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Journal Articles

Durability of U-Zr oxide solid solution in aqueous H$$_2$$O$$_2$$ solution

Kumagai, Yuta; Kusaka, Ryoji; Takano, Masahide; Watanabe, Masayuki

Journal of Nuclear Materials, 625, p.156553_1 - 156553_7, 2026/04

https://doi.org/10.1016/j.jnucmat.2026.156553
 Times Cited Count：0 Percentile：0.00

Uranium-zirconium oxide solid solution, (U, Zr)O$$_2$$, is a representative matrix phase found in fuel debris formed during severe nuclear reactor accidents. Understanding its chemical behavior in oxidative aqueous environments is important for evaluating the potential release of radionuclides during water contact. In this study, we investigated the reactivity of (U, Zr)O$$_2$$ with hydrogen peroxide (H$$_2$$O$$_2$$) in pure water to assess its resistance to oxidative dissolution, because H$$_2$$O$$_2$$ is the dominant oxidant produced by water radiolysis. The dissolution behavior of uranium and zirconium was monitored through repeated H$$_2$$O$$_2$$ exposure experiments, and the solid phases were characterized using Raman micro-spectroscopy and X-ray diffraction. Kinetic modeling was performed to interpret experimental data. The results showed that uranium dissolution occurred initially but decreased significantly upon repeated H$$_2$$O$$_2$$ exposure, while zirconium dissolution proceeded more slowly. Raman analysis revealed only minor surface changes, with limited formation of uranyl peroxide phases. The kinetic simulation reproduced the experimental trends by assuming a small fraction of redox-active surface sites. These findings suggest that the observed durability of (U, Zr)O$$_2$$ against H$$_2$$O$$_2$$-induced oxidative dissolution is not due to the formation of a protective surface layer, but rather reflects the limited redox reactivity of most of the surface. This study provides a quantitative basis for understanding the H$$_2$$O$$_2$$-induced oxidation of (U, Zr)O$$_2$$ in water, relevant to the long-term behavior of fuel debris.

Journal Articles

A Basic study for radioactive nuclides recovery from spent PUREX solvent using adsorbents

Arai, Tsuyoshi*; Nakamura, Fumiya*; Abe, Ryoji*; Ueno, Fuga*; Seko, Noriaki*; Arai, Yoichi; Watanabe, So

Progress in Nuclear Science and Technology (Internet), 7, p.147 - 153, 2025/03

https://doi.org/10.15669/pnst.7.147

no abstracts in English

Journal Articles

Degradation of a lithium cobalt oxide cathode under high voltage operation at an interface with an oxide solid electrolyte

Ito, Kotaro*; Tamura, Kazuhisa; Shimizu, Keisuke*; Yamada, Norifumi*; Watanabe, Kenta*; Suzuki, Kota*; Kanno, Ryoji*; Hirayama, Masaaki*

RSC Applied Interfaces (Internet), 1(4), p.790 - 799, 2024/04

https://doi.org/10.1039/D3LF00251A

LiCoO$$_{2}$$ is widely used as a cathode material in lithium-ion batteries. However, the reversible capacity of LiCoO$$_{2}$$ at high voltage is not well known because of the oxidative degradation of the electrolyte. In this study, a thin-film all-solid-state battery was fabricated with epitaxially grown LiCoO$$_{2}$$ cathode and Li$$_{3}$$PO$$_{4}$$ solid electrolyte as a model battery that operates stably at high voltages, ranging up to 4.6 V, without drastic degradation. However, the charge-discharge capacities of the battery decreased with cycling at 4.7 V. ${it In situ}$ synchrotron X-ray diffraction studies revealed that LiCoO$$_{2}$$ was deactivated via a change in its crystal structure to O1 type, with narrow interlayer distances, at 4.7 V. The reduced distance between the interlayers in the O1 structure possibly prevents the re-intercalation of Li ions, leading to irreversibility.

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

https://doi.org/10.1039/D3SE01636F
 Times Cited Count：2 Percentile：19.40(Chemistry, Physical)

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

https://doi.org/10.1021/acs.nanolett.3c03982
 Times Cited Count：4 Percentile：47.83(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

Two-dimensional metal-organic nanosheets composed of single-molecule magnets; Structural modulation and enhanced magnetism utilizing the steric hindrance effect

Aratani, Ikumi*; Horii, Yoji*; Kotani, Yoshinori*; Osawa, Hitoshi*; Tanida, Hajime; Ina, Toshiaki*; Watanabe, Takeshi*; Yano, Yoko*; Mizoguchi, Akane*; Takajo, Daisuke*; et al.

Journal of Materials Chemistry C, 12(2), p.724 - 735, 2024/01

https://doi.org/10.1039/D3TC03360K
 Times Cited Count：3 Percentile：24.10(Materials Science, Multidisciplinary)

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：8 Percentile：67.89(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：7 Percentile：76.13(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

https://doi.org/10.1021/acs.inorgchem.2c03618
 Times Cited Count：4 Percentile：28.77(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

https://doi.org/10.1016/j.jnucmat.2022.153847
 Times Cited Count：7 Percentile：62.74(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：11 Percentile：78.92(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：4 Percentile：41.78(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

https://doi.org/10.1021/acs.jpclett.2c01550
 Times Cited Count：11 Percentile：64.61(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

https://doi.org/10.1016/j.msea.2021.142531
 Times Cited Count：9 Percentile：47.16(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

https://doi.org/10.1080/00223131.2020.1854881
 Times Cited Count：11 Percentile：66.26(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

https://doi.org/10.1021/acs.jpcb.1c04583
 Times Cited Count：15 Percentile：66.17(Biophysics)

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

https://doi.org/10.1016/j.atmosenv.2020.117856
 Times Cited Count：5 Percentile：15.82(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

https://doi.org/10.1080/00223131.2020.1755734
 Times Cited Count：0 Percentile：0.00(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

https://doi.org/10.2116/analsci.19P155
 Times Cited Count：9 Percentile：30.01(Chemistry, Analytical)

109 (Records 1-20 displayed on this page)