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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

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

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

Current status of Geological disposal by "all-Japan" activities, 6; Post-closure safety assessment (2)

Tachi, Yukio; Saito, Takumi*; Kirishima, Akira*

Nihon Genshiryoku Gakkai-Shi ATOMO$$Sigma$$, 64(5), p.290 - 295, 2022/05

no abstracts in English

Journal Articles

Deep groundwater physicochemical components affecting actinide migration

Kirishima, Akira*; Terasaki, Mariko*; Miyakawa, Kazuya; Okamoto, Yoshihiro; Akiyama, Daisuke*

Chemosphere, 289, p.133181_1 - 133181_12, 2022/04

no abstracts in English

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

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, 11 Pages, 2022/03

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

Speciation on the reaction of uranium and zirconium oxides treated under oxidizing and reducing atmospheres

Uehara, Akihiro*; Akiyama, Daisuke*; Ikeda, Atsushi; Numako, Chiya*; Terada, Yasuko*; Nitta, Kiyofumi*; Ina, Toshiaki*; Takeda-Homma, Shino*; Kirishima, Akira*; Sato, Nobuaki*

Journal of Nuclear Materials, 559, p.153422_1 - 153422_11, 2022/02

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro

2020-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), 1 Pages, 2021/11

no abstracts in English

Journal Articles

Summary results of subsidy program for the "Project of Decommissioning and Contaminated Water Management (Development of Analysis and Estimation Technology for Characterization of Fuel Debris (Development of Technologies for Enhanced Analysis Accuracy and Thermal Behavior Estimation of Fuel Debris))"

Koyama, Shinichi; Nakagiri, Toshio; Osaka, Masahiko; Yoshida, Hiroyuki; Kurata, Masaki; Ikeuchi, Hirotomo; Maeda, Koji; Sasaki, Shinji; Onishi, Takashi; Takano, Masahide; et al.

Hairo, Osensui Taisaku jigyo jimukyoku Homu Peji (Internet), 144 Pages, 2021/08

JAEA performed the subsidy program for the "Project of Decommissioning and Contaminated Water Management (Development of Analysis and Estimation Technology for Characterization of Fuel Debris (Development of Technologies for Enhanced Analysis Accuracy and Thermal Behavior Estimation of Fuel Debris))" in 2020JFY. This presentation summarized briefly the results of the project, which will be available shortly on the website of Management Office for the Project of Decommissioning and Contaminated Water Management.

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:0

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:0 Percentile:0.01(Nuclear Science & Technology)

Journal Articles

The Chemistry of uranium (II); Method and practice

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*

Uran No Kagaku (II); Hoho To Jissen, 143 Pages, 2021/03

This book describes necessary facts when readers would have an opportunity to treat Uranium for experiments. In the content, the method section shows experimental facilities and equipment including method, and the practical section mentions solution and solid state experiments using Uranium and/or radioisotopes.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro

2019-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), P. 20191107_1, 2020/11

no abstracts in English

Journal Articles

The Chemistry of uranium (I); Basics and application

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki

Uran No Kagaku (I); Kiso To Oyo, 184 Pages, 2020/06

This particular book deals with fundamental items related with chemistry of Uranium and consists of basic section and practical section. In the basic section, inorganic and radiochemistry of Uranium was described. On the other hand, in the practical section, the process chemistry related with reprocessing of nuclear fuels and "debris" involved with Fukushima Daiichi Power Plant accident were described. This book is intended for use by scientists, engineers and students in the nuclear industry in their education and/or professional practice.

Journal Articles

Thermodynamic study of the complexation of humic acid by calorimetry

Kimuro, Shingo; Kirishima, Akira*; Kitatsuji, Yoshihiro; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Chemical Thermodynamics, 132, p.352 - 362, 2019/05

 Times Cited Count:6 Percentile:53.99(Thermodynamics)

A combination of potentiometry and calorimetry was used for the determination of the thermodynamic quantities of complexation of generic and groundwater humic acid (HA), which was isolated from deep groundwater at Horonobe, Hokkaido, Japan, with copper (II) ions and uranyl (VI) ions. The apparent complexation constant of Horonobe HA was independent of the pH, whereas that of generic HA was dependent on the pH. This observation indicates that the polyelectrolyte effect of Horonobe HA is negligible because of its small molecular size. In addition, the effect of the heterogeneity of Horonobe HA was not significant. Moreover, the complexation enthalpy of Horonobe HA was consistent with that of homogeneous poly(acrylic acid), which means the complexation of Horonobe HA was not affected by the functional group heterogeneity. Consequently, the characteristic complexation mechanism of Horonobe HA was revealed based on the determined thermodynamic quantities.

