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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.

Journal Articles

Investigation of chemical state of uranium included in simulated waste glass

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

JAEA Reports

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.

Journal Articles

Contribution to upgrade of vitrification technology by synchrotron radiation analysis; From Chemical state analysis of waste glass to development of structural analysis to prove soundness

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.

JAEA Reports

Investigation of simulated waste glass samples prepared from borosilicate glass frit including vanadium

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

JAEA-Research-2018-007.pdf:61.21MB

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.

Journal Articles

Chemical state analysis of simulated corium debris by EXAFS

Okamoto, Yoshihiro; Takano, Masahide

Progress in Nuclear Science and Technology (Internet), 5, p.200 - 203, 2018/11

Chemical state of some simulated corium debris samples containing uranium (fuel), zirconium (fuel cladding), iron (structure material), calcium (cement) and lanthanides (fission products) was investigated by synchrotron radiation based extended X-ray absorption fine structure (EXAFS) analysis. The local structure of uranium for the simulated debris was classified into fluorite UO$$_2$$ structure and C-type structure (stabilized cubic). The U$$_{0.27}$$Zr$$_{0.63}$$Fe$$_{0.05}$$Ca$$_{0.05}$$O$$_2$$ sample, which consists of single phase (C-type), shows slightly shorter U-O distance. It can be concluded that the sample contains pentavalent uranium. The local structure of zirconium for U-Zr-O and U-Zr-Fe-O systems was very close to tetragonal ZrO$$_2$$, while that of zirconium changed to CSZ (calcia stabilized cubic) by adding calcium.

JAEA Reports

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.

Journal Articles

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.

Journal Articles

Evaluation of uranium chemical state in borosilicate glasses by using XAFS measurement

Nagai, Takayuki; Kobayashi, Hidekazu; Okamoto, Yoshihiro; Akiyama, Daisuke*; Sato, Nobuaki*

Photon Factory Activity Report 2017, 2 Pages, 2018/00

no abstracts in English

Journal Articles

Study on Mo structure in simulated dissolved solutions of activated metal waste

Shimada, Asako; Okamoto, Yoshihiro

Photon Factory Activity Report 2017, 2 Pages, 2018/00

no abstracts in English

Journal Articles

Microstructure analysis using X-ray absorption on heat-affected zone of reactor pressure vessel steel

Iwata, Keiko; Takamizawa, Hisashi; Ha, Yoosung; Okamoto, Yoshihiro; Shimoyama, Iwao; Honda, Mitsunori; Hanawa, Satoshi; Nishiyama, Yutaka

Photon Factory Activity Report 2017, 2 Pages, 2018/00

no abstracts in English

Journal Articles

The Significance of bromide in the Brust-Schiffrin synthesis of thiol protected gold nanoparticles

Booth, S. G.*; Uehara, Akihiro*; Chang, S.-Y.*; La Fontaine, C.*; Fujii, Toshiyuki*; Okamoto, Yoshihiro; Imai, Takahito*; Schroeder, S. L. M.*; Dryfe, R. A. W.*

Chemical Science, 8(12), p.7954 - 7962, 2017/12

 Times Cited Count:7 Percentile:44.1(Chemistry, Multidisciplinary)

The two-phase Brust-Schiffrin synthesis of alkane thiol protected metal nanoparticles has been shown to undergo significantly different processes dependent on the precursor species and reactant conditions. In this work X-ray absorption spectroscopy is used in conjunction with liquid/liquid electrochemistry in order to highlight the significance of B$${^-}$$r; to the reaction mechanism. We propose that the observed behavior of [AuBr$${_4}$$]$${^-}$$; species described herein explain a deviation in reported behavior present in the current literature. The reported mechanistic understanding should enable a nanoparticle synthesis with a higher yield and reduce size polydispersity.

Journal Articles

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

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$$_{2}$$ 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$$_{2}$$). It suggests that stable (Ru,Rh)O$$_{2}$$ 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.

