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Journal Articles

Extraction of $$^{99}$$Mo hot atoms made by a neutron capture method from $$alpha$$-MoO$$_{3}$$ to water

Quach, 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:2 Percentile:65.72(Chemistry, Analytical)

Technetium-99m ($$^{99m}$$Tc) is the most widely used medical radioisotope in the world and is produced from molybdenum-99 ($$^{99}$$Mo). Production of $$^{99}$$Mo via the neutron capture method draws attention as an alternative to fission-derived $$^{99}$$Mo due to non-proliferation issues, but the specific radioactivity of $$^{99}$$Mo is extremely low. In this work, a porous $$alpha$$-MoO$$_{3}$$ wire was prepared as an irradiation target in order to improve the specific activity by extracting $$^{99}$$Mo. Porous $$alpha$$-MoO$$_{3}$$ wire is synthesized from Mo metal wire by a two-step heating procedure. The hot atom effect of $$^{99}$$Mo was confirmed by activity and isotope measurements of the porous $$alpha$$-MoO$$_{3}$$ wire after neutron irradiation and the water used for extraction. In term of the extraction effectiveness, the effectiveness of $$^{99}$$Mo extraction in the porous $$alpha$$-MoO$$_{3}$$ wire was comparable to that of commercial $$alpha$$-MoO$$_{3}$$ powder.

Journal Articles

$$beta$$-MoO$$_{3}$$ whiskers in $$^{99}$$Mo/$$^{rm 99m}$$Tc radioisotope production and $$^{99}$$Mo/$$^{rm 99m}$$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

 Times Cited Count:3 Percentile:61.82(Chemistry, Inorganic & Nuclear)

Technetium-99m ($$^{rm 99m}$$Tc) is one of the most important radioisotopes for diagnostic radio-imaging applications. $$^{rm 99m}$$Tc is a daughter product of the $$^{99}$$Mo isotope. There are two methods used to produce $$^{99}$$Mo/$$^{rm 99m}$$Tc: the nuclear fission (n,f) and the neutron capture (n,$$gamma$$) 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,$$gamma$$) method is being developed as a future replacement for the (n,f) method. In this work, $$beta$$-MoO$$_{3}$$ whiskers prepared by the thermal evaporation method and $$alpha$$-MoO$$_{3}$$ particles were irradiated in a nuclear reactor to produce $$^{99}$$Mo/$$^{rm 99m}$$Tc via neutron capture. The irradiated targets were dispersed into water to extract the $$^{99}$$Mo/$$^{rm 99m}$$Tc. As a result, $$beta$$-MoO$$_{3}$$ whisker yielded higher $$^{99}$$Mo extraction rate than that from $$alpha$$-MoO$$_{3}$$. In addition, by comparing the dissolved $$^{98}$$Mo concentrations in water, we clarified a prominent hot-atom of $$beta$$-MoO$$_{3}$$ whiskers. This research is the first demonstration of $$beta$$-MoO$$_{3}$$ being used as an irradiation target in the neutron capture method. On the basis of the results, $$beta$$-MoO$$_{3}$$ is considered a promising irradiation target for producing $$^{99}$$Mo/$$^{rm 99m}$$Tc by neutron capture and using water for the radioisotope extraction process in the future.

Journal Articles

${it Operando}$ structure observation of pyroelectric ceramics during power generation cycle

Kawasaki, Takuro; Fukuda, Tatsuo; Yamanaka, Satoru*; Sakamoto, Tomokazu*; Murayama, Ichiro*; Kato, Takanori*; Baba, Masaaki*; Hashimoto, Hideki*; Harjo, S.; Aizawa, Kazuya; et al.

Journal of Applied Physics, 131(13), p.134103_1 - 134103_7, 2022/04

 Times Cited Count:1 Percentile:10.22(Physics, Applied)

Journal Articles

Two-step-pressurization method in pulsed electric current sintering of MoO$$_{3}$$ for production of $$^{99m}$$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

 Times Cited Count:3 Percentile:14.23(Materials Science, Ceramics)

Pulsed electric current sintering of molybdenum trioxide (MoO$$_{3}$$) was carried out by one- and two-step pressuring methods for fabrication of irradiation target using production of $$^{99}$$Mo and $$^{rm 99m}$$Tc nuclear medicine. At 550$$^{circ}$$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 $$^{98}$$Mo enriched MoO$$_{3}$$ powder.

