English Abstracts1S01: Results of the Hayabusa mission and goal of
preliminary examination of the samples.
TSUCHIYAMA, A.1(1Grad. School of Sci., Osaka Univ.)
The Hayabusa spacecraft arrived at the S-type
asteroid 25143 Itokawa in November 2006, andsucceeded to reveal astounding features of the small
asteroid (535 × 294 × 209 m) [1]. Although thesample collection did not made by normal operations,
it is considered that a small amount of samples, atleast a few particles of approximately ten to a few
hundred micron meters in size, were collected. The
sample capsule was successfully recovered on theearth in June, 2010. After picking up of sample
particles from the sample container, some of themwill be examined preliminarily within one year inprior to detailed analysis phase. The following
scientific achievements will be expected; (1)characterization of the surface material of Itokawa(classification: ordinary LL chondrite or primitive
achondrite, formation age, formation process andconditions, density, etc), (2) processes on an ancestor
boby of Itokawa and accretion into Itokawa(brecciation, degree of impact, etc.), (3) interaction
with space environment (proof of space weathering,isotopic compositions of oxygen and noble gases ofthe solar wind, age of regolith, gardening rate, etc.),and (4) materials fallen onto the surface (primitive
materials, such as organic materials and/or
differentiated granitic fragments).
[1] Fujiwara et al. (2006) Science, 312: 1330.
2S01: Chemistry of Superheavy Elements –Experimental Achievements and Perspectives
Schädel M.1,2(1GSI Helmholtzzentrum für Schwerionenforschung,
Darmstadt, Germany, 2Advanced Science ResearchCenter, Japan Atomic Energy Agency, Tokai, Japan)
Ground-breaking atom-at-a-time experimentswith the lighter superheavy elements (SHE) Rf, Db
and Sg showed properties typical for group 4, 5 and
6 elements, respectively. Recent chemical studies
aimed at (i) unraveling detailed properties of Rf and
Db in aqueous solution, (ii) determining properties of
HsO4 in the gas-phase, and (iii) obtaining firstchemical information from the element 114 region.
Common to all these experiments is - in addition to
obtaining basic chemical knowledge - the quest for

the influence of relativistic effects on chemical
properties of SHE. In parallel to the advancement ofexperimental knowledge, progress in modern
relativistic quantum theory has provided crucial
guidance and understanding. Moreover, chemical
separations were applied for nuclear studies in theregion of deformed doubly-magic 270Hs. The
progress in SHE chemistry was closely linked to
improvements, and to new and automated techniques,from target technology to transport systems,
chemical separation devices, and innovative
detection system. Most recently, coupling ofchemical set-ups to recoil separators opens new
fields in SHE chemistry and provides great
perspectives for the future. Among those are not only
experiments in the element 114 region but also thosepaving the way to the organometallic chemistry oftransactinides.
2S02: Study on hot atom chemical process ofenergetic hydrogen isotopes in carbon-relatedmaterials
OYA, Y.
(1Fac. of Sci., Shizuoka Univ.)
Hydrogen isotope retention behaviors forcarbon-related materials, SiC, graphite, WC andsimultaneous C+-D2+ implanted W for fusion reactor
application were summarized. The deuterium
retention for SiC and graphite (HOPG) was higher
than that for WC and simultaneous C+ implanted W.
XPS spectra indicate that the large chemical shift
was observed for SiC and graphite, but no peak shift
was found for WC and C+ implanted W, indicatingthat most of deuterium was retained in the intrinsic
defects, interstitial sites and/or irradiation defects.
However, in the case of SiC and graphite, deuterium
does not remained in the interstitial site, but bound to
Si and/or C due to high affinity with hydrogenisotope. In the case of simultaneous irradiation, thedeuterium trapping is dynamically proceeded withthe competition between the dissociation of matrix
and chemical trapping of deuterium with constituent
atoms.
2S03: Study on synthesis and properties oftechnetium complexes
YOSHIMURA, T.
(1Grad. School of Sci., Osaka Univ.)− 156 −

Among the various technetium complexes, thechemistryoftechnetium-technetium
bondedcomplexes composed of three or more nuclei is still
limited. In this study, the synthesis, structures, andphysical properties, and electronic structures of thevarious octahedral hexatechnetium complexes andseveral mononuclear technetium complexes were
investigated.
Discrete and polymeric chalcogenide-cappedoctahedral hexatechnetium(III) complexes weresynthesized and structurally characterized. The
Tc-Tc distances in the Tc6Q8 core are longer with theorder of Q = S < Se < Te. Discrete sulfide- andselenide-capped hexatechnetium(III) clusters weresynthesized by the reaction of a discrete molecule ora polymeric complex with excess cyanide. The seriesof the chalcobromide-capped hexatechnetium
complexes were synthesized and characterized.
The redox potentials of the Tc6(23e/24e)
process in the technetium complexes were morepositive than that of the Re6(23e/24e) in thehexarhenium analog. On the other hand, the potentialof Tc6(22e/23e) shifts to negative as compared withthe potential of Re6(22e/23e), which is the oppositeof the tendency usually observed in technetium andrhenium complexes.
The HOMO/LUMO levels in [Tc6Q8(CN)6]4– (Q= S or Se) were determined. The energy level of
HOMO is lowered compared with those of therhenium congeners. The HOMO-LUMO energy gapof the hexatechnetium complexes is smaller than thatof [Re6Q8(CN)6]4–.
The seven-coordinate technetium(IV) andtechnetium(V) complexes were synthesized and theirproperties were investigated.
3S01: New physiological activity of plants
revealed by application of radiation andradioisotopes.
NAKANISHI, T.M.
(Graduate School of Agricultural and Life Sciences,
The Univ. of Tokyo)
Since plants live on only 17 inorganic
elements and water, the application of radiation andradioisotopes opens an important field to analyze
living plant activity.
Though water plays an important role for plant
physiology, the behavior of water itself has not been
known well, mainly because of lacking tools. We
applied neutron beam analysis to image water profile

within a plant, not only above-ground part but also
the roots imbedded in soil.
Morphologicaldevelopment of the root as well as the water uptake
manner of the roots in soil was visualized byconstructing spatial image of the root.
To analyze water movement itself, we employed
positron emitters, 18F and 15O. In the case of 15O,
whose half-life is only 2 min., 15O-water was
supplied to a soybean root and the increase ofradioactivity in the stem was measured. To ourgreat surprise, we found that tremendous amount ofwater was always flowing out from xylem cells,
which was regarded as mere pipe to transport wateror nutrient. The water coming out from xylem cells
was pushing the water already existed to re-enter into
the xylem tissue. That is, what we found was water
circulation in a plant! It was simulated that within
20 min., about half of the water already existed in thestem was replaced with the fresh water coming up
from the root.
In the case of nutrient elements, first of all, we
analyzed thousands of tissue samples of plants alongwith the developmental stage, by an activation
analysis. There was an element specific pattern of
distribution profile within a plant and the features ofthe profile were not changed throughout the life
cycle.
The plants growing in nature showed
specific accumulation of the elements whichreflected the nature of the soils, thus we could
separate the plants according to the production sites.
To analyze the nutrient uptake manner in a living
plant, we developed two types of real-time isotope
imaging systems. One was to image whole plant
and the other was to image microscopic tissue,
remodeling a fluorescent microscope. Using thesesystems, we were able to show how roots accumulateions in culture solution and transfer to theabove-ground part.
In the case of rice,32
P-phosphate uptake manner was compared between
water culture and soil culture. The amount of2
P-phosphate taken up from water culture was very
high, more than 100 times, compared to that of soil
culture.
Nowadays, fluorescent imaging is widely used
but for plant research, radioisotope imaging has two
great advantages. One is that it allows imaging
under light and the other was it enables to handle thenumerical treatment of the image, for the image wasbased on radioactivity.
K101: Role of neutron activation analysis in traceelement analytical methods− 157 −

IMURA, H.
(Grad. School of Natural Sci. & Tech., Kanazawa
Univ.)The k0-standardization method of instrumental
neutron activation analysis (INAA) has been
evaluated by determining the reference materials
associated with air pollution, NIST SRM 1633a(Coal Fly Ash), NIST SRM 2783 (Air Particulate on
Filter Media), and NIES CRM No.8 (Vehicle
Exhaust Particulates). The analytical results of
NIST SRM 1633a obtained by different facilities of
the reactors were consistent each other, and thedeviation from certified (reference) values for 17
elements were within 3%. It was ascertained thatthe present k0 INAA is very accurate. This method
was applied to the aerosol samples taken in Ibaraki
prefecture. Trace element contents in particulatematters with different sizes were determined, and the
distribution of elements and the regional variation
were revealed.
Nondestructive multi-element
INAA is recognized to be still one of the most usefuland important analytical techniques in trace element
analysis.
K102: Importance of radiochemical neutron
activation analysis – in case of the determinationof ultra-trace rare earth elements in rock andmeteorite samples
AIHARA, H., OURA, Y., EBIHARA, M.
(Grad. School of Sci. and Eng., Tokyo Metropolitan
Univ.)
Radiochemical neutron activation analysis(RNAA) involves radiochemical separation andpurification of the target elements after the neutron
irradiation of samples. As matrix elements includinginterfering elements can be removed, RNAA candetermine ultra-trace elements. Here, we show thecase of determining ultra-trace rare earth elements(REEs) in rocks and meteorites.
Geological standard rocks and Allendemeteorite were subjected to RNAA in this study. The
samples were irradiated with neutrons in the JRR-3
reactor of Japan Atomic Energy Agency. The RNAA
procedure for the determination of REEs was mostly
based on Minowa and Ebihara (2003) [1]. In addition
to REEs, U concentrations were determined by using
fissiogenic nuclides.
Ten REEs (La, Ce, Nd, Sm, Eu, Gd, Tb, Tm, Yb

and Lu) were able to be determined. As 140La, 141Ceand 147Nd are produced by neutron-induced fission
reactions on 235U in addition to neutron-capture
reactions of individual target nuclides (139La, 140Ceand 146Nd, respectively), their contributions were
estimated and corrected for. Uranium wasdetermined from the same samples as used for REEs
by using fission products of 140Ba and 140La.
This study clearly indicates that RNAA can be
the most suitable analytical method to determine
very low concentrations of REEs in rock samples.
We are confident that the importance of RNAA will
not be changed even in future.
[1] H. Minowa and M. Ebihara, Anal. Chim. Acta
498 (2003) 25.
K103: The role of neutron activation analysis in
the development of certified reference material
MIURA, T.1, KUROIWA, T.1, NARUKAWA, T.1,
CHIBA, K.1, HIOKI A.1., MATSUE, H.2(1 National Metrology Institute of Japan, AIST, 2
Japan Atomic Energy Agency)
In this talk, I would like to discuss the role ofneutron activation analysis in the development ofcertified reference material.
In 2007, neutron
activation analysis recognized as primary ratio
method by CCQM (consultative committee ofamount of substance-metrology in chemistry). In
addition, neutron activation analysis is well known asa non-destructive analytical method, which candetermine most elements without any chemical
pretreatments, that is, neutron activation analysis isbasically free from a potential risk of loss andcontamination during the sample preparation andmeasurement procedures. In particular, neutron
activation analysis is very useful to determine
mono-isotopic elements in environmental andbiological samples, since the isotope dilution
analysis that is one of the primary ratio methods
cannot be applied to those elements.  I will report
the application of neutron activation analysis for theaccurate determination of As in the arsenobetaine
standard solutions.
K104:
INAA attempting to get a fruitfulnational inventory map “Geochemical Map”
TANAKA, T.1,
(1Center of Chronological Res., Nagoya University)− 158 −

Geochemical Map is the map representing theareal distributions of chemical elements and isotopes
on the terrestrial earth. The map gives chemical
information for environment and resource. Many
elements for many samples must be analyzed to get a
reliable geochemical map in wide area. XRF and
ICP-MS are used for many researchers. I understand,however, INAA is the best techniques for the
purpose. The INAA gives quite reliable data for Au,
Ir, Os, As, Sb, Cr and REE. These are the importantelements for environmental assessment and resource
evaluation. The INAA provide a reliable data evenfor samples which contain hardly dissolvableminerals such as zircon. I will introduce our study in
Aichi~Gifu area, and will demonstrate how the
INAA is useful to draw the reliable geochemical map
to cover Southeast Asia as well as Japan.
K105: Multi-element analysis of environmental
samples by instrumental neutron activation
analysis and multiple prompt gamma-ray
analysis.
MATSUO, M.1, SHOZUGAWA, K.1, TOH, Y.2,
MURAKAMI, Y.3, FURUTAKA, K.2, KIMURA,
A.2, OSHIMA, M.2, KOIZUMI, M.2

2(1Grad. School of Arts & Sci., The Univ. of Tokyo,
Japan Atomic Energy Agency, 3Fukui Univ.)

Instrumental neutron activation analysis(INAA) is one of useful means for analyzing the
distribution of multi-elements in environmental
samples.
We have applied this technique toexamine the concentration and the vertical
distribution of more than 30 elements in estuarine
and tideland sediments by using with prompt
gamma-ray analysis (PGA).
Sediment samples were collected at Yatsutideland vertically.
The sediment cores wereapproximately 50 cm long and then cut into 3-cm
long pieces.
Those pieces were put inoxygen-impenetrable plastic bags with N2 gas
immediately to prevent from air oxidation. We
clarified the vertical distributions of elemental
concentrations by INAA and PGA. As a result, bigchanges of them were found at ca. 25 cm from thesurface in Yatsu tideland sediment core. It isthought that these changes were caused byneighboring reclamation. The vertical distributionsof elemental concentrations were categorized into
four groups according to the correlation matrix. By

applying principal component analysis (PCA), it wassuggested that sulfate ion was reduced underanaerobic environment and then various sulfides
were formed in the sediments. It was supported by
the result of Mössbauer measurement showing thevertical distribution of pyrite (FeS2).
Recently, we have also applied multiple
prompt gamma-ray analysis (MPGA) to pelagic
sediments to examine the K/Ti ratio. The obtained
ratios of sediments and standard reference materials
have shown a good agreement with those by PGA.
K106: Applications of neutron activation analysis
in environmental chemistry. –Presence of
extractable organohalogens (EOX) in wildlife
KAWANO, M.
(Faculty of Agriculture, Ehime Univ.)
Many kinds and large amounts of syntheticorganohalogen compounds are produced and areused in our daily life, and some of them introduced
to the natural environment. In some cases, those
substances that have dispersed in the naturalenvironment are harmful for wildlife and for humans
due to their persistency and their high toxicities.
Neutron activation analysis (NAA) is suitable fortrace amounts in biological samples such as wildlife
in order to understand the levels as organic boundhalogens, namely extractable organohalogens (EOX).
The analytical procedures are as follows: extracting
EOX with organic solvents from the sample, washing
the extract with deionized and distilled water,
fractionating with gel permeation column
chromatography. Finally, NAA were performed with
JRR-3 and JRR-4 of Japan Atomic Energy Agency
located in Ibaraki, Japan. Gamma-ray spectrometry
was performed just after irradiation. The gamma-rays
from 38Cl, 80Br and 82Br, and 128I were measured by
gamma-ray spectrometry. Gas chromatograph (GC)/
Mass spectrometry (MS) was performed with same
samples.
K107: What can you know from trace elements in
old iron?
HIRAI, S.
(Tokyo City Univ.)
The use of iron started for about 4000 years in
the history of mankind.
Iron greatly develops
human civilization, and it is still essential resource.

− 159 −

Iron is called steel or a cast iron by the concentrationof carbon and characteristic property is different.
In the impurity elements of iron, there is something
for which information exists in the iron raw material
has been left.
Arsenic and antimony of the
impurity are important elements for the identificationof source of iron raw material. Namely, the As/ Sb
concentration ratio is an index of source of iron raw
material.
An instrumental neutron activation
analysis is one of the most suitable analyticalmethods for determination of Arsenic and Antimony
in old iron as cultural properties.
However,
applications of the instrumental neutron activation
analysis for cultural properties field in our country
are not enough.
The development of further uses
to this field is expected.

multiple prompt gamma-ray analysis in an integrated
analytical company will be discussed.
Figure 1 shows 2-D spectrum of Cl 1000 µg
added to NIST SRM 1632a (Bituminous Coal)obtained by using STELLA. Figure 2 shows 1-D
spectrum of Cl obtained from the same measurement.
In this case, determination limit of Cl was estimatedto be 10 µg/g. For the other some elements,
determination limits were ranged from 0.x – 10×xµg/g. This method is one of the ideal bulk analysis
methods and the determination limit of Cl seems tobe sufficiently useful in the industrial fields.

K108: A value of multiple prompt gamma-ray
analysis in an integrated analytical company

NAGANO, A.
(S.H.I. Examination & Inspection, Ltd.)SUSHIDA, K.1, KOJIMA. N.1, TANIGUCHI, M.1,
MURAKAMI, Y.2, OSHIMA, M.3, TOH, Y.3,
FURUTAKA, K.3, HARA, K.3, HARADA, H.3,
KIMURA, A.3, KIN, T.3, KOIZUMI, M.3,
NAKAMURA, S.3(Toray Research Center, Inc.1, Research Institute of
Nuclear Engineering, Fukui Univ.2, Japan Atomic
Energy Agency3)

We have executed the contract Charged-Particle
Activation Analysis (CPAA) by using our compact
cyclotron for 20 years or more. CPAA is an analysis
a light element in metallic materials and othermaterials. We have analyzed 3657 samples in theseabout 20 years.The requests of the customers havechiefly analyzed semiconductor materials in CPAA.
In the first stage, this technique was used to develop
the method of manufacturing semiconductormaterials.
The analysis of metallic materials
increased after that, too. However, the number ofrequests has not increased in dramatic form.
And, we have been beginning the contract
Neutron activation analysis by using the equipmentof JRR-3 since 2008. We have executed theanalysis that exceeds 3000 samples by using k0
method. The requests of the customers have chiefly
analyzed environmental sample was analyzed in
NAA.
It seems that the request amount in the future by
300-400 samples par year in our CPAA service. And,
it is forecast that the number of requests doesn’t
expand because our NAA service has the restriction
at the machine time.

Neutron activation analysis has been regarded
to be one of the high sensitive elemental analysis
methods as shown in text books. However, some of
the nuclear reactors for research were stopped anddoors of the other reactors are almost closed. Thus,
utilization of the method in the industrial fields is
opened only in the few nuclear facilities. In thecircumstances, frequency in use of the method in theindustrial fields is extremely going down. On theother hand, we know the rapid development of
ICP-MS from 1988 makes this method to apronominal of the ultra-trace elemental analysis
method. Recently, Japan Atomic Energy Agency
developed GEMINI Prompt Gamma-Ray Analytical
Instruments
and STELLAMultiple Prompt
and promotes
Gamma-Ray Analytical Instrumentsa utilization of Multiple Gamma-Ray analysis.
Toray Research Center, Inc. cooperated to an
acquisition of basic data for MPGA data basethrough the inter-organization atomic energy
research program (2003~) or the promotion researchwith JST (2007~2010). In this presentation, basedon the results of these research programs, a value ofK109: Current request situation of contract
activation analysis service in S.H.I. Examination& Inspection, Ltd. and trend in the future

K110: Current Status of Activation Analysis
Experiments in KURRI
TAKAMIYA, K.1, TAKIMOTO, M.2, SEKIMOTO,
S.1, OKUMURA, R.1, NAKANO, U.1, SHIBATA,
S.1(1Research Reactor Institute, Kyoto Univ., 2Grad.

− 160 −

School of Engineering, Kyoto Univ.)
The operation of KUR with new low-enrichedfuels has been started in May 2010, and neutron
irradiation experiments have been also started inJune 2010. For the purpose of upgrading the various
systems for activation analysis experiments,
improvements of facilities and installations of new
equipments have been carried out in the down periodof KUR. As improvements of facilities, control
systems of pneumatic transport system, gamma-ray
spectrometry systems including an auto sample
changer, and other safe control systems have beendeveloped for the advanced and convenient
activation analysis experiments in safe environment.
And as installations of new equipments, the prompt
gamma-ray analysis equipment and the gamma-ray
spectrometry system composed of a Ge-detector anda well-type NaI(Tl) detector for short-lived nuclei
have been installed. The application range of neutron
activation analysis method in KURRI is expected tospread by those improvements and installations. For
the educational activity of activation analysis method,
the practical training program intended for graduate
students will start in 2010 for the purpose of
attaining basic knowledge and technique of neutron
activation analysis and radiochemical experiments.
K111: Development of MPGA in JRR-3 andJ-PARC
TOH, Y.1, FURUTAKA, K. 1, HARA, K. 1,
HARADA, H. 1, KIMURA, A. 1, KIN, T. 1,
KITATANI, F. 1, KOIZUMI, M. 1, NAKAMURA, S.
1, OSHIMA M. 1, MURAKAMI Y. 2
(1JAEA, 2Fukui Univ.)
A neutron beam line and a detector system for
MPGA were constructed at the neutron guide hall of
JRR-3M at Japan Atomic Energy Agency (JAEA).
The MPGA detector system consists of eight clover
detectors with BGO Compton suppressors.
Accidental coincidence rates increase with a squareof an intensity of a neutron beam, while truecoincidences increase only linearly with an intensityof a neutron beam. Therefore, a neutron attenuatorsystem consisting of acrylic plates was installed in
front of the MPGA beam line. Polymers, foods, andstandard samples were measured using the MPGA
detector system. Hydrogen backgrounds werereduced in gamma-ray spectrum of MPGA.
A pulsed neutron beam is produced by a pulsed

proton beam in J-PARC. Neutron capture crosssection shows sharp peaks, known as resonances, atenergies specific for each isotope. The energy of aneutron can be determined by the TOF method where
the flight time of neutrons is obtained by a timedifference measurement. A signal-to-noise ratio in
gamma-ray spectra of MPGA using TOF for energy
selection will be more improved than that without
TOF.
K112: Promotion of utilization for neutron
activation analysis at JAEA
MATSUE, H.
(Department of Research Reactor and Tandem
Accelerator, Japan Atomic Energy Agency)
In this lecture, activity of utilization promotion
including neutron activation analysis that has stared
as the common promotion project will be introduced
while industrial promotion project of Prompt
gamma-ray analysis by the trial-use program forneutron industrial applications will be introduced.
K113: Networking of neutron activation analysis
people in Asia-Australia.
EBIHARA, M.
(Grad. School of Sci. and Engineer., Tokyo
Metropolitan University)
Research reactors are essential for neutron
activation analysis but their utilizations have been
decreasing worldwide, especially in western
European countries and US. Although Japan seems
to have been following such countries, the current
situation surrounding research reactors utilized forneutron activation analysis is rather stable,considering that the Kyoto University reactor andtwo reactors of JRR-3 and JRR-4 in Japan Atomic
Energy Agency are currently running. However,these reactors were not operated from July 2009 to
March 2010, which caused serious influence to us
both in education and in research.
Nine Asian countries (Bangladesh, China,
Indonesia, Japan, Korea, Malaysia, Philippines,
Thailand and Vietnam) and Australia are allied under
the frame of Forum for Nuclear Cooperation in Asia,
which is financially supported by MEXT and the
Cabinet office. Neutron activation analysis has beenchosen as a project since the FNCA was establishedin 2000. In future, it is desired that the activity of the
FNCA/NAA alliance will be extended so that
unexpected suppression of reactors cannot be fatal in− 161 −

any FNCA countries.
K201: Radionuclides in Diagnostic
Medicine  Present and Future

Nuclear

HATAZAWA J.
(Osaka University Graduate School of Medicine)
The present crisis of diagnostic nuclear
medicine is a shortage of 99Mo-99mTc supply fromover-sea reactors. Several trials demonstrated apotential application of accelerator to produce
abundant amount of 99mTc for medical use. Domestic
production and stable supply is essential in futurenuclear medicine.
In biomedical science, the target is a molecularbasis of disease. 124I is quite useful to label peptides,
nucleic acids, and glycoprotein. The tracing of 52Fe,
62
Zn, and 48Ca may reveal new insight of physiology
in immune system and intracellular signaltransduction.
K202: Targeted radionuclide therapy – Current
status and a perspective
KINUYA, S.
(Dept. Nucl. Med., Kanazawa Univ.)

