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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:0 Percentile:0.01(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:0 Percentile:0.01(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

Study on $$^{rm 99m}$$Tc separation/concentration technology from $$^{99}$$Mo by (n, $$gamma$$) method

Fujita, 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

Journal Articles

Radiochemical research for the advancement of $$^{99}$$Mo/$$^{rm 99m}$$Tc generator by (n, $$gamma$$) 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

no abstracts in English

Journal Articles

Mechanisms responsible for adsorption of molybdate ions on alumina for the production of medical radioisotopes

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:72.56(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$$_{4}$$$$^{2-}$$ or AlMo$$_{6}$$O$$_{24}$$H$$_{6}$$$$^{3-}$$) are adsorbed by electrostatic interaction. Alumina dissolves slightly in an acidic solution to form AlMo$$_{6}$$O$$_{24}$$H$$_{6}$$$$^{3-}$$, which is more easily desorbed than MoO$$_{4}$$$$^{2-}$$. 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$$_{4}$$$$^{2-}$$ ions. These findings will assist researchers in engineering more efficient and stable alumina-based adsorbents for molybdenum adsorption used in medical radioisotope ($$^{99}$$Mo/$$^{99m}$$Tc) generators.

Journal Articles

Dynamic properties on $$^{99}$$Mo adsorption and $$^{rm 99m}$$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

Technetium-99m ($$^{rm 99m}$$Tc), the daughter nuclide of Molybdenum-99 ($$^{99}$$Mo), is the most commonly used radioisotope in radiopharmaceuticals. The research and development (R&D) for the production of $$^{99}$$Mo by the neutron activation method ((n, $$gamma$$) method) has been carried out from viewpoints of no-proliferation and nuclear security, etc. Since the specific activity of $$^{99}$$Mo produced by the (n, $$gamma$$) method is extremely low, developing Al$$_{2}$$O$$_{3}$$ with a large Mo adsorption capacity is necessary to adapt (n, $$gamma$$)$$^{99}$$Mo to the generator. In this study, three kinds of Al$$_{2}$$O$$_{3}$$ specimens with different raw materials were prepared and compared their adaptability to generators by static and dynamic adsorption. MoO$$_{3}$$ pellet pieces (1.5g) were irradiated with 5 MW for 20 min in the Kyoto University Research Reactor (KUR). Irradiated MoO$$_{3}$$ pellet pieces were dissolved in 6M-NaOH aq. In dynamic adsorption, 1 g of Al$$_{2}$$O$$_{3}$$ was filled into a PFA tube ($$phi$$1.59 mm). The $$^{99}$$Mo adsorption capacity of Al$$_{2}$$O$$_{3}$$ specimens under dynamic condition was slightly reduced compared to that under static condition. The $$^{rm 99m}$$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 $$^{99}$$Mo/$$^{rm 99m}$$Tc ratio of dynamic condition was greatly reduced compared to that of static condition. Therefore, the $$^{rm 99m}$$Tc elution property is greatly affected by the method of adsorbing Mo, e.g., the column shape, the linear flow rate, etc.

Journal Articles

Radiochemical research for the advancement of $$^{99}$$Mo/$$^{rm 99m}$$Tc generator by (n, $$gamma$$) method, 3

Fujita, 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

Journal Articles

Research and examination of seismic safety evaluation and function maintenance for important equipment in nuclear facilities

Furuya, Osamu*; Fujita, Satoshi*; Muta, Hitoshi*; Otori, Yasuki*; Itoi, Tatsuya*; Okamura, Shigeki*; Minagawa, Keisuke*; Nakamura, Izumi*; Fujimoto, Shigeru*; Otani, Akihito*; et al.

