Current location of fuel debris chemistry

Sato, Nobuaki*; Kirishima, Akira*; Sasaki, Takayuki*; Takano, Masahide; Kumagai, Yuta; Sato, Soichi; Tanaka, Kosuke

Current Location of Fuel Debris Chemistry, 178 Pages, 2023/11

Considerable efforts have been devoted to the decommissioning of the TEPCO's Fukushima Daiichi Nuclear Power Station (1F) and now the retrieval of fuel debris is being proceeded on a trial basis. It can be said that the succession of science and technology related to debris, that is, human resource development, is important and indispensable. For that reason, we thought that a specific textbook on decommissioning is necessary. Regarding the 1F fuel debris, we still do not know enough, and it would be difficult to describe the details. However, 12 years have passed since the accident, and we have come to understand the situation of 1F to a certain extent. At this stage, it is essential for future development to organize the current situation by combining examples of past severe accidents. Therefore, we presented in this book the current state of fuel debris chemistry research from the perspectives of solid chemistry, solution chemistry, analytical chemistry, radiochemistry, and radiation chemistry.

Phase analysis of simulated nuclear fuel debris synthesized using UO, Zr, and stainless steel and leaching behavior of the fission products and matrix elements

Tonna, Ryutaro*; Sasaki, Takayuki*; Kodama, Yuji*; Kobayashi, Taishi*; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Kumagai, Yuta; Kusaka, Ryoji; Watanabe, Masayuki

Nuclear Engineering and Technology, 55(4), p.1300 - 1309, 2023/04

https://doi.org/10.1016/j.net.2022.12.017

Simulated debris was synthesized using UO, Zr, and stainless steel and a heat treatment method under inert or oxidizing conditions. The primary U solid phase of the debris synthesized at 1473 K under inert conditions was UO, whereas a (U,Zr)O solid solution formed at 1873 K. Under oxidizing conditions, a mixture of UO and (Fe,Cr)UO phases formed at 1473 K whereas a (U,Zr)O solid solution formed at 1873 K. The leaching behavior of the fission products from the simulated debris was evaluated using two methods: the irradiation method, for which fission products were produced via neutron irradiation, and the doping method, for which trace amounts of non-radioactive elements were doped into the debris. The dissolution behavior of U depended on the properties of the debris and aqueous medium the debris was immersed in. Cs, Sr, and Ba leached out regardless of the primary solid phases. The leaching of high-valence Eu and Ru ions was suppressed, possibly owing to their solid-solution reaction with or incorporation into the uranium compounds of the simulated debris.

Structure, stability, and actinide leaching of simulated nuclear fuel debris synthesized from UO, Zr, and stainless-steel

Kirishima, Akira*; Akiyama, Daisuke*; Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Sasaki, Takayuki*; Sato, Nobuaki*

Journal of Nuclear Materials, 567, p.153842_1 - 153842_15, 2022/08

https://doi.org/10.1016/j.jnucmat.2022.153842

To understand the chemical structure and stability of nuclear fuel debris consisting of UO, Zr, and Stainless Steel (SUS) generated by the Fukushima Daiichi Nuclear Power Plant accident in Japan in 2011, simulated debris of the UO-SUS-Zr system and other fundamental component systems were synthesized and characterized. The simulated debris were synthesized by heat treatment for 1 to 12 h at 1600C, in inert (Ar) or oxidative (Ar + 2% O) atmospheres. Np and Am tracers were doped for the leaching tests of these elements and U from the simulated debris. The characterization of the simulated debris was conducted by XRD, SEM-EDX, Raman spectroscopy, and Mssbauer spectroscopy, which provided the major uranium phase of the UO -SUS-Zr debris was the solid solution of UO (s.s.) with Zr(IV) and Fe(II) regardless of the treatment atmosphere. The long-term immersion test of the simulated debris in pure water and that in seawater revealed the macro scale crystal structure of the simulated debris was chemically very stable in the wet condition for a year or more. Furthermore, the leaching test results showed that the actinide leaching ratios of U, Np, Am from the UO-SUS-Zr debris were very limited and less than 0.08 % for all the experiments in this study.

