Uranium-plutonium-oxygen phase diagram; Investigating the solvus of fluorite's exsolution

Vauchy, R.; Hirooka, Shun; Horii, Yuta; Ogasawara, Masahiro*; Sunaoshi, Takeo*; Yamada, Tadahisa*; Tamura, Tetsuya*; Murakami, Tatsutoshi

Journal of Nuclear Materials, 599, p.155233_1 - 155233_11, 2024/10

https://doi.org/10.1016/j.jnucmat.2024.155233

The fluorite exsolution/recombination in UPuO (y = 0.30 and 0.45) and PuO was investigated using differential scanning calorimetry. The results are in relatively good agreement with the literature data, except for plutonia. Our values indicate that the critical temperature of the miscibility gap in Pu-O is 3050 K lower than previously reported. Finally, the systematic experimental procedure allowed us refining the locus of the solvus existing in hypostoichiometric U0PuO, UPuO, and PuO dioxides.

Sintering behavior analysis of compacted dry recycled UPuO powder using master sintering curve theory

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

Journal of Nuclear Materials, 595, p.155072_1 - 155072_11, 2024/07

https://doi.org/10.1016/j.jnucmat.2024.155072

Thermal conductivity measurement of uranium-plutonium mixed oxide doped with Nd/Sm as simulated fission products

Horii, Yuta; Hirooka, Shun; Uno, Hiroki*; Ogasawara, Masahiro*; Tamura, Tetsuya*; Yamada, Tadahisa*; Furusawa, Naoya*; Murakami, Tatsutoshi; Kato, Masato

Journal of Nuclear Materials, 588, p.154799_1 - 154799_20, 2024/01

https://doi.org/10.1016/j.jnucmat.2023.154799

The thermal conductivities of near-stoichiometric (U,Pu,Am)O doped with NdO/SmO, which is major fission product (FP) generated by a uranium-plutonium mixed oxides (MOX) fuel irradiation, as simulated fission products are evaluated at 1073-1673 K. The thermal conductivities are calculated from the thermal diffusivities that are measured using the laser flash method. To evaluate the thermal conductivity from a homogeneity viewpoint of Nd/Sm cations in MOX, the specimens with different homogeneity of Nd/Sm are prepared using two kinds of powder made by ball-mill and fusion methods. A homogeneous Nd/Sm distribution decreases the thermal conductivity of MOX with increasing Nd/Sm content, whereas heterogeneous Nd/Sm has no influence. The effect of Nd/Sm on the thermal conductivity is studied using the classical phonon transport model (A+BT). The dependences of the coefficients A and B on the Nd/Sm content (C and C, respectively) are evaluated as: A(mK/W)=1.70 10 + 0.93C + 1.20C, B(m/W)=2.39 10.

Ionic radii in fluorites

Vauchy, R.; Hirooka, Shun; Murakami, Tatsutoshi

Materialia, 32, p.101934_1 - 101934_12, 2023/12

https://doi.org/10.1016/j.mtla.2023.101934

Lattice parameters of fluorite-structured uranium-americium mixed oxides

Vauchy, R.; Hirooka, Shun; Watanabe, Masashi; Yokoyama, Keisuke; Murakami, Tatsutoshi

Journal of Nuclear Materials, 584, p.154576_1 - 154576_11, 2023/10

https://doi.org/10.1016/j.jnucmat.2023.154576

Machine learning sintering density prediction model for MOX fuel pellet

Kato, Masato; Nakamichi, Shinya; Hirooka, Shun; Watanabe, Masashi; Murakami, Tatsutoshi; Ishii, Katsunori

Nihon Genshiryoku Gakkai Wabun Rombunshi (Internet), 22(2), p.51 - 58, 2023/04

https://doi.org/10.3327/taesj.J22.008

Uranium and Plutonium mixed oxide (MOX) pellets used as fast reactor fuels have been produced from several raw materials by mechanical blending method through processes of ball milling, additive blending, granulation, pressing, sintering and so on. It is essential to control the pellet density which is one of the important fuel specifications, but it is difficult to understand relationships among many parameters in the production. Database for MOX production was prepared from production results in Japan, and input data of eighteen types were chosen from production process and made a data set. Machine learning model to predict sintered density of MOX pellet was derived by gradient boosting regressor, and represented the measured sintered density with coefficient of determination of R=0.996

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

Engineering scale development test of MOX fuel fabrication technology to establish commercialized fast reactor fuel, 1; The O/M ratio preparation tests of sintered pellets

Takato, Kiyoto; Murakami, Tatsutoshi; Suzuki, Kiichi; Shibanuma, Kimikazu; Hatanaka, Nobuhiro; Yamaguchi, Bungo; Tobita, Yoshimasa; Shinozaki, Masaru; Iimura, Naoto; Okita, Takatoshi; et al.

