Horonobe Underground Research Laboratory Project Investigation Program for the Fiscal Year 2025

Nakayama, Masashi; Ishii, Eiichi; Hayano, Akira; Aoyagi, Kazuhei; Murakami, Hiroaki; Ono, Hirokazu; Takeda, Masaki; Mochizuki, Akihito; Ozaki, Yusuke; Kimura, Shun; et al.

JAEA-Review 2025-027, 80 Pages, 2025/09

JAEA-Review-2025-027.pdf:6.22MB

The Horonobe Underground Research Laboratory Project is being pursued by the Japan Atomic Energy Agency to enhance the reliability of relevant technologies for geological disposal of high-level radioactive waste through investigating the deep geological environment within the host sedimentary rocks at Horonobe Town in Hokkaido, north Japan. In the fiscal year 2025, we continue R&D on "Study on near-field system performance in geological environment" and "Demonstration of repository design options". These are identified as key R&D challenges to be tackled in the Horonobe underground research plan for the fiscal year 2020 onwards. In the "Study on near-field system performance in geological environment", we continue to obtain data from the full-scale engineered barrier system performance experiment, and work on the specifics of the full-scale engineered barrier system dismantling experiment. As for "Demonstration of repository design options", the investigation, design, and evaluation techniques are to be systemized at various scales, from the tunnel to the pit, by means of an organized set of evaluation methodologies for confinement performance at these respective scales. Preliminary borehole investigations will be conducted within a 500 m gallery, with the objectives of obtaining rock strength and rock permeability data, as well as surveying the extent of the excavation damaged zone surrounding the test tunnel via tomographic analysis. A planning study for the in-situ construction test will be conducted to investigate the construction of backfill material and watertight plugs. The volume of water inflow associated with the excavation of the 500 m gallery will be observed, and its magnitude will be compared with the range of water inflow predicted in the analysis. The test plan to determine the extent of the excavation damaged zone around the pit, which is planned to be constructed in the 500 m gallery, will be studied to determine the in-situ excavation damaged zone. In addition, the investigation and evaluation methods for the amount of water inflow from fractures and the extent of the excavation damaged zone around the pit will be organized. Concerning the construction and maintenance of the subsurface facilities, excavation of the West Access Shaft and the 500 m gallery will continue. It is anticipated that the construction of the facilities will be completed by the end of the fiscal year 2025. In addition, we continue R&D on the following three tasks in the Horonobe International Project; Task A: Solute transport experiment with model testing, Task B: Systematic integration of repository technology options, and Task C: Full-scale engineered barrier system dismantling experiment.

Effect of Am addition on oxygen potential in (UPuAm)O

Yokoyama, Keisuke; Watanabe, Masashi; Usui, Akane; Seki, Takayuki*; Onishi, Takashi; Kato, Masato

Nuclear Materials and Energy (Internet), 42, p.101908_1 - 101908_6, 2025/03

https://doi.org/10.1016/j.nme.2025.101908

Oxygen potential of high Am content MOX, (UPuAm)O, was measured at 1273 K, 1473 K, 1573 K, and 1623 K. by gas equilibrium method using thermogravimeter. Comparing the measured data with the literature data, it was found that the addition of 15% Am increases the oxygen potential of (U, Pu)O by 100-150 kJ/mol for the same Pu content and O/M ratio. The proportion of cations in the stoichiometric composition was determined as (UUPuAm)O, assuming the presence of Am and partial oxidation of U to U. The relationship between oxygen partial pressure and deviation x from stoichiometry in (UPuAm)O was analyzed by defect chemistry model. The equation to represent the O/M ratio was derived as a function of temperature and oxygen partial pressure. A part of this study includes the results of MEXT Innovative Nuclear Research and Development Program Grant Number JPMXD0219214921.

A Science-based mixed oxide property model for developing advanced oxide nuclear fuels

Kato, Masato; Oki, Takumi; Watanabe, Masashi; Hirooka, Shun; Vauchy, R.; Ozawa, Takayuki; Uwaba, Tomoyuki; Ikusawa, Yoshihisa; Nakamura, Hiroki; Machida, Masahiko

