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Journal Articles

Neutron scattering study of antiferromagnet U$$_{2}$$Pt$$_{6}$$Al$$_{15}$$

Ota, Kyugo*; Matsumoto, Yuji*; Watabe, Yuki*; Kaneko, Koji; Tabata, Chihiro; Haga, Yoshinori

New Physics; Sae Mulli, 73(12), p.1170 - 1173, 2023/12

https://doi.org/10.3938/NPSM.73.1170

We have performed the neutron scattering study of antiferromagnet U$$_{2}$$Pt$$_{6}$$Al$$_{15}$$ with the honeycomb lattice to determine the magnetic structure. U$$_{2}$$Pt$$_{6}$$Al$$_{15}$$ exhibits two phase transitions at $$T_{rm m1}$$ = 9 K and $$T_{rm m2}$$ = 26 K. In phase I at $$T_{rm m1}$$ $$<$$ $$T$$ $$<$$ $$T_{rm m2}$$, the magnetic reflections described by a propagation vector $$kappa$$$$_{rm I}$$ = (1/3, 0, 0) were observed. In phase II at $$T$$ $$<$$ $$T_{rm m1}$$, magnetic reflections of $$kappa$$$$_{rm I}$$ = (1/3, 0, 0) and $$kappa$$$$_{rm II}$$ = (1/2, 0, 0) were observed and the magnetic reflection intensity of $$kappa$$$$_{rm I}$$ = (1/3, 0, 0) is weak but finite. The hysteresis in the temperature dependent intensities is observed across the phase transition at $$T_{rm m1}$$, suggesting that the transition at $$T_{rm m1}$$ is of first order.

Journal Articles

Mutual separation of Am and Cm using ADAAM (alkyl DiAmide AMine) and reduction of volumes for liquid waste generated via batch-wise multistage extractions

Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Suzuki, Hideya*

Journal of Nuclear Science and Technology, 11 Pages, 2023/11

https://doi.org/10.1080/00223131.2023.2283214
 Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)

The mutual separation of Am and Cm is conducted using an alkyl-diamide amine (ADAAM) extractant. ADAAM exhibits extremely high separation factor with respect to Am and Cm separation (5.9) in a nitric acid-$$n$$-dodecane system. The batch-wise multistage extractions are performed using a system containing 0.2 M ADAAM and 1.5 M nitric acid. In this multistage extraction, an organic solvent give 96.5% and 1.06% yields of Am and Cm. After the mutual separation of Am and Cm, an additional extraction step is included to reduce the volumes of these aqueous and organic phases. Taking these steps, Am and Cm can be recovered in just two or three stages in the aqueous phases.

Journal Articles

Extraction of Rh(III) from hydrochloric acid by protonated NTAamide(C6) and analogous compounds and understanding of extraction equilibria by using UV spectroscopy and DFT calculations

Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Kinoshita, Ryoma; Matsumiya, Masahiko*; Shinoku, Kota*; Shiroishi, Hidenobu*

Analytical Sciences, 39(9), p.1575 - 1583, 2023/09

https://doi.org/10.1007/s44211-023-00376-8
 Times Cited Count：0 Percentile：0(Chemistry, Analytical)

Extraction of Rh from HCl can be performed by NTAamide(C6) (hexahexyl-nitrilotriacetamide) and other related compounds into n-dodecane. We use ion-pair extraction of anionic species of Rh-chloride and protonated extractant. Rh behave as anion in hydrochloric acid and the tertiary nitrogen atom in extractant may be protonated to produce the quaternary amine in acidic condition. From the present work, the maximum distribution ratio of Rh(III) is 16. The D(Rh) values are changeable during preparation of the aqueous solutions because different Rh-Cl-H$$_{2}$$O complexes are formed in HCl media and show the slow exchange rate between Cl and H$$_{2}$$O. Using the UV spectrum, Rh-chloride solution having the peak of spectrum at 504 nm can be extracted effectively, where RhCl$$_{4}$$(H$$_{2}$$O)$$^-$$ and RhCl$$_5$$(H$$_2$$O)$$^2$$$$^-$$ exist mainly from DFT calculation. Stoichiometry of one-one complex of Rh and NTAamide is obtained from slope analysis, and 85 mM of concentrated Rh ion can be extracted.

