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

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.

Nuclear criticality benchmark analyses on TRIGA-type reactor systems by using continuous-energy Monte Carlo code MVP with JENDL-5

Yanagisawa, Hiroshi; Umeda, Miki; Motome, Yuiko; Murao, Hiroyuki

JAEA-Technology 2022-030, 80 Pages, 2023/02

JAEA-Technology-2022-030.pdf:2.57MB
JAEA-Technology-2022-030(errata).pdf:0.11MB

Nuclear criticality benchmark analyses were carried out for TRIGA-type reactor systems in which uranium-zirconium hydride fuel rods are loaded by using the continuous-energy Monte Carlo code MVP with the evaluated nuclear data library JENDL-5. The analyses cover two sorts of benchmark data, the IEU-COMP-THERM-003 and IEU-COMP-THERM-013 in the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook, and effective neutron multiplication factors, reactivity worths for control rods etc. were calculated by JENDL-5 in comparison with those by the previous version of JENDL. As the results, it was confirmed that the effective neutron multiplication factors obtained by JENDL-5 were 0.4 to 0.6% greater than those by JENDL-4.0, and that there were no significant differences in the calculated reactivity worths by between JENDL-5 and JENDL-4.0. Those results are considered to be helpful for the confirmation of calculation accuracy in the analyses on NSRR control rod worths, which are planned in the future.

Engineering formulation of the irradiation growth behavior of zirconium-based alloys for light water reactors

Kakiuchi, Kazuo; Amaya, Masaki; Udagawa, Yutaka

Journal of Nuclear Materials, 573, p.154110_1 - 154110_7, 2023/01

https://doi.org/10.1016/j.jnucmat.2022.154110

Advanced concepts in TRISO fuel

Minato, Kazuo; Ogawa, Toru

Comprehensive Nuclear Materials, 2nd Edition, Vol.5, p.334 - 360, 2020/08

https://doi.org/10.1016/B978-0-12-803581-8.11688-1

TRISO coated particle fuel has been developed for the high temperature gas-cooled reactors, which consists of microspherical fuel kernel and coating layers of pyrolytic carbon and silicon carbide. To improve the high temperature stability, the resistance to the chemical attack by fission products and the retention of fission products of the TRISO coated particle fuels, several types of advanced fuels were proposed and tested. Coated particle fuels for fast reactors were also proposed and tested. In this paper, fuel designs, fabrications, characterization techniques and fuel performance of these advanced coated particle fuels are systematically described. This is the updated version of the paper having the same title in Comprehensive Nuclear Materials published in 2012.

Study on plutonium burner high temperature gas-cooled reactor in Japan; Introduction scenario, reactor safety and fabrication tests of the 3S-TRISO fuel

Ueta, Shohei; Mizuta, Naoki; Fukaya, Yuji; Goto, Minoru; Tachibana, Yukio; Honda, Masaki*; Saiki, Yohei*; Takahashi, Masashi*; Ohira, Koichi*; Nakano, Masaaki*; et al.

Nuclear Engineering and Design, 357, p.110419_1 - 110419_10, 2020/02

https://doi.org/10.1016/j.nucengdes.2019.110419

The concept of a plutonium (Pu) burner HTGR is proposed to incarnate highly-effective Pu utilization by its inherent safety features. The security and safety fuel (3S-TRISO fuel) employs the coated fuel particle with a fuel kernel made of plutonium dioxide (PuO) and yttria stabilized zirconia (YSZ) as an inert matrix. This paper presents feasibility study of Pu burner HTGR and R&D on the 3S-TRISO fuel.

Update of JAEA-TDB; Update of thermodynamic data for zirconium and those for isosaccahrinate, tentative selection of thermodynamic data for ternary M-UO-CO system and integration with JAEA's thermodynamic database for geochemical calculations

Kitamura, Akira

JAEA-Data/Code 2018-018, 103 Pages, 2019/03

JAEA-Data-Code-2018-018.pdf:5.66MB
JAEA-Data-Code-2018-018-appendix1(DVD-ROM).zip:0.14MB
JAEA-Data-Code-2018-018-appendix2(DVD-ROM).zip:0.15MB
JAEA-Data-Code-2018-018-appendix3(DVD-ROM).zip:0.19MB

The latest available thermodynamic data were critically reviewed and the selected values were included into the JAEA-TDB for performance assessment of geological disposal of high-level radioactive and TRU wastes. This critical review specifically addressed thermodynamic data for (1) a zirconium-hydroxide system through comparison of thermodynamic data selected by the Nuclear Energy Agency within the Organisation for Economic Co-operation and Development (OECD/NEA), (2) complexation of metal ions with isosaccharinic acid based on the latest review papers. Furthermore, the author performed (3) tentative selection of thermodynamic data on ternary complexes among alkaline-earth metal, uranyl and carbonate ions, and (4) integration with the latest version of JAEA's thermodynamic database for geochemical calculations. The internal consistency of the selected data was checked by the author. Text files of the updated and integrated thermodynamic database have been prepared for geochemical calculation programs of PHREEQC and Geochemist's Workbench.

