International benchmark on radionuclide solubility and speciation for the Long-term In-situ Test (LIT) at Grimsel Test Site (GTS, Switzerland)

Noseck, U.*; Schfer, T.*; Alonso, U.*; Hamamoto, Takafumi*; Havlova, V.*; Hibberd, R.*; Ishidera, Takamitsu; Kitamura, Akira; Klajmon, M.*; Missana, T.*; et al.

Applied Geochemistry, 201, p.106762_1 - 106762_23, 2026/04

https://doi.org/10.1016/j.apgeochem.2026.106762

Thermodynamic benchmark calculations have been performed to better understand the behavior of Se(VI), Tc(VII), U(VI), Np(V), Am(III), Th(IV) and Pu(IV)) in the evolving geochemical conditions of the Long-term In-situ Test (LIT) at the Grimsel Test Site (GTS) and corresponding mock-up experiment. It also aims to identify the status of the geochemical speciation models and databases for these elements. The experiments are simulating the near-field conditions in some radioactive waste repository concept including a bentonite engineered barrier emplaced in crystalline rock and the findings are contributing to the long-term safety assessment of these facilities.

Redox dynamics of cerium ions in soda-lime glass during cooling analyzed by in situ X-ray absorption fine structure

Ozawa, Saki*; Shiozawa, Yudai*; Saijo, Yoshitaka*; Miyajima, Tatsuya*; Matsumura, Daiju; Tsuji, Takuya; Nakase, Masahiko*; Maehara, Terutaka*

Journal of the American Ceramic Society, 109(3), 10 Pages, 2026/00

https://doi.org/10.1111/jace.70621

Optimising sodium incorporation into potassium-activated metakaolin-based alkali-activated materials

Chaerun, R. I.; Sato, Junya; Hiraki, Yoshihisa; Yoshida, Yukihiko; Sato, Tsutomu*; Osugi, Takeshi

Construction and Building Materials, 500, p.144270_1 - 144270_10, 2025/11

https://doi.org/10.1016/j.conbuildmat.2025.144270

Alkali-activated materials (AAMs), particularly those derived from metakaolin, have gained significant attention as sustainable binders for hazardous waste immobilisation, owing to their dense microstructure and chemical durability. Their amorphous aluminosilicate framework enables effective encapsulation of hazardous materials and reduces environmental risks. However, maintaining the stability of this amorphous network is challenging, particularly when sodium (Na)-rich precursors are used, as excess Na) promotes crystallisation and compromises matrix integrity. This study systematically investigates the influence of Na) concentration on the structural stability of metakaolin-based AAMs activated primarily with potassium (K)). The objective is to identify the threshold Na incorporation level that preserves the amorphous structure and maintains chemical stability. Transmission electron microscopy (TEM), Raman spectroscopy, and thermodynamic modelling were employed to examine the structural evolution of K-AAMs across a range of Na:K molar ratios. The results reveal that higher Na:K ratios induce nanopore formation and early crystallisation of Na-rich zeolitic phases, which can reduce matrix stability. In contrast, an optimal Na:K ratio was identified that maintains the amorphous network and preserves the aluminosilicate framework. These findings provide valuable insights into optimising K-AAMs for advanced, durable waste encapsulation technologies.

Study on estimation of radioactivity concentration of biological shielding at Fukushima Daiichi Nuclear Power Station (Contract Research)

Collaborative Laboratories for Advanced Decommissioning Science; NAIS*

JAEA-Research 2025-004, 102 Pages, 2025/08

JAEA-Research-2025-004.pdf:3.33MB

For planning radioactive waste management at the Fukushima Daiichi Nuclear Power Station of the Tokyo Electric Power Company Holdings, Incorporated, estimation of radioactivity is essential with considering both contamination from the damaged fuel and activation during reactor operation; with regard to the latter, biological shielding is an important object due to its large amount. It is difficult to conduct field investigations or collect analysis samples at the site, hence the radioactivity should be estimated by calculative analysis with considering the actual conditions of the constituent materials, especially for activation of minor components and water, which affects the neutron flux. Besides it is important to assess the uncertainties involved in the calculation analysis. In this study, the trace composition and water content in the biological shielding concrete were investigated, and a three-dimensional computational model was constructed for the Unit 2 reactor building at the site to estimate the radioactivity concentration. In order to evaluate the uncertainty in the results, the factors contributing to the uncertainty were extracted and the uncertainty resulted from those factors on the calculation results, i.e. the influence of the diversity of the calculation model the parameters used in the calculation model. Based on the results, the dominant factors contributing to the uncertainty were extracted, and the handling as radioactive waste was discussed.