Journal Articles

Preliminary studies of XANES and DFT calculation of Ru extraction by imino-diacetamide and related compounds

Sasaki, Yuji; Nakase, Masahiko*; Kaneko, Masashi; Kobayashi, Toru; Takeshita, Kenji*; Matsumiya, Masahiko*

Analytical Sciences, 5 Pages, 2023/00

https://doi.org/10.1007/s44211-023-00453-y
 Times Cited Count：0 Percentile：0(Chemistry, Analytical)

We conducted three field researches on Ru-extraction, XANES, and DFT-calculation. The order of the distribution ratio, D(Ru), from acid, HCl $$>$$ H$$_2$$SO$$_4$$ $$>$$ HNO$$_3$$ $$>$$ HClO$$_4$$, by MIDOA is studied by XANES spectra, which indicates the valency change of Ru in HCl media and supports the ion pairing extraction of anionic Ru ion and cationic MIDOA. The same extractant trend, NTAamide $$>$$ MIDOA $$>$$ IDOA, due to D values as the energy gap of HOMO and LUMO could be found by DFT calculation, which suggests that the reaction heat has a positive correlation with extractability for extractant.

Journal Articles

Complex formation of light and heavy lanthanides with DGA and DOODA, and its application to mutual separation in DGA-DOODA extraction system

Nomizu, Daiki; Sasaki, Yuji; Kaneko, Masashi; Matsumiya, Masahiko*; Katsuta, Shoichi*

Journal of Radioanalytical and Nuclear Chemistry, 331(3), p.1483 - 1493, 2022/03

https://doi.org/10.1007/s10967-022-08204-5
 Times Cited Count：4 Percentile：68.71(Chemistry, Analytical)

We studied the successive formation of water soluble DGA (diglycolamide) and DOODA (dioxaoctanediamide) for the mutual separation of Ln in this extraction system. TODGA (tetraoctyl-diglycolamide) and DOODA(C8) (tetraoctyl-dioxaoctanediamide) have the opposite trend to extract light and heavy Ln through Ln-patterns. Metal-complexes of two folding Ln ions with water-soluble DOODA and three folding with DGA are found and their observed formation constants are calculated. The suitable separation condition (aqueous phase: 30 mM DOODA(C2) in 1 M nitric acid, organic phase: 0.1 M TODGA in n-dodecane) of multi-stage extraction (10 $$times$$ 10) is conducted. From the present work, it is clear that La, Pr and Nd are mainly present in aqueous phase, instead Sm-Dy exist in the organic phase.

Journal Articles

Multi-stage extraction and separation of Ln and An using TODGA and DTBA or DTPA accompanying pH adjustment with lactic acid and ethylenediamine

Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Matsumiya, Masahiko*; Nakase, Masahiko*; Takeshita, Kenji*

Separation Science and Technology, 57(16), p.2543 - 2553, 2022/00

https://doi.org/10.1080/01496395.2022.2080707
 Times Cited Count：3 Percentile：29.84(Chemistry, Multidisciplinary)

The mutual separation of actinides (An) from lanthanides (Ln) using the masking agent of DTPA (diethylenetriamine-pentaacetic acid) or DTBA (diethylenetriamine-triacetic acid-bis(diethylacetamide)) in the aqueous phase through DGA extraction, referring TALSPEAK method, is focused. We investigate to obtain the same separation performance using commercially available DTPA on that using DTBA. In this work, we select lactic acid (LA) of pH buffer from 10 organic acids and ethylenediamine (ED) for the pH adjustment. Almost the same D and SF values are obtained among the conditions: TODGA-DTPA-LA-NaOH, TODGA-DTPA-LA-ED, and TODGA-DTBA-LA. The experimental results using batchwise multi-stage extractions show the average yields of Ln (La to Gd) and Am to be 3.73 and 98.1% in the aqueous phase using DGA-DTPA-LA-ED, to be 3.1 and 97.0% using DGA-DTPA-LA-NaOH, and to be 1.61 and 98.7% using DGA-DTBA-LA.

Journal Articles

Mutual separation of Ln and An using TODGA and DTBA with high organic acid concentrations

Sasaki, Yuji; Kaneko, Masashi; Matsumiya, Masahiko*; Nakase, Masahiko*; Takeshita, Kenji*

Solvent Extraction and Ion Exchange, 40(6), p.620 - 640, 2022/00

https://doi.org/10.1080/07366299.2021.2024650
 Times Cited Count：1 Percentile：14.86(Chemistry, Multidisciplinary)

Owing to the chemical behavior of trivalent lanthanide and actinide ions with similar ionic radii, realizing this separation is still challenging. All lanthanides, Am, and Cm can be extracted using diglycolamide (DGA), and relatively high An/Ln separation efficiencies have been obtained using diethylenetriamine-triacetic-bisamide (DTBA). To improve the previous results as well as the separation conditions, we used organic acids for pH adjustment. The advantages of this modification included low HNO$$_{3}$$, DTBA concentrations and pH stability owing to the addition of lactic acid. Under these modified conditions, the recovery rates observed were as follows: 97.1% for Nd with the co-existence of 1.59% Am in organic phase, and 98.4% for Am with the co-existence of 2.95% Nd in aqueous phase.

