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JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 5 (Joint research)

Nagai, Takayuki; Aoyama, Yusuke; Okamoto, Yoshihiro; Shibata, Daisuke*; Asakura, Kiyotaka*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Kikuchi, Tetsuya*; Hatakeyama, Kiyoshi*

JAEA-Research 2025-009, 122 Pages, 2025/11

JAEA-Research-2025-009.pdf:20.77MB

XAFS measurements in the soft X-ray region are suitable for evaluating the chemical state of the surface layer of a measurement sample because the X-ray transmittance is low. This study measured the K-edges of the glass-forming elements boron (B), oxygen (O), sodium (Na), and silicon (Si), as well as the L$$_{3}$$-edge of the waste component cerium (Ce), to verify the differences between the coagulated layer and the inside of simulated waste glasses made from raw glass compositions with increased alumina concentration. As a result, from the B K-edge XANES spectra, the proportion of B-O tetracoordinate sp$$^{3}$$ structures (BO$$_{4}$$) on the surface layer of the coagulated glass samples was higher than that on the cut surface inside the glass samples. On the other hand, the O K-edge XANES spectra showed differences by measuring points for each glass sample, but the trends of those differences varied between the glass samples. The reason is that the molten raw glass with increased alumina concentration has a high viscosity, making it impossible to produce waste glasses with a uniform composition. The Na and Si K-edge spectra showed no differences between the coagulated layer and the inside of glass samples. In addition, the Ce L$$_{3}$$-edge XANES spectra confirmed that the Ce valence in the coagulated layer of glass samples was more oxidized compared to that in the inside of glass samples.

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 4 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2024-014, 54 Pages, 2025/02

JAEA-Research-2024-014.pdf:7.02MB

XAFS measurements in the soft X-ray region are suitable for evaluating the chemical state of the surface layer of a measurement sample because the X-ray transmittance is low. In this study, the purpose of the study was to confirm the difference between the coagulated surface layer and the inside of the simulated waste glasses by measuring the K-edge of the glass constituent elements boron, oxygen, sodium, and silicon, and the L$$_{3}$$ edge of the waste component cerium. As a result, the B K-edge XANES spectra showed that the proportion of B-O tetracoordinate sp$$^{3}$$ structures (BO$$_{4}$$) on the surface layer of the coagulated glass samples was higher than that on the cut surface inside the glass samples, which is expected to improve the water resistance of the coagulated surface. On the other hand, the O K-edge XANES spectra suggested that the O abundance in the coagulated surface layer was lower than that in the cut surface inside the glass samples, and that alkali metal elements may be concentrated in the coagulated surface layer. However, no difference was observed in the Na K-edge XANES spectra between the coagulated surface layer and the cut surface, and no difference was observed in the Si K-edge XANES spectra between the solidified surface and the inside of glass samples. In addition, the Ce L$$_{3}$$-edge XANES spectra confirmed that the Ce valence in the surface layer of coagulated glass samples were oxidized compared to the inside of glass samples.

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 3 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2023-004, 45 Pages, 2023/09

JAEA-Research-2023-004.pdf:6.07MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. To understand the chemical stability of simulated waste glasses, XANES spectra of B K-edge, Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge were measured on the glass surface exposed to the leachate. As a result, it was found that the glass surface exposed to the leachate was changed and it was difficult to obtain a clear XANES spectrum. From the B K-edge XANES spectra on glass surfaces exposed to the leachate, an increase in three-coordination of B-O (BO$$_{3}$$) and a decrease in four-coordination of B-O (BO$$_{4}$$) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge show that as the exposure time in the leachate increases, the Cs present on the glass surface dissolves into the leachate. The XANES spectra of Si K-edge were measured on simulated waste glass surfaces before immersion, and it was confirmed that the change in XANES spectra given by Na$$_{2}$$O concentration had a larger effect than the waste component concentration.

Journal Articles

Soft X-ray absorption spectra of ilmenite family

Agui, Akane; Mizumaki, Masaichiro*; Saito, Yuji; Matsushita, Tomohiro*; Nakatani, Takeshi*; Fukaya, Atsuko*; Torikai, Eiko*

Journal of Synchrotron Radiation, 8(2), p.907 - 909, 2001/03

 Times Cited Count:10 Percentile:51.38(Instruments & Instrumentation)

no abstracts in English

Oral presentation

Basic research programs of vitrification technology for waste volume reduction, 129; Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region

Nagai, Takayuki; Okamoto, Yoshihiro; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

no journal, , 

no abstracts in English

Oral presentation

Structural investigation of simulated radioactive waste glasses by using XAFS measurement

Nagai, Takayuki; Okamoto, Yoshihiro; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

no journal, , 

no abstracts in English

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