Study on Tc separation/concentration technology from Mo by (n, ) method, 2

Fujita, Yoshitaka; Hu, X.*; Yang, Y.*; Kitagawa, Taiga*; Fujihara, Yasuyuki*; Yoshinaga, Hisao*; Hori, Junichi*; Do, T. M. D.*; Suzuki, Tatsuya*; Suematsu, Hisayuki*; et al.

KURNS Progress Report 2023, P. 122, 2024/07

no abstracts in English

-MoO whiskers in Mo/Tc radioisotope production and Mo/Tc extraction using hot atoms

Ngo, 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

https://doi.org/10.1021/acs.inorgchem.3c02125

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.

Radiochemical research for the advancement of Mo/Tc generator by (n, ) method, 4

Fujita, 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

https://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2021/ProgressReport2021_online.pdf#page=134

no abstracts in English

Dynamic properties on Mo adsorption and Tc elution with alumina columns

Fujita, 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

BB2021-0617.pdf:0.77MB

https://doi.org/10.1088/1742-6596/2155/1/012018

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 AlO 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.

Two-step-pressurization method in pulsed electric current sintering of MoO for production of Tc radioactive isotope

Suematsu, 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

https://doi.org/10.1080/21870764.2020.1824326

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 550C 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.

Preparation of potassium and metakaolin based geopolymer foam with millimeter sized open pores for hydrogen recombining catalyst supports

Utsumi, Taro*; Terasawa, Toshiharu*; Kudo, Isamu*; Suzuki, Tsuneo*; Nakayama, Tadachika*; Suematsu, Hisayuki*; Ogawa, Toru

Journal of the Ceramic Society of Japan, 128(2), p.96 - 100, 2020/02

https://doi.org/10.2109/jcersj2.19175

A method to control the millimeter-sized open porosity in geopolymer foam was attempted to produce hydrogen recombining supports for radioactive waste canisters. The raw materials were mixed with silicon powder as a foaming agent. Geopolymer foams with open porosities as high as 81% were obtained by a water bath treatment before pouring the slurry into the mold. The increase in the open porosity of geopolymer foam was observed by an increase in the water bath treatment time. It was thought that the viscosity of slurry increase induced the pores trapped inside the geopolymer foam and connected to form millimeter-sized and open pores. It was concluded that a simple method with a foaming agent and a water bath treatment to prepare geopolymer foams with high open porosity was developed.

Characterization of ZrN, ZrO and '-ZrON nanoparticles synthesized by pulsed wire discharge

Lam, Do Van*; Suematsu, Hisayuki*; Ogawa, Toru

Journal of the American Ceramic Society, 100(10), p.4884 - 4892, 2017/10

https://doi.org/10.1111/jace.15012

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.

Pulsed electric current sintering of MoO and the neutron irradiation tests

Suematsu, 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.

Spark plasma sintering of MoO for production of Tc by neutron irradiation

Suematsu, 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 0.8m 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.

Porosity control of multifunction geopolymer foam

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.