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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

Design of MA(III)/Ln(III) separation process of extraction chromatography technology

Akuzawa, Tadashi*; Kim, S.-Y.*; Kubota, Masahiko*; Wu, H.*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5851 - 5858, 2022/12

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

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:1 Percentile:71.47(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:2 Percentile:88.59(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:1 Percentile:71.47(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:1 Percentile:60.17(Chemistry, Physical)

Journal Articles

Geochemical and grain composition analysis of embankment and debris flow deposits in the Izusan area, Atami City, Shizuoka Prefecture, central Japan

Kitamura, Akihisa*; Okazaki, Sota*; Kondo, Mitsuru*; Watanabe, Takahiro; Nakanishi, Toshimichi*; Hori, Rie*; Ikeda, Masayuki*; Ichimura, Koji; Nakagawa, Yuki; Mori, Hideki*

Shizuoka Daigaku Chikyu Kagaku Kenkyu Hokoku, (49), p.73 - 86, 2022/07

On July 3 2021, a debris flow caused by a landslide from a landfill occurred along the Aizome River in the Izusan area of Atami City, Shizuoka. In this study, debris flow deposits and soil samples were characterized in terms of their sedimentology and geochemically analyzed.

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

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:0.01(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.

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


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

Zeolite-assisted radiolysis of aromatic chlorides mitigating influence of coexisting ions in water matrix

Kumagai, Yuta; Kimura, Atsushi*; Taguchi, Mitsumasa*; Watanabe, Masayuki

Radiation Physics and Chemistry, 191, p.109831_1 - 109831_8, 2022/02

 Times Cited Count:0 Percentile:0.01(Chemistry, Physical)

In this study, we investigated and compared the effects of a high-silica zeolite (HMOR) on the radiation-induced degradation of three aromatic chlorides, 2-chlorophenol (2-ClPh), 2-chloroaniline (2-ClAn), and 2-chlorobenzoic acid (2-ClBA), in order to examine its potential to reduce the influence of ions in water matrix in the irradiation treatment of water-soluble organic compounds. In the presence of ions reactive to radicals, the degradation of 2-ClPh in water was inhibited, but the combined use of HMOR much improved the degradation yield. This improvement was attributed to high performance of HMOR in adsorption of 2-ClPh. Similarly, HMOR was effective for adsorption of 2-ClAn and facilitated the 2-ClAn degradation by irradiation. In contrast, HMOR was poor at adsorption of 2-ClBA and consistently the degradation of 2-ClBA in the water-HMOR mixture was inhibited by the radical scavenger. These results demonstrate that HMOR can mitigate the influence of radical scavengers in water.

Journal Articles

Structural characterization by X-ray analytical techniques of calcium aluminate cement modified with sodium polyphosphate containing cesium chloride

Takahatake, Yoko; Watanabe, So; Irisawa, Keita; Shiwaku, Hideaki; Watanabe, Masayuki

Journal of Nuclear Materials, 556, p.153170_1 - 153170_7, 2021/12

 Times Cited Count:1 Percentile:30.57(Materials Science, Multidisciplinary)

Journal Articles

Coherent eddies transporting passive scalars through the plant canopy revealed by Large-Eddy simulations using the lattice Boltzmann method

Watanabe, Tsutomu*; Takagi, Marie*; Shimoyama, Ko*; Kawashima, Masayuki*; Onodera, Naoyuki; Inagaki, Atsushi*

Boundary-Layer Meteorology, 181(1), p.39 - 71, 2021/10

 Times Cited Count:4 Percentile:47.23(Meteorology & Atmospheric Sciences)

A double-distribution-function lattice Boltzmann model for large-eddy simulations of a passive scalar field is described within and above a plant canopy. For a top-down scalar, for which the plant canopy serves as a distributed sink, the flux of the scalar near the canopy top are predominantly determined by sweep motions originating far above the canopy. By contrast, scalar ejection events are induced by coherent eddies generated near the canopy top. In this paper, the generation of such eddies is triggered by the downward approach of massive sweep motions to existing wide regions of weak ejective motions from inside to above the canopy.

Journal Articles

Development of MA separation process with TEHDGA/SiO$$_{2}$$-P for an advanced reprocessing

Horiuchi, Yusuke; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Kida, Fukuka*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.237 - 244, 2021/10

 Times Cited Count:1 Percentile:30.57(Chemistry, Analytical)

Applicability of tetra2-ehylhexyl diglycolamide (TEHDGA) impregnated adsorbent for minor actinide (MA) recovery from high level liquid waste (HLLW) in extraction chromatography technology was investigated through batch-wise adsorption and column separation experiments. Distribution ratio of representative fission product elements were obtained by the batch-wise experiments, and TEHDGA adsorbent was shown to be preferable to TODGA adsorbent for decontamination of several species. All Ln(III) supplied into the TEHDGA adsorbent packed column was properly eluted from the column, and the applicability of the adsorbent was successfully showed by this study.

JAEA Reports

Carrying-out of whole nuclear fuel materials in Plutonium Research Building No.1

Inagawa, Jun; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Nakada, Masami; Takano, Masahide; Akie, Hiroshi; Shimizu, Osamu; Komuro, Michiyasu; Oura, Hirofumi*; Nagai, Isao*; et al.

JAEA-Technology 2021-001, 144 Pages, 2021/08


Plutonium Research Building No.1 (Pu1) was qualified as a facility to decommission, and preparatory operations for decommission were worked by the research groups users and the facility managers of Pu1. The operation of transportation of whole nuclear materials in Pu1 to Back-end Cycle Key Element Research Facility (BECKY) completed at Dec. 2020. In the operation included evaluation of criticality safety for changing permission of the license for use nuclear fuel materials in BECKY, cask of the transportation, the registration request of the cask at the institute, the test transportation, formulation of plan for whole nuclear materials transportation, and the main transportation. This report circumstantially shows all of those process to help prospective decommission.

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:2 Percentile:30.08(Chemistry, Multidisciplinary)

Journal Articles

Electrochemical studies of uranium (IV) in an ionic liquid-DMF mixture to build a redox flow battery using uranium as an electrode active material

Ouchi, Kazuki; Komatsu, Atsushi; Takao, Koichiro*; Kitatsuji, Yoshihiro; Watanabe, Masayuki

Chemistry Letters, 50(6), p.1169 - 1172, 2021/06

 Times Cited Count:0 Percentile:0(Chemistry, Multidisciplinary)

The electrochemical behavior of uranium (IV) tetrachloride in ionic liquid-DMF mixture was studied for first time in order to build a redox flow battery (RFB) using U as an electrode active material. We found a quasi-reversible U$$^{III}$$/U$$^{IV}$$ couple that could be applied to the anode reaction of the RFB.

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:5 Percentile:67.23(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:6 Percentile:58.16(Chemistry, Physical)

434 (Records 1-20 displayed on this page)