Segawa, Tomoomi; Kawaguchi, Koichi; Kato, Yoshiyuki; Ishii, Katsunori; Suzuki, Masahiro; Fujita, Shunya*; Kobayashi, Shohei*; Abe, Yutaka*; Kaneko, Akiko*; Yuasa, Tomohisa*
Proceedings of 2019 International Congress on Advances in Nuclear Power Plants (ICAPP 2019) (Internet), 9 Pages, 2019/05
A solution of plutonium nitrate and uranyl nitrate is converted into a mixed oxide by microwave heating denitration method. In the present study, for improving the efficiency of microwave heating and achieving high-temperature uniformity to produce homogeneous UO powder, the microwave heating test of potassium chloride and uranyl nitrate solution, and numerical simulation analysis were conducted. The potassium chloride agar was adjusted to the dielectric loss, which is close to that of the uranyl nitrate solution and the optimum support table height was estimated to be 50 mm for denitration of the uranyl nitrate solution by microwave heating. The adiabator improved the efficiency of microwave heating denitration. Moreover, the powder yield was improved by using the adiabator owing to ease of scraping of the denitration product from the bottom of the denitration vessel.
Suzuki, Kiichi; Kato, Masato; Sunaoshi, Takeo*; Uno, Hiroki*; Carvajal-Nunez, U.*; Nelson, A. T.*; McClellan, K. J.*
Journal of the American Ceramic Society, 102(4), p.1994 - 2008, 2019/04
The fundamental properties of CeO were assessed using a range of experimental techniques. The oxygen potential of CeO was measured by the thermogravimetric technique, and a numerical fit for the oxygen potential of CeO is derived based on defect chemistry. Mechanical properties of CeO were obtained using sound velocity measurement, resonant ultrasound spectroscopy and nanoindentation. The obtained mechanical properties of CeO are then used to evaluate the Debye temperature and Gruneisen constant. The heat capacity and thermal conductivity of CeO were also calculated using the Debye temperature and the Gruneisen constant. Finally, the thermal conductivity was calculated based upon laser flash analysis measurements. This result demonstrates that the thermal conductivity has strong dependence upon material purity.
Ikusawa, Yoshihisa; Morimoto, Kyoichi; Kato, Masato; Saito, Kosuke; Uno, Masayoshi*
Nuclear Technology, 205(3), p.474 - 485, 2019/03
This study evaluated the effects of plutonium content and self-irradiation on the thermal conductivity of mixed-oxide (MOX) fuel. Samples of UO fuel and various MOX fuels were tested. The MOX fuels had a range of plutonium contents, and some samples were stored for 20 years. The thermal conductivity of these samples was determined from thermal diffusivity measurements taken via laser flash analysis. Although the thermal conductivity decreased with increasing plutonium content, this effect was slight. The effect of self-irradiation was investigated using the stored samples. The reduction in thermal conductivity caused by self-irradiation depended on the plutonium content, its isotopic composition, and storage time. The reduction in thermal conductivity over 20 years' storage can be predicted from the change of lattice parameter. In addition, the decrease in thermal conductivity caused by self-irradiation was recovered with heat treatment, and recovered almost completely at temperatures over 1200 K. From these evaluation results, we formulated an equation for thermal conductivity that is based on the classical phonon-transport model. This equation can predict the thermal conductivity of MOX fuel thermal conductivity by accounting for the influences of plutonium content and self-irradiation.
Funtai Kogaku Kaishi, 55(10), P. 547, 2018/10
no abstracts in English
Fujita, Shunya*; Abe, Yutaka*; Kaneko, Akiko*; Yuasa, Tomohisa*; Segawa, Tomoomi; Yamada, Yoshikazu; Kato, Yoshiyuki; Ishii, Katsunori
Proceedings of 26th International Conference on Nuclear Engineering (ICONE-26) (Internet), 8 Pages, 2018/07
Mixed uranium oxide and plutonium oxide powder is produced from uranyl nitrate and plutonium nitrate mixed solution by the microwave heating denitration method in the spent fuel reprocessing process. Since the microwave heating method is accompanied by a boiling phenomenon, it is necessary to fully grasp the operating conditions in order to avoid flashing and spilling in the mass production of denitrification technology for the future. In this research, it was confirmed that a potassium chloride aqueous solution as a simulant of uranyl nitrate aqueous solution with high dielectric loss cause loss of microwave at the solution surface as the dielectric loss increased with the increase of KCl concentration by experimental and electromagnetic field analysis, and revealed that the change in the heating condition affects the generation of flushing.
