aliquat 336 from
oxalic acid solution is fast. Moreover, the D

P11values of Mo and W as a function ofsuperheavy element study

concentration of Aliquat 336 were investigated.

KAJI, D.1, MORIMOTO, K.1, WAKABAYASHI,

Slopes in the D value vs. [Aliquat 336] plot on a

Y.1, TAKEYAMA, M.1,2, TOKANAI, F.1,3, ASAI,

logarithmic scale were evaluated to be 2.1 forM.4

Mo and 1.3 for W. This indicates that the net(1Nishina Center, RIKEN, 2Grad. Sch. of Sci.

charge of the extracted anionic oxalate complex

and Eng., Yamagata Univ., 3Faculty of Sci.,of Mo is -2, while that of the extracted W

Yamagata Univ., 4JAEA)

R&D of focal plane detector for

Superheavy

complex is -1, suggesting that chemical species(SHE)

element

devicedevelopment team in RIKEN has developed aof W is different from that of Mo.

new focal plane detector to study on production
P10 Development of a collection apparatus

and decay properties of SHE nuclide using afor recoil products toward the study of thegas-filled recoil separator GARIS and GARIS-II.

deexcitation process of U-235m

Conventional identification method of SHE

1SHIGEKAWA,

Y. ,SHINOHARA, A.

1

1

KASAMATSU,

Y. ,nuclide was based on the genetic relation
between mother and daughter, was obtained1( Grad. Sch. Sci., Osaka Univ.)from measuring the α-decay and spontaneous

235m

U has very low excitation energy (76.8

fission (SF) by Si detector box. So, detailedeV) and decays predominantly by the internal

decay scheme including γ-decay could not be

235m

U is

obtained. In 2013, we newly installed a Si-Ge

caused by the interaction between the nucleus

detector array at the focal plane of GARIS for

and outer-shell electrons, and thus the variation

studying on production and decay properties ofof the decay constant depending on its chemical

reaction products by 248Cm+48Ca. The detector

environment was reported. We are aiming toarray is also useful as a probe for detection of

conversion process. The deexcitation of- 214 -

prompt γ-ray coincided with SF. Before the

CHIYONISHIO, I.6, GOTO, N.5, TSUTO, S.5,

experiment on the 248Cm+48Ca, we calibrated the

NAGAOKA, T.5, OOE, K.5, TANIGUCHI, T.1,

Si-Ge detector array using nuclear reactions of

UENO, S.1, HAYASHI, K.1, YOKOYAMA, A.6

207(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,

Pb(48Ca,2n)253No,

208

Pb(48Ca,xn)256-xNo[x=1,2,3], and 206Pb(48Ca,2n)252No. In this report,

2

RIKEN., 3JAEA., 4Research Center for Elec.

the results on the first α-γ(X) and SF-γ

Photon Sci., Tohoku Univ., 5Grad. School Sci.,

spectroscopic study at the focal plane of GARIS

Niigata Univ., 6Kanazawa Univ.)

will be given in detail.

Studiesonthefluoridecomplexof

Rutherfordium (Rf), a super-heavy element, had
P12

R&D of target for superheavy element
1,2

KAJI, D. , TANAKA , K. , MORIMOTO, K.
1

performedbyacation-exchange

chromatography method in HF/HNO3 solution.

production and its monitoring system
1

been

1

Speciation of the Rf complex is, however, still

2( Nishina Center, RIKEN, Grad. Sch. of Sci.

open question. We, therefore, aim to clarify

and Tech., Tokyo Univ. of Sci.)

cationic fluoride species of Rf in aqueous

In order to produce a superheavy element

solution and to determine its formation constant.

(SHE), it is necessary a target system to standAt present, we focus on the extraction with anagainst high intense heavy-ion irradiation.

acidic chelate extractant, TTA, sensitive to

Conventionally, a thermal damage such as avalence of the metal complex. In the present

melting of target material is avoided using a

study,

gas-cooled rotating target system for the heaviest

chromatography

element

thermalexperiments were performed using carrier-free

conduction, convection, and radiation as a

Zr and Hf radiotracers in HF/HNO3 solution tocooling process of target. It is important in target

examinedevelopment to know the cooling mechanism

TTA-reversed-phase chromatography to Rf.

and the time scale for cooling. So, we measured

Distribution coefficient (Kd) values of Zr and Hf

the target’s temperature increased by heavy-ion

in both the experiments were determined andirradiation

thermometer

were compared in a wide range of the fluoride

without contact. In this report, we will discuss

ion concentration. It is found that the fluoride

about

mechanism.

complexes of Zr and Hf are increasingly formed

Additionally, we will also introduce an on-linewith an increase of fluoride ion concentration.

target monitoring system.

The Kd values obtained in the chromatography

production.

using

the

a

There

radiation

target's

coolingareon-linethe

TTA-reversed-phase
and

batch

applicability

extraction

of

the

experiment agreed well with those by the batch
P13 Adsorption behavior of Zr and Hf bymethod at higher concentrations of fluoride ion.

TTA-reversed-phasefor

Besides, clear difference of Kd values between

aqueous chemistry of a super-heavy element

Zr and Hf was observed in the concentration

Rf

range of > 2×10－5 M. These indicate that thechromatography

FUKUDA, Y.1, KITAYAMA, Y.1, HABA, H.2,
TSUKADA,KIKUNAGA,MURAKAMI,

3

K. ,TOYOSHIMA,

4

H. ,

HUANG,
2,5

M. ,present conditions are promising for our future

3

Rf

2

chromatography.

A. ,

M.

H. ,

KOMORI,2

Y. ,- 215 -

experiment

with

TTA-reversed-phaseP14 Effect of excited states in atom and ion

determination of EFGs. In the present study,

contributing

therefore, we have focused our attention on the

to

the

surface-ionization

efficiency

second excited state of 19F (I = 5/2) fed through

ASAI, M., SATO, T. K., KANEYA, Y.

the(JAEA)

controversial quadrupole moment of the state.

β-

decay

of

19

O

to

determinetheTo determine the first ionization potential of

Because the half-life of 19O is as short as 26.9s,

the heaviest actinide Lr, we have newly

however, it is difficult to introduce the nuclides

developed the surface ionization method which

into samples by usual chemical operations.

can be applied to the elements with short

Therefore, we are now working on thehalf-lives and very low production yields. To testdevelopment of an online PAC measurement

the applicability of this method, we havesystem coupled to an accelerator, where theinvestigated a relationship between ionization

recoilpotentials and surface ionization efficiencies ofreaction ofvarious short-lived lanthanide elements. We

kinetically in the sample of interest, so as tohave found that the effect of excited states indetermine the Q moment by making use of a

atoms and ions largely contributes to thetheoretical EFG.

19

O nuclei produced by the nuclear
18

O(d, p)19O can be implanted

measured ionization efficiencies of lanthanide
elements.

P16 Study of dilute magnetism for Co and
Mn codoped ZnO by means of emission

P15 Development of an online perturbed

Mössbauer spectroscopy

angular correlation measurement system for

KANO, Y.1, SUZUKI, T.1, SATO, W.1,2

the application of the short-lived 19F(←19O)(1Grad. School Nat. Sci., Tech. Kanazawa Univ.,

probe

2
1

Inst. Sci. Eng., Kanazawa Univ.)

1

FUJISAWA, T. , SHIMADA, M. , MIHARA,
2

M. , SATO, W.

1,3

Local structures and dilute magnetism in
Zn1-2xCoxMnxO (where x = 0, 0.01, or 0.03)(1Grad. School Nat. Sci., Tech. Kanazawa Univ.,

synthesized by a solid-phase reaction were2

Grad. School Sci., Osaka Univ., Inst. Sci. Eng.,

investigated by means of X-ray diffraction

Kanazawa Univ.)(XRD) method and Mössbauer spectroscopy.