Journal Articles

Characterization and thermodynamic study of humic acid in deep groundwater at Horonobe, Hokkaido, Japan

Kimuro, Shingo*; Kirishima, Akira*; Nagao, Seiya*; Saito, Takumi*; Amano, Yuki; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Nuclear Science and Technology, 55(5), p.503 - 515, 2018/05

 Times Cited Count:3 Percentile:45.99(Nuclear Science & Technology)

no abstracts in English

Journal Articles

Determination of dissolved natural thorium and uranium in Horonobe and Mizunami Underground Research Laboratory groundwater and its thermodynamic analysis

Sasaki, Takayuki*; Kokami, Takayuki*; Kobayashi, Taishi*; Kirishima, Akira*; Murakami, Hiroaki; Amano, Yuki; Mizuno, Takashi; Iwatsuki, Teruki; Sasamoto, Hiroshi; Miyakawa, Kazuya

Journal of Nuclear Science and Technology, 54(3), p.373 - 381, 2017/03

Trace amounts of natural thorium and uranium in deep groundwater were investigated at two underground research laboratories situated at Horonobe and Mizunami, Japan. The groundwater was sampled from underground boreholes, and the colloid contribution was checked by in situ two size-fractionated ultrafiltration systems. A decrease in the concentration after in situ filtration suggested the presence of natural colloids and suspended matter that were carriers of a portion of the elements. The result of the Th and U concentrations in groundwater after 10 kDa filtration was analyzed thermodynamically using existing hydrogeological and geochemical data such as the mineral components in the groundwater at a given pH, ionic strength, concentration of co-existing ions, redox potential, and solid phase assumed. A crystalline solid phase made the solubility very low compared with that of the amorphous phase, and the solubility agreed well with the concentrations measured.

Journal Articles

Interaction of rare earth elements and components of the Horonobe deep groundwater

Kirishima, Akira*; Kuno, Atsushi*; Amamiya, Hiroki; Kubota, Takumi*; Kimuro, Shingo*; Amano, Yuki; Miyakawa, Kazuya; Iwatsuki, Teruki; Mizuno, Takashi; Sasaki, Takayuki*; et al.

Chemosphere, 168, p.798 - 806, 2017/02

 Times Cited Count:1 Percentile:5.42(Environmental Sciences)

For better understanding of the migration behavior of minor actinides (MA) in deep groundwater, the interaction of doped rare earth elements (REEs) and components in Horonobe deep groundwater was studied. Appx. 10 ppb of rare earth elements, i.e., Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Er, Tm and Yb were doped to the sample groundwater collected from a packed sections in borehole drilled from 140 m depth experiment drift of Horonobe underground research laboratory (URL), Hokkaido, Japan. Then, that groundwater was sequentially filtrated by 0.2 micron pore filter, 10 kDa, 3 kDa and 1 kDa of nominal molecular weight limit (NMWL) ultrafilters by keeping inert condition. After that, the filtrate solutions were analyzed by ICP-MS to determine the concentrations of retained REEs at each filtration steps, while the used filters were analyzed by the neutron activation analysis (NAA) and TOF-SIMS element mapping to know the amount and chemical speciation of trapped fraction of the REEs on each filter. A remarkable relation between the retention ratios of REEs in the filtrate solutions and the ionic radius was observed, i.e., smaller rare earth element solves more in liquid phase under the Horonobe groundwater condition. NAA and TOF-SIMS analyses revealed that certain portions of REEs were trapped by 0.2 micron pore filters as rare earth phosphates which corresponded with the predicted predominant species by a chemical equilibrium calculation for the Horonobe groundwater condition, while small portions of colloidal REEs were trapped by 10 kDa and 3 kDa NMWL ultrafilters. The result suggested that phosphate anion plays an important role in the chemical behavior of REEs in saline (seawater based) groundwater, which could be referred for the prediction of migration behavior of trivalent actinide released from the repository of radioactive waste in far future.

Journal Articles

Recent activities in the field of nuclear waste management

Kitamura, Akira; Kirishima, Akira*

Journal of Nuclear Science and Technology, 52(3), p.448 - 450, 2015/03

 Times Cited Count:1 Percentile:88.84(Nuclear Science & Technology)

The Journal of Nuclear Science and Technology covers a variety of subjects in the field of nuclear waste management, which includes radioactive waste treatment, radioactive waste disposal and environment, decommissioning and dismantling. This summary introduces activities presented in recent years.

Journal Articles

Optical properties of tetravalent uranium complexes in non-aqueous media

Aoyagi, Noboru; Watanabe, Masayuki; Kirishima, Akira*; Sato, Nobuaki*; Kimura, Takaumi

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1095 - 1098, 2015/02

 Times Cited Count:4 Percentile:40.75(Chemistry, Analytical)

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