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O solutionKumagai, Yuta; Kusaka, Ryoji; Takano, Masahide; Watanabe, Masayuki
Journal of Nuclear Materials, 625, p.156553_1 - 156553_7, 2026/04
Times Cited Count：0 Percentile：0.00Uranium-zirconium oxide solid solution, (U, Zr)O, is a representative matrix phase found in fuel debris formed during severe nuclear reactor accidents. Understanding its chemical behavior in oxidative aqueous environments is important for evaluating the potential release of radionuclides during water contact. In this study, we investigated the reactivity of (U, Zr)O with hydrogen peroxide (HO) in pure water to assess its resistance to oxidative dissolution, because HO is the dominant oxidant produced by water radiolysis. The dissolution behavior of uranium and zirconium was monitored through repeated HO exposure experiments, and the solid phases were characterized using Raman micro-spectroscopy and X-ray diffraction. Kinetic modeling was performed to interpret experimental data. The results showed that uranium dissolution occurred initially but decreased significantly upon repeated HO exposure, while zirconium dissolution proceeded more slowly. Raman analysis revealed only minor surface changes, with limited formation of uranyl peroxide phases. The kinetic simulation reproduced the experimental trends by assuming a small fraction of redox-active surface sites. These findings suggest that the observed durability of (U, Zr)O against HO-induced oxidative dissolution is not due to the formation of a protective surface layer, but rather reflects the limited redox reactivity of most of the surface. This study provides a quantitative basis for understanding the HO-induced oxidation of (U, Zr)O in water, relevant to the long-term behavior of fuel debris.
Toigawa, Tomohiro; Hotoku, Shinobu; Kumagai, Yuta; Abe, Yuma*; Oyama, Kanichi*; Fukaya, Hiroyuki; Ban, Yasutoshi; Kida, Takashi; Hasegawa, Satoshi*; Nakano, Masanao*; et al.
Journal of Nuclear Science and Technology, 63(3), p.322 - 327, 2026/03
Times Cited Count：0 Percentile：0.00(Nuclear Science & Technology)The effect of temperature on hydrogen production generated from radiolysis was investigated to determine the associated implications for nuclear fuel reprocessing safety. The hydrogen yield from radiolysis of plutonium nitric acid solution was measured at temperatures up to the boiling temperature of the solution. The results showed no notable temperature dependence even under boiling conditions. The impact of solution agitation on hydrogen production was also assessed, which revealed minor differences in the hydrogen yield between static and agitated conditions at room temperature. These findings suggest that high temperatures or boiling the solution do not considerably enhance hydrogen generation, and provide crucial information for accurately modeling hydrogen risks under severe accidents.
Kawaguchi, Munemichi*; Ikeda, Asuka; Saito, Junichi
Annals of Nuclear Energy, 226, p.111880_1 - 111880_9, 2026/02
Times Cited Count：0 Percentile：0.00(Nuclear Science & Technology)Soma, Yasutaka; Komatsu, Atsushi; Igarashi, Takahiro
Corrosion Science, 128, 29 Pages, 2026/00
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.
Irisawa, Eriko; Kato, Chiaki
Corrosion Science, 256, p.113173_1 - 113173_16, 2025/11
Times Cited Count：4 Percentile：81.08(Materials Science, Multidisciplinary)Jing, Z.*; Yamaguchi, Toshio*; Machida, Shinichi*; Hattori, Takanori; Zhou, Y.*
Journal of Chemical Physics, 163(19), p.194505_1 - 194505_12, 2025/11
Times Cited Count：0 Percentile：0.00(Chemistry, Physical)Ion solvation in a range of gigapascal pressure is of great significance for high-pressure chemical synthesis and the circulation of matter within the Earth's interior. We perform neutron scattering (NS) experiments and molecular dynamics simulations of deuterated aqueous solutions of MCl (M = Li, Na, K, Rb, and Cs) at 0.1 MPa and 0.7 GPa/298 K. An empirical potential structure refinement method analyzes the NS data. Upon compression to 0.7 GPa, the outer-shell water molecules enter the nearest neighbor of ions, and the solvated ion clusters become denser. The hydration factor 
and static hydration number 
based on the orientation distribution of the water dipole in the first solvation shell, show that the compression weakens the hydration ability of the ions. Compression suppresses the diffusion of ions, particularly of the structure-breaking ions. The ionic diffusion coefficient 
residence time of water molecules 
and dynamic hydration number 
indicate that Rb
and Cs exhibit characteristics of structure-making ions under compression. The dynamic properties are more pressure-sensitive than the static structure.