Study on Pu-burner high temperature gas-cooled reactor in Japan; Test and characterization for ZrC coating

Ueta, Shohei; Aihara, Jun; Mizuta, Naoki; Goto, Minoru; Fukaya, Yuji; Tachibana, Yukio; Okamoto, Koji*

Proceedings of 9th International Topical Meeting on High Temperature Reactor Technology (HTR 2018) (USB Flash Drive), 7 Pages, 2018/10

The security and safety fuel (3S-TRISO fuel) employs the coated fuel particle with a fuel kernel made of plutonium dioxide (PuO) and yttria stabilized zirconia (YSZ) as an inert matrix. Especially, a zirconium carbide (ZrC) coating is one of key technologies of the 3S-TRISO, which performs as an oxygen getter to reduce the fuel failure due to internal pressure during the irradiation. R&Ds on ZrC coating directly on the dummy CeO-YSZ kernel have been carried in the Japanese fiscal year 2017. As results of ZrC coating tests by the bromide chemical vapor deposition process, stoichiometric ZrC coatings with 3 - 18 microns of thicknesses were obtained with 0.1 kg of particle loading weight.

Effect of hydrogenation conditions on the microstructure and mechanical properties of zirconium hydride

Muta, Hiroaki*; Nishikane, Ryoji*; Ando, Yusuke*; Matsunaga, Junji*; Sakamoto, Kan*; Harjo, S.; Kawasaki, Takuro; Oishi, Yuji*; Kurosaki, Ken*; Yamanaka, Shinsuke*

Journal of Nuclear Materials, 500, p.145 - 152, 2018/03

https://doi.org/10.1016/j.jnucmat.2017.12.027

Hydrogen absorption behavior on zirconium under -radiolysis of nitric acid solution

Ishijima, Yasuhiro; Ueno, Fumiyoshi; Abe, Hitoshi

Nihon Genshiryoku Gakkai Wabun Rombunshi, 16(2), p.100 - 106, 2017/05

https://doi.org/10.3327/taesj.J16.018

Zirconium (Zr) has been used as a structural material at the spent nuclear fuel reprocessing plant in Japan because of its excellent corrosion resistance against nitric acid solution. And the radiolytic hydrogen is known to be generated in the spent nuclear fuel solution. Zr is known to be highly susceptible to hydrogen embrittlement. Therefore, evaluating the radiolytic hydrogen absorption behavior of Zr in nitric acid solution (HNO) is essential. In this study, immersion tests were conducted on Zr in nitric acid solutions under -ray irradiation to evaluate its radiolytic hydrogen absorption behavior. Results showed that hydrogen concentration on Zr increased both in 1-3 mol/L HNO and pure water at 5 and 7 kGy/h after immersion. The amount of hydrogen absorption on Zr under -ray irradiation had a direct correlation with the radiolytic hydrogen generation value in HNO. The results of glow discharge optical emission spectrometry, thermal desorption spectroscopy, and X-ray diffraction result shows that the absorbed radiolytic hydrogen generated a hydride on the surface of Zr.

The Effect of crystal textures on the anodic oxidization of zirconium in a boiling nitric acid solution

Kato, Chiaki; Ishijima, Yasuhiro; Ueno, Fumiyoshi; Yamamoto, Masahiro

Journal of Nuclear Science and Technology, 53(9), p.1371 - 1379, 2016/09

AA2015-0626.pdf:1.2MB

https://doi.org/10.1080/00223131.2015.1110506

The effects of crystal textures and the potentials in the anodic oxidation of zirconium in a boiling nitric acid solution were investigated to study the stress corrosion cracking of zirconium in nitric acid solutions. The growth of the zirconium oxide film dramatically changed depending on the applied potential at a closed depassivation potential (1.47 V vs. SSE). At 1.5 V, the zirconium oxide film rapidly grows, and its growth exhibits cyclic oxidation kinetics in accordance with a nearly cubic rate law. The zirconium oxide film grows according to the quantity of electric charge, and the growth rate does not depend on the crystal texture in the pretransition region before the cyclic oxidation kinetics. However, the growth and cracking under the thick oxide film depend on the crystal texture in the transition region. On the normal direction side, the oxide film thickness decreases on average since some areas of the thick oxide film are separated from the specimen surface owing to the cracks in the thick oxide. On the rolling direction side, cracks are found under the thick oxide film, which deeply propagate along the RD without an external stress. The cracks under the thick oxide film propagate to the center of the oxide layer. The cracks in the oxide layer propagate in the (0002)Zr plane in the zirconium matrix. The oxide layer consists of string-like zirconium oxide and zirconium hydride. The string-like zirconium oxide contains orthorhombic ZrO in addition to monoclinic ZrO. As one assumption for the mechanism of crack initiation and propagation without an external stress, it is considered that the oxidizing zirconium hydrides precipitate in the (0002)Zr and then the phase transformation from orthorhombic ZrO to monoclinic ZrO in the oxide layer causes the crack propagation in the (0002) plane.