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Mo hot atoms made by a neutron capture method from 
-MoO
to waterQuach, N. M.*; Ngo, M. C.*; Yang, Y.*; Nguyen, T. B.*; Nguyen, V. T.*; Fujita, Yoshitaka; Do, T. M. D.*; Nakayama, Tadachika*; Suzuki, Tatsuya*; Suematsu, Hisayuki*
Journal of Radioanalytical and Nuclear Chemistry, 332(10), p.4057 - 4064, 2023/10
Times Cited Count：0 Percentile：0.01(Chemistry, Analytical)Technetium-99m (
Tc) is the most widely used medical radioisotope in the world and is produced from molybdenum-99 (Mo). Production of Mo via the neutron capture method draws attention as an alternative to fission-derived Mo due to non-proliferation issues, but the specific radioactivity of Mo is extremely low. In this work, a porous -MoO wire was prepared as an irradiation target in order to improve the specific activity by extracting Mo. Porous -MoO wire is synthesized from Mo metal wire by a two-step heating procedure. The hot atom effect of Mo was confirmed by activity and isotope measurements of the porous -MoO wire after neutron irradiation and the water used for extraction. In term of the extraction effectiveness, the effectiveness of Mo extraction in the porous -MoO wire was comparable to that of commercial -MoO powder.
-MoO whiskers in Mo/
Tc radioisotope production and Mo/Tc extraction using hot atomsNgo, M. C.*; Fujita, Yoshitaka; Suzuki, Tatsuya*; Do, T. M. D.*; Seki, Misaki; Nakayama, Tadachika*; Niihara, Koichi*; Suematsu, Hisayuki*
Inorganic Chemistry, 62(32), p.13140 - 13147, 2023/08
Times Cited Count：0 Percentile：0.01(Chemistry, Inorganic & Nuclear)Technetium-99m (Tc) is one of the most important radioisotopes for diagnostic radio-imaging applications. Tc is a daughter product of the Mo isotope. There are two methods used to produce Mo/Tc: the nuclear fission (n,f) and the neutron capture (n,
) methods. Between them, the (n,f) method is the main route, used for approximately 90% of the world's production. However, the (n,f) method faces numerous problems, including the use of highly enriched uranium, the release of highly radioactive waste, and nonproliferation problems. Therefore, the (n,) method is being developed as a future replacement for the (n,f) method. In this work, -MoO whiskers prepared by the thermal evaporation method and -MoO particles were irradiated in a nuclear reactor to produce Mo/Tc via neutron capture. The irradiated targets were dispersed into water to extract the Mo/Tc. As a result, -MoO whisker yielded higher Mo extraction rate than that from -MoO. In addition, by comparing the dissolved 
Mo concentrations in water, we clarified a prominent hot-atom of -MoO whiskers. This research is the first demonstration of -MoO being used as an irradiation target in the neutron capture method. On the basis of the results, -MoO is considered a promising irradiation target for producing Mo/Tc by neutron capture and using water for the radioisotope extraction process in the future.
Tc separation/concentration technology from Mo by (n, ) methodFujita, Yoshitaka; Hu, X.*; Takeuchi, Tomoaki; Takeda, Ryoma; Fujihara, Yasuyuki*; Yoshinaga, Hisao*; Hori, Junichi*; Suzuki, Tatsuya*; Suematsu, Hisayuki*; Ide, Hiroshi
KURNS Progress Report 2022, P. 110, 2023/07
no abstracts in English
Mo/Tc generator by (n, ) method, 4Fujita, Yoshitaka; Seki, Misaki; Ngo, M. C.*; Do, T. M. D.*; Hu, X.*; Yang, Y.*; Takeuchi, Tomoaki; Nakano, Hiroko; Fujihara, Yasuyuki*; Yoshinaga, Hisao*; et al.
KURNS Progress Report 2021, P. 118, 2022/07
no abstracts in English
Fujita, Yoshitaka; Niizeki, Tomotake*; Fukumitsu, Nobuyoshi*; Ariga, Katsuhiko*; Yamauchi, Yusuke*; Malgras, V.*; Kaneti, Y. V.*; Liu, C.-H.*; Hatano, Kentaro*; Suematsu, Hisayuki*; et al.
Bulletin of the Chemical Society of Japan, 95(1), p.129 - 137, 2022/01
Times Cited Count：8 Percentile：76.16(Chemistry, Multidisciplinary)In this work, the mechanisms responsible for the adsorption of molybdate ions on alumina are investigated using in-depth surface analyses carried out on alumina specimens immersed in solutions containing different molybdate ions at different pH values. The obtained results reveal that when alumina is immersed in an acidic solution containing molybdate ions, the hydroxyl groups present on the surface are removed to generate positively charged sites, and molybdate ions (MoO
or AlMo
O
H
) are adsorbed by electrostatic interaction. Alumina dissolves slightly in an acidic solution to form AlMoOH, which is more easily desorbed than MoO. Furthermore, the enhancement in the Mo adsorption or desorption property may be achieved by enriching the surface of the alumina adsorbent with many -OH groups and optimizing Mo solution to adsorb molybdate ions on alumina as MoO ions. These findings will assist researchers in engineering more efficient and stable alumina-based adsorbents for molybdenum adsorption used in medical radioisotope (Mo/Tc) generators.
