Segawa, Tomoomi; Kawaguchi, Koichi; Ishii, Katsunori; Suzuki, Masahiro; Fukasawa, Tomonori*; Fukui, Kunihiro*
Funtai Kogakkai-Shi, 57(9), p.485 - 494, 2020/09
In the spent fuel reprocessing process, a mixed solution of uranyl nitrate and plutonium nitrate is converted into mixed oxide powder by the microwave heating. To evaluate the applicability to the industrial-scale and acquire the characteristics data of the microwave heating denitration of various metal nitrate aqueous solutions based on the knowledge studied in the development of laboratory-scale basic experiments, the microwave heating characteristics and metal oxide powder properties were investigated using cerium nitrate, cobalt nitrate and copper nitrate aqueous solutions. The progress rate of the denitration reaction was depended on the position, and the denitration reaction proceeded faster at the periphery than at the center. The morphologies of the synthesized products were porous and hard dry solid with cerium nitrate aqueous solution, foamed dry solid with cobalt nitrate aqueous solution, and powdery particles with copper nitrate aqueous solution. The denitration ratio and average particle size of the synthesized products increased in the order of the cerium nitrate aqueous solution, the cobalt nitrate aqueous solution, and the copper nitrate aqueous solution. The numerical simulations revealed that the periphery of the bottom surface of the metal nitrate aqueous solution was heated by microwaves. This results consistent with the experimental results in which the denitration reaction started from the periphery of the metal nitrate aqueous solution.
Ukai, Shigeharu*; Ono, Naoko*; Otsuka, Satoshi
Comprehensive Nuclear Materials, 2nd Edition, Vol.3, p.255 - 292, 2020/08
Fe-Cr-based oxide dispersion strengthened (ODS) steels have a strong potential for high burnup (long-life) and high-temperature applications typical for SFR fuel cladding. Current progress in the development of Fe-Cr-based ODS steel claddings is reviewed, including their relevant mechanical properties, e.g. tensile and creep rupture strengths in the hoop directions. In addition, this paper reviewed the current research status on corrosion resistant Fe-Cr-Al-based ODS steel claddings, which are greatly paid attention recently as the accident tolerant fuel claddings for the light water reactor (LWR) and also as the claddings of the lead fast reactors (LFR) utilizing Pb-Bi eutectic (LBE) coolant.
Comprehensive Nuclear Materials, 2nd Edition, Vol.4, p.528 - 563, 2020/08
In spent fuel reprocessing plants, various nitric media are encountered throughout the PUREX process, used in the separation of fission products, uranium, and plutonium. The PUREX process is thus highly corrosive as it takes place at high temperatures under high concentrations of nitric acid solution containing oxidizing metal ions from spent fuel. In this review, the unique chemical properties of nitric acid are first described. Secondly, the process of oxidizing power generation in boiling nitric acid under heat transfer is described using the redox potential and a thermodynamic model of boiling nitric acid. Finally, the corrosion behavior and corrosion acceleration mechanism specific to the reprocessing environments are described from the perspective of solution chemistry.
Furutani, Misa; Kometani, Tatsunari; Nakagawa, Masahiro; Ueno, Yumi; Sato, Junya; Iwai, Yasunori*
Hoken Butsuri (Internet), 55(2), p.97 - 101, 2020/06
Herein, an oxidation catalyst was introduced after heating it to 600C to oxidize tritium gas (HT) existing in exhaust into tritiated water vapor (HTO). This study aims to establish a safer H monitoring system by lowering the heating temperature required for the catalyst. In these experiments, which were conducted in the Nuclear Science Research Institute, Japan Atomic Energy Agency, cupric oxide, hydrophobic palladium/silicon dioxide (Pd/SiO), and platinum/aluminum oxide (Pt/AlO) catalysts were ventilated using standard hydrogen gas. After comparing the oxidation efficiency of each catalyst at different temperatures, we found that the hydrophobic Pd/SiO and Pt/AlO catalysts could oxidize HT into HTO at 25C.
