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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, 61(7), p.883 - 893, 2024/07

 Times Cited Count:2 Percentile:65.72(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

Ion-pairing extraction and their reaction modeling of anionic M-Cl species with cationic NTAamide(C6) extractant and comparison with density functional theory calculations

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

Hydrometallurgy, 222, p.106159_1 - 106159_12, 2023/10

 Times Cited Count:1 Percentile:22.95(Metallurgy & Metallurgical Engineering)

Solvent extraction is conducted using a total of 20 metals revealing high stability constants with Cl and hexahexyl-nitrilotriacetamide (NTAamide(C6)) extractant. The metals used here may behave as anions at high Cl concentrations, and NTAamide(C6), which contains a tertiary N atom, is protonated under acidic conditions. Most of the metal ions in this study display higher distribution ratios (D(M)) from HCl than those from HNO$$_{3}$$, and exhibit 1:1 stoichiometries with NTAamide. Following the experimental results, the association constants and distribution coefficients of the group 12 elements are calculated via ion-pair extraction modeling using density functional theory calculations, and the simulations of D yield calculated values with the same trend as that of the measured values.

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

 Times Cited Count:1 Percentile:22.90(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

Phase analysis of simulated nuclear fuel debris synthesized using UO$$_{2}$$, Zr, and stainless steel and leaching behavior of the fission products and matrix elements

Tonna, Ryutaro*; Sasaki, Takayuki*; Kodama, Yuji*; Kobayashi, Taishi*; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Kumagai, Yuta; Kusaka, Ryoji; Watanabe, Masayuki

Nuclear Engineering and Technology, 55(4), p.1300 - 1309, 2023/04

 Times Cited Count:3 Percentile:65.72(Nuclear Science & Technology)

Simulated debris was synthesized using UO$$_{2}$$, Zr, and stainless steel and a heat treatment method under inert or oxidizing conditions. The primary U solid phase of the debris synthesized at 1473 K under inert conditions was UO$$_{2}$$, whereas a (U,Zr)O$$_{2}$$ solid solution formed at 1873 K. Under oxidizing conditions, a mixture of U$$_{3}$$O$$_{8}$$ and (Fe,Cr)UO$$_{4}$$ phases formed at 1473 K whereas a (U,Zr)O$$_{2+x}$$ solid solution formed at 1873 K. The leaching behavior of the fission products from the simulated debris was evaluated using two methods: the irradiation method, for which fission products were produced via neutron irradiation, and the doping method, for which trace amounts of non-radioactive elements were doped into the debris. The dissolution behavior of U depended on the properties of the debris and aqueous medium the debris was immersed in. Cs, Sr, and Ba leached out regardless of the primary solid phases. The leaching of high-valence Eu and Ru ions was suppressed, possibly owing to their solid-solution reaction with or incorporation into the uranium compounds of the simulated debris.

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

 Times Cited Count:0 Percentile:0.00(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

Combining a lipophilic phenanthroline carboxamide and a hydrophilic diglycolamide to increase the separation factors of adjacent light lanthanides

Simonnet, M.; Sasaki, Yuji; Yaita, Tsuyoshi

Solvent Extraction and Ion Exchange, 41(7), p.857 - 867, 2023/00

 Times Cited Count:2 Percentile:38.77(Chemistry, Multidisciplinary)

Journal Articles

Study on evaluation method of kernel migration of TRISO fuel for High Temperature Gas-cooled Reactor

Fukaya, Yuji; Okita, Shoichiro; Sasaki, Koei; Ueta, Shohei; Goto, Minoru; Ohashi, Hirofumi; Yan, X.

Nuclear Engineering and Design, 399, p.112033_1 - 112033_9, 2022/12

 Times Cited Count:0 Percentile:0.00(Nuclear Science & Technology)

Kernel migration of TRi-structural ISOtropic (TRISO) fuel for High Temperature Gas-cooled Reactor (HTGR) has been analyzed to investigate the potential dominating effects. Kernel migration is a major fuel failure mode and dominant to determine the lifetime of the fuel for High Temperature engineering Test Reactor (HTTR). However, this study shows that the result and reliability depend on the evaluation method. The evaluation method used in this study takes into account of actual distribution of Coated Fuel Particles (CFPs) and the resulting heterogeneous fuel temperature calculation with such distribution. The result shows that the Kernel Migration Rate (KMR) is predicted to be about 10% less compared with the most conservative evaluation.

