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Journal Articles

Ion beam induced luminescence analysis of europium complexes in styrene-divinylbenzene copolymer-coated spherical silica by proton and argon ion beams irradiation

Nakahara, Masaumi; Watanabe, So; Takeuchi, Masayuki; Yuyama, Takahiro*; Ishizaka, Tomohisa*; Ishii, Yasuyuki*; Yamagata, Ryohei*; Yamada, Naoto*; Koka, Masashi*; Kada, Wataru*; et al.

Nuclear Instruments and Methods in Physics Research B, 542, p.144 - 150, 2023/09

 Times Cited Count:0 Percentile:0.02(Instruments & Instrumentation)

The structures of Eu complexes in the adsorbents prepared with various extractants were evaluated by ion beam induced luminescence analysis in an extraction chromatography for minor actinides recovery. The luminescence of Eu was measured with a proton beam obtained from the single-ended accelerator and an argon ion beam obtained from the azimuthally varying field cyclotron in Takasaki Ion Accelerators for Advanced Radiation Application in National Institutes for Quantum Science and Technology. In this study, it was confirmed that the spectral shape of Eu complexes in the adsorbents varied depending on the kinds of extractants, and the correlation between the change in the spectra and the structures of Eu complexes was investigated.

Journal Articles

Development of engineering scale extraction chromatography separation system, 2; Spray drying granulation of silica support for adsorbent

Hasegawa, Kenta; Goto, Ichiro*; Miyazaki, Yasunori; Ambai, Hiromu; Watanabe, So; Watanabe, Masayuki; Sano, Yuichi; Takeuchi, Masayuki

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 5 Pages, 2023/05

Journal Articles

Design of MA(III)/Ln(III) separation process of extraction chromatography technology

Akuzawa, Tadashi*; Kim, S.-Y.*; Kubota, Masahiko*; Wu, H.*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5851 - 5858, 2022/12

 Times Cited Count:3 Percentile:31.61(Chemistry, Analytical)

Journal Articles

Sodium-cooled Fast Reactors

Ohshima, Hiroyuki; Morishita, Masaki*; Aizawa, Kosuke; Ando, Masanori; Ashida, Takashi; Chikazawa, Yoshitaka; Doda, Norihiro; Enuma, Yasuhiro; Ezure, Toshiki; Fukano, Yoshitaka; et al.

Sodium-cooled Fast Reactors; JSME Series in Thermal and Nuclear Power Generation, Vol.3, 631 Pages, 2022/07

This book is a collection of the past experience of design, construction, and operation of two reactors, the latest knowledge and technology for SFR designs, and the future prospects of SFR development in Japan. It is intended to provide the perspective and the relevant knowledge to enable readers to become more familiar with SFR technology.

Journal Articles

Acid dissociation constant of bis(2-ethylhexyl) hydrogen phosphate impregnated in a polymer layer coated on silica microparticles

Miyagawa, Akihisa*; Takeuchi, Masayuki; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Nakatani, Kiyoharu*

Bulletin of the Chemical Society of Japan, 95(4), p.566 - 568, 2022/04

 Times Cited Count:3 Percentile:42.81(Chemistry, Multidisciplinary)

We demonstrate that pKa of extractant impregnated in a polymer phase varies with the cross-linking degree and the coexistence of other extractants, which induces a change in the hydrophobicity of the polymer phase. The results presented herein will be beneficial for the development of novel solid-extraction adsorbents.

Journal Articles

Development of MA separation process with TEHDGA/SiO$$_{2}$$-P for an advanced reprocessing

Horiuchi, Yusuke; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Kida, Fukuka*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.237 - 244, 2021/10

 Times Cited Count:6 Percentile:65.59(Chemistry, Analytical)

Applicability of tetra2-ehylhexyl diglycolamide (TEHDGA) impregnated adsorbent for minor actinide (MA) recovery from high level liquid waste (HLLW) in extraction chromatography technology was investigated through batch-wise adsorption and column separation experiments. Distribution ratio of representative fission product elements were obtained by the batch-wise experiments, and TEHDGA adsorbent was shown to be preferable to TODGA adsorbent for decontamination of several species. All Ln(III) supplied into the TEHDGA adsorbent packed column was properly eluted from the column, and the applicability of the adsorbent was successfully showed by this study.