3

It

It is important to obtain information on local

was found from the XRD patterns that all thestructures surrounding fluorine (F) atoms insamples have a hexagonal wurzite structure oforder to study physical properties of matter

ZnO matrix with no secondary phases detected.

containing F atoms. For that purpose, we have

Local fields at 57Co impurities were measured byadopted the perturbed angular correlation (PAC)

emission Mössbauer spectroscopy, and notechnique, and are trying to measure electric

ferromagnetism

19

was

observed

atroomfield gradient (EFG) at the F probe nucleus, thetemperature. For the spectral analysis, therefore,

only stable isotope in F, by introducing the probe

we assumed two doublet components.

19

The

into samples. However, the ground state of F

values of the isomer shift and quadrupole

does not have quadrupole (Q) moment because

splitting of the main components observed forthe nuclear spin of the state is I = 1/2, signifying

each sample showed good agreement with eachthat the ground state can not be applied for theother within their uncertainties. It was found- 216 -

from their agreement with the literature values

the δ and e2qQ values for 3, 6 and 7 are close tothat Co2+ ions contributing to the main

those

2+

component occupy substitutional Zn

sites. Asoforganoiron

fragments

such

as

FeCp(CO)2 and FeCp(CO)PPh3.

for the minor second component, it wasobserved that its fraction is raised with2+

increasing concentration of the co-dopants, Co
2+

P18

Development of the measurement of

neutron-induced reaction cross-sections of theand Mn , in ZnO. For detailed understanding

minor actinides

of local structures and dilute magnetism in ZnO,TAMURA, N.1, NISHIO, K.2, HIROSE, K.2,

mere room-temperature measurement is not

NISHINAKA, I.2, MAKII, H.2, KIMURA, A.2,

sufficient. We are thus now working on the

OOTA, S.2, ANDREYEV, A.3, VERMEULEN,

introduction of a low-temperature Mössbauer

M.3,

spectrometer in our facility.

NAGAYAMA, T.4, OOE, K.1, GOTO, S.1,

S.3,

GILESPIRE,

M.3,

BWNTLY,

KUDO, H.5
P17

121

Sb

pentacoordinatedof(1Grad. Natural Science Niigata Univ., 2 Japan

Au(I)

Atomic Energy Agency., 3York Univ., 4Ibaragi

Mössbauer

spectrastiboranes

withUniv., 5Niigata Univ.)

fragments
OHNO, S.1, SATO, A.1, TAKAHASHI, M.1,
MATSUKAWA, S.

1

High-level radioactive waste which was
produced by driving the nuclear reactor includes

1( Toho Univ.)long-life nuclides, especially Minor Actinides

Rf2SbAuL (Rf = mono anion of hexacumyl(MA) such as Np, Am, and Cm. MAs are kept

alcohol : L = (PPh3)2, P(p-Tol)3, P(o-Tol)3,

completely isolated from the biosphere, but theirPMes3, PCy3, PEt3, SMe2) are synthesized toradiation may influence the environment for

obtain information on the Sb−Au interactions.

thousands of years to come. To solve that121

Sb Mössbauer spectra of Rf2SbAuP(o-Tol)3

problem, it is suggested reprocessing MAs as(3), Rf2SbAuPEt3 (6) and Rf2SbAuSMe2 (7) are

fuel and transmuting MAs into other short-life

measured at 12 K using a Ca121mSnO3 source (16nuclides by an Accelerator Driven reactor

MBq). The Mössbauer spectra are typical ones

System (ADS). In the development of suchfor trigonal bipyramidal stiboranes and havesystems,large negative quadrupole coupling constants

neutron-induced(e qQ). Isomer shift (δ) and e qQ values for 3, 6

cross-section of MAs are necessary.

22and 7 (δ = 2.39 − 2.45 and e qQ = -22.1 −2-1accurateandfissionprecision
and

data

of

captureThe neutron-induced fission and capture-23.9 mm s ) are intermediate between those ofcross-sections of 241Am which is typical MA

stiboranide [Rf2Sb-][NEt4+] (I : δ = -1.37, e2qQ =have been measured using various techniques.

-1-24.9 mm s ) and a typical pentacoordinated

Our experiment was performed at the JAEA

stiborane Rf2Sb(p-Tol) (A : δ = 4.16, e qQ =J-PARC facility. 241Am sample is sealed up with

-18.3 mm s-1). These results indicate the electron

an aluminum case. Therefore fission fragments

densities in the equatorial plane are greater thancannotthat of A. The same results are obtained for thesimultaneous measurement of prompt neutrons

similar hypervalent Sb compounds having theand gamma-rays by liquid scintillation counters

Sb−M (M = Fe, Ru, Cr, Mo, W) σ bond. Bothallows to decide the cross-sections. In the2- 217 -bemeasured

directly.

However,presentation, the neutron-induced fission and

There is a very valuable sample in thecapture cross-sections obtained by this techniqueenvironmental samples. Therefore, it cannot be

will be demonstrated and discussed the results inmeasured by physical destruction. And so, it

detail.

was attempted that the dummy gamma-ray
source is manufactured by using a 3D printer.
Development of rapid dissolution andAs a result, with the use of a reagent

pre-concentration in sequential analysis of Pu

involving natural radionuclide, it was possible toand Am in soil samples

create a detection efficiency curve to match the

SUZUKI, K., UESUGI, M., YOKOYAMA, A.,

shape of the dummy gamma-ray source.

NAKANISHI, T.

Therefore, it has become possible to create(Gread. School Nat. Sci. Tech., Kanazawa Univ.)

dummy gamma-ray source with high accuracy in

P19

Pu and Am isotopes generated in nuclear fuela short period of time.

are supposed to be released from Fukushima
Nuclear Power Plant in March, 2011. In a

P21 Investigation

sequential analysis at the trace level of Am andStrontium-90 by using Cherenkov Counting

Pu, it is necessary to remove interfering

KAWASAKI, N.1, TAMARI, T.1

substance through repeated purification and(1Kyusyu

separation. In thisAssociation)

study, we aim to establish aforMeasurement

Environmentalof

Evaluation

quantitative analysis of Pu and Am in a soil

Strontium-90 (Sr-90) is one of the most

sample in a rapid manner of the processes. We

important radionuclides among fission products

focused attention on the improvement of the

because of its long half-life and its retention by

problems of dissolution and pre-concentration.

the body.

byGas Proportional Counter (GPC) is often usedammonium nitrate fusion, and the concentration

for the Sr-90 measured in environmental

by manganese di-oxide sorption. Next, we

samples,compared the filtration method with the

Scintillation Counter (LSC) has also been

electrodeposition method for the preparation ofstudied for a long time, it is known thatan americium α-ray source. After that we studied

described

the application of these methods to soil samples

monitoring method.

First,

weexaminedthedissolution

Cerenkovinenvironmental
production

forgamma-ray

2

SAITO, T. , KOIKE, Y. , SUZUKI, R.
1

environmental

Liquidradiation

samples

accurately,itisnecessary to evaluate background and efficiency,
because FOM (figure-of-merit) for LCS is lower

emitting source applied by a 3D printer1by

In order to measure low-level concentrationfrom Fukushima.
P20 Trial

theCounting

2

than GPC. The experiments were carried out to2( Shokei Gakuin Univ., Sch. Sci. & Tech., Meiji

compare FOM with various vials by measuring

Univ.)

the efficiency and the background. The result

When the radioactivity in environmental
samples

was

spectrometry,

quantified

bygamma-raygeometric conditionsof theshows that low density poly-vial (inner Teflon
courting) has high FOM and an advantage
economically.

sample greatly affect the measurement.

- 218 -

P22 Gamma-ray
radionuclides

spectrometry

instandardofsamplewith(1Kyoto University Research Reactor Institute,2

Grad. Sch. Agri., Kyoto Univ.)
A significant amount of Te-127m (1.1×1015

detection efficiency curve using chemicalBq) was released into the environment by thereagents
SUZUKI, R.1, MATUDA, W.1, IWAHANA, Y.1,
2

3

KURIHARA, Y. , NAKAMURA, T. , KOIKE,
Y.

3

Fukushima

nuclear

power

plant

accident.

