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JAEA Reports

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.

Journal Articles

Progress status and future issues of development of analysis and estimation technology for fuel debris characterization, 3; Activities toward enhanced analysis accuracy of fuel debris

Ikeuchi, Hirotomo; Koyama, Shinichi

Nihon Genshiryoku Gakkai-Shi ATOMO$$Sigma$$, 66(2), p.74 - 78, 2024/02

For the steady removal of fuel debris from the TEPCO's Fukushima Daiichi Nuclear Power Station (1F), it is an urgent issue to establish analysis technology and systems for fuel debris samples with unknown properties (unknown samples). For this purpose, through analysis tests using samples with known properties (simulated fuel debris) and discussions among experts, the validity of analysis results and the factors that cause errors has been identified. In addition to knowing the current level of analysis accuracy, studies are being conducted to understand and improve the influencing factors. This paper introduces a part of the development of infrastructure for analysis and evaluation technology of "nuclides and element content."

Journal Articles

UO$$_{2}$$ dissolution in bicarbonate solution with H$$_{2}$$O$$_{2}$$; 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

 Times Cited Count:1 Percentile:0.00(Chemistry, Multidisciplinary)

Upon nuclear waste canister failure and contact of spent nuclear fuel with groundwater, the UO$$_{2}$$ matrix of spent fuel will interact with oxidants in the groundwater generated by water radiolysis. Bicarbonate (HCO$$_{3}$$$$^{-}$$) is often found in groundwater, and the H$$_{2}$$O$$_{2}$$ induced oxidative dissolution of UO$$_{2}$$ 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 H$$_{2}$$O$$_{2}$$ at the UO$$_{2}$$ surface and dissolution of U$$^{VI}$$ in bicarbonate solution (0.1, 1, 10 and 50 mM) was analysed at various temperatures (10, 25, 45 and 60 $$^{circ}$$C). At [HCO$$_{3}$$$$^{-}$$] $$geqq$$ 1 mM, the apparent equilibrium concentration of U$$^{VI}$$ decreased with increasing temperature. This was attributed to the formation of U$$^{VI}$$-bicarbonate species at the surface and a change in the mechanism of H$$_{2}$$O$$_{2}$$ 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$$_{2}$$ in bicarbonate solution as a function of temperature was proposed.

Journal Articles

Double diffusive dissolution model of UO$$_{2}$$ pellet in molten Zr cladding

Ito, Ayumi*; Yamashita, Susumu; Tasaki, Yudai; Kakiuchi, Kazuo; Kobayashi, Yoshinao*

Journal of Nuclear Science and Technology, 60(4), p.450 - 459, 2023/04

 Times Cited Count:0 Percentile:0.00(Nuclear Science & Technology)

Journal Articles

Potential bacterial alteration of nuclear fuel debris; A Preliminary study using simulants in powder and pellet forms

Liu, J.; Dotsuta, Yuma; Sumita, Takehiro; Kitagaki, Toru; Onuki, Toshihiko; Kozai, Naofumi

Journal of Radioanalytical and Nuclear Chemistry, 331(6), p.2785 - 2794, 2022/06

 Times Cited Count:4 Percentile:63.92(Chemistry, Analytical)

Remnant nuclear fuel debris in the damaged nuclear reactors at the Fukushima Daiichi Nuclear Power Plant (FDNPP) has contacted the groundwater containing microorganisms for over ten years. Herein, we report the possibility of bacterial alteration of fuel debris. We investigated the physical and chemical changes of fuel debris simulants (FDS) in the powder and pellet forms via exposure to two ubiquitous bacteria, Pseudomonas fluorescens and Bacillus subtilis. In the experiments using FDS composed of the powders of Fe(0), solid solution of CeO$$_{2}$$ and ZrO$$_{2}$$, and SiO$$_{2}$$, Ce, Zr, and Si were hardly dissolved, while Fe was dissolved, a fraction of the dissolved Fe was present in the liquid phase as Fe(II) and Fe(III), and the rest was precipitated as the nano-sized particles of iron (hydr)oxides. In the experiment using P. fluorescens and FDS pellet pieces prepared by melting the Fe(0) particles and solid solution of CeO$$_{2}$$ and ZrO$$_{2}$$, the bacteria selectively gathered on the Fe(0) particle surface and made corrosion pits. These results suggest that bacteria in groundwater corrode the iron in fuel debris at FDNPP, change fuel debris into porous one, releasing the nano-sized iron (hydr)oxide particles into the water.

