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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:0 Percentile:0.04(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

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:0.01(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

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:1 Percentile:58.67(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:0 Percentile:0(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:0 Percentile:0(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:3 Percentile:38.85(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(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:2 Percentile:31.22(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:3 Percentile:51.91(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:3 Percentile:39.98(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:2 Percentile:31.22(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.

Journal Articles

Solvent extraction of cesium using DtBuDB18C6 into various organic solvents

Sasaki, Yuji; Morita, Keisuke; Kitatsuji, Yoshihiro; Ito, Keisuke*; Yoshizuka, Kazuharu*

Solvent Extraction Research and Development, Japan, 28(2), p.121 - 131, 2021/00

 Times Cited Count:1 Percentile:12.03(Chemistry, Multidisciplinary)

High concentration of Cs is present in high-level radioactive waste. It is well-known that Cs is an alkali element and difficult to extract completely into an organic phase. Crown ether compounds are widely available for Cs extractants; DtBuDB18C6 (di-$$t$$-butyl-dibenzo-18crown6), was used in this study. Organic solvents used for the industrial applications, such as $$n$$-dodecane and 1-octanol, have low solubility concerning the compound; other solvents were employed and tested. In this study, ketone-, ether-, and ester-type solvents showed high solubility for DtBuDB18C6 and DtBuDB18C6, when dissolved in ketones and alcohols, exhibited relatively high Cs distribution ratios ($$D$$(Cs)), closely to 10.

Journal Articles

Separation of rare earth elements by synergistic solvent extraction with phosphonium-based ionic liquids using a $$beta$$-diketone extractant and a neutral ligand

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

Solvent Extraction and Ion Exchange, 39(7), p.764 - 784, 2021/00

 Times Cited Count:2 Percentile:24.57(Chemistry, Multidisciplinary)

We investigated the solvent extraction of four rare earth (RE) elements (Pr, Nd, Tb, and Dy) from Nd-Fe-B magnets using mixtures of 1-(2-thienyl)-4,4,4,-trifluoro-1,3-butanedione (Htta) or 4,4,4-trifluoro-1-phenyl-1,3-butanedione (Hbfa) chelating extractants and tri-n-octylphosphine oxide (TOPO) neutral ligand in phosphonium based ionic liquids. A synergistic effect was observed for the extraction of the RE elements with the combination of extractant and neutral ligand. The separation of Tb(III) and Dy(III) from other RE(III) components was performed with seven extraction cycles.

Journal Articles

Basic research on batchwise multi-stage extractions using TODGA for Dy/Nd separation

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

Analytical Sciences, 36(11), p.1303 - 1309, 2020/11

 Times Cited Count:3 Percentile:21.93(Chemistry, Analytical)

The mutual separation of lanthanides is studied by multi-stage extraction using extractant, DGA (diglycolamide) compounds. Tetraoctyl-DGA (TODGA) has a high extractability to lanthanides and relatively high separation factor (SF) between Dy and Nd (SF: over 20). The complete separation with such SF value can be achieved by multi-stage extraction. Less information on multi-stage extraction compared to batch extraction is presented up to now, thus we conduct the basic study about that. Confirming the experimental data to be identical to the calculation, the sample solution including both metals is employed for the batchwise multi-stage extraction. Ninety-seven % of Dy with under detection limit of Nd can be recovered into the organic phase from Nd with ten times higher concentration than Dy using the condition, 0.1 M TODGA/n-dodecane and 0.3 M HNO$$_{3}$$ by multi-stage extraction of 9$$times$$9 for organic and aqueous phases.

Journal Articles

Solvent extraction of platinum group metals from urban mine by diglycolamide with soft donor atoms

Sasaki, Yuji; Nakase, Masahiko*

Petorotekku, 43(11), p.782 - 787, 2020/11

As analog compounds of DGA (diglycolamide), MIDOA(methylimino-diacetamide) and TDGA(thia-diglycolammide) are used for the extractants of platinum group metals. These extractants can be extracted noble metals and oxyanions, which followed by HSAB theory. The high concentration of these metals can be also extracted by these compounds. The research of metal-complex structures gives the information on the ability and role for complex-formation, which will be useful for the development of novel extractants.

Journal Articles

Extraction and separation between light and heavy lanthanides by $$N,N,N',N'$$-tetraoctyl-diglycolamide from organic acid

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

Chemistry Letters, 49(10), p.1216 - 1219, 2020/10

 Times Cited Count:8 Percentile:50.67(Chemistry, Multidisciplinary)

Lanthanide (Ln) extractions from organic acids to $$n$$-dodecane by $$N,N,N',N'$$-tetraoctyl-diglycolamide (TODGA) were conducted. Four organic acids (lactic acid, malonic acid, tartaric acid, and citric acid) were employed. Although these acids stabilize lanthanides in the aqueous phase, a distribution ratio ($$D$$) greater 1 was obtained for heavy Ln. Ln patterns ($$D$$(Ln) against atomic number of Ln) show maximum values of Ho and Er. In order to obtain high $$D$$ values, the addition of HNO$$_{3}$$ in aqueous phase is found to be effective.

Journal Articles

Research development of separation for nuclear fuel reprocessing and reduction of hazardous substance in high level radioactive waste

Sasaki, Yuji

Kagaku Kogaku, 84(9), p.425 - 427, 2020/09

The reduction of waste volume and hazardous substance though separation methods concerning atomic energy must be requested. As disposal methods or temporary measures, geological disposal, transmutation and interim storage are proposed. In order to perform effectively the disposal methods, the development of separation method of aimed elements is indispensable. Here, the new separation method of U and Pu from spent nuclear fuel and minor actinide separation and fission products from high level radioactive waste are explained.

Journal Articles

Simultaneous separation of Am and Cm from Nd and Sm by multi-step extraction using the TODGA-DTPA-BA-HNO$$_{3}$$ system

Sasaki, Yuji; Morita, Keisuke; Matsumiya, Masahiko*; Nakase, Masahiko*

Radiochimica Acta, 108(9), p.689 - 699, 2020/09

 Times Cited Count:9 Percentile:83.55(Chemistry, Inorganic & Nuclear)

The simultaneous separation of Am and Cm from lanthanides is important for atomic energy fields. All lanthanides, Am, and Cm can be extracted by diglycolamide (DGA). In addition, relatively high separation factors between An and Ln were obtained by the extraction system of TODGA, DTPA (diethylenetriamine-pentaacetic acid) and HNO$$_{3}$$. In this work, DTPA-BA (diethylenetriamine-triacetic-bisamide), which is an improved version of DTPA, was employed for the separation of Ln and An. A relatively high separation factor (approximately 8) for actinides/lanthanides was obtained. Then, the multi-step extraction was performed. Thus, the recoveries of 94.7% for Nd and 4.7% for Am and Cm in organic phase, and 5.3% Nd and 95.3% for Am and Cm in aqueous phase were obtained.

349 (Records 1-20 displayed on this page)