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Journal Articles

Oxygen potential measurement of (U,Pu,Am)O$$_{2 pm x}$$ and (U,Pu,Am,Np)O$$_{2 pm x}$$

Hirooka, Shun; Matsumoto, Taku; Kato, Masato; Sunaoshi, Takeo*; Uno, Hiroki*; Yamada, Tadahisa*

Journal of Nuclear Materials, 542, p.152424_1 - 152424_9, 2020/12

The measurement of oxygen potential was conducted at 1,673, 1,773, and 1,873 K for (U$$_{0.623}$$Pu$$_{0.350}$$Am$$_{0.027}$$)O$$_{2}$$ and at 1,873 and 1,923 K for (U$$_{0.553}$$Pu$$_{0.285}$$Am$$_{0.015}$$Np$$_{0.147}$$)O$$_{2}$$ by using a thermo-gravimeter and an oxygen sensor. Am inclusion in terms of substituting the U significantly increased the oxygen potential. Similarly, the inclusion of Np as a substitute for U increased the oxygen potential; however, the effect was not as large as that with the Pu or Am addition at the same rate. The results were analyzed via defect chemistry and certain defect formations were suggested in the reducing region and the near-stoichiometric region by plotting the relationship between PO$$_{2}$$ and the deviation from the stoichiometry. The equilibrium constants of the defect reactions were arranged to reproduce the experiment such that Am/Np contents were included in the entropy with coefficients fitting the experimental data.

Journal Articles

Oxygen self-diffusion in near stoichiometric (U,Pu)O$$_{2}$$ at high temperatures of 1673-1873 K

Watanabe, Masashi; Kato, Masato; Sunaoshi, Takeo*

Journal of Nuclear Materials, 542, p.152472_1 - 152472_7, 2020/12

The oxygen self-diffusion coefficients in near stoichiometric (U,Pu)O$$_{2}$$ at high temperatures were successfully measured by thermogravimetry combined with the oxygen isotope exchange method. The activation energy for oxygen diffusion in the stoichiometric composition of (U,Pu)O$$_{2}$$ was evaluated from experimental data, and the value was determined to be 248 kJ/mol. In addition, the defect migration energies of (U,Pu)O$$_{2 pm x}$$ were derived, and the oxygen self-diffusion coefficients were evaluated using these. As a result, good agreement was found between the experimental data and the oxygen self-diffusion coefficients calculated using the defect migration energies.

Journal Articles

Effect of O/M ratio on sintering behavior of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2-x}$$

Nakamichi, Shinya; Hirooka, Shun; Kato, Masato; Sunaoshi, Takeo*; Nelson, A. T.*; McClellan, K. J.*

Journal of Nuclear Materials, 535( ), p.152188_1 - 152188_8, 2020/07

Oxygen-to-metal ratio (O/M) of uranium and plutonium mixed oxide depends on its oxygen partial pressure. To attain the desirable microstructure and O/M ratio of sintered pellets, it is important to investigate the relation between the sintering behavior and the atmosphere of sintering process. In this study, sintering behavior of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2}$$ and (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{1.99}$$ in controlled po$$_{2}$$ atmosphere were investigated. It was found activation energy of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{1.99}$$ was higher than that of (Pu$$_{0.3}$$U$$_{0.7}$$)O$$_{2}$$. On the other hand, it was observed grain growth during sintering was suppressed in hypo-stoichiometric composition.

Journal Articles

Physical properties of non-stoichiometric (U,Pu)O$$_{2}$$

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$$_{2}$$. 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$$_{2}$$ are presented. The data set would be available in development of a fuel performance code.

Journal Articles

Post-irradiation examinations of annular mixed oxide fuels with average burnup 4 and 5% FIMA

Cappia, F.*; Tanaka, Kosuke; Kato, Masato; McClellan, K.*; Harp, J.*

Journal of Nuclear Materials, 533, p.152076_1 - 152076_14, 2020/05

 Times Cited Count:0 Percentile:100(Materials Science, Multidisciplinary)

Journal Articles

Pyroelectric power generation from the waste heat of automotive exhaust gas

Kim, J.*; Yamanaka, Satoru*; Murayama, Ichiro*; Kato, Takanori*; Sakamoto, Tomokazu*; Kawasaki, Takuro; Fukuda, Tatsuo; Sekino, Toru*; Nakayama, Tadachika*; Takeda, Masatoshi*; et al.

Sustainable Energy & Fuels (Internet), 4(3), p.1143 - 1149, 2020/03

 Times Cited Count:1 Percentile:100(Chemistry, Physical)

Journal Articles

Direct observation of electronic structure change by resistance random access memory effect in amorphous alumina

Kubota, Masato; Nigo, Seisuke*; Kato, Seiichi*; Amemiya, Kenta*

AIP Advances (Internet), 9(9), p.095050_1 - 095050_4, 2019/09

 Times Cited Count:0 Percentile:100(Nanoscience & Nanotechnology)

We measured the X-ray absorption spectra of amorphous alumina with vacancy-type oxygen defects which exhibits the resistance random access memory effect. For the first time, we detected changes in the electronic structure owing to the memory effect. A major difference in spectrum was observed near the O K-absorption edge.

