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 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 / 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 / HONTA - n-dodecane system are under 10 m/s.

Spallation and fragmentation cross sections for 168 MeV/nucleon Xe ions on proton, deuteron, and carbon targets

Sun, X. H.*; Wang, H.*; Otsu, Hideaki*; Sakurai, Hiroyoshi*; Ahn, D. S.*; Aikawa, Masayuki*; Fukuda, Naoki*; Isobe, Tadaaki*; Kawakami, Shunsuke*; Koyama, Shumpei*; et al.

Physical Review C, 101(6), p.064623_1 - 064623_12, 2020/06

https://doi.org/10.1103/PhysRevC.101.064623

The spallation and fragmentation reactions of Xe induced by proton, deuteron and carbon at 168 MeV/nucleon were studied at RIKEN Radioactive Isotope Beam Factory via the inverse kinematics technique. The cross sections of the lighter products are larger in the carbon-induced reactions due to the higher total kinetic energy of carbon. The energy dependence was investigated by comparing the newly obtained data with previous results obtained at higher reaction energies. The experimental data were compared with the results of SPACS, EPAX, PHITS and DEURACS calculations. These data serve as benchmarks for the model calculations.

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

https://doi.org/10.1007/s10967-019-06808-y

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

https://doi.org/10.1252/kakoronbunshu.44.335

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.

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

https://euronuclear.org/events/topfuel/topfuel2018/fullpapers/TopFuel2018-A0080-fullpaper.pdf

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 60C, 80C 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.

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- 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.

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

https://doi.org/10.1007/s10967-018-5853-x

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

https://doi.org/10.1252/kakoronbunshu.44.135

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.

Mizunami Underground Research Laboratory Project, Annual report for fiscal year 2016

Ishibashi, Masayuki; Hama, Katsuhiro; Iwatsuki, Teruki; Matsui, Hiroya; Takeuchi, Ryuji; Nohara, Tsuyoshi; Onoe, Hironori; Ikeda, Koki; Mikake, Shinichiro; Iyatomi, Yosuke; et al.

JAEA-Review 2017-026, 72 Pages, 2018/01

JAEA-Review-2017-026.pdf:18.23MB

The Mizunami Underground Research Laboratory (MIU) project is being pursued by the Japan Atomic Energy Agency (JAEA) to enhance the reliability of geological disposal technologies through investigations of the deep geological environment in the crystalline host rock (granite) at Mizunami, Gifu Prefecture, central Japan. On the occasion of the research program and management system revision of the entire JAEA organization in 2014, JAEA identified three important issues on the geoscientific research program: "Development of countermeasure technologies for reducing groundwater inflow", "Development of modeling technologies for mass transport" and "Development of drift backfilling technologies", based on the latest results of the synthesizing research and development (R&D). The R&D on three important issues have been carrying out on the MIU project. In this report, the current status of R&D activities and construction in 2016 is summarized.

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

https://doi.org/10.1016/j.jnucmat.2017.07.008

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 95C. The corrosion rate exponentially decreased with effective solute chromium concentration (Cr) 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 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, concentrated nitric acid and addition of oxidizing ions helped to prevent the active dissolution, and suppressed the corrosion rate.