Journal Articles

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

 Times Cited Count:1 Percentile:8.33(Materials Science, Multidisciplinary)

Journal Articles

The Kinetics and mechanism of H$$_{2}$$O$$_{2}$$ decomposition at the U$$_{3}$$O$$_{8}$$ surface in bicarbonate solution

McGrady, J.; Kumagai, Yuta; Watanabe, Masayuki; Kirishima, Akira*; Akiyama, Daisuke*; Kitamura, Akira; Kimuro, Shingo

RSC Advances (Internet), 11(46), p.28940 - 28948, 2021/08

 Times Cited Count:5 Percentile:30.58(Chemistry, Multidisciplinary)

JAEA Reports

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.

Journal Articles

Thorium oxide dissolution in HNO$$_{3}$$-HF mixture; Kinetics and mechanism

Simonnet, M.; Barr$'e$, N.*; Drot, R.*; Le Naour, C.*; Sladkov, V.*; Delpech, S.*

Radiochimica Acta, 107(4), p.289 - 297, 2019/04

 Times Cited Count:3 Percentile:28.63(Chemistry, Inorganic & Nuclear)

Journal Articles

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

 Times Cited Count:19 Percentile:66.31(Materials Science, Multidisciplinary)

Journal Articles

Effects of OH$$^{-}$$ activity and temperature on the dissolution rate of compacted montmorillonite under highly alkaline conditions

Sawaguchi, Takuma; Tsukada, Manabu; Yamaguchi, Tetsuji; Mukai, Masayuki

Clay Minerals, 51(2), p.267 - 278, 2016/05

 Times Cited Count:7 Percentile:22.82(Chemistry, Physical)

The dependences of the dissolution rate of compacted montmorillonite on activity of OH$$^{-}$$ (a$$_{rm OH}$$-) and temperature (T) were investigated. The dissolution rate of montmorillonite ($$R_{rm A}$$) in compacted pure montmorillonite, which was formulized as $$R_{rm A}$$ = 10$$^{4.5}$$ (a$$_{rm OH}$$-)$$^{1.3}$$ e$$^{-55000/RT}$$, was higher than that in the compacted sand-bentonite mixtures: $$R_{rm A}$$ = 3500 (a$$_{rm OH}$$-)$$^{1.4}$$ e$$^{-51000/RT}$$. The difference can be explained by considering the decrease in a$$_{rm OH}$$- in the mixtures accompanied by dissolution of accessory minerals such as quartz and chalcedony. The dissolution rate model developed for pure montmorillonite is expected to be applied to bentonite mixtures if quantification of the decrease in a$$_{rm OH}$$- is achieved somehow.

Journal Articles

Effects of $$alpha$$-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

 Times Cited Count:2 Percentile:7.29(Nuclear Science & Technology)

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 $$alpha$$-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.

Journal Articles

Effects of $$alpha$$-radiation on a direct disposal system for spent nuclear fuel, 1 Review of research into the effects of $$alpha$$-radiation on the spent nuclear fuel, canisters and outside canisters

Kitamura, Akira; Takase, Hiroyasu*

Journal of Nuclear Science and Technology, 53(1), p.1 - 18, 2016/01

 Times Cited Count:4 Percentile:16.67(Nuclear Science & Technology)

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. Focusing especially on the effects of $$alpha$$-radiation in safety assessment, this study has reviewed research into the effects of $$alpha$$-radiation on the spent nuclear fuel, canisters and outside canisters.

Journal Articles

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

 Times Cited Count:44 Percentile:72.77(Geosciences, Multidisciplinary)

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.

Journal Articles

Rapid dissolution techniques with microwave heating devices for solidified products made from non-metallic wastes by plasma melting

Haraga, Tomoko; Kameo, Yutaka; Nakashima, Mikio

Bunseki Kagaku, 55(1), p.51 - 54, 2006/01

 Times Cited Count:4 Percentile:14.28(Chemistry, Analytical)

A relatively large quantity of sample solutions have to be prepared for radiochemical analysis of solidified products yielded by plasma melting treatment of non-metallic radioactive wastes. In order to dissolve the solidified products sample rapidly, dissolution method with microwave heating devices was applied. In a conventional method only by external heating with various mixtures of acids (HNO$$_{3}$$, HF, HClO$$_{4}$$ and H$$_{2}$$SO$$_{4}$$), a 0.1 g amount of the sample was dissolved with difficulty. However, applying the microwave assisted dissolution method, a 1 g amount of the sample was completely dissolved in a shorter time. Thereby the time for dissolution procedures was shortened less than a one-tenth. The present dissolution method was successfully applied to the blast furnace slag as a reference material to determine main elements with good precision.

Journal Articles

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

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 $$pm$$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.

