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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
, L
-edge, and Cs M
, M
-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) and a decrease in four-coordination of B-O (BO) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L, L-edge, and Cs M, M-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 NaO concentration had a larger effect than the waste component concentration.
Nagai, Takayuki
JAEA-Research 2022-014, 84 Pages, 2023/02
JAEA-Research-2022-014.pdf:22.26MB
Most of the simulated waste glasses used for physical property evaluation are processed into a shape suitable for the measurement method from glass gob obtained by slowly cooling molten glass to room temperature. However, the actual vitrified waste glass material is obtained by cooling and being coagulated the glass drained from the bottom of glass melter into the canister. In this study, Raman spectroscopy was performed on the coagulated surface of molten simulated waste glass in the depth direction to evaluate the state of the Si-O bridging structure near the coagulated glass surface. The Raman spectra measured from the surface to the depth direction near the surface of the glasses produced by several melting and coagulation conditions of molten simulated waste glass cullet in the air atmosphere, and it was confirmed that there were changes in these spectra. On the other hand, the raw material glass cullet and the surface of the glass solidified in argon gas atmosphere showed little change in the spectrum in the depth direction, and the Si-O bridging structure near the glass surface was similar. It was also confirmed that the spectrum change in the depth direction measurement was small for the cut surface of the glass, and that the change in the spectrum for the broken glass fracture surface was also small. For glasses with a large change in Raman spectra in the depth direction near the coagulated surface, the molten glass was cooled from the molten state to room temperature in a muffle furnace with air atmosphere. That is, the magnitude of the spectral change with respect to the depth direction depends on the time from the molten state to coagulation. In order to confirm the reason why the number of bridging oxygen in the Si-O bridging structure is small on the coagulated surface of glass, the XANES spectra of Si-K edge and Ce-L3 edge were measured by XAFS on the coagulated surface and the cutting face. As a result, the Si-K edge peak on the coagulated surface is
Nagai, Takayuki; Tone, Masaya; Katsuoka, Nanako; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*
Photon Factory Activity Report 2022 (Internet), 3 Pages, 2023/00
no abstracts in English
Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
JAEA-Research 2022-008, 37 Pages, 2022/10
JAEA-Research-2022-008.pdf:5.27MB
The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and 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. Following results were obtained by XAFS measurements of simulated waste glass surfaces after immersion test to investigate the long chemical stability. (1) As the leaching time of glass samples in immersion test passed, the Cs M, M-edge XANES spectra disappeared and the Fe L, L-edge spectra changed. (2) A new compound was formed on the sample surface after the immersion test, and these changes in the surface state were confirmed by Raman spectroscopy. However, it became difficult to obtain a clear B K-edge XANES spectrum by forming a compound on glass surfaces. The Si K-edge XANES spectra of borosilicate glass frits with different NaO content were measured, and following was confirmed. (1) As the NaO concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The intensity of the Si K-edge peak is maximum when the NaO content in glass frits was about 7wt%.
Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Ota, Toshiaki*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
JAEA-Research 2021-010, 62 Pages, 2022/01
JAEA-Research-2021-010.pdf:6.05MB
The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the local structure and chemical state regarding boron(B), oxygen(O), silicon(Si) and waste elements of iron(Fe), cesium(Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of prepared glass frit and simulated waste glass samples: (1) The effect of NaO concentration on B-O coordination structure is greater than that of the waste elements concentration. (2) The height of pre-edge by O K-edge spectrum depends on the concentration of first transition elements such as Fe in glass samples. Following results were obtained by XAFS measurements of simulated waste glass samples after immersion test to investigate the long chemical stability. (1) A new compound was formed on the sample surface after the immersion test, and changes in the surface state were confirmed by Raman spectroscopy. (2) Cs on the sample surface after immersion test dissolves into the leaching solution. The Si K-edge XANES spectra of borosilicate glass frits and simulated waste glass samples included lanthanides oxide were measured, and following was confirmed. (1) As the NaO concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The peak height of the K-edge of Si differs depending on the kind of lanthanide.
Nagai, Takayuki; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*; Arima, Tatsumi*
Photon Factory Activity Report 2021 (Internet), 2 Pages, 2022/00
no abstracts in English
Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro
2020-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), 1 Pages, 2021/11
no abstracts in English
Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro
2019-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), P. 20191107_1, 2020/11
no abstracts in English
Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Ota, Toshiaki*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
JAEA-Research 2020-009, 48 Pages, 2020/09
JAEA-Research-2020-009.pdf:4.53MB
The local structure of glass-forming elements and waste elements in waste glass varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the local structure and chemical state regarding boron (B), oxygen (O), and waste elements of cerium (Ce), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of prepared glass frit and simulated waste glass samples: (1) The existence ratio of four coordinate sp
structure (BO) tends to increase with increasing NaO content in glass samples. (2) The height of a pre-edge which appears by K-edge XANES spectrum of O is so high that the Fe content in glass samples. Following results were obtained by XAFS measurements of simulated waste glass samples after immersion test to investigate long chemical stability. (1) The existence ratio of four coordinate sp structure (BO) increases by immersion test. (2) Ce which exists in the surface layer is oxidized by immersion test, and much of Cs in surface layer is lost after leach testing. Even if the glass frit form (fiber cartridge or beads) and manufacturing method were changed and a glass sample of the similar chemical composition was prepared, these observed Raman spectra of samples were different.