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

Investigation of total separations using solvent extraction of actinides and fission products

Sasaki, Yuji

Bunri Gijutsu, 52(2), p.103 - 107, 2022/03

We develop all-inclusive partitioning method for actinides and fission products in high-level radioactive waste. This process is based on the sequential solvent extraction. In order to recover Cs and Sr for the management by interim storage, crown ether compounds are employed. For the removal of Pd and Mo due to production of a stable vitrified object, methylimino-dioctylacetamide (MIDOA) is taken as an extractant. DGA can extract both actinides and trivalent lanthanides. In order to separate each other, dietylenetriamine-triacetic-diamide (DTBA) for the stripping reagent of MA. For the mutual separation of Am/Cm, DGA and DOODA extraction system is taken into consideration.

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

 Times Cited Count:7 Percentile:83.23(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

 Times Cited Count:3 Percentile:28.95(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

 Times Cited Count:2 Percentile:18.86(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

Separation of light and middle lanthanides using multistage extraction with diglycolamide extractant

Matsutani, Takafumi; Sasaki, Yuji; Katsuta, Shoichi*

Analytical Sciences, 37(11), p.1603 - 1609, 2021/11

 Times Cited Count:7 Percentile:45.17(Chemistry, Analytical)

We investigated the chemical behavior of lanthanides (Ln) using diglycolamide extractant with multistage extraction. We obtained the breakthrough curves for light and middle Ln. Our study reveals that the metal extraction limit depends on their $$D$$ values and metal concentrations used in the experiments. From the multistage extractions of 15 aqueous phases and 15 organic phases, three curves (extraction curves, back-extraction curves, and separation curves) were obtained by changing the nitric acid concentration. As an example, under a condition of the separation curve experiment (aqueous phase: 0.5 M HNO$$_{3}$$, organic phase: 0.1 M TDDGA ($$N,N,N',N'$$-tetradecyl-diglycolamide) in $$n$$-dodecane), a recovery of more than 99% of Sm in the organic phase with less than 1% Nd can be obtained.

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

 Times Cited Count:0 Percentile:0.00(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

Concepts and basic designs of various nuclear fuels, 5; Fuels for high temperature gas-cooled reactor and molten salt reactor

Ueta, Shohei; Sasaki, Koei; Arita, Yuji*

Nihon Genshiryoku Gakkai-Shi ATOMO$$Sigma$$, 63(8), p.615 - 620, 2021/08

no abstracts in English

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

 Times Cited Count:3 Percentile:30.60(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

Fundamental study on multistage extraction using TDdDGA for separation of lanthanides present in Nd magnets

Sasaki, Yuji; Morita, Keisuke; Matsumiya, Masahiko*; Ono, Ryoma*; Shiroishi, Hidenobu*

JOM, 73(4), p.1037 - 1043, 2021/04

 Times Cited Count:4 Percentile:35.67(Materials Science, Multidisciplinary)

The separation of Dy from Nd is studied from the viewpoint of recycling Dy from Nd magnets. Both metals are lanthanide elements, which means their mutual separation is difficult because of their similar chemical behaviors. All lanthanide elements can be extracted easily by using tetradodecyl-diglycolamide (TDdDGA) extractants, and it has a relatively high separation factor (SF) between Dy and Nd (SF over 10). In the present study, by performing eight extraction steps with the organic phase (0.1M TDdDGA in dodecane), ten steps with an aqueous phase (0.7 M HNO$$_{3}$$ with metals), and six steps with another aqueous phase (0.7 M HNO$$_{3}$$ without metals), approximately 99% Dy was recovered into the organic phase with 1% co-extraction of Nd.