Journal Articles

Pyroelectric power generation from the waste heat of automotive exhaust gas

Kim, J.*; Yamanaka, Satoru*; Murayama, Ichiro*; Kato, Takanori*; Sakamoto, Tomokazu*; Kawasaki, Takuro; Fukuda, Tatsuo; Sekino, Toru*; Nakayama, Tadachika*; Takeda, Masatoshi*; et al.

Sustainable Energy & Fuels (Internet), 4(3), p.1143 - 1149, 2020/03

 Times Cited Count:19 Percentile:64.99(Chemistry, Physical)

Journal Articles

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

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.

Journal Articles

Electrical and crystallographic study of an electrothermodynamic cycle for a waste heat recovery

Kim, J.*; Yamanaka, Satoru*; Nakajima, Akira*; Kato, Takanori*; Kim, Y.*; Fukuda, Tatsuo; Yoshii, Kenji; Nishihata, Yasuo; Baba, Masaaki*; Takeda, Masatoshi*; et al.

Advanced Sustainable Systems (Internet), 2(11), p.1800067_1 - 1800067_8, 2018/11

 Times Cited Count:7 Percentile:25.76(Green & Sustainable Science & Technology)

Journal Articles

Temperature stability of PIN-PMN-PT ternary ceramics during pyroelectric power generation

Moro, Takuya*; Kim, J.*; Yamanaka, Satoru*; Murayama, Ichiro*; Kato, Takanori*; Nakayama, Tadachika*; Takeda, Masatoshi*; Yamada, Noboru*; Nishihata, Yasuo; Fukuda, Tatsuo; et al.

Journal of Alloys and Compounds, 768, p.22 - 27, 2018/11

 Times Cited Count:17 Percentile:62.44(Chemistry, Physical)

Journal Articles

Pyroelectric power generation with ferroelectrics (1-x)PMN-xPT

Kim, J.*; Yamanaka, Satoru*; Nakajima, Akira*; Kato, Takanori*; Kim, Y.*; Fukuda, Tatsuo; Yoshii, Kenji; Nishihata, Yasuo; Baba, Masaaki*; Takeda, Masatoshi*; et al.

Ferroelectrics, 512(1), p.92 - 99, 2017/08

 Times Cited Count:14 Percentile:53.90(Materials Science, Multidisciplinary)

Journal Articles

Relationship between the material properties and pyroelectric-generating performance of PZTs

Yamanaka, Satoru*; Kim, J.*; Nakajima, Akira*; Kato, Takanori*; Kim, Y.*; Fukuda, Tatsuo; Yoshii, Kenji; Nishihata, Yasuo; Baba, Masaaki*; Yamada, Noboru*; et al.

Advanced Sustainable Systems (Internet), 1(3-4), p.1600020_1 - 1600020_6, 2017/04

no abstracts in English

Journal Articles

Novel electrothermodynamic power generation

Kim, Y.*; Kim, J.*; Yamanaka, Satoru*; Nakajima, Akira*; Ogawa, Takashi*; Serizawa, Takeshi*; Tanaka, Hirohisa*; Baba, Masaaki*; Fukuda, Tatsuo; Yoshii, Kenji; et al.

Advanced Energy Materials, 5(13), p.1401942_1 - 1401942_6, 2015/07

 Times Cited Count:18 Percentile:58.88(Chemistry, Physical)

An innovative electro-thermodynamic cycle based on temporal temperature variations using pyroelectric effect has been presented. Practical energy is successfully generated in both $textit{in-situ}$ synchrotron X-ray diffraction measurements under controlled conditions and $textit{Operando}$ real engine dynamometer experiments. The main generating origin is revealed as a combination of a crystal structure change and dipole change phenomenon corresponds to the temperature variation. In particular, the electric field induced 180$$^circ$$ domain switching extremely improves generating power, and the true energy breakeven with temperature variation is firstly achieved.

Oral presentation

Isotope production using novel MoO$$_{3}$$ targets; Contribution by vietnamese institutes, staffs and students

