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Journal Articles

Ion beam induced luminescence analysis of europium complexes in styrene-divinylbenzene copolymer-coated spherical silica by proton and argon ion beams irradiation

Nakahara, Masaumi; Watanabe, So; Takeuchi, Masayuki; Yuyama, Takahiro*; Ishizaka, Tomohisa*; Ishii, Yasuyuki*; Yamagata, Ryohei*; Yamada, Naoto*; Koka, Masashi*; Kada, Wataru*; et al.

Nuclear Instruments and Methods in Physics Research B, 542, p.144 - 150, 2023/09

The structures of Eu complexes in the adsorbents prepared with various extractants were evaluated by ion beam induced luminescence analysis in an extraction chromatography for minor actinides recovery. The luminescence of Eu was measured with a proton beam obtained from the single-ended accelerator and an argon ion beam obtained from the azimuthally varying field cyclotron in Takasaki Ion Accelerators for Advanced Radiation Application in National Institutes for Quantum Science and Technology. In this study, it was confirmed that the spectral shape of Eu complexes in the adsorbents varied depending on the kinds of extractants, and the correlation between the change in the spectra and the structures of Eu complexes was investigated.

Journal Articles

Evaluation of the remaining spent extraction solvent in vermiculite after leaching tests via PIXE analysis

Arai, Yoichi; Watanabe, So; Hasegawa, Kenta; Okamura, Nobuo; Watanabe, Masayuki; Takeda, Keisuke*; Fukumoto, Hiroki*; Ago, Tomohiro*; Hagura, Naoto*; Tsukahara, Takehiko*

Nuclear Instruments and Methods in Physics Research B, 542, p.206 - 213, 2023/09

Journal Articles

Establishing an evaluation method for the aging phenomenon by physical force in fuel debris

Suzuki, Seiya; Arai, Yoichi; Okamura, Nobuo; Watanabe, Masayuki

Journal of Nuclear Science and Technology, 60(7), p.839 - 848, 2023/07

 Times Cited Count:0 Percentile:0.02(Nuclear Science & Technology)

The fuel debris, consisting of nuclear fuel materials and reactor structural materials, generated in the accident of Fukushima Daiichi Nuclear Power Plant can become deteriorated like rocks under the changes of environmental temperature. Although the fuel debris have been cooled by water for 10 years, they are affected by seasonal and/or day-and-night temperature changes. Therefore, in evaluating the aging behavior of the fuel debris, it is essential to consider the changes in environmental temperature. Assuming that the fuel debris are deteriorated, radioactive substances that have recently undergone micronization could be eluted into the cooling water, and such condition may affect defueling methods. We focused on the effect of repeated changes in environmental temperature on the occurrence of cracks, and an accelerated test using simulated fuel debris was carried out. The length of the crack increases with increasing number of heat cycle; therefore, the fuel debris become brittle by stress caused by thermal expansion and contraction. In conclusion, it was confirmed that the mechanical deterioration of the fuel debris is similar to that of rocks or minerals, and it became possible to predict changes in the length of the crack in the simulated fuel debris and environmental model.

Journal Articles

Neutron production in the interaction of 200-MeV deuterons with Li, Be, C, Al, Cu, Nb, In, Ta, and Au

Watanabe, Yukinobu*; Sadamatsu, Hiroki*; Araki, Shohei; Nakano, Keita; Kawase, Shoichiro*; Kin, Tadahiro*; Iwamoto, Yosuke; Satoh, Daiki; Hagiwara, Masayuki*; Yashima, Hiroshi*; et al.

