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JAEA Reports

Study on molybdenum adsorption properties of alumina-based adsorbents and their application to $$^{99}$$Mo/$$^{rm 99m}$$Tc generators using the (n,$$gamma$$) method (Thesis)

Fujita, Yoshitaka

JAEA-Review 2023-010, 108 Pages, 2023/08

JAEA-Review-2023-010.pdf:6.62MB

$$^{rm 99m}$$Tc (technetium-99m) is the most widely used radioisotope in radiopharmaceutical and is decayed from the parent nuclide $$^{99}$$Mo (molybdenum-99). Most of $$^{99}$$Mo is generated as one of the fission products of uranium, but recently, from the viewpoint of nuclear security and nuclear nonproliferation, a uranium-free $$^{99}$$Mo production method is desired. One such method is the (n,$$gamma$$) method, in which $$^{98}$$Mo is irradiated by neutrons. However, since the specific activity of $$^{99}$$Mo produced by this method is extremely low, it is necessary to improve the Mo adsorption and $$^{rm 99m}$$Tc elution property of alumina (Al$$_{2}$$O$$_{3}$$), which is used as a Mo adsorbent, to apply this method to the $$^{99}$$Mo/$$^{rm 99m}$$Tc generator, a device for separation and concentration of $$^{rm 99m}$$Tc from $$^{99}$$Mo. Therefore, the objective of this thesis is to elucidate the parameters effective for improving the performance of alumina for the practical use of the $$^{99}$$Mo/$$^{rm 99m}$$Tc generator using the (n,$$gamma$$) method, and to contribute to the development of alumina columns that may be applicable to low specific activity $$^{99}$$Mo. In this study, alumina with different starting materials was prepared and its applicability as Mo adsorbent for $$^{99}$$Mo/$$^{rm 99m}$$Tc generator was evaluated. The effects of crystal structure and specific surface area of alumina on Mo adsorption properties were clarified, and the Mo adsorption mechanism was elucidated based on the results of surface analysis of alumina. In addition, $$^{rm 99m}$$Tc elution properties and $$^{rm 99m}$$Tc solution quality were evaluated using MoO$$_{3}$$ irradiated in the Kyoto University Research Reactor (KUR), and a new column shape with potential application to generators was proposed based on the experiment results of alumina columns designed for current generators.

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

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

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.

JAEA Reports

Development of fundamental technologies for domestic production of medical radioisotope (technetium-99m); The First and second phase report (FY2014-2020)

Project 6 Meeting Members for Tsukuba International Strategic Zone

JAEA-Review 2021-016, 102 Pages, 2021/11

JAEA-Review-2021-016.pdf:12.76MB

In December 2011, the Prime Minister designated Tsukuba and some areas in Ibaraki Prefecture as "Comprehensive Special Zones". In the Tsukuba International Strategic Zone, nine advanced research and development (R&D) projects are underway with the goal of promoting industrialization of life innovation and green innovation utilizing the science and technology in Tsukuba. In these projects, the domestic production of medical radioisotope (Technetium-99m, $$^{rm 99m}$$Tc) was certified as a new project in October 2013, and R&D have been performed in collaboration with related organizations with Japan Atomic Energy Agency (JAEA) as the project leader. Japan is the third largest consumer of molybdenum-99 ($$^{99}$$Mo) after the United States and Europe, and all $$^{99}$$Mo are imported. Supply will be insufficient if overseas reactors are shut down due to trouble or if transportation (air and land transportations) is stopped due to volcanic eruptions and some accidents. Thus, early domestic production of $$^{99}$$Mo is strongly required. This project is a technology development aimed at domestic production of $$^{99}$$Mo, which is a raw material of $$^{rm 99m}$$Tc used as a diagnostic agent. This report summarizes the activities carried out in the first and second phase of the domestic production of medical radioisotope ($$^{rm 99m}$$Tc) (here referred to as the "Project 6") in Tsukuba International Strategic Zone (FY2014-2020).