us predict therapeutic response of lesions andpossible adverse reaction. Therefore, TRT is patientspecific, tailored treatment. Based on these conceptsof TRT, we would like to propose to call TRT
targeting confirmative therapy (TCT).
Therapeutic effects are currently provided withβ particles of radionuclides. Cells within millimeter
path length of β particles are irradiated, so that it is
not necessary to target all cells in lesions. In addition,
many of them are irradiated by several β rays
(cross-fire effects), making the advantage of TRT
over non-radioactive pharmaceuticals. Αlfa emittersor Auger electron emitters with high LET (linear
energy transfer) and RBE (relative biologicaleffectiveness) are candidates for the next generationof therapeutic radionuclides.
What we have to consider in developing new
therapeutic radiopharmaceuticals is a radiation safetyissue. Non-gamma emitters or radionuclides withlow energy, low-probability gamma
emission
would be better candidates for future targetedradionuclide therapy. For non-gamma emitters, weshould need counterparts possessing gamma
emission as a case of 90Y-111In in order to utilize theadvantage of TCT.
K203:
ApplicationofPharmacological Sciences

In Japan, 4 types of targeted radionuclide
therapies (TRT) are currently available for routine
use, including 131I-sodium iodide for thyroid cancer
and hyperthyroidism, 131I-metaiodobenzylguanidine(MIBG) for malignant neuroendcrine tumors such as
pheochromocytoma and neuroblastoma, 90Y-labaled
murine monoclonal IgG1 for B-cell lymphoma(radioimmunotherapy)(Zevalin®),and89
Sr-strontium chloride (Metastron®) for palliationof painful bone metastases. Because of their targetingmechanisms, TRT is a true form of moleculartargeted therapies.
As many of radionuclides emit γ ray orpositron, in vivo distribution of radiopharmaceuticals
can be delineated by scintigrphic technique withsingle photon computed tomography (SPECT) or
positron emission tomography (PET), which makes
TRT a surely unique therapeutic modality. That is,
we can confirm targeting of radiopharmaceuticals in
lesions. Furthermore, their distribution in normal
tissues can be simultaneously monitored. In addition,
we can obtain changes in their distribution withsequential image acquisition, which provides
pharmacokinetic data on them. These features enable

RI

Imagingin

INOUE, O.
(Division of Health Sciences, Graduate School of
Medicine, Osaka University)[Introduction] Radiotracer method using bemitters such as 3H, 14C, 32P and 35S has been widely
applied in the field of pharmacological sciences
because of its high sensitivity as compared to othermethods. Recently, imaging with positron emission
tomography (PET) becomes one of the key
technologies in the drug developing process. In
therapy assessment of new drug in animals andhumans, PET imaging would be of great value toestimate pharmacokinetics parameters as well as
pharmacological effects (including the adverse
effects). The current state of application of PET
imaging in the development of new drugs will bepresented.
[Pharmacokinetics] Using 11C- or other positron
emitters-labeled
newcompounds,
theirpharmacokinetic studies can be performed in humansubjects with PET imaging. This method is called as‘micro-dosing test’, and absorption, distribution,− 162 −

metabolism and excretion in human can be directly
measured by employing this micro-dosing method.
The method seems to be of value as a screening test
prior to starting clinical trials of the new compounds.
Because of very short half-lives of positron emitters,
the development of new radiosynthesis method isrequired.
[Drug-target interactions] Many compounds
under developing are selective molecules to target
proteins such as receptors and enzymes. Drug-target
interactions in intact whole body either experimental
animals or humans also can be measured by using
selective PET radioligands. For example, themeasurement of receptor occupancy, and rate
constants (association or dissociation) of thecompound for the target molecule could provide
valuable information for preparing the clinicalprotocol. In order to apply this technology for the
new target molecule, the new PET probe should bedesigned and evaluated, which is considerably
difficult subject in future study.
[Pharmacological effects] The most importantand valuable subject in PET imaging fordevelopment of new drugs is to find out the new
biomarker, which enable us to evaluate
pharmacological effects of the new compound in
human especially in patients with target disease. The
efficacy of the new drug can be obtained as changes
in parameters of image.
The development of the new biomarker for PET
imaging is useful for not only monitoring the new
drug treatment, but also early diagnosis of disease as
early as possible.
[Conclusion] PET imaging has high potentials as a
key technology in developing new therapeutic drugs.
The development of new imaging biomarker is themost important subject for the above purpose.
K204: Therapeutic effects for bone metastases
using a-emitting radionuclides, 227Th, 226Th, 223Ra
in rats
WASHIYAMA, K.1, YAMAMURA, T.2, SATOU,
I.2, MITSUGASHIRA, T.3, TAKAHASHI, N.4,
SHINOHARA, A.4, YOKOYAMA, A.5, AMANO,
R.1(1College of Medical, Pharmaceutical and Health
Sciences, Kanazawa Univ., 2Institute for Materials
Res., Tohoku Univ., 3Oarai branch, Institute forMaterials Res., Tohoku Univ., 4Grad. School of Sci.,
Osaka Univ., 5College of Sci. and Engineering,
Kanazawa Univ.)

Due to short range and high liner energy transfer
of alpha particle in human tissue, targeted alphatherapy has been promised for cancer therapy andmany clinical studies have been performed.
Especially, 223Ra has been studied in a phase 3 as atherapeutic agent for bone metastases from prostatecancer. Radium-223 decays to stable 207Pb withemission of about 28 MeV.
We have been studied another alpha-emitting
nuclide 227Th, which is the parent nuclide of 223Ra.
As the half-lives of 227Th and 223Ra are similar, it will
be possible to avoid the high-dose alpha-particles of223
Ra and its progeny nuclides during the initial
blood circulation after administration of 227Th. In
addition, the radioactive growth of 223Ra will prolong
the effective irradiation duration. Thorium-227 emits
alpha-particles with an average energy of 5.9 MeV.
Thorium-226 d is an alpha-emitting radionuclide
which decays with a rapid cascade of 4 alphaparticles with about 28 MeV of total energy. Because
thorium is easy to label with EDTMP, 226Th-EDTMP
is also a promising agent for bone metastases.
In this study, we evaluated the therapeutic effectsofthreebone-seeking
alpha-emitting
223
227
radiopharmaceuticals,
RaCl2,
Th-EDTMP,
226
Th-EDTMP from the point of view of thehalf-lives, and internal dosimetry.
K205: New Molecular Imaging approach using
Electron Tracking Compton Gamma Ray with
Possible Application of new various Radio
Isotopes
TANIMORI, T.1(1Grad. School of Sci., Kyoto University)
We have developed the Electron tracking
Compton Camera (ETCC) with reconstructing the
3-D tracks of the scattered electron in Compton
process for both gamma-ray astronomy and nuclear
medicine.
By measuring the direction  of ascattered electron, the direction of the incident
gamma ray is uniquely determined for an individual
photon. Then ETCC can provide a clear image suchas concentration to tumors in a mouse, which is asimilar imaging ability to human PET. Thus,
ETCC (CC) has a good imaging power over the wide
energy dynamic range (200 - 1500keV) with a wide
field of view (FOV, 3str), and then it is ensured that
this camera has a potential of developing the newreagents for molecular imaging. Already we have

− 163 −

carried out several comparisons of our images withthose of SPECT and PET. Also, multi-tracer image
using I-131 and FDG, and imaging test using several
RIs (ex. 54Mn ,65Zn) emitting higher energy gamma
rays than 511keV for small animals have been
carried out successfully. Recently several new
biomarkers including nano-particles for drugdelivering approach were examined to verify the
merits of ETCC for medical imaging. In addition,
we will present the unique ability of ETCC toreconstruct 3D image only from one directional
observation.
K206: Research and developments of themultiple-molecular imaging GREI and newmolecular imaging probes
ENOMOTO, S.1, 2(1 Grad. School of Med. Dent. Pharm. Sci., Okayama
Univ., 2 Center for Molecular Imaging Science,
RIKEN)
Multiple molecular imaging, whichallows simultaneous visualization of themolecular dynamics in various biologicalprocesses, is required to achieve moreadvanced and precise diagnosis. To realize themultiple molecular imaging, we havedemonstrated the feasibility of semiconductor
Compton cameras for multiple molecularimaging in nuclear medicine. The Compton
camera used in this work comprises two
double-sided orthogonal-strip germanium
detectors, which we call “GREI (Gamma-Ray
Emission Imaging)”. Their excellent energy
resolution enabled discrimination of thenuclides and accurate determination of thescattering angle for γ rays in wide energy
range. In parallel with the systemdevelopment, it is also required that
exploration of imaging probes which havesuitable characteristics for the GREI. The
throughput speed and sensitivity of thepresent prototype is not so powerful thatapproximately 10 hours of data acquisition isneeded for a reasonable image reconstruction.
To satisfy such requirement, we investigatedan experimental model using tumor-bearing
mice and antibody probes. For example,
cetuximab, anti epidermal growth factor
receptor (EGFR) antibody, was labeled with
64Cu and injected to the EGFR-over expressing

tumor-bearing
mouse.
The
similar64
accumulation of Cu in the tumor region was
detected by PET and GREI. Using the GREI,
the in vivo distributions of the multiple
molecules are able to be visualized
simultaneously by labeling with different
radioactive metal nuclide.
K207: The production for nuclear medicine at the
Research Center for Nuclear Physics Osaka
University
TAKAHASHI, N1., KURIYAMA, A1., NAKAI, K1.,
SHINOHARA, A1., HATAZAWA, J2., KANAI, H2.,
HATANAKA, K3.,TAKAHISA , K.3(1Grad. School of Sci., Osaka Univ., 2 Grad. Schoolof Medic., Osaka Univ., 3Rec.Cent.for Nucl. Phys.,
Osaka Univ.)
Recently, positron emission tomography(PET) has
been remarkably developed for visualizing the
distribution of a radionuclide the human andanimal’s body. Now the system is widely used forthe diagnosis of cancer. Clinical application of PET
has been made possible with the development of
ingenious techniques for rapid synthesis ofradiopharmaceuticals, suitable for in vivo studies,using cyclotron within a medical complex.
We selected to produce the radioisotope-labeled
hematoporphyrin for the PET although theradio-pharmaceutical mostly used is the 18F-labeledfluoro-deoxy-glucose which is similar to glucose in52
behavior,We
synthesizedFe(T1/2=8.28h),
62
Zn(T1/2=9.3h) and 124I(T1/2=4.18d) which werepositron emitters by the 52Cr(3He,3n)52Fe,
62
Cu(p,n)62Zn and 124Te(p,n)124I reaction, respectively
with the AVF cyclotron at Research Center for
Nuclear Physics, Osaka University.
The PET imaging used 62Zn and 124I were obtained
and further we plan to them using porphyrin
compounds.
K208: RI production in RIKEN for medical andpharmacological studies.
KANAYAMA, Y.,1 HABA, H.,2 ENOMOTO, S.1,3(1RIKEN CMIS, 2RIKEN Nishina Center ofAccelerator-Based Science. 3Grad. School of
Medicine, Dentistry, and Pharmaceutical Sciences,
Okayama Univ.)− 164 −In

RIKEN

Nishina

CenterforAccelerator-Based Science, we have establishedproduction methods of various radioisotopes (RIs)
including 48V, 65Zn, 89Zr, and 109Cd by use of the
RIKEN Ring Cyclotron and AVF Cyclotron. TheseRIs have been used for tracer studies in medicine,
pharmacology, biology, nuclear chemistry, and so on.
On the other hand, we have developed asemiconductor Compton camera called “GREI”,
which enables the simultaneous visualizing of RI
distributions in wide gamma-ray energy range. In
addition, because of a number of biomolecular
medicines have developed and are considered as
molecular imaging probes, there is growing interestfor production of intermediate-half-life RIs. In
RIKEN Center for Molecular Imaging Science, wehave established the 64Cu (T1/2=12.7 hour)
production method using a small cyclotron.
Moreover, we have started to develop the 65Zn and89
Zr production method. The outlines of these RI
production methods and imaging applications in
RIKEN will be discussed.
K209: Global Medical Isotope Crisis threatens
Nuclear Medicine Diagnoses (99mTc)
NAKAMURA, Y.
JAPAN RADIOISOTOPE ASSOCIATION
Two of the most important isotope producing
reactors, NRU reactor in Canada and HFR reactor in
the Netherlands, are currently shut down. The
production of more than 95% of the available Mo-99
has been performed in only five reactors in the world
including above two reactors. Tc-99m is used inabout 65% of all diagnostic nuclear imaging
procedures, corresponding to about 0.9 million
procedures yearly in Japan. NRU and HFR are
expected to come back online at latest in coming
September. The current medical isotope crisis will be
alleviated after the two reactors returning to service.
However, all of these five reactors are approximately
50 years old. Because the remaining life time ofthese reactors is not long, new reactors being built or
new technology being developed, such as accelerator
methods or the neutron capture of Mo-98 in a reactor,
are proposed for the security of supply of medical
isotopes.
In addition to a problem of the production rate,
the methods using the molybdenum target lead tomuch lower specific activity Mo-99 compared to thefission technology. This would not work with current
Tc-99m generators and would cause a problem with

Tc-99m imaging kits. The new chemical processing
technologies,
manufacturing
Tc-99mradiopharmaceuticals from such low specific activity
Mo-99, are more importantly expected.
K210: Radiochemistry and medical radioisotopes
produced by accelerator neutrons
NAGAI, Y., HATSUKAWA, Y., HARADA, H.,
KIN, T., SEGAWA, M., KONNO, C., OCHIAI, K.,
TAKAKURA, K., IWAMOTO, O., IWAMOTO, N.,
MINATO, F.
(Japan Atomic Energy Agency)99m

Tc with a half-life (T1/2) of 6 h, the daughter
nuclide of 99Mo with T1/2 = 66 h, has been mostwidely used in nuclear medicine for diagnostics. So
far, various reactions such as 100Mo(p,pn)99Mo,
100
Mo(p,2n)99mTc, and 100Mo(γ,n)99Mo were studied
to produce 99Mo or 99mTc. Recently, we proposed a
new route to produce 99Mo via 100Mo(n,2n)99Mo
using fast neutrons from an accelerator. Note that the(n,2n) reaction cross section is quite large, ∼ 1.5 b atneutron energy En ∼ 14 MeV, cross sections forradioactive waste production reactions, such as (n,α),(n,np), (n,p), and (n,γ), at En ∼ 14 MeV are quite
small, and intense ∼ 14 MeV neutrons could beobtained using a small accelerator. In addition, asignificant progress has been achieved in accelerator
technology, which enables us to obtain high flux fastneutrons. These features could allow us to obtain asignificant amount of 99Mo using the proposed
method. We could also obtain various medical
radioisotopes using fast neutrons from accelerators. I
will discuss our works of medical isotope production
and an important role of radiochemistry in the
medical application of the isotopes.
1A01: Nuclear deformation dependence of theexcitation functions of heavy ion fusion reactionin the 139La+16O, 159Tb+16O and 169Tm+16O
systems
KAIYA, H.1, ASANO, A.1, TODA, K.1, TAKEDA,
Y.1, OOE, K.2, KIKUNAGA, H.2, TAKAHASHI, N.2,
YOKOYAMA, A.3(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,
2
Grad. School Sci., Osaka Univ., 3Inst. Sci. Eng.,
Kanazawa Univ.)
We have performed experiments for thesyntheses of heavy elements in the natLa + 16O, 169Tm+ 16O and 159Tb + 16O systems to discuss the effect of− 165 −

nuclear deformation of targets having different
deformations. The evaporation residue cross sections
were measured by using a stack technique and / or a
gas-jet technique. The cross sections were derived
from radioactivities of the products and used forconstructing excitation functions of nuclear fusion. It
was found that the threshold in the fusion reaction
gets lower for the deformed targets. This may be
because the coulomb barrier changes according toconfiguration of the deformed targets and the
projectile. Further discussion will be made with thetheoretical calculation with the ALICE code and the
HIVAP code.
1A02:
Fissionfragment
anisotropy
heavy-ion-induced fission of actinides

in

NISHINAKA, I.1, NISHIO, K.1, TANIKAWA, M.2,
MAKII H.1, WAKABAYASHI, Y.1, MITSUOKA, S.1,
YOKOYAMA, A.3(1Advanced Sci. Res. Center, JAEA, 2Fac. Sci., Univ.
Tokyo, 3Inst. Sci. Eng., Kanazawa Univ.)
In heavy-ion-induced fission of actinides,
fission fragment anisotropy has been found to
become anomalously high compared with that
expected from the standard saddle model. The
pre-equilibrium K-state model suggests that entrance
channel mass asymmetry α=(At-Ap)/(At+Ap) plays animportant role for fission fragment anisotropy inheavy-ion-induced fission of actinides. However, alimited number of experiments have been carried out
to study the effects of different entrance channels
leading to the same compound nucleus. In order tostudy the effects of entrance channel mass
asymmetry α on fission fragment anisotropy, wemeasured fission fragment angular distributions in
the reactions of 22Ne+232Th (α=0.827) and 12C+242Pu(α=0.906), populating the same compound nucleus
254
Fm. At the JAEA tandem accelerator fission
fragments from the compound nucleus at excitationenergies of Eex=56.1, 52.5, 48.8 and 45.2 MeV were
measured by four position-sensitive parallel-plateavalanche counters and a silicon surface barrier
detector. The measured center-of-mass angular
distributions of fission fragments W(θ) provides thefissionfragment
anisotropy
definedas
A=W(180o)/W(90o). The anisotropy for 22Ne+232Th
with small entrance channel mass asymmetry
α=0.827 shows large values compared with those for12
C+242Pu with α=0.906. This implies that entrance
channel mass asymmetry plays a role for fission

fragment anisotropy in the present systems.
1A03:
Cross-section
measurementfor
neutron-induced fission of minor actinides using
Kyoto University lead slowing-down spectrometer
Hirose, K.1, Ohtsuki, T.1, Shibasaki, Y.1, Iwasa,
N.2, Hori, J.3, Sekimoto, S.3, Takamiya, K.3,
Yashima, H.3, Nishio, K.4, Kiyanagi, Y.5(1Research Center for Electron Photon Science,
Tohoku Univ., 2Grad. School of Sci., Tohoku Univ.,
3
Research Reactor Institute, Kyoto Univ., 4JAEA,
5
Grad. School of Eng., Hokkaido Univ.)
The neutron-induced fission cross-sections forminor actinides (MA) have been measured in theneutron energy range from 0.03eV to 2keV using thelead slowing-down spectrometer (KULS) at the
Research Reactor Institute, Kyoto University. The
KULS is a lead cube of 1.5x1.5x1.5m3. Neutrons areproduced by irradiating tantalum plates located in thecenter of the KULS with a 30-MeV pulsed electron
beam. The neutrons are slowed down by inelastic
and elastic scatterings and finally reach to a MA
sample. The neutron energy was determined from thetime-of-flight in the lead material. Although theenergy resolution is about 40%, a high neutron flux
is available using the KULS since the sample can be
irradiated at a small distance, typically 40cm, fromthe neutron production target. Up to now, thecross-sections for 237Np, 241, 242m, 243Am, 245, 248Cm
were obtained. In the presentation, the results of themeasurement, mainly for 248Cm will be shown.
Present study is the result of “Study on nuclear
data by using a high intensity pulsed neutron source
for advanced nuclear system” entrusted to Hokkaido
University by the Ministry of Education, Culture,
Sports, Science and Technology of Japan (MEXT).
1A04: Production and decay properties of 261a,bRf
MURAKAMI, M.1, MURAYAMA, H.1, GOTO, S.2,
KAJI, D.3, MORIMOTO, K.3, HABA, H.3,
KASAMATSU, Y.3,4, KUDOU, Y.3, YONEDA, A.3,
MORITA, K.3, KUDO, H.5(1Grad. School of Sci. and Technol., Niigata Univ.,
2
Center for Instrumental Anal., Niigata Univ.,
3
Nishina Center, RIKEN, 4Grad. School of Sci.,
Osaka Univ., 5Fac. of Sci., Niigata Univ.)
Relatively long-lived isotope of Rf, 261aRf (T1/2= 68 s), has been used in chemistry experiments of− 166 −

Rf. In recent years, it is said that a short-lived isomerof 261Rf, 261bRf (T1/2 = 3 s), exists. Although this
spontaneously fissioning 3-s activity was known
previously, it had been assigned to 262Rf. The aim of
the present work is to clarify existence of theshort-lived isomer of 261Rf by direct production of Rf
isotopes.
Experiments were performed at the RIKEN
linear accelerator (RILAC) facility using a gas-filled
recoil ion separator, GARIS. Rf isotopes were
produced in the reaction of 18O on 248Cm. A
248
Cm2O3 rotating target having a thickness of 230 µg
cm 2 was irradiated by 18O beams of energies of 88.2,
90.2, 94.9, and 101.3 MeV at the middle of the target.
Produced nuclides in the 248Cm(18O, xn)266 xRfreaction were separated from the beam by GARIS,
and implanted into a position sensitive detector
which mounted on the focal plane of GARIS. The
beam was switched ON−OFF repeatedly at constanttime intervals, and the measurements were
performed only in the beam OFF period. In order todistinguish the decays of 261bRf and 262Rf (T1/2 = 47ms), beam ON−OFF time intervals were set to 6 s−6s and 0.1 s−0.1 s, respectively.
−

265

Sg → 261Rf → (257No →) were revised together
with those of 261Rf in our previous 248Cm(18O,5n)experiment.
The
cross
sections
for
the
248
Cm(22Ne,5n)265Sg reactions at 118 MeV wereroughly evaluated to be 200 pb for 265aSg and 170 pb
for 265bSg. In the symposium, the results of the
production of 90Mo and 173W via thenat
Ge(22Ne,xn)90Mo and natGd(22Ne,xn)173W reactions,
respectively, will be also presented for futurechemistry experiments of Sg.
1A06: α-HiB complexation and ion-exchange
behavior of the group-4 elements
as homologues of Rf.

