Shibata, Hiroki; Saito, Hiroaki; Hayashi, Hirokazu; Takano, Masahide
JAEA-Data/Code 2019-023, 138 Pages, 2020/03
Transmutation of minor actinides in the form of nitride fuel by the accelerator driven system has been developed to reduce the radiotoxicity and volume in the radioactive wastes. Nitride fuel behavior under irradiation condition is necessary for its design and development. Nitride fuel performance analysis module based on light water reactor fuel performance code, FEMAXI-7, was developed by introducing fundamental properties of nitride pellet, 9Cr-1Mo ferrite cladding, and Pi-Bi coolant. As a result of test analysis with this module, we have understood that the nitride fuel shows excellent behavior under irradiation due to its high thermal conductivity. We found that, however, it may be a main concern that fuel cladding integrity is maintained during irradiation in which pellet-cladding mechanical interaction is increased by He gas release, low creep rate of nitride pellet at low temperatures, and high creep rate of cladding above 873 K.
Yoneda, Yasuhiro; Harada, Makoto; Takano, Masahide
Transactions of the Materials Research Society of Japan, 44(2), p.61 - 64, 2019/04
We performed three-dimensional observation of simulated fuel debris using Synchrotron Computed Tomography (CT). CT was used to make the inside of fuel debris clear. The CT observation provides that a clear contrast in the zirconia rich part and concrete rich part. Zirconia heavier than concrete moved to the lower part when crystals precipitate and aggregates near the bottom surface. As a result, phase separation occurs. The phase separation is caused by the difference in the composition ratio of zirconia, and can also be observed difference in crystal growth mode by composition ratio.
Wagakuni Shorai Sedai No Enerugi O Ninau Kakunenryo Saikuru; Datsu Tanso Shakai No Enerugi Anzen Hosho; NSA/Commentaries, No.24, p.163 - 167, 2019/03
This article summarizes R&D status of the nitride fuel cycle for minor actinides (MA) transmutation. Status of nitride fuel fabrication, material properties and fuel performance code, pyrochemical reprocessing, and nitrogen-15 enrichment are described.
Okamoto, Yoshihiro; Takano, Masahide
Progress in Nuclear Science and Technology (Internet), 5, p.200 - 203, 2018/11
Chemical state of some simulated corium debris samples containing uranium (fuel), zirconium (fuel cladding), iron (structure material), calcium (cement) and lanthanides (fission products) was investigated by synchrotron radiation based extended X-ray absorption fine structure (EXAFS) analysis. The local structure of uranium for the simulated debris was classified into fluorite UO structure and C-type structure (stabilized cubic). The UZrFeCaO sample, which consists of single phase (C-type), shows slightly shorter U-O distance. It can be concluded that the sample contains pentavalent uranium. The local structure of zirconium for U-Zr-O and U-Zr-Fe-O systems was very close to tetragonal ZrO, while that of zirconium changed to CSZ (calcia stabilized cubic) by adding calcium.
Kumagai, Yuta; Takano, Masahide; Watanabe, Masayuki
Journal of Nuclear Materials, 497, p.54 - 59, 2017/12
We studied oxidative dissolution of uranium and zirconium oxide [(U,Zr)O] in aqueous HO solution. The interfacial reaction is essential for anticipating how a (U,Zr)O-based molten fuel may chemically degrade after a severe accident under influence of ionizing radiation. We conducted our experiments with (U,Zr)O powder and quantitated the HO reaction via dissolved U and HO concentrations. The dissolution yield relative to HO consumption was far less for (U,Zr)O compared to that of UO. The reaction kinetics indicates that most of the HO catalytically decomposed to O at the surface of (U,Zr)O. We confirmed the HO catalytic decomposition via O production (quantitative stoichiometric agreement). In addition, post-reaction Raman scattering spectra of the undissolved (U,Zr)O showed no additional peaks (indicating a lack of secondary phase formation). The (U,Zr)O matrix is much more stable than UO against HO-induced oxidative dissolution.