Hirooka, Shun; Kato, Masato; Watanabe, Masashi
Transactions of the American Nuclear Society, 118, p.1624 - 1626, 2018/06
This study suggested the time development of oxygen-to-metal ratio (O/M) redistribution model with oxygen-related properties in MOX. Irradiation simulation including the suggested O/M redistribution and pore migration with vaporization-condensation model which bares density redistribution was demonstrated. The simulation results showed that O/M redistribution proceeded at lower temperature than density redistribution, which indicated that oxygen diffusion got influential at lower temperature than vaporization-condensation of MOX. Another find was that O/M redistribution was very slow at the surface because temperature kept low. However, near the surface (inside from the surface) where the temperature exceeded 1000 K, O/M redistribution was rather recognizable with oxygen flown from inner region to the near-surface. The results will be evaluated by comparison with post-irradiation examination data.
Hirooka, Shun; Kato, Masato
Journal of Nuclear Science and Technology, 55(3), p.356 - 362, 2018/03
The sound speeds of longitudinal and transverse waves in the uranium-plutonium mixed oxide (MOX) pellets were measured as functions of porosity, oxygen-to-metal ratio (O/M) and plutonium content. The effect of each parameter was well fitted by a linear function and the equations were obtained to calculate the sound speeds. Mechanical properties were evaluated with the sound speeds and the result of Young's modulus showed that porosity was the most important factor to decrease Young's modulus. Temperature dependence on Young's modulus was also evaluated with previously reported thermal expansion. Decrease of Young's modules with increasing temperature was in good agreement with available literature.
Proceedings of 25th International Conference on Nuclear Engineering (ICONE-25) (CD-ROM), 8 Pages, 2017/07
In a recycle system for minor actinides (MAs) currently studied to reduce the degree of hazard and the amount of high-level radioactive wastes, MAs will be recycled by reprocessing and irradiating as mixed oxide (MOX) with plutonium (Pu) and uranium (U) in a fast reactor. MA content is expected to be 5 wt.% in the future recycle system, and MAs might affect irradiation behavior of MA-MOX fuels. The main influences of MA-containing would be increase of fuel temperature and cladding stress, and the important behaviors would be fuel restructuring, redistribution, helium (He) generation and cladding corrosion. The MA-containing influences were evaluated with CEPTAR.V2, including fuel properties and analysis models to evaluate the MA-MOX fuel irradiation behavior, by using the results of highly americium (Am) containing MOX irradiation experiment, B8-HAM, performed in Joyo. The irradiation behavior of Am-MOX fuels could be precisely analyzed and revealed the influences of Am-containing.
Fujita, Shunya*; Abe, Yutaka*; Kaneko, Akiko*; Chonan, Fuminori*; Yuasa, Tomohisa*; Yamaki, Tatsunori*; Segawa, Tomoomi; Yamada, Yoshikazu
Proceedings of 25th International Conference on Nuclear Engineering (ICONE-25) (CD-ROM), 8 Pages, 2017/07
From the observation results, in the process of flushing, the behaviors leading to flushing were classified divided into three types. First type is that first generation bubble from heating leads to flushing. Second type is that nucleate boiling continues during heating and stop, finally single bubble generates and leads to flushing. Third type is defined that gradual evaporation occurs without bubbles. It was revealed that the total quantities of heat released by flushing are approximately equal when assuming the flushing mechanism, it can be triggered that a large amount of micro bubbles are instantaneously generated and grew.