Mo adsorption and Tc elution with alumina columnsFujita, Yoshitaka; Seki, Misaki; Sano, Tadafumi*; Fujihara, Yasuyuki*; Suzuki, Tatsuya*; Yoshinaga, Hisao*; Hori, Junichi*; Suematsu, Hisayuki*; Tsuchiya, Kunihiko
Journal of Physics; Conference Series, 2155, p.012018_1 - 012018_6, 2022/01
Technetium-99m (Tc), the daughter nuclide of Molybdenum-99 (Mo), is the most commonly used radioisotope in radiopharmaceuticals. The research and development (R&D) for the production of Mo by the neutron activation method ((n, ) method) has been carried out from viewpoints of no-proliferation and nuclear security, etc. Since the specific activity of Mo produced by the (n, ) method is extremely low, developing Al
O with a large Mo adsorption capacity is necessary to adapt (n, )Mo to the generator. In this study, three kinds of AlO specimens with different raw materials were prepared and compared their adaptability to generators by static and dynamic adsorption. MoO pellet pieces (1.5g) were irradiated with 5 MW for 20 min in the Kyoto University Research Reactor (KUR). Irradiated MoO pellet pieces were dissolved in 6M-NaOH aq. In dynamic adsorption, 1 g of AlO was filled into a PFA tube (
1.59 mm). The Mo adsorption capacity of AlO specimens under dynamic condition was slightly reduced compared to that under static condition. The Tc elution rate was about 100% at 1.5 mL of milking in dynamic adsorption, while it was around 56-87% in static adsorption. The Mo/Tc ratio of dynamic condition was greatly reduced compared to that of static condition. Therefore, the Tc elution property is greatly affected by the method of adsorbing Mo, e.g., the column shape, the linear flow rate, etc.
Mo/Tc generator by (n, ) method, 3Fujita, Yoshitaka; Seki, Misaki; Namekawa, Yoji*; Nishikata, Kaori; Daigo, Fumihisa; Ide, Hiroshi; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; Hori, Junichi*; et al.
KURNS Progress Report 2020, P. 136, 2021/08
no abstracts in English
for production of Tc radioactive isotopeSuematsu, Hisayuki*; Sato, Soma*; Nakayama, Tadachika*; Suzuki, Tatsuya*; Niihara, Koichi*; Nanko, Makoto*; Tsuchiya, Kunihiko
Journal of Asian Ceramic Societies (Internet), 8(4), p.1154 - 1161, 2020/12
Times Cited Count：3 Percentile：17(Materials Science, Ceramics)Pulsed electric current sintering of molybdenum trioxide (MoO) was carried out by one- and two-step pressuring methods for fabrication of irradiation target using production of Mo and Tc nuclear medicine. At 550
C by the two-step pressurizing method, a relative density of 93.1% was obtained while, by the one-step pressurization method, the relative density was 76.9%. Direct sample temperature measurements were conducted by inserting a thermocouple in a punch. By the two-step pressurizing method, the sample temperature was higher than that by the one-step pressurizing method even almost the same die temperature. From voltage and current waveforms, it was thought that the conductivity of the sample increased by the two-step pressurizing method to increase the sample temperature and the relative density. The two-step pressurization method enables us to prepare dense targets at a low temperature from recycled and coarse-grained Mo enriched MoO powder.
Mo/Tc generator by (n,) method, 2Fujita, Yoshitaka; Seki, Misaki; Namekawa, Yoji*; Nishikata, Kaori; Kato, Yoshiaki; Sayato, Natsuki; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; Hori, Junichi*; et al.
KURNS Progress Report 2019, P. 157, 2020/08
no abstracts in English
Mo/Tc generator by (n,) methodFujita, Yoshitaka; Seki, Misaki; Namekawa, Yoji*; Nishikata, Kaori; Kimura, Akihiro; Shibata, Akira; Sayato, Natsuki; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; et al.
KURNS Progress Report 2018, P. 155, 2019/08
no abstracts in English
and '-Zr
O
N nanoparticles synthesized by pulsed wire dischargeLam, Do Van*; Suematsu, Hisayuki*; Ogawa, Toru
Journal of the American Ceramic Society, 100(10), p.4884 - 4892, 2017/10
Times Cited Count：2 Percentile：10.4(Materials Science, Ceramics)Nanoparticles of ZrN, ZrO and ZrN, '-ZrON were synthesized by pulsed wire discharge. Morphology and phase analyses were carried out by X-ray diffraction and field-emission transmission electron microscopy (FE-TEM). By bright field image observation, electron energy loss spectroscopy (EELS) and selected area electron diffraction (SAD) analyses, those nanoparticles were separately characterized.
