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.

Study on the basic core analysis of the new STACY

Gunji, Satoshi; Yoshikawa, Tomoki; Araki, Shohei; Izawa, Kazuhiko; Suyama, Kenya

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 8 Pages, 2023/10

Since the compositions and properties of the fuel debris are uncertain, critical experiments are required to validate calculation codes and nuclear data used for the safety evaluation. For this purpose, JAEA has been modifying a critical assembly called "STACY". The first criticality of the new STACY is scheduled for spring 2024. This paper reports the consideration results of the core configurations of the new STACY at the first criticality. We prepared two sets of gird plates with different neutron moderation conditions (their intervals are 1.50 cm and 1.27 cm). However, there is a limitation on the number of available UO fuel rods. In addition, we would like to set the critical water heights for the first criticality at around 95 cm. This is to avoid the reactive effect of the aluminum alloy middle grid plates (Approx. 98 cm high). The core configurations for the first criticality satisfying these conditions were constructed by computational analysis. A square core configuration with the 1.50 cm grid plate that is close to the optimum moderation condition needs 261 fuel rods to reach criticality. As to the 1.27 cm grid plate, we considered two core configurations with 1.80 cm intervals by using a checkerboard arrangement. One of them has two regions core configuration with 1.27 and 1.80 cm intervals, and the other has only 1.80 cm intervals. They need 341 and 201 fuel rods for the criticality, respectively. This paper shows these three core configurations and their calculation models.

Debris-simulated core analysis under fuel procurement constraints in new STACY experiments

Araki, Shohei; Gunji, Satoshi; Arakaki, Yu; Yoshikawa, Tomoki; Murakami, Takahiko; Kobayashi, Fuyumi; Izawa, Kazuhiko; Suyama, Kenya

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 8 Pages, 2023/10

New experiments simulating fuel debris in the new criticality assembly, STACY, are designed to contribute to the validation of criticality calculations for criticality control of the fuel debris in the Fukushima Daiichi Nuclear Power Plant accident. In the new STACY experiment, a two-region core consisting of a driver region and a test region was investigated in order to configure a debris-simulated core with under-moderation condition (lattice pitch 1.27-cm) having the constraint of available fuel rod number. The test region with a 1.27-cm lattice pitch is surrounded by the driver region, in which fuel rods are arranged in a checkerboard pattern on a 1.27-cm lattice plate, with a 1.80-cm lattice pitch. Neutron spectra and sensitivity were calculated by using MCNP6 and ENDF/B-VII. The core which has a 1717 test region with 373 fuel rods is the largest two-region core under the constraint. It was found that the core which has a 1717 test region can simulate the neutron spectra of under-moderation condition in a 1313 region inside the test region with the root-mean square percentage error of less than 5%. It was also confirmed that the sensitivity of Si and Ca (n,) reactions when the concrete simulant, was loaded could be simulated.

Validation of integrated thermal power measurement using solution fuel STACY experimental data for modified STACY performance test

Araki, Shohei; Gunji, Satoshi; Arakaki, Yu; Murakami, Takahiko; Yoshikawa, Tomoki; Hasegawa, Kenta; Tada, Yuta; Izawa, Kazuhiko; Suyama, Kenya

Proceedings of 4th Reactor Physics Asia Conference (RPHA2023) (Internet), 4 Pages, 2023/10

To conduct integrated thermal power measurements for the performance test of the modified STACY, we re-analyzed the experimental data measured in the solution fuel STACY using the activation method. We validated its feasibility under the limited number of activation detectors. The re-analyzed results of the activation method by using MVP and PHITS with JENDL-4.0 indicated that the effect of the difference of the position between activation detectors was small enough, and the results agreed with that of the fission product analysis within almost 10%. It is conceivable that the activation method could be adopted instead of the fission product analysis.

Raman identification and characterization of chemical components included in simulated nuclear fuel debris synthesized from uranium, stainless steel, and zirconium

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

Journal of Nuclear Science and Technology, 60(5), p.603 - 613, 2023/05

https://doi.org/10.1080/00223131.2022.2128460

MAAP code analysis focusing on the fuel debris condition in the lower head of the pressure vessel in Fukushima-Daiichi Nuclear Power Station Unit 2

Sato, Ikken; Yoshikawa, Shinji; Yamashita, Takuya; Cibula, M.*; Mizokami, Shinya*

Nuclear Engineering and Design, 404, p.112205_1 - 112205_21, 2023/04

https://doi.org/10.1016/j.nucengdes.2023.112205

Based on updated knowledge from plant-internal investigations, experiments and model simulations until now, the in-vessel phase of Fukushima-Daiichi Nuclear Power Station Unit 2 was analyzed using the MAAP code. In Unit 2, it is considered that the core material enthalpy was relatively low when it relocated to the lower plenum of the pressure vessel, then, cooled by the coolant and solidified there. Although the MAAP code tended to underestimate the degree of core-material oxidation during the relocation, this probable underestimation was compensated for by an existing study that was considered more reliable, so that more realistic debris conditions in the lower plenum could be obtained. Basic validity of the former prediction of the Unit 2 accident progression behavior was confirmed and detailed boundary condition for the later phase was provided. This boundary condition should be utilized for future studies addressing debris reheating process leading to lower head failure and debris relocation toward the pedestal.