−

1A05: Production
of
22
265
Cm( Ne,5n) Sg reaction

265

Sg

via

the

248

HABA, H.1, OOE, K.2, OZEKI, K.1, KASAMATSU,
Y.2, KAJI, D.1, KIKUNAGA, H.1, KUDO, H.3,
KUDOU, Y.1, KOMORI, Y.1, SATO, N.4,
SHINOHARA, A.1, SUMITA, T.1, TSUKADA, K.4,
MORITA, K.1, MORIMOTO, K.1, YONEDA, A.1(1Nishina Center, RIKEN, 2Graduate School of
Science, Osaka Univ., 3Faculty of Science, Niigata
Univ., 4Advanced Science Research Center, JAEA)
We are developing a gas-jet transport system
coupled to the RIKEN gas-filled recoil ion separator
GARIS to start superheavy element chemistry in
RIKEN. In this work, we have investigated theperformance of the system using an isotope ofelement 106, 265Sg, produced in the 248Cm(22Ne,5n)reaction. Alpha-particles of 265Sg separated withGARIS and extracted to a chemistry laboratory weresuccessfully identified with a rotating wheel system
for α-spectrometry under low background conditions.
Based on time-correlated 24 α-α(-α) and 18 α-SF
(Spontaneous Fission) events, two isomeric states in
265
Sg, 265aSg (α energy Eα = 8.84 MeV, half-life T1/2 =6.7 s) and 265bSg (Eα = 8.69 MeV, T1/2 = 15 s), wereidentified. The decay patterns of 265Sg in the chain

KIKUCHI, T.1, TOYOSHIMA, A.2, LI, Z., J.2,
TSUKADA, K.2, ASAI, M.2, SATO, T.K.2, SATO,
N.2, NAGAME, Y. 1,2, KASAMATSU, Y.3, FAN, F.
L.4(1Grad. School of Sci. and Eng., Ibraraki Univ.,
2
Advansed Sci. Research Center, JAEA, 3 Grad.
School of Sci., Osaka Univ., 4Institute of Modern
Phys., Chinese Academy of Sci.)
α-HiB complexation and cation-exchange
behavior of Zr, Hf, and Th as homologues of Rf havebeen studied by a batch method using the carrier-freeradiotracers 88Zr, 175Hf and 234Th. It was found thatthe cation-exchange behavior of Zr, Hf, and Th in
α-HiB / HNO3 reaches equilibrium at 180 min under
the given conditions. The distribution coefficients(Kd values) of Zr and Hf on the cation-exchange resinat [H+] = 0.1 M decreased with an increase of[α-HiB-], reflecting successive formation of α-HiB
complexes of these elements. In contrast, Th and Y
which is used as a representative of the trivalent ion
were strongly adsorbed on the resin under the same
conditions, obviously showing different behavior
from that of Zr and Hf.
1A07: Sulfate complexation of element 104, Rf, in
H2SO4/HNO3 mixed solution ([H+] = 1.0 M)
LI, Z. J.1, TOYOSHIMA, A.1, ASAI, M.1,
TSUKADA, K.1, SATO, T. K.1, SATO, N.1,
KIKUCHI, T.1, SCHÄDEL, M.1, NAGAME, Y.1,
LIANG, X. H.2, KASAMATSU, Y.3, KOMORI, Y.3,
GOTO, S.4,
OOE, K.3, SHINOHARA, A.3,
4
4
MURAYAMA, H. , MURAKAMI, M. , KUDO, H.4,
HABA, H.5, TAKEDA, Y.6, NISHIKAWA, M.6,
YOKOYAMA, A.6, IKARASHI, S.7, SUEKI, K.7,
AND AKIYAMA, K.8− 167 −

(1ASRC, JAEA, 2CIAE, 3Osaka Univ., 4Niigata Univ.,
5
Nishina Center, RIKEN, 6Kanazawa Univ., 7Univ.
of Tsukuba, 8Tokyo Metropolitan Univ. )Cation-exchange behavior of 261Rf (T1/2 = 78 s)
produced in the 248Cm(18O, 5n) reaction was studied
on a “one-atom-at-a-time” scale in H2SO4 (0.15−0.69
M)/HNO3 mixed solutions ([H+] = 1.0 M) using an
automated ion-exchange separation apparatus
coupledwiththedetectionsystemforalpha-spectroscopy. It was found that adsorption
probability (%ads) of 261Rf on cation-exchange resin
decreases with increasing [HSO4-], showing a
successive formation of its sulfate complexes. Rf
exhibited much weaker formation of the complexes
than the lighter homologues Zr and Hf, which isqualitatively in good agreement with theoretical
calculations including relativistic effects.
1A08: On-line isothermal chromatographic
behavior of the group-5 elements Nb and Ta as
homologues of Db
SATO, T. K. 1, TSUKADA, K. 1, ASAI, M. 1,
TOYOSHIMA, A. 1, SATO, N. 1, Li Z.J. 1,
KASAMATSU, Y. 2, KIKUCHI, T. 1, 3, LIANG, X. 1,
KANEYA, Y. 1, 3, NAGAME, Y. 1, SCHDEL, M. 1
(1ASRC, JAEA, 2Osaka Univ., 3Ibaraki Univ.,)
To investigate chemical properties of thetransactinide element dubnium (Db, Z = 105), we
have so far developed an on-line isothermal gas
chromatographic apparatus. In this work, the on-line
experiments with group-5 elements, Nb and Ta,
using short-lived isotopes 88Nb and 170Ta as thehomologues of Db were carried out. We determined
optimum conditions to produce volatile compoundsof the elements. Under the obtained conditions,overall efficiencies of the volatile compounds were
measured as a function of the isothermal temperaturein chlorinating condition with mixture of nitrogengas and the SOCl2 vapor containing 1% oxygen.
Maximum yields of Nb and Ta were about 10 % and
15 %, respectively. Based on the isothermal gas
chromatographic behavior of them, it was found that
Ta compounds would be less volatile than Nb ones.
1A09: Research on gas-phase chemistry forchloride of group-4 elements
MURAYAMA, H.1, KOJIMA, T.1, MURAKAMI,
M.1, GOTO, S.2,KUDO,H.1,

TSUKADA,K.3,ASAI,M.3,TOYOSHIMA,A.3,SA
TO,T,K.3,SATO,N.3,NAGAME,Y.3(1Fac.of Sci.,Niigata Univ., 2 Center for Instrumental
Anal, Niigata Univ., 3JAEA.)
A gas-phase chemical separation is one of themost utilized techniques to study chemical properties
of superheavy elements (SHE). SHE’s produced innuclear reaction are converted to volatile compounds
by chemical reaction. The volatility of SHE
compoundsisdeterminedby
theiradsorption-desorption processes on an isothermal
chromatographic column. In the present work, weinvestigated gas chromatographic behavior ofvolatile chloride compounds of group-4 elements
using a fabricated apparatus for the study of Rf.
The isotopes of Zr and Hf were produced in thenat
Ge(18O,xn) and natGd(18O,xn) reaction, respectively,
at the JAEA tandem accelerator facility. Nuclear
reaction products attached on a carbon cluster weretransported to the gas chromatographic apparatus bya He carrier gas flow.
The transported products were collected on quartz
wool plugged in a quartz tube where a reactive HClgas was added to form volatile chloride compounds.
The formed volatile compounds were then fed into
an isothermal chromatographic quartz column which
is directly connected to the quartz tube. The volatilecompounds of Zr and Hf passing through theisothermal column were collected on a glass filter at
a collection site. The efficiency of the transportationof nuclear reaction products and the formation ofvolatile compounds were determined by γ-ray
spectrometry using a HPGe detector.
The transportation efficiency was about 50%, and the
combined
efficiency
offormation
andre-transportation was about 20%.
Finally, the isothermal chromatogram of Zr and Hf
volatile compounds were measured precisely.
1A10: Electrochemical oxidation of nobelium
using a microchannel-electrode chip
OOE, K.1, KOMORI, Y.1, FUJISAWA, H.1,
KURIYAMA, A.1, TAKAYAMA, R.1, KIKUTANI,
Y.1, KIKUNAGA, H.1,2, KASAMATSU, Y.1,
YOSHIMURA, T.1, TAKAHASHI, N.1, HABA, H.2,
KUDOU, Y.2, EZAKI, Y.2, SHINOHARA, A.1(1Grad. School of Sci., Osaka Univ., 2Nishina
Center, RIKEN)
An electrochemical oxidation experiment of− 168 −

nobelium (No), element 102, has been carried out
using a microchannel-electrode chip which was a
microchip integrated with electrodes. The isotope
255
No (T1/2 = 3.1 min) was produced in the248
Cm(12C,5n) reaction using the RIKEN K70 AVF
cyclotron. The reaction products recoiling out of thetarget were transported by a He/KCl gas-jet transportsystem to a chemistry laboratory. The transported
products were then dissolved in 1 µL of 0.1 M HNO3.
The solution was fed into the microchannel-electrodechip and the potential of 500 or 1250 mV vs. Ag
pseudo-reference electrode was applied to theworking electrode. The effluent was mixed with 0.5
M di(2-ethylhexyl) phosphoric acid in CCl4 solution
and the mixture was shaken for 1 min to separate
No3+ from No2+. The activities of 255No in bothaqueous and organic phases were determined by
α-spectrometry using Si detectors. The oxidation of
No2+ to No3+ was observed at the applied potential of1250 mV, while at the applied potential of 500 mV,
No2+ was not oxidized.
1A11: Relationship between particle size
distributions of radioactive aerosols and theirhalf-lives in an accelerator facility
OSADA, N. 1, SEKIMOTO, S. 2, OKI, Y. 2, SHIBATA,
S. 2(1Graduate School of Engineering, Kyoto University,
2
Research Reactor Institute, Kyoto University)
In accelerator tunnels, aerosols formed byradiation were observed in the air. The radiation
causes chemical and nuclear reactions, and theradiation-induced species are considered to be thesource of the aerosol particles. The aerosols in thefacilities often incorporate various radionuclides. The
decay of the nuclides might influence the particle
size distribution. The Monte Carlo simulation of the
distribution was carried out to elucidate therelationship between the half-lives of theradionuclides and the particle size distribution. It
was assumed that initial particles had a lognormal
size distribution and that some of the aerosol
particles incorporate the radioactive nuclide. The firstsimulation only took account of growth bycondensation. The second simulation took account of
the attachment of radioactive nuclide to the aerosol
particle in addition to the first condensation model.
The growth of the aerosol particles and the decay of
the radionuclides in the aerosol were calculated. The
particle size distribution based on the activity was

also evaluated.
1A12: Temperature dependence of In-beam
Mössbauer spectra of 57Mn implanted into
magnesium oxide
NAGATOMO, T.1, KOBAYASHI, Y. 2, KUBO,
M.K. 1, YAMADA, Y. 3, MIHARA, M. 4, SATO,
W. 5, MIYAZAKI, J. 6, SATO, S. 7, KITAGAWA,
A. 7(1International Christian Univ., 2RIKEN Advanced
Meson Sci. Lab., 3Tokyo Univ. of Science,4
Osaka Univ., 4Kanazawa Univ., 6Nihon Univ.,
7
National Institute of Radiological Sciences)
A study of 57Fe in-beam Mössbauer
spectroscopy using 57Mn provides direct information
on exotic state of unstable nuclear probes and onelectronic properties of the surrounding materials at
the atomic scale. Recently, our detection method was
successfully improved to obtain in-beam Mössbauer
spectra with very large S/N ratio using HIMAC(Heavy Ion Medical Accelerator in Chiba) by
developments of the PPAC detector and theanti-coincidence detection method. Here, we havemeasured the emission Mössbauer spectra of 57Mn
implanted into a simple metal oxide solid MgO ofwhich temperature was controlled. The 57Mn ionswere produced as the projectile fragments of thehigh-energy 58Fe beam. The sample was an MgOpolycrystalline disk (50 mm diameter and 5 mm
thickness) purchased from Furuuchi Chemical Co.
The emission Mössbauer spectra of 57Mn implanted
into the MgO disk were obtained at the temperature
range from 61 K to 623 K. Based on the density
functional calculations, a singlet peak (I.S. = -0.94mm/s) is assigned to high-spin Fe2+ located at a
substitutional site of Mg2+ in MgO crystal. The otherdoublet components are considered to be Fe atoms
located the Mg substitutional sites with vacancies of
Mg or O atoms. Details of temperature dependenceof obtained Mössbauer spectra will be discussed.
1A13: Temperature dependence of Mössbauer
spectrum of 57Mn implanted into sodium fluoride
NAGATOMO, T.1,2, KOBAYASHI, Y.2, YAMADA,
Y.3, SATO, W.4, MIHARA, M.5, MIYAZAKI, J.6,
KUBO, M. K.1, SATO, S.7, KITAGAWA, A.7(1International Christian Univ., 2RIKEN, 3Tokyo
Univ. Sci., 4Kanazawa Univ., 5Osaka Univ., 6Nihon
Univ., 7National Inst. Radiol. Sci.)− 169 −

57

Mn in-beam Mössbauer spectra have beenmeasured for sodium fluoride at 293K, 373K, 473K,
623K and 773K in order to elucidate the chemicaland physical behaviors of trace transition metal
impurity in a simple ionic alkali halide of rock salt
type crystal structure. A singlet Mössbauer peak
was observed at all temperatures for thesubstitutional 57Fe site at the Na+ site of NaF. Two
additional doublet species were observed andinterpreted as 57Fe site with one or more crystal
defects around the 57Fe. At higher temperatures the
population of the defect sites decreased and thesinglet component increased, suggesting that thedefects were annealed and disappeared.
1A14: Studies of Giant Hyperfine Magnetic Fields
in Linear Two-Coordinate Fe Complexes
KOBAYASHI, Y.1, ITO, M.2, MATSUO, T.2, ISHII,
Y.1, WATANABE, I.1, TAMAO, K.2(1Advanced Meson Science Lab., RIKEN,
2Functional Elemento-Organic Chemistry Unit,
RIKEN)
There has been interested in transition-metal
complexes with lowering symmetry of unsaturated
linear two-coordination. It is reported that some ofthese complexes exhibit unique behavior in physicaland chemical properties, notably unusual magnetism.
Recently, we succeeded in synthesizing a linear
coordinate Fe complex with a newly developed“Rind” ligands, Fe[MPhindS]2 and Fe[MPhindNH]2.
“Rind” (R=Me, Ph) is based on a fused-rings-hydrindacenyl structure [1,2]. The X-ray structure
57
Fe
analysis,magnetization
measurement,
Mössbauer spectroscopy, and µSR were performed
to elucidate the physicochemical property of(S–Fe–S=161.4º)
andFe[MPhindS]2
Fe[MPhindNH]2 (N–Fe–N=179.1º).
Mössbauer absorption spectra were measured bya conventional method between 1.6 K and RT underapplied zero-field. The obtained Mössbauer spectra
could be analyzed a single component of symmetricdoublet down to 1.6 K. The derived values of I.S. and
Q.S. at 1.6 K were 0.83(1) mm/s and 1.04(2) mm/s,
respectively. It was assigned from these Mössbauer
parameters that Fe atoms of Fe[MPhindS]2 are inhigh-spin 2+ state. However, the linewidth (FWHM)
was not strongly dependent on temperature, and there
was no evidence of hyperfine magnetic splitting or
relaxation pattern at the lowest temperature. On the

other
hand,
the
Mössbauer
spectraof
Fe[MPhindNH]2 revealed the magnetic relaxation
below 77 K. We will discuss the origin of the giant
hyperfine magnetic fields of linear two-coordinate Fecomplexes.
Ref.:[1] A. Fukazawa et al., J. Am. Chem. Soc., 129,
14165 (2007).
[2] M. Ito et al., J. Am. Chem. Soc., 131, 18024(2009).
1A15: Iron nitride films with high nitrogencontent produced by laser deposition
USUI, R.1, YAMADA, Y.1, KOBAYASHI, Y.2(1Graduate School of Chemical Science andTechnology, the Tokyo University of Science,
2
RIKEN)
Iron nitride has been studied extensively,
because it can exist in many different phases withdifferent structures and properties with various
nitrogen contents. Paramagnetic phase with astoichiometry of FeN were recently discovered;γ’’-FeN and γ’’’-FeN. But only a mixture was found,and the single phases are yet to be obtained. We
performed PLD of Fe metal in N2 atmosphere to
produce iron nitride films deposited onto Al
substrates. The synthesized films were investigatedby Mössbauer spectroscopy, powder XRD and SEM.
Iron nitride films were produced onto Al
substrates at room temperature varying N2 pressure;changing the nitrogen content of the films. When thenitrogen pressure was kept at 70 Pa, γ’’-FeN (δ =0.07 mm/s) and γ ’’’-FeN (δ = 0.63 mm/s) were
produced. The substrate temperatures while PLD waschanged, while the nitrogen pressure was kept at 70
Pa. The sample produced at 100 K had γ’’-FeN as
dominant products, and the yield of γ’’’-FeN
enhanced by increasing the substrate temperature at
300 K. At the highest temperature at 520 K, γ’’’-FeN
became dominant and γ-Fe appeared. In this study, it
was demonstrated that the yields of γ’’-FeN and
γ’’’-FeN were controlled by changing the substratetemperature in PLD.
1A16: Dilute magnetism and Mössbauer spectraof nano SnO2 powders co-doped with Fe and V
ions
KONO, S1., NOMURA, K2., OKABAYASHI, J2.,
YAMADA, Y.1− 170 −

(1Tokyo University of Science.,
Tokyo.)

2

The University of

The magnetic properties of SnO2 are enhancedwith doping Fe concentration, and on the contrary,
the magnetic moments decrease with doping V
concentrations. In order to clarify the dilute
magnetism and to control the magnetic properties,
we study on co-doping effect of SnO2 with V and Fe
ions by Vibration Sample Magnetometer and
Mössbauer spectroscopy. The mixed powders of
SnO2:FenVX ( n=1, 2, x=0.5 ,1 ,2) were prepared by asol-gel method using citric acid and ethylene glycol.
The samples were annealed finally at 550oC for 2
hours. XRD patterns, which were not so affected byco-doping, showed only Rutile structure of SnO2.
SnO2 doped with 0.5%V and 1%Fe showed thestrongest ferromagnetism in those series. In the
Mossbauer spectrum, the magnetic sextet with Bhf=
50.7 T, δ= 0.38 mm/s, and 2ε =0.29 mm/s and Δ=1.14mm/s was observed in addition to two Fe3+
doublets, whereas Mössbauer spectra of the othersamples consisted of magnetic relaxation peaks andparamagnetic doublets. The bulk magnetic properties
may be correlated with the magnetic sextet.
1B01: Measurements of Mercury and Goldconcentrations in samples from tailing dams
which contaminated by Small Scale Mining, using
PGAA and INAA
HATSUKAWA, Y.1, OSAWA, T.1, APPEL, P.2,
ARCILLA, C.3, PEREZ, E. 4
(1JapanAtomic Energy Agency, 2Geological Surveyof Denmark and Greenland, 3Univ. of Philippines,
4
Ateneo Univ.)
Small scale gold mining is widely seen in many
places in the world. During gold extract processing,large amount of mercury was released in theenvironment.
Small-scale gold miners in thePhilippines use orders of magnitude more mercury
for extracting gold than small-scale miners in mostother countries. In the order of 145 tons of mercury
is released per year from some of the small-scale
mining communities. Extrapolated to the wholecountry 200 to 500 tons of mercury is released to theenvironment every year. Most of the mercury willend in the mangrove swamps fringing the coast line.
The mangrove swamps serve as hatching grounds forfish and shellfish the main source of proteins for theFilipinos. Very high concentrations of mercury havebeen found in water which was used for watering
rice paddies.
In this study, we developed determination of mercury
and gold in the crushed rock mines nondestructively
using PGAA and INAA.
Also based on theconcentration of gold and mercury in tailings, wewill optimize conditions of “the state battery
method”. Observed mercury and gold concentrations
in tailings are 2.5 – 393 ppm, 1-3.9 ppm, respectively.
Based on these results, we will optimize theconditions of the state battery method for mercury
clean up project.
1B02: Estimation of anthropogenic influence on
atmosphericenvironment
byanalyzingparticulate matter in snow cover
FUJII, M.1, SHOZUGAWA, K.1, MATSUO, M.1,
TOH, Y.2, MURAKAMI, Y.3, FURUTAKA, K.2,
KIMURA, A.2, OSHIMA, M.2, KOIZUMI, M.2(1Gradate School of Arts and Sciences, The
University of Tokyo, 2Japan Atomic Energy Agency,
3
Fukui University)
Atmospheric aerosols, derived from whether
natural or anthropogenic origin, work as ice nuclei inatmosphere and are captured in snow. They areconserved in snow cover, which shows the state of
atmospheric environment at the time of snowfall.
Therefore, analyzing particulate matter in snow cover,
we can evaluate average atmospheric environment of
one winter season, not that of the moment ofsampling.
We collected snow samples at Hokuriku
Region, Kanto Region and Hokkaido from 2008 to
2010, considering the factor of snowfall, effect ofnorthwest monsoon and existence of local
contaminant. The snow samples were melted atroom temperature and filtered with φ0.22µm
membrane filter to separate particulate matter insnow. Because particulate matter in snow cover has acharacteristic of low concentration and highelemental diversity, we applied multiple prompt
gamma-ray analysis (MPGA) in addition to
instrumental neutron activation analysis (INAA) toelemental analysis. The net weight of particulatematter on the membrane filter is hard to measure, so
we calculated enrichment factor (EF), instead ofconcentration of respective elements, to discuss theresult.
1B03: Bulk chemical analysis of hydrogenous− 171 −

meteoritesbyneutrongamma-ray analysis

inducedpromptIslam, M.A.1, Ebihara, M.1, Matsue, H.2, Kojima, H.3(1Grad. School of Sci. & Eng., Tokyo Metropolitan
Univ., 2Quantum Beam Sci. Directorate, JAEA,
3
National Institute of Polar Research, Tachikawa,Tokyo)
Meteorites are generally heterogeneous in chemicalcomposition. Bulk chemical analysis of meteorites
offers a challenge for representative sampling. In
practice, increasing sample mass introduce neutron
flux perturbation and gamma-ray self attenuation
inside the sample. Moreover, the analyticalsensitivity of the elements changes in the presence ofstrong scatterer like H in the sample. Among therecovered meteorites CI and CM carbonaceouschondrites contain the high abundance of H (up to 2
wt %). In this study, we aimed to determine
element contents in the carbonaceous meteorites byusing neutron induced prompt gamma-ray analysis(PGA). To evaluate analytical sensitivity variation of
the elements with sample mass and H content,
cold-pressed disk (12 mm diameter) samples wereprepared using homogeneous mixture of GSJ basaltic
rock JB-2 and oxalic acid with 2 wt % H. All
samples and standards were irradiated by guided
beam of thermal neutrons at JRR-3M of JAEA. The
analytical sensitivity of the elements remains
constant within the error of counting statistics when adisk mass increases up to 0.5 gm and after that
decreases with increasing of the disk mass. Therefore,in PGA analysis of hydrogenous meteorites (~2 wt%
H) up to 0.5 gm sample, the uncertainty due to theanalytical sensitivity changes can be ignored.
1B04: Simple and high-precision measurement
method of neutron distribution using ink-jet
printer
TAKIMOTO,M.1, TAKAMIYA,K.2, SHIBATA,S.2,
NAKANO.Y.2,
J.H.MOON3,
OKUMURA,R.2,
S.H.KIM3.
(1Grad. School of Engineering, Kyoto Univ.,
2
Research Reactor Institute, Kyoto Univ., 3Korea
Atomic Energy Research Institute)
Neutron flux is an important parameter inneutron activation analysis, radioisotope production
and other neutron irradiation experiments. In the caseof neutron activation analysis, the analyticalaccuracy depends on the estimation of neutron flux at
irradiations. In order to measure neutron flux
accurately, simple and high-precision measurement
method of neutron distribution using an ink-jet
printer has been developed. In this method, neutron
monitors are prepared by applying gold solution on apaper sheet using an ink-jet printer. The prepared
monitor is thin enough to ignore the self-absorption
in neutron irradiation and self-shielding in
gamma-ray measurement, and is also easy to handle.
Measurements of axial neutron distribution at thepositions ofirradiating capsules in neutron
irradiation holes of HANARO, PTS#1 and PTS#3,
were tried using the neutron monitors. As a result, a
trend or fluctuation of neutron fluence cannot be
observed in the case of PTS#1, but there is a positive
trend in PTS#3. This result is consistent with theprevious report of neutron flux measurements using
Au-Al wire monitors. The result of measurements ofneutron distribution using an imaging plate atneutron irradiation facility of KUR will be alsopresented.
1B05: A study on speciation of chromium in soilby X-ray absorption fine structure.
HORI, M., SHOZUGAWA, K., MATSUO, M.
(Grad. School of Arts and Sci., Univ. of Tokyo )Hexavalent chromium (Cr(VI)) is toxic, and
one
of
the
hazardous
materials.
1,5-diphenylcarbazide spectrophotometry is widelyused as determination of Cr(VI) contents inenvironmental samples. However, some problems
are pointed out in this method, namely, there is adifficulty when applying to soil samples. In thisstudy, we applied X-ray absorption fine structure(XAFS) spectroscopy to determination of Cr(VI)contents, that was one of useful means for
nondestructive analysis. In the conventional methods,
the normalization energy of the Cr K-edge in X-ray
absorption near-edge structure (XANES) spectra was
not clearly defined. So, it was difficult to determine
Cr(VI) contents in interstitial water or soil samples
with sufficient accuracy. Therefore, we investigatedto find the best normalization energy in the XANES
spectra.
It was considered that the peak near the whiteline in the spectrum of the standard reference wasdue to d-d transition of Cr (III). The peak observed
near 6010 eV in white line is peculiar to Cr(III),ascribing to the transition of 4A2g→4T2g. By
normalization at this position, we were able to obtain− 172 −

the better calibration curve (R2=0.988).
1P01: Gamma-ray analysis and behavior ofspallation products produced in mercury of theneutron source at J-PARC
Kai, T., Kasugai, Y., Ooi, M., Wakui, T., Kogawa,
H., Haga, K., Hanano, K.
(J-PARC center , Japan Atomic Energy Agency)

