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JAEA Reports

Structural investigation of simulated waste glass surface drained in operation confirmation test of 3rd TVF glass melter

Nagai, Takayuki; Hasegawa, Takehiko*

JAEA-Research 2023-008, 41 Pages, 2023/12

JAEA-Research-2023-008.pdf:7.52MB

To reduce the risks posed by stored the high-level radioactive liquid waste (HAW), Tokai Vitrification Facility (TVF) is working to produce the HAW into vitrified bodies. With the aim of steady vitrification of HAW in TVF, the vitrification technology section has manufactured a new 3rd melter with an improved bottom structure and is working to verify the performance of this melter. In this study, solidified glass samples were taken from simulated vitrified bodies produced by flowing molten glass during the bottom drain-out test in the operation confirmation of the TVF 3rd melter. And the properties of the surface layer and fracture surface of the vitrified bodies were evaluated by using Raman spectroscopy, synchrotron radiation XAFS measurement, and laser ablation inductively coupled plasma atomic emission spectroscopy (LA ICP-AES) analysis. As a result of measuring the surface layer and fracture surface of the solidified samples produced on an actual scale, a slight difference was confirmed between the properties of the surface layer and those of the fracture surface. Since the chemical composition of these simulated vitrified bodies does not contain platinum group elements, it is expected that the glass structure of solidified glass samples is different from that of the actual vitrified body. However, this sample measuring was a valuable opportunity to evaluate samples produced by using the direct energized joule heating method. The properties of cullet used the operation confirmation of the TVF 3rd melter and the cullet of another production lot were measured and analyzed in the same manner under the measuring conditions of solidified glass samples. As a result, it was confirmed that cullet with different producing histories have different glass structures even with the same chemical composition, and that differences in glass structures remain in the glass samples after melting these cullet.

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 3 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2023-004, 45 Pages, 2023/09

JAEA-Research-2023-004.pdf:6.07MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. To understand the chemical stability of simulated waste glasses, XANES spectra of B K-edge, Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge were measured on the glass surface exposed to the leachate. As a result, it was found that the glass surface exposed to the leachate was changed and it was difficult to obtain a clear XANES spectrum. From the B K-edge XANES spectra on glass surfaces exposed to the leachate, an increase in three-coordination of B-O (BO$$_{3}$$) and a decrease in four-coordination of B-O (BO$$_{4}$$) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L$$_{3}$$, L$$_{2}$$-edge, and Cs M$$_{5}$$, M$$_{4}$$-edge show that as the exposure time in the leachate increases, the Cs present on the glass surface dissolves into the leachate. The XANES spectra of Si K-edge were measured on simulated waste glass surfaces before immersion, and it was confirmed that the change in XANES spectra given by Na$$_{2}$$O concentration had a larger effect than the waste component concentration.

Journal Articles

Neutron resonance absorption imaging of simulated high-level radioactive waste in borosilicate glass

Oba, Yojiro; Motokawa, Ryuhei; Kaneko, Koji; Nagai, Takayuki; Tsuchikawa, Yusuke; Shinohara, Takenao; Parker, J. D.*; Okamoto, Yoshihiro

Scientific Reports (Internet), 13, p.10071_1 - 10071_8, 2023/06

 Times Cited Count:0 Percentile:0.01

JAEA Reports

Structural evaluation of coagulated surface of simulated waste glass by using Raman spectroscopy

Nagai, Takayuki

JAEA-Research 2022-014, 84 Pages, 2023/02

JAEA-Research-2022-014.pdf:22.26MB

Most of the simulated waste glasses used for physical property evaluation are processed into a shape suitable for the measurement method from glass gob obtained by slowly cooling molten glass to room temperature. However, the actual vitrified waste glass material is obtained by cooling and being coagulated the glass drained from the bottom of glass melter into the canister. In this study, Raman spectroscopy was performed on the coagulated surface of molten simulated waste glass in the depth direction to evaluate the state of the Si-O bridging structure near the coagulated glass surface. The Raman spectra measured from the surface to the depth direction near the surface of the glasses produced by several melting and coagulation conditions of molten simulated waste glass cullet in the air atmosphere, and it was confirmed that there were changes in these spectra. On the other hand, the raw material glass cullet and the surface of the glass solidified in argon gas atmosphere showed little change in the spectrum in the depth direction, and the Si-O bridging structure near the glass surface was similar. It was also confirmed that the spectrum change in the depth direction measurement was small for the cut surface of the glass, and that the change in the spectrum for the broken glass fracture surface was also small. For glasses with a large change in Raman spectra in the depth direction near the coagulated surface, the molten glass was cooled from the molten state to room temperature in a muffle furnace with air atmosphere. That is, the magnitude of the spectral change with respect to the depth direction depends on the time from the molten state to coagulation. In order to confirm the reason why the number of bridging oxygen in the Si-O bridging structure is small on the coagulated surface of glass, the XANES spectra of Si-K edge and Ce-L3 edge were measured by XAFS on the coagulated surface and the cutting face. As a result, the Si-K edge peak on the coagulated surface is

Journal Articles

Synchrotron analysis of simulated waste glasses different in boron isotope ingredient

Nagai, Takayuki; Tone, Masaya; Katsuoka, Nanako; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*

Photon Factory Activity Report 2022 (Internet), 3 Pages, 2023/00

no abstracts in English

Journal Articles

Structural change by phosphorus addition to borosilicate glass containing simulated waste components

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$$_3$$). 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$$_4$$ structural unit and may deprive the alkali metal coordinated to the molybdate ion.