Ito, Tatsuya; Nagaishi, Ryuji; Kuwano, Ryo*; Gohdo, Masao*; Yoshida, Yoichi*
Radiation Physics and Chemistry, 226, p.112198_1 - 112198_5, 2025/01
Times Cited Count：0 Percentile：0.00(Chemistry, Physical)In recent years, the use of radiation-resistant resins of polyimide and polyether ether ketone becomes increasing as vessels for irradiation and unsealed radioisotope experiments. However, in our radiolysis experiments, the possibility of interaction between radiolysis products of water and the resin was found, suggesting concerns that the resin may affect reactions in water in radiation fields. To clarify the interaction, dichromate (CrO
) reduction and hydrogen peroxide (HO) formation in 
-radiolysis of water were compared with and without the resin. The CrO reduction amount in aqueous solution with the resin became larger than that without the resin at the same dose, indicating the promotion of CrO reduction by the resin. On the other hand, the HO formation in pure water with and without an electron scavenger were almost independent of the presence of resin. These suggested the interaction between hydroxyl radical and the resin in contact with water in radiation fields.
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.
Watanabe, Tomoaki; Yamane, Yuichi
Journal of Nuclear Science and Technology, 61(7), p.958 - 966, 2024/07
Times Cited Count：0 Percentile：0.00(Nuclear Science & Technology)The total fission energy released in a criticality accident involving fissile solution boiling tends to be high because the relatively high fission power continues during boiling. Simulating fission power change correctly during boiling seems essential to estimate the total fission energy. Fission power during boiling changes depending on fissile concentration and volume as the solution evaporates. In this study, we investigated the effect of concentration and volume change on estimated total fission energy for a long time of boiling. We introduced a model calculating the evaporation of fissile solution into the modified quasi-steady-state method to simulate power change during boiling. Three CRAC experiments and the Idaho Chemical Processing Plant (ICPP) criticality accident in 1959 were analyzed. As a result, the calculated energy considering concentration and volume change during boiling reproduced the measured energy well.
Li-glass detector to gamma rays by a coincidence methodIto, Fumiaki*; Lee, J.; Hironaka, Kota; Takahashi, Tone; Suzuki, Satoshi*; Mochimaru, Takanori*; Hori, Junichi*; Terada, Kazushi*; Koizumi, Mitsuo
Nuclear Instruments and Methods in Physics Research A, 1064, p.169465_1 - 169465_9, 2024/07
Times Cited Count：0 Percentile：0.00(Instruments & Instrumentation)Ikeuchi, Hirotomo; Koyama, Shinichi
Nihon Genshiryoku Gakkai-Shi ATOMO
, 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."
Kinoshita, Ryoma; Sasaki, Yuji; Kaneko, Masashi; Matsumiya, Masahiko*; Shinoku, Kota*; Shiroishi, Hidenobu*
Hydrometallurgy, 222, p.106159_1 - 106159_12, 2023/10
Times Cited Count：2 Percentile：13.80(Metallurgy & Metallurgical Engineering)Solvent extraction is conducted using a total of 20 metals revealing high stability constants with Cl and hexahexyl-nitrilotriacetamide (NTAamide(C6)) extractant. The metals used here may behave as anions at high Cl concentrations, and NTAamide(C6), which contains a tertiary N atom, is protonated under acidic conditions. Most of the metal ions in this study display higher distribution ratios (D(M)) from HCl than those from HNO
, and exhibit 1:1 stoichiometries with NTAamide. Following the experimental results, the association constants and distribution coefficients of the group 12 elements are calculated via ion-pair extraction modeling using density functional theory calculations, and the simulations of D yield calculated values with the same trend as that of the measured values.