Otsuka, Satoshi; Tanno, Takashi; Oka, Hiroshi; Yano, Yasuhide; Tachi, Yoshiaki; Kaito, Takeji; Hashidate, Ryuta; Kato, Shoichi; Furukawa, Tomohiro; Ito, Chikara; et al.
2018 GIF Symposium Proceedings (Internet), p.305 - 314, 2020/05
Oxide Dispersion Strengthened (ODS) steel has been developed worldwide as a high-strength and radiation-tolerant steel used for advanced nuclear system. Japan Atomic Energy Agency (JAEA) has been developing ODS steel as the primary candidate material of Sodium cooled Fast Reactor (SFR) high burn-up fuel cladding tube. Application of high burn-up fuel to SFR core can contribute to improvement of economical performance of SFR in conjunction with volume and hazardousness reduction of radioactive waste. This paper described the current status and future prospects of ODS tempered martensitic steel development in JAEA for SFR fuel application.
Watanabe, Masashi; Matsumoto, Taku; Hirooka, Shun; Morimoto, Kyoichi; Kato, Masato
2018 GIF Symposium Proceedings (Internet), p.315 - 320, 2020/05
Recently, a research group studying at Plutonium Fuel Development Facility (PFDF) in Japan Atomic Energy Agency has systematically measured vast amounts of physical properties in the non-stoichiometric (U, Pu)O. Lattice parameter, elastic modulus, thermal expansion, oxygen potential, oxygen chemical diffusion coefficient and thermal conductivity were successfully measured as function of Pu content, O/M ratio and temperature, and the effects of Pu content and O/M ratio on their physical properties were evaluated. In this work, those experimental data are reviewed, and latest experimental data set on the non-stoichiometric (U, Pu)O are presented. The data set would be available in development of a fuel performance code.
Ito, Takashi; Higemoto, Wataru; Shimomura, Koichiro*
Journal of the Physical Society of Japan, 89(5), p.051007_1 - 051007_8, 2020/05
Uwaba, Tomoyuki; Yokoyama, Keisuke; Nemoto, Junichi*; Ishitani, Ikuo*; Ito, Masahiro*; Pelletier, M.*
Nuclear Engineering and Design, 359, p.110448_1 - 110448_7, 2020/04
Coupled computer code analyses of irradiation performance of axially heterogeneous mixed oxide (MOX) fuel elements with high burnup in a fast reactor were conducted. Post-irradiation experiments revealed local concentration of Cs near the interfaces between MOX fuel and blanket columns including the internal blanket of the fuel elements as well as an increase in their cladding diameters. The analyses indicated that the local Cs concentration occurred as a result of Cs axial migration from the MOX fuels toward the blanket pellets near the interfaces. Swelling of the blanket pellets induced by the formation of low-density Cs-U-O compound was not sufficient to cause pellet-to-cladding mechanical interaction (PCMI). The PCMI analyzed in the MOX fuel column regions was insignificant, and the cladding diameter increases were caused mainly by void swelling in cladding and irradiation creep due to fission gas pressure.
Omori, Atsushi*; Akiyama, Eiji*; Abe, Hiroshi*; Hata, Kuniki; Sato, Tomonori; Kaji, Yoshiyuki; Inoue, Hiroyuki*; Taguchi, Mitsumasa*; Seito, Hajime*; Tada, Eiji*; et al.
Zairyo To Kankyo, 69(4), p.107 - 111, 2020/04
To evaluate the effect of oxidants, which are formed by radiolysis of water under gamma ray irradiation, on the corrosion of a carbon steel in humid environment, ozone was introduced as a model oxidant in to humidity-controlled air at 50C in a thermo-hygrostat chamber. Corrosion monitoring was performed by using an Atmospheric Corrosion Monitor-type (ACM) sensor consisting of a carbon steel anode and an Ag cathode. The output current of the ACM sensor was increased with the increase in relative humidity and it was obviously increased with the increase in the introduced ozone concentration at each relative humidity. The results indicate that ozone accelerates the corrosion of the carbon steel. The effect of ozone on the corrosion acceleration is attributed to the fast reduction reaction and fast dissolution reaction in to water compared to that of oxygen.
