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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

Journal Articles

Flexible fuel cycle system for the effective management of plutonium

Fukasawa, Tetsuo*; Hoshino, Kuniyoshi*; Yamashita, Junichi*; Takano, Masahide

Journal of Nuclear Science and Technology, 57(11), p.1215 - 1222, 2020/11

The flexible fuel cycle initiative system (FFCI system) has been developed to reduce spent fuel (SF) amounts, to keep high availability factor for the reprocessing plant and to increase the proliferation resistance for the recovered Pu. The system separates most U from the SF at first, and the residual material called recycle material (RM) which contains Pu, minor actinides, fission products and remaining U will go to Pu(+U) recovery from the RM for Pu utilizing reactor in future. The Pu utilizing reactor is FBR or LWR with MOX fuel. The RM is the buffer material between SF reprocessing and Pu utilizing reactor with compact size and high proliferation resistance, which can suppress the amount of relatively pure Pu. The innovative technologies of FFCI are most U separation and temporary RM storage. They are investigated by the literature survey, fundamental experiments using simulated material and analyses using simulation code. This paper summarizes the feasibility confirmation results of FFCI.

Journal Articles

Application of photoluminescence microspectroscopy; A Study on transfer of uranyl and europium ions on dry silica gel plate

Kusaka, Ryoji; Watanabe, Masayuki

Journal of Nuclear Science and Technology, 57(9), p.1046 - 1050, 2020/09

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

Journal Articles

Preventing nuclear fuel material adhesion on glove box components using nanoparticle coating

Segawa, Tomoomi; Kawaguchi, Koichi; Ishii, Katsunori; Suzuki, Masahiro; Tachihara, Joji; Takato, Kiyoto; Okita, Takatoshi; Satone, Hiroshi*; Suzuki, Michitaka*

Proceedings of 2020 International Conference on Nuclear Engineering (ICONE 2020) (Internet), 6 Pages, 2020/08

To reduce the hold-up of the nuclear fuel materials in the glove box and the external exposure dose, the technology of the MOX powder adhesion prevention by the nanoparticle coating to the acrylic panels of the glove box has been developed. Due to the formation of nano-sized tiny rugged surface, the nanoparticle coating reduced the minimum adhesion force between the UO$$_{2}$$ particles and the acrylic test piece surface with the smallest particle size of about 5 $$mu$$m where desorption was observed, by about one-tenth. Moreover, the nanoparticle coating reduced the amount of the MOX powder adhering to the acrylic test piece to about one-tenth. In this study, it was found that applying the nanoparticle coating to the acrylic panels of glove box can prevent the adhesion of nuclear fuel materials. This method is effective for reducing the hold-up of the nuclear fuel materials in the glove box, the external exposure dose and improving the visibility of the acrylic panels.

Journal Articles

The Chemistry of uranium (I); Basics and application

Sato, Nobuaki*; Kirishima, Akira*; Watanabe, Masayuki

Uran No Kagaku (I); Kiso To Oyo, 184 Pages, 2020/06

This particular book deals with fundamental items related with chemistry of Uranium and consists of basic section and practical section. In the basic section, inorganic and radiochemistry of Uranium was described. On the other hand, in the practical section, the process chemistry related with reprocessing of nuclear fuels and "debris" involved with Fukushima Daiichi Power Plant accident were described. This book is intended for use by scientists, engineers and students in the nuclear industry in their education and/or professional practice.

Journal Articles

$$gamma$$-radiation and H$$_{2}$$O$$_{2}$$ induced oxidative dissolution of uranium(IV) oxide in aqueous solution containing phthalic acid

Kumagai, Yuta; Jonsson, M.*

Dalton Transactions (Internet), 49(6), p.1907 - 1914, 2020/02

 Times Cited Count:0 Percentile:100(Chemistry, Inorganic & Nuclear)

