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JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 3 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2023-004, 45 Pages, 2023/09

JAEA-Research-2023-004.pdf:6.07MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. To understand the chemical stability of simulated waste glasses, XANES spectra of B K-edge, Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge were measured on the glass surface exposed to the leachate. As a result, it was found that the glass surface exposed to the leachate was changed and it was difficult to obtain a clear XANES spectrum. From the B K-edge XANES spectra on glass surfaces exposed to the leachate, an increase in three-coordination of B-O (BO$$_{3}$$) and a decrease in four-coordination of B-O (BO$$_{4}$$) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge show that as the exposure time in the leachate increases, the Cs present on the glass surface dissolves into the leachate. The XANES spectra of Si K-edge were measured on simulated waste glass surfaces before immersion, and it was confirmed that the change in XANES spectra given by Na$$_{2}$$O concentration had a larger effect than the waste component concentration.

JAEA Reports

Acquisition of saltwater infiltration behavior data in unsaturated compacted bentonite

Sato, Hisashi*; Takayama, Yusuke; Suzuki, Hideaki*; Sato, Daisuke*

JAEA-Data/Code 2023-010, 47 Pages, 2023/09

JAEA-Data-Code-2023-010.pdf:1.45MB

When a high-level radioactive waste repository is constructed in a coastal area, it is necessary to fully evaluate the impact of seawater-based groundwater on engineered barriers, including buffer materials. In this report, one-dimensional saltwater infiltration tests were conducted to obtain data to understand the impact of seawater-based groundwater on the migration phenomena of water and solutes in the buffer material during the transient period. As a result, it was confirmed that the infiltration rate increased as the NaCl concentration in the infiltration solution increased. And it was confirmed that the water content ratio distribution changed as the NaCl concentration in the infiltration solution increased. As a result of analysis of the chloride ion concentration of the post-test specimens confirmed that chloride ion enrichment was occurred with infiltration. As a result of verifying the mechanism by which chloride ion enrichment occurs, it was confirmed that the phenomenon of chloride ion enrichment due to infiltration depends on the initial water content ratio.

Journal Articles

Investigation of the electronic structure of the Mg$$_{99.2}$$Zn$$_{0.2}$$Y$$_{0.6}$$ alloy using X-ray photoelectron spectroscopy

Miyazaki, Hidetoshi*; Akatsuka, Tatsuyoshi*; Kimura, Koji*; Egusa, Daisuke*; Sato, Yohei*; Itakura, Mitsuhiro; Takagi, Yasumasa*; Yasui, Akira*; Ozawa, Kenichi*; Mase, Kazuhiko*; et al.

Materials Transactions, 64(6), p.1194 - 1198, 2023/06

We investigated the electronic structure of the Mg$$_{99.2}$$Zn$$_{0.2}$$Y$$_{0.6}$$ alloy using hard and soft X-ray photoemission spectroscopy and electronic band structure calculations to understand the mechanism of the phase stability of this material. Electronic structure of the Mg$$_{99.2}$$Zn$$_{0.2}$$Y$$_{0.6}$$ alloy showed a semi-metallic electronic structure with a pseudo-gap at the Fermi level. The observed electronic structure of the Mg$$_{99.2}$$Zn$$_{0.2}$$Y$$_{0.6}$$ alloy suggests that the presence of a pseudogap structure is responsible for phase stability.

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:33.72(Nuclear Science & Technology)

Journal Articles

STEM-EELS/EDS chemical analysis of solute clusters in a dilute mille-feuille-type Mg-Zn-Y alloy

Sato, Yohei*; Egusa, Daisuke*; Miyazaki, Hidetoshi*; Kimura, Koji*; Itakura, Mitsuhiro; Terauchi, Masami*; Abe, Eiji*