Chemical Kinetic Uncertainty Quantification in Hydrogen Combustion Computational Fluid Dynamics Simulation for ENACCEF2 Experiment

Motegi, Kosuke; Matsumoto, Toshinori; Shiotsu, Hiroyuki

Proceedings of 21st International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-21) (Internet), 10 Pages, 2025/08

Pressure-induced elongation of hydrogen-oxygen bond in sodium silicate melts

Ohashi, Tomonori*; Sakamaki, Tatsuya*; Funakoshi, Kenichi*; Steinle-Neumann, G.*; Hattori, Takanori; Yuan, L.*; Suzuki, Akio*

Journal of Mineralogical and Petrological Sciences (Internet), 120(1), p.240926a_1 - 240926a_13, 2025/06

https://doi.org/10.2465/jmps.240926a

We explore the structures of dry and hydrated (HO and DO) NaSiO melt at 0-6 GPa and 1000-1300 K and glasses recovered from high pressure and temperatures by in-situ neutron and X-ray diffraction. The structures of the melts at 0-10 GPa and 3000 K are also investigated by ab-initio molecular dynamics simulation. In-situ neutron experiments revealed that the D-O distance increases with compression due to the formation of -O-D-O- bridging species, which is reproduced by the molecular dynamics simulations. The pressure-induced -O-D-O- formation reflects a more rigid incorporation of hydrogen, which acts as a mechanism for the experimentally observed higher solubility of water in silicate melts. Together with shrinking modifier domains, this process dominates the compression behavior of hydrous NaSiO melt, whereas the compression of dry NaSiO at 0-10 GPa and 3000 K is governed largely by bending of the Si-O-Si angle. The molecular dynamics simulations on hydrous NaSiO melts further suggest that the sodium ions are scavenged from its network-modifying role via 2(Si-O + Na) Si-(O-Si-O) + 2Na and Si-O + Na + Si-OH Si-(O-H-O-Si) + Na with increasing pressure.

Investigation on multi-dimensional short-term behaviour through benchmark analysis of a large-volume sodium combustion experiment

Sonehara, Masateru; Okano, Yasushi; Uchibori, Akihiro; Oki, Hiroshi*

Journal of Nuclear Science and Technology, 62(5), p.403 - 414, 2025/05

https://doi.org/10.1080/00223131.2024.2441427

For sodium-cooled fast reactors, understanding sodium combustion behaviour is crucial for managing sodium leakage accidents. In this study, we perform benchmark analyses of the Sandia National Laboratories (SNL) T3 experiment using the multi-dimensional thermal hydraulic code AQUA-SF. Conducted in an enclosed space with a large vessel volume of 100 m and a sodium mass flow rate of 1 kg/s, the experiment highlighted the multi-dimensional effects of local temperature increase shortly after sodium injection. This study aims to extend the capabilities of AQUA-SF by focusing on the simulation of these multi-dimensional temperature variations, in particular the formation of high temperature regions at the bottom of the vessel. The proposed models include the temporary stopping of sodium droplet ignition and spray combustion of sodium splash on the floor. Furthermore, it has been shown that additional heat source near the floor is essential to enhance the reproduction of the high temperature region at the bottom. Therefore, case studies including sensitivity analyses of spray cone angle and prolonged combustion of droplets on the floor are conducted. This comprehensive approach provides valuable insights into the dynamics of sodium combustion and safety measures in sodium-cooled fast reactors.

