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

http://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2018/KURNS_Progress_Report2018_web.pdf

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.

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.

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

http://pfwww.kek.jp/acr/2018pdf/u_reports/pf18b0060.pdf

no abstracts in English

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.

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.

Electronic structure and magnetic properties of the half-metallic ferrimagnet MnVAl 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

https://doi.org/10.1103/PhysRevB.97.035143

We have studied the electronic structure of ferrimagnetic MnVAl 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 XAS and XMCD spectra are reproduced by spectral simulations based on density-functional theory, indicating the itinerant character of the Mn 3 states. On the other hand, the V 3 electrons are rather localized since the ionic model can qualitatively explain the V L XAS and XMCD spectra. This picture is consistent with local excitations revealed by the V L RIXS.

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

https://doi.org/10.3327/taesj.J16.024

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 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). It suggests that stable (Ru,Rh)O 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.

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

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 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 1200C, so it would be possible to acquire excellent data by improving the shapes of the sample cell.

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

http://pfwww.kek.jp/acr/2015pdf/part_b/pf15b0070.pdf

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.