JAEA Reports

Evaluation of the mass transfer coefficients for the minor actinide separation; Evaluation by the single drop method

Sakamoto, Atsushi; Kibe, Satoshi*; Kawanobe, Kazunori*; Fujisaku, Kazuhiko*; Sano, Yuichi; Takeuchi, Masayuki; Suzuki, Hideya*; Tsubata, Yasuhiro; Ban, Yasutoshi; Matsumura, Tatsuro

JAEA-Research 2021-003, 30 Pages, 2021/06

JAEA-Research-2021-003.pdf:1.81MB

Japan Atomic Energy Agency has been developing a solvent extraction process called SELECT to recover minor actinides (MA) from spent nuclear fuel. In the SELECT process, TDdDGA, HONTA, and ADAAM are used as the extractants for MA + Ln corecovery, MA/Ln separation and Am/Cm separation, respectively. These extractants do not contain phosphorus (P), and consist of carbon (C), hydrogen (H), oxygen (O), and nitrogen (N). In this study, in order to give beneficial information for designing flowsheet, the mass transfer coefficients of Ln between HNO$$_{3}$$ solution and TDdDGA or HONTA / n-dodecane solvent were evaluated by the single drop technique. Prior to the evaluation of mass transfer coefficient, we had optimized the structure of the single drop apparatus to improve accuracy of the measurement. Based on the mass transfer coefficients obtained in HNO$$_{3}$$ / TDdDGA-n-dodecane system, Ln behaviors in the counter-current extraction and back-extraction using mixer-settlers and centrifugal contactors were estimated by simple calculation, and they had a good agreement with our previous experimental results. We also confirmed the mass transfer coefficients of Ln in HNO$$_{3}$$ / HONTA - n-dodecane system are under 10$$^{-6}$$ m/s.

Journal Articles

Improvement in flow-sheet of extraction chromatography for trivalent minor actinides recovery

Watanabe, So; Senzaki, Tatsuya; Shibata, Atsuhiro; Nomura, Kazunori; Takeuchi, Masayuki; Nakatani, Kiyoharu*; Matsuura, Haruaki*; Horiuchi, Yusuke*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 322(3), p.1273 - 1277, 2019/12

 Times Cited Count:4 Percentile:31.89(Chemistry, Analytical)

Journal Articles

Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

Otaka, Toshiki*; Sato, Tatsumi*; Ono, Shimpei; Nagoshi, Kohei; Abe, Ryoji*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Nakatani, Kiyoharu*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

 Times Cited Count:9 Percentile:40.49(Chemistry, Analytical)

Journal Articles

Simulation of fluidity, dispersion and mass transfer in an annular centrifugal contactor

Sano, Yuichi; Sakamoto, Atsushi; Takeuchi, Masayuki; Misumi, Ryuta*; Kunii, Kanako*; Todoroki, Kei*; Nishi, Kazuhiko*; Kaminoyama, Meguru*

Kagaku Kogaku Rombunshu, 44(6), p.335 - 340, 2018/11

Concerning an annular centrifugal contactor which has high throughput and separation performance, the effect of operational condition on fluidic and dispersion behavior, which are important to improve the contactor performance, was investigated by computational fluid dynamics (CFD) analysis based on the turbulence model, and the calculated results were validated by experimental data. The liquid phase in the annular zone was gradually divided into two regions vertically with increasing the rotor speed and decreasing the flowrate, and the liquid flow moved toward the center of the housing bottom was generated in the lower annular zone under any operational condition. The droplet size of the dispersed phase in the annular zone decreased with increasing the rotor speed and decreasing the flowrate. These calculation results showed a good agreement with experimental data. The CFD analysis considering mass transfer between aqueous and organic phases was also attempted, and it was confirmed that the change of extraction performance with the rotor speed showed the same tendency as the experimental result.