EPJ Web of Conferences, 284, p.01041_1 - 01041_4, 2023/05

Intensive fast neutron sources using deuteron accelerators have been proposed for the study of medical RI production, radiation damage for fusion reactor materials, nuclear transmutation of radioactive waste, and so on. Neutron production data from various materials bombarded by deuterons are required for the design of such neutron sources. In the present work, we have conducted a systematic measurement of double-differential neutron production cross sections (DDXs) for a wide atomic number range of targets (Li, Be, C, Al, Cu, Nb, In, Ta, and Au) at an incident energy of 200 MeV in the Research Center for Nuclear Physics (RCNP), Osaka University. A deuteron beam accelerated to 200 MeV was transported to the neutron experimental hall and focused on a thin target foil. Emitted neutrons from the target were detected by two different-size EJ301 liquid organic scintillators located at two distances of 7 m and 20 m, respectively. The neutron DDXs were measured at six angles from 0$$^{circ}$$ to 25$$^{circ}$$). The neutron energy was determined by a conventional time-of-flight (TOF) method. The measured DDXs were compared with theoretical model calculations by the DEUteron-induced Reaction Analysis Code System (DEURACS) and PHITS. The result indicated that the DEURACS calculation provides better agreement with the measured DDXs than the PHITS calculation.

Journal Articles

Raman identification and characterization of chemical components included in simulated nuclear fuel debris synthesized from uranium, stainless steel, and zirconium

Kusaka, Ryoji; Kumagai, Yuta; Watanabe, Masayuki; Sasaki, Takayuki*; Akiyama, Daisuke*; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Science and Technology, 60(5), p.603 - 613, 2023/05

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

Journal Articles

Treatment of U contaminated waste generated from nuclear fuel fabrication process, 1; Ce(IV) recovery by temperature swing extraction with monoamides

Iwamoto, Toshihiro; Saito, Madoka*; Takahatake, Yoko; Watanabe, So; Watanabe, Masayuki; Naruse, Atsuki*; Tsukahara, Takehiko*

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 4 Pages, 2023/05

Applicability of temperature swing extraction technology employing monoamides was examined for uranium contaminated waste treatment procedure. Separation experiments on simulated target solution with three kinds of monoamides with different structure showed that Ce(IV) in the solution was selectively recovered by the temperature swing extraction operation. Based on the experiments, an appropriate monoamide for the procedure was selected.

Journal Articles

Development of engineering scale extraction chromatography separation system, 2; Spray drying granulation of silica support for adsorbent

Hasegawa, Kenta; Goto, Ichiro*; Miyazaki, Yasunori; Ambai, Hiromu; Watanabe, So; Watanabe, Masayuki; Sano, Yuichi; Takeuchi, Masayuki

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 5 Pages, 2023/05

Journal Articles

Phase analysis of simulated nuclear fuel debris synthesized using UO$$_{2}$$, Zr, and stainless steel and leaching behavior of the fission products and matrix elements

Tonna, Ryutaro*; Sasaki, Takayuki*; Kodama, Yuji*; Kobayashi, Taishi*; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Kumagai, Yuta; Kusaka, Ryoji; Watanabe, Masayuki

Nuclear Engineering and Technology, 55(4), p.1300 - 1309, 2023/04

 Times Cited Count:0 Percentile:0.02(Nuclear Science & Technology)

Simulated debris was synthesized using UO$$_{2}$$, Zr, and stainless steel and a heat treatment method under inert or oxidizing conditions. The primary U solid phase of the debris synthesized at 1473 K under inert conditions was UO$$_{2}$$, whereas a (U,Zr)O$$_{2}$$ solid solution formed at 1873 K. Under oxidizing conditions, a mixture of U$$_{3}$$O$$_{8}$$ and (Fe,Cr)UO$$_{4}$$ phases formed at 1473 K whereas a (U,Zr)O$$_{2+x}$$ solid solution formed at 1873 K. The leaching behavior of the fission products from the simulated debris was evaluated using two methods: the irradiation method, for which fission products were produced via neutron irradiation, and the doping method, for which trace amounts of non-radioactive elements were doped into the debris. The dissolution behavior of U depended on the properties of the debris and aqueous medium the debris was immersed in. Cs, Sr, and Ba leached out regardless of the primary solid phases. The leaching of high-valence Eu and Ru ions was suppressed, possibly owing to their solid-solution reaction with or incorporation into the uranium compounds of the simulated debris.