JAEA Reports

XAFS measurement of simulated waste borosilicate glass samples (Joint research)

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$$^{2}$$ type boron (BO$$_{3}$$) from sp$$^{3}$$ type boron (BO$$_{4}$$). Addition of waste elements to a glass frit increases the percentage of BO$$_{3}$$ and decreases that of BO$$_{4}$$. By decreasing the SiO$$_{2}$$/Al$$_{2}$$O$$_{3}$$ ratio or increasing the (SiO$$_{2}$$+B$$_{2}$$O$$_{3}$$)/Al$$_{2}$$O$$_{3}$$ ratio in the glass composition, the BO$$_{3}$$ percentage increases and the BO$$_{4}$$ percentage decreases. Addition of P$$_{2}$$O$$_{5}$$ decreases the BO$$_{3}$$ percentage and increases the BO$$_{4}$$ percentage. Following results were obtained from XAFS measurement of the waste elements. Cerium (Ce) valence is more reduced with the increase of the B$$_{2}$$O$$_{3}$$ content. Addition of P$$_{2}$$O$$_{5}$$ 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 B$$_{2}$$O$$_{3}$$ 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.

Journal Articles

Ion species/energy dependence of irradiation-induced lattice structure transformation and surface hardness of Ni$$_{3}$$Nb and Ni$$_{3}$$Ta intermetallic compounds

Kojima, Hiroshi*; Kaneno, Yasuyuki*; Ochi, Masaaki*; Semboshi, Satoshi*; Hori, Fuminobu*; Saito, Yuichi*; Ishikawa, Norito; Okamoto, Yoshihiro; Iwase, Akihiro*

Materials Transactions, 58(5), p.739 - 748, 2017/05

 Times Cited Count:1 Percentile:82.18(Materials Science, Multidisciplinary)

Bulk samples of Ni$$_{3}$$Nb and Ni$$_{3}$$Ta intermetallic compounds were irradiated with 16 MeV Au, 4.5 MeV Ni, 4.5 MeV Al, 200 MeV Xe and 1.0 MeV He ions, and the change in near-surface lattice structure was investigated by means of the grazing incidence X-ray diffraction (GIXD)and EXAFS. The Ni$$_{3}$$Nb and Ni$$_{3}$$Ta lattice structures transform from the ordered structures (orthorhombic and monoclinic structures for Ni$$_{3}$$Nb and Ni$$_{3}$$Ta, respectively) to the amorphous state by the Au, Ni, Al and Xe ion irradiations. Irrespective of such heavy ion species or energies, the lattice structure transformation to the amorphous state almost correlate with the density of energy deposited through elastic collisions.

Journal Articles

Development of cesium-free mineralization for decontamination and reuse of radioactive contaminated soil in Fukushima

Shimoyama, Iwao; Honda, Mitsunori; Kogure, Toshihiro*; Baba, Yuji; Hirao, Norie*; Okamoto, Yoshihiro; Yaita, Tsuyoshi; Suzuki, Shinichi

Photon Factory News, 35(1), p.17 - 22, 2017/05

We introduce Cs-free mineralization (CFM) for Cs removal and reuse of radioactive-contaminated soil in Fukushima and report recent work conducted in the BL27A beamline in Photon Factory. In this work, we investigated compositional and structural changes of Cs-sorbed weathered biotite (WB) before and after heating treatment with addition of NaCl-CaCl$$_{2}$$ salts under low-pressure condition, to study Cs desorption mechanism from clay minerals. X-ray fluorescence spectroscopy clarified that almost all Cs and K were removed with the salts at 700 $$^{circ}$$C. On the other hand, Ca increased with heating temperature. X-ray diffraction and transmission electron microscopy analysis clarified that phase transitions from WB to some Ca-rich silicate minerals, e.g., augite, were caused by the heating treatment with the salt. Based on these results, CFM is proposed for Cs removal utilizing the mechanism in which large monovalent cations are discharged with accompanying the phase transition. We also discuss the role of Cl in this reaction showing chemical bonding change of Cl observed using X-ray absorption spectroscopy in the early stage of the chemical reaction.

