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Journal Articles

Structural change by phosphorus addition to borosilicate glass containing simulated waste components

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$$_3$$). 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$$_4$$ structural unit and may deprive the alkali metal coordinated to the molybdate ion.

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 2 (Joint research)

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$$_{5}$$, M$$_{4}$$-edge XANES spectra disappeared and the Fe L$$_{3}$$, L$$_{2}$$-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 Na$$_{2}$$O content were measured, and following was confirmed. (1) As the Na$$_{2}$$O 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 Na$$_{2}$$O content in glass frits was about 7wt%.

JAEA Reports

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

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 Na$$_{2}$$O 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 Na$$_{2}$$O 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.

JAEA Reports

Structural investigation of simulated waste glass samples by using XAFS measurement in soft X-ray region (Joint research)

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$$^{3}$$ structure (BO$$_{4}$$) tends to increase with increasing Na$$_{2}$$O 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$$^{3}$$ structure (BO$$_{4}$$) 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.

JAEA Reports

XAFS measurement of simulated waste glass samples (Joint research)

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.

JAEA Reports

Investigation of simulated waste glass samples prepared from borosilicate glass frit including vanadium

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.

Journal Articles

Chemical state analysis of rhodium in simulated waste glass by synchrotron-radiation-based XAFS and imaging XAFS techniques

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Inose, Takehiko*; Sato, Seiichi*

Nihon Genshiryoku Gakkai Wabun Rombunshi, 16(4), p.180 - 190, 2017/12

X-ray absorption fine structure (XAFS) and imaging XAFS analyses were performed to elucidate chemical state of rhodium in the simulated waste glass. The chemical forms of Rh in the glass were evaluated to be 84% RhO$$_{2}$$ and 16% metal/alloy as the result of linear combination analysis of EXAFS data. According to the imaging XAFS analysis, the chemical form of Rh which was located together with Ru was mainly oxide (RhO$$_{2}$$). It suggests that stable (Ru,Rh)O$$_{2}$$ solid solution exists in the simulated glass. On the other hand, that of Rh of which distribution did not accord with Ru in the glass was mainly metallic. In the case of metallic Rh in the glass, it tended to become an aggregation form. It can be concluded that the chemical state of Rh was much affected by the existence and distribution of Ru element.

Oral presentation

Investigation of borosilicate glass containing alkali and rare-earth by Raman spectroscopy

Nagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Nishizawa, Daiji; Oyama, Koichi; Kobayashi, Hidekazu; Yamashita, Teruo; Amamoto, Ippei

no journal, , 

Raman spectrometry was performed for the borosilicate glass samples which added alkali oxides or rare-earth oxides, and the influence of the Raman spectrum of the glass sample by addition of their oxides was evaluated.

Oral presentation

Elemental analysis of simulated waste glass by laser ablation ICP-AES, 1; Optimizing of YAG-5HG laser irradiation conditions and examples of elemental analysis

Nishizawa, Daiji; Inose, Takehiko*; Yamakawa, Atsushi*; Oyama, Koichi; Nagai, Takayuki

no journal, , 

no abstracts in English

Oral presentation

Elemental analysis of simulated waste glass by laser ablation ICP-AES, 2; Comparison of LA method with solution method and application to elemental analysis of simulated waste glass

Inose, Takehiko*; Nishizawa, Daiji; Yamakawa, Atsushi*; Oyama, Koichi; Nagai, Takayuki

no journal, , 

no abstracts in English

Oral presentation

Examination of cyclic voltammetry of molten borosilicate glass

Nagai, Takayuki; Nishizawa, Daiji; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Seki, Katsumi*; Oyama, Koichi; Kano, Shigeru

no journal, , 

no abstracts in English

Oral presentation

Investigation of the chemical form of ruthenium compounds in the vitrification process, 1; Synthetic experiments of sodium ruthenates using ruthenium and sodium nitrates

Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

no journal, , 

no abstracts in English

Oral presentation

Oral presentation

Elemental analysis of simulated waste glass by laser ablation ICP-AES, 4; Verification of quantitative analysis of various elements in simulated waste glass

Inose, Takehiko*; Nishizawa, Daiji; Oyama, Koichi; Miyauchi, Atsushi; Nagai, Takayuki

no journal, , 

no abstracts in English

Oral presentation

Redox behavior of RuO$$_{2}$$ particles in borosilicate glass melts

Nagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Seki, Katsumi*

no journal, , 

no abstracts in English

Oral presentation

Investigation of the chemical form of ruthenium compounds in the vitrification process, 2; Reactions of sodium ruthenates and raw materials for vitrification such as SiO$$_{2}$$

Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

no journal, , 

no abstracts in English

Oral presentation

Elemental analysis of simulated waste glass by laser ablation ICP-AES, 5; Application of LA-ICP-AES for inactive mock-up test of vitrification process

Inose, Takehiko*; Nishizawa, Daiji*; Miyauchi, Atsushi; Oyama, Koichi; Yamakawa, Atsushi*; Nagai, Takayuki

no journal, , 

no abstracts in English

Oral presentation

Investigation of the chemical form of ruthenium compounds in the vitrification process, 3; Reactions of lanthanide nitrates and ruthenium nitrates included in a liquid waste

Nagai, Takayuki; Sasage, Kenichi; Oyama, Koichi; Sato, Nobuaki*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

no journal, , 

no abstracts in English

Oral presentation

Application of laser ablation ICP-AES for inactive mock-up test of vitrification process

Oyama, Koichi; Inose, Takehiko*; Miyauchi, Atsushi; Nishizawa, Daiji*; Nagai, Takayuki

no journal, , 

no abstracts in English

Oral presentation

Elemental analysis of borosilicate glass by laser ablation ICP-AES

Inose, Takehiko*; Oyama, Koichi; Miyauchi, Atsushi; Nishizawa, Daiji*; Nagai, Takayuki

no journal, , 

no abstracts in English

30 (Records 1-20 displayed on this page)