Neutrons are produced by spallation reactions
by proton beam (3GeV, 1MW) irradiation on
mercury in the Material and life science experimental
facility at J-PARC. Mercury was designed to bedrained into a shielded tank to reduce the radiationby the spallation products. However it was confirmedthat some spallation products (mainly 188Ir, daughterof 188Pt) adhering to the inner surface increased thedose after the draining. To get more information theauthors sampled mercury (~120 g) and the adhesive
substances (black powder). Then, behaviors of thespallation products in mercury are discussed.
Twelve nuclides, 203Hg, 188Pt, 189Ir, 188Ir, 185Os,
175
Hf, 173Lu, 172Lu, 146Eu, 113Sn, 110mAg, 88Y, wereidentified in the mercury specimen by gamma-ray
spectroscopy. The amounts of radioactivity were in
the range between several to around hundred
percents relative to calculation. Only 110mAg was notfound in the adhesive substances. It is expected that
other elements than mercury take important role tobehavior of the spallation products since the content
ratios of the elements were calculated to be in theorder of ppb, and the elements (tin and europium)
having higher solubility than silver were found inboth specimens. For example, iron, which is
expected to be a dominant impurity (caused byerosion of stainless steel pipes), dose not react withsilver. On the other hand, iron reacts with tin.
1P02: Study on the reversed phase extractive
chromatography in micro-columns for speciationof rutherfordium
TAKEDA,Y.1, ARAKI,M.1, YOKOYAMA,A.2,
HABA,H.3, KIKUNAGA,H.3(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,
2Inst. Sic. Eng., Kanazawa Univ., 3RIKEN)
For the purpose of speciation of rutherfordium,a superheavy element, in solution, we aim to obtainliquidliquid extraction data of Rf by means ofreversed  phase chromatography with stationary

phase containing chelate extractant, TTA. TTA
extracts quadrivalent metal ions preferentially, and,that is, we can obtain a specific complex formation
constant of Rf. In this work, we filled micro columns with stationary phase containing TTA, andmeasured percent adsorption of Zr and Hf,
homologues of Rf, in the tracer scale as a function of[F ].This results coincide with macro  scale
experiments in the following respects. Adsorption
values decrease with increase of [F ] and good
separation between Hf and Zr is expected around [F]eq=6.010-5 M. Therefore, the percent adsorption
measurement with the microcolumns is considered
to be applied for the Rf experiment.
1P03: Study on the adsorption rate of Zr and Hf
as homologues of element 104, Rutherfordium, on
cation-exchange resin in H2SO4 solutions .
IKARASHI, S.1, SUEKI, K.1, TSUKADA, K.2,
NAGAME, Y.2(1Pure & Appl. Sci., Univ. Tsukuba, 2Advanced Sci.
Res. Center., JAEA)
It was reported that the cation-exchange
chromatographic behavior of Zr and Hf ashomologues of element 104, Rf, in H2SO4 solutions
was not consistent with the distribution coefficientsobtained in the batch experiment. In the present
study, the adsorption rates of Zr and Hf on the
cation-exchange resin in H2SO4 solutions were
investigated in order to lead to the quantitative
discussion of the chromatography. It was obtained
the adsorption rates of 88Zr and 175Hf on the
cation-exchange resin (MCI GEL CK08Y, H+ form)
in 0.1 M H2SO4 at 15, 25 and 45 as functions of
the shaking times. The results showed that theequilibrium of cation-exchange was reached at 70-80
seconds and that the adsorption rates on the
cation-exchange resin were not changed between 1545 in the present condition. In H2SO4/HNO3
mixed solution ([H+]eq=1.0 M), the adsorption rate
was similar to those of 88Zr and 175Hf on the
cation-exchange resin in H2SO4 solution.
1P04: Development and evaluation of a liquid
scintillation detector for aqueous chemistry ofsuperheavy elements
KOMORI, Y.1, OOE, K. 1, KURIYAMA, A. 1,
TAKAYAMA, R. 1, KIKUTANI, Y. 1, KIKUNAGA,
H. 2, KASAMATSU, Y. 1, YOSHIMURA, T. 1,− 173 −TAKAHASHI, N. 1, SHINOHARA, A. 1
(1Grad. School of Sci., Osaka Univ., 2Nishina Center,
RIKEN)We are planning to develop an on-line liquid
scintillation detection system coupled to an
ion-exchange column or a liquid-liquid extraction
apparatus for aqueous chemistry of superheavy
elements. In this work, we have developed a liquid
scintillation detector with α/β discrimination for
on-linemeasurements
andevaluated
its
performances. From the results, it has been foundthat the detector has a counting efficiency ofapproximately 96% for 241Am and a FWHM ofapproximately 310 keV for the 4784 keV α-energy of226
Ra at the sample volume of 1 mL. The energy
resolution became worse with increasing the amountof the sample solution in the detector cell. Next, testof the on-line measurement with the developed
detector was performed. Aqueous solution including241
Am and 152Eu was introduced into the detector cell
together with an emulsifier scintillator and mixed byan electromagnetic stirrer under the detection
chamber and stirring bar in the glass cell. After well
mixing, α-particle detection with a goodenergy-resolution and a discrimination between αand β-events have been achieved.
1P05: Anion-exchange behavior of the group-6
elements in HF/HNO3 mixed solutions - Towards
the study of ion-exchange behavior of 106Sg –LIANG, X. 1,2, LI, Z., TSUKADA, K. 1,
TOYOSHIMA, A. 1, ASAI, M. 1, SATO, T.K. 1,
SATO, N. 1, KIKUCHI, T. 1,3, KANEYA, Y. 1,3,
NAGAME, Y.1(1CIAE, China, 2ASRC, JAEA, 3Ibaraki Univ.)
Anion-exchange behavior of the group-6
elements, W and Mo, in HF and HNO3 mixed
solutions has been studied by a batch method using
the carrier-free radiotracers 181W (T1/2 = 121.2 d) and93m
Mo (T1/2 = 6.9 h). The long-lived isotope 181W was
produced in the 181Ta(p, n) reaction at the JAEA
tandem accelerator. The 181W isotope was chemicallyseparated from the Ta target material, and was
dissolved with 10-4 – 1.0 M HF and 0.1 M HNO3
mixed solutions for batch experiments. On the other
hand, the short-lived isotope 93mMo was produced in
the 93Nb(p, n) reaction. The recoiling products fromthe Nb target were transported to a chemicallaboratory with a He/KF gas-jet system, and weredissolved with HF and HNO3 mixed solution. The
solutions containing 181W or 93m Mo were mixed with
5 – 200 mg anion exchange resin CA08Y.
Radioactivities of the solution were assayed for γ-ray
spectrometry, and then distribution coefficients (Kds)of these elements were determined. It was found that
the Kd values of W depend strongly on theconcentration of HF, while those of Mo are almost
constant as a function of [HF] under the given
conditions.
1P06: Measurement of excitation function ofLu(p,xn)175Hf

nat

KIKUTANI, Y.1, OOE, K.1, KOMORI, Y.1,
FUJISAWA, H.1, KURIYAMA, A.1, TAKAYAMA,
R.1, KIKUNAGA, H.2, KASAMATSU, Y.1,
TAKAHASHI,
N.1,
YOSHIMURA,
T.1,
1
SHINOHARA, A.
(1Grad. School of Sci., Osaka Univ., 2Nishina
Center, RIKEN)
We are planning to study the solvent extraction
behavior of element 104, rutherfordium (Rf) and thelighter homologues of Rf, zirconium (Zr) andhafnium (Hf). The 88Zr (T1/2 = 83.9 d) and 175Hf (T1/2= 70.0 d) nuclides are needed for the solvent
extraction experiments of Zr and Hf. However, there
is no data of the excitation function ofnatLu(p,xn)175Hf reaction and the data is required for
efficient production of 175Hf. In this work, theexcitation function of natLu(p,xn)175Hf reaction atenergies up to 14 MeV has been measured for the
first time. Activation method and stacked foil
technique were used to measure cross section of thenatLu(p,xn)175Hf reaction. The target stacks consistingof lutetium, iron and cupper foils were irradiated by a
14 MeV proton beam from the AVF cyclotron at
Research Center for Nuclear Physics (RCNP), Osaka
University. Gamma-rays of the radionuclides
produced in these samples were measured with agermanium semiconductor detector. As a result, theobtained excitation function of the natLu(p,xn)175Hf
reaction shows the maximum value of 140 mb at the
proton energy of about 10.3 MeV.
1P07: Measurement of Pa-231 photofission
cross-section by the fission track method ( )1

NISHIKAWA, M., 2OHTUKI, T., 2HIROSE, K.,
SATO, W., 3YOKOYAMA, A., 3NAKANISHI, T.
( 1Grad. School Nat. Sci. Tech., Kanazawa Univ.,3− 174 −

2
3

Res. Center for Electron Photon Sci., Tohoku Univ.,
Inst. Sci. Eng., Kanazawa Univ. )Fission track method has been applied to thedetection of photofission events of 231Pa. For thedetection of fission fragments, quartz and muscovite
were used as solid state track detectors. The target
nuclide 231Pa was sandwiched between pieces ofquartz and muscovite for irradiation withbremsstrahlug at a Linac facility of Tohoku Univ.
together with the natural uranium (natU) and 232Th
targets used as references. After the irradiation, thedetectors were subjected to chemical etching andobserved for track counting using a microscope inorder to evaluate the photofission cross-section of231
Pa. At 20 MeV of the maximum bremsstrahlung
energy, in our previous work, the fission
probabilities of 231Pa relative to natU and 232Th were
determined to be around 2 and around 6, respectively,
before. In the present study, the photofission
probability of 231Pa to that of natU was determined to
be around 2 at 18 MeV of the relevant energy. This
result might exhibit a saturation behavior even down
to the energy.
1P08: Development of a surface ionizer coupled toa gas-jet transport system for the measurement of
the first ionization potential of Lr
SATO, N.1, ASAI, M.1, TSUKADA, K.1, SATO,
T.1, TOYOSHIMA, A.1, LI, Z. J.1, KIKUCHI,
T.1,2, KANEYA, Y.1,2, ICHIKAWA, S.3,
NAGAME, Y.1, SCHÄDEL, M.1(1ASRC, JAEA, 2Ibaraki Univ., 3Nishina Center,
RIKEN)
It is important to determine the first ionization
potentials (IPs) of the heaviest elements with atomic
number Z > 100 to understand their valence
electronic structure affected by relativistic effects.
Due to low production rates and short half-lives of
the heaviest nuclides, IPs of these elements have notbeen so far determined. We are developing asurface-ionization-type ion source coupled to agas-jet transport system in the Isotope Separator
On-Line (ISOL) at the JAEA tandem accelerator
facility to measure IP of the heaviest actinide,
lawrencium (Lr, Z = 103). In the symposium, wereport the present status of the development of theapparatus. Production yields of 256Lr (half-life = 27 s)that is used for the IP measurement, in the249,250,251
Cf(11B, xn), 243Am(18O, 5n) and 248Cm(14N,6n) reactions will be also presented.
1P09: Development of Si-CdTe detector array for
Nuclear spectroscopy of superheavy nuclides
TAKEYAMA, M. 1, KAJI, D. 2, MORIMOTO, K. 2,
TOKANAI, F. 1
(1Yamagata Univ, 2Nishina Center, RIKEN)
Nuclear spectroscopy for understanding of
nuclear structure is one of the hot topic in nuclear
physic on the superheavy nuclides. Now, we arepreparing the start-up of the nuclear spectroscopic
study at the focal plane of GARIS or GARIS-II in
RIKEN.
We pay attention to the CdTe detector as
γ(X)-ray detector instead of the Ge detector.
The CdTe detector has strong points like ashigh absorption due to its high atomic number andhigh density, high energy resolution with low leakcurrent due to wide band gap energy even at room
temperature, and low cost to get the detector. Then,
we developed a prototype of a new Si-CdTe detector
array for alpha(e)-gamma spectroscopy ofsuperheavy nuclides. Basic characteristics, such asenergy resolution, time resolution, and backgroundcondition, of the Si-CdTe detector array wasinvestigated by standard source of 241Am and 3 mix
source including 241Am, 244Cm, and 237Np.
1P10: Gamma-ray analysis and behavior ofspallation products produced in mercury of theneutron source at J-PARC
Kai, T., Kasugai, Y., Ooi, M., Wakui, T.,
Kogawa, H., Haga, K., Hanano, K.
(J-PARC center , Japan Atomic Energy Agency)
Neutrons are produced by spallation reactions
by proton beam (3GeV, 1MW) irradiation on
mercury in the Material and life science experimental
facility at J-PARC. Mercury was designed to bedrained into a shielded tank to reduce the radiationby the spallation products. However it was confirmedthat some spallation products (mainly 188Ir, daughterof 188Pt) adhering to the inner surface increased thedose after the draining. To get more information theauthors sampled mercury (~120 g) and the adhesive
substances (black powder). Then, behaviors of thespallation products in mercury are discussed.
Twelve nuclides, 203Hg, 188Pt, 189Ir, 188Ir, 185Os,
175
Hf, 173Lu, 172Lu, 146Eu, 113Sn, 110mAg, 88Y, were

− 175 −

identified in the mercury specimen by gamma-ray
spectroscopy. The amounts of radioactivity were in
the range between several to around hundred
percents relative to calculation. Only 110mAg was notfound in the adhesive substances. It is expected that
other elements than mercury take important role tobehavior of the spallation products since the content
ratios of the elements were calculated to be in theorder of ppb, and the elements (tin and europium)
having higher solubility than silver were found inboth specimens. For example, iron, which is
expected to be a dominant impurity (caused byerosion of stainless steel pipes), dose not react withsilver. On the other hand, iron reacts with tin.
1P11: GARIS-II commissioning #1
KAJI, D. 1, HABA, H. 1, KASAMATSU, Y. 1,
KUDOU, Y. 1, MORIMOTO, K. 1, MORITA, K. 1,
OZEKI, K. 1, SUMITA, T. 1, YONEDA, A. 1, SATO,
N. 2, WAKABAYASHI, Y. 2, MURAKAMI, M. 3,
TOKANAI, F. 4, NAMAI, S. 4
(1Nishina Center, RIKEN, 2Advanced Science
Research Center, JAEA, 3Niigata Univ, 4Yamagata
Univ)
We developed a new gas-filled recoil ion
separator GARIS-II for actinide-based asymmetricfusion (hot fusion) study. The 1st operation of
GARIS-II was performed by using standard 241Am
source and 0 degree recoil atom of 208Pb target
produced by Rutherford scattering. The GARIS-II
consists of five magnets arranged in a Qv-D-Qh-Qv-D
configuration. This configuration is the first designfor the purpose of SHE study. At first, balance ofmagnet field strength was tuning for each magnet bystandard 241Am source with the activity of 21 kBq. A
solid angle of GARIS-II was measured to be about
18.4 msr. This value almost reproduced an evaluatedvalue by the computer code TRANSPORT. The solid
angle is increased from 12.2 to 18.4 msr,
approximately 1.5 times higher than GARIS.
The 2nd step of GARIS-II operation was investigatedby 0 degree recoil atom of 208Pb target produced by
Rutherford scattering. Image size at focal plane of
GARIS-II was investigated by changing the He
gas-pressure in GARIS-II chamber.
1P12: Development of data acquisition system forshort-time decay by using Flash ADC
MORIMOTO, K.1, KAJI, D.1, BABA, H.1,

TOKANAI, F.2( 1Nishina Center, RIKEN, 2Yamagata Univ.)
A data acquisition (DAQ) system has been
upgraded for super heavy element research
performed using the Gas-filled Recoil Ion Separator(GARIS).
Super heavy elements studied by using GARIS
and GARIS-II, especially in the heaviest region on
the nuclear chart, may have a very short life. The
original GARIS readout electronics cannot separate
sequential decays that occur at intervals shorter than
5 s because of the pileup in the shaping amplifier.
We modified the original readout system by using
Flash ADC so that it can be used to detect shorter
decay intervals.
The system was used in experiments to search
for a new isotope 234Bk in the reaction
197
Au(40Ar,3n). A total of 119 decay chains wereobserved; all the decay chains were assigned tosubsequent decays from 234Bk. 218Ra and 214Rn,
which have very short life times (15.6 s and 0.27
s, respectively) were contained in the decay chains.
Sequential fast decay of these isotopes was clearlyobserved in the digitized preamplifier signal.
In this presentation, the modified DAQ system
in detail as well as the observed data in theexperiment search for the 234Bk will be described.
1P13: Development of New Time of Flight
Detector with a Large Diameter for Experimentof the Search for Superheavy Elements.
MAYAMA, K.1, MORIMOTO, K.2, KAJI, D.2,
TOKANAI, F.1(1Grad. School of Sci., Yamagata Univ., 2Nishina
Center, RIKEN)
A new time-of-flight (TOF) detector with alarge effective area was developed for actinide-based
asymmetric fusion (hot fusion) study by gas-filled
recoil ion separators of GARIS and GARIS-II.
A system of time-of-flight (TOF) detectors anda position sensitive silicon detector (PSD) array areimportant roles for particle identification in fusion
study. Especially, the TOF detectors are used for two
purposes. One is to measure the time-of-flight of theparticles coming into the PSD array to get the
information of the mass number of recoil atom. The
other is to distinguish decay signals in PSD arrayused in anti-coincidence mode.
In the case of hot fusion study, the image size

− 176 −

in the focal plane of the separator becomes wide
spread, because of multiple scattering of the recoil
ion by the filling gas atoms. Therefore, we developed
a new TOF detector with very large effective area of
120 mm in a diameter. As a first step of fundamental
operation, a uniformity of detection efficacy wasinvestigated by alpha particles from 241Am standard
source.
1P14: Development of an ionization chamber for
nuclide identification of the superheavy elements
SUMITA, T.1,2, OZEKI, K.2, MORIMOTO, K.2,
KAJI, D.2, HABA, H.2, KASAMATSU, Y.3,
KUDOU, Y.2, YONEDA, A.2, MORITA, K.2,
CHIBA, J.1(1Tokyo Univ. of Science., 2Nishina Center, RIKEN,
3Osaka Univ.)
In the superheavy element region, the direct
measurements of atomic number Z and mass number
A of produced nucleus is one of the most challenging
tasks. In the region of large Z, the density ofelectron-hole pairs is too high in using silicondetectors in the search experiments. As a result, it isthought that the precise measurement of the kinetic
energy is not possible.
In this work, we operated ionization chamberwith low pressure for reducing the density ofionization electrons and developed it for the purposeof precise measuring of the kinetic energy. We usedalpha particles from an 241Am source and performed
performance evaluations so far. This time, we
performed it with the 11B beam at the tandem
electrostatic accelerator in RIKEN.
We have measured the pulse height in eachelectrode while changing pressure. As a present
result, measured values didn’t accord with the valuesof the energy loss from calculation. It is thought that
this because of the particle and the energy
dependence of W-value. And the energy resolution
was 2.13% in 4109.0 keV. We estimated standard
deviations of mass for A=300 using this value andtime resolution of Time-Of-Flight detector in the
search experiments.
1P15: Study of Reactivity for Lanthanide
Metallofullerenes Using Radiochemical Method
AKIYAMA, K., FURUKAWA, H., TAKEUCHI,
E., HAMANO, T., KUBUKI, S.
(Grad. School of Sci. and Eng., Tokyo Metropolitan

Univ.)
Metallofullerenes are potential material for theconstruction of the drag deriver system which takes
radioisotopes to the targeted organs. Our motivation
is to synthesize the hydrophilic metallofullerene
derivatives for the medical and pharmaceuticalapplications. In this session, we will report thesynthesis and reactivity of metallofulleropyrrolidinesfor La, Ce, Pr, Nd, and Gd metallofullerenes.
Metallofullerenes samples were irradiatedthermal neutrons in the JRR-3M research reactor of
JAEA. These irradiated samples were refluxed inwell dehydrated toluene with paraformaldehyde andN-methylglycine. After removal of residual reactant
by distilled water, resulting solutions werecondensed and injected into an HPLC column of
Buckyprep. Eluate from the column was collected
and detected their gamma-ray by Ge semiconductor
detector.
Comparing HPLC chromatogram of “before
reflux” with that of “after reflux”, it was found thatthe intensity of the elution peak derived from
La@C82 was decreased and that new peaks which
derived from La@C82 derivatives were observed
around 27 min and 55 min. Based on this result,
HPLC elution peaks derived from metallofullerene
derivatives of Ce, Pr, Nd, and Gd were also collected
and detected their activity. As the results, we could
not find significant differences in the reactivity
between these metallofullerenes.
1P16: Separation of Metallofullerenes
hollow species using Lewis acid.

from

HAMANO, T., TAKEUCHI, E., AKIYAMA, K.,
KUBUKI, S.
(Tokyo Metropolitan University)
Stevenson et al. reported that metallic nitride
endohedral fullerenes and oxometallic fullerenes
were separated from hollow species by using Lewis
acids such as AlCl3 or FeCl3. In this study, we
confirmed that this method could be applicable forthe separation of metallofullerenes encapsulating
lanthanide elements from hollow fullerenes. The
extraction ratio of metallofullerenes was investigatedas a function of weight of added AlCl3 and reaction
time. Weight of AlCl3 was varied from 5.1mg to106.5mg with 30min reaction time. Reaction time
was also varied between 5min to 3h with 15mg of
AlCl3. As a result, extraction ratio of− 177 −

metallofullerene was reached to be about 50% in thecase of more than 25mg of AlCl3 being added and of
more than 30min of reaction time. The most ofresidual metallofullerene which could not berecovered is expected to be a insoluble substancesuch as polymerized metallofullerene. In conclusion,
it is found that at least 50% of metallofullerenes werecollected even if added excess quantity of AlCl3 or
took plenty of reaction time.
1P17: Recovery of molybdenum by using
pyridine resin from simulant irradiated nuclear
fuel solution
SUZUKI, T.1, IKEDA, Y.1, HONDA, M.2,
ASANUMA, N.2, OSAKA, M.3(1Res. Lab. Nucl. Reactors, Tokyo Tech, 2Faculty ofEng. Tokai Univ., 3Oarai Res. & Dev. Center,
JAEA.)
There are many amounts of molybdenum innuclear fuels irradiated in nuclear reactors. If
molybdenum is immediately recovered after
irradiation, we can obtain molybdenum-99.
Molybdenum-99 is well-known as mother isotope oftechnetium-99m. Since the life time ofmolybdenum-99 is not so long, if we waiting several
years after irradiation, the molybdenum without theradioactive isotope can be obtained. We have been
studying the molybdenum recovery by using pyridine
resin. First, the distribution coefficients ofmolybdenum and zirconium, which is known foraccompanying elements with molybdenum, were
evaluated in nitric acid solution and in hydrochloric
acid solution. Second, the separation experiment ofmolybdenum and zirconium was investigated bychromatography. From result obtained by theirinvestigation, we confirmed that the molybdenum
can be recovered using hydrochloric acid system.
Finally, we confirmed the recovery of molybdenum
from simulant irradiated nuclear fuel solution bychromatography using pyridine resin in hydrochloric
acid solution.
1P18: Synthesis and properties of hexatechnetium
cluster complexes with mixed cap ligands ofsulfide and chloride
OMOTE, T.1, YOSHIMURA, T.1, TAKAYAMA,
T.2, SEKINE, T.3, SHINOHARA, A.1(1Grad. School of Sci., Osaka Univ., 2 Daido Inst. of
Tech., 3 CAHE, Tohoku Univ.)

