Development of technology for separating Am-241 in aged plutonium

Emori, Tatsuya; Kitatsuji, Yoshihiro; Ban, Yasutoshi

JAEA-Technology 2024-025, 20 Pages, 2025/03

JAEA-Technology-2024-025.pdf:1.65MB

Radioisotope Thermoelectric Generators (RTGs) using the decay heat of Pu-238 has been applied for outer planet missions far from Jupiter, where solar power is limited. However, no facilities are available to produce Pu-238 for space probes in Japan. Moreover, the use of nuclear materials for the space exploration is difficult in term of the regulation. Thus, we focused on Am-241 whose half-life is around 432 years as an alternative heat source for RTGs. This report describes the procedure of separating Am-241 decayed from Pu-241 in aged plutonium oxide. Two experiments were performed: one using solid-liquid extraction and the other combining liquid-liquid extraction and solid-liquid extraction. Packed columns were used in the experiments, with their number reduced by less than one-fifth in the latter experiment compared to the former. Furthermore, the time required for separation in the latter experiment was less than half that of the former. We performed the separation experiments six times, collecting a total of approximately 0.43 g of Am-241 as an oxalate salt.

Development of a dissolution method for analyzing the elemental composition of fuel debris using sodium peroxide fusion technique

Nakamura, Satoshi; Ishii, Sho*; Kato, Hitoshi*; Ban, Yasutoshi; Hiruta, Kenta; Yoshida, Takuya; Uehara, Hiroyuki; Obata, Hiroki; Kimura, Yasuhiko; Takano, Masahide

Journal of Nuclear Science and Technology, 62(1), p.56 - 64, 2025/01

https://doi.org/10.1080/00223131.2024.2381553

A dissolution method for analyzing the elemental composition of fuel debris using the sodium peroxide (NaO) fusion technique has been developed. Herein, two different types of simulated debris materials (such as solid solution of (Zr,RE)O and molten core-concrete interaction products (MCCI)) were taken. At various temperatures, these debris materials were subsequently fused with NaO in crucibles, which are made of different materials, such as Ni, AlO, Fe, and Zr. Then, the fused samples are dissolved in nitric acid. Furthermore, the effects of the experimental conditions on the elemental composition analysis were evaluated using inductively coupled plasma-atomic emission spectroscopy (ICP-AES), which suggested the use of a Ni crucible at 923 K as an optimum testing condition. The optimum testing condition was then applied to the demonstration tests with Three Mile Island unit-2 (TMI-2) debris in a shielded concrete cell, thereby achieving complete dissolution of the debris. The elemental composition of TMI-2 debris revealed by the proposed dissolution method has good reproducibility and has an insignificant contradiction in the mass balance of the sample. Therefore, this newly developed reproducible dissolution method can be effectively utilized in practical applications by dissolving fuel debris and estimating its elemental composition.

Recovery of minor actinides from HLW using Hexaoctyl nitrilotriacetamide (HONTA) by mixer-settler extractors

Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsubata, Yasuhiro

Proceedings of International Conference on Nuclear Fuel Cycle (GLOBAL2024) (Internet), 4 Pages, 2024/10

A continuous counter-current extraction experiment was performed by mixer-settler extractors to recover minor actinides (MA; Am and Cm) from high-level liquid waste. Using hexaoctyl nitrilotriacetamide (HONTA) as an extractant, 0.17 g of MA was recovered in a MA fraction.

A Demonstration test to separate minor actinides in high-level liquid waste by -hexaoctyl nitrilotriacetamide (HONTA) using mixer-settler extractors in a hot cell

Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsubata, Yasuhiro

Solvent Extraction Research and Development, Japan, 31(1), p.1 - 11, 2024/00

https://doi.org/10.15261/serdj.31.1

A demonstration test was performed to separate minor actinides (MA; Am and Cm) by -hexaoctyl nitrilotriacetamide (HONTA) as an extractant using mixer-settler extractors installed in a hot cell. A high-level liquid waste containing MA, and rare earths (RE; Y, La, Nd, and Eu) was used as the feed. HONTA diluted to 0.05 mol/dm in -dodecane was fed as the organic phase, and a part of the organic phase was reused without solvent regeneration. HONTA effectively extracted MA, whereas RE were less extractable. Consequently, the Y, La, Nd, and Eu ratios distributed to a RE fraction were 99.9%, 99.2%, 61.8%, and 81.4%, respectively. The Am and Cm ratios distributed to an MA fraction were 86.8% and 74.7%, respectively, and a substantial amount of MA (0.12 g) was recovered in the MA fraction by the end of the cumulative duration of 40 h.

Efficient separation of americium by a mixed solvent of two extractants, a diamideamine and a nitrilotriacetamide

