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JAEA Reports

Utilization of gamma ray irradiation at the WASTEF Facility

Sano, Naruto; Yamashita, Naoki; Watanabe, Masaya; Tsukada, Manabu*; Hoshino, Kazutoyo*; Hirai, Koki; Ikegami, Yuta*; Tashiro, Shinsuke; Yoshida, Ryoichiro; Hatakeyama, Yuichi; et al.

JAEA-Technology 2023-029, 36 Pages, 2024/03

JAEA-Technology-2023-029.pdf:2.47MB

At the Waste Safety Testing Facility (WASTEF), the gamma ray irradiation device "Gamma Cell 220" was relocated from the 4th research building of the Nuclear Science Research Institute in FY2019, and the use of gamma ray irradiation has begun. Initially, Fuel Cycle Safety Research Group, Fuel Cycle Safety Research Division, Nuclear Safety Research Center, Sector of Nuclear Safety Research and Emergency Preparedness, the owner of this device, conducted the tests as the main user, but since 2022, other users, including those outside the organization, have started using it. The gamma ray irradiation device "Gamma Cell 220" is manufactured by Nordion International Inc. in Canada. Since it was purchased in 1989, the built-in 60Co radiation source has been updated once, and safety research related to nuclear fuel cycles, etc. It is still used for this purpose to this day. This report summarizes the equipment overview of the gamma ray irradiation device "Gamma Cell 220", its permits and licenses at WASTEF, usage status, maintenance and inspection, and future prospects.

Journal Articles

Contrast dependence of scattering profiles for poly(ethylene glycol) in water; Investigation by small-angle neutron scattering with $$^{3}$$He spin filter and small-angle X-ray scattering

Ryoki, Akiyuki*; Watanabe, Fumi*; Okudaira, Takuya*; Takahashi, Shingo*; Oku, Takayuki; Hiroi, Kosuke; Motokawa, Ryuhei; Nakamura, Yo*

Journal of Chemical Physics, 160(11), p.114907_1 - 114907_9, 2024/03

Journal Articles

Intercalative and non-intercalative photo-recharge using all-solid-state cells for solar energy conversion and storage

Yoshimoto, Masataka*; Tamura, Kazuhisa; Watanabe, Kenta*; Shimizu, Keisuke*; Horisawa, Yuhei*; Kobayashi, Takeshi*; Tsurita, Hanae*; Suzuki, Kota*; Kanno, Ryoji*; Hirayama, Masaaki*

Sustainable Energy & Fuels (Internet), 8(6), p.1236 - 1244, 2024/03

 Times Cited Count:0

Photo-rechargeable systems, which can efficiently convert and store solar energy into chemical energy within single devices, are essential to harness sunlight effectively. Photo-(de)intercalation plays a pivotal role in the functionality of photorechargeable systems. Nevertheless, the photo-(de)intercalation process has not been conclusively confirmed owing to potential interference from side reactions, such as the decomposition of liquid electrolytes and the elution of electrode materials. In this study, we successfully demonstrated photo-responsive Li$$^{+}$$-deintercalation using an all-solid-state thin-film battery comprised of epitaxially-grown anatase TiO$$_{2}$$ doped with Nb (a-TiO$$_{2}$$:Nb) as the cathode. Under light irradiation, Li$$^{+}$$-deintercalation occurred and was subsequently reversibly intercalated into a-TiO$$_{2}$$:Nb during discharge.

Journal Articles

Stable photoelectrochemical reactions at solid/solid interfaces toward solar energy conversion and storage

Watanabe, Kenta*; Horisawa, Yuhei*; Yoshimoto, Masataka*; Tamura, Kazuhisa; Suzuki, Kota*; Kanno, Ryoji*; Hirayama, Masaaki*

Nano Letters, 24(6), p.1916 - 1922, 2024/02

 Times Cited Count:1 Percentile:0.02(Chemistry, Multidisciplinary)

Electrochemistry has extended from reactions at solid/liquid interfaces to those at solid/solid interfaces. In this study, we achieve the stable photoelectrochemical reaction at the semiconductor-electrode/solid-electrolyte interface in Nb-doped anatase-TiO$$_{2}$$ (a-TiO$$_{2}$$:Nb)/Li$$_{3}$$PO$$_{4}$$ (LPO)/Li all-solid-state cell. The oxidative currents of a-TiO$$_{2}$$:Nb/LPO/Li increase upon light irradiation when a-TiO$$_{2}$$:Nb is located at a potential that is more positive than its flat-band potential. The photoelectrochemical reaction at the semiconductor/solid-electrolyte interface is driven by the same principle as that at semiconductor/liquid-electrolyte interfaces. Thus, we extend photoelectrochemistry to all-solid-state systems composed of solid/solid interfaces.

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

 Times Cited Count:0 Percentile:0.02(Instruments & Instrumentation)

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.

JAEA Reports

Differential pressure rise event for filters of HTTR primary helium gas circulators, 1; Investigation of differential pressure rise event

Nemoto, Takahiro; Arakawa, Ryoki; Kawakami, Satoru; Nagasumi, Satoru; Yokoyama, Keisuke; Watanabe, Masashi; Onishi, Takashi; Kawamoto, Taiki; Furusawa, Takayuki; Inoi, Hiroyuki; et al.