Hirooka, Shun; Kato, Masato
Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Next Generation Nuclear Systems for Sustainable Development (FR-17) (USB Flash Drive), 6 Pages, 2017/06
Young's modulus of MOX pellets was evaluated by measuring the sound velocities of longitudinal and transverse waves in the pellets as functions of porosity, oxygen-to-metal ratio (O/M) and plutonium content. The results showed that porosity was the most important factor that 20% of the porosity decreased Young's modulus by neatly 100 GPa while O/M and plutonium content could change the Young's modulus by ~20 GPa. From the measured sound velocities, temperature dependence on Young's modulus and specific heat capacity were calculated on the Debye model by leveraging the thermal expansion data. The temperature dependence that Young's modulus decreases with increasing temperature is in good agreement with literature data. The specific heat capacity also agrees with that of calculated value by Kopp's method, taken the Schottky term and the excited term into account.
Maeda, Seiichiro; Oki, Shigeo; Otsuka, Satoshi; Morimoto, Kyoichi; Ozawa, Takayuki; Kamide, Hideki
Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Next Generation Nuclear Systems for Sustainable Development (FR-17) (USB Flash Drive), 10 Pages, 2017/06
The next generation fast reactor is being investigated in Japan, aiming at several targets such as "safety", "reduction of environmental burden" and "economic competitiveness". As for the safety aspect, FAIDUS concept is adopted to avoid re-criticality in core destructive accidents. The uranium-plutonium mixed oxide fuel, in which minor actinide elements are included, will be applied to reduce the amount and potential radio-toxicity of radioactive wastes. The high burn-up fuel is pursued to reduce fuel cycle cost. The candidate concept of the core and fuel design, which could satisfy various design criteria by design devisals, has been established. In addition, JAEA is investigating material properties and irradiation behavior of MA-MOX fuel. JAEA is developing the fuel design code especially for the fuel pin with annular pellets of MA-bearing MOX. Furthermore, JAEA is developing oxide dispersion strengthened (ODS) ferritic steel cladding for the high burnup fuel.
Watanabe, Masashi; Sunaoshi, Takeo*; Kato, Masato
Defect and Diffusion Forum, 375, p.84 - 90, 2017/05
The oxygen chemical diffusion coefficient in (U, Pu)O was determined by thermo-gravimetry as functions of the Pu content, oxygen-to-metal ratio and temperature. The surface reaction was considered in the diffusion coefficient determination. The activation energy for the chemical diffusion coefficient was 60 kJ/mol and 65 kJ/mol, respectively, in (UPu)O and (UPu)O.
Kato, Masato; Nakamura, Hiroki; Watanabe, Masashi; Matsumoto, Taku; Machida, Masahiko
Defect and Diffusion Forum, 375, p.57 - 70, 2017/05
The basic properties of PuO were reviewed, and the equilibrium defects in PuO were evaluated from the experimental data of the oxygen potential and electrical conductivity as well as the Ab-initio calculation results. Consistency among various properties was confirmed, and the mechanistic models for thermal property representations were derived.
Kato, Masato; Watanabe, Masashi; Matsumoto, Taku; Hirooka, Shun; Akashi, Masatoshi
Journal of Nuclear Materials, 487, p.424 - 432, 2017/04
Oxygen potential of (U,Pu)O was evaluated based on defect chemistry using an updated experimental data set. The relationship between oxygen partial pressure and deviation in (U,Pu)O was analyzed, and equilibrium constants of defect formation were determined as functions of Pu content and temperature. Brouwer's diagrams were constructed using the determined equilibrium constants, and a relational equation to determine O/M ratio was derived as functions of O/M ratio, Pu content and temperature. In addition, relationship between oxygen potential and oxygen diffusion coefficients were described.
Karisma, A. D.*; Hamaba, Taishu*; Fukasawa, Tomonori*; Huang, A.-N.*; Segawa, Tomoomi; Fukui, Kunihiro*
Review of Scientific Instruments, 88(2), p.024101_1 - 024101_8, 2017/02
Microwave heating direct denitration method is used in the nuclear fuel reprocessing process. In order to develop a single-mode-type microwave heating thermogravimetry apparatus which can perform detailed analysis of the characteristics of microwave heating, the temperature dependence of microwave absorption is verified. The temperature distribution, microwave absorption efficiency, and dielectric properties of a CuO pellet that was heated by the microwave irradiation were investigated. The temperature distribution in the CuO pellet due to one-way travel of the microwave in the apparatus was accurately reproduced by a three-dimensional numerical simulation of the electromagnetic field. The numerically determined temperature dependency of the CuO absorption efficiency was found to be in very good agreement with published data.