Although the radioactive Te may cause internalradiation exposure in living beings at the early1( Graduate School of Science and Technology,
2

Meiji Univ., Org. Strategic Coordination. Res.
3stage of the accident, little is known about theenvironmental behavior of tellurium includingIntellect. Prop., Meiji Univ., School of Science

radioactive Te. In this study, the uptake andand Technology, Meiji Univ.)

retention of Te and Cs was experimentally

Detection

efficiency

HP-Ge

investigated in radish cultivar (Raphanus sativus

spectrometer must be known in order tovar. sativus). The plants were grown indetermine activities from the gamma-ray spectrahydroponic media for about 30 days, exposed toobserved.

Detection efficiency is generally

media containing 1.0 ppm of Te and Cs for 2 hr,

calculatedwithradioactivity

and continued to culture for 7 and 10 days. The

standard volume sources. The radioactivity

concentrations of Te and Cs in the harvested

standard

severaltaproot and leaves were quantified by ICP-MS.

radioisotopes were only used in radiation

Since the chemical form of Te changes

controlled area. In the general laboratories,

depending on pH, two types of solutions withradioisotopes can’t be used for measurement ofdifferent pH (3.2-3.8 and 6.3-6.8) were used. In

environmental radioactivity. In this study, thethe plants soaked to the solution of pH 3.2-3.8,

detection efficiency curve was obtained by using

the concentrations of Te and Cs varied largely

KCl and LaF3 as commercially available

among individual plants, and the relative

chemical

detection

standard deviation (RSD) was 4-117%. On theefficiency curve was validated by quantitative

other hand, when the pH6.3-6.8 solution wasmeasurement of geochemical reference rockused, the differences of Te and Cs concentrations

sampleamong the individual plants were small, and theactivities

volumeReferencecontain

Determinedradioactive

value

the

of

sources

reagent.

and

of

was

standard

insample.

agreement

with

RSD was 6-17%. The concentrations of Te andanalytical results. The efficiency calibration

Cs under neutral conditions were higher thanusing commercially available regents will bethose under acidic conditions. Therefore, it was

useful outside radiation controlled area.

suggested that variation of pH considerably
effected uptake and retention of Te and Cs.

P23

Effect of pH on the Uptake andRetention of Tellurium and Cesium in Radish

P24 The behavior of radioactive cesium in(Raphanus sativus var. sativus) Cultured

the northern and eastern region of Nagano

under Hydroponic Condition

prefecture

FUJIWARA,

1K. ,TAKAHASHI,

1

T. ,

MATSUO,

K.1,

KOMATSU,

K.2,

KINOUCHI, T.1, FUKUTANI, S.1, HATTORI,

MURAMATSU, H.3, KONDO, Y.3

Y.2, TAKAHASHI, S.1,2(1Grad. Sch. Edu., Shinshu Univ., 2Dept. of- 219 -

Chem. Fac. of Edu., Shinshu Univ., 3Lake Nojiri

Meiji Univ., 3FURE, Fukushima Univ. 4Sci. &Naumann Elephant Museum.)Engr., Meiji Univ.)

The radioactivity measurement of variousThe

environmental samples (soil, water, leaf, plant,

Fukushima

fish, and so on) in Nagano has been performed(FDNPP) accident brought about radioactive

using

contamination in the aqueous environment byhyperpure

germanium

detector

to

Tokyo

Electric

Dai-ichiPower

NuclearCompany’s

Power

Plant

investigate the behavior of radioactive cesium

134

from Fukushima Daiichi nuclear power plant.

30.07 y) released from reactors. At present,

Radioacive materials from the reactors would

activity concentrations of

migrate as radioactive aerosols, attaching tomigrated in environmental water are not

non-radioactive aerosols suspended in surface air.

significantly

Thus, a potential radiation plume from theconcentrations in Tamagawa River watershed ofreactor site could reach to wide area of easternTokyo Metropolitan area have been determined

and central Japan, including Nagano Prefecture;

to investigate behavior of Fukushima-derived

indeed, we first found several fission products

134

on March 15, 2011. Since the aerosol particles

sediments were collected at 15 samplingattached radioactive materials efficiently deposit

locations in the Tamagawa River watershed. The

on the ground through the processes of wet

concentrations of 134Cs and 137Cs dissolved indepositions, the radioactive materials widely andriver water have been observed by gamma-ray

variously distribute on the ground surface after

spectrometry combined with the concentration

wet depositions, migrating or being transported

method using ammonium molybdophosphatethrough various changes in environment. For the(AMP). The dissolved 134Cs and 137Cs were notabsorption into the body of a plant, radioactivity

detected in upstream within Okutama area. On

Cs andhigh.

134

Cs andTrace-level

137

Cs

activity137

Cs. The water samples and

Cs included in various leaves collected in

the other hand, dissolved 134Cs and 137Cs in

our university campus ranged between 1 and 10

midstream and downstream in Tamagawa River

Bq/kg, almost decreasing since 2011. For thewatershed were detected.

of

134

Cs (half-life: 2.06 y) and 137Cs (half-life:

deposition into soil,

134

Cs radioactivity in soils at

Mt. Madarao ranged from 50 to 300 Bq/kg.
There seems to be a correlation between

134

Cs

concentration and altitude.

P26

I-129 concentrations in soil samples

collected at East Japan area -- Influence of
the Fukushima Daiichi nuclear plant accident--

P25 Monitoringofradiocesiumin

YAMAMICHI, M., OHKI Y., BAMBA S.,

Tamagawa River watershed after Tokyo

OHTA, Y.

Electronic Power Company’s Fukushima(Japan Chemical Analysis Center)
A large amount of radioactive materials were

Dai-ichi Nuclear Power Plant Accident
1

R. ,

Y. ,

released after the Fukushima Daiichi nuclear

IWAHANA, Y. , NOGAWA, N. , NAKAMURA,

plant accident in 2011, resulting in large-scale

AOBAYASHI,
1

4

T. , KOIKE, Y.
1

KURIHARA,2

3

4

deposition of radionuclides onto the ground. In
2( Grad. Sch. Sci. & Engr., Meiji Univ., Org. forthis study, we measured I-129 in surface soil

the Strategic Coord. of Res. & Intell. Prop.,

samples collected in East Japan area to evaluate- 220 -

the influence of the accident.

has been needed to analyze radioactive pollution

Soil samples were collected in 10 prefecturesof water and soils on paddy fields because of

in 2010 and 2012, before and after the accident.

effective reduction of radioactivity in crops. In

Iodine was volatized from the samples by using

this research, we have tried to analyze

electric combustion-tube furnace and trappedradioactivity

into aqueous solution. Stable iodine (I-127)

radioactively-contaminated water including clay

concentrations were determined by ICP-MS.

soils.

(137Cs)of

Test sample water including soils wasAfter adding carrier, iodine in aqueous solution
was purified through solvent extraction andprepared

converted

AMS

radioactively-contaminated soil into pure water.

(Accelerator Mass Spectrometer) measurement.

The sample was separated into coarse and fineI-129/I-127 ratios were determined by using

particles and solvent with a sieve (sieve gauge:

AMS at JAEA Mutsu site. Finally, I-129

125µm) and a filter paper (diameter: 25µm).

concentrations were derived from I-129/I-127

Fine particles under 25µm, which passed

ratios and I-127 concentrations.

through the filter paper, were flocculated by theintosilveriodidefor

Increase of I-129 concentrations was found inthroughelectrocoagulation

mixturemethod

and

of

then

were

the soil samples collected in 9 of 10 prefecturescollected with another filter paper. Radioactivity

excludingI-129(137Cs) of each classified component wasconcentrations after and before the accident

measured by a face-type NaI(Tl) scintillation

ranged from 1.2 to 3.6. The atomic ratios ofsystem

I-129/I-127 also increased. These results indicate

measurement.

Ibaraki.

Theratiosofconstructed

for

low

radioactivity

the influence of I-129 released by the accident.

Measurement results showed that about 80%

In the soil sample of Ibaraki, conspicuousof the total-radioactivity (137Cs) of the test

increase was not observed because of thesample came from the fine particles (underrelatively high background of I-129 due to a

125µm). The particles under 25µm were able tonuclear fuel reprocessing plant located in theberegion.

electrocoagulation

filtered

from

the

solvent

method.