Yoneda, Yasuhiro; Tsuji, Takuya; Matsumura, Daiju; Okamoto, Yoshihiro; Takaki, Seiya; Takano, Masahide
Transactions of the Materials Research Society of Japan, 42(2), p.23 - 26, 2017/04
ZnN is a possible candidate for the diluent material for nitride fuels containing transuranium elements. Pellets of inert matrix material ZrN, and surrogate nitride fuel material DyZrN, are fabricated for the purpose of investigating the crystal structure. Lattice parameters of DyZrN followed the Vegard's low, in spite of the large lattice mismatch ( 7%) between DyN and ZrN. Local structure analysis was performed by X-ray absorption fine structure (XAFS) and atomic pair-distribution function (PDF) methods. The Zr-N nearest neighbor bond distance changed as changing the Dy composition. The complex local structure of DyN and ZrN is related to the preferable effects of ZrN.
Sudo, Ayako; Nishi, Tsuyoshi; Shirasu, Noriko; Takano, Masahide; Kurata, Masaki
Journal of Nuclear Science and Technology, 52(10), p.1308 - 1312, 2015/10
For understanding the control blade degradation mechanism of BWR, the thermodynamic database for the fuel assembly materials is a useful tool. Although iron, boron, and carbon ternary system is a dominant phase diagram, phase relation data is not sufficient for the region in which the boron and carbon compositions are richer than the eutectic composition. The phase relations of three samples were analyzed by X-ray diffraction, scanning electron microscope and energy dispersed X-ray spectrometry. The results indicate that Fe(B,C) phase only exists in the intermediate region at 1273 K and that the solidus temperature widely maintains at about 1400 K for all three samples, which are different from the calculated data using previous thermodynamic database. The difference might be originated from the over-estimations of the interaction parameter between boron and carbon in Fe(B,C).
Nishi, Tsuyoshi; Nakajima, Kunihisa; Takano, Masahide; Kurata, Masaki; Arita, Yuji*
Journal of Nuclear Materials, 464, p.270 - 274, 2015/09
no abstracts in English
Yamagishi, Isao; Odakura, Makoto; Ichige, Yoshiaki; Kuroha, Mitsuhiko; Takano, Masahide; Akabori, Mitsuo; Yoshioka, Masahiro*
Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1113 - 1119, 2015/09
The characteristics of insoluble residues in fine suspension at the Rokkasho Reprocessing Plant were analyzed. The insoluble residues were washed with oxalic acid solution to dissolve zirconium molybdate residues. XRD profiles of unwashed residues showed the presence of a noble metal alloy, zirconium molybdate, and zirconia, but zirconium molybdate was not found after washing. More than 50% of the Sb-125 and Pu in thee residues was washed out as well. The noble metal alloy composed of Mo, Tc, Ru, Rh, and Pd occupied more than 90% of the total weight of 12 elements (Ca, Cr, Fe, Ni, Zr, Mo, Tc, Ru, Rh, Pd, Te, and U) found in the residues. In consideration of the chemical forms of 12 elements, the alloy-to-residue weight ratio was evaluated to be 64% and 78% with and without 18% of an unknown component, respectively.
Sato, Takumi; Shibata, Hiroki; Hayashi, Hirokazu; Takano, Masahide; Kurata, Masaki
Journal of Nuclear Science and Technology, 52(10), p.1253 - 1258, 2015/08
In order to explore the applicability of the chlorination by MoCl as a potential pretreatment technique for waste treatment of fuel debris by pyrochemical methods, chlorination experiments of UO and (UZr)O simulated fuel debris were carried out in two steps: the first one is a chlorination reaction by homogeneous heating, the second one is a volatilization of molybdenum by-product by heating under temperature gradient condition. Most of UO and (UZr)O powder were converted to UCl or UCl and ZrCl mixture at 573 K, respectively. In the case of (UZr)Osintered particle, most of sample was converted to the chlorides because the products evaporated and be separated from sample surface at 773 K, while only the surface of the sample disk was converted to the chlorides at 573 and 673 K. Most of molybdenum by-product and ZrCl were separated from UCl by volatilization at 573 K.
Nabara, Yoshihiro; Suwa, Tomone; Takahashi, Yoshikazu; Hemmi, Tsutomu; Kajitani, Hideki; Ozeki, Hidemasa; Sakurai, Takeru; Iguchi, Masahide; Nunoya, Yoshihiko; Isono, Takaaki; et al.
