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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.

Journal Articles

Structural change of borosilicate glass by neutron irradiation

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.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

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

JAEA Reports

Synchrotron radiation based XAFS analysis of the simulated nuclear waste glass samples prepared by bottom drain test in the full-scale mock-up melter (KMOC) (Contract research)

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Kano, Shigeru; Himeno, Haruyuki*; Kobayashi, Hiroshi*; Nakatani, Mikio*

JAEA-Research 2018-013, 18 Pages, 2019/03

JAEA-Research-2018-013.pdf:1.98MB

The chemical state and local structure of some elements in the simulated nuclear waste glass samples (20 batches) prepared by bottom drain test in the full scale mock-up tests using KMOC melter were investigated by synchrotron radiation based X-ray absorption fine structure (XAFS) analysis. As a result of the analysis of cerium element, it was confirmed that the oxidation proceeds gently as the batch advanced. For manganese, iron, and zinc, there was almost no difference between batches, which seemed to be stabilized by getting into the frame structure of the borosilicate glass. There were no elements that seemed to be clearly crystalline except for platinum group elements. Remarkable precipitation was hardly observed in zirconium and molybdenum with the imaging analysis.

Journal Articles

Contribution to upgrade of vitrification technology by synchrotron radiation analysis; From Chemical state analysis of waste glass to development of structural analysis to prove soundness

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki

Yoyuen Oyobi Koon Kogaku, 62(1), p.11 - 17, 2019/01

The vitrified radioactive waste is a multicomponent material containing many kinds of elements. Synchrotron radiation XAFS with element selectivity is suitable for analysis of elements in the waste. From the XAFS analysis, the chemical state and the local structure of each element were clarified. Imaging XAFS technique was used as an analysis based on element distribution in the glass. The imaging XAFS is effective for analysis of elements that are less soluble in the glass like molybdenum and platinum group elements. It was clarified from the simultaneous imaging XAFS analyses of multiple elements that the chemical form of rhodium is strongly dominated by the distribution correlation with ruthenium. We proposed multi - scale structural analyses with wide angle scattering, PDF analysis, small angle scattering in order to evaluate the soundness of the vitrified waste.

Journal Articles

Evaluation of uranium chemical state in borosilicate glasses by using XAFS measurement

Nagai, Takayuki; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*

Photon Factory Activity Report 2018 (Internet), 2 Pages, 2019/00

no abstracts in English

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.

JAEA Reports

XAFS measurement of simulated waste glass samples prepared from borosilicate glass frit including phosphorus pentaoxide (Joint research)

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.

Journal Articles

Selection of borosilicate glass composition for neutron irradiation test

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.

Journal Articles

Synchrotron radiation based X-ray absorption study for upgrade of nuclear waste vitrification technique

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki

Hoshako, 31(4), p.274 - 280, 2018/07

As a method for disposal of nuclear waste, the use of vitrification technique is very promising. In this technique, many kinds of elements should be involved stably in the glass and chemical state of these elements in the glass must be confirmed in order to guarantee stability of the glass. We have used synchrotron based X-ray absorption fine structure (XAFS) technique, in which the element selectivity is utilized, to obtain the chemical state of each element in many kinds of simulated glass samples. In addition, imaging XAFS technique has been used to clarify correlation between constituent elements. We are going to contribute to research and development of the vitrification technique by using synchrotron radiation based XAFS analyses. In this article, we introduce results of the high energy XAFS of high temperature slag samples, the imaging study of high temperature borosilicate glass samples and the imaging XAFS analysis of platinum group metals in the borosilicate glass samples.

Journal Articles

Investigation of chemical state of uranium included in glass

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

Journal Articles

Electronic structure and magnetic properties of the half-metallic ferrimagnet Mn$$_{2}$$VAl probed by soft X-ray spectroscopies

Nagai, Kodai*; Fujiwara, Hidenori*; Aratani, Hidekazu*; Fujioka, Shuhei*; Yomosa, Hiroshi*; Nakatani, Yasuhiro*; Kiss, Takayuki*; Sekiyama, Akira*; Kuroda, Fumiaki*; Fujii, Hitoshi*; et al.

Physical Review B, 97(3), p.035143_1 - 035143_8, 2018/01

AA2017-0644.pdf:1.01MB

 Times Cited Count:4 Percentile:54.91(Materials Science, Multidisciplinary)

We have studied the electronic structure of ferrimagnetic Mn$$_{2}$$VAl single crystals by means of soft X-ray absorption spectroscopy (XAS), X-ray absorption magnetic circular dichroism (XMCD), and resonant soft X-ray inelastic scattering (RIXS). We have successfully observed the XMCD signals for all the constituent elements. The Mn L$$_{2,3}$$ XAS and XMCD spectra are reproduced by spectral simulations based on density-functional theory, indicating the itinerant character of the Mn 3$$d$$ states. On the other hand, the V 3$$d$$ electrons are rather localized since the ionic model can qualitatively explain the V L$$_{2,3}$$ XAS and XMCD spectra. This picture is consistent with local $$dd$$ excitations revealed by the V L$$_{3}$$ RIXS.

Journal Articles

Evaluation of uranium chemical state in borosilicate glasses by using XAFS measurement

Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*

Photon Factory Activity Report 2017, 2 Pages, 2018/00

no abstracts in English

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*

Nippon 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.

