Annual report on the environmental radiation monitoring around the Tokai Reprocessing Plant FY2022

Kokubun, Yuji; Nakada, Akira; Seya, Natsumi; Koike, Yuko; Nemoto, Masashi; Tobita, Keiji; Yamada, Ryohei*; Uchiyama, Rei; Yamashita, Daichi; Nagai, Shinji; et al.

JAEA-Review 2023-046, 164 Pages, 2024/03

JAEA-Review-2023-046.pdf:4.2MB

The Nuclear Fuel Cycle Engineering Laboratories conducts environmental radiation monitoring around the reprocessing plant in accordance with the "Safety Regulations for Reprocessing Plant of JAEA, Part IV: Environmental Monitoring". This report summarizes the results of environmental radiation monitoring conducted during the period from April 2022 to March 2023 and the results of dose calculations for the surrounding public due to the release of radioactive materials into the atmosphere and ocean. In the results of the above environmental radiation monitoring, many items were affected by radioactive materials emitted from the accident at the Fukushima Daiichi Nuclear Power Plant of Tokyo Electric Power Company, Incorporated (changed to Tokyo Electric Power Company Holdings, Inc. on April 1, 2016), which occurred in March 2011. Also included as appendices are an overview of the environmental monitoring plan, an overview of measurement methods, measurement results and their changes over time, meteorological statistics results, radioactive waste release status, and an evaluation of the data which deviated of the normal range.

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.

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.

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.

Carrying-out of whole nuclear fuel materials in Plutonium Research Building No.1

Inagawa, Jun; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Nakada, Masami; Takano, Masahide; Akie, Hiroshi; Shimizu, Osamu; Komuro, Michiyasu; Oura, Hirofumi*; Nagai, Isao*; et al.

JAEA-Technology 2021-001, 144 Pages, 2021/08

JAEA-Technology-2021-001.pdf:12.98MB

Plutonium Research Building No.1 (Pu1) was qualified as a facility to decommission, and preparatory operations for decommission were worked by the research groups users and the facility managers of Pu1. The operation of transportation of whole nuclear materials in Pu1 to Back-end Cycle Key Element Research Facility (BECKY) completed at Dec. 2020. In the operation included evaluation of criticality safety for changing permission of the license for use nuclear fuel materials in BECKY, cask of the transportation, the registration request of the cask at the institute, the test transportation, formulation of plan for whole nuclear materials transportation, and the main transportation. This report circumstantially shows all of those process to help prospective decommission.

Preliminary missions for the decommissioning of the laboratory building No.1 for the plutonium research program

Segawa, Yukari; Horita, Takuma; Kitatsuji, Yoshihiro; Kumagai, Yuta; Aoyagi, Noboru; Nakada, Masami; Otobe, Haruyoshi; Tamura, Yukito*; Okamoto, Hisato; Otomo, Takashi; et al.

JAEA-Technology 2016-039, 64 Pages, 2017/03

JAEA-Technology-2016-039.pdf:5.24MB

The laboratory building No.1 for the plutonium research program (Bldg. Pu1) was chosen as one of the facilities to decommission by Japan Atomic Energy Agency Reform in September, 2013. The research groups, users of Bldg. Pu1, were driven by necessity to remove used equipment and transport nuclear fuel to other facilities from Bldg. Pu1. Research Group for Radiochemistry proactively established the Used Equipment Removal Team for the smooth operation of the removal in April, 2015. The team classified six types of work into the nature of the operation, removal of used equipment, disposal of chemicals, stabilization of mercury, stabilization of nuclear fuel, transportation of nuclear fuel and radioisotope, and survey of contamination status inside the glove boxes. These works were completed in December, 2015. This report circumstantially shows six works process, with the exception of the approval of the changes on the usage of nuclear fuel in Bldg. Pu1 to help prospective decommission.