Journal Articles

Prediction of stability constants for novel chelates design in minor actinides partitioning over lanthanides using density functional theory calculation

Kaneko, Masashi; Sasaki, Yuji; Wada, Eriko*; Nakase, Masahiko*; Takeshita, Kenji*

Chemistry Letters, 50(10), p.1765 - 1769, 2021/10

https://doi.org/10.1246/cl.210402
 Times Cited Count：0 Percentile：0(Chemistry, Multidisciplinary)

Density functional theory calculation is applied to predict the stability constants for Eu$$^{3+}$$ and Am$$^{3+}$$ complexes in aqueous solution for molecular modelling of novel separation agents for minor actinides over lanthanides. Logarithm of experimental stability constants correlates with calculated complex formation enthalpies with high reproducibility (R$$^{2}$$ $$>$$ 0.98). Prediction of stability constants of novel chelates is demonstrated and indicates a potential availability of the derivatives of diethylenetriaminepentaacetic acid type chelate in acidic condition and enhancement of Am$$^{3+}$$ selectivity over Eu$$^{3+}$$.

Journal Articles

Density functional modeling of Am$$^{3+}$$/Eu$$^{3+}$$ selectivity with diethylenetriaminepentaacetic acid and its bisamide chelates.

Kaneko, Masashi; Sasaki, Yuji; Matsumiya, Masahiko*; Nakase, Masahiko*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 58(5), p.515 - 526, 2021/05

https://doi.org/10.1080/00223131.2020.1842267
 Times Cited Count：3 Percentile：35.51(Nuclear Science & Technology)

Density-functional theory calculations were applied to molecular structure and complex formation reaction modelings of metal ion complexes with diethylenetriaminepentaacetic acid (DTPA) and its bisamide (DTPABA) chelates to understand the metal ions selectivity between Am$$^{3+}$$ and Eu$$^{3+}$$. The calculated complexes with DTPA and DTPABA chelates reproduced the coordination geometries of experimental crystal structures. Calculated Gibbs free energies of the complex formation reactions indicated that Am$$^{3+}$$ ion forms higher stable complexes with both chelates than Eu$$^{3+}$$ ion, being consistent with the experimental results. The higher Am$$^{3+}$$ selectivity over Eu$$^{3+}$$ was suggested to originate in the larger bond overlap between Am$$^{3+}$$ 5f-orbital and N 2s, 2p-orbital. This mean that the covalent contribution between metal ion and donor atoms differentiates the complex formation stabilities, leading to the Am$$^{3+}$$/Eu$$^{3+}$$ selectivity. We expect that this study contributes to systematize the origin of metal ions selectivity and to accelerate novel ligands exploration.

Journal Articles

Reduction and resource recycling of high-level radioactive wastes through nuclear transmutation; Isolation techniques of Pd, Zr, Se and Cs in simulated high level radioactive waste using solvent extraction

Sasaki, Yuji; Morita, Keisuke; Ito, Keisuke; Suzuki, Shinichi; Shiwaku, Hideaki; Takahashi, Yuya*; Kaneko, Masaaki*; Omori, Takashi*; Asano, Kazuhito*

Proceedings of International Nuclear Fuel Cycle Conference (GLOBAL 2017) (USB Flash Drive), 4 Pages, 2017/09

no abstracts in English

Journal Articles

Extraction and separation of Se, Zr, Pd, and Cs including long-lived radionuclides

Sasaki, Yuji; Morita, Keisuke; Suzuki, Shinichi; Shiwaku, Hideaki; Ito, Keisuke; Takahashi, Yuya*; Kaneko, Masaaki*

Solvent Extraction Research and Development, Japan, 24(2), p.113 - 122, 2017/06

http://doi.org/10.15261/serdj.24.113

The solvent extraction of Se, Zr, Pd, and Cs from nitric acid into 1-octanol (OC) and dodecane has been performed. These elements include long-lived radionuclides in spent nuclear fuels, so a simple separation method is indispensable for the development of the treatment of high-level liquid radioactive waste. It was found that Se can be extracted using phenylenediamine, Zr can be extracted using tetraoctyl diglycolamide and di-2-ethylhexyl phosphoric acid, and Pd can be extracted using (methylimino)bis(dioctylacetamide) and hexaoctylnitrilotriacetamide. These elements can be recovered in over 90% yield by these extractants from nitric acid into OC. A distribution ratio of Cs of greater than 1 can be obtained using di-t-butyldibenzo-18-crown-6. It is clear that 90% recovery of Cs can be achieved using an extraction solvent with ten times the volume of the aqueous phase.

