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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

Behavior of light elements in iron-silicate-water-sulfur system during early Earth's evolution

Iizuka, Riko*; Goto, Hirotada*; Shito, Chikara*; Fukuyama, Ko*; Mori, Yuichiro*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; Kagi, Hiroyuki*

Scientific Reports (Internet), 11(1), p.12632_1 - 12632_10, 2021/06

 Times Cited Count:0 Percentile:0.01(Multidisciplinary Sciences)

The Earth's core consist of Fe-Ni alloy with some light elements (H, C, O, Si, S etc.). Hydrogen (H) is the most abundant element in the universe and one of the promising candidates. In this study, we have investigated the effects of sulfur(S) on hydrogenation of iron-hydrous silicate system containing saturated water in the ideal composition of the primitive Earth. We observed a series of phase transitions of Fe, dehydration of the hydrous mineral, and formation of olivine and enstatite with increasing temperature. The FeS formed as the coexisting phase of Fe under high-pressure and temperature condition, but its unit cell volume did not increase, suggesting that FeS is hardly hydrogenated. Recovered samples exhibited that H and S can be incorporated into solid Fe, which lowers the melting temperature as Fe(H$$_{x}$$)-FeS system. No detection of other light elements (C, O, Si) in solid Fe suggests that they dissolve into molten iron hydride and/or FeS in the later process of Earth's core-mantle differentiation.

Journal Articles

Study on gamma-ray-degradation of adsorbent for low pressure-loss extraction chromatography

Miyazaki, Yasunori; Sano, Yuichi; Okamura, Nobuo; Watanabe, Masayuki; Koka, Masashi*

QST-M-29; QST Takasaki Annual Report 2019, P. 72, 2021/03

no abstracts in English

Journal Articles

Structural characterization of Eu-HONTA complexes by IBIL and EXAFS analyses

Watanabe, So; Sano, Yuichi; Okada, Makoto*; Matsuura, Haruaki*; Hagura, Naoto*; Kada, Wataru*

Nuclear Instruments and Methods in Physics Research B, 477, p.60 - 65, 2020/08

 Times Cited Count:1 Percentile:0.02(Instruments & Instrumentation)

IBIL and EXAFS analyses were applied on strucutral analysis of Eu complex formed in adsorbent developed for extraction chromatography. Those analyses revealed slight structural difference between adsorbent and solvent systems.

Journal Articles

Structure refinement of black phosphorus under high pressure

Akahama, Yuichi*; Miyakawa, Masashi*; Taniguchi, Takashi*; Sano, Asami; Machida, Shinichi*; Hattori, Takanori

Journal of Chemical Physics, 153(1), p.014704_1 - 014704_5, 2020/07

 Times Cited Count:2 Percentile:45.83(Chemistry, Physical)

The structure refinement of black phosphorus was performed at pressures of up to 3.2 GPa at room temperature by powder neutron diffraction techniques. The bond lengths and bond angles between the phosphorus atoms at pressures were precisely determined and confirmed to be consistent with those of the previous single crystal X-ray analysis [Brown and Randqvist, Acta Cryst. 19, 684 (1965)]. Although lattice parameters exhibited an anisotropic compressibility, the covalent P1-P2 and P1-P3 bond lengths were almost independent of pressure and only the P3-P1-P2 bond angle was reduced significantly. On the basis of our results, the significant discrepancy in the bond length reported by Cartz et al. [J. Chem. Phys. 71, 1718 (1979)] has been solved. Our structural data will contribute to the elucidation of the Dirac semimetal state of black phosphorus under high pressure.

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:0 Percentile:0(Chemistry, Analytical)

Journal Articles

Structure change of monoclinic ZrO$$_{2}$$ baddeleyite involving softenings of bulk modulus and atom vibrations

Fukui, Hiroshi*; Fujimoto, Manato*; Akahama, Yuichi*; Sano, Asami; Hattori, Takanori

Acta Crystallographica Section B; Structural Science, Crystal Engineering and Materials (Internet), 75(4), p.742 - 749, 2019/08

 Times Cited Count:2 Percentile:39.26(Chemistry, Multidisciplinary)

Monoclinic ZrO$$_{2}$$ baddeleyite exhibits anomalous softenings of bulk modulus and atom vibrations with compression. We have investigated the pressure evolution of the structure by neutron powder diffraction combined with ab-initio calculations. The present results showed that the anomalous pressure response of the bulk modulus is related not to the change in the bonding characters but to the deformation of an oxygen sublattice, especially one of layers made of oxygens in the crystallographic $$a$$* plane. The layer consists of two parallelograms; one is rotating with little distortion and the other is being distorted with increasing pressure. This deformation of this layer makes one of Zr-O distances long, resulting in the softening of some atom vibrational modes.

