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.

Chemical species of cesium and iodine in condensed vaporized microparticles formed by melting nuclear fuel components with concrete materials

Onuki, Toshihiko*; Ye, J.*; Kato, Tomoaki; Liu, J.; Takano, Masahide; Kozai, Naofumi; Utsunomiya, Satoshi*

Environmental Science; Processes & Impacts, 25(7), p.1204 - 1212, 2023/07

https://doi.org/10.1039/D3EM00074E

To elucidate chemical forms of Cs and I in microparticles produced via the Fukushima Daiichi Nuclear Power Plant accident and released into the atmosphere, we analyzed Cs and I in condensed vaporized particles (CVP) produced by melting experiments using nuclear fuel components containing CsI with concrete. CVPs consisted of many round particles containing Cs and I of diameters less than several tens of micrometers. Two kinds of particles were present: one containing large amounts of Cs and I, suggesting the presence of CsI, and the other containing small amounts of Cs and I with large Si contents. Most of CsI from both particles were dissolved in water. On the contrary, some fractions of Cs remained from the latter particles. These results suggest that Cs was incorporated in CVPs along with Si to form water low-soluble CVPs

Surface analyses of CsOH chemisorbed on concrete and aggregate at around 200C

Luu, V. N.; Nakajima, Kunihisa

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 9 Pages, 2023/05

https://doi.org/10.1299/jsmeicone.2023.30.1940

Chemical interaction between Sr vapor species and nuclear reactor core structure

Mohamad, A. B.; Nakajima, Kunihisa; Miwa, Shuhei; Osaka, Masahiko

Journal of Nuclear Science and Technology, 60(3), p.215 - 222, 2023/03

https://doi.org/10.1080/00223131.2022.2092227

Formation of MPd (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd using cadmium chloride

Hayashi, Hirokazu; Shibata, Hiroki; Sato, Takumi; Otobe, Haruyoshi

Journal of Radioanalytical and Nuclear Chemistry, 332(2), p.503 - 510, 2023/02

https://doi.org/10.1007/s10967-023-08760-4

The formation of MPd (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu-type GdPd ( = 0.4081 0.0001 nm) and NpPd ( = 0.4081 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi-type NpPd. Chlorination of the MPd (M = Gd, Np) samples was accomplished by the solid-state reaction using cadmium chloride at 673 K in a dynamic vacuum. Pd-rich solid solution phase saturated with Cd and an intermetallic compound PdCd were obtained as by-products of MCl formation.

Cohesive/Adhesive strengths of CsOH-chemisorbed SS304 surfaces

Li, N.*; Sun, Y.*; Nakajima, Kunihisa; Kurosaki, Ken*

Journal of Nuclear Science and Technology, 11 Pages, 2023/00

https://doi.org/10.1080/00223131.2023.2231447

During the Fukushima Daiichi nuclear power plant (1F) accident, an overwhelming amount of the cesium remaining in the pressure vessel could have been deposited onto 304 stainless steel (SS304) steam separators and dryers, both with large surface areas. During 1F's decommissioning, the deposited cesium is a safety hazard as it can generate radioactive dust. However, the cohesive and adhesive strengths of CsOH-chemisorbed oxide scales are yet to be defined. In this study, we investigated how CsOH-chemisorption affects the cohesive and adhesive strengths between oxide scales and SS304 substrates with a scratch tester. The scratch test results revealed that the cohesive strengths of the oxide scales decreased after CsOH-chemisorption, while adhesive failure could not be reached.

