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Journal Articles

Durability of U-Zr oxide solid solution in aqueous HO solution

Kumagai, Yuta; Kusaka, Ryoji; Takano, Masahide; Watanabe, Masayuki

Journal of Nuclear Materials, 625, p.156553_1 - 156553_7, 2026/04

https://doi.org/10.1016/j.jnucmat.2026.156553

Times Cited Count：0 Percentile：0.00(Materials Science, Multidisciplinary)

Uranium-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.

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

https://doi.org/10.1039/D2RA08131H

Times Cited Count：4 Percentile：24.13(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 $_{3}$ $^{-}$ ] 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

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

https://doi.org/10.1039/D1RA05580A

Times Cited Count：7 Percentile：27.58(Chemistry, Multidisciplinary)

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).

JAEA Reports

Present status of chemical analysis of uranyl nitrate solution used for the criticality experiments in NUCEF

Haga, Takahisa*; Gunji, Kazuhiko; Fukaya, Hiroyuki; Sonoda, Takashi; Sakazume, Yoshinori; Sakai, Yutaka; Niitsuma, Yasushi; Togashi, Yoshihiro; Miyauchi, Masakatsu; Sato, Takeshi; et al.

JAERI-Tech 2004-005, 54 Pages, 2004/02

JAERI-Tech-2004-005.pdf:2.06MB

Criticality experiments using uranyl nitrate solution fuel are being conducted at STACY (the Static Experiment Critical Facility) and TRACY (the Transient Experiment Critical Facility) in NUCEF (the Nuclear Fuel Cycle Safety Engineering Research Facility). Chemical analyses of the solution have been carried out to take necessary data for criticality experiments, for treatment and control of the fuel, and for safeguards purpose at the analytical laboratory placed in NUCEF. About 300 samples are analyzed annually that provide various kinds of data, such as uranium concentration, isolation acid concentration, uranium isotopic composition, concentration of fission product (FP) nuclides, tri-butyl phosphoric acid (TBP) concentration, impurities in the solution fuel and so on. This report summarizes the analytical methods and quality management of the analysis for uranyl nitrate solution relating to the criticality experiments.

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

https://doi.org/10.3327/jnst.41.126

Times Cited Count：8 Percentile：47.00(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.

Journal Articles

Reactivity effect measurement of neutron interaction between two slab cores containing 10% enriched uranyl nitrate solution without neutron isolater

Tonoike, Kotaro; Miyoshi, Yoshinori; Okubo, Kiyoshi

Journal of Nuclear Science and Technology, 40(4), p.238 - 245, 2003/04

https://doi.org/10.3327/jnst.40.238

Times Cited Count：2 Percentile：18.08(Nuclear Science & Technology)

The reactivity effect of neutron interaction between two identical units containing low enriched (10% $^{235}$ enrichment) uranyl nitrate solution was measured in the STACY. The unit has 350mm of thickness and 690mm of width and distance between those two units was adjustable from 0mm to 1450mm. Condition of the solution was about 290gU/L in uranium concentration, about 0.8N in free nitric acid molarity, 2427 $^{circ}$ C in temperature and about 1.4g/cm $^{3}$ in solution density. The reactivity effect was estimated from variation of critical solution level from 495mm to 763mm depending on the core distance. The reactivity effect was also evaluated by the solid angle method and a computational method using the continuous energy Monte Carlo code MCNP-4C and the nuclear data library JENDL3.2. Comparison of those estimations is presented.

Journal Articles

Behavior of simulated spent fuel in subcritical water

Mineo, Hideaki; Suzuki, Tadashi; Morita, Yasuji

Proceedings of 2nd International Symposium on Supercritical Fluid Technology for Energy and Environment Applications (Super Green 2003), p.334 - 338, 2003/00

Behavior of spent nuclear fuel in subcritical water was investigated to look at the feasibility of fission-products (FPs) separation without organic solvent. The study employed unirradiated UO $_{2}$ particles simulating spent fuel burned up to 45,000MWdt $^{-1}$ , which includes FP elements in oxide form: Sr, Zr, Mo, Ru, Rh, Pd, Ag, Ba, La, Ce, Pr, Nd and Sm. Also, alloy particles consisted of Mo, Ru, Rh and Pd were prepared to simulate the metallic phase of FP. 12.728 g of the fuel and 52 mg of the alloy were placed in a 10 ml pressure vessel, where subcritical water was fed. The temperature was 523, 573, 623 and 663K, while the pressure was kept at 29MPa. Dissolved fraction decreased with elevating temperature. It was found that more than 5% of Ba, Mo and Pr were respectively dissolved. The dissolved fraction of Sr and Rh were about 1%, and about 0.3% for Zr. La, Ce, Nd and Sm, indicated almost the same result as U, which was about 0.1%. It was suggested that the subcritical water could separate portion of FP. Further study would be carried out with smaller-sized fuel.

Journal Articles

Kinetic parameter $beta_{rm eff}/ell$ measurement on low enriched uranyl nitrate solution with single unit cores (600, 280T, 800) of STACY

Tonoike, Kotaro; Miyoshi, Yoshinori; Kikuchi, Tsukasa*; Yamamoto, Toshihiro

Journal of Nuclear Science and Technology, 39(11), p.1227 - 1236, 2002/11

https://doi.org/10.3327/jnst.39.1227

Times Cited Count：22 Percentile：77.07(Nuclear Science & Technology)

Kinetic parameter $beta_{rm eff}/ell$ of low enriched uranyl nitrate solution was measured by the pulsed neutron source method in the STACY. This measurement was repeated systematically over several uranium concentrations from 193.7 gU/ to 432.1 gU/. Used core tanks were two cylindrical tanks whose diameters are 600 mm and 800 mm and one slab tank which has 280 mm thickness and 700 mm width. In this report, experimental data such as solution conditions, critical solution level for each solution condition, subcritical solution levels where measurements were conducted, measured decay time constants of prompt neutron and extrapolated $beta_{rm eff}/ell$ values are described as well as basic principle of the pulsed neutron source method. $beta_{rm eff}/ell$ values were evaluated also by computation with the diffusion code CITATION in SRAC and the nuclear data library JENDL 3.2. Both experimental and computational $beta_{rm eff}/ell$ values show good agreement.

Journal Articles

Nuclear characteristics evaluation for a supercritical experiment facility using low-enriched uranium solution fuel, TRACY

Nakajima, Ken

Proceedings of International Conference on the New Frontiers of Nuclear Technology; Reactor Physics, Safety and High-Performance Computing (PHYSOR 2002) (CD-ROM), 8 Pages, 2002/10

The nuclear characteristics of TRACY, such as the criticality, the $_{eff}$ / ratio, the peak power, the energy of pulse, and the total energy, have been evaluated using the experimental data. TRACY is a supercritical reactor fueled with low-enriched uranyl nitrate aqueous solution to simulate criticality accidents in a fuel processing facility, such as a spent-fuel reprocessing plant. In this evaluation, the availability of criticality calculation and the models to evaluate the power and energy have been studied.