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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

https://doi.org/10.1080/00223131.2023.2236104
 Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)

Journal Articles

Current location of fuel debris chemistry

Sato, Nobuaki*; Kirishima, Akira*; Sasaki, Takayuki*; Takano, Masahide; Kumagai, Yuta; Sato, Soichi; Tanaka, Kosuke

Current Location of Fuel Debris Chemistry, 178 Pages, 2023/11

Considerable efforts have been devoted to the decommissioning of the TEPCO's Fukushima Daiichi Nuclear Power Station (1F) and now the retrieval of fuel debris is being proceeded on a trial basis. It can be said that the succession of science and technology related to debris, that is, human resource development, is important and indispensable. For that reason, we thought that a specific textbook on decommissioning is necessary. Regarding the 1F fuel debris, we still do not know enough, and it would be difficult to describe the details. However, 12 years have passed since the accident, and we have come to understand the situation of 1F to a certain extent. At this stage, it is essential for future development to organize the current situation by combining examples of past severe accidents. Therefore, we presented in this book the current state of fuel debris chemistry research from the perspectives of solid chemistry, solution chemistry, analytical chemistry, radiochemistry, and radiation chemistry.

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

https://doi.org/10.1080/00223131.2022.2128460
 Times Cited Count：1 Percentile：29.26(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

https://doi.org/10.1016/j.net.2022.12.017
 Times Cited Count：2 Percentile：68.31(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

Application of high-energy-resolution X-ray absorption spectroscopy at the U L$$_{3}$$-edge to assess the U(V) electronic structure in FeUO$$_{4}$$

Yomogida, Takumi; Akiyama, Daisuke*; Ouchi, Kazuki; Kumagai, Yuta; Higashi, Kotaro*; Kitatsuji, Yoshihiro; Kirishima, Akira*; Kawamura, Naomi*; Takahashi, Yoshio*

Inorganic Chemistry, 61(50), p.20206 - 20210, 2022/12

https://doi.org/10.1021/acs.inorgchem.2c03208
 Times Cited Count：4 Percentile：34.43(Chemistry, Inorganic & Nuclear)

FeUO$$_{4}$$ was studied to clarify the electronic structure of U(V) in a metal monouranate compound. We obtained the peak splitting of HERFD-XANES spectra utilizing high-energy-resolution fluorescence detection-X-ray absorption near edge structure (HERFD-XANES) spectroscopy at the U L$$_{3}$$-edge, which is a novel technique in the U(V) compounds. Theoretical calculations revealed that the peak splitting was caused by splitting the 6d orbital of U(V). Such distinctive electronic states are of major interest to researchers and engineers working in various fields, from fundamental physics to the nuclear industry and environmental sciences for actinide elements.

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

https://doi.org/10.1016/j.jnucmat.2022.153847
 Times Cited Count：3 Percentile：66.21(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

https://doi.org/10.1016/j.jnucmat.2022.153842
 Times Cited Count：5 Percentile：76.47(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

https://doi.org/10.1080/00223131.2021.2023055
 Times Cited Count：2 Percentile：50.96(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

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

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

https://doi.org/10.1039/D1RA05580A
 Times Cited Count：5 Percentile：36.83(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

https://doi.org/10.1080/00223131.2020.1854881
 Times Cited Count：7 Percentile：65.65(Nuclear Science & Technology)

Journal Articles

Extreme ultraviolet free electron laser seeded with high-order harmonic of Ti:sapphore laser

Togashi, Tadashi*; Takahashi, Eiji*; Midorikawa, Katsumi*; Aoyama, Makoto; Yamakawa, Koichi; Sato, Takahiro*; Iwasaki, Atsushi*; Owada, Shigeki*; Okino, Tomoya*; Yamanouchi, Kaoru*; et al.

Optics Express (Internet), 19(1), p.317 - 324, 2011/01

https://doi.org/10.1364/OE.19.000317
 Times Cited Count：96 Percentile：96.43(Optics)

The 13th harmonic of a Ti:sapphire (Ti:S) laser in the plateau region was injected as a seeding source to a 250-MeV free-electron-laser (FEL) amplifier. When the amplification conditions were fulfilled, strong enhancement of the radiation intensity by a factor of 650 was observed. The random and uncontrollable spikes, which appeared in the spectra of the Self-Amplified Spontaneous Emission (SASE) based FEL radiation without the seeding source, were found to be suppressed drastically to form to a narrow-band, single peak profile at 61.2 nm. The properties of the seeded FEL radiation were well reproduced by numerical simulations. We discuss the future precept of the seeded FEL scheme to the shorter wavelength region.