Journal Articles

Radioactive Cs in the severely contaminated soils near the Fukushima Daiichi Nuclear Power Plant

Kaneko, Makoto*; Iwata, Hajime; Shiotsu, Hiroyuki; Masaki, Shota*; Kawamoto, Yuji*; Yamasaki, Shinya*; Nakamatsu, Yuki*; Imoto, Jumpei*; Furuki, Genki*; Ochiai, Asumi*; et al.

Frontiers in Energy Research (Internet), 3, p.37_1 - 37_10, 2015/09

https://doi.org/10.3389/fenrg.2015.00037

The mobility of the aggregates of submicron-sized sheet aluminosilicate in the surface environment is a key factor controlling the current Cs migration in Fukushima.

Journal Articles

Anharmonic Pr guest modes in Pr(Os$$_{1-x}$$Ru$$_x$$)$$_4$$Sb$$_{12}$$ investigated by inelastic X-ray scattering

Tsutsui, Satoshi; Kaneko, Koji; Miyazaki, Ryoichi*; Higashinaka, Ryuji*; Aoki, Yuji*; Kobayashi, Riki*; Wakimoto, Shuichi; Baron, A. Q. R.*; Sugawara, Hitoshi*; Sato, Hideyuki*

JPS Conference Proceedings (Internet), 3, p.011060_1 - 011060_5, 2014/06

https://doi.org/10.7566/JPSCP.3.011060

Journal Articles

Current status of a new polarized neutron reflectometer at the intense pulsed neutron source of the Materials and Life Science Experimental Facility (MLF) of J-PARC

Takeda, Masayasu; Yamazaki, Dai; Soyama, Kazuhiko; Maruyama, Ryuji; Hayashida, Hirotoshi; Asaoka, Hidehito; Yamazaki, Tatsuya; Kubota, Masato; Aizawa, Kazuya; Arai, Masatoshi; et al.

Chinese Journal of Physics, 50(2), p.161 - 170, 2012/04

http://psroc.org/cjp/issues.php?vol=50&num=2

Journal Articles

Inelastic neutron scattering study on low-energy excitations of the heavy-fermion superconductor PrOs$$_4$$Sb$$_{12}$$

Kuwahara, Keitaro*; Iwasa, Kazuaki*; Kogi, Masafumi*; Kaneko, Koji; Metoki, Naoto; Raymond, S.*; M$'e$asson, M.-A.*; Flouquet, J.*; Sugawara, Hitoshi*; Aoki, Yuji*; et al.

Physica B; Condensed Matter, 385-386(Part 1), p.82 - 84, 2006/11

https://doi.org/10.1016/j.physb.2006.05.109
 Times Cited Count：3 Percentile：17.99(Physics, Condensed Matter)

We report inelastic neutron scattering experiments performed to investigate the low energy magnetic excitations on single crystals of the heavy-fermion superconductor PrOs$$_4$$Sb$$_{12}$$. The observed excitation clearly softens at a wave vector Q=(1,0,0), which is the same as the modulation vector of the field-induced antiferro-quadrupolar ordering, and its intensity at Q=(1,0,0) is smaller than that around the zone center. This result directly evidences that this excitonic behavior is derived mainly from nonmagnetic quadrupolar interactions. Furthermore, the narrowing of the linewidths of the excitations below the superconducting transition temperature indicates the close connection between the superconductivity and the excitons.

JAEA Reports

Measurements of $$^{238}$$U doppler effect in the soft neutron spectra using FCA (Joint research)

Ando, Masaki; Kawasaki, Kenji*; Okajima, Shigeaki; Fukushima, Masahiro; Matsuura, Yutaka*; Kaneko, Yuji*

JAERI-Research 2005-026, 39 Pages, 2005/09

JAERI-Research-2005-026.pdf:4.37MB

$$^{238}$$U Doppler effect measurements in moderated neutron spectra (uranium fuel and MOX simulated fuel) were carried out using FCA for the purpose of contributing to the improvement in prediction accuracy for Doppler coefficient in LWR. In the mockup cores for MOX fuel, the measurements were performed in different neutron spectra, where the voidage of moderator material was varied systematically. The experimental data were obtained using cylindrical uranium samples with different outer diameter up to 800$$^{circ}$$C. Analyses were performed using a standard code system designed to analyze fast reactor mock-up experiments at FCA with the use of the JENDL-3.2 library. The results of the analyses showed that the calculation accuracy did not depend on the types of the core fuel or the Doppler samples. The calculated values agreed with the experimental ones within the experimental error. Any dependency of the prediction accuracy on the neutron spectra was not observed in the MOX simulated fuel cores.

