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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

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.

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: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

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

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

Age-hardening mechanisms of heterogeneous-nanostructured SUS316LN stainless steel fabricated by heavy cold rolling

Miura, Hiromi*; Watanabe, Chihiro*; Aoyagi, Yoshiteru*; Oba, Yojiro; Kobayashi, Masakazu*; Yoshinaga, Naoki*

Materials Science & Engineering A, 833, p.142531_1 - 142531_12, 2022/01

 Times Cited Count:3 Percentile:57.69(Nanoscience & Nanotechnology)

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:70.19(Nuclear Science & Technology)

Journal Articles

Stoichiometry of lanthanide-phosphate complexes at the water surface studied using vibrational sum frequency generation spectroscopy and DFT calculations

Kusaka, Ryoji; Watanabe, Masayuki

Journal of Physical Chemistry B, 125(24), p.6727 - 6731, 2021/06

 Times Cited Count:8 Percentile:50.56(Chemistry, Physical)

Journal Articles

Role of advection in atmospheric ammonia; A Case study at a Japanese lake basin influenced by agricultural ammonia sources

Kubota, Tomohiro; Kuroda, Hisao*; Watanabe, Mirai*; Takahashi, Akiko*; Nakazato, Ryoji*; Tarui, Mika*; Matsumoto, Shunichi*; Nakagawa, Keita*; Numata, Yasuko*; Ouchi, Takao*; et al.

Atmospheric Environment, 243, p.117856_1 - 117856_9, 2020/12

 Times Cited Count:2 Percentile:11.13(Environmental Sciences)

The dry and wet depositions of atmospheric ammonia (NH$$_{3}$$) is one of the important pathways of nitrogen loads to aquatic ecosystems. Crop and livestock agriculture, one of the largest emitters of NH$$_{3}$$ in Asian countries, are known to cause high spatial and seasonal variation of NH$$_{3}$$ and influence the surrounding lake basin areas via its dry and wet deposition. However, the spatial characteristics of the NH$$_{3}$$ concentration in basin scale are not completely understood for regulation in NH$$_{3}$$ emission. Here we aim to clarify dominant factors of spatial and seasonal variations of the NH$$_{3}$$ concentration in a eutrophic lake basin surrounded by agricultural areas in Japan. Passive sampling over various land use categories in the basin was conducted at 36 sites in total from October 2018 to January 2020. Interestingly, the observed NH$$_{3}$$ concentration near the livestock houses were higher in winter than summer, which was inconsistent with knowledge of seasonal changes of current NH$$_{3}$$ emission inventory based on temperature-driven volatilization process. Comparing monthly NH$$_{3}$$ concentrations with various meteorological factors, we suggested the importance of seasonal advection of NH$$_{3}$$ from high emission sources to which has been rarely paid attention by the previous past studies. As for this, should be considered for lake ecosystem management since deposition of NH$$_{3}$$ is known to be closely related to the ecological processes such as phytoplankton blooming.

Journal Articles

Application of photoluminescence microspectroscopy; A Study on transfer of uranyl and europium ions on dry silica gel plate

Kusaka, Ryoji; Watanabe, Masayuki

Journal of Nuclear Science and Technology, 57(9), p.1046 - 1050, 2020/09

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

Journal Articles

Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

Otaka, Toshiki*; Sato, Tatsumi*; Ono, Shimpei; Nagoshi, Kohei; Abe, Ryoji*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Nakatani, Kiyoharu*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

 Times Cited Count:7 Percentile:34.17(Chemistry, Analytical)

Journal Articles

Mechanism of phase transfer of uranyl ions; A Vibrational sum frequency generation spectroscopy study on solvent extraction in nuclear reprocessing

Kusaka, Ryoji; Watanabe, Masayuki

Physical Chemistry Chemical Physics, 20(47), p.29588 - 29590, 2018/12

 Times Cited Count:17 Percentile:69.73(Chemistry, Physical)

Mechanistic understanding of solvent extraction of uranyl ions (UO$$_{2}$$$$^{2+}$$) by tributyl phosphate (TBP) will help improve the technology for the treatment and disposal of spent nuclear fuels. So far, it has been believed that uranyl ions in the aqueous phase are adsorbed to a TBP-enriched organic/aqueous interface, form complexes with TBP at the interface, and are extracted into the organic phase. Here we show that uranyl-TBP complex formation does not take place at the interface using vibrational sum frequency generation (VSFG) spectroscopy and propose an alternative extraction mechanism that uranyl nitrate, UO$$_{2}$$(NO$$_{3}$$)$$_{2}$$, passes through the interface and forms the uranyl-TBP complex, UO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(TBP)$$_{2}$$, in the organic phase.

