Oxygen potential of neodymium-doped UPuAmO uranium-plutonium-americium mixed oxides at 1573, 1773, and 1873 K

Vauchy, R.; Sunaoshi, Takeo*; Hirooka, Shun; Nakamichi, Shinya; Murakami, Tatsutoshi; Kato, Masato

Journal of Nuclear Materials, 580, p.154416_1 - 154416_11, 2023/07

https://doi.org/10.1016/j.jnucmat.2023.154416

Toward long-term storage of nuclear materials in MOX fuels fabrication facility

Hirooka, Shun; Nakamichi, Shinya; Matsumoto, Taku; Tsuchimochi, Ryota; Murakami, Tatsutoshi

Frontiers in Nuclear Engineering (Internet), 2, p.1119567_1 - 1119567_7, 2023/03

https://doi.org/10.3389/fnuen.2023.1119567

Storage of plutonium (Pu)-containing materials requires extremely strict attention in terms of physical safety and material accounting. Despite the emphasized importance of storage management, only a few reports are available in the public, e.g., experience in PuO storage in the UK and safety standards in the storage of Pu-containing materials in the US. Japan also stores more U-Pu mixed oxide (MOX) mostly in powder form. Adopting an appropriate storage management is necessary depending on the characteristics of MOX items such as raw powder obtained by reprocessing of spent Light Water Reactor fuels, research and development on the remains of fuel fabrication, which can contain organic materials, and dry-recycled powder during fuel fabrication. Stagnation in fuel fabrications and experience in degradation of MOX containers during extended period of storage have led to the review of the storage method in the Plutonium Fuel Development Center in Japan Atomic Energy Agency. The present work discusses the various nuclear materials, storage methods, experience in degradation of containers that occur during storage, and strategies for future long-term storage.

Liquid phase sintering of alumina-silica co-doped cerium dioxide CeO ceramics

Vauchy, R.; Hirooka, Shun; Watanabe, Masashi; Yokoyama, Keisuke; Sunaoshi, Takeo*; Yamada, Tadahisa*; Nakamichi, Shinya; Murakami, Tatsutoshi

Ceramics International, 49(2), p.3058 - 3065, 2023/01

https://doi.org/10.1016/j.ceramint.2022.09.295

Sintering and microstructural behaviors of mechanically blended Nd/Sm-doped MOX

Hirooka, Shun; Horii, Yuta; Sunaoshi, Takeo*; Uno, Hiroki*; Yamada, Tadahisa*; Vauchy, R.; Hayashizaki, Kohei; Nakamichi, Shinya; Murakami, Tatsutoshi; Kato, Masato

Journal of Nuclear Science and Technology, p.1 - 11, 2023/00

https://doi.org/10.1080/00223131.2023.2192725

Additive MOX pellets are fabricated by a conventional dry powder metallurgy method. NdO and SmO are chosen as the additive materials to simulate the corresponding soluble fission products dispersed in MOX. Shrinkage curves of the MOX pellets are obtained by dilatometry, which reveal that the sintering temperature is shifted toward a value higher than that of the respective regular MOX. The additives, however, promote grain growth and densification, which can be explained by the effect of oxidized uranium cations covering to a pentavalent state. Ceramography reveals large agglomerates after sintering, and Electron Probe Micro-Analysis confirms that inhomogeneous elemental distribution, whereas XRD reveals a single face-centered cubic phase. Finally, by grinding and re-sintering the specimens, the cation distribution homogeneity is significantly improved, which can simulate spent nuclear fuels with soluble fission products.

Materials science and fuel technologies of uranium and plutonium mixed oxide

Kato, Masato; Machida, Masahiko; Hirooka, Shun; Nakamichi, Shinya; Ikusawa, Yoshihisa; Nakamura, Hiroki; Kobayashi, Keita; Ozawa, Takayuki; Maeda, Koji; Sasaki, Shinji; et al.

Materials Science and Fuel Technologies of Uranium and Plutonium mixed Oxide, 171 Pages, 2022/10

https://doi.org/10.1201/9781003298205

Innovative and advanced nuclear reactors using plutonium fuel has been developed in each country. In order to develop a new nuclear fuel, irradiation tests are indispensable, and it is necessary to demonstrate the performance and safety of nuclear fuels. If we can develop a technology that accurately simulates irradiation behavior as a technology that complements the irradiation test, the cost, time, and labor involved in nuclear fuel research and development will be greatly reduced. And safety and reliability can be significantly improved through simulation of nuclear fuel irradiation behavior. In order to evaluate the performance of nuclear fuel, it is necessary to know the physical and chemical properties of the fuel at high temperatures. And it is indispensable to develop a behavior model that describes various phenomena that occur during irradiation. In previous research and development, empirical methods with fitting parameters have been used in many parts of model development. However, empirical techniques can give very different results in areas where there is no data. Therefore, the purpose of this study is to construct a scientific descriptive model that can extrapolate the basic characteristics of fuel to the composition and temperature, and to develop an irradiation behavior analysis code to which the model is applied.