Suematsu, Hisayuki*; Ngo, M. C.*; Quach, N. M.*; Fujita, Yoshitaka; Do, T. M. D.*; Nakayama, Tadachika*; Suzuki, Tatsuya*; Nguyen, V. T.*; Niihara, Koichi*

no journal, , 

Radiopharmacies have been used in various medical diagnoses/therapies and their market has been growing by ten times in fifteen years. In particular, $$^{99m}$$Tc has been widely used in gamma ray diagnoses. $$^{99}$$Mo, the raw material for $$^{99m}$$Tc, is currently produced as a fission product by irradiating highly enriched uranium in nuclear reactors. Efforts are being made worldwide to reduce the use of uranium from the perspective of nuclear non-proliferation. A $$^{98}$$Mo(n,$$gamma$$)$$^{99}$$Mo reaction in low enriched uranium reactors can be an alternative method. In this research, we revealed that $$beta$$-MoO$$_{3}$$, a low-temperature phase of MoO$$_{3}$$, as a neutron irradiation target promotes the diffusion of $$^{99}$$Mo from the target to water due to the hot atom effect. Utilizing this phenomenon can contribute to the stable supply of $$^{99}$$Mo and $$^{99m}$$Tc. The first nuclear reaction in/water dispersion experiments using an $$alpha$$-MoO$$_{3}$$ powder target was carried out in Dalat Nuclear Reactor, Vietnam Atomic Energy Institute to show the hot atom effect. Then, the water recovery efficiency was dramatically improved using a novel $$beta$$-MoO$$_{3}$$ whisker target by Vietnamese students and staffs. Their contributions to this research will be explained in the presentation.

Oral presentation

Spark plasma sintering of MoO$$_{3}$$ for production of $$^{99m}$$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$$_{3}$$ was carried out for production of $$^{99m}$$Tc from $$^{98}$$Mo by the (n,$$gamma$$) method in a nuclear reactor. Powder of MoO$$_{3}$$ with an average grain size of 0.8$$mu$$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 $$sim$$ 200$$^{circ}$$C/min to 500 $$sim$$ 600$$^{circ}$$C 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 550$$^{circ}$$C, a sintered bulk of MoO$$_{3}$$ with a relative density of 98% was obtained. These properties are good enough for separation of $$^{99m}$$Tc and recycle of Mo.

Oral presentation

Sintering evaluation using coarse-grained MoO$$_{3}$$ powder for a radioisotope production

Sato, Soma*; Nanko, Makoto*; Suzuki, Tsuneo*; Nakayama, Tadachika*; Suematsu, Hisayuki*; Niihara, Koichi*; Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

Oral presentation

Two step pressurization in pulsed electric current sintering of MoO$$_{3}$$ for production of radioactive isotopes

Suematsu, Hisayuki*; Seki, Misaki*; Sato, Soma*; Nanko, Makoto*; Tsuchiya, Kunihiko; Nishikata, Kaori; Suzuki, Tsuneo*; Nakayama, Tadachika*; Niihara, Koichi*

no journal, , 

no abstracts in English

Oral presentation

Pulsed Electric Current Sintering of MoO$$_{3}$$ for Production of Radioactive Isotopes

Suematsu, Hisayuki*; Sato, Soma*; Seki, Misaki*; Nanko, Makoto*; Nishikata, Kaori; Suzuki, Yoshitaka; Tsuchiya, Kunihiko; Suzuki, Tsuneo*; Nakayama, Tadachika*; Niihara, Koichi*

no journal, , 

$$^{99m}$$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 $$^{235}$$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 $$^{98}$$Mo by neutrons in a reactor to form $$^{98}$$Mo and then to decay to $$^{99m}$$Tc. As the target, MoO$$_{3}$$ pellets are required. However, because of the low evaporation temperature (700 $$^{circ}$$C) and coarse grain size of $$^{98}$$Mo enriched powder, it was difficult to obtain high density MoO$$_{3}$$ pellets. To overcome this problem, a two-step loading method in pulsed electric current sintering was carried out in this study.

Oral presentation

Nuclide separation by water for development of $$^{99}$$Mo/$$^{99m}$$Tc generator for medical

Seki, Misaki*; Suematsu, Hisayuki*; Nakayama, Tadachika*; Suzuki, Tsuneo*; Niihara, Koichi*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko; Duong Van, D.*

no journal, , 

no abstracts in English

Oral presentation

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.

Oral presentation

Pulsed electric current sintering of MoO$$_{3}$$ 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$$_{3}$$ was carried out for a high density target to produce $$^{99m}$$Tc from $$^{98}$$Mo in a nuclear reactor. The green compacts of MoO$$_{3}$$ were heated in a PECS apparatus with a heating rate of 100 $$^{circ}$$C/min to 450 - 550 $$^{circ}$$C in vacuum and changing the pressurization profile from 0 to 40 MPa. After two step pressurization for sintering at 550 $$^{circ}$$C, the sintered MoO$$_{3}$$ 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$$_{3}$$ in vacuum. This oxygen depleted MoO$$_{3-x}$$ grains showed low electrical resistivity and formed a current path in the sintered body to increase the temperature to increase the relative density.

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