Nagai, Takayuki; Okamoto, Yoshihiro; Akiyama, Daisuke*; Uehara, Akihiro*; Fujii, Toshiyuki*; Sekimoto, Shun*
KURNS Progress Report 2019, P. 257, 2020/08
To understand the influence of glass structural change by neutron irradiation and boron isotope composition, glass samples were made from enrichment boric acid reagents and neutron irradiation of those samples was carried out in Pn-2 of KUR. The structural change of glass sample after the irradiation will be estimated in 2020FY. Before neutron irradiation test of glass samples, the Si-O bridging structure difference by boron isotope composition compared by using a Raman spectrometry.
Nagai, Takayuki; Shimoyama, Iwao; Okamoto, Yoshihiro; Akiyama, Daisuke*; Arima, Tatsumi*
Photon Factory Activity Report 2019 (Internet), 3 Pages, 2020/00
no abstracts in English
Nagai, Takayuki; Sasage, Kenichi; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamagishi, Hirona*; Ota, Toshiaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Takahashi, Tomoe*; et al.
JAEA-Research 2019-003, 94 Pages, 2019/09
JAEA-Research-2019-003.pdf:7.92MB
The local structures of glass-forming elements and waste elements would change by the chemical composition of waste glass including those elements. In this study, simulated waste glass samples were prepared from borosilicate glass frit including phosphorus (P) or vanadium (V), and we investigated local structures of boron, sodium, and waste elements in these P glass and V glass samples by using synchrotron XAFS measurements in soft and hard X ray region.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*; Uehara, Akihiro*; Fujii, Toshiyuki*; Sekimoto, Shun*
KURNS Progress Report 2018, P. 105, 2019/08
To understand this structural change of a borosilicate glass by a neutron irradiation in detail, the irradiation test was carried out in KUR in 2017FY. The glass structure was estimated by using Raman spectrometry in 2018FY. Comparing with the Raman spectra of glass samples before and after irradiation, it could be observed the change of peak height of Si-O bridging structure by the irradiation.
Nagai, Takayuki; Akiyama, Daisuke*; Sato, Nobuaki*; Okamoto, Yoshihiro
"Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Danamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (Heisei-30-Nendo) (CD-ROM), P. 20181080_1, 2019/06
no abstracts in English
Nagai, Takayuki; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*
Photon Factory Activity Report 2018 (Internet), 2 Pages, 2019/00
no abstracts in English
Nagai, Takayuki; Okamoto, Yoshihiro; Shiwaku, Hideaki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Hirono, Kazuya*; Homma, Masanobu*; Kobayashi, Hiromi*; Takahashi, Tomoe*; et al.
JAEA-Research 2018-007, 87 Pages, 2018/11
JAEA-Research-2018-007.pdf:61.21MB
To select the chemical composition of a glass frit which can increase the waste content, the simulated waste glass samples prepared from a borosilicate glass frit including vanadium (V) were investigated by using Laser Ablation (LA) ICP-AES analysis, Raman spectrometry, and synchrotron XAFS measurement in this study on foundation business of the Agency for Natural Resources and Energy.
Nagai, Takayuki; Kobayashi, Hidekazu; Shimamura, Keisuke; Oyama, Koichi; Sasage, Kenichi; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*
JAEA-Research 2018-005, 72 Pages, 2018/09
JAEA-Research-2018-005.pdf:28.2MB
Addition of radioactive waste to a borosilicate glass frit affects the local structures of glass-forming elements and waste elements in a waste glass produced in a vitrification process. In this study, simulated waste glass samples were prepared from borosilicate glass frit including phosphorus pentaoxide, and we investigated local structures of sodium (Na), boron (B), and waste elements in these glass samples by using synchrotron XAFS measurements in soft and hard X ray region.
Nagai, Takayuki; Uehara, Akihiro*; Fujii, Toshiyuki*
KURRI Progress Report 2017, P. 128, 2018/08
In this study, to understand the structural change of a borosilicate glass by a neutron irradiation in detail, the neutron irradiation test was carried out for 50 min in the Pn-2 of the Kyoto University Research Reactor (KUR). The structural change of glass sample after the irradiation will be estimated in 2018FY. Before the irradiation test, the glass composition was selected to estimate a structural change accurately by Raman spectrometry and 2 kinds of Li free borosilicate glass for the irradiation test samples were prepared.
Nagai, Takayuki; Akiyama, Daisuke*; Sato, Nobuaki*
Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten Kenkyu Seika Hokokusho (Heisei-29-Nendo) (CD-ROM), 1 Pages, 2018/04
no abstracts in English
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*
Photon Factory Activity Report 2017, 2 Pages, 2018/00
no abstracts in English