IEEE Transactions on Applied Superconductivity, 25(3), p.4200305_1 - 4200305_5, 2015/06
Hayashi, Hirokazu; Nishi, Tsuyoshi; Takano, Masahide; Sato, Takumi; Shibata, Hiroki; Kurata, Masaki
NEA/NSC/R(2015)2 (Internet), p.360 - 367, 2015/06
Uranium-free nitride fuel was chosen as the first candidate for transmutation of long-lived minor actinides (MA) using accelerator-driven system (ADS) under the double strata fuel cycle concept by Japan Atomic Energy Agency (JAEA). The advantages of nitride fuel are good thermal properties and large mutual solubility among actinide elements. A pyrochemical process is proposed as the first candidate for the reprocessing of the spent nitride fuel, because this technique has some advantages over aqueous process, such as the resistance to radiation damage, which is an important issue for the fuels containing large amounts of highly radioactive MA. This paper overviews the recent progress and future R&D plan of the study on the nitride fuel cycle technology in JAEA.
Otobe, Haruyoshi; Kitatsuji, Yoshihiro; Kurata, Masaki; Takano, Masahide
Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 11 Pages, 2014/10
The chemical and transport behaviors of Pu and U in the corroded debris must be understood for the criticality safety control of Pu and U in the debris, especially for the removal operations and storage. Therefore, the chemical changes of UO and PuO powders, disks and U and Pu metal disks in HO aqueous solution have been checked, where HO is formed by the radiolysis of HO. As a result, UO changed to hydrated uranium peroxide, whereas the PuO remained unchanged. U metal was more reactive with HO aqueous solution than Pu metal. The chemical changes of the mixed UO/PuO powders in HO aqueous solution have been investigated. The dried slurry of the middle zone of HO aqueous solution was mainly composed of hydrated uranium peroxide, whereas the dried powder of the bottom zone was mainly composed of PuO.
Takano, Masahide; Nishi, Tsuyoshi; Shirasu, Noriko
Journal of Nuclear Science and Technology, 51(7-8), p.859 - 875, 2014/07
To predict phase relationships in the solidified core melt of Fukushima Daiichi Nuclear Power Plants, the solidified melt samples among core materials were prepared by arc melting. Phases and compositions in the samples were determined by X-ray diffraction, microscopy and elemental analysis. The only oxide phase formed is (U,Zr)O. The stable metallic phases are Fe-Cr-Ni alloy and FeZr-type (Fe,Cr,Ni)(Zr,U) intermetallic. The borides, ZrB and (Fe,Cr,Ni)B, are solidified in the metallic part. Annealing at 1773 K under an oxidizing atmosphere resulted in the oxidation of uranium and zirconium in the alloy and ZrB, instead the (Fe,Cr,Ni)B and Fe-Cr-Ni alloy became dominant. The metallic zirconium content in the melt is found to be a key factor that determines the phase relationships. As a basic mechanical property, the microhardness of each phase was measured. The borides showed notably higher hardness than any other oxide and metallic phases.
Takano, Masahide; Hayashi, Hirokazu; Minato, Kazuo
Journal of Nuclear Materials, 448(1-3), p.66 - 71, 2014/05
A powder sample of curium nitride (CmN) containing 0.35%-PuN and 3.59%-AmN was prepared by carbothermic nitridation of the oxide. The lattice expansion induced by self-irradiation damage at room temperature was measured as a function of time. The saturated a/a value was 0.43%, which is greater than those for transuranium dioxides available in literature. The undamaged lattice parameter at 2971 K was determined to be 0.502610.00006 nm. Temperature dependence of the lattice parameter was measured by a high temperature X-ray diffractometer in the temperature range up to 1375 K. The linear thermal expansion of the lattice from 293 to 1273 K is 0.964% and the corresponding thermal expansion coefficient is 9.84 10 K. Comparing with the other actinide nitrides, it was found that CmN lies between the higher expansion nitrides (PuN and AmN) and the lower expansion nitrides (UN and NpN).
Nishi, Tsuyoshi; Arai, Yasuo; Takano, Masahide; Kurata, Masaki
JAEA-Data/Code 2014-001, 45 Pages, 2014/03
The purpose of this study is to prepare a property database of nitride fuel needed for the fuel design of accelerator-driven system (ADS) for transmutation of minor actinide (MA). Nitride fuel of ADS is characterized by high content of Pu and MA as principal components, and addition of a diluent material such as ZrN. Experimental data or evaluated values from the raw data on properties Pu and MA nitrides, and nitride solid solutions containing ZrN are collected and summarized, which cover the properties needed for the fuel design of ADS. They are expressed as an equation as much as possible for corresponding to a variety conditions. Error evaluation is also made as much as possible. Since property data on transuranium (TRU) nitrides are often lacking, those on UN and (U,Pu)N are substitutionally shown in such cases in order to facilitate the fuel design with a tolerable accuracy by complementing the database.
