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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, 60(12), p.1586 - 1594, 2023/12

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

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:33.72(Nuclear Science & Technology)

Journal Articles

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:75.85(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

Basic study on a novel single-end readout type radiation distribution sensing method using an optical fiber

Terasaka, Yuta; Watanabe, Kenichi*; Uritani, Akira*

Hoshasen (Internet), 47(3), p.89 - 96, 2022/10

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:71.05(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:3 Percentile:80.29(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:56.43(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 dynamic PRA methodology for external hazards (Application of CMMC method to severe accident analysis code)

Li, C.-Y.; Watanabe, Akira*; Uchibori, Akihiro; Okano, Yasushi

Dai-26-Kai Doryoku, Enerugi Gijutsu Shimpojiumu Koen Rombunshu (Internet), 4 Pages, 2022/07

Identifying accident scenarios that could lead to severe accidents and evaluating their frequency of occurrence are essential issues. This study aims to establish the methodology of the dynamic Probabilistic Risk Assessment (PRA) for sodium-cooled fast reactors that can consider the time dependency and the interdependence of each event. Specifically, the Continuous Markov chain Monte Carlo (CMMC) method is newly applied to the SPECTRA code, which analyzes the severe accident conditions of nuclear reactors, to develop an evaluation methodology for typical external hazards. Currently, a fault-tree model of air coolers of decay heat removal system is implemented as the CMMC method, and a series of preliminary analysis of the plant's transient characteristics under the scenario of volcanic ashfall has been conducted.

Journal Articles

Theoretical and experimental estimation of the relative optically stimulated luminescence efficiency of an optical-fiber-based BaFBr:Eu detector for swift ions

Hirata, Yuho; Sato, Tatsuhiko; Watanabe, Kenichi*; Ogawa, Tatsuhiko; Parisi, A.*; Uritani, Akira*

Journal of Nuclear Science and Technology, 59(7), p.915 - 924, 2022/07

 Times Cited Count:5 Percentile:92.56(Nuclear Science & Technology)

The reliability of dose assessment with radiation detectors is an important feature in various fields, such as radiotherapy, radiation protection, and high-energy physics. However, many detectors irradiated by high linear energy transfer (LET) radiations exhibit decreased efficiency called the quenching effect. This quenching effect depends not only on the particle LET but strongly on the ion species and its microscopic pattern of energy deposition. Recently, a computational method for estimating the relative efficiency of luminescence detectors was proposed following analysis of microdosimetric specific energy distributions simulated using the particle and heavy ion transport code system (PHITS). This study applied the model to estimate the relative optically stimulated luminescence (OSL) efficiency of BaFBr:Eu detectors. Additionally, we measured the luminescence intensity of BaFBr:Eu detectors exposed to $$^{4}$$He, $$^{12}$$C and $$^{20}$$Ne ions to verify the calculated data. The model reproduced the experimental data in the cases of adopting a microdosimetric target diameter of approximately 30-50 nm. The calculated relative efficiency exhibit ion-species dependence in addition to LET. This result shows that the microdosimetric calculation from specific energy is a successful method for accurately understanding the results of OSL measurements with BaFBr:Eu detectors irradiated by various particles.

Journal Articles

First demonstration of a novel single-end readout type position-sensitive optical fiber radiation sensor based on wavelength-resolved photon counting

Terasaka, Yuta; Watanabe, Kenichi*; Uritani, Akira*

Nuclear Instruments and Methods in Physics Research A, 1034, p.166793_1 - 166793_6, 2022/07

 Times Cited Count:1 Percentile:56.43(Instruments & Instrumentation)

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.

Journal Articles

Strain distribution visualization of punched electrical steel sheets using neutron Bragg-edge transmission imaging

Sasada, Seiji*; Takahashi, Yoshihito*; Takeuchi, Keisuke*; Hiroi, Kosuke; Su, Y. H.; Shinohara, Takenao; Watanabe, Kenichi*; Uritani, Akira*

Japanese Journal of Applied Physics, 61(4), p.046004_1 - 046004_8, 2022/03

Journal Articles

Development of reacting jet evaluation model based on engineering approaches with particle method for improvement of LEAP-III code

Kosaka, Wataru; Uchibori, Akihiro; Takata, Takashi; Yanagisawa, Hideki*; Watanabe, Akira*; Jang, S.*

Proceedings of 19th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-19) (Internet), 11 Pages, 2022/03

For the safety assessment of a steam generator (SG) in a sodium-cooled fast reactor, the analysis code LEAP-III can evaluate the water leak rate during the long-term event progress including the tube failure propagation triggered by an occurrence of a small water leak in a failed heat transfer tube in SG. The LEAP-III has the advantage in completing the calculation with low computational cost since it consists of semi-empirical formulae and one-dimensional equations of conservation. However, an evaluation model of temperature distribution by the reacting jet provides wider high temperature region than the experimental data. As a result, LEAP-III shows excessive conservativeness in some case. A Lagrangian particle method code based on engineering approaches has been developed in order to improve this model to get more realistic temperature distribution. In this method, the jet behavior and chemical reaction are simulated using Newton's equation of motion with several engineering approximations instead of solving multi-dimension multiphase thermal hydraulic equations with sodium-water reaction. In this study, interparticle interaction force model was added, and also the chemical reaction and gas-liquid heat transfer evaluation models were improved. We conducted a test analysis, and compared the results by this particle method with the ones by SERAPHIM, that is a mechanistic analysis code for multi-dimensional multiphase flow considering compressibility and sodium-water reaction. Through this test analysis, it confirmed that this particle method has the basic capability to get a realistic temperature distribution with low computational cost, and also to predict tube failure occurrence by coupled with LEAP-III.

Journal Articles

Unstructured-mesh simulation of sodium-water reaction in tube bundle system by SERAPHIM code

Uchibori, Akihiro; Shiina, Yoshimi*; Watanabe, Akira*; Takata, Takashi*

Proceedings of 19th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-19) (Internet), 12 Pages, 2022/03

An unstructured mesh-based analysis method has been integrated into the sodium-water reaction analysis code, SERAPHIM, in our recent studies. In this study, numerical analysis of an experiment on sodium-water reaction in a tube bundle domain was performed to investigate the effect of the unstructured mesh. The unrealistic behavior appeared in the coarse structured mesh was improved by the unstructured mesh. The numerical result in the case of the unstructured mesh reproduced the peak value of the temperature in the reacting flow.

Journal Articles

The Chemistry of thorium, plutonium and MA

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kobayashi, Taishi*

The Chemistry of Thorium, Plutonium and MA, 254 Pages, 2022/03

The chemistry of nuclear materials such as Thorium (Part 1) and Plutonium (Part 2) was described in relation from the fundamentals on solid chemistry and solution chemistry to the practicals on the experiment and evaluation method in detail. Minor actinides such as Neptunium, Americium, Curium and Protoactinium, was introduced the basics on the solid and solution chemistry.

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

High-spatial-resolution measurement of magnetization distribution using polarized neutron imaging

Sasada, Seiji*; Hiroi, Kosuke; Osanai, Kenta*; Shinohara, Takenao; Watanabe, K.*; Uritani, Akira*

Japanese Journal of Applied Physics, 60(12), p.126003_1 - 126003_6, 2021/12

 Times Cited Count:0 Percentile:8.23(Physics, Applied)

207 (Records 1-20 displayed on this page)