Journal Articles

Ultra-fast pulse radiolysis; A Review of the recent system progress and its application to study on initial yields and solvation processes of solvated electrons in various kinds of alcohols

Muroya, Yusa*; Lin, M.; Han, Z.*; Kumagai, Yuta; Sakumi, Akira*; Ueda, Toru*; Katsumura, Yosuke

Radiation Physics and Chemistry, 77(10-12), p.1176 - 1182, 2008/10

https://doi.org/10.1016/j.radphyschem.2008.05.035
 Times Cited Count：18 Percentile：74.42(Chemistry, Physical)

In order to study radiation-induced fast phenomena, a new pulse radiolysis system with higher time resolution based on pulse-and-probe method was developed and utilized for practical work. A few picosecond electron beam generated from a linear accelerator, in which a laser photocathode RF-gun is introduced, was synchronized with a femtosecond laser pulse which is employed as the analyzing light. The synchronization precision between them was suppressed within 1.6 ps (rms). Converting the fundamental laser into white light continuum or optical parametric amplification allows to measure in the wide wavelength from visible to infrared region.

Journal Articles

Instability of synchronization between laser and beam depending on environmental noise at photocathode RF gun

Uesaka, Mitsuru*; Iijima, Hokuto; Ueda, Toru*; Muroya, Yusa*; Sakumi, Akira*; Kumagai, Noritaka*; Tomizawa, Hiromitsu*

Proceedings of 1st Annual Meeting of Particle Accelerator Society of Japan and 29th Linear Accelerator Meeting in Japan, p.628 - 630, 2004/08

no abstracts in English

Journal Articles

Spatial variation of D$$alpha$$ line spectral profile and emission process in the divertor region of JT-60U

Kumagai, Akira*; Kubo, Hirotaka; Takenaga, Hidenobu; Suzuki, Shingo; Shimizu, Katsuhiro; Asakura, Nobuyuki; Shimada, Michiya

Plasma Physics and Controlled Fusion, 42(5), p.529 - 543, 2000/05

https://doi.org/10.1088/0741-3335/42/5/304
 Times Cited Count：13 Percentile：39.64(Physics, Fluids & Plasmas)

no abstracts in English

Journal Articles

Spectroscopic study of JT-60U divertor plasma

Kubo, Hirotaka; Higashijima, Satoru; Takenaga, Hidenobu; Kumagai, Akira*; Shimizu, Katsuhiro; Sugie, Tatsuo; Suzuki, Shingo; Sakasai, Akira; Asakura, Nobuyuki

NIFS-PROC-44, p.65 - 68, 2000/01

no abstracts in English

JAEA Reports

Transport studies in boundary and divertor plasmas of JT-60U

Kumagai, Akira*

JAERI-Research 99-017, 151 Pages, 1999/03

JAERI-Research-99-017.pdf:6.39MB

no abstracts in English

Journal Articles

Carbon impurity behavior in W-shaped pumped divertor of JT-60U

Higashijima, Satoru; Kubo, Hirotaka; Sugie, Tatsuo; Shimizu, Katsuhiro; Sakasai, Akira; Asakura, Nobuyuki; Sakurai, Shinji; Hosogane, Nobuyuki; Konoshima, Shigeru; Tamai, Hiroshi; et al.

Journal of Nuclear Materials, 266-269, p.1078 - 1083, 1999/00

https://doi.org/10.1016/S0022-3115(98)00562-5
 Times Cited Count：7 Percentile：49.64(Materials Science, Multidisciplinary)

no abstracts in English

Journal Articles

Operational performance of JT-60U W-shaped divertor

Hosogane, Nobuyuki; Tamai, Hiroshi; Higashijima, Satoru; Kubo, Hirotaka; Sakasai, Akira; Takenaga, Hidenobu; Itami, Kiyoshi; Sakurai, Shinji; Asakura, Nobuyuki; Konoshima, Shigeru; et al.

Journal of Nuclear Materials, 266-269, p.296 - 301, 1999/00

https://doi.org/10.1016/S0022-3115(98)00820-4
 Times Cited Count：14 Percentile：70.45(Materials Science, Multidisciplinary)

no abstracts in English

Journal Articles

The Spectral profile of the He I singlet line (667.82nm) emitted from the divertor region of JT-60U

Kubo, Hirotaka; Takenaga, Hidenobu; Kumagai, Akira*; Higashijima, Satoru; Suzuki, Shingo*; Sugie, Tatsuo; Sakasai, Akira; Itami, Kiyoshi

Plasma Physics and Controlled Fusion, 41(6), p.747 - 757, 1999/00

https://doi.org/10.1088/0741-3335/41/6/304
 Times Cited Count：20 Percentile：55(Physics, Fluids & Plasmas)

no abstracts in English

50 (Records 1-20 displayed on this page)