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.

The Chemistry of thorium, plutonium and MA

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki; Sasaki, Takayuki*; Uehara, Akihiro*; Takeda, Shino*; Kitatsuji, Yoshihiro; Otobe, Haruyoshi; Kobayashi, Taishi*

The Chemistry of Thorium, Plutonium and MA, 254 Pages, 2022/03

The chemistry of nuclear materials such as Thorium (Part 1) and Plutonium (Part 2) was described in relation from the fundamentals on solid chemistry and solution chemistry to the practicals on the experiment and evaluation method in detail. Minor actinides such as Neptunium, Americium, Curium and Protoactinium, was introduced the basics on the solid and solution chemistry.

Thermodynamic interpretation of uranium(IV/VI) solubility in the presence of -isosaccharinic acid

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11

https://doi.org/10.1016/j.jct.2019.06.006

The effect of -isosaccharinic acid (ISA) on the solubility and redox of tetravalent and hexavalent uranium (U(IV), U(VI)) was investigated in the hydrogen ion concentration (pH) range of 613 and at total ISA concentration ([ISA]) = 1010 mol/dm. The dependence of U(IV) solubility on pH and [ISA] suggested the existence of U(OH)(ISA) as a dominant species within the investigated pH range of 612. For the U(VI)-ISA system, UO(OH)(ISA) was suggested as a dominant species at pH 713. The formation constants of the U(IV)-ISA and U(VI)-ISA complexes were determined by least-squares fitting of the solubility data. The solubility of U(IV) and U(VI) in the presence of ISA and its effect on the redox behavior were thermodynamically interpreted based on the obtained constants.

Status of development on LaB filament arc-driven multi-cusp ion source for iBNCT

Shibata, Takanori*; Takagi, Akira*; Ikegami, Kiyoshi*; Sugimura, Takashi*; Nammo, Kesao*; Naito, Fujio*; Kobayashi, Hitoshi*; Kurihara, Toshikazu*; Honda, Yosuke*; Sato, Masaharu*; et al.

Proceedings of 15th Annual Meeting of Particle Accelerator Society of Japan (Internet), p.385 - 387, 2018/10

Nanoscale spatial analysis of clay minerals containing cesium by synchrotron radiation photoemission electron microscopy

Yoshigoe, Akitaka; Shiwaku, Hideaki; Kobayashi, Toru; Shimoyama, Iwao; Matsumura, Daiju; Tsuji, Takuya; Nishihata, Yasuo; Kogure, Toshihiro*; Okochi, Takuo*; Yasui, Akira*; et al.

Applied Physics Letters, 112(2), p.021603_1 - 021603_5, 2018/01

https://doi.org/10.1063/1.5005799

A synchrotron radiation photoemission electron microscope (SR-PEEM) was applied to demonstrate pinpoint analysis of micrometer-sized weathered biotite clay particles with artificially adsorbed cesium (Cs) atoms. Despite the insulating properties of the clay, we observed the spatial distributions of constituent elements (Si, Al, Cs, Mg, Fe) without charging issues. We found that Cs atoms were likely to be adsorbed evenly over the entire particle. Spatially-resolved X-ray absorption spectra (XAS) of the Cs M-edge region showed Cs to be present in a monocation state (Cs). Further pinpoint XAS measurements were also performed at the Fe L-edge to determine the chemical valence of the Fe atoms. Our results demonstrate the utility of SR-PEEM as a tool for spatially-resolved chemical analyses of various environmental substances, which is not limited by the poor conductivity of samples.

Thermodynamic model for Zr solubility in the presence of gluconic acid and isosaccharinic acid

Kobayashi, Taishi*; Teshima, Takeshi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Nuclear Science and Technology, 54(2), p.233 - 241, 2017/02

https://doi.org/10.1080/00223131.2016.1255573

Zr solubility in the presence of gluconic acid (GLU) and isosaccharinic acid (ISA) was investigated as a function of hydrogen ion concentration (pH) and the total concentration of GLU or ISA. The dependence of the increase in Zr solubility on the pH and GLU concentration suggested the existence of Zr(OH)(GLU) in the neutral pH region and Zr(OH)(GLU)(GLU) in the alkaline pH region above pH 10 as the dominant species in the presence of 10 - 10 mol/dm (M) GLU. In the presence of ISA, the dominant species Zr(OH)(ISA) and Zr(OH)(ISA)(ISA) were proposed to occur in the neutral and alkaline pH regions, similar to those found in the presence of GLU. From X-ray diffraction analysis, the solubility-limiting solid phase in the presence of GLU and ISA was considered to be Zr(OH)(am). The formation constants of the Zr gluconate and isosaccharinate complexes were determined by least squares fitting analysis of the solubility data, and the obtained values were discussed in comparison with those of tetravalent actinides.