A Study of HO-induced oxidative degradation of simulated fuel debris

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Hoshasen Kagaku (Internet), (113), p.61 - 64, 2022/04

The severe accident at TEPCO's Fukushima Daiichi Nuclear Power Station resulted in generation of fuel debris. The fuel debris is in contact with water and the radiolysis of water can accelerate degradation of the debris. The analysis of particles sampled from inside or near the damaged reactors indicates the complicated compositions of the fuel debris. It is challenging to estimate the effect of water radiolysis on such a complicated material. Therefore, in this study, we investigated the potential degradation process by leaching experiments of simulated fuel debris in aqueous HO solution. The results show that the reaction of HO induced uranium dissolution from most of the samples and then formation of uranyl peroxides. In contrast, a sample that had U-Zr oxide solid solution as the major phase exhibited remarkable resistance to HO. These findings revealed that the degradation of the simulated debris reflects the reactivity and stability of the uranium phase in the matrices.

Speciation on the reaction of uranium and zirconium oxides treated under oxidizing and reducing atmospheres

Uehara, Akihiro*; Akiyama, Daisuke*; Ikeda, Atsushi; Numako, Chiya*; Terada, Yasuko*; Nitta, Kiyofumi*; Ina, Toshiaki*; Takeda-Homma, Shino*; Kirishima, Akira*; Sato, Nobuaki*

Journal of Nuclear Materials, 559, p.153422_1 - 153422_11, 2022/02

https://doi.org/10.1016/j.jnucmat.2021.153422

Distribution of studtite and metastudtite generated on the surface of UO; Application of Raman imaging technique to uranium compound

Kusaka, Ryoji; Kumagai, Yuta; Yomogida, Takumi; Takano, Masahide; Watanabe, Masayuki; Sasaki, Takayuki*; Akiyama, Daisuke*; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Science and Technology, 58(6), p.629 - 634, 2021/06

https://doi.org/10.1080/00223131.2020.1854881

Investigation of chemical state of uranium included in simulated waste glass

Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro

2019-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), P. 20191107_1, 2020/11

no abstracts in English

Structural change of borosilicate glass by neutron irradiation

Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*; Uehara, Akihiro*; Fujii, Toshiyuki*; Sekimoto, Shun*

KURNS Progress Report 2018, P. 105, 2019/08

https://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2018/KURNS_Progress_Report2018_web.pdf

To understand this structural change of a borosilicate glass by a neutron irradiation in detail, the irradiation test was carried out in KUR in 2017FY. The glass structure was estimated by using Raman spectrometry in 2018FY. Comparing with the Raman spectra of glass samples before and after irradiation, it could be observed the change of peak height of Si-O bridging structure by the irradiation.

Thermodynamic study of the complexation of humic acid by calorimetry

Kimuro, Shingo; Kirishima, Akira*; Kitatsuji, Yoshihiro; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Chemical Thermodynamics, 132, p.352 - 362, 2019/05

https://doi.org/10.1016/j.jct.2019.01.011

A combination of potentiometry and calorimetry was used for the determination of the thermodynamic quantities of complexation of generic and groundwater humic acid (HA), which was isolated from deep groundwater at Horonobe, Hokkaido, Japan, with copper (II) ions and uranyl (VI) ions. The apparent complexation constant of Horonobe HA was independent of the pH, whereas that of generic HA was dependent on the pH. This observation indicates that the polyelectrolyte effect of Horonobe HA is negligible because of its small molecular size. In addition, the effect of the heterogeneity of Horonobe HA was not significant. Moreover, the complexation enthalpy of Horonobe HA was consistent with that of homogeneous poly(acrylic acid), which means the complexation of Horonobe HA was not affected by the functional group heterogeneity. Consequently, the characteristic complexation mechanism of Horonobe HA was revealed based on the determined thermodynamic quantities.

Characterization and thermodynamic study of humic acid in deep groundwater at Horonobe, Hokkaido, Japan

Kimuro, Shingo*; Kirishima, Akira*; Nagao, Seiya*; Saito, Takumi*; Amano, Yuki; Miyakawa, Kazuya; Akiyama, Daisuke*; Sato, Nobuaki*

Journal of Nuclear Science and Technology, 55(5), p.503 - 515, 2018/05

https://doi.org/10.1080/00223131.2017.1416690

no abstracts in English