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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
). 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
structural unit and may deprive the alkali metal coordinated to the molybdate ion.
Asahi, Yoshimitsu; Shimamura, Keisuke*; Kobayashi, Hidekazu; Kodaka, Akira
JAEA-Technology 2021-026, 50 Pages, 2022/03
JAEA-Technology-2021-026.pdf:6.29MB
In Tokai Reprocessing Plant, the highly active liquid waste derived from a spent fuel reprocessing is vitrified with a Liquid-Fed Ceramic Melter (LFCM) embedded in Tokai Vitrification Facility (TVF). For an LFCM, the viscosity of melted glass is increased by the deposition of oxidation products of platinum group elements (PGE) and the PGE-containing glass tends to settle to the melter's bottom basin even after draining glass out. Removal of the PGE-containing glass is needed to avoid the Joule heating current from being affected by the glass, it requires time-consuming work to remove. For the early accomplishment of vitrifying the waste, Japan Atomic Energy Agency is planning to replace the current melter with the new one in which the amount of PGE sediments would be reduced. In the past design activities for the next melter, several kinds of shapes in regard to the furnace bottom and the strainer were drawn. Among these designs, the one in which the discharge ratio of PGE-containing glass would be as much as or greater than the current melter and which be able to perform similar operational sequences done in the current melter is selected here. Firstly, an operational sequence to produce one canister of vitrified waste is simulated for three melter designs with a furnace bottom shape, using 3D thermal-hydraulic calculations. The computed temperature distribution and its changes are compared among the candidate structures. After discussions about the technical and structural feasibilities of each design, a cone shape with a 45
slope was selected as the bottom shape of the next melter. Secondly, five strainer designs that fit the bottom shape above mentioned are drawn. For each design, the fluid drag and the discharge ratio of relatively high viscosity fluid resting near the bottom are estimated, using steady or unsteady CFD simulation. By draining silicone oil from acrylic furnace models, it was confirmed experimentally that there are no vortices
Okamoto, Yoshihiro; Kobayashi, Hidekazu; Shiwaku, Hideaki; Sasage, Kenichi; Hatakeyama, Kiyoshi*; Nagai, Takayuki
Journal of Non-Crystalline Solids, 551, p.120393_1 - 120393_8, 2021/01
Times Cited Count：5 Percentile：30.89(Materials Science, Ceramics)The chemical state of ruthenium in simulated iron phosphate radioactive waste glass was investigated by conventional X-ray absorption fine structure (XAFS) and imaging XAFS analyses. The EXAFS analysis suggested that ruthenium was contained as glass phase when content of the waste components was less than 10wt.% in 30 mol%Fe
O
-PO
base glass. In other samples, crystalline RuO was predominant. According to the imaging XAFS analysis, RuO particles in all samples had length smaller than 50
m. Aggregations of RuO, which are found in nuclear waste borosilicate glass, were not seen in any of the iron phosphate glass samples.
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.
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.
Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*
Photon Factory Activity Report 2017, 2 Pages, 2018/00
no abstracts in English
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
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.
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.
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.
Amamoto, Ippei; Kobayashi, Hidekazu; Kitamura, Naoto*; Takebe, Hiromichi*; Mitamura, Naoki*; Tsuzuki, Tatsuya*; Fukayama, Daigen*; Nagano, Yuichi*; Jantzen, T.*; Hack, K.*
Journal of Nuclear Science and Technology, 53(10), p.1467 - 1475, 2016/10
Times Cited Count：3 Percentile：28.28(Nuclear Science & Technology)The iron phosphate glass (IPG) medium is known to be a high-efficiency glass medium, therefore we try to evaluate its applicability to immobilize sludge bearing radioactive nuclides arising from treatment of contaminated water at the stricken Fukushima Daiichi Nuclear Power Plant. For this study, many physical and chemical properties of target materials are necessary to evaluate the behaviours of IPG medium and its waste forms. Inevitably, it will entail the need for many and varied types of experiments to be carried out under high temperature. It is therefore rational to apply appropriate theoretical analysis first so as to reduce the number of experimental run. For this reason, some necessary thermodynamic values for theoretical analysis were estimated by CALPHAD approach followed by making up the calculated phase diagrams. By comparison with experimental results, they were found to be reliable for evaluating the behaviours of IPG medium and its waste forms.
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.