dissolution in bicarbonate solution with HO; The Effect of temperatureMcGrady, J.; Kumagai, Yuta; Kitatsuji, Yoshihiro; Kirishima, Akira*; Akiyama, Daisuke*; Watanabe, Masayuki
RSC Advances (Internet), 13(40), p.28021 - 28029, 2023/09
Times Cited Count：3 Percentile：19.64(Chemistry, Multidisciplinary)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.
pellet in molten Zr claddingIto, 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)Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*
Separation and Purification Technology, 308, p.122943_1 - 122943_7, 2023/03
Times Cited Count：5 Percentile：19.48(Engineering, Chemical)HNO leaching is used in recycling Pd metal from spent products that primarily contain Ag, and most Pd residues are separated from solutions containing Ag(I). However, a small amount of Pd(II) often remains in these Ag(I) solutions. Therefore, the separation of Pd(II) and Ag(I) in HNO solutions is essential to promote efficient Pd recycling. In this study, the separation of Pd(II) and Ag(I) in HNO solutions was investigated using four N-donor-type adsorbents functionalized with amine (R-Amine), iminodiacetic acid (R-IDA), pyridine (R-Py), or bis-picolylamine (R-BPA). R-Amine, R-IDA, and R-Py selectively adsorbed Pd(II) over Ag(I), Cu(II), Ni(II), and Fe(III) from HNO solutions (0.3-7 M), but R-Amine exhibited a lower Pd adsorption efficiency. In contrast, 
90% of Pd(II), Ag(I), and Cu(II) were adsorbed by R-BPA over the entire range of HNO concentrations. Structural analyses of the adsorbed metal ions using Fourier transform infrared spectroscopy and extended X-ray absorption fine structure spectroscopy revealed the separation mechanisms of the N-donor-type adsorbents. Pd(II) adsorption on R-IDA, R-Py, and R-BPA occurred via Pd(II) coordination of the functional groups (iminodiacetic acid, pyridine, and bis-picolylamine, respectively), whereas that on R-Amine occurred via anion exchange of NO with [Pd(NO)
]. The coordinative adsorption mechanisms resulted in the higher Pd(II) adsorption behaviors of R-IDA, R-Py, and R-BPA. HCl (5.0 M) and thiourea (0.1 M) eluents desorbed 83% of Pd(II) from R-IDA and 95% from R-Py, respectively. R-Py was the most effective Pd(II) adsorbent based on adsorption selectivity and desorption efficiency.
/Fe(0) by bacteriaLiu, 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.
and CrUOAkiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*
Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09
Times Cited Count：7 Percentile：62.74(Materials Science, Multidisciplinary)FeUO, CrUO, and Fe
Cr
UO are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO and CrUO, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm
in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that FeCrUO was composed of a uranyl-like structure in its lattice regardless of its "x"' value. M
ssbauer measurements indicated that the Fe in FeUO and FeCrUO were trivalent. Furthermore, FeCrUO lost its symmetry around Fe
with increasing electron densities around Fe, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO and CrUO. Thermogravimetric measurements for UO, FeUO, and CrUO showed that the temperature at which FeUO decomposed under an oxidizing condition (approximately 800 C) was significantly lower than the temperature at which the decomposition of CrUO started (approximately 1250 C). Based on these results, we concluded that the decomposition of FeUO was triggered by an "in-crystal" redox reaction, i.e., Fe 
U
Fe
U
, which would not occur in the CrUO lattice because Cr could never be reduced under the investigated condition. Finally, the existence of Cr in FexCrUO effectively suppressed the decomposition of the FeCrUO crystal, even at a very low Cr content.
Murayama, Masahiro*; Higashiyama, Toyohiro*; Harazono, Yuki*; Ishii, Hirotake*; Shimoda, Hiroshi*; Okido, Shinobu*; Taruta, Yasuyoshi
IEICE Transactions on Information and Systems, E105-D(6), p.1211 - 1224, 2022/06
Times Cited Count：1 Percentile：9.82(Computer Science, Information Systems)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：41.78(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 and ZrO, and SiO, 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 and ZrO, 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.