It

by

the

was

also

Further investigation will be needed toconfirmed that the radioactivity of the resultant

evaluate the distribution of I-129 in wider areasolvent was about one order lower than thein Japan.

particles,

which indicatesthatradioactive

cesium in the soil is not easily soluble in water.
P27 A trial of radioactivity measurement onradioactively-contaminated water including

P28 Tritium concentrations in Atmosphericclay soils

environment

YANO, Y., ZUSHI, N., SATO, F., KATO, Y.,

Prefecture（2013～2014）

IIDA, T.

TAGOMORI, H.1,TAMARI, T.1, KAWAMURA,(Osaka Univ.)

H.1

In Japan, a large amount of radioactive(1Kyushumaterials has been released from the Fukushima

Association)

Daiichi nuclear power plant in March, 2011. It- 221 -

andrain

Environmentalat

Fukushima

Evaluation

After FDNPP accident, the tritium levels inriver water, pond water, and seawater in

Edu., Tohoku Univ., 8Grad. Sch. Dent., Tohoku

Fukushima Prefecture were investigated, theUniv.)

recentresults

show

that

those

tritium

The Fukushima Daiichi Nuclear Power Plant

concentrations (except the seawater close to(FDNPP) accident released large amounts of

FDNPP) are almost same as pre-accident level.

radioactive substances into the environment. In

But the data about atmospheric tritium are veryorder

few. We present the recent tritium levels of

biokinetics of radionuclides and for dose

atmospheric HTO and rain at Fukushimaassessment of internal exposure brought by thePrefecture.

FDNPP accident, we determined the activity

toprovidebasic

information

for

Atmospheric HTO and rain were continuously

concentration of radionuclides in the organs ofcollected each month from Oct 2013 at Tamura

300 cattle, 50 pigs within a 20-km radius around

City (Fukushima Pref.) and Fukuoka City

the FDNPP. The radioactivity of the samples(control site). The HTO collected on molecular

was determined by gamma-ray spectrometry

sieve 3A (MS-3A) were desorbed by heating

using three HPGe detectors. In all the specimens

400℃ with flowing N2 gas. The rain sample was

examined, deposition of Cs-134 and Cs-137 wasenriched electrically. The sample mixed withobserved.

scintillation

uLLT,

deposition of radionuclides with relatively short

PerkinElmer) was measured 1000 min by low

half-lives was detected, such as Ag-110m in the

background liquid scintillation counter (LB-5,

liver and Te-129m in the kidney. Regression

LB-7, Hitachi Aloka).

analysis showed a linear correlation between the

cocktail(UltimaGold

Furthermore,organ-specific

The atmospheric concentrations of HTO fromradiocesium activity concentration in whole

Oct 2013 to April 2014 in Tamura city andperipheral blood (PB) and that in each organ.

Fukuoka city were below 1 Bq/L, and there wereThus, the activity concentration of Cs-134 andno significant difference between two samplingCs-137 in an organ can be estimated from that insites.

PB. The level of radioactive cesium in theorgans of fetus and infants were higher than that

P29

Distribution of Artificial Radionuclides

of

the

corresponding

maternalorgan,in Abandoned animals in the Ex-evacuation

respectively. Furthermore, radiocesium activity

Zone of the Fukushima Daiichi Nuclear

concentration in organs was found to be

Power Plant Accident

dependent on the feeding conditions and the

1

1

1

KINO, Y. , IRISAWA, A. , KOARAI, K. ,2

2

geographic location of the cattle.

3

SUZUKI, M. , URUSHIHARA, Y. , ABE, Y. ,YAMASHIRO, H.4, FUKUDA, T.5, ISOGAI, E.5,
6

1,7

7

KOBAYASHI, J. , OKA, T. , SEKINE, T. ,8

SHINODA, H. , FUKUMOTO, M.

2

1

2

( Dept. Chem., Tohoku Univ.,

P30

between137

Csconcentration in river water and inventory incatchment

Dept. Path.,

Relationship
areas

in

eastern

Fukushima

Prefecture, Japan

3

IDAC, Tohoku Univ., NRCPD, Obihiro Univ.

OCHIAI, S.1, UEDA, S.1, HASEGAWA, H.1,

Agr. Veter. Med., 4Fac. Agr., Niigata Univ.,

KAKIUCHI, H.1, AKATA, N.1,2, OTSUKA, Y.1,

5

Grad. Sch. Agr. Sci., Tohoku Univ., 6Sch. Food,HISAMATSU, S.1

Agr. Env. Sci., Miyagi Univ. 7Inst. Excel. High.

(1Institute for Environmental Sciences, 2Present- 222 -

Affiliation:

National

InstituteforFusioninput of radioactive depositions into the Sea ofJapan, the FDNPP-derived 134Cs was detected in

Science)
To investigate the factors controlling 137Cs

estuary sediments as well as riverine particles inconcentrations in river water, dissolved andthe Agano River which has the upper branch inparticulate 137Cs concentrations were measured

Fukushima Prefecture and meets the Sea ofat 16 sampling points in seven river systems

Japan-side

underduringPrefecture). In the present study, we examine the2013. The

distribution of 134Cs in the Agano River and thenormalflow

June–September inconditions

2012

and

concentration of dissolved 137Cs exhibited astrong correlation with the average

137

Cs

estuaryofarea

centraland

Honshudiscussthe(Niigatatransportmechanisms of the riverine particles.

inventory in the catchment area of eachsampling point, whereas the concentration ofparticulate

137

Cs exhibited no clear relationshipwith the inventory. These results demonstratethat concentrations of dissolved

137

Cs in point

P32 Penetration of actinoids and fission
products

inmortar andestimationof

distribution using a partition equilibrium
model

samples of river water under normal flow

KINOSHITA, N.1, OISHI, K.1, TORII, K.1,

conditions are determined primarily by the 137Cs

SUEKI, K.2, YOKOYAMA, A.3

inventory of the catchment area upstream of the(1Shimizu corp., 2Sch. Sci. Eng., Tsukuba Univ.,

point.

3

Coll. Sci. Eng., Kanazawa Univ.)
Radionuclides on surface concrete wouldThis work was performed under contract withpenetrate deeply by contact with precipitation

the government of Aomori Prefecture, Japan.

and polluted water. The penetration is one of
P31 Migration pattern of riverine particles

problem for decommissioning and demolition ofin the Agano River; implications from thethe building of Fukushima Daiichi Nuclear

FDNPP-derived low-level

134

Power

Cs

YONEOKA, S.1, UEMURA, H.1, INOUE, M.1,
1

1

1

OCHIAI, S. , NAGAO, S. , YAMAMOTO, M. ,HAMAJIMA, Y.

1

Plant.

sholudbeplanned prior to works on the demolition.
Scraping the contaminated part is required todecontaminate(1LLRL, Kanazawa Univ.)

Decontamination

insideofthebuilding.

Radioactive strontium, uranium and plutonium,

The FDNPP accident released large amounts

etc. are present in the polluted water in the134

Cs to the atmosphere and to land and sea

building as well as radioactive cesium. In thesurfaces over a wide region, particularly thepresent work, basic data of the penetration into

Pacific Ocean-side of eastern Japan. In addition,

the concrete were obtained to estimate the depth

marine sediments around the FDNPP were also

for decontamination.

ofsubjected to radiocesium contamination byDistribution coefficients, Kd, of Sr, Cs, U, Pu,

highly contaminated seawater as well as direct

and Am in a mortar sample were measured. In

deposition on the sea surface and discharge ofaddition, 85Sr, 137Cs, and 238U solution wereriverine materials. On the other hand, regardlesspassed through a column in which pulverizedof isolation from the ocean currents that pass themortar was filled. Concentrations of the nuclides

FDNPP and the small contribution by direct

decrease exponentially with the depth. The- 223 -

profiles in the mortar column were compared

the evaluation of the residual ratios. An

with the profiles estimated with a partition

improvement in the determination of degradedequilibrium model. The profiles based on the

DMI should be achieved for the evaluation.

model agree well with the experimental profiles.
Scraping a few millimeter would give enough

P34

decontamination for isotopes of Cs, U, Pu, andconcentrations in environmental samples inAm., while several centimeter of scraping would

Ishikawa Prefecture

be required to remove Sr.

