Investigation of effects of nano interfacial phenomena on dissolution aggregation of alpha nanoparticles by using micro nano technologies (Contract research); FY2023 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Institute of Science Tokyo*

JAEA-Review 2025-026, 72 Pages, 2025/11

JAEA-Review-2025-026.pdf:7.97MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2023. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2022, this report summarizes the research results of the "Investigation of effects of nano interfacial phenomena on dissolution aggregation of alpha nanoparticles by using micro nano technologies" conducted in FY2023. To ensure the safety of retrieval and storage management of nuclear fuel debris generated by the Fukushima-Daiichi Nuclear Power Station accident, understanding of dissolution-denaturation behavior of the fuel debris alpha particles is one of the most crucial issues. This research aims to create novel microfluidic real-time measurement device for elucidating dissolution, aggregation, and denaturation processes of metal oxide nanoparticles under various solution environments, and clarify their nano-size and interfacial effects. In this year, we conducted bulk and micro dissolution tests of simulated fuel debris particles (UO mechanical-treated nanoparticles, UO chemical-treated nanoparticles, and (U,Zr)O nanoparticles), and successfully clarified that the effects of particle sizes, reaction times, and HO concentrations on the dissolution behavior of each nanoparticle. In particular, it was found that (U,Zr)O nanoparticles have different degrees of Zr catalytic reactions depending on HO concentrations, resulting in the generation of different amounts of gas and U. Moreover, we developed a new microfluidic device which enables to instantly react the nanoparticles with HO solutions, and determined dynamic aggregation and dissolution rates of the nanoparticles. The research was carried out in close collaboration with UK researchers, and achieved the expected goal of this year.

Investigation of effects of nano interfacial phenomena on dissolution aggregation of alpha nanoparticles by using micro nano technologies (Contract research); FY2022 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*

JAEA-Review 2024-022, 59 Pages, 2024/09

JAEA-Review-2024-022.pdf:4.27MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2022. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2022, this report summarizes the research results of the "Investigation of effects of nano interfacial phenomena on dissolution aggregation of alpha nanoparticles by using micro nano technologies" conducted in FY2022. To ensure the safety of retrieval and storage management of nuclear fuel debris generated by the Fukushima Daiichi Nuclear Power Station accident, understanding of dissolution-denaturation behavior of the fuel debris alpha particles is one of the most crucial issues. This research aims to create novel microfluidic real-time measurement device for elucidating dissolution, aggregation, and denaturation processes of metal oxide nanoparticles under various solution environments, and clarify their nano-size and interfacial effects.

UO dissolution in bicarbonate solution with HO; The Effect of temperature

McGrady, J.; Kumagai, Yuta; Kitatsuji, Yoshihiro; Kirishima, Akira*; Akiyama, Daisuke*; Watanabe, Masayuki

RSC Advances (Internet), 13(40), p.28021 - 28029, 2023/09

https://doi.org/10.1039/D2RA08131H

Upon nuclear waste canister failure and contact of spent nuclear fuel with groundwater, the UO matrix of spent fuel will interact with oxidants in the groundwater generated by water radiolysis. Bicarbonate (HCO) is often found in groundwater, and the HO induced oxidative dissolution of UO in bicarbonate solution has previously been studied under various conditions. Temperatures in the repository at the time of canister failure will differ depending on the location, yet the effect of temperature on oxidative dissolution is unknown. To investigate, the decomposition rate of HO at the UO surface and dissolution of U in bicarbonate solution (0.1, 1, 10 and 50 mM) was analysed at various temperatures (10, 25, 45 and 60 C). At [HCO] 1 mM, the apparent equilibrium concentration of U decreased with increasing temperature. This was attributed to the formation of U-bicarbonate species at the surface and a change in the mechanism of HO decomposition from oxidative to catalytic. At 0.1 mM, no obvious correlation between temperature and U dissolution was observed, and thermodynamic calculations indicated this was due to a change in the surface species. A pathway to explain the observed dissolution behaviour of UO in bicarbonate solution as a function of temperature was proposed.

An Experimental study on the degradation of UO/Fe(0) by bacteria

Liu, J.; Dotsuta, Yuma; Kitagaki, Toru; Takano, Masahide; Onuki, Toshihiko; Kozai, Naofumi

Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR2022) (Internet), 2 Pages, 2022/10

Nuclear fuel debris, consisting primarily of nuclear fuel and structural material, was formed during the Fukushima Daiichi NPP accident and exists in the cooling water accumulated in the primary containment vessels. Microorganisms living in groundwater may come into contact with the fuel debris and react with it. To assess the degradation of fuel debris, it is necessary to evaluate the interactions between microorganisms and fuel debris. Here we performed an experimental study on bacterial degradation. A mixed powder of UO and Fe(0) was used as a fuel debris simulant. Bacillus subtilis, which is widespread bacteria in nature and thought to be present at the accident site, was used. The mixed powder was exposed to the Bacillus subtilis in a liquid medium for some days. It was found that the oxidative dissolution of the U(IV) and Fe(0) was accelerated by B. subtilis. A fraction of the dissolved U(VI) was precipitated together with iron precipitates which are probably amorphous Fe(III) hydroxides. The study indicates that microorganisms would cause the degradation of fuel debris.