Journal Articles

High temperature gas-cooled reactors

Takeda, Tetsuaki*; Inagaki, Yoshiyuki; Aihara, Jun; Aoki, Takeshi; Fujiwara, Yusuke; Fukaya, Yuji; Goto, Minoru; Ho, H. Q.; Iigaki, Kazuhiko; Imai, Yoshiyuki; et al.

High Temperature Gas-Cooled Reactors; JSME Series in Thermal and Nuclear Power Generation, Vol.5, 464 Pages, 2021/02

As a general overview of the research and development of a High Temperature Gas-cooled Reactor (HTGR) in JAEA, this book describes the achievements by the High Temperature Engineering Test Reactor (HTTR) on the designs, key component technologies such as fuel, reactor internals, high temperature components, etc., and operational experience such as rise-to-power tests, high temperature operation at 950$$^{circ}$$C, safety demonstration tests, etc. In addition, based on the knowledge of the HTTR, the development of designs and component technologies such as high performance fuel, helium gas turbine and hydrogen production by IS process for commercial HTGRs are described. These results are very useful for the future development of HTGRs. This book is published as one of a series of technical books on fossil fuel and nuclear energy systems by the Power Energy Systems Division of the Japan Society of Mechanical Engineers.

Journal Articles

Synergistic solvent extraction of lanthanide ions with mixtures of D2EHPA and MIDPA in phosphonium-based ionic liquids

Matsumiya, Masahiko*; Nomizu, Daiki*; Tsuchida, Yusuke*; Sasaki, Yuji

Hydrometallurgy, 199, p.105539_1 - 105539_8, 2021/02

 Times Cited Count:4 Percentile:26.64(Metallurgy & Metallurgical Engineering)

The synergistic solvent extraction of lanthanide(III) with mixtures of di-(2-ethylhexyl)phosphoric acid (D2EHPA, A) and monoisodecyl phosphoric acid (MIDPA, B) in phosphonium-based ionic liquid was investigated. In the case of D2EHPA or MIDPA single extractant system, Ln(III) (Ln = Pr and Nd) was extracted as [LnA$$_{3}$$HA] or [LnB$$_{3}$$HB], respectively, the extracted species of Tb(III) or Dy(III) were determined by slope analysis. According to the equilibrium constants ($$K_{rm A}$$, $$K_{rm B}$$ and $$K_{rm AB}$$) and the formation constants ($$beta_{1}$$, $$beta_{1}$$ and $$beta_{3}$$), it was found that the extracted complex [TbHA$$_{2}$$B$$_{2}$$ or [DyHA$$_{2}$$B$$_{2}$$] was more stable than [LnA$$_{3}$$HA] or [LnB$$_{3}$$HB]. The synergistic extraction effects were investigated to study the possibility of separating Dy(III) from Pr(III) and Nd(III) according to their separation factors.

Journal Articles

Trichotomic separation of light and heavy lanthanides and Am by batchwise multi-stage extractions using TODGA

Matsumiya, Masahiko*; Tsuchida, Yusuke*; Sasaki, Yuji; Ono, Ryoma*; Nakase, Masahiko*; Takeshita, Kenji*

Journal of Radioanalytical and Nuclear Chemistry, 327(1), p.597 - 607, 2021/01

 Times Cited Count:3 Percentile:20.42(Chemistry, Analytical)

To achieve trichotomic separation of light lanthanides (Ln), heavy Ln, and Am, batchwise multi-stage extractions using tetraoctyl-diglycolamide (TODGA) extractant from organic acids are studied. Malonic acid (MA) has high solubility in water and is used as the main component of the aqueous phase. It is clear that the separation factor (SF) for Nd/Am from MA and that for La/Am from MA + HNO$$_{3}$$ are both around 30. The light Ln (e.g., La and Ce) flowed-out in 1 M MA+0.05 M HNO$$_{3}$$ (1st soln.), Am is recovered into 3 M MA (2nd soln.), and middle and heavy Ln (Nd and other heavy Ln) are back-extracted into 0.1 M TEDGA/water (3rd soln.). This extraction method can give 95% recovery of Am with total Ln of less than 16% present in high-level radioactive waste.

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