This study aims to reveal possible involvements of organic acids in the oxidative dissolution of UO$$_{2}$$. Using phthalic acid as a model compound, we have measured adsorption on UO$$_{2}$$ and investigated effects on the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ and on oxidative dissolution induced by $$gamma$$-irradiation. Significant adsorption of phthalic acid was observed even at neutral pH. However, the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ in phthalic acid solution induced oxidative dissolution of U(VI) similarly to aqueous bicarbonate solution. These results indicate that even though phthalic acid adsorbs on the UO$$_{2}$$ surface, it is not involved in the interfacial reaction by H$$_{2}$$O$$_{2}$$. In contrast, the dissolution of U by irradiation was inhibited in aqueous phthalic acid solution, whereas H$$_{2}$$O$$_{2}$$ generated by radiolysis was consumed by UO$$_{2}$$. The inhibition suggests that radical species derived from phthalic acid was involved in the redox reaction process of UO$$_{2}$$.

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

Journal Articles

Electronic structure of UTe$$_2$$ studied by photoelectron spectroscopy

Fujimori, Shinichi; Kawasaki, Ikuto; Takeda, Yukiharu; Yamagami, Hiroshi; Nakamura, Ai*; Homma, Yoshiya*; Aoki, Dai*

Journal of the Physical Society of Japan, 88(10), p.103701_1 - 103701_5, 2019/10

 Times Cited Count:4 Percentile:25.43(Physics, Multidisciplinary)

Journal Articles

$$^{125}$$Te-NMR study on a single crystal of heavy fermion superconductor UTe$$_2$$

Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Hattori, Taisuke; Higa, Nonoka; Nakamine, Genki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Nakamura, Ai*; Shimizu, Yusei*; et al.

Journal of the Physical Society of Japan, 88(7), p.073701_1 - 073701_4, 2019/07

 Times Cited Count:13 Percentile:5.64(Physics, Multidisciplinary)

We report $$^{125}$$Te-NMR studies on a newly discovered heavy fermion superconductor UTe$$_2$$. Using a single crystal, we have measured the $$^{125}$$Te-NMR Knight shift $$K$$ and spin-lattice relaxation rate $$1/T_1$$ for fields along the three orthorhombic crystal axes. The data confirm a moderate Ising anisotropy for both the static ($$K$$) and dynamical susceptibilities ($$1/T_1$$) in the paramagnetic state above about 20 K. Around 20 K, however, we have observed a sudden loss of NMR spin-echo signal due to sudden enhancement of the NMR spin-spin relaxation rate $$1/T_2$$, when the field is applied along the easy axis of magnetization (=$$a$$ axis). This behavior suggests the development of longitudinal magnetic fluctuations along the $$a$$ axis at very low frequencies below 20 K.

Journal Articles

Time-controlled synthesis of the 3D coordination polymer U(1,2,3-Hbtc)$$_{2}$$ followed by the formation of molecular poly-oxo cluster {$rm U$_{14}$$} containing hemimellitate uranium(IV)

Dufaye, M.*; Martin, N. P.*; Duval, S.*; Volkringer, C.*; Ikeda, Atsushi; Loiseau, T.*

RSC Advances (Internet), 9(40), p.22795 - 22804, 2019/07

 Times Cited Count:4 Percentile:38.54(Chemistry, Multidisciplinary)

Two coordination compounds bearing tetravalent uranium (UIV)) were synthesized in the presence of tritopic hemimellitic acid in acetonitrile with a controlled amount of water (H$$_{2}$$O/U $${approx}$$ 8) and structurally characterized. The slow hydrolysis reaction together with the partial decomposition of the starting organic reactants into oxalate and acetate molecules induces the generation of such a large poly-oxo cluster with fourteen uranium centers. Structural comparisons with other closely related uranium-containing clusters, such as the {$rm U$_{12}$$}$ cluster based on the association of inner core [U$_{6}$$O$$_{8}$$] with three dinuclear sub-units {$rm U$_{2}$$}, were performed.