Journal Articles

Chemical state analysis of high-temperature molten slag components by using high-energy XAFS

Okamoto, Yoshihiro; Osugi, Takeshi; Akabori, Mitsuo; Kobayashi, Toru; Shiwaku, Hideaki

Journal of Molecular Liquids, 232, p.285 - 289, 2017/04

 Times Cited Count:2 Percentile:78.31(Chemistry, Physical)

High energy XAFS measurement using cerium K-edge was performed to study the chemical state of cerium in high-temperature molten slag (SiO$$_{2}$$-CaO-Fe$$_{2}$$O$$_{3}$$-CeO$$_{2}$$). It was found from the change in the nearest Ce-O distance obtained from EXAFS analysis and the energetic shift of the white line peak observed in XANES analysis that oxidation state of cerium was tetravalent in the molten state and trivalent in solid state. The Debye-Waller factor of the nearest Ce-O pair in solid slag was very large even at room temperature, and the change in its value upon heating and melting was very small. This result suggests that cerium is highly disordered and stable in solid slag.

Journal Articles

Local structure analysis of ZrN, and Dy$$_{0.5}$$Zy$$_{0.5}$$N surrogate materials for fast reactor nitride fuel

Yoneda, Yasuhiro; Tsuji, Takuya; Matsumura, Daiju; Okamoto, Yoshihiro; Takaki, Seiya; Takano, Masahide

Transactions of the Materials Research Society of Japan, 42(2), p.23 - 26, 2017/04

ZnN is a possible candidate for the diluent material for nitride fuels containing transuranium elements. Pellets of inert matrix material ZrN, and surrogate nitride fuel material Dy$$_{0.5}$$Zr$$_{0.5}$$N, are fabricated for the purpose of investigating the crystal structure. Lattice parameters of Dy$$_{1-x}$$Zr$$_x$$N followed the Vegard's low, in spite of the large lattice mismatch ($$sim$$ 7%) between DyN and ZrN. Local structure analysis was performed by X-ray absorption fine structure (XAFS) and atomic pair-distribution function (PDF) methods. The Zr-N nearest neighbor bond distance changed as changing the Dy composition. The complex local structure of DyN and ZrN is related to the preferable effects of ZrN.

JAEA Reports

Preliminary missions for the decommissioning of the laboratory building No.1 for the plutonium research program

Segawa, Yukari; Horita, Takuma; Kitatsuji, Yoshihiro; Kumagai, Yuta; Aoyagi, Noboru; Nakada, Masami; Otobe, Haruyoshi; Tamura, Yukito*; Okamoto, Hisato; Otomo, Takashi; et al.

JAEA-Technology 2016-039, 64 Pages, 2017/03

JAEA-Technology-2016-039.pdf:5.24MB

The laboratory building No.1 for the plutonium research program (Bldg. Pu1) was chosen as one of the facilities to decommission by Japan Atomic Energy Agency Reform in September, 2013. The research groups, users of Bldg. Pu1, were driven by necessity to remove used equipment and transport nuclear fuel to other facilities from Bldg. Pu1. Research Group for Radiochemistry proactively established the Used Equipment Removal Team for the smooth operation of the removal in April, 2015. The team classified six types of work into the nature of the operation, removal of used equipment, disposal of chemicals, stabilization of mercury, stabilization of nuclear fuel, transportation of nuclear fuel and radioisotope, and survey of contamination status inside the glove boxes. These works were completed in December, 2015. This report circumstantially shows six works process, with the exception of the approval of the changes on the usage of nuclear fuel in Bldg. Pu1 to help prospective decommission.

295 (Records 1-20 displayed on this page)