JAEA-Technology 2013-026, 42 Pages, 2013/10

JAEA-Technology-2013-026.pdf:3.17MB

In order to cope with making a commercial fast reactor fuel burn-up higher, oxygen-to-metal (O/M) ratio in the fuel specification is designed to 1.95. As the test for the fabrication of such low O/M ratio pellets, two kinds of O/M ratio preparation tests of different reduction mechanism were done. In the first test, we evaluated the technology to prepare the O/M ratio low by annealing the sintered pellets in production scale. In addition, we know from past experience that O/M ratio of the sintered pellets can be reduced by residual carbon when the de-waxed pellets with high carbon content are sintered. Thus, in another test, the green pellets containing a large amount of organic additives were sintered and we evaluated the technology to produce the low O/M ratio sintered pellets by the reduction due to residual carbon. From the first test results, we found a tendency that the higher annealing temperature or the longer annealing time resulted in the lower O/M ratio. However, the amount of O/M ratio reduction was small and it is estimated that a substantial annealing time is necessary to prepare the O/M ratio to 1.95. It is considered that reducing O/M ratio by annealing was difficult because atmosphere gas containing oxygen released from pellets remained and the O/M ratio was changed to the value equilibrated with the gas having high oxygen potential. From another test results, it was confirmed that O/M ratio was reduced by the reduction due to residual carbon. We found that it was important to manage an oxygen potential of atmosphere gas in a sintering furnace low to reduce the O/M ratio effectively.

Prevention of segregation of pore former by granulating with MOX powder in low density pellet fabrication for fast breeder reactors

Murakami, Tatsutoshi; Aono, Shigenori

Proceedings of 5th International Granulation Workshop (CD-ROM), 10 Pages, 2011/06

Japan Atomic Energy Agency has been working to advance fabrication technology of mixed plutonium-uranium oxide fuel pellets for fast breeder reactors. In brief, the usual fabrication method of MOX pellets for FBRs consists of granulating raw MOX powder by a tabletting method, followed by pressing into compacts. Then, the compacts are sintered to get the MOX pellets. For the FBR "MONJU", MOX pellets having low density are required as the fuel pellets. The low density pellets are fabricated by adding an organic additive called a "pore former" to the MOX powder. The pore former is thermally decomposed and pores are incorporated into MOX pellets by sintering the compacts containing the pore former. In the past, the pore former was blended with the granulated MOX powder after the granulation process. But the pore former became segregated from the granulated MOX powder during feeding to the press machine, because the specific gravity of pore former is significantly lower than that of granulated MOX powder. In order to solve the problem, blending the raw MOX powder with the pore former was carried out before the granulation process to keep the pore former in the granulated MOX powder. As the result, segregation of pore former was prevented.

Confirmation tests for fabrication of low density MOX pellet for FBR

Murakami, Tatsutoshi; Suzuki, Kiichi; Hatanaka, Nobuhiro; Hanawa, Yukio; Shinozaki, Masaru; Murakami, Shinichi; Tobita, Yoshimasa; Kawasaki, Takeshi; Kobayashi, Yoshihito; Iimura, Naoto; et al.

JAEA-Technology 2008-017, 97 Pages, 2008/03

JAEA-Technology-2008-017.pdf:2.76MB

Low density MOX pellets for FBR "MONJU" have not been fabricated in Plutonium Fuel Fabricating Facility (PFPF) for these 9 years since completion of the first reload fuel for "MONJU" in 1995. In this period, about 60 % of machines in the pellet fabrication process of PFPF have been replaced with new ones, and fabrication of MOX pellets for "JOYO" has been continued using these machines. Concerning the feed MOX powders for "MONJU", the amount of decay heat has been increased with increase of accumulated Am-241 in this period. In addition, powder characteristic of recycled MOX powder which is one of feed powders, MH-MOX powder, UO powder and recycled MOX powder, was significantly changed by replacing former processing machine used for scrap recycling with improved one. Using MOX powder with increased decay heat and recycled MOX powder processed by new machine, a series of low density MOX pellet fabrication tests were conducted to confirm pellet fabrication conditions for current pellet fabrication machines from October in 2004 to August in 2006. As a conclusion, it was confirmed that low density MOX pellets could be fabricated using these feed powders and replaced machines by adjusting pellet fabrication conditions adequately. This report summarizes the results of a series of low density MOX pellet fabrication tests.