Zhang, Z,*; Wang, H.*; Yoshikawa, Hirofumi*; Matsumura, Daiju; Hatao, Shuya*; Ishikawa, Satoshi*; Ueda, Wataru*
ACS Applied Materials & Interfaces, 12(5), p.6056 - 6063, 2020/02
Kumagai, Yuta; Jonsson, M.*
Dalton Transactions (Internet), 49(6), p.1907 - 1914, 2020/02
This study aims to reveal possible involvements of organic acids in the oxidative dissolution of UO. Using phthalic acid as a model compound, we have measured adsorption on UO and investigated effects on the reaction between HO and UO and on oxidative dissolution induced by -irradiation. Significant adsorption of phthalic acid was observed even at neutral pH. However, the reaction between HO and UO in phthalic acid solution induced oxidative dissolution of U(VI) similarly to aqueous bicarbonate solution. These results indicate that even though phthalic acid adsorbs on the UO surface, it is not involved in the interfacial reaction by HO. In contrast, the dissolution of U by irradiation was inhibited in aqueous phthalic acid solution, whereas HO generated by radiolysis was consumed by UO. The inhibition suggests that radical species derived from phthalic acid was involved in the redox reaction process of UO.
Suzuki, Ryohei*; Tani, Yukinori*; Naito, Hirotaka*; Miyata, Naoyuki*; Tanaka, Kazuya
Catalysts, 10(1), p.44_1 - 44_15, 2020/01
We prepared biogenic Mn oxides (BMOs) using strain KR21-2, and subsequently conducted single or repeated treatment experiments in Cr(NO) at pH6.0. Under aerobic conditions, newly formed BMOs exhibited a rapid production of Cr(VI) without a significant release of Mn(II), demonstrating that newly formed BMO mediates a catalytic oxidation of Cr(III) with a self-regeneration step of reduced Mn. In anaerobic solution, newly formed BMOs showed a cessation of Cr(III) oxidation in the early stage of the reaction, and subsequently had a much smaller Cr(VI) production with significant release of reduced Mn(II).
Matsumura, Daiju; Tsuji, Takuya; Yoshii, Kenji
Materials Chemistry and Physics, 238, p.121885_1 - 121885_5, 2019/12
We have conducted X-ray absorption spectroscopy study for perovskite cobaltite PrSrCoO (00.5) to understand Sr doping effect and magnetocaloric measurement for PrSrCoO to reveal the origin of magnetic anomaly at around 110 K. The extended X-ray absorption fine structure (EXAFS) measurements at the Co -edge suggest that the average valence value of Co ions increases, the interatomic distance of Co-O bonding decreases, and the local distortion of CoO octahedron increases as Sr is doped in PrCoO. The interatomic distance of Co-O bonding shrinks more greatly for the larger doping region. No temperature dependent electronic and structural changes were observed from Co -edge X-ray absorption spectra in the whole thermal range studied (17-300 K). The magnetocaloric effect of PrSrCoO indicates the change of magnetic structure at 110 K.
Aihara, Jun; Yasuda, Atsushi*; Ueta, Shohei; Ogawa, Hiroaki; Honda, Masaki*; Ohira, Koichi*; Tachibana, Yukio
Nippon Genshiryoku Gakkai Wabun Rombunshi, 18(4), p.237 - 245, 2019/12
Development of fabrication and inspection technologies of oxidation resistant fuel element for improvement of safety of high temperature gas-cooled reactors (HTGRs) in severe oxidation accident was carried out. Simulated coated fuel particles (CFPs), alumina particles, were over-coated with mixed powder of Si, C and small amount of resin to form over-coated particles, and over-coated particles were molded and hot-pressed to sinter simulated oxidation resistant fuel elements with SiC/C mixed matrix. Simulated oxidation resistant fuel elements with matrix whose Si/C mole ratio is 1.00 were fabricated. Failure fraction of CFPs in fuel elements is one of very important inspection subjects of HTGR fuel. It is essential that CFPs are extracted from fuel elements without additional failure. Development of method for extraction of CFPs was carried out. Desolation of SiC by KOH method or pressurized acidolysis method should be applied to extraction of CFPs.