Journal Articles

Characteristics of TPDN/SiO$$_{2}$$-P adsorbent for MA(III) recovery

Kofuji, Hirohide; Watanabe, So; Takeuchi, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.61 - 65, 2018/11

Journal Articles

Corrosion behaviour of FeCrAl-ODS steels in nitric acid solutions with several temperatures

Takahatake, Yoko; Ambai, Hiromu; Sano, Yuichi; Takeuchi, Masayuki; Koizumi, Kenji; Sakamoto, Kan*; Yamashita, Shinichiro

Proceedings of Annual Topical Meeting on Reactor Fuel Performance (TopFuel 2018) (Internet), 9 Pages, 2018/10

The corrosion behaviour of FeCrAl-ODS steels for the accident tolerant fuel cladding of LWRs were investigated in nitric acid solutions for the reprocessing process of spent fuels. The corrosion tests were carried out at 60$$^{circ}$$C, 80$$^{circ}$$C and the boiling point of the solutions, and the specimens were then analysed by XPS. The corrosion remarkably progressed at the boiling point, and the highest corrosion rate was 0.22 mm/y. In the oxide film, the atomic concentration of Fe was lower, than that in the base material, and those of Cr and Al were higher. The results show that the corrosion of FeCrAl-ODS steels in hot nitric acid solution is not severe because of the high corrosion resistance of the oxide film formed on the material; hence, the corrosion resistance of the new cladding materials in the dissolution process of spent fuel is acceptable for reprocessing operations.

Journal Articles

Flow behavior in annular centrifugal extractors with different vessel sizes

Misumi, Ryuta*; Todoroki, Kei*; Kunii, Kanako*; Nishi, Kazuhiko*; Kaminoyama, Meguru*; Sano, Yuichi; Sakamoto, Atsushi; Takeuchi, Masayuki

Kagaku Kogaku Rombunshu, 44(5), p.285 - 291, 2018/09

Annular centrifugal extractors have been anticipated for use as extractors in spent nuclear fuel recycling. The extraction rate and the liquid-liquid dispersion are related to the flow pattern in the vessel. However, no study has clarified flow patterns in vessels of various scales. For this study, flow pattern characteristics are quantified for extractors of two scales. An extractor has a mixing zone around the vessel bottom and a separation zone in the cylindrical rotor. For this experiment, distilled water was fed into the vessel. Flow behavior in the mixing zone was observed from a side view using a digital video camera at various rotor speeds and supply flow rates for extractors of two scales. In some cases, the liquid horizontal velocity vectors in the mixing zone were measured using particle image velocimetry. Results demonstrate that flow behaviors in the mixing zone in both scales of extractors are classifiable as three types, changing with operational conditions: Type A, Type B, and a Transition regime. For the Type A state, the mixing zone is fully filled with liquid from the vessel bottom up to the lower edge of the rotor. In the Type B state, the zone with existing liquid is vertically divisible into two regions. Lower rotor speeds and higher flow rates tend to produce Type A state flow behavior. The boundary operational condition between Type A and the Transition regime are correlated with the normalized supply flow rate and pumping capacity of the rotor, which is evaluated from liquid surface level in a rotor formed by centrifugal force. Furthermore, the fluid velocity in the mixing zone is roughly proportional to the rotor surface circumferential speed irrespective of the vessel scale.