The octahedral hexanuclear cluster complexes
having 24 valence electrons are known to showinteresting photophysical and redox properties. In the
recentstudy
conducted
byus,
severalchalcohalide-cappedhexatechnetium(III)andhexarhenium(III) cluster complexes were synthesized
and investigated about their chemical properties. In
the present study, the new hexatechnetium(III)cluster complexes, (PPh4)3[Tc6(µ3-S7Cl)Cl6] and(PPh4)3[Tc6(µ3-S6Cl2)Cl6] were synthesized and thephysical properties were investigated. The complex
was produced by the high temperature reaction ofelemental 99Tc, S, and K2[TcCl6] with excess amountof KCl at 850. The reaction mixture was separated
by column chromatography. Two different kinds ofbrown crystals, (PPh4)2[Tc6(µ3-S6Cl2)Cl6] andwereobtained.
In(PPh4)3[Tc6(µ3-S7Cl)Cl6]
acetonitrile solution, their UV-Vis spectra show thebroad absorption bands of the cluster core with thoseof (PPh4)+. In addition, it was found that the
spectrum of (PPh4)3[Tc6(µ3-S7Cl)Cl6] shifts tolong-wavelengthcompared
with
that
of
(Bu4N)3[Re6(µ3-S7Cl)Cl6].
1P19: Production of no-carrier-added 177Lu forradioimmunotherapy
HASHIMOTO, K., WATANABE, Sa., ISHIOKA, S.
N.
(Japan Atomic Energy Agency)
Lutetium-177 is considered to have potential
for application in radioimmunotherapy, because it
has favorable physical characteristics. We havesucceeded in the production of high purity
no-carrier-added (nca) 177Lu of capable of labelingantibodies using reversed-phase ion-pair liquid
chromatography. However, in this separation, nca
177
Lu could not be completely separated from morethan 3 mg of Yb2O3 target. For this reason, theradioactivity of nca 177Lu produced by our separation
method is limited less than GBq. Therefore, for therealization of the large scale production, we
considered the adoption of a coarse separation
between Lu and Yb by using LnResin column before
reversed-phase ion-pair liquid chromatography. In
this study, the maximum weight of Yb2O3 capable ofthe separation between Lu and Yb by using LnResincolumn chromatography followed by reversed-phaseion-pair liquid chromatography was investigated. It
was found that in less than 10 mg of Yb2O3 targets− 178 −

loaded on the LnResin column, the weight of Yb2O3
in the 177Lu fraction was less than 2 mg. Therefore
about 10 mg of Yb2O3 target was considered to be
maximum weight of Yb2O3 capable of the separation
between Lu and Yb by using LnResin column
followed by reversed-phase ion-pair liquid
chromatography.
1P20: Flux correction for photon Activation
Analysis
OURA, Y., EBIHARA, M.
(Grad. School of Sci. and Engi., Tokyo Metropolitan
Univ.)
In
photonactivation
analysisusingbremsstrahlung from an electron LINAC, samples tobe irradiated are stacked along an electron beam.
Since photon flux comes down towards downstream
samples, photon flux in each sample should becorrected to obtain an accurate determination value.
We usually use Au foils for the flux correction, using
197
Au(γ, n)196Au reaction. In this study we comparedsome metal foil monitors with Au monitor to get
effectual correction way. Quartz filter samples withseveral kinds of monitors were irradiated bybremsstrahlung with 25 MeV of end point energy for
20 minutes. Decreasing rate of radioactivity inmonitors was different from each induced
radionuclides, and the rate was found to be correlatedwith Q value of a reaction producing radionuclide:the rate of decreasing became significant withdecrease of absolute Q value. In the case of 420
minutes of irradiation time, the same systematic wasalso observed, but the difference of decreasing rate
among monitors were smaller than the irradiation for
20 minutes. Appropriate monitor should be selected
to obtain an accurate determination value.
1P21: Determination of trace amount of nickel byphoton activation analysis
SEKIMOTO, S. 1, HIROSE, K. 2, TAKIMOTO, M. 3,
OHTSUKI, T. 2, SHIBATA, S. 1
(1KURRI, 2Research Center for Electron Photon
Science, Tohoku Univ., 3Graduate School ofEngineering, Kyoto Univ.)
Trace amount of nickel in high-purity metal
samples was determined by Photon Activation
analysis (PAA). It was confirmed that PAA wasable to determine about 0.015 μg of nickel in thehigh-purity iron oxide sample within uncertainty of
20 % and that PAA used in this work made it
possible to determine 1% of Ni at least in a few μg ofmagnetic spherules.
Photon activation analysis was carried out
using the Electron Linear Accelerator at the ResearchCenter for Electron Photon Science, Tohoku
University. Samples, reference standards and gold
foils as the fluence rate monitor of photons wereenclosed in a quartz tube for irradiation withbremsstrahlung photons.
The accelerator was
operated at electron energy of 30 MeV with a meancurrent of around 0.11 mA for 8-10 hours. The
quartz tube was placed just after a platinum converterand cooled with running tap water.
Then, applying PAA to the determination of
trace amount of nickel in cosmic spherules, nickel
was able to be determined by PAA more accurately
than by instrumental neutron activation analysis
which has so far been applied to analysis of spherule
samples.
1P22: Hydrotreating of Kuwait Atmospheric
Residue - Structural analysis of Nickel and
Vanadium by XAFS Spectroscopy
KAWASAKI, N.1, KAWAMURA, H.1, OKAMURA,
M.1, HIRAYAMA, S.2, OFUCHI, H.2, HONMA, T.2,
MOCHIDA, I.3(1Kyushu Environmental Evaluation Association, 2
JASRI/SPring-8, 3 Kyushu University)
Nickel and vanadium are the most abundant trace
metals in petroleum. Typically, metal-containing
compounds are high boiling and entrained in the
distillation
bottoms(residuum)ofcrude.
Additionally, metal complexes concentrate them in
the asphaltene fraction of the residuum. To convert
from residuum to clean fuels with higher
value-added, it is necessary that included these
metals remove from the residuum and apply
residuum to Hydrodesulfurization (HDS). However,
the metals (nickel and vanadium) that could not be
removed are causes of disturbing the catalytic
function used with HDS.
The objective of this study is that the local
structures of Ni and V in Kuwait asphaltene, thefollowing HDS catalyst are measured by XAFS
spectroscopy. In the result, nickel and vanadium aresuggested that similar with porphyrin-V andporphyrin-Ni in asphaltene, distinct from chemical
state in catalyst.

− 179 −

41

1P23: Development of Ca-AMS at University ofTsukuba
KINOSHITA, N.1, MATSUMURA, M.1, SASA,
K.1, TAKAHASHI, T.1, SUEKI, K.2, OURA, Y.3(1Tandem Accel. Complex, Univ. of Tsukuba, 2Grad.
School of Pure and Applied Sci, Univ. of Tsukuba,
3
Grad. School of Sci. Eng., Tokyo Metropolitan
Univ.)
Accelerator mass spectrometry (AMS) is anuseful tool for low level measurement of long life
radioisotopes. In the AMS, high terminal voltage isrequired for a sufficient isobaric separation withincrease of atomic number. AMS of calcium-41 is
not carried out in Japan and has a potential in dating
and medical science. 41Ca-AMS using the 12 UD
peletron tandem accelerator at University of Tsukuba
is appropriate measurement for the background. We
have been developing 41Ca-AMS system.
Commercial reagents of CaF2 and CaH2 weremixed with some materials used for a pilot beam
which controls terminal voltage of the accelerator.
From mixed sample of CaF2 and ZnO, 14 nA of40
Ca19F3 and 23 nA of 66Zn16O2 (pilot beam of40
Ca19F3 ) were extracted. Besides, from sample of
CaH2 and MgO, 4 nA of 40CaH and 2 nA of 26Mg16O(pilot beam of 40CaH2 ) were extracted. On the other
hand, from sample of CaH2 which was irradiatedusing neutron and LiCl, 0.5 nA of 40CaH3 wasextracted, and 147 counts of 41Ca were detected in 15
minutes using a ΔE-E counter. The 41Ca/40Ca atom
ratio was estimated to be 3.1×10 8 from the beam
current of 40CaH3 and count rate of 41Ca.
−

−

−

−

neutron activation analysis (INAA). We determinedthe concentrations of Mg, Al, Sc, Ti, V, Cr, Mn, Fe,
Co, Zn, Cs and Ta in 30 samples of eye-shadow.
The concentrations of Al, Cs and Sc wereconstant within 30% in relative error. It suggests thatthese elements are included in major components.
There were correlation between the concentrations ofFe, Mn and Co which were more rich in dark brownor black samples than white or whitish samples. Alldata of the concentration of Zn were able to be
divided into two groups, below 50 ppm and several
thousand ppm. Zinc values were different between
packages made by respective producer. One sample
in viridian color shows extremely high Cr
concentration of about 1% which is 1000 times
higher than that of the other samples. A chromium
pigment might be included in this sample.
1P25: Improvements in precision of measurementof carbon isotope ratio with accelerator mass
spectrometry
Saito-Kokubu, Y. 1, Nishizawa, A. 2, Suzuki, M.
2, Ohwaki, Y. 2, Nishio, T. 2, Matsubara, A. 1,
Ishimaru, T1.
(1 Geological Isolation Research and Development
Directorate, JAEA, 2 Pesco Corp., Ltd.)

−

−

−

−

−

1P24: Determination of metallic elements in eye
cosmetics by instrumental neutron activation
analysis
MINOWA, H.1, FURUTA, E.2, OKADA, Y.3(1Jikei Univ. School of Medicine, 2Ochanomizu
Univ., 3Tokyo City Univ.)

There are a lot of cheap cosmetics in themarket, meanwhile these adverse effect on health isfrequently
overlooked.
Colorful
cosmetics
particularly for eye makeup often have toxic
heavy-metal elements as pigments. In this work, forthe purpose of the determination of metallic elements
in cosmetics and the estimation of toxicity of them,the eye cosmetics were analyzed by instrumental

In order to obtain a stable ion beam formeasurement of precise isotope ratio of carbon byaccelerator mass spectrometry, three improvements
to JAEA-AMS-TONO were performed.
1. A cesium-beam sputter source is used to
produce the ion beam of carbon. Cesium vapor isprovided from a reservoir to the ion source. As
their distance is long, a heater on a feed pipe wasinstalled to prevent the vapor from condensing.
2. Charge stripping is performed by passing theion beams through an electron stripping gas at aterminal in an accelerator. The efficiency of thecharge stripping depends on pressure of the stripping
gas which is affected by peripheral temperatures. A
flow control valve of the stripper gas was wrapped inglass wool and aluminum foil as heat insulators tostabilize the pressure.
3. Beam line geometry from the exit of anaccelerator tank to detectors was optimized byadjusting the position of the beam guide tubes.
Standard samples of NIST 4990c were measured.
Relative standard deviations of 14C/12C ratios in 12
reputable measurements of 1 sample before and after
the improvements were about 2% and 0.5%,− 180 −

respectively. Therefore the improvements enhanced
stability of the ion beam.
1P26: Observation of local fields in zinc oxidewith the 111Cd probe
KOMATSUDA, S.1, SATO, W.2, OHKUBO, Y.3(1Grad. School Nat. Sci. Tech. Kanazawa Univ., 2Inst.
Sci. Eng., Kanazawa Univ., 3Res.Reactor Inst.,
Kyoto Univ.)
Zinc Oxide (ZnO) is strongly expected as asemiconductor in a wide field of industries. The
conductivity of semiconductors varies depending on
the doping methods and the density of impurities. To
control the conductivity of semiconductors, it isimportant to understand the functions of impurities in
ZnO at an atomic scale. In our previous study, local
fields in polycrystalline ZnO doped with 0.5 at.%indium (In) were measured by means of thetime-differential perturbed angular correlation(TDPAC) method with the 111Cd (←111In) probe,
resulting in the detection of unexpected
conduction-electron behavior at the probe sites. We
infer that this phenomenon was caused by so-called“aftereffect’’ typically accompanying the electron
capture decay of 111In. In this work, we measured
local fields in polycrystalline ZnO with the 111Cd(←111mCd) probe in order to investigate if theoscillatory structures of spectra are damped in thesame way as the case for the 111Cd (←111In) probe.
When introducing the 111Cd (←111mCd) probe, aneutron capture product of 110CdO, in the samples; itis essential to examine optimum condition foruniform diffusion of the probe. We therefore tried tosynthesize samples at various annealing temperaturesand chemical constituents. In this paper, showing
parameter values such as the electric fields gradients,
we discuss the aftereffect with respect to temperaturedependence of spectral damping.
1P27: Synthesis and magnetic properties in Fe
ferromagnetic
andMn
co-doped
SnO2
semiconductors
OKABAYASHI, J.1, NOMURA, K.1, KONO, S.2,
YAMADA, Y.2(1The University of Tokyo, 2Tokyo University of
Science)
Ferromagnetic nanoparticles of diluted
transition metal of both Fe and Mn co-doped into

SnO2 were synthesized by a sol-gel method. Fe andMn co-doped SnO2 enhanced the magnetization,
which
showedthemaximumsaturation
magnetization value at 0.5% Mn and 1% Fe
co-doping. With further increasing the amounts of
Mn doping into 1% Fe-doped SnO2 host, themagnetic-field dependence of magnetization showed
the decrease in saturation magnetization. We foundthat the coexistence of Fe and Mn ions contributes tothe increase of the magnetization. Secondary phaseformation is excluded from the concentration
dependences of magnetization and Mossbauer
spectra. Broad magnetic relaxation peaks in
Mossbauer spectra are related to the enhancement of
the saturation magnetization. In the presentation, we
discuss the co-doping effects into SnO2 for theroom-temperature ferromagnetism.
1P28: Temperature dependence of In-beam
Mössbauer spectra of 57Mn implanted intoalminuum oxide
NAGATOMO, T.1, KOBAYASHI, Y. 2, KUBO,
M.K. 1, YAMADA, Y. 3, MIHARA, M. 4, SATO,
W. 5, MIYAZAKI, J. 6, SATO, S. 7, KITAGAWA,
A. 7(1International Christian Univ., 2RIKEN Advanced
Meson Sci. Lab., 3Tokyo Univ. of Science,4
Osaka Univ., 4Kanazawa Univ., 6Nihon Univ.,
7
National Institute of Radiological Sciences)
Aluminum oxide (Al2O3) has been extensively
investigated in materials science since its opticalproperty is controllable by the nature and amount of
impurities. In spite of the long history of studies,
there still remain unresolved problems of the color
changes arising from the presence of impurities.
The objective of this work is thus to investigate theinteracting nature of Fe ions implanted as impurities
with the Al2O3 matrix by in-beam Mössbauer
spectroscopy with the 57Fe(57Mn) probe. Here, wehave measured the emission Mössbauer spectra of57
Mn implanted into Al2O3 of which temperature wascontrolled. The 57Mn ions were produced as the
projectile fragments of the high-energy 58Fe beam.
The sample was an Al2O3 single crystal plate (27 mm
x 27 mm and 5 mm thickness). The emission
Mössbauer spectra of 57Mn implanted into Al2O3
were obtained at the temperature range from 92 K toroomtemperature.
Detailsoftemperaturedependence of obtained Mössbauer spectra will be
discussed.

− 181 −

1P29: Mössbauer absorption anomaly of gamma
radiation via nuclear level anticrossing
Nakajo, S1., Horinouchi, S2., Suzuki, H2., Nagata, K1.,
Nakagami, K1., Muramatsu, H2.
(1Grad. School of Edu., Shinshu Univ., 2Fac of Edu.,
Shinshu Univ.)
We have already reported a proof-of-principle
experiment,
demonstrating
electromagneticallyinduced transparency (EIT) with gamma radiation for
the Mössbauer effect using the level-crossing
technique. In the extensive studies so far, we foundthat the new eigenstates might be observed.
We synthesized a single crystal of FePSe3 bysolid phase reaction in the vacuum-shielded tube
(Vycol glass tube) including the mixture of
stoichiometric amounts of Fe, P, Se at 840 forabout 1 month. A powder sample of FePSe3 wasmade by grinding the crystal.
From the analyses of a series of Mössbauer
spectra taken at various temperatures, we determinethat at 20K the states |I=3/2, m=-3/2and |I=3/2,
m=1/2cross and are mixed.
In the Mössbauer spectrum taken with thepowder sample, the absorption line that corresponds
to mg=1/2 me=1/2 transition was observed to be
not a singlet but a doublet. So we conclusively
considered that when two nuclear levels cross andare mixed, two newly generated eigenstates repellingeach other could be observed experimentally under acertain situation.
1P30: Mössbauer spectroscopy
synthesized kimzeyites.
1

2

of

thermal3

KAWASE, M. , YAMAKAWA, J. , KAMIJYO, R. ,SAITO, T.4(1Fac. Biosci., Nagahama Inst. Biosci. technol, 2Fac.
Sci., Okayama Univ., 3Grad. Sci., Osaka Univ.,
4Radioisotope Res. Center, Osaka Univ.)
Kimzeyite belongs to garnet minerals and hasa chemical form of Ca3(Zr,Ti)2(Si,Al,Fe3+)3O12.
Garnet minerals are well known to show an excellent
long-term stability of their structure. This property
attracts an attention as potential storage media ofradioactive nuclear waste. Kimzeyite is also
considered as potential storage media because Hf cansubstitute Zr in kimzeyite. In order to use garnets
as potential storage media, several composition ofkimzeyites were synthesized at several temperatures
under 1000 kg/cm2 by using hydrothermal method.
X-ray powder diffraction measurement confirmedthat the obtained products were kimzeyite. In order
to examine the state of Fe in obtained kimzeyite, 57Fe
Mössbauer spectra were measured. Fe occupies not
only tetrahedral site but also octahedral site as in thecase of yttrium iron garnet. Fe is found to be as
Fe3+ ion in both tetrahedral and octahedral sites.
1P31: Spin-state change accompanied bystructural change in the mixed crystals ofassembled
complexes
bridgedby
1,3-bis(4-pyridyl)propane
DOTE, H.1, INOUE, K.1, NAKASHIMA, S.2(1Grad. School of Sci., Hiroshima Univ., 2N-BARD,
Hiroshima Univ.)
(X=S,
Se,
BH3;
Fe(NCX)2(bpp)2
bpp=1,3-bis(4-pyridyl)propane has very rare
structure which is 2D interpenetrated, while
Fe(NCX)2(bpp) 22(benzene) has 1D chain structure.
By releasing benzene molecules, the host frameworkchanged to 2D interpenetrated structure.
The
desorbed complex enclathrated benzene molecules
again and host frame work returned to 1D chain
structure. In the present study, we performed mixed
metals experiment to know the mechanism of thestructural change accompanied by sorption ofbenzene molecules.
The reversible structuralchange of host framework was tried to explain by
two factors: the crystal stability by making up theinterstitial space and the conformer stability incoordinated bridging ligand.
1P32: The study of f1 configuration having small
axial anisotropy
OHTA, S., YAMAMURA, T., SHIRASAKI, K.,
SATOH, I., SHIKAMA, T.
(Institute for Materials Research, Tohoku Univ.)
As a member of light actinides, pentavalent or
hexavalent uranium is characteristic of [UO2]n+ (n =1 or 2) structure, so called "-yl structure", where twooxygen atoms are bonded to metal ion in axial
symmetry. Magnetisms in pentavalent or hexavalent
neptunyl or plutonyl have been explained by strong
axial ligand field. Among the 5f-electronic states,
uranyl(V) UO2+ is considered to be the mostfundamental configuration (5f1). UO2+ is− 182 −

thermodynamically unstable in the presence of
protons due to a disproportionation reaction (2UO2++ 4H+  UO22+ + U4+ + 2H2O), the study of thechemical properties of this system has been greatly
constrained. On the uranium redox-flow battery
proposed by our group, uranyl(V) is of greatsignificance that is essential as the positive active
material. We were measured at magnetic
susceptibility of uranyl(V) complexes having 5f1
state. The room tempreture effective magneton
moment (µeff) for β-diketonato complexes were
determined to be 1.74, 1.66 and 1.58µB/U5+. Notethat the estimated moment values are below thetheoretical value of 2.54 calculated for the free f1 ion(U5+) by in the L-S coupling scheme. The relatively
smaller value of µeff at the room temperature isbelieved to be caused by the increased ligand field
imposed on the uranium(V) center.
1P33: Stability constants of minor actinides andlanthanides with dithiocarbamate.
MIYASHITA, S., KITATSUJI, Y., KIMURA, T.
(JAEA)The Stability constants of trivalent minor actinides(An3 ; 241Am and 244Cm) and lanthanides (Ln3 ; Eu)
with
Ammonium
pyrrolidinedithiocarbamate(APDC) in aqueous solution were investigated. The
stability constants were obtained by back-extraction
technique using di(2-ethylhexyl)phosphoric acid
(HDEHP) as follows. Aqueous phase was acetic
buffer solution from 0.02 to 0.10 mol/cm3 containing
various concentrations of APDC. Organic phase wastoluene or benzene solution containing HDEHP andtrace amounts of the extracted radionuclide such as
241
Am or 244Cm. Eqvolumes of the aqueous phaseand the organic phase were mixed in vial and wereshaken 30 minutes at 298 K. The results show thatminor
actinides
stronglyinteracted
withdithiocarbamate. From those results, the obtained
stability constants (βn, n = 1, 2) for Am are
logβ1(Am) = 2.5 ± 0.3, logβ2(Am) = 4.3 ± 0.2 at 298
K.
++

1P34: Development of an on-line detection
apparatus using liquid scintillation detectors foranalysis of spent nuclear fuel
YOSHIMURA,
T.1,
KIKUNAGA,
H.1,2,SHINOHARA, A.1(1Grad. School of Sci., Osaka Univ., 2Nishina Center,

RIKEN)We have developed an on-line detection
apparatus using a capillary electrophoresis system
and liquid scintillation detectors for analysis of spent
nuclear fuel. The detectors have been coupled to thecapillary electrophoresis system by using a solvent
extraction technique of flow injection analysis. In
this work, the apparatus have been evaluated byusing a mixture sample of lanthanides, U, Am, Cm,
Cf, Cs, Sr, and Tc. From the results, it has been foundthat only the lanthanides and actinides are extracted
into a liquid scintillation cocktail and introduced into
the detectors in the condition of this experiment. The
lanthanides and actinides have been able to be
distinguished by lifetime discrimination of theemission from the scintillation cocktail. Moreover,the energy resolution of the detectors let us todistinguish the α-particles from the trivalentactinides and U.
1P35: Separation of U/Pu/Am for Safeguards
Environmental Samples
MIYAMOTO, Y., ESAKA, F., MAGARA M.,
KIMURA, T.
(Nuclear Science and Engineering Directorate,
JAEA)
For accurate analyses of Pu in a Pu oxide /MOX particle, the sample should be chemicallyseparated from Am and U. The mass of 241Am whichis daughter nuclide of 241Pu and total mass of apolyatomic ion 238U1H induced from U overlap withthose of 241Pu and 239Pu, respectively. These
interferences lead to systematic error in thequantitative and isotopic analyses of Pu. In this work,
two types of chemical separation technique of U, Pu,
and Am were examined. One is an anion-exchange
separation, and the other is an extraction separation
with the TRU resin. Plutonium, U, and Nd which isanalogous to Am in the chemical behaviors weresuccessfully separated with the both ananion-exchange column combined with HCl media
and a TRU extraction column combined withascorbic acid for reduction of Pu. The
decontamination factors between the elements ofinterest were more than 300 in case of theanion-exchange separation.
1P36: Study on dissipative behavior of radon gas
using groundwater− 183 −

1

1

2

2

Yamada, N. , Uesugi, M. , Sato, W. , Yokoyama, A. ,Nakanishi, T.2(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,
2Inst. Sci. Eng., Kanazawa Univ.)
In the determination of radon in water sample,
particular attention should be given to the radon loss
from the sample. Estimation of the radon loss fromthe sample until the onset of measurement is very
difficult. In addition, Rn loss process is associatedwith solubility of Rn gas. It is affected by solvent
and temperature etc. In other word, they affectdissipative behavior of Rn gas. However, thisbehavior has not been clearly understood. In thiswork, in order to clarify that, laboratory experiments
by using the spring water mentioned above were
performed. For example, we observed the elapsed
time variations of depth profiles of Rn loss using the
5L of sample water in a beaker. It was found that
residual Rn in water tends to decrease with water
depth. Concentrations of residual Rn in water wereconstant from the surface to bottom after still
standing for 24 h. Because the water temperature waslower than the air temperature, convection waspresumably generated in the beaker and this could bea cause of water depth dependence of Rn loss. We
need to obtain further experimental data to clarify thedissipative process of Rn.
1P37: Well water analysis
environmental monitoring

as

a

part

of

KO, S.1, TANAKA, Y.1, OKA, M.1, TSUJIUCHI,
M.2, FUKAGAI, J.2, MIZUOCHI, T.2, TAKEISHI,
M.1(1Japan Nuclear Fuel Limited, 2Tokyo Electric Power
Environmental Engineering Co., Inc.)
Since 1989, we have performed environmental
monitoring at Rokkasho village around Rokkasho
reprocessing plant (RRP). The objects of themonitoring include well water, whose data were notfrequently reported. We showed the concentration of90
Sr in well water at site Obuchi-2 ranged 0.8 ~ 14
mBq/L and had increasing trend since 2003. It wasapproved that this trend was attributed to naturalfluctuation because other artificial nuclides were notdetected and specific activity of 90Sr was constantsince 2003. It was obvious that the 90Sr originatedfrom fallout of past nuclear tests, but thisphenomenon attracts interest from geochemical

viewpoint, so we conducted research to clarify themechanism. We compared the concentration of 90Sr,
stable Sr, electric conductivity etc in the water andsoil samples taken from nearby points. Because theconcentration of 90Sr in well water had goodcorrelation with stable Sr, electric conductivity andother ions, we assumed 90Sr fluctuated along withother soluble substances. Because the increasing
trend started before the active test of RRP (since
March 2006), and large scale land reclamation was
conducted in upstream part until 2003, we assumed
the behavior of 90Sr and other substances was
influenced by change of hydrological condition ofsurrounding environment.
1P38: The improvement of detection limit for
Cs-137 in soil using Ge detector with AMP
procedure
TAMARI, T., KAWASAKI, N.
(Kyushu Environmental Evaluation Association)
In some case, many of gamma ray peaks fromnatural radionuclides such as K-40, U-series,
Th-series, disturb the detection of Cs-137 in soil with
Ge detector. We applied the ammonium
molybdophosphase (AMP) precipitation method to
remove these natural radionuclides. The recovery of
Cs was obtained by AAS measurement of thedilution that dissolved the fraction of AMP
precipitation in NaOH. The gamma spectrum of
AMP shows the peak of Cs-137 more definitive, andsignificant improvement of detection limit. The
results of AMP precipitation method were consistent
with direct measurement.
1P39: Determination of long-lived radionuclides
I and 36Cl in soils from Futaba area, Fukushima
prefecture

129

KITAGAWA, J.,1,2 AMANO, T., 1,2 SUEKI, K., 1,2
SASA, K., 1,2 TAKAHASHI, T., 2 KINOSHITA, N., 2
TOSAKI, Y., 3 MATSUSHI, Y., 4 MATSUZAKI, H.,
5
MIURA, T. 6
(1Pure & Appl. Sci., Univ. Tsukuba, 2Appl. Accel.
Div., Univ. Tsukuba, 3GSJ, AIST, 4DPRI, Kyoto
Univ., 5School Eng., Univ. Tokyo, 6NMIJ, AIST)I  (half-life: 1.57  107 yr) and 36Cl
(half-life: 3.01  105 yr) are important long-lived
radionuclides used as environmental tracers. They
are produced both naturally and through human− 184 −