Proceedings of ASME 2021 Pressure Vessels and Piping Conference (PVP 2021) (Internet), 6 Pages, 2021/07

Since the Fukushima accident, with the higher safety requirements of nuclear facilities in Japan, suppliers, manufacturers and academic societies have been actively considering the reconstruction of the safety of nuclear facilities from various perspectives. The Nuclear Regulation Authority has formulated new regulatory standards and is in operation. The new regulatory standards are based on defense in depth, and have significantly raised the levels of natural hazards and have requested to strengthen the countermeasures from the perspective of preventing the simultaneous loss of safety functions due to common factors. Facilities for dealing with specific serious accidents are required to have robustness to ensure functions against earthquakes that exceed the design standards to a certain extent. In addition, since the probabilistic risk assessment (PRA) and the safety margin evaluation are performed to include the range beyond the design assumption in the safety improvement evaluation, it is very important to extent the special knowledge in the strength of important equipment for seismic safety. This paper summarizes the research and examination results of specialized knowledge on the concept of maintaining the functions of important seismic facilities and the damage index to be considered by severe earthquakes. In the other paper, the study on reliability of seismic capacity analysis for important equipment in nuclear facilities will be reported.

JAEA Reports

Manufacture of substitutive assemblies for MONJU reactor decommissioning

Sakakibara, Hiroshi; Aoki, Nobuhiro; Muto, Masahiro; Otabe, Jun; Takahashi, Kenji*; Fujita, Naoyuki*; Hiyama, Kazuhiko*; Suzuki, Hirokazu*; Kamogawa, Toshiyuki*; Yokosuka, Toru*; et al.

JAEA-Technology 2020-020, 73 Pages, 2021/03

JAEA-Technology-2020-020.pdf:8.26MB

The decommissioning is currently in progress at the prototype fast breeder reactor Monju. Fuel assemblies will be taken out of its core for the first step of the great task. Fuel assemblies stand on their own spike plugged into a socket on the core support plate and support with adjacent assemblies through their housing pads each other, resulting in steady core structure. For this reason, some substitutive assemblies are necessary for the purpose of discharging the fuel assemblies of the core. Monju side commissioned, therefore, Plutonium Fuel Development Center to manufacture the substitutive assemblies and the Center accepted it. This report gives descriptions of design, manufacture, and shipment in regard to the substitutive assemblies.

Journal Articles

Effect on $$^{99}$$Mo-adsorption/$$^{99m}$$Tc-elution properties of alumina with different surface structures

Fujita, Yoshitaka; Seki, Misaki; Sano, Tadafumi*; Fujihara, Yasuyuki*; Kitagawa, Tomoya*; Matsukura, Minoru*; Hori, Junichi*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko

Journal of Radioanalytical and Nuclear Chemistry, 327(3), p.1355 - 1363, 2021/03

AA2020-0805.pdf:0.77MB

 Times Cited Count:3 Percentile:43.41(Chemistry, Analytical)

We prepared three types of Al$$_{2}$$O$$_{3}$$ with different surface structures and investigated $$^{99}$$Mo-adsorption/$$^{99m}$$Tc-elution properties using [$$^{99}$$Mo]MoO$$_{3}$$ that was irradiated in the Kyoto University Research Reactor. Al$$_{2}$$O$$_{3}$$ adsorbed [$$^{99}$$Mo]molybdate ions in solutions at different pH; the lower was the pH, the higher was the Mo-adsorption capacity of Al$$_{2}$$O$$_{3}$$. The $$^{99m}$$Tc-elution properties of molybdate ion adsorbed Al$$_{2}$$O$$_{3}$$ were elucidated by flowing saline. Consequently, it was suggested that $$^{99}$$Mo-adsorption/desorption properties are affected by the specific surface of Al$$_{2}$$O$$_{3}$$ and $$^{99m}$$Tc-elution properties are affected by the crystal structure of Al$$_{2}$$O$$_{3}$$.

Journal Articles

Radiochemical research for the advancement of $$^{99}$$Mo/$$^{rm 99m}$$Tc generator by (n,$$gamma$$) method, 2

Fujita, 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

Journal Articles

Experimental study of Gamow-Teller transitions via the high-energy-resolution $$^{18}$$O($$^3$$He,$$t$$)$$^{18}$$F reaction; Identification of the low-energy "super" -Gamow-Teller state

Fujita, Hirohiko*; Fujita, Yoshitaka*; Utsuno, Yutaka; Yoshida, Kenichi*; Adachi, Tatsuya*; Algora, A.*; Csatl$'o$s, M.*; Deaven, J. M.*; Estevez-Aguado, E.*; Guess, C. J.*; et al.

