Experimental verification of operational conditions for the 3rd glass melter in TVF

Asahi, Yoshimitsu; Fukuda, Shigeki; Shiramizu, Daiki; Miyata, Koshi; Tone, Masaya; Katsuoka, Nanako; Maeda, Yuta; Aoyama, Yusuke; Niitsuma, Koichi; Kobayashi, Hidekazu; et al.

JAEA-Technology 2024-024, 271 Pages, 2025/03

JAEA-Technology-2024-024.pdf:33.98MB
JAEA-Technology-2024-024-hyperlink.zip:31.96MB

A glass melter for the vitrification process of highly active liquid waste in the Tokai Reprocessing Plant, TVF's 3rd melter, was built, and the glass of 18 vitrified waste canisters in weight was melted and poured through a cold test operation. The molten glass surface was covered by a cold cap from feeding fiberglass cartridges saturated with non-radioactive simulant liquid waste as raw material, whose components are equivalent to actual waste. Differences in inherent characteristics of the thermal behavior between the 2nd and the 3rd melter due to the difference in design were considered to establish the procedure to control the new melter. The melter's condition was stabilized at a higher glass temperature and the cooling of 1 kW less in each of the two main electrodes, compared to the 2nd one. Under 39 kW joule heating of the main electrodes with 26 Nm3/h coolant flow rate, it showed the capability to finish heating the bottom furnace in 5 hours before pouring, 2 hours shorter than the 2nd melter. Measurements of the temperature distributions in molten glass and casing surface yielded data that is efficient for developing a simulation model. After Platinum Group Elements (PGE) concentration saturates in the molten glass, feeding raw material and discharging glass were suspended to examine a holding state, indicating PGE settling could retard. During the holding test, observation of the melting process of the cold cap declared that the surface was covered by a thin layer with almost non-fluidity. It will be a reason for choosing the no-slip condition of a fluid calculation, even in the hot-top condition. The investigation of PGE discharging behavior by analyzing the elemental composition of poured glass showed the accumulated PGE amount in the 3rd melter is small compared to the 2nd melter. Inspection of the melter inside after draining out concluded that there were neither significant residual glass nor refractory fragments.

Effect of Mn substitution on the electronic structure for Mn-doped indium-tin oxide films studied by soft and hard X-ray photoemission spectroscopy

Otsuki, Daiki*; Ishida, Tatsuhiro*; Tsutsumi, Naoya*; Kobayashi, Masaki*; Inagaki, Kodai*; Yoshida, Teppei*; Takeda, Yukiharu; Fujimori, Shinichi; Yasui, Akira*; Kitagawa, Saiki*; et al.

Physical Review Materials (Internet), 7(12), p.124601_1 - 124601_6, 2023/12

https://doi.org/10.1103/PhysRevMaterials.7.124601

Design details of bottom shape for the 3rd glass melter in TVF

Asahi, Yoshimitsu; Shimamura, Keisuke*; Kobayashi, Hidekazu; Kodaka, Akira

JAEA-Technology 2021-026, 50 Pages, 2022/03

JAEA-Technology-2021-026.pdf:6.29MB

In Tokai Reprocessing Plant, the highly active liquid waste derived from a spent fuel reprocessing is vitrified with a Liquid-Fed Ceramic Melter (LFCM) embedded in Tokai Vitrification Facility (TVF). For an LFCM, the viscosity of melted glass is increased by the deposition of oxidation products of platinum group elements (PGE) and the PGE-containing glass tends to settle to the melter's bottom basin even after draining glass out. Removal of the PGE-containing glass is needed to avoid the Joule heating current from being affected by the glass, it requires time-consuming work to remove. For the early accomplishment of vitrifying the waste, Japan Atomic Energy Agency is planning to replace the current melter with the new one in which the amount of PGE sediments would be reduced. In the past design activities for the next melter, several kinds of shapes in regard to the furnace bottom and the strainer were drawn. Among these designs, the one in which the discharge ratio of PGE-containing glass would be as much as or greater than the current melter and which be able to perform similar operational sequences done in the current melter is selected here. Firstly, an operational sequence to produce one canister of vitrified waste is simulated for three melter designs with a furnace bottom shape, using 3D thermal-hydraulic calculations. The computed temperature distribution and its changes are compared among the candidate structures. After discussions about the technical and structural feasibilities of each design, a cone shape with a 45 slope was selected as the bottom shape of the next melter. Secondly, five strainer designs that fit the bottom shape above mentioned are drawn. For each design, the fluid drag and the discharge ratio of relatively high viscosity fluid resting near the bottom are estimated, using steady or unsteady CFD simulation. By draining silicone oil from acrylic furnace models, it was confirmed experimentally that there are no vortices

Epitaxial thin film growth of europium dihydride

Komatsu, Yuya*; Shimizu, Ryota*; Wilde, M.*; Kobayashi, Shigeru*; Sasahara, Yuki*; Nishio, Kazunori*; Shigematsu, Kei*; Otomo, Akira*; Fukutani, Katsuyuki; Hitosugi, Taro*

Crystal Growth & Design, 20(9), p.5903 - 5907, 2020/09

https://doi.org/10.1021/acs.cgd.0c00602

Local structure study of the iron-based systems of BaFeAs and LiFeAs by X-ray PDF and XAFS analyses

Li, S.*; Toyoda, Masayuki*; Kobayashi, Yoshiaki*; Ito, Masayuki*; Ikeuchi, Kazuhiko*; Yoneda, Yasuhiro; Otani, Akira*; Matsumura, Daiju; Asano, Shun*; Mizuki, Junichiro*; et al.

Physica C, 555, p.45 - 53, 2018/12

https://doi.org/10.1016/j.physc.2018.10.003

-dependence of local distortions in BaFeAs and LiFeAs by X-ray PDF and XAFS methods. Although PDF data exhibit anomaly at the structure transition temperature, EXAFS data exhibit no anomaly. Data supporting the local orthorhombicity at 300 K in the tetragonal phase for BaFeAs. Arguments on the origins of the 4-fold symmetry breaking in the ground average structure of the tetragonal phase.

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.