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), P. 20181080_1, 2019/06

no abstracts in English

Journal Articles

Study on decontamination of steel surface contaminated with uranium hexafluoride by acidic electrolytic water

Nakayama, Takuya; Nomura, Mitsuo; Mita, Yutaka; Yonekawa, Hitoshi*; Bunbai, Misako*; Yaita, Yumi*; Murata, Eiichi*; Hosaka, Katsumi*; Sugitsue, Noritake

Proceedings of 2019 International Congress on Advances in Nuclear Power Plants (ICAPP 2019) (Internet), 8 Pages, 2019/05

Clearance of contaminated metal is important for recycling and volume reduction of radioactive waste. Among applicable decontamination technologies, immersion method with ultrasonic cleaning is considered to be effective for metal materials having various shapes. in this study is to demonstrate decontamination of carbon steel contaminated by uranium hexafluoride to the target level for clearance (less than 0.04 Bq/cm$$^{2}$$), and minimize secondary waste. In this test, acidic electrolytic water, dilute hydrochloric acid, dilute sulfuric acid and ozone water with various pH and redox potential were used as decontamination solutions to be tested. We found that acidic electrolytic water is effective solution for decontamination of carbon steel contaminated by uranium hexafluoride. It could be decontaminate less than target level for clearance, and reduced secondary waste relatively.

Journal Articles

Environmental research on uranium at the Ningyo-Toge Environmental Engineering Center, JAEA

Sato, Kazuhiko; Yagi, Naoto; Nakagiri, Toshio

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 6 Pages, 2019/05

no abstracts in English

Journal Articles

Effect of H$$_{2}$$O$$_{2}$$ concentration on oxidative dissolution of U$$_{2}$$O

Kumagai, Yuta

Hoshasen Kagaku (Internet), (107), p.77 - 78, 2019/04

Reaction of hydrogen peroxide (H$$_{2}$$O$$_{2}$$) with uranium dioxide (UO$$_{2}$$) oxidizes U(IV) to water-soluble U(VI). In the concept of direct geological disposal of spent nuclear fuel, this reaction is expected to induce dissolution of UO$$_{2}$$ matrix of the spent fuel. This study investigate effect of H$$_{2}$$O$$_{2}$$ concentration on the kinetics and the yield of U(VI) dissolution of this reaction. A series of experiments of the reaction of H$$_{2}$$O$$_{2}$$ with UO$$_{2}$$ powder dispersed in water has been carried out. The experimental results reveal that increase in the H$$_{2}$$O$$_{2}$$ concentration slows down the reaction and decreases the yield of U(VI) dissolution. This observation suggests that a reaction intermediate is generated in the course of the H$$_{2}$$O$$_{2}$$ reaction on the surface of UO$$_{2}$$.

Journal Articles

Impact of stoichiometry on the mechanism and kinetics of oxidative dissolution of UO$$_{2}$$ induced by H$$_{2}$$O$$_{2}$$ and $$gamma$$-irradiation

Kumagai, Yuta; Fidalgo, A. B.*; Jonsson, M.*

Journal of Physical Chemistry C, 123(15), p.9919 - 9925, 2019/04

 Times Cited Count:4 Percentile:38.13(Chemistry, Physical)

Radiation-induced oxidative dissolution of uranium dioxide (UO$$_{2}$$) is one of the most important chemical processes of U driven by redox reactions. We have examined the effect of UO$$_{2}$$ stoichiometry on the oxidative dissolution of UO$$_{2}$$ induced by hydrogen peroxide (H$$_{2}$$O$$_{2}$$) and $$gamma$$-ray irradiation. By comparing the reaction kinetics of H$$_{2}$$O$$_{2}$$ between stoichiometric UO$$_{2.0}$$ and hyper-stoichiometric UO$$_{2.3}$$, we observed a significant difference in reaction speed and U dissolution kinetics. The stoichiometric UO$$_{2.0}$$ reacted with H$$_{2}$$O$$_{2}$$ much faster than the hyper-stoichiometric UO$$_{2.3}$$. The U dissolution from UO$$_{2.0}$$ was initially much lower than that from UO$$_{2.3}$$, but gradually increased as the oxidation by H$$_{2}$$O$$_{2}$$ proceeded. The $$gamma$$-ray irradiation induced the U dissolution that is analogous to the kinetics by the exposure to a low concentration (0.2 mM) of H$$_{2}$$O$$_{2}$$. The exposure to higher H$$_{2}$$O$$_{2}$$ concentrations caused lower U dissolution and resulted in deviation from the U dissolution behavior by $$gamma$$-ray irradiation.