Journal Articles

Direct observation of quadrupolar excitons in the heavy-fermion superconductor PrOs$$_4$$Sb$$_12$$

Kuwahara, Keitaro*; Iwasa, Kazuaki*; Kogi, Masafumi*; Kaneko, Koji; Metoki, Naoto; Raymond, S.*; M$'e$asson, M.-A.*; Flouquet, J.*; Sugawara, Hitoshi*; Aoki, Yuji*; et al.

Physical Review Letters, 95(10), p.107003_1 - 107003_4, 2005/09

https://doi.org/10.1103/PhysRevLett.95.107003
 Times Cited Count：96 Percentile：92.15(Physics, Multidisciplinary)

We report inelastic neutron scattering experiments performed to investigate the low energy magnetic excitations on single crystals of the heavy-fermion superconductor PrOs$$_4$$Sb$$_{12}$$. The observed excitation clearly softens at a wave vector $$Q$$ = (1,0,0), which is the same as the modulation vector of the field-induced antiferro-quadrupolar ordering, and its intensity at $$Q$$ = (1,0,0) is smaller than that around the zone center. This result directly evidences that this excitonic behavior is derived mainly from nonmagnetic quadrupolar interactions. Furthermore, the narrowing of the linewidths of the excitations below the superconducting transition temperature indicates the close connection between the superconductivity and the excitons.

Journal Articles

Magnetic excitations in the heavy-fermion superconductor PrOs$$_4$$Sb$$_{12}$$

Raymond, S.*; Flouquet, J.*; Kuwahara, Keitaro*; Iwasa, Kazuaki*; Kogi, Masafumi*; Kaneko, Koji; Metoki, Naoto; Sugawara, Hitoshi*; Aoki, Yuji*; Sato, Hideyuki*

Physica B; Condensed Matter, 359-361, p.898 - 900, 2005/06

https://doi.org/10.1016/j.physb.2005.01.256
 Times Cited Count：2 Percentile：11.66(Physics, Condensed Matter)

The low lying magnetic excitations of the unconventional heavy fermion superconductor PrOs$$_4$$Sb$$_{12}$$ were studied by inelastic neutron scattering on single crystalline sample. The crystal field excitation first evidenced at 0.7 meV on powder samples is found to have a minimum of energy at the zone boundary corresponding to the wavevector of antiferro-quadrupolar instability. The evolution of the magnetic excitation spectrum under magnetic field confirms the singlet ground state.

Journal Articles

Magnetic excitations in heavy-fermion superconductor PrOs$$_{4}$$Sb$$_{12}$$

Kuwahara, Keitaro*; Iwasa, Kazuaki*; Kogi, Masafumi*; Kaneko, Koji; Araki, Shingo; Metoki, Naoto; Sugawara, Hitoshi*; Aoki, Yuji*; Sato, Hideyuki*

Journal of the Physical Society of Japan, 73(6), p.1438 - 1441, 2004/06

https://doi.org/10.1143/JPSJ.73.1438
 Times Cited Count：64 Percentile：87.39(Physics, Multidisciplinary)

no abstracts in English

Journal Articles

Neutron scattering study on the field-induced antiferro-quadrupolar ordering in the heavy fermion superconductor PrOs$$_{4}$$Sb$$_{12}$$

Metoki, Naoto; Kaneko, Koji; Araki, Shingo; Kogi, Masafumi*; Iwasa, Kazuaki*; Kuwahara, Keitaro*; Bernhoeft, N.*; Mignot, J.-M.*; Gukasov, A.*; Sato, Hideyuki*; et al.

Journal of Magnetism and Magnetic Materials, 272-276(Suppl.), p.e91 - e92, 2004/05

https://doi.org/10.1016/j.jmmm.2003.11.315
 Times Cited Count：1 Percentile：7.12(Materials Science, Multidisciplinary)

no abstracts in English

73 (Records 1-20 displayed on this page)