for production of Tc by neutron irradiationSuematsu, Hisayuki*; Sato, Soma*; Nanko, Makoto*; Tsuchiya, Kunihiko; Nishikata, Kaori; Suzuki, Tsuneo*; Nakayama, Tadachika*; Niihara, Koichi*
no journal, ,
Spark plasma sintering of MoO was carried out for production of Tc from Mo by the (n,) method in a nuclear reactor. Powder of MoO with an average grain size of 0.8
m and a purity of 99.99% was pressed in a graphite die with a diameter of 20 mm. Then, the green compact was heated in a spark plasma sintering apparatus with heating rates of 100 
200C/min to 500 600C in vacuum. After holding the temperature for 5 min, the sample was quenched. The sintered samples were characterized by powder X-ray diffraction for phase identifications, electron energy loss spectroscopy for compositional analyses and scanning electron microscopy for grain size measurements. After sintering at 550C, a sintered bulk of MoO with a relative density of 98% was obtained. These properties are good enough for separation of Tc and recycle of Mo.
powder for a radioisotope productionSato, Soma*; Nanko, Makoto*; Suzuki, Tsuneo*; Nakayama, Tadachika*; Suematsu, Hisayuki*; Niihara, Koichi*; Tsuchiya, Kunihiko
no journal, ,
no abstracts in English
for production of radioactive isotopesSuematsu, Hisayuki*; Seki, Misaki*; Sato, Soma*; Nanko, Makoto*; Tsuchiya, Kunihiko; Nishikata, Kaori; Suzuki, Tsuneo*; Nakayama, Tadachika*; Niihara, Koichi*
no journal, ,
no abstracts in English
for Production of Radioactive IsotopesSuematsu, Hisayuki*; Sato, Soma*; Seki, Misaki*; Nanko, Makoto*; Nishikata, Kaori; Suzuki, Yoshitaka; Tsuchiya, Kunihiko; Suzuki, Tsuneo*; Nakayama, Tadachika*; Niihara, Koichi*
no journal, ,
Tc has been utilized as a radioactive isotope in medical applications. The majority of this isotope has been separated from nuclear fission products in testing reactors with highly enriched 
U fuel. However, these reactors have been shut down because of the age and the nuclear security reasons. On the other hand, a nuclear reaction method has been proposed. This method is to irradiate Mo by neutrons in a reactor to form Mo and then to decay to Tc. As the target, MoO pellets are required. However, because of the low evaporation temperature (700 C) and coarse grain size of Mo enriched powder, it was difficult to obtain high density MoO pellets. To overcome this problem, a two-step loading method in pulsed electric current sintering was carried out in this study.
Mo/Tc generator for medicalSeki, Misaki*; Suematsu, Hisayuki*; Nakayama, Tadachika*; Suzuki, Tsuneo*; Niihara, Koichi*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko; Duong Van, D.*
no journal, ,
no abstracts in English
Ogawa, Toru; Utsumi, Taro*; Terasawa, Toshiharu*; Kudo, Isamu*; Suzuki, Tsuneo*; Nakayama, Tadachika*; Suematsu, Hisayuki*
no journal, ,
For the fuel debris management, we develop the preparation techniques for highly porous geopolymer, which would be used as the matrix of neutron absorber as well as hydrogen recombiner. By adding silicon powder to the raw materials, and hot water in mixing, we demonstrated the capability to prepare geopolymer with high fractions of open pores.
and the neutron irradiation testsSuematsu, Hisayuki*; Seki, Misaki; Nakayama, Tadachika*; Nishikata, Kaori; Nanko, Makoto*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko
no journal, ,
Pulsed electric current sintering (PECS) of MoO was carried out for a high density target to produce Tc from Mo in a nuclear reactor. The green compacts of MoO were heated in a PECS apparatus with a heating rate of 100 C/min to 450 - 550 C in vacuum and changing the pressurization profile from 0 to 40 MPa. After two step pressurization for sintering at 550 C, the sintered MoO bulk had a relative density of 94%, which was higher than that of one step pressurization. Direct temperature measurements near the sample were carried out. The results indicated that the sample temperature was higher for the two step than for the one step pressurization even in the same die temperature experiments. By the low pressure in two step pressurization, it was thought that open pores remained in the sintered body to reduce MoO in vacuum. This oxygen depleted MoO
grains showed low electrical resistivity and formed a current path in the sintered body to increase the temperature to increase the relative density.
150C temperature rangeDo, Thi-Mai-Dung*; Nhut, V. L.*; Murakami, Kenta*; Suematsu, Hisayuki*; Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Miradji, F.; Osaka, Masahiko
no journal, ,
The interaction between CsMoO with concrete within the temperature range of 600150C in Ar gas is studied. It seems that there is no reaction between CsMoO aerosol particles with concrete at these temperatures. However, because of the hygroscopic property, CsMoO aerosol particles change to the liquid phase and quickly diffused inside the concrete bulk.
SiO
Do, Thi Mai Dung*; Ngarayana, I.*; Nguyen, H. D.*; Murakami, Kenta*; Suematsu, Hisayuki*; Koide, Manabu*; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
no journal, ,
CsSiO powder was synthesized by wet method using cesium carbonate powder and colloidal silica 40 wt.% suspension in HO as starting materials. The characteristic of CsSiO is investigated by using X-ray diffraction, Raman and Thermogravimetry-differential scanning calorimetry. The structure of CsSiO was analyzed by Transmission Electron Microscope.