Dissolution and precipitation behaviors of zircon under the atmospheric environment

Kitagaki, Toru; Yoshida, Kenta*; Liu, P.*; Shobu, Takahisa

npj Materials Degradation (Internet), 6(1), p.13_1 - 13_8, 2022/02

https://doi.org/10.1038/s41529-021-00214-0

Review and evaluation on the surface area of vitrified products of high-level waste; Surface area increase factors due to fracturing and their bases for the performance assessment of geological disposal

Igarashi, Hiroshi

JAEA-Review 2020-006, 261 Pages, 2020/09

JAEA-Review-2020-006.pdf:4.42MB

A literature review was conducted on the increase in surface area of vitrified products of HLW due to the fracturing caused by cooling during glass pouring process and by mechanical impact, from the perspective of a parameter of the radionuclide release model in the performance assessment of geological disposal system studied overseas. The review was focused on the value of surface area increase factor set as a parameter in the model, the experimental work to evaluate an increase in surface area, and how the parameters on surface area were determined based on the experimental results. The surface area obtained from the experiments executed in Japan was also discussed in comparison with the overseas studies. On the basis of the investigation, the effects of various conditions on the surface area were studied, such as a diameter of vitrified product, cooling condition during and after the glass pouring, impact on vitrified products during their handling, environment after the closure of disposal facility, and others. The causes of fracturing are associated with the phenomena or events in the waste management process such as production, transport, storage, and disposal. The surface area increase factors set in the nuclide release model of the glass and their bases were reviewed. In addition, the measured values and the experimental methods for surface increase factors published so far were compared. Accordingly, the methods for measuring surface area as the bases were identified for these factors set in the models. The causes of fracturing and features of these factors were studied with respect to the relation with the waste management process. The results from the review and assessment can contribute to the expanding the knowledge for the conservative and realistic application of these factors to performance assessment, and to the developing and upgrading of safety case as a consequence.

Flow-accelerated corrosion of type 316L stainless steel caused by turbulent lead-bismuth eutectic flow

Wan, T.; Saito, Shigeru

Metals, 8(8), p.627_1 - 627_22, 2018/08

https://doi.org/10.3390/met8080627

Effects of -radiation on a direct disposal system for spent nuclear fuel, 2; Review of research into safety assessments of direct disposal of spent nuclear fuel in Europe and North America

Kitamura, Akira; Takase, Hiroyasu*; Metcalfe, R.*; Penfold, J.*

Journal of Nuclear Science and Technology, 53(1), p.19 - 33, 2016/01

https://doi.org/10.1080/00223131.2015.1014874

Not only geological disposal of vitrified waste generated by spent fuel (SF) reprocessing, but also the possibility of disposing of SF itself in deep geological strata (hereinafter "direct disposal of SF") may be considered in the Japanese geological disposal program. In the case of direct disposal of SF, the radioactivity of the waste is higher and the potential effects of the radiation are greater. Specific examples of the possible effects of radiation include: increased amounts of canister corrosion; generation of oxidizing chemical species in conjunction with radiation degradation of groundwater and accompanying oxidation of reducing groundwater; and increase in the dissolution rate and the solubility of SF. Therefore, the influences of radiation, which are not expected to be significant in the case of geological disposal of vitrified waste, must be considered in safety assessments for direct disposal of SF. Focusing especially on the effects of -radiation in safety assessment, this study has reviewed safety assessments in countries other than Japan that are planning direct disposal of SF. The review has identified issues relevant to safety assessment for the direct disposal of SF in Japan.

Experimental and modeling study on long-term alteration of compacted bentonite with alkaline groundwater

Yamaguchi, Tetsuji; Sakamoto, Yoshifumi; Akai, Masanobu; Takazawa, Mayumi; Iida, Yoshihisa; Tanaka, Tadao; Nakayama, Shinichi

Physics and Chemistry of the Earth, 32(1-7), p.298 - 310, 2007/00

https://doi.org/10.1016/j.pce.2005.10.003

Dissolution rate of montmorillonite, diffusivity of hydroxide ion and permeability coefficient in compacted sand-bentonite mixtures were experimentally determined and formulated. A coupled mass-transport/chemical-reaction code was developed to predict variation in permeability of engineered bentonite barrier with alkaline fluid by using the formulae.

Study on electrolytic reduction of pertechnetate in nitric acid solution for electrolytic extraction of rare metals for future reprocessing

Asakura, Toshihide; Kim, S.-Y.; Morita, Yasuji; Ozawa, Masaki*

Journal of Nuclear and Radiochemical Sciences, 6(3), p.267 - 269, 2005/12

https://doi.org/10.14494/jnrs2000.6.3_267

An electrolytic extraction (EE) method, i.e. electro-reductive deposition, of Tc from nitric acid aqueous solution was studied for future reprocessing. After 30 min of constant potential electrolysis by carbon electrode at -0.3 V vs. SSE (Standard Silver Electrode), Tc concentration in 3 M nitric acid decreased to 93 % of the initial value, which corresponds to 7 % of deposition. With co-existence of Pd, the value reached to 15 % of deposition equivalent by electrolysis at 0.0 V vs. SSE for 60 min. An acceleration effect of Pd on Tc deposition (promoter effect) was suggested. The concentration, however, increased to the initial value after further electrolysis and competing re-dissolution of deposited Tc was also suggested. In cyclic voltammetry measurements, it was found that the deposit from Tc-Pd-Ru-Rh solution dissolved easier than that from Pd-Ru-Rh did. In electrolyzed Tc solution, an absorption peak at 482 nm was found. It can be attributed to the complex with nitrite anion, and the complex formation is proposed as one possible mechanism of Tc re-dissolution.