Journal Articles

Application of M$$_{V}$$-edge XANES to determination of U oxidation state in zircon

Tanaka, Kazuya; Takahashi, Yoshio*

Geochemical Journal, 53(5), p.329 - 331, 2019/00

 Times Cited Count:0 Percentile:100(Geochemistry & Geophysics)

We examined three natural zircon samples with different amounts of radiation doses using M$$_{V}$$-edge and L$$_{III}$$-edge U X-ray absorption near-edge structure (XANES). Analysis of XANES spectra at both M$$_{V}$$-edge and L$$_{III}$$-edge suggested that the oxidation state of U in the zircon sample with the highest radiation dose is tetravalent. The XANES spectra of the two other samples with lower radiation doses suggested a mixture of U(IV) and U(VI), while the possibility of U(V) was not excluded. This is the first work on the application of M$$_{V}$$-edge U XANES to the oxidation state of U in natural zircon.

Journal Articles

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

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

Photon Factory Activity Report 2018 (Internet), 2 Pages, 2019/00

no abstracts in English

Journal Articles

Mechanism of phase transfer of uranyl ions; A Vibrational sum frequency generation spectroscopy study on solvent extraction in nuclear reprocessing

Kusaka, Ryoji; Watanabe, Masayuki

Physical Chemistry Chemical Physics, 20(47), p.29588 - 29590, 2018/12

 Times Cited Count:6 Percentile:39.62(Chemistry, Physical)

Mechanistic understanding of solvent extraction of uranyl ions (UO$$_{2}$$$$^{2+}$$) by tributyl phosphate (TBP) will help improve the technology for the treatment and disposal of spent nuclear fuels. So far, it has been believed that uranyl ions in the aqueous phase are adsorbed to a TBP-enriched organic/aqueous interface, form complexes with TBP at the interface, and are extracted into the organic phase. Here we show that uranyl-TBP complex formation does not take place at the interface using vibrational sum frequency generation (VSFG) spectroscopy and propose an alternative extraction mechanism that uranyl nitrate, UO$$_{2}$$(NO$$_{3}$$)$$_{2}$$, passes through the interface and forms the uranyl-TBP complex, UO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(TBP)$$_{2}$$, in the organic phase.

Journal Articles

Effect of surface conditions of the filament used in thermal ionization mass spectrometry on an uranium isotopic measurement

Taguchi, Shigeo; Miyauchi, Hironari*; Horigome, Kazushi; Yamamoto, Masahiko; Kuno, Takehiko

Bunseki Kagaku, 67(11), p.681 - 686, 2018/11

In thermal ionization mass spectrometry, de-gassing is one of the important treatments to release impurities of filaments and to minimize the influence of background. In this work, the effect of the surface change in the tungsten filament induced by the conductively heating treatment on uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement has been investigated. It was found that the conductively heating treatment of the filament has the effect of smoothing the surface of the filament and also has the effect of improving the deposition of the sample on the filament surface. As a result of either these effects, the precision of uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement was improved.

Journal Articles

Separation technique using column chromatography for safeguards verification analysis of uranium and plutonium in highly-active liquid waste by isotope dilution mass spectrometry

Yamamoto, Masahiko; Taguchi, Shigeo; Horigome, Kazushi; Kuno, Takehiko

Proceeding IAEA Symposium on International Safeguards; Building Future Safeguards Capabilities (Internet), 8 Pages, 2018/11

In this study, the single-column extraction chromatographic separation has been developed for analysis of U and Pu in highly active liquid waste by isotope dilution mass spectrometry (IDMS). The commercially available TEVA$$^{textregistered}$$ resin is selected as an extraction chromatography resin. The U is chromatographically separated from fission products (FP) elements by nitric acid while Pu(IV) is adsorbed on the resin. After that, Pu is eluted by reducing to Pu(III). The method has been successfully achieved the separation with yielding the enough recovery and sufficient decontamination factors for subsequent IDMS analysis. The column dose rate after the FP removal is decreased to the background. The analytical results obtained by the developed method are in a good agreement with those of the conventional method. It provides simple and rapid separation and expected that the method can be applied to join IAEA/Japan on-site analytical laboratory.

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