Materials Transactions, 64(5), p.950 - 954, 2023/05

Dilute Mg-Zn-Y alloy with a mille-feuille structure (MFS) exhibits a mechanical strength comparable to Mg-Zn-Y alloy with long period stacking/ordered (LPSO) structure through kink deformation. In order to deepen understanding the thermal stability of the MFS-type Mg alloys, it is required to clarify the solute cluster structures composed of Zn and Y in solute enriched stacking faults (SESFs). In this study, electron energy-loss and energy dispersive X-ray spectroscopy based on scanning transmission electron microscopy (STEM-EELS/EDS) were conducted to investigate the electronic structure and composition of Zn and Y in the SESFs of the MFS-Mg alloy. Zn-L2,3 spectra indicated that the valence charges of Zn in the dilute Mg alloy were different from that of the LPSO-type Mg-Zn-Y alloy. In addition, the intensity ratio of L3/L2 in Y-L2,3 spectrum of the dilute MFS-Mg alloy was larger than that of the LPSO-Mg alloy, reflecting the electron occupancies of 4d3/2 and 4d5/2 orbitals of Y atoms were different from those of the LPSO-Mg alloys. STEM-EELS analysis of the SESF composition in the dilute MFS-Mg alloy indicated that the Zn/Y ratio should be lower than that of the LPSO-Mg alloy, which was confirmed also by STEM-EDS measurements. These results indicate that the cluster structure in the SESFs of the dilute MFS-Mg alloy should be different from the ideal Zn6Y8 cluster in the LPSO-type Mg-Zn-Y alloys.

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:75.85(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

Multiple mechanisms in proton-induced nucleon removal at $$sim$$100 MeV/nucleon

Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; G$'o$mez-Ramos, M.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Cai, B. S.*; Yuan, C. X.*; Brown, B. A.*; et al.

Physical Review Letters, 130(17), p.172501_1 - 172501_8, 2023/04

 Times Cited Count:2 Percentile:90.46(Physics, Multidisciplinary)

We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient $$^{14}$$O nucleus with large Fermi-surface asymmetry at $$sim$$100 MeV/nucleon. Our results provide the first quantitative contributions of multiple reaction mechanisms including the quasifree knockout, inelastic scattering, and nucleon transfer processes. It is shown that the inelastic scattering and nucleon transfer, usually neglected at such energy regime, contribute about 50% and 30% to the loosely bound proton and deeply bound neutron removal, respectively.

JAEA Reports

Assessment of the infiltration behaviour of buffer material in seawater-type groundwater environments using a coupled THMC analysis model (Contract research)

Suzuki, Hideaki*; Takayama, Yusuke; Sato, Hisashi*; Watahiki, Takanori*; Sato, Daisuke*

JAEA-Research 2022-013, 41 Pages, 2023/03

JAEA-Research-2022-013.pdf:3.99MB

It is anticipated that the coupled thermal-hydraulic-mechanical and chemical (THMC) processes will occur, involving an interactive process with radioactive decay heat arising from the vitrified waste, infiltration of groundwater from the host rock into the buffer material, swelling pressure of buffer material due to its saturation and chemical reaction between bentonite and pore-water in the near-field of a geological disposal system for high-level radioactive waste repository. In order to evaluate these phenomena in the near-field, the THMC model has been developed. In this study, For the purpose of evaluating the near-field infiltration behavior in seawater-type groundwater environment, a hydraulic model was set in which the permeability of the buffer material change depending on the salt concentration in the pore-water. In order to evaluate the drying phenomenon of the buffer material due to waste heat, a temperature gradient water transfer model was set in consideration of the dependence of temperature and pore-water saturation. The THMC analysis of the in-situ experiment of engineered barrier system (EBS) experiment at the Horonobe Underground Research Laboratory was carried out. The validity of the model was then checked through comparison with measured data.