JAEA-Technology 2023-005, 33 Pages, 2023/05

JAEA-Technology-2023-005.pdf:5.25MB

During shut down of the HTTR (High Temperature engineering Test Reactor) RS-14 cycle, an increasing trend of filter differential pressure for the helium gas circulator was observed. In order to investigate this phenomenon, the blower of the primary helium purification system was disassembled and inspected. As a result, it is clear that the silicon oil mist entered into the primary coolant due to the deterioration of the charcoal filter performance. The replacement and further investigation of the filter are planning to prevent the reoccurrence of the same phenomenon in the future.

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:1 Percentile:31.61(Nuclear Science & Technology)

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:1 Percentile:72.91(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

JAEA-Review-2022-078.pdf:2.64MB

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

Ion beam induced luminescence spectra of europium complexes in silica-based adsorbent

Nakahara, Masaumi; Watanabe, So; Ishii, Yasuyuki*; Yamagata, Ryohei*; Yamada, Naoto*; Koka, Masashi*; Yuyama, Takahiro*; Ishizaka, Tomohisa*; Kada, Wataru*; Hagura, Naoto*

QST-M-39; QST Takasaki Annual Report 2021, P. 62, 2023/02

In an extraction chromatography method for minor actinides recovery, analysis for the structure of complex in a silica-based adsorbent has been studied to separate minor actinides efficiently. In this study, Eu was used as simulated material of minor actinides, and silica-based adsorbents containing Eu complex were prepared. The ion beam induced luminescence spectra of Eu complexes in silica-based adsorbents were measured, and the basic data for the structures of Eu complexes were obtained.

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

Clogging properties of HEPA filter induced by loading of soot from burned glove-box panel materials

Tashiro, Shinsuke; Ono, Takuya; Amano, Yuki; Yoshida, Ryoichiro; Watanabe, Koji*; Abe, Hitoshi

Nuclear Technology, 208(10), p.1553 - 1561, 2022/10

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

To contribute to the confinement safety evaluation of the radioactive materials in the Glove box (GB) fire accident, combustion tests with the Polymethyl methacrylate (PMMA) and the Polycarbonate (PC) as typical panel materials for the GB have been conducted with a relatively large scale apparatus. As the important data for evaluating confinement safety, the release ratio and the particle size distribution of the soot generated from the burned materials were obtained. Furthermore, the rise of the differential pressure ($$Delta$$P) of the high efficiency particle air (HEPA) filter by the soot loading was also investigated. As results, the release ratio of the soot from the PC was about seven times as large as the PMMA. In addition, it was found that the behavior of the rise of the $$Delta$$P with soot loading could be represented uniformly regardless of kinds of combustion materials by considering effect of the loading volume of the soot particle in the relatively low loading region.

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:3 Percentile:68.71(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

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:4 Percentile:78.52(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:53.91(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:5 Percentile:70.33(Chemistry, Physical)

Journal Articles

Investigation of physical properties of glove for glove-box and estimation of its life-time

Kobayashi, Daisuke; Yamamoto, Masahiko; Nishida, Naoki; Miyoshi, Ryuta; Nemoto, Ryo*; Hayashi, Hiroyuki*; Kato, Keisuke; Nishino, Saki; Kuno, Takehiko; Kitao, Takahiko; et al.

Nihon Hozen Gakkai Dai-18-Kai Gakujutsu Koenkai Yoshishu, p.237 - 240, 2022/07

All gloves attached to glove-box in Tokai Reprocessing Plant have a fixed expiration date and have to be replaced every 4-year. However, degrees of glove deterioration are different depending on its usage environment (frequency, chemicals, radiation, etc.), because of rubber products. Therefore, physical properties such as tensile strength, elongation, hardness of gloves are measured, and the life-time of gloves are estimated. As a result, gloves without any defects in its appearance have enough physical property for acceptance criteria of new glove. The extrapolated physical property of glove is sufficiently larger than the reported values of damaged glove. No deterioration in physical properties of gloves, that are periodically replaced without any defects in its appearance, is observed and the usable life-time of the glove is estimated to be 8 years.

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.

JAEA Reports

Annual report on the environmental radiation monitoring around the Tokai Reprocessing Plant FY2020

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

JAEA-Review 2021-062, 163 Pages, 2022/02

JAEA-Review-2021-062.pdf:2.87MB

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 2020 to March 2021. 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

Structures of magnetic excitations in the spin-$$frac{1}{2}$$ kagome-lattice antiferromagnets Cs$$_{2}$$Cu$$_{3}$$SnF$$_{12}$$ and Rb$$_{2}$$Cu$$_{3}$$SnF$$_{12}$$

Saito, Mutsuki*; Takagishi, Ryunosuke*; Kurita, Nubuyuki*; Watanabe, Masari*; Tanaka, Hidekazu*; Nomura, Ryuji*; Fukumoto, Yoshiyuki*; Ikeuchi, Kazuhiko*; Kajimoto, Ryoichi

Physical Review B, 105(6), p.064424_1 - 064424_15, 2022/02

 Times Cited Count:6 Percentile:73.14(Materials Science, Multidisciplinary)

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