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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

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.

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

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

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.

Journal Articles

A Storm-induced flood and associated nearshore dispersal of the river-derived suspended $$^{137}$$Cs

Uchiyama, Yusuke*; Tokunaga, Natsuki*; Azuma, Kohei*; Kamidaira, Yuki; Tsumune, Daisuke*; Iwasaki, Toshiki*; Yamada, Masatoshi*; Tateda, Yutaka*; Ishimaru, Takashi*; Ito, Yukari*; et al.

Science of the Total Environment, 816, p.151573_1 - 151573_13, 2022/04

 Times Cited Count:5 Percentile:71.31(Environmental Sciences)

no abstracts in English

Journal Articles

Improving the safety of the high temperature gas-cooled reactor "HTTR" based on Japan's new regulatory requirements

Hamamoto, Shimpei; Shimizu, Atsushi; Inoi, Hiroyuki; Tochio, Daisuke; Homma, Fumitaka; Sawahata, Hiroaki; Sekita, Kenji; Watanabe, Shuji; Furusawa, Takayuki; Iigaki, Kazuhiko; et al.

Nuclear Engineering and Design, 388, p.111642_1 - 111642_11, 2022/03

 Times Cited Count:0 Percentile:33.72(Nuclear Science & Technology)

Following the Fukushima Daiichi Nuclear Power Plant accident in 2011, the Japan Atomic Energy Agency adapted High-Temperature engineering Test Reactor (HTTR) to meet the new regulatory requirements that began in December 2013. The safety and seismic classifications of the existing structures, systems, and components were discussed to reflect insights regarding High Temperature Gas-cooled Reactors (HTGRs) that were acquired through various HTTR safety tests. Structures, systems, and components that are subject to protection have been defined, and countermeasures to manage internal and external hazards that affect safety functions have been strengthened. Additionally, measures are in place to control accidents that may cause large amounts of radioactive material to be released, as a beyond design based accident. The Nuclear Regulatory Commission rigorously and appropriately reviewed this approach for compliance with the new regulatory requirements. After nine amendments, the application to modify the HTTR's installation license that was submitted in November 2014 was approved in June 2020. This response shows that facilities can reasonably be designed to meet the enhanced regulatory requirements, if they reflect the characteristics of HTGRs. We believe that we have established a reference for future development of HTGR.

JAEA Reports

Impact assessment for internal flooding in HTTR (High temperature engineering test reactor)

Tochio, Daisuke; Nagasumi, Satoru; Inoi, Hiroyuki; Hamamoto, Shimpei; Ono, Masato; Kobayashi, Shoichi; Uesaka, Takahiro; Watanabe, Shuji; Saito, Kenji

JAEA-Technology 2021-014, 80 Pages, 2021/09

JAEA-Technology-2021-014.pdf:5.87MB

In response to the new regulatory standards established in response to the accident at TEPCO's Fukushima Daiichi Nuclear Power Station in March 2011, measures and impact assessments related to internal flooding at HTTR were carried out. In assessing the impact, considering the characteristics of the high-temperature gas-cooled reactor, flooding due to assumed damage to piping and equipment, flooding due to water discharge from the system installed to prevent the spread of fire, and flooding due to damage to piping and equipment due to an earthquake. The effects of submersion, flooding, and flooding due to steam were evaluated for each of them. The impact of the overflow of liquids containing radioactive materials outside the radiation-controlled area was also evaluated. As a result, it was confirmed that flooding generated at HTTR does not affect the safety function of the reactor facility by taking measures.

Journal Articles

The Kinetics and mechanism of H$$_{2}$$O$$_{2}$$ decomposition at the U$$_{3}$$O$$_{8}$$ surface in bicarbonate solution

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

RSC Advances (Internet), 11(46), p.28940 - 28948, 2021/08

 Times Cited Count:4 Percentile:39.59(Chemistry, Multidisciplinary)

Journal Articles

Distribution of studtite and metastudtite generated on the surface of U$$_{3}$$O$$_{8}$$; Application of Raman imaging technique to uranium compound

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

Journal of Nuclear Science and Technology, 58(6), p.629 - 634, 2021/06

 Times Cited Count:7 Percentile:67.5(Nuclear Science & Technology)

JAEA Reports

Hydrochemical investigation at the Mizunami Underground Research Laboratory; Compilation of groundwater chemistry data in the Mizunami Group and the Toki Granite (fiscal year 2019)

Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Aosai, Daisuke*; Hara, Naohiro*

JAEA-Data/Code 2020-012, 80 Pages, 2020/10

JAEA-Data-Code-2020-012.pdf:3.55MB

Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2019. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.