Journal Articles

Crystal structure change of katoite, Ca$$_{3}$$Al$$_{2}$$(O$$_{4}$$D$$_{4}$$)$$_{3}$$, with temperature at high pressure

Kyono, Atsushi*; Kato, Masato*; Sano, Asami; Machida, Shinichi*; Hattori, Takanori

Physics and Chemistry of Minerals, 46(5), p.459 - 469, 2019/05

 Times Cited Count:0 Percentile:100(Materials Science, Multidisciplinary)

To reveal the decomposition mechanism with temperature under high-pressure, crystal structure of a hydrogrossular, katoite Ca$$_{3}$$Al$$_{2}$$(O$$_{4}$$D$$_{4}$$)$$_{3}$$ has been studied by in-situ neutron diffraction at 8 GPa. Although unusual expansion behavior was discerned at 200-400$$^circ$$C, the unit cell was continuously expanded up to 850$$^circ$$C. At 900$$^circ$$C, katoite was decomposed, indicating that pressure strongly increases dehydration temperature from 300$$^circ$$C to 900$$^circ$$C. On release of pressure, the katoite reappear together with corundum and portlandite. At 8 GPa, CaO$$_{8}$$ and AlO$$_{6}$$ polyhedra expand with temperature up to 850$$^circ$$C by about 8% and 13%, respectively. On the other hand, tetrahedral interstices are isotopically squeezed by about 10%: due to the expansion of above polyhedra. The neighboring D-D distance remains almost unchanged in this temperature range, while the O-D bond distance shrinks drastically just before decomposition. This finding suggests that the shortening of O-D distance caused by the D-D repulsion destabilizes the O-D bond, which induces the thermal decomposition of katoite.

Journal Articles

Thermal and mechanical properties of CeO$$_{2}$$

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$$_{2}$$ were assessed using a range of experimental techniques. The oxygen potential of CeO$$_{2}$$ was measured by the thermogravimetric technique, and a numerical fit for the oxygen potential of CeO$$_{2}$$ is derived based on defect chemistry. Mechanical properties of CeO$$_{2}$$ were obtained using sound velocity measurement, resonant ultrasound spectroscopy and nanoindentation. The obtained mechanical properties of CeO$$_{2}$$ are then used to evaluate the Debye temperature and Gruneisen constant. The heat capacity and thermal conductivity of CeO$$_{2}$$ 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.

JAEA Reports

Activity median aerodynamic diameter relating to contamination at Plutonium Fuel Research Facility in Oarai Research and Development Center; Particle size analysis for plutonium particles using imaging plate

Takasaki, Koji; Yasumune, Takashi; Hashimoto, Makoto; Maeda, Koji; Kato, Masato; Yoshizawa, Michio; Momose, Takumaro

JAEA-Review 2019-003, 48 Pages, 2019/03

JAEA-Review-2019-003.pdf:3.81MB

June 6, 2017, at Plutonium Fuel Research Facility in Oarai Research and Development Center of JAEA, when five workers were inspecting storage containers containing plutonium and uranium, resin bags in a storage container ruptured, and radioactive dust spread. Though they were wearing a half face mask respirator, they inhaled radioactive materials. In the evaluation of the internal exposure dose, the aerodynamic radioactive median diameter (AMAD) is an important parameter. We measured 14 smear samples and a dust filter paper with imaging plates, and estimated the AMAD by image analysis. As a result of estimating the AMAD, from the 14 smear samples, the AMADs are 4.3 to 11 $$mu$$m or more in the case of nitrate plutonium, and the AMADs are 5.6 to 14 $$mu$$m or more in the case of the oxidized plutonium. Also, from the dust filter paper, the AMAD is 3.0 $$mu$$m or more in the case of nitrate plutonium, and the AMAD is 3.9 $$mu$$m or more in the case of the oxidized plutonium.

Journal Articles

The Effects of plutonium content and self-irradiation on thermal conductivity of mixed oxide fuel

Ikusawa, Yoshihisa; Morimoto, Kyoichi; Kato, Masato; Saito, Kosuke; Uno, Masayoshi*

Nuclear Technology, 205(3), p.474 - 485, 2019/03

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

This study evaluated the effects of plutonium content and self-irradiation on the thermal conductivity of mixed-oxide (MOX) fuel. Samples of UO$$_{2}$$ 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.

Journal Articles

Electrical and crystallographic study of an electrothermodynamic cycle for a waste heat recovery

Kim, J.*; Yamanaka, Satoru*; Nakajima, Akira*; Kato, Takanori*; Kim, Y.*; Fukuda, Tatsuo; Yoshii, Kenji; Nishihata, Yasuo; Baba, Masaaki*; Takeda, Masatoshi*; et al.

Advanced Sustainable Systems (Internet), 2(11), p.1800067_1 - 1800067_8, 2018/11

 Times Cited Count:1 Percentile:82.39(Green & Sustainable Science & Technology)

Journal Articles

Isotope-selective microscale imaging of radioactive Cs without isobaric interferences using sputtered neutral mass spectrometry with two-step resonant ionization employing newly-developed Ti:Sapphire lasers

Sakamoto, Tetsuo*; Morita, Masato*; Kanenari, Keita*; Tomita, Hideki*; Sonnenschein, V.*; Saito, Kosuke*; Ohashi, Masaya*; Kato, Kotaro*; Iguchi, Tetsuo*; Kawai, Toshihide*; et al.