Kobayashi, Masato*; Saito, Masahiko*; Iwatani, Takafumi*; Nakayama, Masashi; Tanai, Kenji; Fujita, Tomoo; Asano, Hidekazu*
JAEA-Research 2015-018, 14 Pages, 2015/12
JAEA-Research-2015-018.pdf:5.43MB
JAEA and RWMC concluded the letter of cooperation agreement on the research and development of radioactive waste disposal in April, 2005, and have been carrying out the collaboration work based on the agreement. JAEA have been carrying out the Horonobe URL Project which is intended for a sedimentary rock in the Horonobe town, Hokkaido, since 2001. In the project, geoscientific research and research and development on geological disposal technology are being promoted. Meanwhile, The Agency for Natural Resources and Energy, Ministry of Economy, Trade and Industry has been promoting construction of equipments for the full-scale demonstration of engineered barrier system and operation technology for high-level radioactive waste disposal since 2008, to enhance public's understanding to the geological disposal of HLW, e.g. using underground facility. RWMC received an order of the project in fiscal year 2014 continuing since fiscal year 2008. Since topics in this project are included in the Horonobe URL Project, JAEA carried out this project as collaboration work continuing since fiscal year 2008. This report summarizes the results of the research on engineering technology carried out in this collaboration work in fiscal year 2014.
Fujita, Tomoo; Tanai, Kenji; Nakayama, Masashi; Sawada, Sumiyuki*; Asano, Hidekazu*; Saito, Masahiko*; Yoshino, Osamu*; Kobayashi, Masato*
JAEA-Research 2014-031, 44 Pages, 2015/03
JAEA-Research-2014-031.pdf:16.11MB
Japan Atomic Energy Agency (JAEA) and Radioactive Waste Management Funding and Research Center (RWMC) concluded the letter of cooperation agreement on the research and development of radioactive waste disposal in April, 2005, and have been carrying out the collaboration work based on the agreement. JAEA have been carrying out the Horonobe Underground Research Laboratory (URL) Project which is intended for a sedimentary rock in the Horonobe town, Hokkaido, since 2001. In the project, geoscientific research and research and development on geological disposal technology are being promoted. Meanwhile, the government (the Agency for Natural Resources and Energy, Ministry of Economy, Trade and Industry) has been promoting construction of equipments for the full-scale demonstration of engineered barrier system (EBS) and operation technology for high-level radioactive waste (HLW) disposal since 2008, to enhance public's understanding to the geological disposal of HLW, e.g. using underground facility. RWMC received an order of the project in fiscal year 2012 (2011/2012) continuing since fiscal year 2008 (2008/2009). Since topics in this project are included in the Horonobe URL Project, JAEA carried out this project as collaboration work continuing since fiscal year 2008. This report summarizes the results of engineering technology carried out in this collaboration work in fiscal year 2013. In fiscal year 2013, emplacement tests using buffer material block for the vertical emplacement concept were carried out and visualization tests for water penetration in buffer material were carried out.
Nakatsuka, Noboru; Sato, Haruo; Tanai, Kenji; Nakayama, Masashi; Sawada, Sumiyuki*; Asano, Hidekazu*; Saito, Masahiko*; Yoshino, Osamu*; Tsukahara, Shigeki*; Hishioka, Sosuke*; et al.
JAEA-Research 2013-034, 70 Pages, 2014/01
JAEA-Research-2013-034.pdf:9.11MB
Japan Atomic Energy Agency (JAEA) and Radioactive Waste Management Funding and Research Center (RWMC) concluded the letter of cooperation agreement on the research and development of radioactive waste disposal in April, 2005, and have been carrying out the collaboration work based on the agreement. JAEA have been carrying out the Horonobe Underground Research Laboratory (URL) Project which is intended for a sedimentary rock in the Horonobe town, Hokkaido, since 2001. In the project, geoscientific research and research and development on geological disposal technology are being promoted. Meanwhile, the government (the Agency for Natural Resources and Energy, Ministry of Economy, Trade and Industry) has been promoting construction of equipments for the full-scale demonstration of engineered barrier system and operation technology for high-level radioactive waste (HLW) disposal since 2008, to enhance public's understanding to the geological disposal of HLW, e.g. using underground facility. RWMC received an order of the project in fiscal year 2012 (2011/2012) continuing since fiscal year 2008 (2008/2009). Since topics in this project are included in the Horonobe URL Project, JAEA carried out this project as collaboration work continuing in fiscal year 2008. This report summarizes the results of engineering technology carried out in this collaboration work in fiscal year 2012. In fiscal year 2012, part of the equipments for emplacement of buffer material was produced and visualization test for water penetration in buffer material were carried out.