High-temperature gaseous reaction of cesium with siliceous thermal insulation; The Potential implication to the provenance of enigmatic Fukushima cesium-bearing material

Rizaal, M.; Nakajima, Kunihisa; Saito, Takumi*; Osaka, Masahiko; Okamoto, Koji*

ACS Omega (Internet), 7(33), p.29326 - 29336, 2022/08

https://doi.org/10.1021/acsomega.2c03525

Decommissioning of the Plutonium Research Building No.1 (Plan and Present Status)

Komuro, Michiyasu; Kanazawa, Hiroyuki; Kokusen, Junya; Shimizu, Osamu; Honda, Junichi; Harada, Katsuya; Otobe, Haruyoshi; Nakada, Masami; Inagawa, Jun

JAEA-Technology 2021-042, 197 Pages, 2022/03

JAEA-Technology-2021-042.pdf:16.87MB

Plutonium Research Building No.1 was constructed in 1960 for the purpose of establishing plutonium handling technology and studying its basic physical properties. Radiochemical research, physicochemical research and analytical chemistry regarding solutions and solid plutonium compounds had been doing for the research program in Japan Atomic Energy Agency (JAEA). In 1964, the laboratory building was expanded and started the researching plutonium-uranium mixed fuel and reprocessing of plutonium-based fuel, playing an advanced role in plutonium-related research in Japan. Since then, the research target has been expanded to include transplutonium elements, and it has functioned as a basic research facility for actinides. The laboratory is constructed by concrete structure and it has the second floor, equipped with 15 glove boxes and 4 chemical hoods. Plutonium Research Building No.1 was decided as one of the facilities to be decommissioned by Japan Atomic Energy Agency Reform Plan in September 2014. So far, the contamination survey of the radioactive materials in the controlled area, the decontamination of glove boxes, and the consideration of the equipment dismantling procedure have been performed as planned. The radioisotope and nuclear fuel materials used in the facility have been transfer to the other facilities in JAEA. The decommissioning of the facility is proceeding with the goal of completing by decommissioning the radiation controlled area in 2026. In this report, the details of the decommissioning plan and the past achievements are reported with the several data.

Phase stability of Cs-Si-O and Cs-Si-Fe-O compounds on stainless steel

Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko

Journal of Nuclear Science and Technology, 59(3), p.345 - 356, 2022/03

https://doi.org/10.1080/00223131.2021.1971576

During a severe accident (SA) such as the Fukushima Daiichi Nuclear Power Plant accident, fission products (FP) can be retained on the surface of structural materials in reactors. Cesium (Cs) is an important FP, and various Cs compounds such as Cs silicates are formed on the surface of stainless steel (SS) in a reactor during a SA. We calculated total energies of Cs-Si-O compounds for evaluation on phase stability within an adiabatic approximation. The calculations indicate that CsSiO is the most stable of the Cs-Si-O compounds. We calculated, furthermore, total energies of Cs-Si-Fe-O compounds. These calculations indicate that Cs-Si-Fe-O compounds are more stable than C-Si-O compounds and that CsSiFeO is the most stable of these C-Si-O and Cs-Si-Fe-O compounds within an adiabatic approximation. The results of our present calculations and our previous experiments lead to the conclusion that Cs-Si-Fe-O compounds can be stably formed on SS surface by Cs chemisorption.

Cesium chemistry in the LWR severe accident and towards the decommissioning of Fukushima Daiichi Nuclear Power Station

Osaka, Masahiko; Goullo, M.*; Nakajima, Kunihisa

Journal of Nuclear Science and Technology, 59(3), p.292 - 305, 2022/03

https://doi.org/10.1080/00223131.2021.1997664

Research on the fission product chemistry made after the severe accident of the Fukushima Daiichi Nuclear Power Station were reviewed with focus on the Cesium chemistry in terms of two regimes, namely the accidental source term and the long-term source term via aqueous phase towards the decommissioning. For the accidental source term, Cs chemical interaction with Mo, B and Si were reviewed. Regarding the unique issue of long-term source term via aqueous phase, Cs penetration into concrete and fuel debris leaching were mentioned as the main sources of FPs. Efforts on the preparation of thermodynamic data for the Cs complex oxides were described. All these Cs chemical behaviors should be modelled and validated/verified through the analysis and evaluation of the actual samples including fuel debris that would be taken from the Fukushima Daiichi Nuclear Power Station in near future.