Journal Articles

CFD analysis for U extraction in a centrifugal contactor

Sano, Yuichi; Sakamoto, Atsushi; Kofuji, Hirohide; Takeuchi, Masayuki

Proceedings of 21st Pacific Basin Nuclear Conference (PBNC 2018) (USB Flash Drive), p.314 - 318, 2018/09

The effect of operational condition of the annular centrifugal contactor (ACC) on U extraction behavior was investigated by computational fluid dynamics (CFD) analysis considering mass transfer between aqueous and organic phases, and the calculation results were validated experimentally. The CFD analysis with ANSYS FLUENT was carried out using the Eulerian multi-fluid approach with a standard k-$$varepsilon$$ turbulence model. In order to calculate the droplet size of the dispersed phase and mass transfer between aqueous and organic phases, user-defined functions (UDF) were created. The changes of U extraction performance, i.e. U stage efficiency, with the rotor speed and the O/A ratio (= organic flowrate / aqueous flowrate) were calculated, and these showed a good agreement with experimental results.

Journal Articles

Am, Cm recovery from genuine HLLW by extraction chromatography

Watanabe, So; Sano, Yuichi; Kofuji, Hirohide; Takeuchi, Masayuki; Shibata, Atsuhiro; Nomura, Kazunori

Journal of Radioanalytical and Nuclear Chemistry, 316(3), p.1113 - 1117, 2018/06

 Times Cited Count:9 Percentile:62.99(Chemistry, Analytical)

Journal Articles

Rotor speed and supply flow rate effects on flow behavior in an annular centrifugal extractor

Misumi, Ryuta*; Kunii, Kanako*; Todoroki, Kei*; Nishi, Kazuhiko*; Kaminoyama, Meguru*; Sano, Yuichi; Sakamoto, Atsushi; Takeuchi, Masayuki

Kagaku Kogaku Rombunshu, 44(3), p.135 - 141, 2018/05

 Times Cited Count:1 Percentile:4.87(Engineering, Chemical)

Annular centrifugal extractors have been used in spent nuclear fuel reprocessing, but the relation between the extraction rate and flow pattern in the vessel remains unclear. This study quantifies characteristics of the flow pattern to clarify this relation. An extractor produces a mixing zone around the vessel bottom and a separation zone in the rotor. The horizontal velocity of the liquid in the mixing zone was measured using particle image velocimetry at various rotor speeds and supply flow rates. Flow behaviors in the mixing zone are of three types, changing with operational conditions: Type A, Type B, and a transition regime. At lower rotor speeds and high supply flow rates, the mixing zone is fully filled with liquid from the vessel bottom up to the lower edge of the rotor: the Type A flow state. At high rotor speeds and low supply flow rates, the zone with existing liquid is vertically divisible into two regions: near the vanes and around the bottom of the rotor, which is the Type B flow state. A transition regime is also observed between Type A and Type B state. In each region surrounding the two vanes on the vessel bottom and the vessel wall, the liquid flowed in the direction of rotor rotation along the vessel wall. Liquid flow altered by the vane flowed toward the center of vessel bottom. The liquid then entered the separation zone through the orifice at the rotor bottom. For the Type A state, the horizontal velocity distribution was roughly proportional to the rotor speed. For the Type B state, the horizontal velocities around the vessel bottom were lower than those of Type A and were not proportional to the rotor speed. Presumably, the liquid fed into the vessel went directly to the rotor instead of passing between the two vanes attached to the vessel bottom.

Journal Articles

Partitioning of plutonium by acid split method with dissolver solution derived from irradiated fast reactor fuel with high concentration of plutonium

Nakahara, Masaumi; Sano, Yuichi; Nomura, Kazunori; Takeuchi, Masayuki

Journal of Chemical Engineering of Japan, 51(3), p.237 - 242, 2018/03

 Times Cited Count:2 Percentile:9.06(Engineering, Chemical)

For evaluating the Pu partitioning behavior under the condition of high Pu concentration in the feed solution by the acid split method, the counter current experiment was carried out. The Pu content in the U/Pu product was 1.51 times higher than that in the feed solution. In the Pu partitioning section, Pu polymerization and third phase formation were observed, and the operation of centrifugal contactors was stable.