JAEA Reports

Annual report on the environmental radiation monitoring around the Tokai Reprocessing Plant FY2021

Nakada, Akira; Kanai, Katsuta; Seya, Natsumi; Nishimura, Shusaku; Futagawa, Kazuo; Nemoto, Masashi; Tobita, Keiji; Yamada, Ryohei*; Uchiyama, Rei; Yamashita, Daichi; et al.

JAEA-Review 2022-078, 164 Pages, 2023/03


Environmental radiation monitoring around the Tokai Reprocessing Plant has been performed by the Nuclear Fuel Cycle Engineering Laboratories, based on "Safety Regulations for the Reprocessing Plant of Japan Atomic Energy Agency, Chapter IV - Environmental Monitoring". This annual report presents the results of the environmental monitoring and the dose estimation to the hypothetical inhabitant due to the radioactivity discharged from the plant to the atmosphere and the sea during April 2021 to March 2022. In this report, some data include the influence of the accidental release from the Fukushima Daiichi Nuclear Power Station of Tokyo Electric Power Co., Inc. (the trade name was changed to Tokyo Electric Power Company Holdings, Inc. on April 1, 2016) in March 2011. Appendices present comprehensive information, such as monitoring programs, monitoring methods, monitoring results and their trends, meteorological data and discharged radioactive wastes. In addition, the data which were influenced by the accidental release and exceeded the normal range of fluctuation in the monitoring, were evaluated.

Journal Articles

Lanthanide and actinide ion complexes containing organic ligands investigated by surface-enhanced infrared absorption spectroscopy

Hirata, Sakiko*; Kusaka, Ryoji; Meiji, Shogo*; Tamekuni, Seita*; Okudera, Kosuke*; Hamada, Shoken*; Sakamoto, Chihiro*; Honda, Takumi*; Matsushita, Kosuke*; Muramatsu, Satoru*; et al.

Inorganic Chemistry, 62(1), p.474 - 486, 2023/01

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Journal Articles

A Raman spectroscopy study of bicarbonate effects on UO$$_{2+x}$$

McGrady, J.; Kumagai, Yuta; Watanabe, Masayuki; Kirishima, Akira*; Akiyama, Daisuke*; Kimuro, Shingo; Ishidera, Takamitsu

Journal of Nuclear Science and Technology, 9 Pages, 2023/00

 Times Cited Count:0 Percentile:0.02(Nuclear Science & Technology)

Journal Articles

Design of MA(III)/Ln(III) separation process of extraction chromatography technology

Akuzawa, Tadashi*; Kim, S.-Y.*; Kubota, Masahiko*; Wu, H.*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5851 - 5858, 2022/12

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

Journal Articles

Study on the relation between the crystal structure and thermal stability of FeUO$$_{4}$$ and CrUO$$_{4}$$

Akiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09

 Times Cited Count:2 Percentile:63.62(Materials Science, Multidisciplinary)

FeUO$$_{4}$$, CrUO$$_{4}$$, and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO$$_{4}$$ and CrUO$$_{4}$$, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm$$^{-1}$$ in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ was composed of a uranyl-like structure in its lattice regardless of its "x"' value. M$"o$ssbauer measurements indicated that the Fe in FeUO$$_{4}$$ and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ were trivalent. Furthermore, Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ lost its symmetry around Fe$$^{mathrm{III}}$$ with increasing electron densities around Fe$$^{mathrm{III}}$$, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO$$_{4}$$ and CrUO$$_{4}$$. Thermogravimetric measurements for UO$$_{2}$$, FeUO$$_{4}$$, and CrUO$$_{4}$$ showed that the temperature at which FeUO$$_{4}$$ decomposed under an oxidizing condition (approximately 800 $$^{circ}$$C) was significantly lower than the temperature at which the decomposition of CrUO$$_{4}$$ started (approximately 1250 $$^{circ}$$C). Based on these results, we concluded that the decomposition of FeUO$$_{4}$$ was triggered by an "in-crystal" redox reaction, i.e., Fe$$^{mathrm{III}}$$ $${+}$$ U$$^{mathrm{V}}$$ $$rightarrow$$ Fe$$^{mathrm{II}}$$ $${+}$$ U$$^{mathrm{VI}}$$, which would not occur in the CrUO$$_{4}$$ lattice because Cr$$^{mathrm{III}}$$ could never be reduced under the investigated condition. Finally, the existence of Cr$$^{mathrm{III}}$$ in FexCr$$_{1-x}$$UO$$_{4}$$ effectively suppressed the decomposition of the Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ crystal, even at a very low Cr content.