JAEA Reports

Hydrochemical investigation at the Mizunami Underground Research Laboratory; Compilation of groundwater chemistry data in the Mizunami group and the Toki granite (fiscal year 2018)

Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Aosai, Daisuke*; Kumamoto, Yoshiharu*; Iwatsuki, Teruki

JAEA-Data/Code 2019-019, 74 Pages, 2020/03

JAEA-Data-Code-2019-019.pdf:3.53MB

Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2018. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.

Journal Articles

Enhancement of element production by incomplete fusion reaction with weakly bound deuteron

Wang, H.*; Otsu, Hideaki*; Chiga, Nobuyuki*; Kawase, Shoichiro*; Takeuchi, Satoshi*; Sumikama, Toshiyuki*; Koyama, Shumpei*; Sakurai, Hiroyoshi*; Watanabe, Yukinobu*; Nakayama, Shinsuke; et al.

Communications Physics (Internet), 2(1), p.78_1 - 78_6, 2019/07

 Times Cited Count:7 Percentile:56.64(Physics, Multidisciplinary)

Searching for effective pathways for the production of proton- and neutron-rich isotopes through an optimal combination of reaction mechanism and energy is one of the main driving forces behind experimental and theoretical nuclear reaction studies as well as for practical applications in nuclear transmutation of radioactive waste. We report on a study on incomplete fusion induced by deuteron, which contains one proton and one neutron with a weak binding energy and is easily broken up. This reaction study was achieved by measuring directly the cross sections for both proton and deuteron for $$^{107}$$Pd at 50 MeV/u via inverse kinematics technique. The results provide direct experimental evidence for the onset of a cross-section enhancement at high energy, indicating the potential of incomplete fusion induced by loosely-bound nuclei for creating proton-rich isotopes and nuclear transmutation of radioactive waste.

Journal Articles

Study on loss-of-cooling and loss-of-coolant accidents in spent fuel pool, 1; Overview

Kaji, Yoshiyuki; Nemoto, Yoshiyuki; Nagatake, Taku; Yoshida, Hiroyuki; Tojo, Masayuki*; Goto, Daisuke*; Nishimura, Satoshi*; Suzuki, Hiroaki*; Yamato, Masaaki*; Watanabe, Satoshi*

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05

In this research program, cladding oxidation model in SFP accident condition, and numerical simulation method to evaluate capability of spray cooling system which was deployed for spent fuel cooling during SFP accident, have been developed. These were introduced into the severe accident codes such as MAAP and SAMPSON, and SFP accident analyses were conducted. Analyses using Computational Fluid Dynamics (CFD) code were conducted as well for the comparison with SA code analyses and investigation of detail in the SFP accident. In addition, three-dimensional criticality analysis method was developed as well, and safer loading pattern of spent fuels in pool was investigated.

JAEA Reports

Hydrochemical investigation at the Mizunami Underground Research Laboratory; Compilation of groundwater chemistry data in the Mizunami group and the Toki granite (fiscal year 2017)

Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Hayashida, Kazuki*; Aosai, Daisuke*; Kumamoto, Yoshiharu*; Iwatsuki, Teruki

JAEA-Data/Code 2018-021, 76 Pages, 2019/03

JAEA-Data-Code-2018-021.pdf:3.78MB

Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2017. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.

JAEA Reports

Hydrochemical investigation at the Mizunami Underground Research Laboratory; Compilation of groundwater chemistry data in the Mizunami group and the Toki granite (fiscal year 2016)

Watanabe, Yusuke; Hayashida, Kazuki; Kato, Toshihiro; Kubota, Mitsuru; Aosai, Daisuke*; Kumamoto, Yoshiharu*; Iwatsuki, Teruki

JAEA-Data/Code 2018-002, 108 Pages, 2018/03

JAEA-Data-Code-2018-002.pdf:6.53MB

Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the effect of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2016 and 2014 to 2016, respectively. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.

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