Advanced reactor experiments for sodium fast reactor fuels (ARES) project; Transient irradiation experiments for metallic and MOX fuels

Jensen, C. B.*; Wachs, D. M.*; Woolstenhulme, N. E.*; Ozawa, Takayuki; Hirooka, Shun; Kato, Masato

Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Sustainable Clean Energy for the Future (FR22) (Internet), 9 Pages, 2022/04

Development of fuel performance analysis code, BISON for MOX, named Okami; Analyses of pore migration behavior to affect the MA-bearing MOX fuel restructuring

Ozawa, Takayuki; Hirooka, Shun; Kato, Masato; Novascone, S.*; Medvedev, P.*

Journal of Nuclear Materials, 553, p.153038_1 - 153038_16, 2021/09

https://doi.org/10.1016/j.jnucmat.2021.153038

To evaluate the O/M dependence of pore migration regarding fuel restructuring at the beginning of irradiation, we are developing BISON for MOX in cooperation with INL and have installed pore migration model considering vapor pressure of vapor species and thermal conductivity for MOX. The O/M dependence of fuel restructuring observed in MA-bearing MOX irradiation experiment in Joyo was evaluated by the 2-dimensional analyses. Four MA-bearing MOX pins with different O/M ratio and pellet/cladding gap size were irradiated in Joyo B14 experiment. Remarkable restructuring of stoichiometric MA-bearing MOX fuels was observed in PIE, and could be evaluated by considering the influence of O/M ratio on vapor pressure. Also, a central void assumes to move toward wide-gap side when the pellet eccentricity taking place, but 2-dimentional analyses on pellet transverse section revealed that the central void formation observed in PIE would be inconsistent with a direction of the pellet eccentricity.

Effect of O/M ratio on sintering behavior of (PuU)O

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

https://doi.org/10.1016/j.jnucmat.2020.152188

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 (PuU)O and (PuU)O in controlled po atmosphere were investigated. It was found activation energy of (PuU)O was higher than that of (PuU)O. On the other hand, it was observed grain growth during sintering was suppressed in hypo-stoichiometric composition.

Oxygen potential and self-irradiation effects on fuel temperature in Am-MOX

Ikusawa, Yoshihisa; Hirooka, Shun; Uno, Masayoshi*

2018 GIF Symposium Proceedings (Internet), p.321 - 327, 2020/05

Research and development of Minor actinides (MAs) bearing MOX fuel for fast reactor has been proceeding from the viewpoint of reducing radioactive waste. In order to develop, MA bearing MOX, it is indispensable to clarify the influence of MA addition on irradiation behavior. The addition of Americium (Am) to MOX affects vapor pressure and thermal conductivity, which are important properties from the perspective of evaluating fuel temperature. This is because vapor pressure affects fuel restructuring, and thermal conductivity affects fuel temperature distribution. Focusing on these physical properties, this study evaluates the influence of Am on fuel temperature using irradiation behavior analysis code to contribute to the development of MA-bearing MOX fuel. An increase in Am content decreases the thermal conductivity and increases the oxygen potential of oxide fuel. Because vapor pressure increases with increasing Am content, pore migration is accelerated, and the central void diameter increases with increasing Am content. As a result, after formation of the central void, the influence of Am content on the fuel center temperature is mild. Alpha particles generated by radioactive decay of transuranium elements cause lattice defects in the oxide fuel pellets. It is well known that this phenomenon, which is called self-irradiation, affects thermal conductivity. Since americium is the typical alpha radioactive nucleus, to evaluate fuel temperature of Am-MOX is necessary to take account of the influence of self-irradiation damage on thermal conductivity. Self-irradiation decreases thermal conductivity, and as the Am content increases, the rate of decrease in thermal conductivity is accelerated. Because it recovers with temperature rise, the decrease in thermal conductivity due to self-irradiation damage has very little effect on fuel center temperature. These results suggest that Am-MOX fuel could be irradiated under the same conditions as conventional MOX fuel.

Sound speeds in and mechanical properties of (U,Pu)O

Hirooka, Shun; Kato, Masato

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

https://doi.org/10.1080/00223131.2017.1397564

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.