Journal Articles

Selective recovery of thorium and uranium from leach solutions of rare earth concentrates in continuous solvent extraction mode with primary amine N1923

Nguyen, T. H.*; Le Ba, T.*; Tran, C. T.*; Nguyen, T. T.*; Doan, T. T. T.*; Do, V. K.; Watanabe, Masayuki; Pham, Q. M.*; Hoang, S. T.*; Nguyen, D. V.*; et al.

Hydrometallurgy, 213, p.105933_1 - 105933_11, 2022/08

 Times Cited Count:5 Percentile:80.83(Metallurgy & Metallurgical Engineering)

A continuous counter-current extraction for the selective recovery of thorium (Th) and uranium (U) from the Yen Phu (Vietnam) rare earth concentrate leach solutions was systematically studied. The primary amine N1923 was used as an extractant which was prepared in the isoparaffin IP-2028 diluent. Thorium and uranium were selectively recovered in a hydrometallurgical circuit established by continuous mixer-settler extraction, scrubbing, and back-extraction at the laboratory scale. The desired purity of Th and U can be achieved by managing the volume ratio of organic to aqueous phase (O/A ratio) in the corresponding steps. Highly pure Th and U were recovered from the pregnant back-extraction liquor and the raffinate, respectively, which have satisfactory properties for further processing of the subsequent nuclear materials.

Journal Articles

Structure, stability, and actinide leaching of simulated nuclear fuel debris synthesized from UO$$_{2}$$, Zr, and stainless-steel

Kirishima, Akira*; Akiyama, Daisuke*; Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Sasaki, Takayuki*; Sato, Nobuaki*

Journal of Nuclear Materials, 567, p.153842_1 - 153842_15, 2022/08

 Times Cited Count:3 Percentile:77.29(Materials Science, Multidisciplinary)

To understand the chemical structure and stability of nuclear fuel debris consisting of UO$$_{2}$$, Zr, and Stainless Steel (SUS) generated by the Fukushima Daiichi Nuclear Power Plant accident in Japan in 2011, simulated debris of the UO$$_{2}$$-SUS-Zr system and other fundamental component systems were synthesized and characterized. The simulated debris were synthesized by heat treatment for 1 to 12 h at 1600$$^{circ}$$C, in inert (Ar) or oxidative (Ar + 2% O$$_{2}$$) atmospheres. $$^{237}$$Np and $$^{241}$$Am tracers were doped for the leaching tests of these elements and U from the simulated debris. The characterization of the simulated debris was conducted by XRD, SEM-EDX, Raman spectroscopy, and M$"o$ssbauer spectroscopy, which provided the major uranium phase of the UO $$_{2}$$-SUS-Zr debris was the solid solution of U$$^{mathrm{IV}}$$O$$_{2}$$ (s.s.) with Zr(IV) and Fe(II) regardless of the treatment atmosphere. The long-term immersion test of the simulated debris in pure water and that in seawater revealed the macro scale crystal structure of the simulated debris was chemically very stable in the wet condition for a year or more. Furthermore, the leaching test results showed that the actinide leaching ratios of U, Np, Am from the UO$$_{2}$$-SUS-Zr debris were very limited and less than 0.08 % for all the experiments in this study.

