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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.
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.
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.
Mitsui, Seiichiro
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.
Okamoto, Yoshihiro; Nagai, Takayuki; Kaneko, Koji; Motokawa, Ryuhei; Haga, Yoshinori; Yamanaka, Keisuke*; Ota, Toshiaki*
2017-Nendo Seika Kokaigata Riyo Seika Hokokusho (Ritsumeikan Daigaku SR Senta), p.33 - 36, 2018/00
The high-level radioactive waste solution which generated from a spent nuclear fuel reprocessing process are mixed with a borosilicate glass frit in a vitrification process, and a chemical stable glass solidified body is produced. To understand local structure of light elements included in a glass solidified body, we carried out a B K-edge XANES measurement of raw glass frits and simulated radioactive waste glasses. As a result of this estimation of boron local structure in glass samples, it was found that the sp
type boron (BO
) percentage increases and the sp
type (BO
) percentage by increasing the sodium content in glass frits.
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
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.
Amamoto, Ippei
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.
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 260,000
700,000 years depending on models. These results imply more strong isolation capability of the waste glass than that estimated in the overall safety report.
Okamoto, Yoshihiro; Shiwaku, Hideaki; Nakada, Masami; Komamine, Satoshi*; Ochi, Eiji*; Akabori, Mitsuo
Journal of Nuclear Materials, 471, p.110 - 115, 2016/02
Times Cited Count：6 Percentile：49.29(Materials Science, Multidisciplinary)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 1
10
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.
Tsuzuki, Tatsuya*; Mitamura, Naoki*; Amamoto, Ippei
Shakai, Kankyo Hokokusho 2014 (Internet), p.6 - 7, 2014/10
no abstracts in English
Inagaki, Yaohiro*; Mitsui, Seiichiro*; Makino, Hitoshi*; Ishiguro, Katsuhiko*; Kamei, Gento*; Kawamura, Kazuhiro*; Maeda, Toshikatsu; Ueno, Kenichi*; Bamba, Tsunetaka*; Yui, Mikazu*
Genshiryoku Bakkuendo Kenkyu, 10(1-2), p.69 - 84, 2004/03
no abstracts in English
; ; Shimizu, Kazuhiko; Miyahara, Kaname; ; Seo, Toshihiro; Fujita, Tomoo
JNC TN1410 2000-008, 100 Pages, 2000/10
JNC-TN1410-2000-008.pdf:4.23MB
no abstracts in English
*
JNC TJ8400 2000-017, 74 Pages, 2000/02
JNC-TJ8400-2000-017.pdf:1.71MB
The report concerns the improvement of the method measuring thermal conductivity of buffer materials using a thermistor probe and the measurement of thermal conductivity of compacted bentonites and mixtures of bentonite and silica sand using the proposed method measuring thermophysical properties. The method measuring thermal conductivity is improved in accuracy and the apparatus is improved so as to measure easily with more short time. The calculated values of the conventional correlations predicting thermal conductivity of bentonite and mixture were compared with the exising and present data of thermal conductivity of bentonites and mixtures. The correlation proposed by Sakashita and Kumada can predict the best fitted values with the data of the bentonites and Fricke and Bruggeman correlations are fitted with the data for the mixtures with practical accuracy.
*; *; Tanai, Kenji
JNC TN8400 99-048, 85 Pages, 1999/11
This paper reports the results of design analysis and trial manufacturing of full-scale titanium-carbon steel composite overpacks. The overpack is one of the key components of the engineered barrier system, hence, it is necessary to confirm the applicability of current technique in their manufacture. The required thickness was calculated according to mechanical resistance analysis, based on models used in current nuclear facilities. The Adequacy of the calculated dimensions was confirmed by finite-element methods. To investigate the necessity of a radiation shielding function of the overpack, the irradiation from vitrified waste has been calculated. As a result, it was shown that shielding on handling and transport equipment is a more reasonable and practical approach than to increase thickness of overpack to attain a self-shielding capability. After the above investigation, trial manufacturing of full-scale model of titanium-carbon steel composite overpack has been carried out. For corrosion-resistant material, ASTM Grade-2 titanium was selected. The titanium layer was bonded individually to a cylindrical shell and flat cover plates (top and bottom) made of carbon steel. For the cylindrical shell portion, a cylindrically formed titanium layer was fitted to the inner carbon steel vessel by shrinkage. For the flat cover plates (top and bottom), titanium plate material was coated by explosive bonding. Electron beam welding and gas metal arc welding were combined to weld of the cover plates to the body. No significant failure was evident from inspections of the fabrication process, and the applicability of current technology for manufacturing titanium-carbon steel composite overpack was confirmed. Future research and development items regarding titanium-carbon steel composite overpacks are also discussed.
Bamba, Tsunetaka; *; Tamura, Yukito; *; Yonezawa, Chushiro; Carter, P.*
Analytical Sciences, 14, p.389 - 394, 1998/04
Times Cited Count：11 Percentile：38.79(Chemistry, Analytical)no abstracts in English
Department of Hot Laboratories
JAERI-Review 97-001, 118 Pages, 1997/02
JAERI-Review-97-001.pdf:4.36MB
no abstracts in English