Journal Articles

Effect of seawater components on corrosion behavior of SUS316L in nitric acid solution containing metal ions

Ambai, Hiromu; Nishizuka, Yusuke*; Sano, Yuichi; Uchida, Naoki; Iijima, Shizuka; Shiwaku, Hideaki; Yaita, Tsuyoshi

Journal of Nuclear Science and Technology, 56(2), p.193 - 200, 2019/02

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

During the accident that occurred at the Fukushima Daiichi Nuclear Power Plant, a large volume of seawater was introduced as coolant into the storage pools for spent nuclear fuel. If this fuel is reprocessed, some components of seawater will be mixed with the nitric acid solution containing metal ions in the reprocessing process where stainless steels are used as structural material. In this study, we investigated the effect of seawater components in high active liquid waste (HAW) containing nitric acid and metal ions as fission products on the corrosion behavior of SUS316L stainless steel. Corrosion tests were conducted in surrogate HAW containing artificial seawater (ASW). Intergranular corrosion was observed in the HAW with ASW, where Ru increased the corrosion potential to the transpassive region. An increase in the amount of ASW led to a decrease in the corrosion rate and suppression of intergranular corrosion. Interactions between Ru ions and seawater components, such as chloride ions, were indicated by the results of extended Xray absorption fine structure spectroscopy and cyclic voltammetry analyses of the solution containing ASW and HAW.

Journal Articles

Influences of pore and particle sizes of CMPO/SiO$$_{2}$$-P adsorbent on extraction chromatography process

Watanabe, So; Sano, Yuichi; Sanda, Shuhei*; Sakurai, Shota*; Arai, Tsuyoshi*

Nihon Ion Kokan Gakkai-Shi, 30(1), p.8 - 16, 2019/01

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

Electrochemical properties of zirconium in highly concentrated plutonium nitrate solution

Nakahara, Masaumi; Sano, Yuichi; Abe, Hitoshi

Progress in Nuclear Science and Technology (Internet), 5, p.52 - 55, 2018/11

For evaluating the secular change of Pu evaporator made of Zr in the commercialized nuclear fuel reprocessing plant, electrochemical experiments were carried out with Pu nitrate solutions. The open circuit potentials of Zr increased with increasing Pu, HNO$$_{3}$$ concentrations and temperature. However, these experimental results imply that Zr has high corrosion resistance in Pu nitrate solutions.

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:4 Percentile:47(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:0 Percentile:0(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:1 Percentile:8.4(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

Effect of Ru chemical form on corrosion behavior of structural materials in spent fuel reprocessing process

Sano, Yuichi; Ambai, Hiromu; Takahatake, Yoko

Aichi Shinkurotoron Hikari Senta 2017-Nendo Kokyoto Riyo Seika Hokokusho (Internet), 1 Pages, 2018/00

In order to elucidate the mechanism of corrosion in the reprocessing process and propose a method for suppressing corrosion, the effect of coexisting substances on the chemical form of Ru in nitric acid solution containing seawater components was evaluated. The result of XAFS measurement for Ru showed the structural change around a Ru atom due to the interaction with chloride ion, which will suppress the corrosion promoting action of Ru in nitric acid solution.

JAEA Reports

Proceedings of the Research Conference on Cementitious Composites in Decommissioning and Waste Management (RCWM2017); June 20th and 21st, 2017, Tomioka Town Art&Media Center, Tomioka, Futaba, Fukushima, Japan

Sano, Yuichi; Ashida, Takashi

JAEA-Review 2017-021, 180 Pages, 2017/11

JAEA-Review-2017-021.pdf:86.98MB

Collaborative Laboratories for Advanced Decommissioning Science (CLADS) is responsible to promote international cooperation in the R&D activities on the decommissioning of Fukushima Daiichi Nuclear Power Station and to develop the necessary human resources. CLADS held the Research Conference on Cementitious Composites in Decommissioning and Waste Management (RCWM2017) on 20th and 21st June, 2017. This report compiles the abstracts and the presentation materials in the above conference.

Journal Articles

Microanalysis of silica-based adsorbent for effective recovery of radioactive elements

Sano, Yuichi; Watanabe, So; Matsuura, Haruaki*; Nagoshi, Kohei*; Arai, Tsuyoshi*

Journal of Nuclear Science and Technology, 54(10), p.1058 - 1064, 2017/10

 Times Cited Count:3 Percentile:41.49(Nuclear Science & Technology)

For effective recovery of radioactive elements by adsorbents using polymer-immobilized silica (SiO$$_{2}$$-P) supports, the microstructure of SiO$$_{2}$$-P particles impregnated with CMPO as extractants and their change with the crosslinking degree of polymer (CDP) were investigated using STXM and EXAFS analyses; further, their relation with adsorption/elution behavior was discussed. The adsorption/elution tests using adsorbents with a different CDP demonstrated that a higher CDP inhibited the elution of adsorbed metal ions from the adsorbent. The results of STXM and EXAFS analyses suggested that adsorption by CMPO proceeds through the entire area in the adsorbent and the local structure around adsorbed metal ions is similar irrespective of the CDP. Conversely, STXM analyses implied the capture of eluents such as H$$_{2}$$O by polymers with high CDP, which suppresses the prompt elution of adsorbed metal ions from the adsorbent.

262 (Records 1-20 displayed on this page)