Development of technologies for enhanced analysis accuracy of fuel debris; Summary results of the 2020 fiscal year (Subsidy program for the project of decommissioning and contaminated water management)

Ikeuchi, Hirotomo; Koyama, Shinichi; Osaka, Masahiko; Takano, Masahide; Nakamura, Satoshi; Onozawa, Atsushi; Sasaki, Shinji; Onishi, Takashi; Maeda, Koji; Kirishima, Akira*; et al.

JAEA-Technology 2022-021, 224 Pages, 2022/10

JAEA-Technology-2022-021.pdf:12.32MB

A set of technology, including acid dissolving, has to be established for the analysis of content of elements/nuclides in the fuel debris samples. In this project, a blind test was performed for the purpose of clarifying the current level of analytical accuracy and establishing the alternative methods in case that the insoluble residue remains. Overall composition of the simulated fuel debris (homogenized powder having a specific composition) were quantitatively determined in the four analytical institutions in Japan by using their own dissolving and analytical techniques. The merit and drawback for each technique were then evaluated, based on which a tentative flow of the analyses of fuel debris was constructed.

Uranium dissolution and uranyl peroxide formation by immersion of simulated fuel debris in aqueous HO solution

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

Journal of Nuclear Science and Technology, 59(8), p.961 - 971, 2022/08

https://doi.org/10.1080/00223131.2021.2023055

We investigated potential degradation of fuel debris caused by HO, which is the oxidant of major impact from water radiolysis. We performed leaching experiments on different kinds of simulated debris comprising U, Fe, Cr, Ni, and Zr in an aqueous HO solution. Chemical analysis of the leaching solution showed that U dissolution was induced by HO. Raman analysis after the leaching revealed that uranyl peroxides were formed on the surface of the simulated debris. These results demonstrate that uranyl peroxides are possible alteration products of fuel debris from HO reaction. However, the sample in which the main uranium-containing phase was a U-Zr oxide solid solution showed much less uranium dissolution and no Raman signal of uranyl peroxides. Comparison of these results indicates that formation of an oxide solid solution of Zr with UO improves the stability of fuel debris against HO reaction.

Step-by-step challenge of debris characterization for the decommissioning of Fukushima-Daiichi Nuclear Power Station (FDNPS)

Kurata, Masaki; Okuzumi, Naoaki*; Nakayoshi, Akira; Ikeuchi, Hirotomo; Koyama, Shinichi

Journal of Nuclear Science and Technology, 59(7), p.807 - 834, 2022/07

https://doi.org/10.1080/00223131.2022.2040393

Immediately after the 1F-accident, various attempts have been made to evaluate the fuel debris characteristics toward the decommissioning of 1F. The present review outlines those attempts. In the years immediately following the 1F-accident, the knowledge obtained from the 1F-site (especially from the damaged reactors of Units 1, 2 and 3) was extremely limited. The approximate location of fuel debris was investigated by muon tomography, and its characteristics were roughly estimated based on the past findings such as the results of the Three Mile Island-II accident investigation in the United States, which gave us information of prototypical accident scenarios and debris characteristics for pressurized water reactor accident. After that, various internal investigation robots were developed, and from 2017, investigation of the inside of the reactor containment vessel was started using these robots. Consequently, these three units were found to have core damage status and debris distribution that were rather different from what had been expected based on the typical accident scenario of a pressurized water reactor. In parallel, a small amount of U-bearing particle was recovered from the smear samples of these robots. The analysis of these particles is ongoing to get information relevant to fuel debrsi body. Furthermore, international collaboration is ongoing mainly under OECD/NEA, including accident analysis and debris characterization. From now on, one need to further understand 1F-accident scenario and progress debris characterization based on these 1F-site information.

Evaluation of critical experimental core configurations to simulate non-uniform fuel debris

Gunji, Satoshi; Araki, Shohei; Suyama, Kenya; Izawa, Kazuhiko

Proceedings of International Conference on Physics of Reactors 2022 (PHYSOR 2022) (Internet), 10 Pages, 2022/05

The fuel debris is expected to have not only heterogeneous but also non-uniform compositions. Therefore, the calculation method used in their criticality management is required to be validated experimentally. In this study, several core configurations of a new critical assembly "STACY" of JAEA with non-uniform arrangements of uranium oxide fuel rods, concrete rods and stainless steel rods, which are components of the fuel debris, were studied. In each case, the median value of 100 sample patterns was larger than the mean effective multiplication factor. It was also confirmed that there are differences in the effective multiplication factor of more than one dollar by the pattern changing, and that the neutron spectra can change significantly by changing the local neutron moderation conditions. In particular, the effective multiplication factor became smaller when over-moderated regions with large water-to-fuel ratios were formed in the core configurations due to increases in thermal neutron absorption. Such criticality experiments with non-uniform arrangements of multiple compositions will be useful to evaluate the validity of the calculation code.