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
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; 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), 20181080_1 Pages, 2019/06
no abstracts in English
Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Kano, Shigeru; Himeno, Haruyuki*; Kobayashi, Hiroshi*; Nakatani, Mikio*
JAEA-Research 2018-013, 18 Pages, 2019/03
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.
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.
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
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
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.
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.
Maizo Bunkazai Nyusu, (171), p.10 - 17, 2018/03
As part of research and development of geological disposal, "natural analogues" have been applied to validate concept of models and evaluation methodologies for performance assessment. By introducing domestic and overseas research results on natural analogues, this paper presents how we have utilized knowledge of excavated archaeological artifacts for geological disposal studies.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*
Photon Factory Activity Report 2017, 2 Pages, 2018/00
no abstracts in English
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 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.
Journal of the Society of Inorganic Materials, Japan, 24(391), p.393 - 401, 2017/11
Glass is a non-crystalline solid, as such, it is relatively easy to change its composition to control its characteristics. The borosilicate glass, which is produced by the addition of boron oxide into sodium-lime glass, possesses excellent heat-resistant properties and mechanical strength. It has a wide variety of uses. The borosilicate glass is applied as the vitrified medium for radioactive wastes to immobilize and stabilize them for long term. The glass form which is loaded with high-level radioactive waste is called the vitrified waste. This paper classified the radioactive waste and describes treatment and production methods of vitrified waste, its characteristics, disposal method and also introduces alternative vitrified medium.
Nagai, Takayuki; Kobayashi, Hidekazu; Sasage, Kenichi; Ayame, Yasuo; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*
JAEA-Research 2017-005, 54 Pages, 2017/06
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 type boron (BO) from sp type boron (BO). Addition of waste elements to a glass frit increases the percentage of BO and decreases that of BO. By decreasing the SiO/AlO ratio or increasing the (SiO+BO)/AlO ratio in the glass composition, the BO percentage increases and the BO percentage decreases. Addition of PO decreases the BO percentage and increases the BO percentage. Following results were obtained from XAFS measurement of the waste elements. Cerium (Ce) valence is more reduced with the increase of the BO content. Addition of PO 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 BO 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.
Oe, Toshiaki*; Wakasugi, Keiichiro
Genshiryoku Bakkuendo Kenkyu (CD-ROM), 24(1), p.27 - 32, 2017/06
The report estimates the life-time of the waste glass dissolution in the geologic disposal environment. The overall safety report on the geologic disposal in Japan showed very short life-time of approximately 70,000 years under pessimistic assumptions ignoring the temperature decrease due to radioactive decay and dissolution rate reduction due to surface shrinkage. These factors are physically established phenomena and may not be excluded. The dissolution models including these factors of temperature and surface area decreases are discussed and used for re-evaluation. Three fracture models are presented for evaluating the surface area decreases; a single plate, monotonic spheres, spheres having power-law distribution. All models have the same initial volume as the waste glass block for mass conservation and the total surface areas are 10 times higher than the initial pristine block because of the fracture development during production. The results indicate the retention time of 50% of initial mass exceed 100,000 years even by different fracture models and the dissolution life-times are expected for 260,000700,000 years depending on models. These results imply more strong isolation capability of the waste glass than that estimated in the overall safety report.
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
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
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.
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
Okamoto, Yoshihiro; Shiwaku, Hideaki; Nakada, Masami; Komamine, Satoshi*; Ochi, Eiji*; Akabori, Mitsuo
Journal of Nuclear Materials, 471, p.110 - 115, 2016/02
Extended X-ray Absorption Fine Structure (EXAFS) analyses were performed to evaluate REDOX (REDuction and OXidation) state of platinoid elements in simulated high-level nuclear waste glass samples prepared under different conditions of temperature and atmosphere. At first, EXAFS functions were compared with those of standard materials such as RuO. Then structural parameters were obtained from a curve fitting analysis. In addition, a fitting analysis used a linear combination of the two standard EXAFS functions of a given elements metal and oxide was applied to determine ratio of metal/oxide in the simulated glass. The redox state of Ru was successfully evaluated from the linear combination fitting results of EXAFS functions. The ratio of metal increased at more reducing atmosphere and at higher temperatures. Chemical form of rhodium oxide in the simulated glass samples was RhO unlike expected RhO. It can be estimated rhodium behaves according with ruthenium when the chemical form is oxide.
Goto, Takahiro*; Mitsui, Seiichiro; Takase, Hiroyasu*; Kurosawa, Susumu*; Inagaki, Manabu*; Shibata, Masahiro; Ishiguro, Katsuhiko*
MRS Advances (Internet), 1(63-64), p.4239 - 4245, 2016/00
NUMO and JAEA have conducted a joint research since FY2011, which is designed to enhance the methodology of repository design and performance assessment in preliminary investigation stage for deep geological disposal of radioactive waste. As a part of this joint research, we have been developing glass dissolution models which consider various processes in EBS, such as precipitation of Fe-silicates associated with iron overpack corrosion, and Si transport through corrosion products in the cracked overpack. The objectives of the modeling work are to evaluate relative importance of relevant processes and to identify further R&D issues towards development of a convincing safety case. Sensitivity analyses suggested that predicted glass dissolution time ranges from 110 to 110 years or more due to uncertainties in the current understanding of the key processes, namely precipitation of Fe-silicates and transport characteristics of the altered glass layer.
Tokai Reprocessing Technology Development Center
JAEA-Evaluation 2015-012, 83 Pages, 2015/12
Japan Atomic Energy Agency (hereafter referred as "JAEA") consulted the "Evaluation Committee of Research and Development Activities for Fast Reactor Cycle" to assess the issue on "Research and Development on Reprocessing of Nuclear Fuel Materials" conducted by JAEA during the period from FY2010 to FY2014. In response to the JAEA's request, the committee assessed the R&D programs and the activities of JAEA related to the issue and concluded the mission was accomplished. This evaluation was performed based on the "General guideline for the evaluation of government R&D activities", the "Guideline for evaluation of R&D in Ministry of Education, Culture, Sports, Science and Technology (MEXT)" and the "Operational rule for evaluation of R&D activities" by JAEA.
Tsuzuki, Tatsuya*; Mitamura, Naoki*; Amamoto, Ippei
Shakai, Kankyo Hokokusho 2014 (Internet), p.6 - 7, 2014/10
no abstracts in English