Pukari, M.*; Takano, Masahide
Journal of Nuclear Materials, 444(1-3), p.7 - 13, 2014/01
Pellets of inert matrix material ZrN, and surrogate nitride fuel material (DyZr)N, are fabricated for the purpose of investigating the origin and the effect of carbon and oxygen impurity concentrations. Oxygen concentrations of up to 1.2 wt% are deliberately introduced into the materials with two separate methods. The achievable pellet densities of these materials, as a function of O content, sintering temperature and dimensional powder properties are determined. O dissolved into (Dy,Zr)N increases the achievable densities to a larger extent than if dissolved into ZrN. The segregation of O-rich phases in ZrN indicates a low O solubility in the material. Oxygen pick-up during the fabrication of the product as well as its exposure to air is demonstrated. The quality of the materials is monitored by the systematic analysis of O, N and C contents throughout the fabrication and sintering processes, supported by XRD and SEM analyses.
Pukari, M.*; Takano, Masahide; Nishi, Tsuyoshi
Journal of Nuclear Materials, 444(1-3), p.421 - 427, 2014/01
Nitride fuel with the composition (PuZr)N is fabricated for studying the sinterability of nitride fuel as a function of oxygen concentration in the material. Oxygen concentration of up to 0.6 wt% evidently enhances the densification of the material. Increasing the sintering temperature from 1923 to 1973 K improves the sintered pellet densities by up to 3.8%TD. In addition, the measured thermophysical and electrical properties of (PuZr)N reveal that the values are close to those of PuN. Oxygen concentration of 0.34 wt% in (Pu,Zr)N is a consequence of the fabrication process, considering the relatively pure ZrN (0.03 wt% O) and PuN (0.08 wt% O) powders initially fabricated.
Nishi, Tsuyoshi; Takano, Masahide; Arai, Yasuo; Kurata, Masaki
Dai-34-Kai Nippon Netsu Bussei Shimpojiumu Koen Rombunshu, p.199 - 201, 2013/11
By installing the laser flash apparatus and the drop calorimeter in the glove box, the thermal diffusivity and the heat capacity measurements of nitride containing MA elements of long-lived radioactive nuclides were enabled. The sample holder and the platinum container were designed to measure the thermal diffusivity and the heat capacity of very small quantity of MA nitride samples. The thermal conductivities of MA nitride increased with temperature, unlike that of conventional oxide-type nuclear fuels. In addition, the thermal conductivities of MA nitride decreased with increasing Am contents. The thermal conductivity of ZrN-based MA nitride, which is proposed as a candidate material for the ADS fuel, was fitted to equations as functions of the temperature and ZrN concentration. The predicted values agreed well with the experimental ones, indicating that the thermal conductivity of nitride fuel for ADS can be predicted for a practical design.
Hayashi, Hirokazu; Takano, Masahide; Kurata, Masaki; Minato, Kazuo
Journal of Nuclear Materials, 440(1-3), p.477 - 479, 2013/09
Neptunium trichloride of high purity was synthesized by the solid-state reaction of neptunium nitride, which was prepared from the oxide by the carbothermic reduction method, and cadmium chloride in a similar manner as reported for synthesis of AmCl. Lattice parameters of hexagonal NpCl were determined from the X-ray diffraction pattern to be a = 0.7421 0.0006 nm and c = 0.4268 0.0003 nm, which fairly agree with the reported values (a = 0.742 0.001 nm and c = 0.4281 0.0005 nm). Melting temperature of NpCl was measured with about 1 mg of the sample which was hermetically encapsulated in a gold crucible using a differential thermal analyzer with heating and cooling rate of 10 K/min in an argon gas flow (50 mL/min). The melting temperature of NpCl was determined to 1070 3 K, which is close to the recommended value 107530 K, which was derived from the mean value of the melting temperature for UCl(1115K) and that for PuCl (1041 K).