Journal Articles

Effect of collapse behavior on changes in swelling pressure of bentonite during swelling pressure test

Takayama, Yusuke; Sato, Daisuke*; Kikuchi, Hirohito*

Genshiryoku Bakkuendo Kenkyu (CD-ROM), 29(2), p.101 - 111, 2022/12

Swelling pressure tests have been conducted to understand the swelling properties of bentonite which is planned to be used as a buffer material in repositories for the geological disposal of radioactive waste. It has been reported that the swelling pressure obtained by swelling pressure test increases monotonically or temporarily decreases after increasing with the passage of the time depending on the initial water content. In this study, swelling pressure tests were conducted under several different initial water content conditions, and the change in wet density distribution inside the specimen during the swelling pressure tests was observed by X-ray CT measurement. It was confirmed that the presence or absence of collapse behavior and its magnitude affect the shape of the change in swelling pressure. When the collapse deformation was large, the amount of temporary decrease in swelling pressure was large. On the other hand, swelling pressure increased monotonically when there was no deformation due to collapse.

Journal Articles

Spatial distribution and preferred orientation of crystalline microstructure of lead-bismuth eutectic

Ito, Daisuke*; Sato, Hirotaka*; Odaira, Naoya*; Saito, Yasushi*; Parker, J. D.*; Shinohara, Takenao; Kai, Tetsuya; Oikawa, Kenichi

Journal of Nuclear Materials, 569, p.153921_1 - 153921_6, 2022/10

 Times Cited Count:1 Percentile:33.72(Materials Science, Multidisciplinary)

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:71.05(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:80.29(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:56.43(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

Quantitative X-ray diffraction analysis of solute-enriched stacking faults in $$hcp$$-Mg alloys based on peak asymmetry analysis

Egusa, Daisuke*; Manabe, Ryo*; Kawasaki, Takuro; Harjo, S.; Sato, Shigeo*; Abe, Eiji*

Materials Today Communications (Internet), 31, p.103344_1 - 103344_6, 2022/06

 Times Cited Count:4 Percentile:62.5(Materials Science, Multidisciplinary)

JAEA Reports

Stabilization treatment of nuclear fuel material contained with organic matter

Senzaki, Tatsuya; Arai, Yoichi; Yano, Kimihiko; Sato, Daisuke; Tada, Kohei; Ogi, Hiromichi*; Kawanobe, Takayuki*; Ono, Shimpei; Nakamura, Masahiro; Kitawaki, Shinichi; et al.

JAEA-Testing 2022-001, 28 Pages, 2022/05

JAEA-Testing-2022-001.pdf:2.33MB

In preparation for the decommissioning of Laboratory B of the Nuclear Fuel Cycle Engineering Laboratory, the nuclear fuel material that had been stored in the glove box for a long time was moved to the Chemical Processing Facility (CPF). This nuclear fuel material was stored with sealed by a polyvinyl chloride (PVC) bag in the storage. Since it was confirmed that the PVC bag swelled during storage, it seems that any gas was generated by radiolysis of the some components contained in the nuclear fuel material. In order to avoid breakage of the PVC bag and keep it safety for long time, we began the study on the stabilization treatment of the nuclear fuel material. First, in order to clarify the properties of nuclear fuel material, radioactivity analysis, component analysis, and thermal analysis were carried out. From the results of thermal analysis, the existence of organic matter was clarified. Then, ion exchange resin with similar thermal characteristics was selected and the thermal decomposition conditions were investigated. From the results of these analyzes and examinations, the conditions for thermal decomposition of the nuclear fuel material contained with organic matter was established. Performing a heat treatment of a small amount of nuclear fuel material in order to confirm the safety, after which the treatment amount was scaled up. It was confirmed by the weight change after the heat treatment that the nuclear fuel material contained with organic matter was completely decomposed.

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

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

 Times Cited Count:2 Percentile:56.43(Materials Science, Multidisciplinary)

Journal Articles

Validation of ATDMs at early after the lF accident using air dose rate estimated by airborne concentration and surface deposition density

Moriguchi, Yuichi*; Sato, Yosuke*; Morino, Yu*; Goto, Daisuke*; Sekiyama, Tsuyoshi*; Terada, Hiroaki; Takigawa, Masayuki*; Tsuruta, Haruo*; Yamazawa, Hiromi*

KEK Proceedings 2021-2, p.21 - 27, 2021/12

no abstracts in English

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

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:67.5(Nuclear Science & Technology)

219 (Records 1-20 displayed on this page)