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

https://doi.org/10.1007/s10967-022-08658-7

Development of MA separation process with TEHDGA/SiO-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

https://doi.org/10.1007/s10967-021-07940-4

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.

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

https://doi.org/10.1038/s41598-021-91801-3

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)-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.

Neutron diffraction study of hydrogen site occupancy in FeSi at 14.7 GPa and 800 K

Mori, Yuichiro*; Kagi, Hiroyuki*; Kakizawa, Sho*; Komatsu, Kazuki*; Shito, Chikara*; Iizuka, Riko*; Aoki, Katsutoshi*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; et al.

Journal of Mineralogical and Petrological Sciences, 116(6), p.309 - 313, 2021/00

https://doi.org/10.2465/jmps.210825

The Earth's core is believed to contain some light elements because it is 10% less dense than pure Fe under the corresponding pressure and temperature conditions. Hydrogen, a promising candidate among light elements, has phase relations and physical properties that have been investigated mainly for the Fe-H system. This study specifically examined an Fe-Si-H system using in-situ neutron diffraction experiments to investigate the site occupancy of deuterium of hcp-FezSi hydride at 14.7 GPa and 800 K. Results of Rietveld refinement indicate hcp-FeSi hydride as having deuterium (D) occupancy of 0.24(2) exclusively at the interstitial octahedral site in the hcp lattice. The effect on the site occupancy of D by addition of 2.6 wt% Si into Fe (FeSi) was negligible compared to results obtained from an earlier study of an Fe-D system (Machida et al., 2019).

Influence of plutonyl ion on electrochemical characterization of zirconium in plutonium nitrate solutions

Nakahara, Masaumi; Sano, Yuichi; Nomura, Kazunori

Radiochimica Acta, 108(9), p.701 - 706, 2020/09

https://doi.org/10.1515/ract-2019-3228

To evaluate the corrosion behavior of a Pu evaporator made from Zr in a reprocessing plant, the influence of PuO was investigated with Pu nitrate solutions in electrochemical experiments. The maximum open circuit potential of Zr in the Pu nitrate solution was approximately 1 V in the Pu nitrate solution containing 7 mol dm HNO. However, there were no significant changes at high PuO concentrations, and Zr showed high corrosion resistance under our experimental conditions.

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

https://doi.org/10.1063/5.0012870

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.

Structure change of monoclinic ZrO 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

https://doi.org/10.1107/S2052520619007923

Monoclinic ZrO 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 * 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.

Influences of pore and particle sizes of CMPO/SiO-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

https://doi.org/10.5182/jaie.30.8

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

https://doi.org/10.15669/pnst.5.52

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 concentrations and temperature. However, these experimental results imply that Zr has high corrosion resistance in Pu nitrate solutions.

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

https://doi.org/10.1252/kakoronbunshu.44.285

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.