Journal Articles

The Structure of a lanthanide complex at an extractant/water interface studied using heterodyne-detected vibrational sum frequency generation

Kusaka, Ryoji; Watanabe, Masayuki

Physical Chemistry Chemical Physics, 20(4), p.2809 - 2813, 2018/01

 Times Cited Count:14 Percentile:62.6(Chemistry, Physical)

Solvent extraction plays an integral part in the separation and purification of metals. Because extractants generally used as complexing agents for metal extractions, such as di-(2-ethylhexyl)phosphoric acid (HDEHP) for lanthanide extractions, are amphiphilic, they come to the organic/water interface, and the interface plays a crucial role as the site of the formation of metal complexes and subsequent transfer reaction to an organic phase. Despite the importance of the interface for solvent extractions, however, molecular-level structure of the interface is unclear because of experimental difficulty. Here we studied structure of a trivalent europium (Eu$$^{3+}$$) complex with HDEHP formed at HDEHP monolayer/water interface by heterodyne-detected vibrational sum frequency generation (HD-VSFG) spectroscopy. The study on the HDEHP/water interface enables us to investigate the structure of the interfacial Eu$$^{3+}$$ complex by excluding the migration of Eu$$^{3+}$$ into an organic phase after the complex formation at the interface. The interface-selective vibrational Im$$chi$$$$^{(2)}$$ spectra observed by HD-VSFG of HDEHP/Eu(NO$$_{3}$$)$$_{3}$$ aqueous solution interface in the 2800-3500 cm$$^{-1}$$ region indicate that Eu$$^{3+}$$ at the HDEHP/water interface is bonded by HDEHP from the air side and by water molecules from the water side. To the best of our knowledge, such metal complex structures have not been identified in the organic or water solutions.

Journal Articles

Magnetic Bragg dip and Bragg edge in neutron transmission spectra of typical spin superstructures

Mamiya, Hiroaki*; Oba, Yojiro; Terada, Noriki*; Watanabe, Norimichi*; Hiroi, Kosuke; Shinohara, Takenao; Oikawa, Kenichi

Scientific Reports (Internet), 7(1), p.15516_1 - 15516_8, 2017/11

 Times Cited Count:1 Percentile:11.95(Multidisciplinary Sciences)

no abstracts in English

Journal Articles

Microscopic analyses of complexes formed in adsorbent for Mo and Zr separation chromatography

Abe, Ryoji*; Nagoshi, Kohei*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Matsuura, Haruaki*; Takagi, Hideaki*; Shimizu, Nobutaka*; Koka, Masashi*; Sato, Takahiro*

Nuclear Instruments and Methods in Physics Research B, 404, p.173 - 178, 2017/08

 Times Cited Count:5 Percentile:46.25(Instruments & Instrumentation)

Journal Articles

Analysis on ex-vessel loss of coolant accident for a water-cooled fusion DEMO reactor

Watanabe, Kazuhito; Nakamura, Makoto; Tobita, Kenji; Someya, Yoji; Tanigawa, Hisashi; Uto, Hiroyasu; Sakamoto, Yoshiteru; Araki, Takao*; Asano, Shiro*; Asano, Kazuhito*

Proceedings of 26th IEEE Symposium on Fusion Engineering (SOFE 2015), 6 Pages, 2016/06

Safety studies of a water-cooled fusion DEMO reactor have been performed. In the event of the blanket cooling pipe break outside the vacuum vessel, i.e. ex-vacuum vessel loss of coolant accident (ex-VV LOCA), the pressurized steam and air may lead to damage reactor building walls which have confinement function, and to release the radioactive materials to the environment. In response to this accident, we proposed three cases of confinement strategies. In each case, the pressure and thermal loads to the confinement boundaries and total mass of tritium released to outside the boundaries were analyzed by accident analysis code MELCOR modified for fusion reactor. These analyses developed design parameters to maintain the integrity of the confinement boundaries.

Journal Articles

Study of safety features and accident scenarios in a fusion DEMO reactor

Nakamura, Makoto; Tobita, Kenji; Gulden, W.*; Watanabe, Kazuhito*; Someya, Yoji; Tanigawa, Hisashi; Sakamoto, Yoshiteru; Araki, Takao*; Matsumiya, Hisato*; Ishii, Kyoko*; et al.

Fusion Engineering and Design, 89(9-10), p.2028 - 2032, 2014/10

 Times Cited Count:13 Percentile:71.02(Nuclear Science & Technology)

After the Fukushima Dai-ichi nuclear accident, a social need for assuring safety of fusion energy has grown gradually in the Japanese (JA) fusion research community. DEMO safety research has been launched as a part of BA DEMO Design Activities (BA-DDA). This paper reports progress in the fusion DEMO safety research conducted under BA-DDA. Safety requirements and evaluation guidelines have been, first of all, established based on those established in the Japanese ITER site invitation activities. The amounts of radioactive source terms and energies that can mobilize such source terms have been assessed for a reference DEMO, in which the blanket technology is based on the Japanese fusion technology R&D programme. Reference event sequences expected in DEMO have been analyzed based on the master logic diagram and functional FMEA techniques. Accident initiators of particular importance in DEMO have been selected based on the event sequence analysis.

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