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 2 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

JAEA-Research 2022-008, 37 Pages, 2022/10

JAEA-Research-2022-008.pdf:5.27MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of simulated waste glass surfaces after immersion test to investigate the long chemical stability. (1) As the leaching time of glass samples in immersion test passed, the Cs M$$_{5}$$, M$$_{4}$$-edge XANES spectra disappeared and the Fe L$$_{3}$$, L$$_{2}$$-edge spectra changed. (2) A new compound was formed on the sample surface after the immersion test, and these changes in the surface state were confirmed by Raman spectroscopy. However, it became difficult to obtain a clear B K-edge XANES spectrum by forming a compound on glass surfaces. The Si K-edge XANES spectra of borosilicate glass frits with different Na$$_{2}$$O content were measured, and following was confirmed. (1) As the Na$$_{2}$$O concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The intensity of the Si K-edge peak is maximum when the Na$$_{2}$$O content in glass frits was about 7wt%.

Journal Articles

Study on the relation between the crystal structure and thermal stability of FeUO$$_{4}$$ and CrUO$$_{4}$$

Akiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09

 Times Cited Count:2 Percentile:71.05(Materials Science, Multidisciplinary)

FeUO$$_{4}$$, CrUO$$_{4}$$, and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO$$_{4}$$ and CrUO$$_{4}$$, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm$$^{-1}$$ in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ was composed of a uranyl-like structure in its lattice regardless of its "x"' value. M$"o$ssbauer measurements indicated that the Fe in FeUO$$_{4}$$ and Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ were trivalent. Furthermore, Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ lost its symmetry around Fe$$^{mathrm{III}}$$ with increasing electron densities around Fe$$^{mathrm{III}}$$, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO$$_{4}$$ and CrUO$$_{4}$$. Thermogravimetric measurements for UO$$_{2}$$, FeUO$$_{4}$$, and CrUO$$_{4}$$ showed that the temperature at which FeUO$$_{4}$$ decomposed under an oxidizing condition (approximately 800 $$^{circ}$$C) was significantly lower than the temperature at which the decomposition of CrUO$$_{4}$$ started (approximately 1250 $$^{circ}$$C). Based on these results, we concluded that the decomposition of FeUO$$_{4}$$ was triggered by an "in-crystal" redox reaction, i.e., Fe$$^{mathrm{III}}$$ $${+}$$ U$$^{mathrm{V}}$$ $$rightarrow$$ Fe$$^{mathrm{II}}$$ $${+}$$ U$$^{mathrm{VI}}$$, which would not occur in the CrUO$$_{4}$$ lattice because Cr$$^{mathrm{III}}$$ could never be reduced under the investigated condition. Finally, the existence of Cr$$^{mathrm{III}}$$ in FexCr$$_{1-x}$$UO$$_{4}$$ effectively suppressed the decomposition of the Fe$$_{x}$$Cr$$_{1-x}$$UO$$_{4}$$ crystal, even at a very low Cr content.

Journal Articles

Nanoscopic structure of borosilicate glass with additives for nuclear waste vitrification

Motokawa, Ryuhei; Kaneko, Koji; Oba, Yojiro; Nagai, Takayuki; Okamoto, Yoshihiro; Kobayashi, Taishi*; Kumada, Takayuki; Heller, W. T.*

Journal of Non-Crystalline Solids, 578, p.121352_1 - 121352_7, 2022/02

 Times Cited Count:3 Percentile:23.99(Materials Science, Ceramics)

JAEA Reports

Structural investigation of borosilicate glasses by using XAFS measurement in Soft X-ray region (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Ota, Toshiaki*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

JAEA-Research 2021-010, 62 Pages, 2022/01

JAEA-Research-2021-010.pdf:6.05MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the local structure and chemical state regarding boron(B), oxygen(O), silicon(Si) and waste elements of iron(Fe), cesium(Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of prepared glass frit and simulated waste glass samples: (1) The effect of Na$$_{2}$$O concentration on B-O coordination structure is greater than that of the waste elements concentration. (2) The height of pre-edge by O K-edge spectrum depends on the concentration of first transition elements such as Fe in glass samples. Following results were obtained by XAFS measurements of simulated waste glass samples after immersion test to investigate the long chemical stability. (1) A new compound was formed on the sample surface after the immersion test, and changes in the surface state were confirmed by Raman spectroscopy. (2) Cs on the sample surface after immersion test dissolves into the leaching solution. The Si K-edge XANES spectra of borosilicate glass frits and simulated waste glass samples included lanthanides oxide were measured, and following was confirmed. (1) As the Na$$_{2}$$O concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The peak height of the K-edge of Si differs depending on the kind of lanthanide.