Ito, Takashi; Higemoto, Wataru; Koda, Akihiro*; Shimomura, Koichiro*
Applied Physics Letters, 115(19), p.192103_1 - 192103_4, 2019/11
Kasahara, Shigeki; Chimi, Yasuhiro; Hata, Kuniki; Hanawa, Satoshi
Zairyo To Kankyo, 68(9), p.240 - 247, 2019/09
In order to study environment assisted cracking mechanism of stainless steel under BWR primary coolant condition, effects of applied load on oxidation in the vicinity of crack tips of CT specimens were evaluated. Loaded CT specimens were immersed in an aqueous condition at 290C as a simulated BWR coolant condition, and microstructural observation on oxide near the tips of pre-cracks was carried out. Oxide inner layers, which consisted of fine grain magnetite containing Fe and Cr were formed, and oxide outer layers consisting of large grains of FeO were observed to cover the inner layers. FEM analysis of stress and strain in the loaded CT specimen suggests that both of dislocations due to localized plastic deformation and elastic strain could play important roles to accelerate inner oxide formation in the vicinity of the crack tip of the specimens.
Hoshako, 32(4), p.185 - 198, 2019/07
Synchrotron radiation photoelectron spectroscopy is a beneficial technique for precise analysis of chemical states of solid surfaces. Owing to its high luminosity, it ensures availability of termed synchrotron radiation real-time photoelectron spectroscopy which enables "" observation of chemical reactions with gas molecules occurring at surfaces. In this review, oxygen adsorption reactions in the oxidation of silicon single crystal surfaces are focused. Through the demonstration of our research, the usefulness of synchrotron radiation real-time photoelectron spectroscopy to study molecular adsorption reactions at solid surfaces is briefly described and the future perspective would also be shown.
Yamanouchi, Michihiko*; Oyamada, Tatsuro*; Sato, Koichi*; Ota, Hiromichi*; Ieda, Junichi
IEEE Transactions on Magnetics, 55(7), p.1400604_1 - 1400604_4, 2019/07
Ogawa, Shuichi*; Yoshigoe, Akitaka; Takakuwa, Yuji*
Vacuum and Surface Science, 62(6), p.350 - 355, 2019/06
Thermal oxidation of Si substrate is an indispensable process for the Si device fabrication. However, the influence of oxidation induced strain cannot be ignored for thin films. Synchrotron radiation real-time photoelectron spectroscopy was used as a method to measure simultaneously oxidation induced strain and oxidation rate. It was found that the acceleration of interfacial oxidation induced by thermal strain was observed for the rapid thermal oxidation. The results can be explained by the model in which point defects caused by strain become reaction sites at the SiO/Si interface.
Ota, Masakazu; Tanaka, Taku*
Journal of Environmental Radioactivity, 201, p.5 - 18, 2019/05
CH released from deep underground radioactive waste disposal facilities can be a belowground source of CO owing to microbial oxidation of CH to CO in soils. Environmental C models assume that the transfer of CO from soil to plant occurs via foliar uptake of CO. Nevertheless, the importance of CO root uptake is not well understood. In the present study, belowground transport and oxidation of CH were modeled and incorporated into an existing land surface CO model (SOLVEG-II) to assess the importance of root uptake on CO transfer to plants. Performance of the model in calculating the belowground dynamics of CH was validated by simulating a field experiment of CH injection into subsoil. The model was then applied to C transfer in a hypothetical ecosystem impacted by continuous CH input from the water table (bottom of one-meter thick soil). In a shallowly rooted ecosystem with rooting depth of 11 cm, foliar uptake of CO was significant, accounting for 80% of the C accumulation in the leaves. In a deeply rooted ecosystem (rooting depth of 97 cm), where the root penetrated to depths close to the water-table, more than half (63%) the C accumulated in the leaves was transferred by the root uptake. We found that CO root uptake in this ecosystem depended on the distribution of methane oxidation in the soil; all C accumulated in the leaves was transferred by the root uptake when methane oxidation occurred at considerable depths (e-folding depths of 20 cm, or 80 cm). These results indicate that CO root uptake contributes significantly to CO transfer to plants if CH oxidation occurs at great depths and roots penetrate deeply into the soil.