Journal Articles

Corrosion behavior of ODS steels with several chromium contents in hot nitric acid solutions

Tanno, Takashi; Takeuchi, Masayuki; Otsuka, Satoshi; Kaito, Takeji

Journal of Nuclear Materials, 494, p.219 - 226, 2017/10

BB2016-1307.pdf:0.6MB

 Times Cited Count:17 Percentile:85.35(Materials Science, Multidisciplinary)

Oxide dispersion strengthened (ODS) steel cladding tubes have been developed for fast reactors. 9 chromium ODS and 11Cr-ODS tempered martensitic steels are prioritized for the candidate material in research being carried out at JAEA. In this work, fundamental immersion tests and electro-chemical tests of 9 to 12Cr-ODS steels were systematically conducted in various nitric acid solutions at 95$$^{circ}$$C. The corrosion rate exponentially decreased with effective solute chromium concentration (Cr$$_{eff}$$) and nitric acid concentration. Addition of oxidizing ions also suppressed the corrosion rate. According to polarization curves and surface observations in this work, the combination of low Cr$$_{eff}$$ and dilute nitric acid could not prevent the active dissolution at the beginning of immersion, and the corrosion rate was high. In comparison, higher Cr$$_{eff}$$, concentrated nitric acid and addition of oxidizing ions helped to prevent the active dissolution, and suppressed the corrosion rate.

Journal Articles

Micro-PIXE analysis on adsorbent of extraction chromatography for MA(III) recovery

Takahatake, Yoko; Watanabe, So; Kofuji, Hirohide; Takeuchi, Masayuki; Nomura, Kazunori; Sato, Takahiro*

International Journal of PIXE, 26(3&4), p.73 - 83, 2017/09

BB2016-1248.pdf:0.36MB

JAEA has been conducting research and development of MA(III) recovery from HLLW by extraction chromatography technology for reduction in amount and environmental impact of radioactive waste. The behavior of adsorbed cations inside the adsorbent packed in a column is necessary to be evaluated for improvement of the adsorbent or flow-sheet to achieve targeted MA(III) recovery performance. In this paper, micro-PIXE analysis was carried out on the particles sampled from various positions of the column to reveal the behavior of cations inside the packed column with CMPO/SiO $$_{2}$$-P adsorbent. Simple experiment and data analysis were shown to be effective to reveal inside of the column, and formation and transportation of the adsorption bands were observed for some cations which are extractable by the CMPO extractant. Some part of Zr(IV) and Mo(VI) were found to remain inside the column without distinct transportation even after the elution operation.

Journal Articles

Effect of chloride ion on corrosion behavior of SUS316L-grade stainless steel in nitric acid solutions containing seawater components under $$gamma$$-ray irradiation

Sano, Yuichi; Ambai, Hiromu; Takeuchi, Masayuki; Iijima, Shizuka; Uchida, Naoki

Journal of Nuclear Materials, 493, p.200 - 206, 2017/09

 Times Cited Count:7 Percentile:56.89(Materials Science, Multidisciplinary)

Concerning the Fukushima Daiichi Nuclear Power Plant accident, we investigated the effect of chloride ion on the corrosion behavior of SUS316L stainless steel, which is a typical material for the equipment used in reprocessing, in HNO$$_{3}$$ solution containing seawater components, including under the $$gamma$$-ray irradiation condition. Electrochemical and immersion tests were carried out using a mixture of HNO$$_{3}$$ and artificial seawater (ASW). In the HNO$$_{3}$$ solution containing high amounts of ASW, the cathodic current densities increased and uniform corrosion progressed. This might be caused by strong oxidants, such as Cl$$_{2}$$ and NOCl, generated in the reaction between HNO$$_{3}$$ and Cl$$^{-}$$ ions. The corrosion rate decreased with the immersion time at low concentrations of HNO$$_{3}$$, while it increased at high concentrations. Under the $$gamma$$-ray irradiation condition, the corrosion rate decreased due to the suppression of the cathodic reactions by the reaction between the above oxidants and HNO$$_{2}$$ generated by radiolysis.

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