Journal Articles

Synchrotron analysis of simulated waste glasses different in boron isotope ingredient

Nagai, Takayuki; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*; Arima, Tatsumi*

Photon Factory Activity Report 2021 (Internet), 2 Pages, 2022/00

no abstracts in English

Journal Articles

Crystal structure of U$$_{1-y}$$Ln$$_{y}$$O$$_{2-x}$$ (Ln = Gd, Er) solid solution

Pham, V. M.*; Arima, Tatsumi*; Inagaki, Yaohiro*; Idemitsu, Kazuya*; Akiyama, Daisuke*; Nagai, Takayuki; Okamoto, Yoshihiro

Journal of Nuclear Materials, 556, p.153189_1 - 153189_9, 2021/12

 Times Cited Count:0 Percentile:16.97(Materials Science, Multidisciplinary)

The crystal structure change was evaluated for (1-x)UO$$_{2}$$-xLnO$$_{1.5}$$ (Ln=Gd or Er; x = 0 to 0.4) samples sintered at 1973 K for 8 h under Ar and Ar-10%H$$_{2}$$ atmospheres. The effect of LnO$$_{1.5}$$ doping on the crystal structure of UO$$_{2}$$ was investigated by X-ray diffraction (XRD) and X-ray absorption fine structure (XAFS). LnO$$_{1.5}$$ doping into UO$$_{2}$$ reduced the lattice parameter of UO$$_{2}$$-LnO$$_{1.5}$$ solid solutions up to 40mol% LnO$$_{1.5}$$. The lattice parameters of these samples were comparable to those of stoichiometric (U,Ln)O$$_{2.00}$$ solid solutions, that is, the O/M ratios were close to 2.00. The U L$$_{3}$$-edge XANES analysis showed that higher U oxidation states of +5 or +6 formed, in addition to + 4. The EXAFS analysis indicated that the interatomic distances of U-O and Gd-O decreased with increasing x, whereas those of Er-O may not decrease monotonically.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

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

2020-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), 1 Pages, 2021/11

no abstracts in English

Journal Articles

XAFS analysis of ruthenium in simulated iron phosphate radioactive waste glass

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:3 Percentile:32(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$$_{2}$$O$$_{3}$$-P$$_{2}$$O$$_{5}$$ base glass. In other samples, crystalline RuO$$_{2}$$ was predominant. According to the imaging XAFS analysis, RuO$$_{2}$$ particles in all samples had length smaller than 50$$mu$$m. Aggregations of RuO$$_{2}$$, which are found in nuclear waste borosilicate glass, were not seen in any of the iron phosphate glass samples.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

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

2019-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), P. 20191107_1, 2020/11

no abstracts in English

JAEA Reports

Structural investigation of simulated waste glass samples by using XAFS measurement in soft X-ray region (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Ota, Toshiaki*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

JAEA-Research 2020-009, 48 Pages, 2020/09

JAEA-Research-2020-009.pdf:4.53MB

The local structure of glass-forming elements and waste elements in waste glass varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the local structure and chemical state regarding boron (B), oxygen (O), and waste elements of cerium (Ce), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of prepared glass frit and simulated waste glass samples: (1) The existence ratio of four coordinate sp$$^{3}$$ structure (BO$$_{4}$$) tends to increase with increasing Na$$_{2}$$O content in glass samples. (2) The height of a pre-edge which appears by K-edge XANES spectrum of O is so high that the Fe content in glass samples. Following results were obtained by XAFS measurements of simulated waste glass samples after immersion test to investigate long chemical stability. (1) The existence ratio of four coordinate sp$$^{3}$$ structure (BO$$_{4}$$) increases by immersion test. (2) Ce which exists in the surface layer is oxidized by immersion test, and much of Cs in surface layer is lost after leach testing. Even if the glass frit form (fiber cartridge or beads) and manufacturing method were changed and a glass sample of the similar chemical composition was prepared, these observed Raman spectra of samples were different.

Journal Articles

Structural change of borosilicate glass by boron isotope composition

Nagai, Takayuki; Okamoto, Yoshihiro; Akiyama, Daisuke*; Uehara, Akihiro*; Fujii, Toshiyuki*; Sekimoto, Shun*

KURNS Progress Report 2019, P. 257, 2020/08

To understand the influence of glass structural change by neutron irradiation and boron isotope composition, glass samples were made from enrichment boric acid reagents and neutron irradiation of those samples was carried out in Pn-2 of KUR. The structural change of glass sample after the irradiation will be estimated in 2020FY. Before neutron irradiation test of glass samples, the Si-O bridging structure difference by boron isotope composition compared by using a Raman spectrometry.

Journal Articles

Investigation of chemical state of simulated waste glasses by using XAFS measurement

Nagai, Takayuki; Shimoyama, Iwao; Okamoto, Yoshihiro; Akiyama, Daisuke*; Arima, Tatsumi*

Photon Factory Activity Report 2019 (Internet), 3 Pages, 2020/00

no abstracts in English

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.

205 (Records 1-20 displayed on this page)