YASUIKE, K., ISHIKAWA, T., SASAKI, C.,

Temporal variations of carbon-14

MATSUDA, N., ITAZU, H., YAMADA, Y.
P33 Stability of DMPU and DMI for(Facul. Pharm. Sci., Hokuriku Univ.)

1

2

2

NOGAMI, M. , TANAKA, Y. , MIYAKE, K. ,1

3

NISHIDA, T. , SUZUKI, T. , IKEDA, Y.

3

1

14

C concentrations in

The variation of

selective U(VI) precipitation against heating

atmospheric CO2 samples collected every 10
days was measured in Dairahonmachi (36.5°N,

2( School of Sci. Eng. Res., Kinki Univ., Dep.

136.7°E) Kanazawa and Shikamachi (37.0oN,

Electric Electronic Eng., Kinki Univ., 3Res. Lab.

136.8oE) Hakui, Ishikawa Prefecture, Japan in

Nucl. React., Tokyo Tech.)2013. The variation of 14C concentrations in

Cyclicurea

compounds

arepotential

atmospheric

CO2

in

Dairahonmachi

kept

precipitants with selectivity to U(VI) in acidic

constant from April to the middle of June,

nitric acid solutions. Two candidate cyclic urea

increased gradually to the early of September

compounds,

and decreased to December. The result in

1,3-dimethyl-3,4,5,6-tetrahydro-2(1H)-pyrimidi

Shikamachi

none

Dairahonmachi. We have already published the(DMPU,

6-membered

ring)

and

was

similar

to

that

of

result that the long-term variation of

14

5-membered ring) were heated in HNO3 toconcentrations

wasevaluate the quantitative stability. Heating wasmeasured in Ohkuwamachi (36.6°N, 136.6°E),

carried out for HNO3 up to 4 mol•dm-3 (=M)

Kanazawa from 1991 to 2000. The trend of the

1,3-dimethyl-2-imidazolidinone

(DMI,

o

in

atmospheric

CO2

Ccontaining 1 M DMPU at max. 70 C up to 6 h.

variation of 14C concentrations in atmospheric

The residual ratio of the compounds was

CO2 in Dairahonmachi was similar of that inevaluated by the 1H NMR spectra.

Ohkuwamachi. The rice samples were collected

It was revealed that the degradation of DMPU

in the same sampling points of atmospheric CO2
2013.

ComparedtheCsamplesthan with increasing concentration of HNO3.

concentrations in rice with the variation of those

The residual ratio of DMPU was found to be ca.

in atmospheric CO2, the 14C concentrations in

50% for the sample of 6 h heating in 4 M HNO3

rice were closely the variation of those in

o

in

14

was more enhanced with increasing temperature

at 50 C. For DMI, nearly no degradation was

atmospheric CO2. It was found that the 14C

found to occur by heating for 6 h in 1 M HNO3

concentrations in atmospheric CO2 of summeroC. While, much more distinguished

had the influence on those in rice when rice wasdegradations were observed for the sample

grown up. In other words, it's possible to use theheated in higher concentration of HNO3 and at

14

at 50

higher temperature, resulting in the difficulty in- 224 -C concentration of the rice as an index of the

14

C concentration in atmospheric CO2 in the

period while rice grows up.

P36

Quality assurance of 129I analysis by

AMS
P35

Variations of tritium concentrations

andcarbon-14

concentrations

in

KAKIUCH, H.1, AKATA, N.2, KAWAMURA
H.3, TENNICHI, M.3, HISAMATSU, S.1

environmental samples in Kanazawa city,(1Institute for Environmental Sciences, 2National

Ishikawa prefecture after the accident at theInstitute

Fukushima No. 1 nuclear power plant

Environmental Evaluation Association)
locatedino(40 57’66”N,(Facul. Pharm. Sci., Hokuriku Univ.)

Fusion3

KyushuScience,

The spent nuclear fuel reprocessing plant

YASUIKE, K., KIZAKI, A., SHIMADA, Y.,
YAMADA, Y.

for

Rokkasho,o

141 21’87”E)

Aomori,

Japan

is

going

in

Environmental tritium decreased to levels

operation tests with actual spent nuclear fuels,

lower than 1 Bq/L in 2000 in Kanazawa cityand releases a limited amount of 129I into the(36.5oN, 136.7oE), Ishikawa Prefecture, Japan. A

surrounding environment. We will determine 129I

large amount of tritium was released from theconcentrations

Fukushima No.1 nuclear power plant caused byenvironment in Rokkasho Village, for evaluation

theof the effects of the release on the environmental

damageofthenuclearreactors

in

by

AMS

in

surrounding

consequence of the Great East Japan Earthquake

129

on 11 March 2011. In this study, we measured

analysis by certified reference materials.

129

I

This work was performed under contract withthe variation of tritium concentration in the
precipitation of Kanazawa city after the day of

I concentration level. We confirmed

the Government of Aomori Prefecture.

the Fukushima No.1 nuclear disaster. One of theinteresting result is that dramatic increases in the

P37 Establishment of Analytical Method fortritium

Technetium-99 in Soilconcentrationof

131.64Bq/L

and99.95Bq/L were observed on 30 May and 13

INOUE, K.1, FUJITA, H.1, HATSUKAWA, Y.1

June in the variation pattern of the tritium(1JAEA.)

concentration in the precipitation of Kanazawa

Technetium-99(99Tc) is one of the mostcity, although no marked change was observed

important radionuclides for the environmental

in the period from April up to the end of May.

monitoring because of the long half-life and highThis was done to estimate the influence of thefission yield. However,tritium released into the environment by thedetermined in routine monitoring due to the low

Fukushima No.1 nuclear disaster on the tritium

concentration and pure soft beta ray emitter.

concentration in the precipitation of Kanazawa

Therefore, an analytical method of 99Tc was

1499

Tc has not been

C concentrations indeveloped for environmental soil samples. In

atmospheric CO2 samples collected every 10

this research, the pretreatment procedures of soildays was measured in Kanazawa City fromwere examined using both combustion and acid

March to September in 2011. The effect by theleaching methods.

city. The variation of

At first, 10 g of soil sample in which 99Tc (2Fukushima No.1 nuclear disaster was not find inthevariation

atmospheric CO2.

of

14

C

concentrations

inBq) was added was used in recovery test of bothmethods, respectively. In the combustion method,- 225 -

99

Tc was volatilized at 1000ºC and trapped tosequential

alkaline solution in a combustion apparatus. In

developed to obtain only the iodine sticking to

extraction

method

was

newly

99

the soil organic component. The stable iodine

Tc in these samples wascan be quantified by direct analysis of thepurified with an extraction chromatographic

fraction and 129I can be quantified by Accelerator

resin (Eichrom, TEVA), and was measured by

Mass Spectrometry (AMS) with the method of

inductively coupled plasma mass spectrometerthe fraction added with carrier. The fraction of

the leaching method, Tc was leached with 3 M
HCl for 2 hours.

99

Tc by

the organic component for 127I and 129I can be

the combustion method was lower than 40%, but

evaluated respectively by comparing with thethe recovery by the leaching method wasother fraction and/or with the total concentration

approximately 80%.

obtained by the bulk analysis (e.g. by the(ICP-MS). As a result, the recovery of99

99

Then, Tc was added to 50 g of soil sample,

pyrohydrolysis).

and it was analyzed by the previous leaching
method.

Asaresult,therecovery wasapproximately 70%. So the leaching method
99

P39

224

Ra/228Ra ratios in coastal lagoon andthe water dyanamics in Lakes Nakaumi andcould be applied to the Tc measurement of the

Shinjikosurface soil samples as a pretreatment procedure.

NOMURA, R.1, INOUE, M.2, KOFUJI, H.3(1Shimane Univ.,

P38

A study for aging effect of I-127 and3

In general, water dynamics in lagoon water
2

3

HONDA, M. , MATSUZAKI, H. , SAITO, T. ,4

NAGAI, H. , SUEKI, K.