Physical Review C, 100(3), p.034618_1 - 034618_13, 2019/09

AA2019-0318.pdf:1.1MB

 Times Cited Count:12 Percentile:76.08(Physics, Nuclear)

no abstracts in English

Journal Articles

Radiochemical research for the advancement of $$^{99}$$Mo/$$^{rm 99m}$$Tc generator by (n,$$gamma$$) method

Fujita, 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

Journal Articles

Detailed study of the structure of the low-energy magnetic excitations in overdoped La$$_{1.75}$$Sr$$_{0.25}$$CuO$$_{4}$$

Ikeuchi, Kazuhiko*; Kikuchi, Tatsuya*; Nakajima, Kenji; Kajimoto, Ryoichi; Wakimoto, Shuichi; Fujita, Masaki*

Physica B; Condensed Matter, 536, p.717 - 719, 2018/05

 Times Cited Count:2 Percentile:10.13(Physics, Condensed Matter)

To examine the detailed structure of low-energy magnetic excitations in a high-transition-temperature superconducting cuprate with heavily hole-doping, we performed inelastic neutron scattering experiments on La$$_{1.75}$$Sr$$_{0.25}$$CuO$$_{4}$$. We observed clear dispersion relations of the previously reported incommensurate (IC) magnetic correlations at $$Q_{rm tet}$$ = (0.5 $$pm$$ $$delta$$, 0.5)/(0.5, 0.5 $$pm$$ $$delta$$). In addition, we show the emergence of continuum magnetic excitations with a ring shape centered at $$Gamma$$ point $$Q_{rm tet}=(0.5, 0.5)$$ in a constant energy spectrum at $$T$$ = 50 K. The radius of the ring ($$r$$ = 0.109) is smaller than the incommensurability ($$delta$$ = 0.118). This suggests that the origin of the ring-like excitations is different from that of the IC magnetic correlations, and the low-energy magnetic excitations of the La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ system are inherently composed of these two kinds of excitations.

Journal Articles

Fe-impurity-induced magnetic excitations in heavily over-doped La$$_{1.7}$$Sr$$_{0.3}$$Cu$$_{0.95}$$Fe$$_{0.05}$$O$$_{4}$$

Ikeuchi, Kazuhiko*; Kikuchi, Tatsuya*; Nakajima, Kenji; Kajimoto, Ryoichi; Wakimoto, Shuichi; Fujita, Masaki*

Journal of Physics; Conference Series, 969(1), p.012024_1 - 012024_5, 2018/04

 Times Cited Count:1 Percentile:52.34(Physics, Applied)

Journal Articles

Development of grouting technologies for geological disposal of high level waste in Japan, 1; Preliminary study for in-situ grout injection test in crystalline rock mass test site

Nakanishi, Tatsuro; Fujita, Tomoo; Tsuda, Hidenori; Tanaka, Tatsuya*; Uyama, Masao*; Onishi, Yuzo*

Dai-41-Kai Gamban Rikigaku Ni Kansuru Shimpojiumu Koenshu (CD-ROM), p.71 - 76, 2012/01

Grouting technology is fundamental to the safe and efficient construction of underground facilities for the geological disposal of high level waste in Japan. The Japan Atomic Energy Agency has been developing grouting materials and technologies with consideration to the long term chemical interactions between the grout material and the natural barrier rock mass. An in-situ grout injection test has been carried out at the Grimsel Test Site to optimize grouting design.

Journal Articles

Advanced-ORIENT cycle project; Summary of phase I fundamental studies

Koyama, Shinichi; Suzuki, Tatsuya*; Ozawa, Masaki*; Kurosawa, Kiyoko*; Fujita, Reiko*; Mimura, Hitoshi*; Okada, Ken*; Morita, Yasuji; Fujii, Yasuhiko*

Procedia Chemistry, 7, p.222 - 230, 2012/00

 Times Cited Count:2 Percentile:70.77(Chemistry, Analytical)