Journal Articles

Uranium dissolution and uranyl peroxide formation by immersion of simulated fuel debris in aqueous H$$_{2}$$O$$_{2}$$ solution

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Journal of Nuclear Science and Technology, 59(8), p.961 - 971, 2022/08

 Times Cited Count:2 Percentile:63.62(Nuclear Science & Technology)

We investigated potential degradation of fuel debris caused by H$$_{2}$$O$$_{2}$$, which is the oxidant of major impact from water radiolysis. We performed leaching experiments on different kinds of simulated debris comprising U, Fe, Cr, Ni, and Zr in an aqueous H$$_{2}$$O$$_{2}$$ solution. Chemical analysis of the leaching solution showed that U dissolution was induced by H$$_{2}$$O$$_{2}$$. Raman analysis after the leaching revealed that uranyl peroxides were formed on the surface of the simulated debris. These results demonstrate that uranyl peroxides are possible alteration products of fuel debris from H$$_{2}$$O$$_{2}$$ reaction. However, the sample in which the main uranium-containing phase was a U-Zr oxide solid solution showed much less uranium dissolution and no Raman signal of uranyl peroxides. Comparison of these results indicates that formation of an oxide solid solution of Zr with UO$$_{2}$$ improves the stability of fuel debris against H$$_{2}$$O$$_{2}$$ reaction.

Journal Articles

Development of heavy element chemistry at interfaces; Observing actinide complexes at the oil/water interface in solvent extraction by nonlinear vibrational spectroscopy

Kusaka, Ryoji; Watanabe, Masayuki

Journal of Physical Chemistry Letters (Internet), 13(30), p.7065 - 7071, 2022/08

 Times Cited Count:2 Percentile:61.67(Chemistry, Physical)

Journal Articles

Geochemical and grain composition analysis of embankment and debris flow deposits in the Izusan area, Atami City, Shizuoka Prefecture, central Japan

Kitamura, Akihisa*; Okazaki, Sota*; Kondo, Mitsuru*; Watanabe, Takahiro; Nakanishi, Toshimichi*; Hori, Rie*; Ikeda, Masayuki*; Ichimura, Koji; Nakagawa, Yuki; Mori, Hideki*

Shizuoka Daigaku Chikyu Kagaku Kenkyu Hokoku, (49), p.73 - 86, 2022/07

On July 3 2021, a debris flow caused by a landslide from a landfill occurred along the Aizome River in the Izusan area of Atami City, Shizuoka. In this study, debris flow deposits and soil samples were characterized in terms of their sedimentology and geochemically analyzed.

Journal Articles

Acid dissociation constant of bis(2-ethylhexyl) hydrogen phosphate impregnated in a polymer layer coated on silica microparticles

Miyagawa, Akihisa*; Takeuchi, Masayuki; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Nakatani, Kiyoharu*

Bulletin of the Chemical Society of Japan, 95(4), p.566 - 568, 2022/04

 Times Cited Count:1 Percentile:21.66(Chemistry, Multidisciplinary)

We demonstrate that pKa of extractant impregnated in a polymer phase varies with the cross-linking degree and the coexistence of other extractants, which induces a change in the hydrophobicity of the polymer phase. The results presented herein will be beneficial for the development of novel solid-extraction adsorbents.

Journal Articles

A Study of H$$_{2}$$O$$_{2}$$-induced oxidative degradation of simulated fuel debris

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Hoshasen Kagaku (Internet), (113), p.61 - 64, 2022/04

The severe accident at TEPCO's Fukushima Daiichi Nuclear Power Station resulted in generation of fuel debris. The fuel debris is in contact with water and the radiolysis of water can accelerate degradation of the debris. The analysis of particles sampled from inside or near the damaged reactors indicates the complicated compositions of the fuel debris. It is challenging to estimate the effect of water radiolysis on such a complicated material. Therefore, in this study, we investigated the potential degradation process by leaching experiments of simulated fuel debris in aqueous H$$_{2}$$O$$_{2}$$ solution. The results show that the reaction of H$$_{2}$$O$$_{2}$$ induced uranium dissolution from most of the samples and then formation of uranyl peroxides. In contrast, a sample that had U-Zr oxide solid solution as the major phase exhibited remarkable resistance to H$$_{2}$$O$$_{2}$$. These findings revealed that the degradation of the simulated debris reflects the reactivity and stability of the uranium phase in the matrices.

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