Analytical Sciences, 34(11), p.1265 - 1270, 2018/11

 Times Cited Count:4 Percentile:67.24(Chemistry, Analytical)

Journal Articles

Temperature stability of PIN-PMN-PT ternary ceramics during pyroelectric power generation

Moro, Takuya*; Kim, J.*; Yamanaka, Satoru*; Murayama, Ichiro*; Kato, Takanori*; Nakayama, Tadachika*; Takeda, Masatoshi*; Yamada, Noboru*; Nishihata, Yasuo; Fukuda, Tatsuo; et al.

Journal of Alloys and Compounds, 768, p.22 - 27, 2018/11

 Times Cited Count:6 Percentile:33.7(Chemistry, Physical)

Journal Articles

Modeling and simulation of redistribution of oxygen-to-metal ratio in MOX

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.

Journal Articles

Effect of a raw material powder on sintered CeO$${2}$$ pellets by 28 GHz microwave irradiation

Akashi, Masatoshi; Matsumoto, Taku; Kato, Masato

Transactions of the American Nuclear Society, 118, p.1391 - 1394, 2018/06

In this study, CeO$${2}$$ pellet sintering by irradiating microwave at a frequency of 28 GHz was carried out to investigate the effect of particle diameter of raw powder on the density of sintered pellet. The highest bulk density is 94.2 %T.D. under the condition of 30 min holding at 1473 K. The bulk density decreases with increasing the particle diameter of used raw powder. On the other hand, all of the apparent density of sintered pellet is more than 93.5 %T.D.. The difference between the bulk density and the apparent density is caused by the difference of open porosity for each sample pellet. It seems that the high density sintered pellets with porous structure are obtained because sample pellet is heated internally and uniformly in microwave sintering.

Journal Articles

Sound speeds in and mechanical properties of (U,Pu)O$$_{2-x}$$

Hirooka, Shun; Kato, Masato

Journal of Nuclear Science and Technology, 55(3), p.356 - 362, 2018/03

 Times Cited Count:1 Percentile:73.25(Nuclear Science & Technology)

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.

Journal Articles

Pyroelectric power generation with ferroelectrics (1-x)PMN-xPT

Kim, J.*; Yamanaka, Satoru*; Nakajima, Akira*; Kato, Takanori*; Kim, Y.*; Fukuda, Tatsuo; Yoshii, Kenji; Nishihata, Yasuo; Baba, Masaaki*; Takeda, Masatoshi*; et al.

Ferroelectrics, 512(1), p.92 - 99, 2017/08

 Times Cited Count:6 Percentile:49.21(Materials Science, Multidisciplinary)

Journal Articles

Oxide-metal ratio dependence of central void formation of mixed oxide fuel irradiated in fast reactors

Ikusawa, Yoshihisa; Maeda, Koji; Kato, Masato; Uno, Masayoshi*

Nuclear Technology, 199(1), p.83 - 95, 2017/07

 Times Cited Count:1 Percentile:79.18(Nuclear Science & Technology)

Based on thermal computation results obtained using an irradiation behavior analysis code, we have evaluated the effect of O/M ratio on fuel restructuring from the results of PIEs for the B14 irradiation test fuel, which was a mixed oxide fuel and was irradiated in the experimental reactor Joyo. The thermal computation results showed that fuel restructuring in the stoichiometric oxide fuel was accelerated, though the fuel temperature in the stoichiometric oxide fuel was evaluated as lower than that of the hypo-stoichiometric one. We explained this behavior as follows: first, the fuel temperature decreased due to the high thermal conductivity at stoichiometry; second, the pore migration velocity increased due to the increase in vapor pressure caused by the high vapor pressure of UO$$_{3}$$, which was derived from the high oxygen potential at stoichiometry. In addition, our results indicated that the central void diameter strongly depended on not only fuel temperature, but also vapor pressure.

Journal Articles

Conceptual design of engineering-scale plant applied the simplified MA-bearing fuel fabrication process

Yamada, Yoshikazu; Segawa, Tomoomi; 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), 8 Pages, 2017/06

Japan Atomic Energy Agency (JAEA) have proposed the transmutation of minor actinides by fast reactors as a way to contribute significantly to the reduction of the volume and the potential radiotoxicity of radioactive wastes. In order to achieve this goal, it is important to introduce a fully automated and remote operation fuel fabrication plant with shielded hot cells and manipulators. JAEA's facilities including Plutonium Fuel Production Facility (PFPF) have fabricated MOX fuel. On the basis of the operational and technical experience obtained in above facilities, the conceptual design of engineering-scale plant applied the simplified MA-bearing fuel fabrication process with shielded hot cells and manipulator was done. It will be able to fabricate high MA-bearing fuel and to perform the maintenance and repairing of each equipment with manipulators. This plant will be constructed based on this concept and development plan.

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