129

nuclear activities. The majority of 129I has previously
been accumulated in surface soils by global fallout,
whereas the behavior of 36Cl has not been understoodin detail. The aims of this work are to determine 129I
and 36Cl activities in soils, and to compare the two
nuclides on their environmental distributions.
Isotopic ratios of 129I/I and 36Cl/Cl were determinedby accelerator mass spectrometry (AMS). In addition,
to investigate soils in more detail, we determinedorganic matter content in soils by loss on ignition(LOI) and 137Cs concentration in soils by an HPGe
detector. Samples were collected at 8 points from
Futaba area, Fukushima prefecture. We investigatedthe distribution of long-lived radionuclides in surface
soils (0~10 cm) at all points and 1 meter depth
profile at one point.
1P40: Metalbindingcharacterization
hemocyanin purified from liver of squidof

FUJIMOTO K., MORITA T.
(National Research Institute of Fisheries Science,
Fisheries Research Agency)
One of the artificial radionuclides, silver-108m,
is still detected in liver sample of flying squid caught
around Japan. We purified a silver binding proteinfrom liver of squid and identified it as respiration
pigment hemocyanin. Here we show the metalbinding characterization of hemocyanin with 9radioactive elements. Silver showed good binding(0.34 µg-Ag/mg-protein (p)) to hemocyanin
compared to bovine serum albumin (BSA), which
was used for negative control. The amount of silverbond to hemocyanin was not apparently decreased byaddition of copper ion. The result suggested thatthe binding site of silver was not the center of copper
binding site. Although Cadmium was bond tohenocyanin at a high rate (3.9 µg-Cd/mg-p), thesame amount of cadmium was bond to BSA
suggesting that the cadmium binding is not specific.
Strontium, calcium, cobalt, manganese and zinc werealso bond to hemocyanin.
The bindings ofstrontium and cobalt were not inhibited by additionof copper ion. On the other hand, the bindings ofthe other three metal elements were competitively
inhibited by copper suggesting that these metals may
be bond to copper binding site. Cesium andtechnetium were not bond to hemocyanin.
1P41: Role of Radiochemistry inComprehensive Nuclear-Test-Ban Treaty

theYonezawa, C.
(Center for the Promotion of Disarmament and
Non-Proliferation, Japan Institute of International
Affairs)
Verification of nuclear explosion under theComprehensive Nuclear-Test-Ban-Treaty (CTBT) is
carried out by remote monitoring of geophysicalsignals and radionuclides through international
monitoring system (IMS) and on-site inspection(OSI). Radioxenon nuclides including 131mXe, 133mXe,
133
Xe and 135Xe, and radionuclide particles as well asgeophysical signal are automatically monitored by
the IMS. Gamma-ray monitoring and radionuclide
analysis are important inspection technologies for
OSI. Both gamma-ray dose and energy spectrum aremonitored from air and on the ground to narrow
down the inspection area. Radionuclide analysis ofenvironmental samples is performed to determine theevent as a nuclear explosion. In addition toradionuclide analysis in the IMS and the OSI,
radiochemists are requested to consult the national
authorities for an explanation of scientific data to
make national decision pursuant to the Treaty. Roleof and anticipation to radiochemistry in the CTBT
are presented.
1P42: Annual variation of 14C isotope ratio inplant samples (tree rings or rice) by AMSINOUE, A.1, MURAMATSU, Y.1, MATSUZAKI,
H.2, YOSHIDA, S.3(1Gakushuin Univ., 2University of Tokyo., 3NIRS.)
14

C (T1/2 ; 5730yr)
is produced in theatmosphere by the reaction of cosmic ray withnitrogen. Plants remove 14CO2 from the atmosphere
together with 12,13CO2 by photosynthesis. Tree ringsor rice grains have 14C/12C ratios related to that in theatmosphere. The ratios in the atmosphere are affectedby solar activity. We have determined 14C/12C
ratios in tree rings of Yaku-cedar from AC1000 to
1100. As a result, we observed a peak of the ratios
around AC1150, suggesting the solar activity would
be weaken in this period.
We also measured 14C/12C ratios in grains of ricecollected from 1950 to 2009, to estimate thevariation of atmospheric 14C levels which were
influenced by nuclear weapons testing. The highest
peak of 14C/12C ratio was found around 1963 andthen it decreased gradually.

− 185 −

Tree rings of pine collected from the vicinity ofChernobyl NPP to assess the release of 14C at theaccident, which occurred in 1986. A peak of 14C/12C
ratio clearly observed in the tree ring of 1986. Inorder to know the distribution of 14C in this tree ring,
we will determine both early and late wood.
1P43: Distribution of Pu isotopes and Am-241
concentration in the Eastern Pacific
TAKIMOTO, K. 1, NAGAOKA,M. 1, SUMI, T. 1,
KINOSHITA, N. 2,YOKOYAMA, A. 3
NAKANISHI, T. 3
(1 Grad. School Nat. Sci. Tech., Kanazawa Univ., 2
      3
Inst. Sci. Eng., Kanazawa Univ.)
Geographical and depth distributions ofanthropogenic radionuclides of Pu-238, 239, 240,and Am-241 were studied in the Eastern Pacific in
2003. From a result of analyses of Pu isotopes andAm-241 in seawater columns and sediment columns,
it was found that the Pu-239, 240, Pu-238 andAm-241 inventories in water columns are 0.78-5.11
Bq/cm2, 0.62-1.95 Bq/cm2, and 5.32-21.7 Bq/cm2,
respectively, while the Pu-239, 240, and Pu-238
inventories in sediment columns are 0.34-1.26
Bq/cm2 and 0.01-005 Bq/cm2, respectively. The
value of Pu-238/Pu-239, 240 activity ratios ofwater-column
coincided
with
that
of
sediment-column in stations of North Pacific andEquatorial Pacific. They agree with that of global
fallout. Therefore, the Pu isotopes in these sea areas
are considered to originate from global fallout. On
the other hand, the Pu-238/Pu-239,240 activity ratios
in seawater of South Pacific indicate a high value of
0.05-0.11, so that it might be affected by the releaseof Pu-238 from the SNAP-9A artificial satellite
accident.
1P44: Distribution of Pu isotopes in asize-fractionated surface soil sample in northern
China
ZHENG, J.,1 DONG, W.,1,2 YAMADA, M.,1 WGUO,
Q. J.2(Nat. Inst. Radiol. Sci.,1 Beijing Univ.,2)
Two years ago, in the 52th Radiochemistry
symposium, we reported the Pu activity level and theisotopic characteristics in soils in Gansu Province,
northwest China. In this work, we present a recent

investigation on the distribution of Pu isotopes in asize-fractionated surface soil sample collected in a
grassland in Jining, the Inner Mongolia, in
northeastern China. Soil grain size fractions were
determined with sieves. This surface soil consisted ofsand (> 53 μm, 89.6%), with silt and clay (< 53 μm)
contributing ca. 11%. Plutonium isotopes wereanalyzed using SF-ICP-MS after digestion with
HNO3-HClO4-HF and ion-exchange chromatographic
separation/purification. The activities of 239+240Pu
ranged from 0.10 to 0.52 mBq/g, and decreased
nearly exponentially with increasing particle size ofthe soil due to a decreasing surface area. The activityof 239+240Pu in the finest particle (<25μm) which canbe transported to long-distance in the dust event, wasca. 5 times higher than that in the coarse particles(600-1000 μm). In contrast to the significant
variation of 239+240Pu activity, the atom ratios of240
Pu/239Pu did not show any variation, they ranged
from 0.169 to 0.200, with a mass-weighted mean of
0.185 ± 0.025, indicating that Pu originated fromglobal fallout. Although more studies are needed, theresults obtained in this study provided further
evidence to support the hypothesis that the temporalchange of 239+240Pu deposition in eastern Asia iscontrolled by the long-range transport of suspended
soil dust particles originating from the East Asianarid and desert areas.
1P45: QUANTITATIVE ANALYSIS OFENVIRONMENTAL RADIONUCLIDES IN
IMPORTED FOOD- ON THE IMPORTEDFOOD FROM CHINA
MORITA-MURASE, Y., MASHINO, T.
(Faculty of Pharmacy, Keio Univ.)
The food imported from China and its
neighboring countries were heated to 450 with anelectric furnace and were made ashes, then measured
with a Ge spectrometer. Based on the counting rate(cps) of the full energy peak, the concentration of theγ-emitting radionuclides (Bq/kg) was determined.
From the ash sample, which was heated again to500, 90Sr was separated by the oxalate method.
After secular equilibrium between 90Sr and 90Y wasattained, the samples were measured with a liquid
scintillation spectrometer using the modified integral
counting method. The concentration of radionuclide(Bq/kg) were: tea leaves; 137Cs(0.17±0.02 
1.08±0.06), 90Sr(3.74±0.55  12.6±2.8), 40K(450 2100), the frozen food; 137Cs(ND  0.14±0.02 ,− 186 −

90

Sr(ND, except for one sample), dried sea fish;137
Cs(0.055±0.014  0.13±0.02). The concentrationof 40K, 226Ra, 228Ra in the frozen food were lower
than average concentration of these nuclides in thesoil. The results obtained here do not seem to include
an urgent problem of hygiene. However, we have toemphasize that 90Sr and 137Cs must be removed fromthe food and the feed of livestock, because these
nuclides are condensed by the food chain, andaccumulated in a human body.
1P46: Measurement of tritium concentrations inrain and airmass backtrajectory analysis

Yokoyama, H.1, Sugihara, S.2, Momoshima, N.2,
Tanaka, M. 3, Uda, T. 3
(1Grad. School of Sci., Kyushu Univ., 2RIC, Kyushu
Univ., 3NIFS)
Tritium is a radioactive isotope of hydrogenwith 12.33 years half-life and is produced naturally
in the upper atmosphere by interaction withsecondary cosmic radiation. A large quantity oftritium will be used as a fuel at nuclear fusion reactor
that would be a potential source of environmental
tritium in future. Tritium concentrations in rain waterin Fukuoka city and Toki city were determined by
combination of electrolytic enrichment and liquid
scintillation counting. The average of tritium
concentrations observed in rain in Fukuoka and Toki
were 0.79 ± 0.33 Bq/l (2005/5~2009/7) and 0.38 ±0.14 Bq/l (2007/6~2010/3) respectively. A cyclicseasonal variation is observed in both cities: high in
winter/spring and low in summer/autumn. Tritium
concentration in rain in Toki has however showing asmaller variation compare with that in Fukuoka. The
back trajectory analysis of airmass suggests that therain clouds arrived at Fukuoka from the Eurasia
continent give rain with higher tritium concentration
than those from the Pacific Ocean. The seasonalvariation observed in tritium concentration is
concluded to be originated from migration pathwayof airmass which is strongly dependent upon
meteorological factors. In symposium, we also report
the result of the back trajectory for Toki city anddiscuss the difference of tritium concentrations inboth cities.
1P47: Seasonal variations of 228Ra, 226Ra, and228
Th activities in surface water on the east side of
the East China Sea and their implications

Yoshida, K.1, Inoue, M.1, Kiyomoto, Y.2, Kofuji, H.3,
Nagao, S.1, Hamajima, Y.1, Yamamoto, M.1(1LLRL Kanazawa Univ., 2Seikai National Fisheries
Research Institute, 3Japan Marine Science
Foundation)
In the surface of the East China Sea (ECS), theKuroshio water (KW) and the continental shelf water(CSW) are mixed, then the mixed water injects into
the Japan Sea as Tsushima current. To understandmaterial transport from ECS to the Japan Sea, themixing mechanism of two water mass should be
elucidated. The surface sea water samples werecollected at 5 sites on the east side of ECS in 2-3
months interval during the Yoko Maru and Soyo
Maru expeditions, and 226Ra, 228Ra, and 228Th
activities were measured using low-backgroundγ-spectrometry. The  228Ra/226Ra and 228Th/228Ra
activity ratios among the samples exhibited notableseasonal variation (228Ra/226Ra = 0.4-2.7; 228Th/228Ra= 0.1-0.4) accompanying the changes of salinity(31.3-34.5). These changes are hypothesized to cause
the change by altering the mixing ratio of 228Ra-richand high-particle CSW within the ECS. However,the variation of 228Th/228Ra ratio does not closely
agree with the mixing ratio of CSW (228Ra/226Ra andsalinity). In this study, we compare the seasonalvariation of 228Ra/226Ra and 228Th/228Ra activity ratios
in surface water and discuss the transport of watermass and particle reactive materials in ESC.
1P48: A new system of Pb-210 measurement for
sedimentation rates at the Geological Survey ofJapan
KANAI, Y.1, SAITO, Y.1, Yang, Z.2 and Fan, D.2(1Geol. Surv. of Japan, AIST, 2Ocean Univ. ofChina )We have measured the sedimentation rates oflakes and sea bottom sediments by use of thewell-type Ge semi-conductor detectors at the
Geological Survey of Japan, AIST. Now we renewed
the measurement system because they became oldand sometimes had trouble with the detector. In thispresentation we show the details of the newmeasurement system and some results of
sedimentation rates at the Huanghe estuary that were
measured in this system. The system is composed of
the well-type Ge detector (Ortec GLW-120230-S), J
type cryostat and shielding (Pb 115mm, Fe 48mm,
Cd 2mm, Cu 20mm, acryl 5mm). The continuous− 187 −

background level of gamma spectrum decreased
when the J type cryostat was used rather than thevertical type cryostat was. The oxygen free copper(OFC) materials also lowered the background level(continuous and peak) than the Al materials. The
bottom sediments were taken at the Huanghe estuary
in 2009 using gravity corer and the activities oflead-210, lead-214 and cesium-137 were measured.
1P49: Estimation on transport of riverine
suspended solids in Satoyama area using 137Cs and210
Pbex as geochemical tracers
TOKUNARI, T. 1, SUZUKI, T. 1, OCHIAI, S. 2,
NAGAO, S. 2, YAMAMOTO, Y. 2
(1Grad. School of Sci., Kanazawa Univ., 2Low Level
Radioactivity Lab., Kanazawa Univ.)
Investigation of sediment transport in river
systems is important to make protection of foodproduction and sediment disaster. In this study,
riverine suspended solids (SS) have collected in the
Kumaki River, which runs through abandoned
Satoyama area in Noto Peninsula. To estimate themain source of SS, surface soil samples were alsocollected from managed and unmanaged forest, andpaddy field. The samples were analyzed for 137Cs and210
Pbex by gamma spectrometry. The low 137Cs /210Pbex
activity ratios are found in surface samples ofabandoned paddy rice field associated withaccumulation of 210Pbex relative to 137Cs. The low
ratio of 137Cs /210Pbex is also found in surface soil
samples of unmanaged forest because heavy rainerodes surface soil. The river bottom sediments show
relatively low 137Cs /210Pbex activity ratio in thewatershed area that runs through unmanaged forest,
paddy rice field, and abandoned paddy rice field.
These results indicate that in the Kumaki basin,
particle transport processes are controlled by surface
soil erosion from the forest area and paddy field by
washout of heavy rain.
1P50: Determination of trace elements andtransformation of proteins in pancreas ofzinc-deficient mice
MURAMATSU,
W.1,
SHIMOYAMA,
H.1,
YAMAMOTO, O.2, KAWASHIMA, M.1, TANAKA,
H.1, IKEDA, Y.2, SUGANUMA, H.2, YANAGA,
M.2(1Graduate School of Science, Shizuoka University,
2
Radioscience Research Laboratory, Faculty of

Science, Shizuoka University)
Concentrations of trace elements and proteinsin pancreas of Zn-deficient and control mice were
investigated. Eight weeks old male mice of ICR
strain were divided into two groups; one was fed
with Zn-deficient diet, and the other with control diet.
After a week, their pancreases were removed andevery four pancreases of each group were together
homogenized in a Tris buffer. Then, a cytosol
fraction was separated from the homogenate by
centrifugal separation method. SDS-PAGE and 2D
electrophoresis were carried out. Proteins in thecytosolic fraction were also separated into twenty
fractions by gel-filtration chromatography. After that,
SDS-PAGE was performed for each fraction. New
bands were found on the gel for a few fractions of
Zn-deficient mice. Bradford protein assay and atomic
absorption spectroscopy were also performed foreach fraction. For concentration of protein in all
fractions, there were no significant differences
between two groups. On the other hand,concentrations of zinc in several fractions of
Zn-deficient group were decreased. These results
indicate that some zinc-bound proteins may exist for
apo-proteins.
1P51: Effects of zinc deficiency on behavior oftrace elements and change of metalloprotein intestes in mice
Tanaka, H.1, Shimoyama, H.1, Ikeda, Y.2, Yanaga,
M.2(1Graduate School of Science, Shizuoka University,
2
Radioscience Research Laboratory, Faculty of
Science, Shizuoka University)
Zinc is one of the most important essentialtrace elements. Zinc deficiency leads to skin injury,
alopecia, growth retardation, loss of sense and so on.
The production of testosterone and spermatogenesis
are also affected by zinc deficiency. Eight weeks oldmale mice of ICR strain were divided two groups.
One is Zn-def. group fed with Zn-def. diet, and otheris control group fed with control diet. After a week,
their testes were removed and every four testes ofeach group were together homogenized in a Tris
buffer. Then, a cytosol fraction was separated fromhomogenate by centrifugal separation method.
SDS-PAGE and two-dimensional electrophoresis
were carried out. When the positions and thenumber of the protein spots in gel two-dimensionaly− 188 −

developed the cytosolic fraction of Zn-def. mice
were compared with those of control ones,
significant differences were found between them.
1P52: Evaluation for olfactory transportmechanism of intranasally administered 201Tl
NAGAOKA, M.1, TAN, A.2, WASHIYAMA, K.3,
AMANO, R.3(1Grad. School Medical Sci., Kanazawa Univ., 2Fac.
3
Med.
Kanazawa
Univ.,
CollegeMed.
Pharmaceutical and Health Sci., Kanazawa Univ.,)
Our laboratory has found that the migration of
a portion of heavy-metal ions such as 201Tl+ canaccess to the brain bypassing the Blood-Brain Barrier
via olfactory neurons. This phenomenon is referred
to as an olfactory transport, clinical development ofolfactory functional diagnosis using this pathway is
now undergoing. However, its transport mechanism
has not proven yet. In this study, for elucidation of
the mechanism, we studied the intranasal delivery to
the brain by using 201TlCl and 99mTc-MIBI, both ofthem were used for myocardial perfusion imaging.
Moreover, we weighed the inhibition effect for thebrain of three inhibitors, ouabain, cholchicine, andfurosemide, by using double tracers, 201Tl and 54Mn.
Anesthetized ICR male mice were intranasallyadministered the prepared solutions mixed with 201Tl
and 99mTc-MIBI or 54Mn into the right nostril. In thisexperiment, mice were pretreated with intranasal
administered inhibitor. The animals were sacrificed 1,
3, 6, 12, 24 hours, and 3, and 7days after double
tracer administration. While uptake of 201Tl into theolfactory bulb was gradually increased with time,
uptake of 99mTc-MIBI was not observed. Bothouabain and cholchicine treated group, uptake of201
Tl into the brain was not affected by theirinhibitors.
1P53: Synthesis of
188
Re-[(CO)3 (H2O)3]+

186,188

Re-MAG3

and186,

KURIHARA, Y.1, 2, NOGAWA, N.2, HASHIMOTO,
K.3, KOIKE, Y.2, MORIKAWA, N.2 and IJIRI, K.2(1Org. Strategic Coordinat. Res. Intellect. Prop.,
Meiji Univ., 2RIC, Univ. Tokyo, 3Japan Atomic
Energy Agency)
Both 186Re (β raymax 1.08 MeV) and 188Re (βraymax 2.12 MeV) are expected as therapeutic nuclide
in the cancer treatment and the pain easing.

186,188
Re-MAG3
Synthesisof186,(mercaptoacetyltriglycine)complexand188+
Re-[(CO)3 (H2O)3] (tricarbonyl) complex were
examined under various conditions

1P54: Treatment for osteoblastic metastasis inrats using α-particle emitting 227Th-EDTMPWASHIYAMA, K. 1, YACHIDA, T. 2, SATOU, I. 3,
YAMAMURA, T. 3, AMANO, R. 1
(1College of Medical, Pharmaceutical and Health
Sciences, Kanazawa Univ., 2Sch. of Health Sciences,
Kanazawa Univ., 3Institute Material Res., Tohoku
Univ.)
Most patients with advanced breast, prostate,or lung carcinoma develop metastases. Especially,bone metastases cause severe pain, so there havebeen many attempts such as surgical invention,
chemotherapy, external radiation therapy, and so on.
However, many of these treatments are limited intheir efficacy or duration and have significant side
effects.
Due to the high LET and short range of
α-particles in tissue, α-emitting nuclides arepromising for the treatment of bone metastases.
Reduction of bone marrow exposure can be achieved
due to the short range of α-particles. In this study, weevaluated the therapeutic effect of α-emitting
227
Th-EDTMP for osteoblastic metastasis in rats.
Copenhagen strain rats were inoculated with3
3x10 cells of syngeneic prostate cancer cell line
MAT-LyLu into the right tibia. One week after cell
inoculation, 250kBq/kg b.w. of 227Th-EDTMP wasinjected into rats via tail vein. During 4 weeks aftercell inoculation, antitumor effect and pain palliation
effect were examined using tumor volume
measurement and von Frey filament test,
respectively.
The von Frey filament test showed bone pain
palliation 2 weeks after cell inoculation. Tumor
growth were inhibited 17 days after cell inoculation,
however there were no tumor growth inhibition on
21 days after cell inoculation.
1P55: Reduction of the cosmic ray components of
the Ge detector utilizing the thin plastic
scintillators for anticoincidence
HAMAJIMA, Y.
(LLRL, Kanazawa Univ.)− 189 −

The contribution of cosmic ray components on
background of Ge detector is reduced by means of anactive anti-coincidence detector system. In order toinsert into lead shield and cover 2π geometry of Ge
detector, five thin plastic scitillators (PSs) (180 mm x
180 mm, and 3 mm in thickness; ELJENTECHNOLOGY; EJ-200) connected with five
wavelength shifting fibers (1 mm in diameter;
BICRON BCF-91A) that was coupled to one thin
PMT (1/2”; HAMAMATSU H3165-10) through fiveclear fibers and photo-couplers has been developed.
The PSs system was inserted into the passive shieldof Ge detector. All events were recorded in list mode.
Relative efficiency of PSs, time spectra, timedependences of coincidence events, multiple
coincidence
events,andcoincidence
andanti-coincidence spectra were re-tested. This thin PSs
system has sufficiently thickness to detect cosmic raycomponents and expects to reduce more than 50% of
those induced background components.
1P56: Correlation between the particle size
distribution of radioactive aerozols and theirhalf-lives -Based on the experimental results in
120 GeV proton target stationSEKIMOTO, S. 1, YASHIMA, H. 1, OSADA, N. 1,
OKI, Y. 1, SHIBATA S. 1, MATSUMURA, H. 2,
TOYODA, A. 2, OISHI, K. 3, MATSUDA, N. 4,
KASUGAI, Y. 4, SAKAMOTO, Y. 4, NAKASHIMA,
H. 4, LEVELING, A. 5, LAUTENSCHLAGER, G. 5,
BOEHNLEIN, D. J. 5, VAZIRI, K. 5, MOKHOV, N. 5
(1KURRI, 2KEK, 3SHIMIZU CORP., 4JAEA,
5FNAL)
In Anti-proton target station (AP0) in Fermi
National Accelerator Laboratory, the Inconel target is
irradiated by ultra-high energy protons at 120 GeV.
In terms of external and internal exposure, it isimportant to understand the behavior of radioactive
aerosols in an accelerator target room. In this work,
we separated radioactive aerosols collected from thetarget room of AP0 into several samples according toparticle size by using the impactor method, andobtained particle size distribution of radioactive
aerosols
associatedwithcorresponding
radio-nuclides through measuring activity of various
radio-nuclides in those samples by gamma-ray
spectrometry. Consequently, it was found that theparticle size distribution of radioactive aerosols tends
to depend on their half-lives of their corresponding
radio-nuclides. Based on the results, the behavior

and the formation mechanism of radioactive aerosolsin the target room will be considered in detail.
Additionally, to obtain the information about smaller
size of radioactive aerosols than those separated by
the impactor method we collected radioactive
aerosols in the same place as noted above using thegraded screen array (GSA) method. We also intend
to present the results obtained by GSA method.
1P57: Simple determination method for 99Tc inradioactive waste arising from research facilities
KAMEO, Y., ISHIMORI, K., HOSHI,WATANABE, K., TAKAHASHI, K.
(Japan Atomic Energy Agency)A.,