Journal of the American Ceramic Society, 107(5), p.2998 - 3011, 2024/05

https://doi.org/10.1111/jace.19609

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

Oxygen potential, oxygen diffusion, and defect equilibria in UO

Watanabe, Masashi; Kato, Masato

Frontiers in Nuclear Engineering (Internet), 1, p.1082324_1 - 1082324_9, 2023/01

https://doi.org/10.3389/fnuen.2022.1082324

Since the oxygen potential and the oxygen coefficient of UO have a significant impact on fuel performance, many experimental data have been obtained. However, experimental data of the oxygen potential and the oxygen diffusion coefficient in the high temperature region above 1673 K are very limited. In the present study, we aimed to obtain these data and analyze them by defect chemistry. The oxygen potentials and the oxygen chemical diffusion coefficient of UO were measured by the gas equilibrium method in the near stoichiometric region at temperatures ranging from 1673 to 1873 K. A data set of oxygen potentials was made together with literature data and analyzed by defect chemistry. The oxygen potential of UO was determined as a function of O/U ratio and temperature, and an equation representing the relationship was derived. The oxygen chemical diffusion coefficient values obtained in this study were reasonably close to the literature values. The oxygen partial pressure dependence of the oxygen chemical diffusion coefficients was predicted from the evaluated results of the oxygen potential data, but no clear dependence was observed.

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.

Defect equilibria and thermophysical properties of CeO based on experimental data and density functional theory calculation result

Watanabe, Masashi; Nakamura, Hiroki; Suzuki, Kiichi; Machida, Masahiko; Kato, Masato

Journal of the American Ceramic Society, 105(3), p.2248 - 2257, 2022/03

https://doi.org/10.1111/jace.18249

Properties of CeO were evaluated by DFT simulation to determine band gap, Frenkel defect formation energy and defect migration energy. Band gap and Frenkel defect formation energy were used to analyze defect equilibria. Oxygen partial pressure dependence of defect equilibria was evaluated based on oxygen potential experimental data and DFT calculation, and a Brouwer diagram was derived. The defect formation energies, including Frenkel defect, electron-hole pair and so on, were determined and used to evaluate the properties, including oxygen diffusion coefficients, electrical conduction, heat capacity and thermal conductivity. Mechanisms of various properties were discussed for a deeper understanding based on defect chemistry, and the relationship among properties were systematically described.

Multi-stepwise pulse calorimetry for accurate, efficient measurements of thermophysical properties over a wide temperature range

Watanabe, Hiromichi*; Morimoto, Kyoichi; Watanabe, Masashi; Kato, Masato; Arita, Yuji*; Konashi, Kenji*

Thermochimica Acta, 693, p.178763_1 - 178763_6, 2020/11

https://doi.org/10.1016/j.tca.2020.178763

Multi-stepwise pulse calorimetry is proposed for accurate, efficient measurements of thermophysical properties of not only ideal but also practical samples over a wide temperature range. In a single experiment for a few seconds, the sample is rapidly heated from 298 K up to the final step-temperature of around 2850 K in a multi-stepwise fashion with numerous step-temperatures, at each of which the sample attains a steady-state condition while it is maintained for an instant. The proposed calorimetry is suitable for measuring enthalpy at numerous different temperatures, because multiple enthalpy-change values between the brief steady-state conditions can be obtained in a single experiment. As a feasibility demonstration, the specific enthalpy and its uncertainty in the temperature range 10502850 K have been determined for Mo and W, respectively. The measured enthalpies and emissivities are compared with the corresponding standard data.

Physical properties of non-stoichiometric (U,Pu)O

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. 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 are presented. The data set would be available in development of a fuel performance code.

Density Functional Theory (DFT)-based bonding analysis correlates ligand field strength with Ru Mssbauer parameters of ruthenium-nitrosyl complexes

Kaneko, Masashi; Kato, Akane*; Nakashima, Satoru*; Kitatsuji, Yoshihiro

Inorganic Chemistry, 58(20), p.14024 - 14033, 2019/10

https://doi.org/10.1021/acs.inorgchem.9b02024

We applied density functional theory calculations to ruthenium-nitrosyl complexes, which are known to exist in high-level radioactive waste, to give a theoretical correlation between Ru Mssbauer spectroscopic parameters ( and ) and ligand field strength () for the first time. The structures of the series of complexes, [Ru(NO)L] (L = Br, Cl, NH, CN), were modeled based on the corresponding single-crystal X-ray coordinates. The comparisons of the geometries and total energies between the different spin states suggested that the singlet spin state of [Ru(II)(NO)L] complexes were the most stable. The calculated results of both the and values reproduced the experimental results by reported previously and increased in the order of L = Br, Cl, NH, CN. Finally, we estimated the ligand field strength () based on molecular orbitals, assuming C symmetry and showed the increase of values in that order, being consistent with well-known spectrochemical series of ligands. The increase attributes to the strengthening of the abilities of -donor and -acceptor of the L-ligands to the Ru atom, resulting in the increase of the values.