Investigation of sorption behavior of Cs in a river-sea system boundary area after the Fukushima Dai-ichi Nuclear Power Plant accident

Takata, Hyoe*; Wakiyama, Yoshifumi*; Wada, Toshihiro*; Hirao, Shigekazu*; Aono, Tatsuo*; Nakanishi, Takahiro; Misono, Toshiharu; Shiribiki, Takehiko; Aoyama, Michio*

Marine Chemistry, 262, p.104384_1 - 104384_6, 2024/05

https://doi.org/10.1016/j.marchem.2024.104384

Synchrotron analysis of coagulated surface of simulated waste glasses

Nagai, Takayuki; Katsuoka, Nanako; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*

Photon Factory Activity Report 2023 (Internet), 3 Pages, 2024/00

https://pfwww.kek.jp/acr/2023pdf/u_reports/pf23b0063.pdf

no abstracts in English

Annual report for FY2021 on the activities of Naraha Center for Remote Control Technology Development (April 1, 2021 - March 31, 2022)

Akiyama, Yoichi; Shibanuma, So; Yanagisawa, Kenichi*; Yamada, Taichi; Suzuki, Kenta; Yoshida, Moeka; Ono, Takahiro; Kawabata, Kuniaki; Watanabe, Kaho; Morimoto, Kyoichi; et al.

JAEA-Review 2023-015, 60 Pages, 2023/09

JAEA-Review-2023-015.pdf:4.78MB

Naraha Center for Remote Control Technology Development (NARREC) was established in Japan Atomic Energy Agency to promote a decommissioning work of Fukushima Daiichi Nuclear Power Station (Fukushima Daiichi NPS). NARREC consists of a Full-scale Mock-up Test Building and Research Management Building. Various test facilities are installed in these buildings for the decommissioning work of Fukushima Daiichi NPS. These test facilities are intended to be used for various users, such as companies engaged in the decommissioning work, research and development institutions, educational institutions and so on. The number of NARREC facility uses was 84 in FY2021. We participated booth exhibitions and presentations on the decommissioning related events. Moreover, we also contributed to the development of human resources by supporting the 6th Creative Robot Contest for Decommissioning. As a new project, "Narahakko Children's Classroom" was implemented for elementary school students in Naraha Town. This report summarizes the activities of NARREC in FY2021, such as the utilization of facilities and equipment of NARREC, the development of remote-control technologies for supporting the decommissioning work, arrangement of the remote-control machines for emergency response, and training for operators by using the machines.

UO dissolution in bicarbonate solution with HO; 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

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.

Dry synthesis of brannerite (UTiO) by mechanochemical treatment

Akiyama, Daisuke*; Mishima, Tomoki*; Okamoto, Yoshihiro; Kirishima, Akira*

High Temperature Materials and Processes, 42(1), p.20220268_1 - 20220268_9, 2023/04

https://www.degruyter.com/document/doi/10.1515/htmp-2022-0268/html

A powder mixture of UO and TiO was mechanochemically treated in a planetary ball mill under Ar atmosphere for 1 h using a tungsten carbide vial and balls as the milling medium. Such mechanochemical (MC) treatment reduced the crystallinity of UO and TiO. The mechanochemically treated powder mixture was heated at 973-1573K for 6 h under Ar atmosphere and analyzed by X-ray diffraction analysis, scanning electron microscopy-energy-dispersive X-ray spectroscopy, and X-ray absorption fine structure analysis. UTiO did not form below 1373K without MC treatment and only the starting materials were observed. At 1473 and 1573K, a small amount of UTiO and equal amounts of UTiO and UO were formed, respectively. The mechanochemically treated sample produced nearly pure UTiO containing small amounts of UO impurities when heated above 1173K for 6 h. UTiO was highly crystalline and uniform regardless of the synthesis temperature.

Synchrotron analysis of simulated waste glasses different in boron isotope ingredient

Nagai, Takayuki; Tone, Masaya; Katsuoka, Nanako; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*

Photon Factory Activity Report 2022 (Internet), 3 Pages, 2023/00

https://pfwww.kek.jp/acr/2022pdf/u_reports/pf22b0056.pdf

no abstracts in English

Study on the relation between the crystal structure and thermal stability of FeUO and CrUO

Akiyama, 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

https://doi.org/10.1016/j.jnucmat.2022.153847

FeUO, CrUO, and FeCrUO 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. Mssbauer 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.

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.

Deep groundwater physicochemical components affecting actinide migration

Kirishima, Akira*; Terasaki, Mariko*; Miyakawa, Kazuya; Okamoto, Yoshihiro; Akiyama, Daisuke*

Chemosphere, 289, p.133181_1 - 133181_12, 2022/04

https://doi.org/10.1016/j.chemosphere.2021.133181

no abstracts in English

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.