On disposal of radioactive waste packages, anevaluation of radioactivity inventories in the
packages is required. Technetium-99 is one of theimportant nuclides from the viewpoint of safetyassessment for disposal of radioactive wastes,
because of its very long half life. In the present study,a simple 99Tc determination method was developed
for surface contaminated metal wastes. First,
pretreatment conditions for removing 99Tc from thesurface of metal were studied. It was found thatrecovery of 99Tc by soaking with acids was higher
than that by alkali fusion with sodium hydroxide.
More than 90% of 99Tc could be recovered from thesample solution containing large amounts of iron(>0.5g) using a solid phase extraction resin(TEVA-Resin). In the separation using the resin, therecovery of 99Tc was good agreement with that of Re,
which was added as a tracer. Finally, the simple 99Tc
determination method was successfully applied toactual radioactive metal waste samples arising fromJapan Power Demonstration Reactor of the JAEA.
2A01:
Electronic
structureofchalcogenide−capped octahedral hexatechnetium
complexes
YOSHIMURA, T.1, TAKAYAMA, T.2, SEKINE,
T.3, KINO, Y.4, SHINOHARA, A.1(1Grad. School of Sci., Osaka Univ., 2Daido Univ.,
3
CAHE, Tohoku Univ., 4Grad. School of Sci.,
Tohoku Univ.)
The HOMO/LUMO levels, the frequency of
the C≡N stretching bands, and the electronictransition energies in [Tc6Q8(CN)6]4– (Q = S or Se)
were determined by DFT calculations. The LUMO is− 190 −

localized on the technetium atoms in both
hexatechnetium complexes. The HOMOs are
localized on the Tc6Q8 core. The plot of the energy
level of HOMO in [M6Q8(CN)6]4– (M = Tc, Re; Q =S, Se) against the redox potential of the M6(23e/24e)
process exhibits a good linear correlation. The
HOMO-LUMO energy gap of the hexatechnetium
complexes is approximately 0.6 eV (4800 cm–1)
smaller than that of [Re6Q8(CN)6]4–.
Electronic singlet transitions from the HOMO
regions to the LUMO regions were also calculatedusing TD-DFT method. The TD-DFT calculationsforbothsulfideandselenide-cappedhexatechnetium complexes indicate that thesubstantially allowed singlet transitions in the rangeof 400-500 nm are ascribed to the Tc6Q8
core-centered. The longer wavelength shift of theselenide-capped complex at the lowest energy
electronic transition compared to that of thesulfide-capped complex in the hexatechnetium
complex shows the same trend in the experimental
UV-vis data in acetonitrile.
2A02: Synthesis and Redox Properties
Bis(salophen)uranium Type Complexesof(1Japan Atomic Energy Agency, 2Kyoto Institute forInteresting Chemistry)
Neptunium(V) ion is reduced by electrolysis
through two reduction paths, i.e. the chemical
reaction with Np(III) produced from Np(IV) by
electrode reaction and the electrocatalytic reduction
by adsorbed hydrogen atom on platinum electrodesurface. Based on the electrocatalytic reduction,
development of rapid and selective electrolytic
reduction of Np(V) to Np(IV) is expected. A
flow-through electrode of glassy carbon (GC) fiber
platinized by electrodeposition was examined in thepresent study. Although Np(V) was reduced toNp(III) at the much negative potential at aflow-through electrode of normal GC, stepwise
reductions of Np(V) to Np(IV) and Np(IV) to Np(III)were observed on the potential-current relation ofelectrolysis at platinized GC electrode. The
overpotential of reduction of Np(V) to Np(IV) was
decreased. This electrolysis method enables us toprepare Np(IV) rapidly without producing Np(III).
Np(V) in the mixture solution of Np and U was also
reduced to Np(IV) selectively, not accompanied with
reduction of U(VI).

Matsuda, K., Yoshimura, T., Shinohara, A.
(Grad. School of Sci., Osaka Univ.)

2A04: The new methods for preparing trivalenturanium and its structure and magnetis

The substituent effect to the redox properties
of uranium complexes produced by the reaction ofUCl4 with bis-salophen type ligands (H2(R1/R2) =N,N’-(4,5-R1-1,2-phenylene)bis(5-R2-2-hydroxybenz
ylidenimine), (R1/R2) = Cl/Cl (1), Cl/OMe (2) werestudied. In 2, two ligands coordinate to a uranium
atom to give eight-coordinate structure. The twoligands are oriented head-to-tail conformation. Thismay be due to the steric hindrance of the substituent
groups at R1 and R2 positions. The U-O (av. 2.24(4)Å) and U-N (av. 2.62(4) Å) distances are resemble
those of the congeners. The redox potentials of 1 and2 were measured by cyclic voltammetry in CH2Cl2.
The plot of the redox potentials versus Hammett
constants (para effect) shows linear correlations. This
indicates that the electron donating/withdrawing
ability of the donor atoms directly affects to theredox potential of the actinide center.

YAMAMURA, T., OHTA, S., SHIRASAKI, K.,
SATOH, I., SHIKAMA, T.
(Institute for Materials Research, Tohoku Univ.)

2A03: Selective electrocatalytic reduction of
Np(V) to Np(IV) at a flow-through electrode
KITATSUJI Y.1, KIMURA T.1, KIHARA S.2

The uranium(III) compounds have attracted
large interests in the coordination chemistry,
catalysis, magnetism and separation chemistry.
Uranium(III) compounds are prepared under
reducing condition because of its instability against
rapid oxidation. In the preparation of uranium(III)organometallic complexes, halides such as iodide
and chloride have been used as the important starting
material. Uranium(III) triiodides such as UI3 andUI3(thf)4 (thf = tetrahydrofuran), which has been
prepared for uranium metal, have played a major rolein synthesis of uranium(III) organometallic
complexes. We have developed a new method toprepare UCl3(thf)1.5 combining mercury-cathodeelectroreduction
andthevacuumdrying.
UCl3(thf)1.5
wasmeasuredthetemperature-dependent magnetic susceptibility andthe effective magnetic moment was determined to be
3.58 µB, which is near to the expected value for f3− 191 −

(3.64 µB/U3+). And crystal structure was determinedat pyridine adduct of uranium (III) chloride complex.
This compound is convenient for use as starting
material because of easy dissolution into various
polar solvents. We report a simple and easy
preparation method of uranium(III) chlorides fromuranium oxide. And the structure and the magnetismof the prepared uranium(III) chloride with solvent
adduct were studied in solid state.
2A05: Solvent extraction of heavy actinides (III)with HDEHP
R.1,

K.1,

Y.1,

OOE,
KOMORI,
TAKAYAMA,
1
FUJISAWA, H. , KURIYAMA, A.1, KIKUTANI,
Y.1, KIKUNAGA, H.2, KASAMATSU, Y.1,
YOSHIMURA, T.1, TAKAHASHI, N.1, SAITO,TOYOSHIMA,
A.4,
ASAI,
M.4,
T.3,
MITSUGASHIRA, T.4, SHINOHARA, A.1(1Grad. School of Sci., Osaka Univ., 2Nishina
Center, RIKEN, 3Radioisotope Res. Center, Osaka
Univ., 4JAEA)The extraction behavior of trivalent actinides
(Am,
Cm,
Cf,
Es,
and
Fm)
with
di(2-ethylhexyl)phosphoric acid, HDEHP, into
benzene has been studied together with a series oflanthanides.
Fermium-250 (T1/2 = 30 min) was produced in
the 238U(16O,4n) reaction using the AVF cyclotron of
RCNP, Osaka University. The reaction products
recoiling out of the target were transported through a
Teflon capillary to a chemistry laboratory. The
transported products were deposited on a Naflon
sheet for 30 min and were then dissolved with 0.2
mL of 0.1 M HNO3. The aqueous phase was mixed
with 0.2 mL of  0.1-0.3 M HDEHP-benzene
solution and was then shaken for 10 min. After phaseseparation by centrifugation, 0.16 mL aliquots of thetwo phases pippeted were separately evaporated todryness on 2 Ta dishes, which were subjected to
α-particle spectrometry with Si PIN photodiodedetectors. The extraction constants Kex were
determined by the slope analysis for the variation of
the distribution ratio as a function of theconcentration of HDEHP. The Kex values oflanthanides, Am, Cm, Cf, and Es were also
determined by the batch-wise extraction experiments
using non-radioactive lanthanides and radiotracer of241
Am, 243Cm, 249Cf, and 253Es. We found that theextraction constant of Fm is smaller than that of Dy
in spite of the similar ionic radii, while the Kex valuesof other actinides are almost the same as those ofeach lanthanide with a similar ionic radius.
2A06: Challenge for establishing a simplified
separation process of trivalent minor actinides
using novel R-BTP adsorbents
USUDA, S.1, KURAOKA, E.1, LIU, R.1, XU, Y.1,
KIM, S.Y.1, YAMAZAKI, H.1, ISHII, K.1, WAKUI,
Y.2, HAYASHI, H.2(1 Tohoku Univ. CYRIC., 2 AIST Tohoku)
In order to directly separate trivalent minor
actinides (MA: Am, Cm) from fission products (FP)containing rare earths (RE) in high level radioactive
liquid waste (HLLW), the authors have beenchallenging for establishing a simplified MA
separation process by extraction chromatography.
We have attempted a new type of nitrogen-donor
ligand,R-BTP(BTP:
2,6-bis(5,6-dialkyl-1,2,4-triazin-3-yl)pyridine, R: alkyl
group) as an extractant because it shows highextraction selectivity for Am(III) over RE(III). It wasreported that the R-BTP extractants showed different
properties such as adsorbability and stability byhaving different alkyl groups. Therefore, novel
R-BTP extraction adsorbents were prepared byimpregnating appropriate R-BTP ligands into theporous silica/polymer composite support (SiO2-P
particles).
This presentation deals with i) adsorption anddesorption properties of Am and FP in simulated
HLLW solution containing HNO3 onto theisohexyl-BTP adsorbent, ii) hydrolytic and radiolytic
stabilities of the adsorbents were examined, and iii)
other type of R-BTP adsorbents were also preparedand investigated.
2A07: Basic research of spent fuel reprocessing
process based on sulfurization: (1) sulfurization of
tracer doped sample
KIRISHIMA, A.1, Ohnishi, T.2, SATO, N.1(1IMRAM, Tohoku Univ., 2Oarai Center, JAEA)
For the recovery of fissile materials from spent
nuclear fuel, we have proposed a novel reprocessing
process based on selective sulfurization of fission
products (FPs). The key concept of this process isutilization of unique chemical property of carbon
disulfide (CS2), i.e., it works as a reductant for U3O8
but works as a sulfurizing agent for trivalent− 192 −

actinides and lanthanides. In this study, actinide
tracers (236Pu, 239Np, 241Am) and FP traces (152Eu,
137
Cs, 90Sr) were doped to U3O8 to prepare asimulated spent fuel sample. This RI tracer doped
sample was sulfurized at a range of temperature 300
to 550 oC by flowing CS2 gas for 1 hour. Aftersulfurization, the sample was immersed into 1M
nitric acid solution and shaken for 1 hr at 50 oC.
Then, the solution was separated by suction filtration
to determine the relative concentration of eachelements in the solution by alpha- and gamma-ray
spectrometry. The separation ratios of FPs from U
and Pu and the applicability of this procedure for the
spent fuel reprocessing are discussed in thepresentation.
2A08:
A
newly
developed
rhenium/technetium-99m separation methodfrom molybdenum matrix
TAGAMI, K.1, UCHIDA, S.1, NAGATSU, K.2,
KAGIYA, S.3(1Office of Biospheric Assessment for Waste
Disposal, Natl. Inst. Radiol. Sci., 2Molecular Imaging
Center, Natl. Inst. Radiol. Sci., 3Tokyo Nuclear
Services Co. Ltd.)
It is necessary to develop new separation
methods for technetium-99m (99mTc) frommolybdenum (Mo) to use domestically produced
99m
Tc in radiopharmaceuticals. National Institute ofRadiological Sciences plans to develop its own
method for 99mTc supply using 100Mo (p, 2n) 99mTc
reaction. To separate 99mTc from Mo, a sequential
use of Tc-selective extraction chromatographic resin(TEVA resin, Eichrom) and anion exchange resin(Dowex 1X4, Muromachi Kagaku Kogyo) wasinvestigated. Rhenium (Re) was used as a chemical
analogue of 99mTc. Our goal is to obtain a high Mo
recovery for reuse, minimize Mo concentration of <1 µg/mL in the final Re/Tc fraction, and recover
Re/Tc into HCl solution. In the present procedure
Mo powder was dissolved in a mixture of H2O2 andNH4OH, and then Re was added. After extraction of
Re on TEVA resin from the Mo solution, Re wasrecovered with 8N HNO3 at almost 100% recovery.
Mo remained in the Re fraction was removed using
Dowex 1X4 and finally Re was eluted with 6N HCl
solution. Mo concentration was low enough (< 1µg/mL) and Re recovery was about 60-70%. When
we used the method for 99mTc, total recovery of
85-88% was achieved.

2A09: Productions of 52Fe and 62Zn and Synthesisof iron- and zinc-hematoporphyrin complexes for
PET imaging
KURIYAMA, A.1, OOE, K.1, KOMORI, Y.1,
FUJISAWA,H.1, TAKAYAMA, R.1, KIKUTANI,
Y.1,
KIKUNAGA,
H.2,
NAKAI,
K.1,
YOSHIMURA,
T.1,
TAKAHASHI,
N.1,
1
1
KASAMATSU, Y. , SHINOHARA, A.
(1Grad. School of Sci., Osaka Univ., 2Nishina Center,
RIKEN)
Iron-52- and zinc-62-labeled hematoporphyrinwould be promising reagent for the cancer diagnosis
because it is known that porphyrin-based molecules
accumulate in the cancer cells. In this work, we
studied the rapid separation methods for 52Fe and62
Zn tracers from the target materials and thesynthesis of iron- and zinc-labeled hematoporphyrin
complexes in a tracer scale for PET imaging. The
isotopes 52Fe and 62Zn were produced in the natCr(3He,xn) 52Fe and natNi (α,xn) 62Zn reactions,
respectively, using thce AVF cyclotron at ResearchCenter for Nuclear Physics, Osaka University. The
Cr2O3 and Ni powders were mixed with KCl powder
and used as the target materials.  The reaction
products attached to KCl were dissolved in aqueous
HCl solutions of pH 3 and separated from theinsoluble target materials, namely Cr2O3 and Ni. The
amounts of radioactivities of 52Fe and 62Zn separated
from the targets were measured by γ-spectrometryusing
Ge
detectors.
Zinc-65-labeled
hematoporphyrin was successfully synthesized in a
tracer scale. We succeeded in rapid synthesis of theiron-hematoporphyrin complex by using microwave.
The synthesis of 55Fe-labeled hematoporphyrin will
be performed in a tracer scale.
2A10: Study of the 188W-188Re generator using
PZC
KURIHARA, Y.1, 2, NOGAWA, N.2, HASHIMOTO,
K.3, KOIKE, Y.2, MORIKAWA, N.2 and IJIRI, K.2(1Org. Strategic Coordinat. Res. Intellect. Prop.,
Meiji Univ., 2RIC, Univ. Tokyo, 3Japan Atomic
Energy Agency)
Re-188 (β raymax 2.12 MeV) is expected astherapeutic nuclide in the cancer treatment and thepain easing. Poly Zirconium Compound (PZC) has
the adsorption capacity of the tungsten tens of times
or more the alumina. The basic experiment was− 193 −

done for preparation the small size and practical188
W-188Re generator using PZC with different
synthesis conditions. Adsorption yield of 188W to
PZC ranged from 40% to 100% by heating of 90
and 180 minutes.
2B01: Studies on hot atom chemical behavior ofenergetic ions in solids(XXIII)-Study of Retention Behavior of Hydrogen
Isotopes in Boron Film Deposited on SS-316 –FUJISHIMA,T.1,,KOBAYASHI,M.1,KURATA,R.1,
OSUO,J.1,SUZUKI,M.1,HAMADA,A.1,MATSUOK
A,K.1,ASHIKAWA,N.2,SAGARA,A.2,OYA,Y.1,OK
UNO,K.1(1 Radiosci. Res. Lab. Fac. of Sci., Shizuoka Univ., 2
NIFS.)
Boronization has been applied as one of themost effective techniques for first wall conditioningin Large Helical Device (LHD). Boron is easily
bound to impurities and the impurity-containedboron film will be formed. It is considered thatenergetic tritium from plasma will be implanted andretain into boron film. It is thought that chemical
state of oxygen would influence the retention
behavior of hydrogen isotopes due to the stablehydrogen trapping by oxygen.. In the present study,
the influence of oxide layer on deuterium retention
was studied using two different substrate of silicon
and SS-316.
The boron films were prepared by the plasma
CVD apparatus on the SS-316 and the silicon
substrates, and deuterium ions (D2+) were implanted
into the films with ion fluencies of 1.0 × 1022 D+ m-2
The chemical states and the atomic ratio of boron
films were evaluated by XPS and the deuterium
desorption behavior was revealed by TDS.
The major chemical state of boron on silicon is B-O
bond, while that on SS316 is B2O3.In D2 TDS spectra
for SS316 substrates, three D2 desorption stages werelocated around 500 K, 630K and 780 K, indicatingthat these stages were desorption processes of
deuterium trapped as B-D-B, B-D and B-O-D bonds.
The deuterium retention for SS316 is less than forsilicon, suggesting that deuterium desorption
behavior depend on changing chemical state of boron
film for oxygen layer.
2B02: Studies on hot atom chemical behavior ofenergetic ions in solids(XXIV) ~Elucidation ofchemical behavior of deuterium in tungsten undersimultaneous energetic triple ion (C+, D2+ andHe+) implantation
KAWASAKI, K.1, KURATA, R.1, KOBAYASHI,
M.1, OSUO, J.1, SUZUKI, M.1, HAMADA, A.1,
MATSUOKA, K.1, SAGARA, A.2, YOSHIDA, N.3,
OYA, Y.1, OKUNO, K.1(1Radiosci. Res. Lab. Fac. of Sci., Shizuoka Univ.,
2
NIFS., 3Res. Inst. for App. Mech., Kyushu Univ.)
In D-T fusion reactors, the combination usageof tungsten and CFC has been considered as plasma
facing materials especially for the divertor. During
plasma operation, it is anticipated that carbon will be
sputtered by energetic particles and implanted into
the surface of tungsten with energetic hydrogenisotopes and helium from plasma. Therefore, it ispredicted that simultaneous implantation of carbon
and helium affects on hydrogen isotopes retention
including tritium. In the view point of tritium
recycling, elucidation of tritium retention behavior intungsten under the simultaneous ion implantation is
one of the most important issue. In this study, D2+, C+
and He+ were implanted into tungsten simultaneously
and the deuterium retention behavior in tungsten wasinvestigated by means of TDS and XPS. Comparing
the D2 TDS spectrum for D2+-C+-He+ implanted
tungsten to those for D2+-C+ and D2+-He+ implanted
one, it was found that D2 TDS spectrum for
D2+-C+-He+ implanted tungsten showed almost thesame D2 desorption stage as that for D2+-He+
implanted one at 400-600K, and the D2 desorption
stages around 800 K observed in D2 TDS spectrum
for D2+-C+ implanted tungsten were not appeared.
These facts indicate that implanted He+ prevents thetrapping of D as C-D bond and by irradiation defects.
2B03: Studies on hot atom chemical behavior ofenergetic ions in solids (XXII)- Annihilation
behavior of irradiation defects generated in
gamma-ray irradiated lithium oxideMIYAHARA, Y. 1, KOBAYASHI, M. 1, KURATA,
R. 1, OSUO, J. 1, SUZUKI, M. 1, HAMADA, A. 1,
MATSUOKA, K. 1, FUJII, T. 2, YAMANA, H. 2,
OYA, Y. 1, OKUNO, K. 1
1Radiosci. Res. Lab., Fac. of Sci., Shizuoka Univ.,
2
Res. Reactor Institute, Kyoto Univ.
In blanket systems for the D-T fusion reactor,
it is considered that ternary lithium oxides will be
introduced as a tritium breeder by reactions of− 194 −

6

Li(n,α)T and 7Li(n,n’α)T. After generation of tritium,
it will lose its energy and be trapped by irradiation
defects induced by high energy radiation. Many
studies have reported that behaviors of irradiation
defects during annealing processes are associatedwith tritium trapping and detrapping, andannihilation behaviors of irradiation defects
associated with tritium release show two processes
attributed by recombination or aggregation.
Therefore, it is important to understand theannihilation behaviors of irradiation defects. On theother hand, gamma-ray irradiation  can induce
irradiation defects by only electron excitation process.
Then, in this study, the annihilation kinetics ofirradiation defects in gamma-ray irradiated Li2O
were clarified by Electron Spin Resonance (ESR).
From the ESR spectra, F+-center and O--center wereformed as irradiation defects. According to theisochronal annealing experiments, it was indicatedthat F+-center and O--center were disappeared by therecombination and F-center aggregation (FA) was
formed at the temperature range of 300 - 475 K. The
activation energy for recombination of F+-center andO--center was calculated by the results of isothermal
annealing experiment to be 0.36 eV.
2B04: Mössbauer Spectra of New Cathode Active
Material for Lithium Ion Battery
NISHIDA, T.1,2
 (1Fac. Humanity-oriented Sci. Eng., Kinki Univ.,
2
Grad. School Advanced Sci. Eng., Kinki Univ.)
Mössbauer spectra of cathode for lithium ion
battery, in which LiFeVPOx glass is used as acathode active material, show a reduction of FeIII to
FeII after discharge to 2.0 V, while an oxidation of
FeII to FeIII after charge to 4.0 V. Isomer shift of
FeIII (0.43 mm s-1) and that of FeII (1.14 mm s-1)
indicate the presence of structural units of FeO6
octahedra, as is the case for several phosphateglasses. Heat treatment of LiFeVPOx glass results in
an increase in the specific capacity of the lithium ion
battery from 50 to 150 mAh g-1, due to a structural
relaxation of the glass network accompanied by anincrease in the number of polaron occupying the
conduction band (CB). The author wishes the
Mössbauer spectroscopy to be actively utilized forthe resource and energy development.
2B05: Crystal structures and Mössbauer spectraof ZrO2–LnO1.5 (Ln = Dy, Yb) and CeO2–GdO1.5

solid solutions
TAKAHASHI, M.1, IMAI, K.1, MATSUKAWA, S.1,
YAMAMOTO, E.2, NAKAMURA, A.2(1Dep. of Sci., Toho Univ., 2Adv. Sci. Res. Cent.,
JAEA)
PowderX-ray
diffraction(XRD)
measurements of Zr1-yLnyO2–y/2 (Zr–Ln; Ln = Dy,
Yb), prepared by a calcination at 1450 °C, show that
Zr–Dy system forms a disordered defect-fluorite (F)phase (0.12 ≤ y ≤ 0.65) and C-phase (0.80 < y), whileδ-phase (Zr3Yb4O12) appears as mixed phases in the
middle range (0.42 ≤ y ≤ 0.80), sandwiched with
F-phase (0.10 ≤ y ≤ 0.42) and C-phase (0.8 < y). In
Ce–Gd system, only single phases, F- ( y ≤0.30) andC-phase ( 0.30 < y), are found. 155Gd Mössbauer
spectra of Ce-Gd system show that Gd3+ ions in
C-phase occupy 24d site, oxygen defects (VO)occuping face-diagonally in an octant, preferentiallyto the 8b site, VO’s at body-positions, and theiroccupancies increase rapidly with decreasing y from
1.0 to 0.50, and local structures become almost thesame as those of F-phase below y = 0.50. The
distortion of 8b site increases with increase in Ce
content (from y = 1.0 to 0.50), while symmetry of
24d site increases gradually.
2B06: Observation of local fields in a perovskite
La0.7Ca0.3MnO3SATO, W.1, MINAMI, D.2, OSA, A.3, SATO, T. K.3,
OHKUBO, Y.4(1Inst. Sci. Eng., Kanazawa Univ., 2Grad. School
Sci. Tech, Kanazawa Univ., 3Japan Atomic Energy
Agency, 4Res. Reactor Inst., Kyoto Univ.)
Perovskite manganese oxides are known to
exhibit the effect of colossal magnetoresistance(CMR), a phenomenon that electrical resistivity
undergoes a drastic change as large as five to six
orders of magnitude by the magnetic transition.
Because of this unique physical property, muchattention has been given to these oxides aiming at
wide industrial applications. In order to realize
practical use of these compounds, it is of importanceto obtain information on local fields in the material
as well as macroscopic quantities such as resistivity
and magnetization. From this point of view, wehave applied the time-differential perturbed angularcorrelation (TDPAC) method to a study of a
Powderperovskite La0.7Ca0.3MnO3 (Tc~245 K).