Verification of direct coupling code system using FRENDY version 2 and GENESIS for light water reactor lattices

Fujita, Tatsuya; Yamamoto, Akio*

Journal of Nuclear Science and Technology, 62(2), p.179 - 196, 2025/02

https://doi.org/10.1080/00223131.2024.2410918

This study newly established a direct coupling code system consisting of the nuclear data processing code FRENDY version 2, and the three-dimensional heterogeneous transport code GENESIS (FRENDY-V2/GENESIS) for easy implementation of the random-sampling-based uncertainty quantification considering the implicit effect due to nuclear cross-section (XS) perturbations. The multi-group macroscopic XSs prepared for GENESIS were generated by FRENDY version 2, where the Dancoff factor was calculated by the neutron current method. Then the background XSs were evaluated based on the Carlvik two-term rational approximation. The infinite multiplication factor (k-infinity) and the fission reaction rate distribution in UO and MOX lattice geometries were compared with MVP3 to verify the calculation accuracy of FRENDY-V2/GENESIS. The sensitivity analyses on the discretization conditions such as the ray tracing of the method of characteristics were also carried out. Through several comparisons between FRENDY-V2/GENESIS and MVP3, FRENDY-V2/GENESIS with the SHEM 361-group structure calculates the k-infinity within approximately 50 pcm and the fission reaction rate distribution within approximately 0.1% by the root mean square, respectively. Consequently, the applicability of FRENDY-V2/GENESIS was verified, and FRENDY-V2/GENESIS can be used to discuss the implicit effect due to multi-group XS perturbations.

Enhancement of random sampling by a combined approach of control variates and Latin hypercube sampling for uncertainty quantification in light water reactor lattice calculations

Fujita, Tatsuya

Journal of Nuclear Science and Technology, 62(5), p.470 - 479, 2025/01

https://doi.org/10.1080/00223131.2024.2448320

This study confirmed the efficiency of a combined approach of the control variates (CV) and the Latin hypercube sampling (LHS), which enhanced the random-sampling-based uncertainty quantification due to cross-section (XS) covariance data, by considering the effect of statistical variation and also performed the sensitivity analyses on the influence due to the selection of alternative parameter to apply CV. The convergence performance for the uncertainty of infinite multiplication factor (k-infinity) during the random sampling was compared between several efficient sampling techniques such as the antithetic sampling (AS), LHS, CV, and the combined approaches of them in the PWR-UO fuel assembly geometry. The k-infinity uncertainty was evaluated by statistically processing several times Serpent2 calculations using perturbed ACE-formatted XS files based on ENDF/B-VIII.0. CV+LHS was more efficient than AS, LHS, and CV+AS. In addition, sensitivity analyses were performed to select alternative parameters used in CV. The 33 mini fuel lattice calculation can improve the efficiency of CV+LHS. The reason was qualitatively considered that this calculation can capture the influence of XS covariance data for Gd isotopes. Consequently, the applicability of CV+LHS for the improvement of convergence performance to evaluate the k-infinity uncertainty during the random sampling was confirmed.

Thermodynamic properties and revised Helgeson-Kirkham-Flowers equations of state parameters of the hydrated and dehydrated monomeric silica species at = 0.01-600C, = 1-3000 bars, = 0.35-1.1 g cm, and = 0

Walker, C. S.*; Arthur, R. C.*; Anraku, Sohtaro; Sasamoto, Hiroshi; Mihara, Morihiro

Applied Geochemistry, 175, p.106086_1 - 106086_17, 2024/11

https://doi.org/10.1016/j.apgeochem.2024.106086

The thermodynamic properties and revised Helgeson-Kirkham-Flowers equation of state (r-H-K-F EoS) parameters of the hydrated (Si(OH)(aq), SiO(OH) and SiO(OH)) and fictive dehydrated (SiO(aq), HSiO and SiO) monomeric silicon species are used extensively to describe the pH, composition, temperature, and pressure dependence of formation/breakdown reactions of all silicon-bearing compounds globally. Experimental log10 equilbrium constant, K values describing the formation reactions of the hydrated and dehydrated monomeric silicon species were therefore compiled from the literature, extrapolated to zero ionic strength by specific ion interaction theory as required and used to derive their thermodynamic properties and r-H-K-F EoS parameters. Consideration of all formation reactions in the same study provides a collective, internally consistent update to the thermodynamic properties and r-H-K-F EoS parameters of the monomeric silicon species that can provide a satisfactory match to the experimental log10 K values at = 0.01-600C, = 1-3000 bars, = 0.35-1.1 g cm, and zero ionic strength. These temperature and pressure limits comfortably bracket t=0.01-100C and P =1-270 bars relecant to the geological disposal of radioactive wastes at depths of up to 1 km.