Adv.-ORIENT cycle strategy has been proposed as a basic concept for trinitarian research on separation, transmutation and utilization of nuclides and elements based on FBR fuel cycle. Validation of principal separation method and related safety research were performed from 2006 through 2011 as Phase I program. First, more than 90% of Cs could be recovered from the actual spent fuel [IXC(I) step]. The next is the adsorption of the platinum group metals (PGM), lanthanides, Am and Cm were separated by using a tertiary pyridine-type resin (TPR) as ion exchange steps [IXC(II, III, IV) steps]. The separated PGM metals will be supplied to the electrochemical extraction [CEE step]. As experiment for safety issues, Hastelloy-B at RT and Ta at 90$$^{circ}$$C were confirmed their anti-corrosive in highly concentrated HCl media. Thermo-chemical stability for TPR was verified. Issues to be solved for next phase based on the final results of phase I program.

Journal Articles

Advanced-ORIENT cycle, its scientific progress and prospect for engineering feasibility

Koyama, Shinichi; Yamagishi, Isao; Suzuki, Tatsuya*; Ozawa, Masaki*; Fujita, Reiko*; Okada, Ken*; Tatenuma, Katsuyoshi*; Mimura, Hitoshi*; Fujii, Yasuhiko

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 8 Pages, 2011/12

Effective separation of MA and LLFP, transmutation and utilization were the main directions of Advanced OREINT Cycle project. Study for each integrant technology was concluded as first trial of the project. TPR enabled to separate MA/Ln and then Am/Cm precisely from spent fuel in HCl and HNO$$_{3}$$ media. CEE method could separate the light PGM and Tc by HCl media. Recovery of Cs from simulated HLLW coul be achieved more than 90 %. In addition, the perspective for next phase was proposed.

Journal Articles

Current status and future plans of advanced ORIENT cycle strategy

Koyama, Shinichi; Suzuki, Tatsuya*; Mimura, Hitoshi*; Fujita, Reiko*; Kurosawa, Kiyoko*; Okada, Ken*; Ozawa, Masaki

Progress in Nuclear Energy, 53(7), p.980 - 987, 2011/09

 Times Cited Count:5 Percentile:38.41(Nuclear Science & Technology)

Individual basic researches of separation step were performed in the Advanced ORIENT Cycle project. High separation selectivity for Cs and Sr by novel nano adsorbents AMP-SG (D) and D18C6-MC were confirmed, respectively. TPR well adsorbed Pd and Tc in dilute HCl condition. Formation of rare metal fission product RMFP-deposit Pt electrodes from SHLLW was verified, and it was confirmed that high catalytic reactivity on electrolytic production of hydrogen. As experiment for engineering feasibility, Hastelloy-B at RT and Ta at 90$$^{circ}$$C were confirmed their anti-corrosive in highly concentrated HCl media. Thermo-chemical stability for TPR was verified in either HCl or HNO$$_{3}$$ media toward its practical use in the separation process. Issues to be solved for optimization based on the results of lab-scale experiment have revealed in this study.

Journal Articles

Development of function-graded proton exchange membrane for PEFC using heavy ion beam irradiation

Shiraki, Fumiya*; Yoshikawa, Taeko*; Oshima, Akihiro*; Oshima, Yuji*; Takasawa, Yuya*; Fukutake, Naoyuki*; Oyama, Tomoko*; Urakawa, Tatsuya*; Fujita, Hajime*; Takahashi, Tomohiro*; et al.

Nuclear Instruments and Methods in Physics Research B, 269(15), p.1777 - 1781, 2011/08

 Times Cited Count:8 Percentile:53.06(Instruments & Instrumentation)

The graded energy deposition of heavy ion beam irradiation to polymeric materials was utilized to synthesize a novel proton exchange membrane (PEM) with the graded density of sulfonic acid groups toward the thickness direction. Stacked Poly(tetrafluoroethylene-co-hexafluoropropylene) (FEP) films were irradiated by Xe$$^{54+}$$ ion beam with the energy of 6 MeV/u under a vacuum condition. Irradiated films were grafted with styrene monomer and then sulfonated. The membrane electrode assembly (MEA) fabricated by the function graded PEM showed improved fuel cell performance in terms of voltage stability. It was expected that the function-graded PEM could control the graded concentration of sulfonic acid groups in PEM.

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