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:1 Percentile:47.54(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

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

Biomolecule-assisted synthesis of hierarchical multilayered boehmite and alumina nanosheets for enhanced molybdenum adsorption

Saptiama, I.*; Kaneti, Y. V.*; Yuliarto, B.*; Kumada, Hiroaki*; Tsuchiya, Kunihiko; Fujita, Yoshitaka; Malgras, V.*; Fukumitsu, Nobuyoshi*; Sakae, Takeji*; Hatano, Kentaro*; et al.

Chemistry; A European Journal, 25(18), p.4843 - 4855, 2019/03

 Times Cited Count:14 Percentile:55.95(Chemistry, Multidisciplinary)

The effective utilization of various biomolecules for creating a series of mesoporous boehmite ($$gamma$$-AlOOH) and gamma-alumina ($$gamma$$-Al$$_{2}$$O$$_{3}$$) nanosheets with unique hierarchical multilayered structures is demonstrated. The nature and concentration of the biomolecules strongly influence the degree of the crystallinity, the morphology, and the textural properties of the resulting $$gamma$$-AlOOH and $$gamma$$-Al$$_{2}$$O$$_{3}$$ nanosheets, allowing for easy tuning. The hierarchical $$gamma$$-AlOOH and $$gamma$$-Al$$_{2}$$O$$_{3}$$ multilayered nanosheets synthesized by using biomolecules exhibit enhanced crystallinity, improved particle separation, and well-defined multilayered structures compared to those obtained without biomolecules. More impressively, these $$gamma$$-AlOOH and $$gamma$$-Al$$_{2}$$O$$_{3}$$ nanosheets possess high surface areas up to 425 and 371 m$$^{2}$$/g, respectively, due to their mesoporous nature and hierarchical multilayered structure. When employed for molybdenum adsorption toward medical radioisotope production, the hierarchical $$gamma$$-Al$$_{2}$$O$$_{3}$$ multilayered nanosheets exhibit Mo adsorption capacities of 33.1$$sim$$40.8mg-Mo/g.

Journal Articles

Development of novel alumina adsorbent applying mesoporous process

Fukumitsu, Nobuyoshi*; Yamauchi, Yusuke*; Saptiama, I.*; Ariga, Katsuhiko*; Hatano, Kentaro*; Kumada, Hiroaki*; Fujita, Yoshitaka; Tsuchiya, Kunihiko

Isotope News, (760), p.15 - 18, 2018/12

no abstracts in English

Journal Articles

Neutron irradiation effect of high-density MoO$$_{3}$$ pellets for Mo-99 production

Fujita, Yoshitaka; Nishikata, Kaori; Namekawa, Yoji*; Kimura, Akihiro; Shibata, Akira; Sayato, Natsuki; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; Zhang, J.*

KURRI Progress Report 2017, P. 126, 2018/08

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

R&D on $$^{99}$$Mo/$$^{99m}$$Tc separation-concentration apparatus based on solvent extraction and column chromatography

Tsuchiya, Kunihiko; Suzuki, Yoshitaka; Nishikata, Kaori; Shibata, Akira; Nakamura, Natsuki; Tanase, Masakazu*; Shiina, Takayuki*; Ota, Akio*; Kawabata, Masako*; Takeuchi, Nobuhiro*

no journal, , 

no abstracts in English

Oral presentation

Supply of $$^{99}$$Mo; Production in research reactors

Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

Oral presentation

Status of production and application of radioisotopes in Japan

Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

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

Domestic production of medical radioisotope (technetium-99m)

Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

Oral presentation

Development of high performance Mo adsorbents

Fukumitsu, Nobuyoshi*; Yamauchi, Yusuke*; Saptiama, I.*; Ariga, Katsuhiko*; Hatano, Kentaro*; Kumada, Hiroaki*; Fujita, Yoshitaka; Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

Oral presentation

Development of effective adsorbent for Molybdenum

Fukumitsu, Nobuyoshi*; Yamauchi, Yusuke*; Saptiama, I.*; Ariga, Katsuhiko*; Hatano, Kentaro*; Kumada, Hiroaki*; Fujita, Yoshitaka; Tsuchiya, Kunihiko

no journal, , 

no abstracts in English

29 (Records 1-20 displayed on this page)