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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.
Okamoto, Yoshihiro; Shiwaku, Hideaki; Shimamura, Keisuke*; Kobayashi, Hidekazu; Nagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
Journal of Nuclear Materials, 570, p.153962_1 - 153962_13, 2022/11
Simulated nuclear waste glass samples containing phosphorus, which increase the solubility of molybdenum, were prepared and analyzed using synchrotron X-ray Absorption Fine Structure (XAFS) analysis for some constituent elements and Raman spectroscopic analysis of their complex structure. Changes in local structure and chemical state due to different phosphorus additions and waste loading rates were systematically studied. Consequently, no crystalline phase due to the molybdate compound was observed even at a maximum waste content of 30 wt% (corresponding to 1.87 mol% MoO
). Oxidation proceeded when the waste-loading rate was increased, whereas the reduction proceeded when phosphorus was added. In some cases, the effects of oxidation and reduction were offset. The local structure around specific elements can be classified as follows; Zn that is affected mainly by the waste-loading rate, Ce that is affected by both the waste-loading rate and phosphorus addition, and Zr element that is not affected by either of them. From the comparison between the analytical results of Mo and other elements, it was considered that the added phosphorus exists as a free PO
structural unit and may deprive the alkali metal coordinated to the molybdate ion.
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.
Okamoto, Yoshihiro; Kobayashi, Hidekazu; Shiwaku, Hideaki; Sasage, Kenichi; Hatakeyama, Kiyoshi*; Nagai, Takayuki
Journal of Non-Crystalline Solids, 551, p.120393_1 - 120393_8, 2021/01
Times Cited Count：5 Percentile：30.89(Materials Science, Ceramics)The chemical state of ruthenium in simulated iron phosphate radioactive waste glass was investigated by conventional X-ray absorption fine structure (XAFS) and imaging XAFS analyses. The EXAFS analysis suggested that ruthenium was contained as glass phase when content of the waste components was less than 10wt.% in 30 mol%FeO-PO base glass. In other samples, crystalline RuO was predominant. According to the imaging XAFS analysis, RuO particles in all samples had length smaller than 50
m. Aggregations of RuO, which are found in nuclear waste borosilicate glass, were not seen in any of the iron phosphate glass samples.
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; 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; 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.
Saito, Shigeru; Fukaya, Kiyoshi*; Ishiyama, Shintaro; Sato, Ikuo*; Kusuhashi, Mikio*; Hatakeyama, Tsuyoshi*; Takahashi, Heishichiro*; Kikuchi, Mitsuru
JAERI-Tech 2002-047, 51 Pages, 2002/05
JAERI-Tech-2002-047.pdf:3.42MB
no abstracts in English
Saito, Shigeru; Fukaya, Kiyoshi; Ishiyama, Shintaro; Eto, Motokuni; Sato, Ikuo*; Kusuhashi, Mikio*; Hatakeyama, Tsuyoshi*; Takahashi, Heishichiro*; Kikuchi, Mitsuru
Journal of Nuclear Materials, 283-287(Part1), p.593 - 596, 2000/12
Times Cited Count：1 Percentile：12.1(Materials Science, Multidisciplinary)no abstracts in English
Saito, Shigeru; Fukaya, Kiyoshi; Ishiyama, Shintaro; Sato, Ikuo*; Kusuhashi, Mikio*; Hatakeyama, Tsuyoshi*; Takahashi, Heishichiro*; Kikuchi, Mitsuru
JAERI-Tech 2000-047, 64 Pages, 2000/08
JAERI-Tech-2000-047.pdf:6.05MB
no abstracts in English
Ishiyama, Shintaro; Fukaya, Kiyoshi; Eto, Motokuni; Kikuchi, Mitsuru; Sato, Ikuo*; Kusuhashi, Mikio*; Hatakeyama, Tsuyoshi*; Takahashi, Heishichiro*
Nihon Genshiryoku Gakkai-Shi, 42(2), p.116 - 123, 2000/02
Times Cited Count：2 Percentile：19.44(Nuclear Science & Technology)no abstracts in English
Saito, Shigeru; Fukaya, Kiyoshi; Ishiyama, Shintaro; Eto, Motokuni; Sato, Ikuo*; Kusuhashi, Mikio*; Hatakeyama, Tsuyoshi*; Takahashi, Heishichiro*; Kikuchi, Mitsuru
JAERI-Tech 99-076, p.53 - 0, 1999/10
no abstracts in English
Nagai, Takayuki; Nishizawa, Daiji; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Seki, Katsumi*; Oyama, Koichi; Kano, Shigeru
no journal, ,
no abstracts in English
Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
no journal, ,
no abstracts in English
particles in borosilicate glass meltsNagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Seki, Katsumi*
no journal, ,
no abstracts in English
Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
no journal, ,
no abstracts in English
Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
no journal, ,
no abstracts in English
Nagai, Takayuki; Kobayashi, Hidekazu; Hatakeyama, Kiyoshi*; Sato, Seiichi*; Okamoto, Yoshihiro
no journal, ,
no abstracts in English
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Seki, Katsumi*
no journal, ,
no abstracts in English