LLRL, Kanazawa Univ.,

Japan Marine Sci. Found.)I-129 used sequential extraction
1

2

5

are able to understand by examining the salinityof brackish water. However, the presumed water1( Grad. Sch. Pure Appl. Sci. Univ. of Tsukuba,

dynamics cannot present the time series changes

2of waters. Otherwise we are able to understand3

The Univ. Museum, The Univ. of Tokyo, Nucl.
4

5

Prof. Sch., Univ. of Tokyo, Nihon Univ., Pure

the water mixing processes of old and new

Appl. Sci. Univ. of Tsukuba)

waters, by applying radioactive elements, such

Some of resent studies reported about the
aging effect of iodine isotopes between stable

as a short-life element as 224Ra (t1/2=3.66d) and along-life 228Ra(t1/2=5.75y) in coastal lagoon.

iodine (127I ) and 129I (T1/2=1.57×107y): theWe examined the 224Ra/228Ra ratios of bothformer has been coming from the sea for thesurface and deep waters from 20 locations inyears of more than millennial scale, the latter has

Lake Shinjiko.

been generating from atmospheric nuclear

water

testing, spent nuclear fuel reprocessing plants inimpregnated acrylic fiber.

Europe since 1960’s. Some amount of

129

I was

were

Both 224Ra and 228Ra in thecollected

by

using

a

Mn-

Measurement of224

Ra was carried out within one and a half days

also released from the Fukushima Dai-ichi

by a Delayed Coincidence Counting system

nuclear power plant accident at 2011.

(RaDeCC) for α-decay and 228Ra was measured

To investigate the aging effect of the
Fukushima accident derived 129I in soil, it isby a γ spectrometry after one month of 224Ra
examination.
The results indicate the 224Ra/228Ra ratios inimportant to know what kind of component the129

I combines with. In this study a progressive

the surface water were 0.3-0.48 in western part

- 226 -

and 0.19-0.20 in eastern part of Lake Shinjiko.

of low concentrations of 10Be and 26Al by

The deep water was generally lower than thoseAMSof the surface, suggesting that the deep water is

SAITO-KOKUBU, Y.1, MATSUBARA, A.1,

more stagnant and old in age. We judged Ra

FUJITA, N.1, NISHIO, T.2, OHWAKI, Y.2,

isotopes in water were derived from a shallow

SANADA, K.2, NISHIZAWA, A.2, MIYAKE,

coastal area and were not from deep water.

M.2(1JAEA, 2Pesco Corp., Ltd.)

Migration pattern of the Tsushima

Cosmogenic nuclides of 10Be and 26Al are

Warm Current; Implication from 228Ra/226Ra

used especially for estimation of exposure age

ratio

and erosion rate of rock. In order to measure

P40

1

1

FURUSAWA, Y. , SHIROTANI, Y. , INOUE,

traces of 10Be and 26Al by accelerator mass

M.1,

spectrometry

YOSHIDA,

K.1,

FUJIMOTO,

2

K.2,

3

(AMS)

in

these

estimation,

10

Be and 26Al for

MINAKAWA, M. , SHIOMOTO, A. , NAGAO,

reagents with low levels of

S.1, YAMAMOTO, M.1, HAMAJIMA, Y.1,

carrier and so on are required. In this study,

KOFUJI, H.

1

ratios of 10Be/9Be or 26Al/27Al in several reagents(1LLRL, Kanazawa Univ., 2Nat. Res. Inst. Fish.
3

Sci., Tokyo Univ. Agricul.)

were compared. The reagents were oxides forevaluation of background in measurement and

The circulation of the surface water in the Sea

standard

solutionsforatomicabsorptionof Japan is primarily governed by the lateralspectrometry (AAS) or inductively coupled

movements of the Tsushima Warm Current.

plasma optical emission / mass spectrometry

Radium isotopes are continually supplied from

(ICP) for carrier and evaluation of process blank.

the shallow shelf and coastal sediment in the

The ratios were measured in JAEA-AMS-TONO.

continental-sideSea.

The ratios of 10Be/9Be in the Be oxides and theReflecting the short half-life of 228Ra (5.75 y),

Be standard solutions were approximately 10-15 -within the Honshu Island-side of the Sea of

10-14 levels. The Be standard solutions for AAS

Japan as well as the East China Sea, 228Ra

and ICP supplied by Merck had lower ratios of

exhibits marked temporal and lateral variations,10being caused by the seasonal change of thechemical. In this poster presentation, we willmixing ratio of 228Ra-rich continental shelf water

report the ratios of 26Al/27Al in several Al

and the 228Ra-depleted Kuroshio Current water.

reagents.

Therefore,

of

the

East

China

Be/9Be than those supplied by Wako and Kanto

228

Ra is the strong tracer for the

migration patterns of the Tsushima Warm

P42

Current. In the present study, employing

bronze implement

low-background γ-spectrometry, we conducted

ODA, H.1, TSUKAMOTO, T.2, YAMADA, T 2,

observations in the lateral profiles of 228Ra/226Ra

KATO, T.1

ratio on surface in the Sea of Japan in July of(1Cen. Chronological Res., Nagoya Univ.,

2009–2014 and assess the migration patterns of2

Possibility of radiocarbon dating toGangoji Institute Res. Cultural Property)
Verdigristhe Tsushima Warm Current in summer.

is

rust

generatedinbronzeimplement. It is produced from Cu contain in
P41 Selection of reagents for measurement

bronze and CO2 in the atmosphere. Once

- 227 -

verdigris is formed, it has the property which

HCl and HNO3 aqueous solutions in contact.

prevents formation of a new verdigris more. If

The activity ratios of 224Ra/228Ra and 228Th/232Th

extraction and radiocarbon dating of the carbon

in the leachates from an Ishikawaite increased

contained in verdigris become possible, the age

with an increase in pH of the HCl and HNO3

in which the rust was formed is obtained, andaqueous solutions, while those of 230Th/232Th

also estimation of the age for which bronze ware

and

226

Ra/228Ra

decreased.

The

leaching

224

Ra, which is formed through four

was used may be realized. In this study,

behavior of

therefore, we searched for the condition of

decay processes of 232Th, was different from thatcarbon extraction from verdigris. Verdigris isof 228Ra, which is formed by a single decay of

decomposed by heating in an evacuated glass

232

tube. As the result, it became clear by heating atleached more effectively thanTh. 228Th, decay products of 232Th, was also232

Th. The224

1 h and 250°C or more that CO2 was extracted

leaching efficiency ofwith 90% or more of yield. Next, the verdigris

estimated to be mainly dependent on thesamples were extracted from the bronze

difference in the history of decay processes

implements of known archaeological age and thewhich have formed the nuclides. However, 226Ra

radiocarbon dating of them was performed. The

and 230Th, which are decay products of 238U,

calibrated

showed different leaching behavior from 224Ra

radiocarbon

ages

includedtheRa and228

Th was228

Th. The difference in the leachingcorresponding archaeological ages. Considering

anda time lag from burying or rejection of bronze

efficiency of 226Ra and 230Th may be attributed

implement

to the ratio of U/Th in the mineral.

toarchaeological

generation
ageofshouldbeverdigris,
older

than
7

10

calibrated radiocarbon ages. Although, this result

P44shows that the time lag can be neglected and thatconcentrations in the atmosphere near theverdigris is a suitable sample for radiocarbon

Earth's surface

dating.

SATO, H.1, TSUJITA, K.1, YAMAGATA, T.2,

Variation

of

Be

and

Be

NAGAI, H.2, MATSUZAKI, H.3
P43

Activity ratios of thorium and radium

Univ., 2Humanities and Sciences., Nihon Univ.,

isotopes leached from Ishikawaite
K.1,

KOMATSUBARA,3R. ,SHIOBARA,

Y.2,

KURIHARA,

NAKAMURA, T. , KOIKE, Y.

3

The Univ. Museum., The Univ of Tokyo.)