Segawa, Tomoomi; Fukasawa, Tomonori*; Huang, A.-N.*; Yamada, Yoshikazu; Suzuki, Masahiro; Fukui, Kunihiro*
Chemical Engineering Science, 153, p.108 - 116, 2016/10
The influence of the heating method and rate on the morphology of CuO powders synthesized from Cu(NO)3HO aqueous solutions by denitration was investigated. The median diameter of the obtained powder was found to decrease as the heating rate increased, independent of the heating method. The microwave heating method remarkably reduced the particle size and enhanced the irregularity and disorder of the shape and surface of the particles, which were found to be more widely distributed. In contrast, the microwave hybrid heating method yielded the most spherical particles with the smoothest surface. It was also found that this heating method sharpened the particle size distribution and had higher energy efficiency than the MW method. Numerical simulations also indicated a difference in the energy efficiency between these two methods. The simulations also revealed that the hybrid method could heat the whole reactor more uniformly with a lower microwave output.
Okazaki, Hiro; Shibano, Koya; Abe, Katsuo; Sumi, Mika; Kayano, Masashi; Kageyama, Tomio; Mason, P.*
Proceedings of INMM 57th Annual Meeting (Internet), 7 Pages, 2016/07
The reference materials used for accountancy analysis by IDMS, referred to as LSD spikes allows to obtain accurate measurement results for a variety of nuclear materials under potentially difficult handling or measurement conditions. Because of expected difficulties in a stably long term supply of plutonium reference materials, which are the main source of plutonium for LSD spikes preparation, the JAEA's PFDC decided to evaluate the possibility of using domestically available MOX powders as a plutonium source material for LSD spikes. Therefore, PFDC started to separate, purify and characterize plutonium in MOX powders for plutonium reference materials (MOX-Pu) preparation that are suitable for source of LSD spikes in cooperation with the US DOE's NBL. The detailed preparation procedure of the latest MOX-Pu standard material and results of intercomparison for verification are presented.
Transactions of the American Nuclear Society, 114, p.987 - 988, 2016/06
In Japan, uranium and plutonium mixed oxide (MOX) has been developed as fuels of sodium-cooled fast reactors. The developing MOX fuels come in variety of O/M ratio, Pu content, minor actinide (MA) content and density. We have studied a science based fuel technology to evaluate fuel behaviors in fabrication process and irradiation condition of such various fuels. The technologies which are constructed based on experimental database can apply to mechanistic evaluation of fuel behaviors. To develop the science based fuel technology, many different varieties of basic properties have been investigated, and experimental database was constructed. And a mechanistic physical property model has been studied. The models contribute to describe various behaviors in fuel fabrication process and irradiation condition.
Watanabe, Masashi; Kato, Masato; Sunaoshi, Takeo*
Transactions of the American Nuclear Society, 114, p.1081 - 1082, 2016/06
Many studies on the oxygen potential of UO have been carried out so far. However, the oxygen potential data for UO near the stoichiometric composition in the high temperature region (1673-1873 K) are limited. In this work, the oxygen potential data of UO were extended to high temperature range of 1673-1873 K by gas equilibrium method. The measured data were analyzed based on a defect chemistry model.
Kato, Masato; Ikusawa, Yoshihisa; Sunaoshi, Takeo*; Nelson, A. T.*; McClellan, K. J.*
Journal of Nuclear Materials, 469, p.223 - 227, 2016/02
Thermal expansion of (UPu)O (x = 0, 0.01, 0.02, 0.03) and (UPu)O was measured with a dilatometer in an oxygen partial pressure-controlled atmosphere. The oxygen partial pressure was controlled to hold a constant oxygen-to-metal ratio in the (U,Pu)O during the measurement. Thermal expansion slightly increased with the decrease in oxygen-to-metal ratio. The relationship was derived to describe thermal expansion.