Self-radiation effects and glassy nature of magnetic transition in AmO revealed by O-NMR

Tokunaga, Yo; Nishi, Tsuyoshi; Nakada, Masami; Ito, Akinori*; Sakai, Hironori; Kambe, Shinsaku; Homma, Yoshiya*; Honda, Fuminori*; Aoki, Dai*; Walstedt, R. E.*

Physical Review B, 89(21), p.214416_1 - 214416_8, 2014/06

https://doi.org/10.1103/PhysRevB.89.214416

The magnetic phase transition near K in AmO has been investigated microscopically by means of O NMR. To avoid complexities arising from sample aging associated with the alpha decay of Am, all measurements have been performed within 40 days after sample synthesis. Even during such a short period, however, a rapid change of NMR line shape has been observed at 1.5 K, suggesting that the ground state of AmO is very sensitive to disorder. We have also confirmed the loss of O NMR signal intensity over a wide temperature range below , and more than half of oxygen nuclei are undetectable at 1.5 K. This behavior reveals the persistence of slow and distributed spin fluctuations down to temperatures well below . In the paramagnetic state, strong NMR line broadening and spatially inhomogeneous spin fluctuations have been observed. The results are all indicative of short-range, spin-glass-like character for the magnetic transition in this system.

DFT study on the electronic structure and chemical state of americium in an (Am,U) mixed oxide

Suzuki, Chikashi; Nishi, Tsuyoshi; Nakada, Masami; Tsuru, Tomohito; Akabori, Mitsuo; Hirata, Masaru; Kaji, Yoshiyuki

Journal of Physics and Chemistry of Solids, 74(12), p.1769 - 1774, 2013/12

https://doi.org/10.1016/j.jpcs.2013.07.006

We investigated the electronic state of a CaF-type (Am,U) mixed oxide using the all-electron full potential linear augmented plane wave method and compared it with those of AmO, AmO, UO, and LaUO. The valence of Am in the mixed oxide was close to that of AmO and the valence of U in the mixed oxide was pentavalent. The electronic structure of AmO was different from that of AmO, particularly just above the Fermi level. In addition, the electronic states of Am and U in the mixed oxide were similar to those of trivalent Am and pentavalent U oxides. These electronic states reflected the high oxygen potential of AmO and the heightened oxygen potential resulting from the addition of Am to UO and also suggested the occurrence of charge transfer from Am to U in the solid solution process.

High-temperature X-ray imaging study of simulated high-level waste glass melt

Okamoto, Yoshihiro; Nakada, Masami; Akabori, Mitsuo; Komamine, Satoshi*; Fukui, Toshiki*; Ochi, Eiji*; Nitani, Hiroaki*; Nomura, Masaharu*

Denki Kagaku Oyobi Kogyo Butsuri Kagaku, 81(7), p.543 - 546, 2013/07

https://doi.org/10.5796/electrochemistry.81.543

The molten state of simulated high-level waste glass and the behavior of ruthenium element in the melt were investigated by using synchrotron radiation based X-ray imaging technique. Melting, generating and moving of bubbles, condensation and sedimentation of ruthenium element were observed dynamically in continuous 12-bit gray-scale images from the CCD camera. X-ray intensity was obtained easily by digitizing gray-scale values in the image. The existence of ruthenium element is emphasized as a black color in the CCD image at X-ray energy higher than the Ru K-absorption edge. Position sensitive imaging X-ray absorption fine structure (XAFS) measurement was also performed to clarify the chemical state of ruthenium element in the melt.

High-temperature X-ray imaging study of simulated high-level waste glass melt

Okamoto, Yoshihiro; Nakada, Masami; Akabori, Mitsuo; Komamine, Satoshi*; Fukui, Toshiki*; Ochi, Eiji*; Nitani, Hiroaki*; Nomura, Masaharu*

Proceedings of 4th Asian Conference on Molten Salt Chemistry and Technology & 44th Symposium on Molten Salt Chemistry, Japan, p.47 - 52, 2012/09

The molten state of the simulated high-level waste glass and the behavior of ruthenium element in the melt were investigated by using synchrotron radiation based X-ray imaging technique. Melting, generating and moving of bubbles, condensation and sedimentation of ruthenium element were observed dynamically in continuous 12-bit gray-scale images from the CCD camera. The existence of ruthenium in the X-ray CCD image was emphasized over the energy of Ru K-absorption edge. X-ray intensity was obtained easily by digitalizing gray-scale values in the image. Position sensitive imaging X-ray absorption fine structure (XAFS) measurement was performed to clarify the chemical state of ruthenium element in the melt.