4

NOMURA,

3(1Grad. Sch. Integrated Basic Sciences., Nihon

K. ,

3

Concentrations of

7

Be and10

Be in theatmosphere near the Earth’s surface were1

( Graduate school of Science and Technology,
2

measured at Tokyo during 2002 to 2013. Almost

Meiji University, Organization for the Strategic

same seasonal variations were observed for 2002

Coordination of Research and Intellectual

to 2013: Be isotopes concentrations and isotopic

Properties, Meiji University,

3

Department ofApplied Chemistry, Meiji University,

4

The

University of Tokyo)

ratios of 10Be/7Be were high during March toJune by Stratosphere-Troposphere exchange(STE), and in other periods, concentrations were224

controlled by the vertical mixing in theTh from Ishikawaite,

troposphere. The annual average of 7Be and 10Be

radioactive mineral, was observed along pH ofconcentrations and the relative 7Be and 10Be

Th,

230

Th and

232

Ra,

228

Ra,

The leaching behavior of
228

Ra,

226

- 228 -

concentrations calculated from the neutron flux

MASUDA, Y.1, YAMAGATA, T.2, HASEGAWA,

which observed in Delaware, were compared.

A.1, TAZOE, H.3, MATSUZAKI, H.4, NAGAI,

These values become maximum at 2009, and theH.2

residence time of Be isotopes were estimated to(1Grad. Sch. of IBS, Nihon Univ., 2CHS, Nihon

about 2 years.

Univ., 3Inst. of REM, Hirosaki univ., 4MALT,
Univ. of Tokyo)
228

228

Th/ Ra ratio in

We collected seawater from the Northernseawater from the East China Sea and the Sea

North Pacific during R/V Hakuho-Maru KH12-4

of Japancruise and investigated the distributions of 7Be

SHIROTANI, Y.1, FURUSAWA, Y.1, INOUE,(T1/2=53.3 day) andM.1,

concentration of

P45

Lateral profile of

NAGAO,

S.1,

M.1,

1

1

seawater were 20-110 and 150-1050 atoms/cm3,

TAKIKAWA,

T.3,

respectively. The concentration of 7Be was high

HAMAJIMA, Y. , UEMURA, H. , KOFUJI, H. ,A.2,

Be (1.36×106y). The

YAMAMOTO,

1

MORIMOTO,

10

FUJIMOTO, K.4

7

Be and10

Be in surface

in the western north Pacific and low in the

1

2( LLRL, Kanazawa Univ., HyARC, Nagoya

eastern north Pacific. And 10Be was almost

Univ., 3Nat. Fish. Univ., 4Nat. Res. Inst. Fish.

constant throughout all sampling point (except

Sci.)

for the BD07 and BD15 station). Because of two

The East China Sea is an area of highstations lied high biological productivity, we

productivity. Therefore, studies of material

considered deposition rate from the surface of

cycling have been conducted from the viewpoint

Be was faster, and the concentration of theof particle transport as well as water circulation.

surface seawater had become low.

Th (half-life, 1.91 y) in

We showed vertical profile of 7Be and 10Be.

seawater is predominantly governed by biogenic

The estimated 7Be flux from the atmosphere toparticle behavior, and therefore the combination

the sea surface were 0.013-0.048 atoms/cm2/sec.

of 228Th and 228Ra activities (228Th/228Ra ratio) in

And the mean residence time of Be when usedseawater samples is useful for the study ofas a surface 10m were 0.13-0.80 year. There wasscavenging processes. In the East China Sea, thea correlation between mean residence time of the

228

Be

Activity of reactive

228

228

Th/ Ra ratio of surface waters is low except

for a wide variation in the Kuroshio-dominated

and

the

maximum

concentrationofchlorophyll a.

area. On the other hand, the scavenging
mechanism is not clarified in surface of the Sea

P47 Anofdissolution method using oxalic acid forJapan.

In

low-backgroundthepresent

study,

using

gamma-spectrometry,we

optimizationofmagnetitecosmogenic nuclide exposure age dating
H.1,

SUEKI,

K.2,

investigate the lateral and seasonal variations of

MATSUMURA,

228

MATSUMURA, M.2, SASA, K.2, NISHIIZUMI,

China Sea and the Sea of Japan and assesses the

K.3

scavenging mechanisms of 228Th in these areas.

(1KEK, 2Univ. of Tsukuba, 3UC Berkeley)

Th/228Ra ratio in surface waters from the East

The cosmogenic nuclide exposure age dating
P46
10

7

Distribution of Cosmogenic Be and

Be in the Northern North Pacificby accelerator mass spectrometry (AMS) of thelong half-life radionuclides produced in the rock- 229 -

on the earth surface by secondary cosmic rays ismolecule were not negligible. In order toused for geomorphological study etc. The

increase

determination of

10

Be and

26

the

yield

of

radioactive

Al in quartz is ametallofullerenes, it is very promising to employ

main method for the cosmogenic nuclide

the recoil of nuclear reaction by fast neutron

exposure age dating. Here, we suggested thefrom the viewpoint of reducing the radiation

cosmogenic nuclide exposure age dating using

damage. In this session, we will report themagnetite as a new method. In the magnetite

synthesis of 85Sr@C60 using nuclear recoil of

method, it is possible that five nuclides (10Be,

8626

neutron.

Al, 36Cl, 41Ca, and 53Mn) more than quartz

Sr (n, 2n) 85Sr reaction by 14 MeV fast
Mixture of C60 with strontium salts such as

method can be measured by AMS. In our
10

Cl

Sr(NO3)2 and SrC2O4 were employed for thein magnetite separated from a basalt obtained attarget materials. These samples were irradiatedthe Atacama Desert in Chili were measured. A

by fast neutron in Fusion Neutronics Source atcosmic-rays exposure age could be obtained

Japan Atomic Energy Agency. After theprevious study, concentrations of

10

Be and36

36

from the Be and Cl concentrations and it wasirradiation, CS2, aniline, and HClaq were passed

confirmed that the magnetite method is effective.

through the irradiated samples on the filter to

However, improvement in initial magnetite

dissolve C60, Sr@C60, and strontium salts,

dissolution was required due to long dissolution

respectively.

time and large solution volume. Therefore, insolutions were measured by Ge detector. As athis study, magnetite dissolution conditions were

result, about 0.75% of radioactivity was

optimized by dissolution examinations using

observed in the aniline solution from SrC2O4

commercial magnetite. The optimized solution,

sample. This result strongly suggests thattemperature, and time for 1-g magnetite are

Sr@C60 was efficiently produced by fast neutron

15-mL aqueous solution of 5-g oxalic acid

irradiation of SrC2O4/C60 target.

The

gamma-ray

from

these

dihydrate, 70°C, and 6 days, respectively.
P49 Preparation of
P48

Synthesisofendohedral

85-Sr

109

Cd for fee-based

distribution at the RIKEN AVF cyclotron

metallofullerene by nuclear recoil using high

WAKITANI, Y.1, 2, YANO, S.1. 2, YAMADA, T.1,

energy neutron

2

MIYASHITA,

Y.1,

AKIYAMA,

K.1,, HABA, H.1, SHIBATA, S.1, TAKAHASHI,

K.1

HATHUKAWA, Y.2, CHIBA, K.1, TADAI, T.1,

(1RIKEN Nishina Center, 2Japan Radioisotope

SATO, Y.1, KUBUKI, S.1

Association)

1

2

Purified radioisotopes such as 65Zn, 109Cd, and( Tokyo Metropolitan Univ., JAEA.)
To obtain an endohedral metallofullerenes

88

Y have been distributed to the general public inwith high specific radioactivity using nuclear

collaboration between RIKEN Nishina Centerrecoil phenomena, many experiments have beenforperformed so far. However, production yield ofRadioisotope

Association

metallofullerene by nuclear recoil using highCadmium-109

was

LET radiation was found to be very small

109

because radiation damages to targeted fullerene

plate in a natural isotopic abundance with a

Accelerator

Based-Science

and

since

produced

Japan
2007.

by

the

109

Ag(d,2n) Cd reaction by irradiating a Ag

- 230 -

24-MeV deuteron beam from the RIKEN AVF
cyclotron.

So

109

far,

Cd

was

chemicallyradio-strontium solution isusefulin theevaluation for the performance of newly

separated by filtrating the AgCl precipitatesdeveloped techniques.

prepared after dissolving the irradiated Ag target.

investigated a novel procedure to prepare the

However, the chemical yield of this procedure

purified 85Sr solution having a high specificwas ~75%, not high enough, because of theradioactivity using a no-carrier-added technique.