Journal Articles

Comparison of the corrosion behavior of austenitic and ferritic/martensitic steels exposed to static liquid Pb-Bi at 450 and 550 $$^{circ}$$C

Kurata, Yuji; Futakawa, Masatoshi; Saito, Shigeru

Journal of Nuclear Materials, 343(1-3), p.333 - 340, 2005/08

 Times Cited Count:78 Percentile:97.56(Materials Science, Multidisciplinary)

In order to study effects of temperature and alloying elements on corrosion behavior in liquid Pb-Bi which will be used for an accelerator driven system (ADS), corrosion tests of various steels were conducted under static liquid Pb-Bi condition. The tests were performed in oxygen-saturated liquid Pb-Bi at 450$$^{circ}$$C and 550$$^{circ}$$C for 3000h. Oxide films were formed during corrosion at 450$$^{circ}$$C and 550$$^{circ}$$C. Corrosion depth of steels decreased at 450$$^{circ}$$C with increasing Cr content of steels. Austenitic stainless steels containing Ni didn't exhibit appreciable dissolution of Ni and Cr at 450$$^{circ}$$C. The thick ferrite layer produced by dissolution of Ni and Cr was found in JPCA and type 316ss at 550$$^{circ}$$C. For this reason the corrosion depth of austenitic stainless steels, JPCA and type 316ss became large. A Si-added austenitic stainless steel showed good corrosion resistance at 550$$^{circ}$$C because a protective oxide film formed on the steel prevented dissolution of Ni and Cr into liquid Pb-Bi.

JAEA Reports

Report on the fuel treatment facility operation

Kokusen, Junya; Seki, Masakazu; Abe, Masayuki; Nakazaki, Masato; Kida, Takashi; Umeda, Miki; Kihara, Takehiro; Sugikawa, Susumu

JAERI-Tech 2005-004, 53 Pages, 2005/03

JAERI-Tech-2005-004.pdf:5.92MB

This report presents operating records of dissolution of uranium dioxide and concentration of uranyl nitrate solution and acid removal, which have been performed from 1994 through 2003, for the purpose of feeding 10% and 6% enriched uranyl nitrate solution fuel to Static Experimental Critical Facility(STACY) and Transient Experimental Critical Facility(TRACY) in Nuclear Fuel Safety Engineering Facility(NUCEF).

Journal Articles

Electrochemical behaviors of PuN and (U, Pu)N in LiCl-KCl eutectic melts

Shirai, Osamu; Kato, Tetsuya*; Iwai, Takashi; Arai, Yasuo; Yamashita, Toshiyuki

Journal of Physics and Chemistry of Solids, 66(2-4), p.456 - 460, 2005/02

 Times Cited Count:8 Percentile:36.48(Chemistry, Multidisciplinary)

Electrochemical behaviors of PuN and (U, Pu)N in the LiCl-KCl eutectic melt containing UCl$$_{3}$$ and PuCl$$_{3}$$ at 773 K were investigated by cyclic voltammetry. The electrochemical dissolution of PuN and (U, Pu)N began nearly at -1.0 V vs. the Ag/AgCl reference electrode. The rest potentials of PuN and (U, Pu)N were observed at about 0.15 V more negative potential than that of UN since the equilibrium potential of UN is about 0.15 V more positive than that of PuN. In the cyclic voltammogram measured by using (U, Pu)N as the working electrode, a steep rise of the positive current was observed at more positive potential than -0.4 V in analogy with the cyclic voltammogram measured by using UN as the working electrode. In addition, there were two anodic current waves in the voltammogram with (U, Pu)N, though the wave form was not clear. This indicates that UN and PuN would be dissolved independently irrespective of formation of the solid solution, (U, Pu)N.

Journal Articles

An Investigation into dissolution rate of spent nuclear fuel in aqueous reprocessing

Mineo, Hideaki; Isogai, Hikaru; Morita, Yasuji; Uchiyama, Gunzo*

Journal of Nuclear Science and Technology, 41(2), p.126 - 134, 2004/02

 Times Cited Count:7 Percentile:44.60(Nuclear Science & Technology)

A simple equation was proposed for the dissolution rate of spent LWR fuel, of which the change in the dissolution area was estimated by taking into account of the area of the cracks occurring due to thermal shrinkage of the pellets during irradiation. The applicability of proposed equation was examined using LWR fuel dissolution test results in the present study as well as the results obtained by other workers. The equation showed good agreements with the dissolution test results obtained from spent fuel pellets and pulverized spent fuel. It was indicated that the proposed equation was simple and would be useful for the prediction of dissolution of spent LWR fuels. However, the initial effective dissolution area, the parameter of the equation, was found to depend on the temperature, which could not be explained by the proposed equation. Further studies on the role of other factors affecting dissolution rate, such as nitrous acid, in the dissolution of spent fuel was required.

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