JAEA Reports

XAFS measurement of simulated waste borosilicate glass samples (Joint research)

Nagai, Takayuki; Kobayashi, Hidekazu; Sasage, Kenichi; Ayame, Yasuo; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*

JAEA-Research 2017-005, 54 Pages, 2017/06

JAEA-Research-2017-005.pdf:16.17MB

Addition of radioactive waste to a borosilicate frit affects the local structures of boron (B) and waste elements in a waste glass. Synchrotron XAFS measurement was applied to investigate the local structural changes by using simulated waste borosilicate glass samples. Following results were obtained by the B K-edge XAFS analysis. It was confirmed that B K-edge XAFS analysis enables us to discriminate sp$$^{2}$$ type boron (BO$$_{3}$$) from sp$$^{3}$$ type boron (BO$$_{4}$$). Addition of waste elements to a glass frit increases the percentage of BO$$_{3}$$ and decreases that of BO$$_{4}$$. By decreasing the SiO$$_{2}$$/Al$$_{2}$$O$$_{3}$$ ratio or increasing the (SiO$$_{2}$$+B$$_{2}$$O$$_{3}$$)/Al$$_{2}$$O$$_{3}$$ ratio in the glass composition, the BO$$_{3}$$ percentage increases and the BO$$_{4}$$ percentage decreases. Addition of P$$_{2}$$O$$_{5}$$ decreases the BO$$_{3}$$ percentage and increases the BO$$_{4}$$ percentage. Following results were obtained from XAFS measurement of the waste elements. Cerium (Ce) valence is more reduced with the increase of the B$$_{2}$$O$$_{3}$$ content. Addition of P$$_{2}$$O$$_{5}$$ has a tendency to reduce the Ce valence and to enhance deposition of Zr oxide. Deposition of ruthenium compounds separated from glass phase can not be improved by changing the B$$_{2}$$O$$_{3}$$ content. This study was performed as a part of the project, "Improvement of vitrification process of high-level radioactive liquid wastes" on the foundation business of the Agency for Natural Resources and Energy.

Journal Articles

Chemical behavior of platinum group compounds in the vitrification process condition

Nagai, Takayuki; Akiyama, Daisuke*; Sato, Nobuaki*; Sasage, Kenichi

Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten Kenkyu Seika Hokokusho (Heisei-28-Nendo) (CD-ROM), 1 Pages, 2017/03

no abstracts in English

Journal Articles

High temperature Fe-K edge XANES spectrum measurement in preparing iron phosphate glass frit by using hot thermo-couple heating system

Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro

Photon Factory Activity Report 2016, 2 Pages, 2017/00

To estimate the valence state of iron in the preparation process of iron phosphate glass frit, mixtures of ferric oxide and phosphoric acid was heated and XANES spectra of Fe-K edge was measured in this study. This report described the situation of high temperature XAFS measurement and results of this study.

JAEA Reports

XAFS measurement of simulated waste glass samples (Borosilicate glass including vanadium)

Nagai, Takayuki; Kobayashi, Hidekazu; Sasage, Kenichi; Ayame, Yasuo; Okamoto, Yoshihiro; Shiwaku, Hideaki; Matsuura, Haruaki*; Uchiyama, Takafumi*; Okada, Yukiko*; Nezu, Atsushi*; et al.

JAEA-Research 2016-015, 52 Pages, 2016/11

JAEA-Research-2016-015.pdf:37.48MB

The local structure of waste elements in simulated waste glasses including V was estimated by using synchrotron XAFS measurement in this study. The results are as follows. (1) V has a high possibility which exists in the glass phase in the case of frit, and V can regard both samples as stable 4 coordination structure. (2) Zn, Ce, Nd, Zr, and Mo exist in the glass phase, and the difference is admitted by the percentage of Ce(III) and Ce(IV) by the composition. (3) Ru is separated from the glass phase as RuO$$_{2}$$ crystalline, both of metal and oxide exist in Rh, and Pd is separated out as metal. (4) It was confirmed that the regularity of the local structure of Zr and Mo in the molten glasses retreats as a result of the XAFS measurement at high temperature. (5) The XAFS measurement of molten glasses were performed at 1200$$^{circ}$$C, so it would be possible to acquire excellent data by improving the shapes of the sample cell.

Journal Articles

Investigation of ruthenium compounds in the vitrification process condition

Nagai, Takayuki; Sato, Nobuaki*; Sasage, Kenichi

Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten Kenkyu Seika Hokokusho (Heisei-27-Nendo) (CD-ROM), 2 Pages, 2016/03

no abstracts in English

Journal Articles

Influence of borosilicate glass by neutron irradiation

Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Uehara, Akihiro*; Fujii, Toshiyuki*

Photon Factory Activity Report 2015, Part B, 2 Pages, 2016/00

To investigate the characterization damage of a borosilicate glass by a neutron irradiation, the glass sample after neutron irradiation was estimated by using the Raman spectrophotometry and the synchrotron XAFS measurement. As a result, we confirmed that the Si-O bridge structure of a borosilicate glass and the containing element valence in the glass were changed by the neutron irradiation.

167 (Records 1-20 displayed on this page)