109

Cd into AgCl. Therefore,

coprecipitation of
weinvestigated

the improvement

of

the

Strontium-85
nat

was

In this work, we

produced

in

the

85

Rb(d,x) Sr reaction by irradiating a RbCl disk

chemical yield by chromatographic separation

in a natural isotopic abundance with a 24-MeV

with HBr solutions by an anion exchange resin

deuteron beam from the RIKEN AVF cyclotron.

(Dowex 1X8, 100-200 mesh). The Ag wasStrontium-85 was chemically purified by theeluted with 7 M HBr from the column of anion

two-step chromatographic separation with a Sr

109

Cd was recovered with 3 M

resin (Eichrom, 100-150 mesh) and a cation

HNO3. The chemical yield was remarkably

exchange resin (Dowex 50WX8, 200-400 mesh).

improved to be 98% by the newly applied

The radioactivity of 85Sr was determined byresin and then109

procedure. The radioactivity of

Cd wasγ-ray spectrometry using a Ge detector. The

determined by γ-ray spectrometry using a Ge

chemical impurity and specific activity of thedetector.

waspurified solution were evaluated with ICP-MS

determined to be >99.9%. The chemical

for a control sample which was treated by the

impurity and specific activity of the purified

same chemical procedure as the irradiatedsolution evaluated with ICP-MS will also be

sample.

Theradionuclidic

puritypresented.

In the present experimental conditions, theproduction yield of 85Sr was about 3 MBq µA-1

P50 Preparation

of

85

Sr

for

fee-based

solution was 89%. The radionuclidic purity was

distribution at the RIKEN AVF cyclotron
YANO, S.1,2, WAKITANI, Y.1,2, YAMADA, T.1,2,1

1h-1. The chemical yield of the purified 85Sr

1

determined to be >99.9%. It was suggested that

HABA, H. , KANAYA, J. , SHIBATA, S. ,a high specific activity of 100 MBq µg-1 or more

TAKAHASHI, K.1

can be achieved by the use of present chemical(1RIKEN Nishina Center, 2Japan Radioisotope

separation procedure.

Association)
Purified radioisotopes such as 65Zn, 109Cd, and

P51 The substituent dependence on the88

Y have been distributed to the general public inyield of the unpaired electrons of soft X-ray

collaboration between RIKEN Nishina Center

irradiated pyrimidine DNA-bases

for

OKA, T.1,2, YOKOYA, A.3, FUJII, K.3, KINO,

Accelerator

Based-Science

and

Japan

Radioisotope Association since 2007. After the

Y.4, SEKINE, T.1

Fukushima

Plant(1Inst. Excel. High. Edu., Tohoku Univ., 2Dep.

accident in 2011, discharged radio-strontium

Chem., Grad. Sch. Sci., Tohoku Univ., 3ASRC,

analyses are carried out and also some new

JAEA, 4Dep. Chem., Tohoku Univ.)

Dai-ichiNuclearPower

In order to clarify the mechanism of DNA

extraction techniques are developed for analysesinvarioussubstances.

Carrier-freedamage induced by K-shell ionization of- 231 -

nitrogen and oxygen atoms, we measured

and specific radioactivity by arc discharge

short-lived ‘in situ’ ESR spectra of pyrimidine

method is extremely difficult. In addition, it isDNA-base molecules at a synchrotron soft x-ray

found that this method has some risks such as

beamline BL23SU in SPring-8 (Hyogo, Japan)

radioactive

during the monochromatic soft X-ray irradiation.

by-product of C60.

contamination

by

soot

as

a

In order to overcome these problems, we tried

The ESR intensity for cytosine was significantly

synthesize

14enhanced by the K-shell ionization, whereas thattoC-labeled

C60 usingtotal

for thymine was not enhanced. These results

synthesis method because this method issuggest that cytosine favors to form the unpaired

possible to improve the yield and specificelectron species. Further, by changing theradioactivity of C60 without any radioactive soot.

substituent of the pyrimidine bases, we foundout that the ESR intensities of pyrimidine bases

P53 Production of medical radioisotope 90Y

werewith fast neutrons by the Be(p,n) reaction

strongly

correlated

with

the

electronegativity of substituent, such as halogen

TAKEDA, S.1,2, TSUKADA, K.2, SATO, T.K.2,

atoms. The substituent effect of the pyrimidine

ASAI, M.2, NAGAI, Y.2, SAKAMA, M.3

ring in the DNA damage processes will be(1Tokushimareported.

Radiological Science, HBS, Tokushima Univ.)

Univ.,

2

JAEA,

3

Depart.

The radioisotope (RI) for nuclear medicine is
P52

Study toward total synthesis ofgiven an important role for a diagnosis with a

14

C-labeled C60

high sensitivity and medical treatment for cancer

TADAI, T., AKIYAMA, K., KUBUKI, S.

today. In this study, we tried to optimize an(Tokyo Metroporitan University)

effective production condition for 90Y, which has

Fullerene (C60) is one of the most promising

been used for the nuclear medicine, by using amaterial in the organic chemistry, medical, andfast

cosmetic field. For an application to the medical

Particularly, in this experiment, we paiedand cosmetic field, it is required to investigate

attention to a proton beam of 15-30 MeV

detail pharmacokinetics of C60 because it isprovided from the small size cyclotron, which

pointed out that some nanomaterials including

has been introduced into a medical institution for

fullerenes have nano-toxicity. The radiotracer

medical care such as the PET, coupled with amethod using C60 labeled with a radioactive

beryllium target, since the coupling has been

14

neutronprovidedinanaccelerator.

carbon atom such as C in its carbon framework

reported a high energy neutron can be producedis one of the most effective methods to study theeffectively. In this presentation we will reportpharmacokineticsofthe excitation function of 90mY with the incident

14

C-labeled C60 has been reported by Scrivens

proton energy and evaluate the influence ofand coworkers using arc discharge method forby-products.

of

C60.

Production

the first time. Recently, we succeeded to produce
14

C-labeled C60 with the highest specific

P54 Solvent extraction of astatine-211 forradioactivity to date by using a slightly

radiopharmaceutical use and its chemical

improved Scrivens’s method. However it isform in the extraction process

found that the increase in the production yield

TANIGUCHI, T.1, MAEDA, E.1, MURAKAMI,- 232 -

K.2, NISHINAKA, I.3, TAKAHASHI, N.4,
WASHIYAMA, K.5, YOKOYAMA, A.2(1Grad. School Nat. Sci., Tech. Kanazawa Univ.,
2Inst. Sci. Eng., Kanazawa Univ., 3ASRC, Japan

Atomic Energy Agency., 4Grad. School Sci.
Osaka Univ., 5Sch. of Health Sci., College ofMed., Pharma. Health Sci., Kanazawa Univ.)
The 211At isotope with a half-life of 7.2 h has
attracted attention as a promising α-emitter forradionuclide therapy. However, the chemical
properties of astatine isotopes are not wellknown for application in radionuclide therapy.
We focused on the DIPE-HCl extraction to study
the chemical forms of astatine in the extraction
process.

The

resultswill

contributeunderstanding the process of introducing

to
211

At

isotopes into the medicine.
We produced astatine isotopes by the reactionof 209Bi(α, 3n)210At using the AVF cyclotron of
RCNP in Osaka University. Astatine species
were taken out from the irradiated targets
through dry distillation and collected withvarious concentrations of HCl. The At species
were extracted from the HCl solutions into equalvolumesofdiisopropylether(DIPE).

The

γ-activity of each phase in extraction wasmeasured by a HPGe detector to obtain the
distribution ratio of astatine isotope.
Dependence of the distribution ratio on theconcentration of HCl was observed for DIPE.
Distribution ratios are positively correlated with
the HCl concentration more than 2 M, but are
negatively correlated with that less than 2 M.
Besides, chloride ion concentrations were foundin the present study to make some effect on the
DIPE-HCl extraction as well as those ofhydrogen ion.

- 233 -