Using X-ray absorption near edge structure to evaluate adsorption properties of rare earths and nitrogen by difference of their interactions

Minowa, Kazuki*; Watanabe, So; Nakase, Masahiko*; Takahatake, Yoko; Miyazaki, Yasunori; Ban, Yasutoshi; Matsuura, Haruaki*

Nuclear Instruments and Methods in Physics Research B, 556, p.165496_1 - 165496_6, 2024/11

https://doi.org/10.1016/j.nimb.2024.165496

In this study, X-ray absorption near edge structure (XANES) spectral analysis and column experiments were used to verify the selectivity of rare earth (RE) ions by alkyl diamide amine (ADAAM) adsorbent. In addition, the interactions between the N atoms of ADAAM and RE ions were evaluated to determine whether any of the RE ions are a valid simulant for developing a mutual separation process for minor actinides (MAs) in highly radioactive liquid waste. It was confirmed that La and Ce interacted with the amine N atom of ADAAM and they showed a peak shift of the N-K edge XANES spectrum; this finding suggested that a soft interaction is an essential factor influencing ion selectivity. Therefore, the selection factor of RE ions by ADAAM adsorbent was similar to that of MAs. It was concluded that RE ions are reasonable species to simulate MAs.

Impact of MOX fuel use in light-water reactors; Long-term radiological consequences of disposal of high-level waste in a geological repository

Minari, Eriko*; Kabasawa, Satsuki; Mihara, Morihiro; Makino, Hitoshi; Asano, Hidekazu*; Nakase, Masahiko*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 60(7), p.793 - 803, 2023/07

https://doi.org/10.1080/00223131.2022.2146016

Cost-reduced depletion calculation including short half-life nuclides for nuclear fuel cycle simulation

Okamura, Tomohiro*; Katano, Ryota; Oizumi, Akito; Nishihara, Kenji; Nakase, Masahiko*; Asano, Hidekazu*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 60(6), p.632 - 641, 2023/06

https://doi.org/10.1080/00223131.2022.2131646

The Okamura explicit method (OEM) for depletion calculation was developed by modifying the matrix exponential method for dynamic nuclear fuel cycle simulation. The OEM suppressed the divergence of the calculation for short half-life nuclides, even for long time steps. The computational cost of the OEM was small, equivalent to the Euler method, and it maintained sufficient accuracy for the fuel cycle simulation.

User manual of NMB4.0

Okamura, Tomohiro*; Nishihara, Kenji; Katano, Ryota; Oizumi, Akito; Nakase, Masahiko*; Asano, Hidekazu*; Takeshita, Kenji*

JAEA-Data/Code 2021-016, 43 Pages, 2022/03

JAEA-Data-Code-2021-016.pdf:3.06MB

The quantitative prediction and analysis of the future nuclear energy utilization scenarios are required in order to establish the advanced nuclear fuel cycle. However, the nuclear fuel cycle consists of various processes from front- to back-end, and it is difficult to analyze the scenarios due to the complexity of modeling and the variety of scenarios. Japan Atomic Energy Agency and Tokyo Institute of Technology have jointly developed the NMB code as a tool for integrated analysis of mass balance from natural uranium needs to radionuclide migration of geological disposal. This user manual describes how to create a database and scenario input for the NMB version 4.0.

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

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.

NMB4.0: Development of integrated nuclear fuel cycle simulator from the front to back-end

Okamura, Tomohiro*; Katano, Ryota; Oizumi, Akito; Nishihara, Kenji; Nakase, Masahiko*; Asano, Hidekazu*; Takeshita, Kenji*

EPJ Nuclear Sciences & Technologies (Internet), 7, p.19_1 - 19_13, 2021/11

https://doi.org/10.1051/epjn/2021019

Nuclear Material Balance code version 4.0 (NMB4.0) has been developed through collaborative R&D between Tokyo Institute of Technology and JAEA. Conventional nuclear fuel cycle simulation codes mainly analyze actinides and are specialized for front-end mass balance analysis. However, quantitative back-end simulation has recently become necessary for considering R&D strategies and sustainable nuclear energy utilization. Therefore, NMB4.0 was developed to realize the integrated nuclear fuel cycle simulation from front- to back-end. There are three technical features in NMB4.0: 179 nuclides are tracked, more than any other code, throughout the nuclear fuel cycle; the Okamura explicit method is implemented, which contributes to reducing the numerical cost while maintaining the accuracy of depletion calculations on nuclides with a shorter half-life; and flexibility of back-end simulation is achieved. The main objective of this paper is to show the newly developed functions, made for integrated back-end simulation, and verify NMB4.0 through a benchmark study to show the computational performance.

Density functional modeling of Am/Eu 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

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 and Eu. 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 ion forms higher stable complexes with both chelates than Eu ion, being consistent with the experimental results. The higher Am selectivity over Eu was suggested to originate in the larger bond overlap between Am 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/Eu selectivity. We expect that this study contributes to systematize the origin of metal ions selectivity and to accelerate novel ligands exploration.

Selection of nuclides for mass-balance analysis of fission products

Okamura, Tomohiro*; Oizumi, Akito; Nishihara, Kenji; Nakase, Masahiko*; Takeshita, Kenji*

JAEA-Data/Code 2020-023, 32 Pages, 2021/03

JAEA-Data-Code-2020-023.pdf:1.67MB

Nuclear Material Balance code (NMB code) have been developed in Japan Atomic Energy Agency. The NMB code will be updated with the function of mass balance analysis at the backend process such as reprocessing, vitrification and geological disposal. In order to perform its analysis with high accuracy, it is necessary to expand the number of FP nuclides calculated in the NMB code. In this study, depletion calculation by ORIGEN code was performed under 3 different burn-up conditions such as spent uranium fuel from light water reactor, and nuclides were selected from 5 evaluation indexes such as mass and heat generation. In addition, the FP nuclides required to configure a simple burnup chain with the same calculation accuracy as ORIGEN in the NMB code was selected. As the result, two lists with different number of nuclides, such as "Detailed list" and a "Simplified list", were created.

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

https://doi.org/10.1007/s10967-020-07464-3

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 are both around 30. The light Ln (e.g., La and Ce) flowed-out in 1 M MA+0.05 M HNO (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.

Extraction and separation between light and heavy lanthanides by -tetraoctyl-diglycolamide from organic acid

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

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

https://doi.org/10.1246/cl.200431

Lanthanide (Ln) extractions from organic acids to -dodecane by -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 () greater 1 was obtained for heavy Ln. Ln patterns ((Ln) against atomic number of Ln) show maximum values of Ho and Er. In order to obtain high values, the addition of HNO in aqueous phase is found to be effective.