Kobayashi, Hidekazu; Amamoto, Ippei; Yokozawa, Takuma; Yamashita, Teruo; Nagai, Takayuki; Kitamura, Naoto*; Takebe, Hiromichi*; Mitamura, Naoki*; Tsuzuki, Tatsuya*
Proceedings of 15th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2013) (CD-ROM), 6 Pages, 2013/09
no abstracts in English
as the dominant sludge constituent generated from the treatment of water used for cooling the stricken power reactorsAmamoto, Ippei; Kobayashi, Hidekazu; Yokozawa, Takuma; Yamashita, Teruo; Nagai, Takayuki; Kitamura, Naoto*; Takebe, Hiromichi*; Mitamura, Naoki*; Tsuzuki, Tatsuya*
Proceedings of 15th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2013) (CD-ROM), 8 Pages, 2013/09
The great amount of water used for cooling the stricken power reactors at Fukushima Dai-ichi has resulted in accumulation of "remaining water". As the remaining water is subsequently contaminated by FPs, etc., it is necessary to decontaminate it in order to reduce the volume of liquid radioactive waste and to reuse it again for cooling the reactors. Various techniques are being applied to remove FP, etc. and to make stable waste forms. One of the methods using the iron phosphate glass as a medium is being developed to stabilize the strontium-bearing sludge whose main component is BaSO. From the results hitherto, the iron phosphate glass is regarded as a potential medium for the target sludge.
Shigetomi, Hiroshi*; Oka, Kiyoshi; Oi, Hidekazu*; Furukawa, Naoto*; Yoshida, Shozo*; Kawaguchi, Ryuji*; Nagai, Akira*; Haruta, Shoji*; Yanase, Yasuhito*; Akasaka, Julia*; et al.
Nihon Reza Igakkai-Shi, 33(2), p.131 - 135, 2012/08
no abstracts in English
Taniguchi, Naoki; Suzuki, Hiroyuki; Kawasaki, Manabu; Naito, Morimasa; Kobayashi, Masato*; Takahashi, Rieko*; Asano, Hidekazu*
Corrosion Engineering, Science and Technology, 46(2), p.117 - 123, 2011/04
Times Cited Count：9 Percentile：47.01(Materials Science, Multidisciplinary)Carbon steel has been selected as one of the candidate materials for overpack for geological disposal of high-level radioactive waste in Japan. Corrosion of carbon steel is divided into two types; general corrosion and localized corrosion. In this study, propagation behaviors of general and localized corrosions (pitting corrosion and crevice corrosion) were investigated by immersion tests of carbon steel under aerobic condition. The results of the immersion tests showed that the growth rate of corrosion was strongly dependent on the environmental condition and steel type, but the upper limit of pitting factor (the ratio of the maximum corrosion depth and the average corrosion depth) was approximately determined by only average corrosion depth. Based on these experimental data and literature data, an empirical model that predicts the maximum corrosion depth of an overpack from average corrosion depth was developed by applying the extreme value statistical analysis using the Gumbel distribution function.
Kobayashi, Masato*; Yokoyama, Yutaka*; Takahashi, Rieko*; Asano, Hidekazu*; Taniguchi, Naoki; Naito, Morimasa
Corrosion Engineering, Science and Technology, 46(2), p.212 - 216, 2011/04
Times Cited Count：4 Percentile：29.02(Materials Science, Multidisciplinary)The corrosion behaviour of a carbon steel weld joint under anaerobic conditions was investigated to estimate the long-term integrity of the carbon steel overpack. The weld specimens in this study were produced using three welding methods: GTAW, GMAW and EBW. General corrosion was observed for each immersion specimen and the weld joint corrosion rate was the same as or less than that of the base metal. The hydrogen concentration absorbed during immersion testing was less than 2.48
10
mol kg[Fe]
(0.05 ppm) after three years, a value regarded as having little influence on hydrogen embrittlement. The susceptibility to hydrogen embrittlement was highest in the base metal, suggesting that there was little adverse effect on the weld joint from welding. The welded carbon steel overpack is assumed to maintain its resistance to corrosion as a disposal container for the expected lifetime under anaerobic underground conditions.
Cr
TeKobayashi, Masaki*; Ishida, Yukiaki*; Hwang, J. I.*; Song, G. S.*; Fujimori, Atsushi; Yang, C. S.*; Lee, L.*; Lin, H.-J.*; Huang, D.-J.*; Chen, C. T.*; et al.
New Journal of Physics (Internet), 10, p.055011_1 - 055011_15, 2008/05
Times Cited Count：15 Percentile：64.38(Physics, Multidisciplinary)