Issues concerning the determination of solubility products of sparingly soluble crystalline solids; Solubility of HfO(cr)

Rai, D.*; Kitamura, Akira; Rosso, K. M.*; Sasaki, Takayuki*; Kobayashi, Taishi*

Radiochimica Acta, 104(8), p.583 - 592, 2016/08

https://doi.org/10.1515/ract-2015-2540

Solubility studies were conducted with HfO(cr) solid as a function of acid concentrations. These studies involved (1) using two different amounts of the solid phase, (2) acid washing the bulk solid phase, (3) preheating the solid phase to 1400 C, and (4) heating amorphous HfO(am) suspensions to 90 C to ascertain whether the HfO(am) converts to HfO(cr) and to determine the solubility from the oversaturation direction. Based on the results of these treatments it is concluded that the HfO(cr) contains a small fraction of less crystalline, but not amorphous, material [HfO(lcr)] and this, rather than the HfO(cr), is the solubility-controlling phase in the range of experimental variables investigated in this study. The solubility data are interpreted using both the Pitzer and SIT models. The log of the solubility product of HfO(cr) is estimated. The observation of a small fraction of less crystalline higher solubility material is consistent with the general picture that mineral surfaces are often structurally and/or imperfect leading to a higher solubility than the bulk crystalline solid. This study stresses the urgent need, during interpretation of solubility data, of taking precautions to make certain that the observed solubility behavior for sparingly-soluble solids is assigned to the proper solid phase.

Establishment of experimental system for Mo/Tc production by neutron activation method

Ishida, Takuya; Shiina, Takayuki*; Ota, Akio*; Kimura, Akihiro; Nishikata, Kaori; Shibata, Akira; Tanase, Masakazu*; Kobayashi, Masaaki*; Sano, Tadafumi*; Fujihara, Yasuyuki*; et al.

JAEA-Technology 2015-030, 42 Pages, 2015/11

JAEA-Technology-2015-030.pdf:4.82MB

The research and development (R&D) on the production of Mo/Tc by neutron activation method ((n, ) method) using JMTR has been carried out in the Neutron Irradiation and Testing Reactor Center. The specific radioactivity of Mo by (n, ) method is extremely low compared with that by fission method ((n,f) method), and as a result, the radioactive concentration of the obtained Tc solution is also lowered. To solve the problem, we propose the solvent extraction with methyl ethyl ketone (MEK) for recovery of Tc from Mo produced by (n, ) method. We have developed the Mo/Tc separation/extraction/concentration devices and have carried out the performance tests for recovery of Tc from Mo produced by (n, ) method. In this paper, in order to establish an experimental system for Mo/Tc production, the R&D results of the system are summarized on the improvement of the devices for high-recovery rate of Tc, on the dissolution of the pellets, which is the high-density molybdenum trioxide (MoO) pellets irradiated in Kyoto University Research Reactor (KUR), on the production of Tc, and on the inspection of the recovered Tc solutions.

Dismantlement of large fusion experimental device JT-60U

Ikeda, Yoshitaka; Okano, Fuminori; Sakasai, Akira; Hanada, Masaya; Akino, Noboru; Ichige, Hisashi; Kaminaga, Atsushi; Kiyono, Kimihiro; Kubo, Hirotaka; Kobayashi, Kazuhiro; et al.

Nihon Genshiryoku Gakkai Wabun Rombunshi, 13(4), p.167 - 178, 2014/12

https://doi.org/10.3327/taesj.J14.007

The JT-60U torus was disassembled so as to newly install the superconducting tokamak JT-60SA torus. The JT-60U used the deuterium for 18 years, so the disassembly project of the JT-60U was the first disassembly experience of a fusion device with radioactivation in Japan. All disassembly components were stored with recording the data such as dose rate, weight and kind of material, so as to apply the clearance level regulation in future. The lessons learned from the disassembly project indicated that the cutting technologies and storage management of disassembly components were the key factors to conduct the disassembly project in an efficient way. After completing the disassembly project, efforts have been made to analyze the data for characterizing disassembly activities, so as to contribute the estimation of manpower needs and the radioactivation of the disassembly components on other fusion devices.

Thermal transient test and strength evaluation of a tubesheet structure made of Mod.9Cr-1Mo steel, 1; Test model design and experimental results

Ando, Masanori; Hasebe, Shinichi; Kobayashi, Sumio; Kasahara, Naoto*; Toyoshi, Akira*; Omae, Takahiro*; Enuma, Yasuhiro*

Nuclear Engineering and Design, 275, p.408 - 421, 2014/08

AA2013-0395.pdf:2.65MB

https://doi.org/10.1016/j.nucengdes.2014.04.032

To clarify the failure mode of a semispherical tubesheet structure originally designed for SG in the JSFR, a cyclic thermal loading test was performed using a tubesheet model test structure. The tubesheet model made of Mod.9Cr-1Mo steel was subjected to 1,873 cycles of severe thermal transient loads using a large-scale sodium loop, in which sodium heated to 600C and 250C was flowed repeatedly with periods for each transient of 2 and 1 h, respectively. After the test, the test model was inspected by PT. Then, observation using a SEM and hardness testing were performed. A thermal-hydraulic analysis was also performed to validate the measured temperature history during the thermal transient. Through these examinations and evaluation with thermal-hydraulic analysis, the manner of failure in the tubesheet under cyclic thermal loading is discussed.