− 195 −

La0.7Ca0.3MnO3 was synthesized by a conventional
solid-state reaction in air. For the introduction of
the parent nuclides of the 111Cd probe into the sample,
twodifferent
ways
were
adopted:anion-implantation method and a chemical synthesis.
After the introduction of the parent nuclides, thesample was annealed at 1473 K and TDPAC
measurements were performed.
The TDPAC
spectra suggest that the majority of the probe atoms
reside in a unique site. In the presentation, thetransferred field from Mn ions at the probe nucleus isdiscussed based on the temperature dependence ofthe spectra.
2B07: Activity ratio of 210Pb/226Ra in the volcanic
products

has been actually used for measuring sedimentation
rates of lake and coastal sediments. The objectives ofthis study are to measure the vertical distributions of210
Pb concentrations in precious corals and to
estimate the radial growth rate. The radial growthrate of the skeleton can be estimated by the gradualdecreases in 210Pb concentrations measured from thesurface inwards. The radial growth rate of the redcoral skeleton is estimated to be 0.22 mm/year, so
slow that it would take as long as 50 years for acolony to grow to 22 mm in diameter.
2B09: Nuclear reaction rates for nucleosynthesisof the p-nucleus Sm-146
KINOSHITA, N.1, MORITA, Y. 2, YOKOYAMA, A.
, HAMAJIMA, Y. 3, MASUMOTO, K. 4,
YASHIMA, H. 5, SEKIMOTO, S. 5, HIROSE, K. 6,
OHTSUKI, T. 6, TAKAHASHI, N. 7, PAUL, M. 8
(1Tandem Accel. Complex, Univ. of Tsukuba, 2Inst.
Sci. Tech., Kanazawa Univ., 3LLRL, Kanazawa Univ.,
4
Radiat. Res. Center, KEK. 5KUR, Kyoto Univ., 6Res.
Center. Electron Photon Sci., Tohoku Univ., 7Grad.
School Sci., Osaka Univ., 8Racah Inst., Hebew Univ.)
2

KURIHARA, Y.1, 2, KOIKE, Y.2, SATO, J.3(1Org. Strategic Coordinat. Res. Intellect. Prop.,
Meiji Univ., 2RIC, Univ. of Tokyo, 3Meiji Univ.)
Observations were carried out on the activity
ratio of 210Pb/226Ra in the products from Unzen (1993
AD eruption), Sakura-jima (1779 AD, 1946 AD,
1976 AD, 1977 AD and 1978 AD eruptions) and
Izu-Oshima (1421 AD eruption) volcanoes, Japan.
Measurement of 210Pb/226Ra activity ratio in thesamples was made by gamma-ray spectrometry.
The 210Pb/226Ra activity ratio in the samples ranged
from 0.9 to 3.7. It is suggested that the 210Pb/226Ra< 1 (210Pb deficits) in the samples result from thecontinuous degassing of 222Rn, a precursor of 210Pb in
the decay series, from the shallow magma chamber.
On the other hand, the 210Pb/226Ra > 1 (210Pb
excesses) in the samples are often attribute to theaccumulation of 222Rn in the magma chamber. The
samples with large 210Pb excesses, however, have anobservable amount of 137Cs, which indicates thecontamination of the deposition of atmospheric 210Pb.
2B08: Determination of the growth rate ofprecious corals using the natural radionuclide
YAMADA, M.1, IWASAKI, N.2, SUZUKI, A.3,
ZHENG, J.1(1Environ. Rad. Effects Res. Group, Natl. Inst.
Radiol. Sci., 2Kochi Univ., 3GSJ, AIST)
Lead-210 is a naturally occurring radionuclideof the U-238 decays series with a half-life of 22.3
years. 210Pb is a natural marker suitable for dating
events that have occurred over the past 100 years and

The p-nuclei are not able to be produced fromneutron capture process because they are neutron
deficient. They are supposed to be produced in the
network reaction including emission of neutron or
capture of proton above temperature of 1×109 K. We
focus on the Sm-146 isotope, which was abundant in
the early history of the solar system, from view pointof the astrophysical nucleosynthesis. There are somepossible paths to synthesize the isotope through147
Sm(γ,n), 147Sm(γ,pβ ), and 146Nd(p,nβ ), etc. We
have measured cross sections of 147Sm(γ,n)146Sm and147
Sm(γ,p)146Pm and 146Nd(p,n)146Pm to investigate
the paths and the 146Sm production rate of each path.
The isotopes of 146Sm and 146Pm produced in
bremsstrahlung irradiation and proton irradiation
were measured by gamma spectrometry andaccelerator mass spectrometry to obtain the crosssections.
As a results, we determined the cross sections
146
Nd(p,n)146Pm down to 3.5 MeV. The crossofsections of this work are compared with theoretical
calculation using the NON-SMOKER code for each
incident energy and used to estimate astrophysicalreaction rate. The data are useful to discuss thesynthesis path to the 146Sm isotope from comparison
betweenastrophysicalreaction
rates
of
146
146
Sm(γ,n)146Sm,
Sm(γ,p)146Pm,
and− 196 −

−

−

146

Nd(p,n)146Pm.

2B10: Study on transport of dissolved organic
matter in the Tokachi River system
NAGAO, S.1, FUJITAKE, N.2, TANAKA, T.1,
ARAMAKI, N.3, KODAMA, H.4, YAMAMOTO, M.
1, UCHIDA, M. 3, SHIBATA, Y. 3
(1LLRL, Kanazawa Univ., 2Grad. School of Agr. Sci.,
Kobe Univ., 3Chem. Division, NIES, 4Anal. Res.
Center, Saga Univ.)

Humic substances are the largest fraction ofdissolved organic matter in natural waters and consistof humic (HA) and fulvic acids (FA). The
characteristics of aquatic HA and FA are important tounderstand the sources and dynamics of aquatic
humic substances in river systems. This study reports
the downward trend in ∆ 14C and δ13C of dissolved
HA and FA isolated from river waters along theTokachi River, which is located in Hokkaido Island
in Japan. The HA and FA were isolated from the riverwaters at three stations from the upper to lower
Tokachi River using the XAD extraction method in
2003-2005. Stable carbon isotopic ratio is
determined by mass spectrometry and is reported inδ13C notation versus the VPDB standard.
Radiocarbon in humus samples was determinedusing accelerator mass spectrometry at the JAEA and
NIES. The ∆ 14C and δ13C values of FA are younger
and lighter than those of HA. The ∆ 14C of fulvic
acids decrease from +22‰ in the upper site to –58‰
in the lowest site. The downward trend is similar
with that of HA. These results suggest that the supplyof older HA and FA from watershed increase
downward along the Tokachi River.
3B01: Radiocarbon age, calligraphical style andkiwamefuda certificate of kohitsugire calligraphy
ODA, H.1, IKEDA, K.2, YASU, H.3(1Center for Chronological Res., Nagoya Univ.,
2
Faculty of Letters, Chuo Univ., 3Taga High School.)Radiocarbon ages of wooden samples
generally disagree with their archaeological or
historical ages mainly because the samples madefrom long-lived species or seasoned wood indicate
old radiocarbon ages. Although Japanese paper isalso wooden sample, it was made from branchesof shrubs. Old paper is seldom used for
calligraphy because it repels India ink and is

unsuitable for elegant handwriting. Therefore,
it can be considered that Japanese paper is asuitable sample for radiocarbon dating. In thisstudy, we measured radiocarbon ages of ancientJapanese calligraphies called kohitsugire anddocuments of known age. The results
demonstrated that the radiocarbon ages
correspond to the years in which they were
written. Most of kohitsugire have traditional
certificates (called kiwamefuda) which identify thecalligraphists. Paleographical study, however, showsthat there are some kohitsugire whose calligraphicalstyles are incompatible with the descriptions of the
kiwamefuda certificates, for example, kohitsugire
attributed to Nakatoni no Kamatari (614-669) by the
kiwamefuda seems to be written in the 10th – 14th
century, and kohitsugire attributed to Prince
Munetaka (1242–1274) has a calligraphical style ofthe 11th century. Therefore, in this study, we applied
radiocarbon dating to these kohitsugire. Theirradiocarbon ages corresponded to the paleographicalages and suggested that kiwamefuda does notnecessarily agree with the years in which thecalligraphy was written.
3B02: Measurements of 36Cl/Cl in soil by using
multi-step extractions
AMANO, T.1, SUEKI, K.1, TAMARI, M.1,
KITAGAWA, J.1, SASA, K.2, NAGASHIMA, Y.2,
TAKAHASHI, T.2, KINOSHITA, N.2, KUROSUMI,
K.2, TOSAKI, Y.3, MATSUSHI, Y.4, BESSHO, K.5,
MATSUMURA, H.5(1Grad. School of Pure and Applied Sci., Univ. of
Tsukuba, 2AMS Group, Tandem Accel. Complex,
Univ. of Tsukuba, 3Crustal Fluid RG, GSJ, AIST,
4
Mt. Haz. Sec., Geo Dis. Div., DPRI, Kyoto Univ.,
5High Ener. Accel. Res. Organ.)
Chlorine in soil is present in various chemical
forms. From our previous studies, it has been
confirmed that depth profiles of 36Cl/Cl isotopic
ratios for chlorides which have higher fluidity
underground show maximum around surface layer.
In this work, we tried to investigate the relationshipbetween several types of chlorine which was
supplied from different reservoirs. The following
extraction methods were carried out with surface
soils of several sites and 36Cl/Cl isotopic ratio of eachsample was measured with accelerator mass
spectroscopy (AMS) at UTTAC;
A) Chlorides were extracted with dilute nitric acid− 197 −

(inorganic soluble phase).
B) Organochlorines were resolved with hydrogen
peroxide after acid extraction (organic phase).
C) Chlorine in minerals was taken out by combustion
from residue (mineral phase).
It was found that some sort of interaction between
chloride and organochlorine in soil was consideredfrom the 36Cl/Cl ratio. On the other hand, the 36Cl/Cl
ratio in mineral phase showed features different fromsoluble and organic phase. There might be anotherprocess on existing in mineral phase which isdifferent from soluble and organic phase.
3B03: Studies on the secular variation of 129I/127I
ratios in the atmospheric fallout in Tokyo andAkita using AMS
Toyama, C.1, Uchida, Y.1, Ito, E.1, Muramatsu, Y.1,
Igarashi, Y.2, Matsuzaki, H.3(1Gakushuin University, 2Meteorological ResearchInstitute, 3The University of Tokyo)
Iodine-129 is one of the most importantradionuclides in environmental safety. In this study,
we have developed an appropriate separation
procedure of iodine from atmospheric fallout
samples for determining 129I/127I ratios by accelerator
mass spectrometry (AMS). Samples used in thisstudy were collected from Tokyo and Akita from1963 to 2003 by Meteorological Research Institute.
The analytical results showed that the secularvariation of 129I/127I ratios in the atmospheric fallout
was different from that of 90Sr and 137Cs. Thissuggested that the variation of 129I/127I ratios observed
was not due to the nuclear bomb tests. High 129I/127I
ratios (up to 8×10-8) found after 1980 indicate that
contribution from the other sources (e.g. possibly
from nuclear spent fuel reprocessing plants) might beimportant to understand the increase of the ratios.
Moreover, an increasing tendency of 127I in theatmospheric fallout with time was observed, of
which reason is still unknown.
3B04: Determination of iodine in estuarine biota
by ICP-OES
FUJITA, K.1, SHIRASAKA, J.2, TAGAMI, K.1,
UCHIDA, S.1(1National Institute of Radiological Sciences,
2
Tokyo Nuclear Services Co.)
Some marine biota are known as iodine

accumulators, and thus they could also absorb along-lived radioiodine (iodine-129) released to themarine environment. However, not all marine biota
contain high amount of iodine. In this study,
estuarine biota samples were used to develop a
simple iodine measurement method. A 0.1-g portionof each sample was weighed in a PFA vial, andMilli-Q water and Tetramethylammonium hydroxide(TMAH) were added. The mixture was heated at 60
˚C for 15h and then diluted with Milli-Q water.
Finally, iodine in the solution was measured byinductively coupled plasma optical emission
spectroscopy (ICP-OES).
There are three major wavelengths for iodine;
however nitrogen and phosphorus have neighboringlines to two wavelengths of iodine. Therefore
182.976 nm was selected for an optimum wavelengthfor iodine analysis. The detection limit of the present
method was 150 mg/kg when a 0.1-g of sample
powder was used. The results for a standard
reference material (NIES No. 9, reference value: 520
mg/kg) obtained by this method showed a good
agreement (544±44 mg/kg). This method could be
successfully applied to determination of iodine inestuarine biota.
3B05: Application of 85Kr dating to groundwaterin Kumamoto Area, JapanMOMOSHIMA, N1., INOUE, F.2, SUGIHARA, S.1,
SHIMADA, J.3, ONO, M.3, IKAWA, R.4, KAGABU,
M.3, YAMAGUCHI, K.5, OHTA, T.6, MAHARA,
Y.6, TANIGUCHI, M.7(1Radioisotope Center, Kyushu Univ., 2Grad. Schoolof Sci., Kyushu Univ., 3Grad. School of Sci. andTech., Kumamoto Univ., 4Fac. Sci., Kumamoto
Univ., 4Groundwater Res. Group, Geol. Surv. Jpn.,
6
Res. Reactor Inst., Kyoto Univ., 7Res. Inst.
Humanity Nature)
Groundwater age was determined by 85Kr/Kr
specific activity of gases dissolved in groundwater at
Kumamoto Area, in which newly developed Kr
extraction system and liquid scintillation counting
technique for 85Kr were applied. Apparent mean
residence times observed were 8.2 ± 0.7 y and 20.7 ±0.6 y for the groundwater taken from a well at
recharge area and that from an artesian borehole atthe discharge area, respectively showing a consistent
age trend estimated from the observed groundwaterflow system of Kumamoto Area and also that
determined using environmental tritium. Similar− 198 −

mean residence time of 85Kr and tritium wasobserved at the discharge area but the mean
residence time of 85Kr at the recharge area wasyounger compared to that of tritium, probably due tomixing of river water containing recent high 85Kr
concentration in this region into groundwater flow
coming from the northern upland’s recharge area.
The mean residence time of the groundwater flow
coming from northern upland area and a travelingtime of the groundwater between two sampling
points were estimated by a simple model assuming
mixing the river water with the groundwater and apiston flow between two sampling points.
3B06: An approach toward identification ofradioxenon sources for nuclear explosion
verification
YONEZAWA, C.1, ODA, T.2, YAMAMOTO, Y.2(1Center for the Promotion of Disarmament and
Non-Proliferation, Japan Institute of International
Affairs, 2Nuclear Non-Proliferation Science andTechnology Center, Japan Atomic Energy Agency)
Radioxenon  nuclides including 131mXe,
133m
Xe, 133Xe and 135Xe have been used for detectionof nuclear explosion, because these nuclides can beeasily leaked out from even underground due to theirlarge fission yield and inert chemical property.
Twenty seven radioxenon monitoring stations havebeen installed in the world including Takasaki, Japan,
to detect the nuclear explosion as a verification
system of the Comprehensive Nuclear-Test-Ban
Treaty (CTBT). Irrelevant radioxenon to the nuclear
explosion has been occasionally detected at themonitoring stations, which makes difficult todistinguish from the nuclear explosion. These areconsidered as the radioxenon sources: nuclear power
and research reactors; spent fuel reprocessing
facilities; nuclear particle accelerators; hospitals;
natural background from lithosphere; and flow fromoversea. We estimate annual discharged radioxenon
activities of each emission source, except for theflow from oversea, using published information andevaluate the radioxenon counts of the Takasaki
monitoring
station.
An
approachtowardidentification of radioxenon sources using
atmospheric transportation modeling and radioxenon
emission data is also presented.
3B07: Separation of Ba and Ra using thedifference of their adsorption to manganesedioxideHINAMI, S.1, SATO, W.2, YOKOYAMA, A.2,
NAKANISHI, T.2(1Grad. School Nat. Sci. Tech., Kanazawa Univ.,
2Inst. Sci. Eng., Kanazawa Univ.)
In general, the quantitative determination ofradium in water sample is carried out by gamma-ray
measurementsof
precipitate
obtainedbycoprecipitation of radium with barium sulfate.
Barium reagents usually contain some amount ofradium. Therefore the use of barium reagent islimited due to the interference of radium in thebarium reagent. In this work, we have investigated
the separation of radium from barium reagent using
the difference of adsorption properties of barium andradium cations to manganese dioxide. The adsorption
rate and the distribution ratio for the elements showthat manganese dioxide adsorbs radium cations in
preference to barium cations and that the adsorptionof barium and radium cations follows the
stoichiometric ion-exchange mechanism.
3B08: Plating method of Po from acid solutions
onto a stainless-steel disk
UESUGI, M.1, YOKOYAMA, A.2, NAKANISHI,
T.2(1Grad. School Nat. Sci. Tech., Kanazawa Univ., 2Inst. Sci. Eng., Kanazawa Univ.)
A plating method has been devised for trace
amounts of polonium (Po) from acid solutions withhigh yield onto a stainless-steel disk. The conditions
for effective deposit of Po were examined for anelectrodeposition method other than the spontaneousdeposition method. In this work, 209Po isotope wasadded to electrolysis solutions, and Po recovery wasmeasured under various conditions such as platingtime, electrolysis current, temperature, major anion
species, and co-presence of other metal-ions. It was
found that the electrodeposition method provided agood recovery and selectivity from HCl (0.5-6 M),
HNO3 (0.5-2 M), H2SO4 (0.5-6 M) and H3PO4 (0.5-6M) solutions. The optimized conditions for Po
deposition were 0.2-0.3A (~100 mA/cm2) inelectrolysis current, plating for 2 hours in room
temperature. Besides, interfering ions were notdeposited in acid solutions over 0.5 M. The
electrodeposition of Po from acid solution is
concluded to be more effective and rapid, than the− 199 −

spontaneous deposition.
3B09: Optimization of Automated Sequential
Anion-Exchange Separation of Ultra-trace
Elements
MIYAMOTO, Y., YASUDA, K., MAGARA, M.,
KIMURA, T.
(Nuclear Science and Engineering Directorate,
JAEA)
From these ratios of trace U, Th, Pb andlanthanides in an environmental sample, information
on origin and history of the sample can be obtained.
The key elements should be separated from theco-existing and interfering elements in a sample toanalyze accurately the abundance and isotopic ratiosof the key elements by ICP-MS. The sequential
separation technique of these elements with a single
anion-exchange column has been developed. In thiswork, the pressurized sequential separation systemwith compressed air, a switching valve, and Teflon
tubes was examined to make up an automatedseparation system. An eluent in a Teflon tube wasintroduced to an anion-exchange column withpressurized air. The eluents were changed by aswitching valve. The separation was optimized forsome parameters including the flow rate of eluentsand the composition of eluents. The mixture of
CH3COOH and HNO3 was effective for the
separation of Fe from U. The composition of 65
vol.% CH3COOH and 1M HNO3 was the best for the
separation. This pressurized separation system
improved the resolution of separation peaks andreduced the separation time compared with theprevious gravity flow separation.
3B10: Development of elemental and isotopic
analyses of uranium, thorium, and macro
elements in the environment using an automaticSPE
injectionequipment
coupledto
ICP-DRC-MS
SAKAMA, M.1, SAZE, T.2, KITADE, T.3,
SHIKINO, O.4(1 School Health Sci., Univ. Tokushima, 2 RIC, Univ.
Tokushima, 3 M&S Instruments Inc., 4 PerkinElmer
Japan Co., Ltd.)Beginning in FY2009, funding for theequipment cost of ICP-MS analytical system wasallowed to insert it in the budget of The University ofTokushima. The aim of equipping this new system is
to educate the undergraduate students in the
Department of Radiologic Science to understand andtrain advanced elemental and isotopic analyses,
which are also available for their graduation
researches on radiologic sciences. In addition, thissystem also will be effectively shared among
biomedical researchers who are with faculties of
medicine, dentistry, and pharmaceutical sciences at
Kuramoto Campus in The University of Tokushima.
In particular, the present ICP-MS analysis will be
expected to contribute to measure quantitatively trace
and macro amounts of metal elements (metallomics)
relative to environmental radioactivity, biology,
medicine, and so on. Until now, we have developed
the integrated analysis system carried out fromdecomposing various samples, to isolate target
elements automatically by a SPE (Solid Phase
Extraction) method, and to measure their signal
intensities quantitatively mass-separated using an
unique ICP-DRC-MS (Dynamic Reaction Cell) type.
In this presentation, we have reported theexperimental condition under this development.
3B11: Feasibility of using globalfallout 236U toconstruct the circulation of seawater
SAKAGUCHI, A. 1, YAMAMOTO, M. 2,
KADOKURA, A. 1, YOSHIDA, K. 2, STEIER, P. 3
(1Grad. School of Sci., Hiroshima Univ., 2LLRL,
Kanazawa Univ., 3VERA, Univ. of Vienna)
The global fallout 236U (Τ =2.342×107 y,
α-decay) level in soil was deduced frommeasurements of 236U, 239+240Pu and 137Cs in surface
soils which are solely influenced by global fallout. A
total of 12 soil cores from the depths of 0-10, 0-20
and 0-30 cm were collected at a flat forest area inJapan. Concentrations of 239+240Pu and 238U were
determined by α-particle spectrometry, while the236
U/238U ratio was measured with accelerator mass
spectrometry (AMS). Consistent 236U/239Pu ratios
between 0.212 to 0.253 were found. Using this ratio,
the total global fallout of 236U on the earth isestimated to be as much as ca. 900 kg. Thisknowledge will contribute to the promotion ofresearch on U isotopes, including 236U, for the fieldsofgeo-resources,waste
managementandgeochemistry. The application of global fallout 236U
to the water circulation in the "miniature ocean",Japan sea, will be discussed in our presentation.

− 200 −

1/2

3B12: Uptake of Uranium by Spinach Plants
after Application of Elevated Amount of
Phosphatic Fertilizers to Upland Field Soil
MORIKAMI, Y.1, NOBUMORI, T.1, TAGAMI, K.2(1Okayama Prefectural Institute for Environmental
Science and Public Health, 2National Institute ofRadiological Sciences)
Phosphatic fertilizers made from phosphaterocks usually contain high amounts of uranium sothat it is sometimes listed as naturally occurring
radioactive materials (NORM). It would be possiblethat plant can absorb U from this type of fertilizer
just after its application to agricultural soils because
U in the fertilizer may be more mobile than thatoriginated from soil. In order to clarify the effect ofphosphatic fertilizer application for U uptake byagricultural crops from soil, we cultivated spinach
plants on six different fertilizer concentration fields
in Okayama city. Concentrations of U in the plant atharvest, and those in soil samples for several times
during planting period were measured. We found thatconcentrations of U in spinach samples and those of
the extract from the soil with water were wellcorrelated. Also, concentrations of U and Al inspinach were highly correlated. From these results, it
was implied that spinach plants would absorb watersoluble U with water through roots.

contaminated by uranium originating from fertilizers,
whereas the low ratios occur in lithogenic materials.
Therefore, the 230Th/232Th ratios in deposition allow
us to separate local and remote fractions of thethorium deposition. The results reveal that both local
and remote fractions of the thorium deposition
showed seasonal variations with high in spring
although the remote fraction is dominant withinseason. The local 232Th deposition showed a smaller
peak in early spring, corresponding to local dust
storm event.

3B13: Thorium deposition observed at Tsukuba
HIROSE, K.1, KIKAWADA, Y.1, IGARASHI, Y.2(1Facul. Sci. & Tech. Sophia Univ., 2Geochem. Res.
Dep, Meteor. Res. Inst.)
Monthly depositions of thorium isotopes at
Tsukuba, Japan during the period 1990-2007 were
determined. The monthly 232Th deposition showed atypical seasonal variation with inter-annual
variability. Especially, a marked peak of the 232Th
deposition as did 239,240Pu occurred in spring. The
seasonal change of the monthly 232Th deposition isclosely related to those of the Kosa events. Highmonthly depositions of thorium in spring might
originate from soil particles, as did 239,240Pu.
However, the inter-annual variation of the annual232
Th deposition did not coincide with that of theKosa event frequency. The 230Th/232Th activity ratios
in deposition samples showed large variability; its
higher ratios were observed in early spring. The
higher 230Th/232Th ratios reflect local soils− 201 −