Suzuki, Hideya*; Ban, Yasutoshi

Analytical Sciences, 39(8), p.1341 - 1348, 2023/08

https://doi.org/10.1007/s44211-023-00344-2

The Japan Atomic Energy Agency (JAEA) has proposed the Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation (SELECT) process by solvent extraction as a new separation technology to recover minor actinides (MA) from high-level liquid waste (HLLW) produced by spent fuel reprocessing. The MA separation in the SELECT process comprises the batch recovery of MA and rare earths (RE) from HLLW, MA/RE separation, and Am/Cm separation. Three highly practical extractants are used in the MA separation. Furthermore, this flow configuration facilitates the preparation of nitric acid concentrations in the aqueous phase. However, the separation factor between Cm and Nd in the MA/RE separation is small ( = 2.5), requiring many extraction stages for continuous extraction in a mixer-settler. Therefore, this study investigated the separation of only Am from an aqueous nitric acid solution containing MA (Am and Cm) and RE using an organic phase mixed with two extractants alkyl diamideamine with 2-ethylhexyl alkyl chains (ADAAM(EH)) and hexa-n-octylnitrilotriacetamide (HONTA) used in the SELECT process. Under high-concentration nitric acid conditions, Am and La, Ce, Pr, Nd (light lanthanides) were extracted in the ADAAM(EH) + HONTA mixed solvent, whereas Cm, medium, and heavy lanthanides, and Y were partitioned in the aqueous phase. Subsequently, only light lanthanides could be back extracted from the ADAAM(EH) + HONTA mixture solvent containing Am and light lanthanides in low nitric acid concentrations. Furthermore, Am could be easily stripped with 0.2 M or 5 M nitric acid. This method does not require the mutual separation of Cm and Nd, which have low separation factors. Am can be efficiently separated by one extraction and two back-extractions, reducing the number of steps in the SELECT process.

Study on the mechanism of radiolytic degradation of an extractant for minor actinides separation

Toigawa, Tomohiro; Kumagai, Yuta; Yamashita, Shinichi*; Ban, Yasutoshi; Matsumura, Tatsuro

UTNL-R-0502 (Internet), 2 Pages, 2022/04

This report summarizes the results obtained in FY2020 at the Electron Linac Facility of the University of Tokyo. The radiolysis process of -hexaoctyl nitrilotriacetamide (HONTA), which is expected to be used as an extractant in a separation process for minor actinides, diluted in dodecane was investigated by pulse radiolysis experiments. The radical cation and the triplet-excited state of HONTA were observed in the nanosecond time region. The transition from the radical cation to the triplet excited state was slowed down by adding electron scavengers, and further, the reactivity of the triplet excited state was also suppressed.

Re-examinations of MA fuel composition for accelerator-driven system and its heat removal

Sugawara, Takanori; Moriguchi, Daisuke*; Ban, Yasutoshi; Tsubata, Yasuhiro; Takano, Masahide; Nishihara, Kenji

JAEA-Research 2021-008, 63 Pages, 2021/10

JAEA-Research-2021-008.pdf:4.43MB

This study aims to perform the neutronics calculations for accelerator-driven system (ADS) with a new fuel composition based on the SELECT process developed by Japan Atomic Energy Agency because the previous studies had used the ideal MA (minor actinide) fuel composition without uranium and rare earth elements. Through the neutronics calculations, it is shown that two calculation cases, with/without neptunium, satisfy the design criteria. Although the new fuel composition includes uranium and rare earth elements, the ADS core with the new fuel composition is feasible and consistent with the partitioning and transmutation (P&T) cycle. Based on the new fuel composition, the heat removal during fuel powder storage and fuel assembly assembling is evaluated. For the fuel powder storage, it is found that a cylindrical tube container with a length of 500 [mm] and a diameter of 11 - 21 [mm] should be stored under water. For the fuel assembly assembling, CFD analysis indicates that the cladding tube temperature would satisfy the criterion if the inlet velocity of air is larger than 0.5 [m/s]. Through these studies, the new fuel composition which is consistent with the P&T cycle is obtained and the heat removal with the latest conditions is investigated. It is also shown that the new fuel composition can be practically handled with respect to heat generation, which is one of the most difficult points in handling MA fuel.

Evaluation of the mass transfer coefficients for the minor actinide separation; Evaluation by the single drop method

Sakamoto, Atsushi; Kibe, Satoshi*; Kawanobe, Kazunori*; Fujisaku, Kazuhiko*; Sano, Yuichi; Takeuchi, Masayuki; Suzuki, Hideya*; Tsubata, Yasuhiro; Ban, Yasutoshi; Matsumura, Tatsuro

JAEA-Research 2021-003, 30 Pages, 2021/06

JAEA-Research-2021-003.pdf:1.81MB

Japan Atomic Energy Agency has been developing a solvent extraction process called SELECT to recover minor actinides (MA) from spent nuclear fuel. In the SELECT process, TDdDGA, HONTA, and ADAAM are used as the extractants for MA + Ln corecovery, MA/Ln separation and Am/Cm separation, respectively. These extractants do not contain phosphorus (P), and consist of carbon (C), hydrogen (H), oxygen (O), and nitrogen (N). In this study, in order to give beneficial information for designing flowsheet, the mass transfer coefficients of Ln between HNO solution and TDdDGA or HONTA / n-dodecane solvent were evaluated by the single drop technique. Prior to the evaluation of mass transfer coefficient, we had optimized the structure of the single drop apparatus to improve accuracy of the measurement. Based on the mass transfer coefficients obtained in HNO / TDdDGA-n-dodecane system, Ln behaviors in the counter-current extraction and back-extraction using mixer-settlers and centrifugal contactors were estimated by simple calculation, and they had a good agreement with our previous experimental results. We also confirmed the mass transfer coefficients of Ln in HNO / HONTA - n-dodecane system are under 10 m/s.

Production of the minor actinide sources using the electrodeposition method

Nakamura, Satoshi; Kimura, Takahiro; Ban, Yasutoshi; Tsubata, Yasuhiro; Matsumura, Tatsuro

JAEA-Technology 2020-009, 22 Pages, 2020/08

JAEA-Technology-2020-009.pdf:2.92MB

Partitioning and transmutation technology division is planning to measure fission rate ratios that contribute to validate nuclear data of minor actinides (MA). For this purpose, MA sources for fission chambers were prepared using electrodeposition method. The radioactivity of each MA source was quantified, and its uncertainty was evaluated. Seven types of MA sources with different radioactivity were prepared using four nuclides of Np, Am, Am, and Cm. A Cm source solution of which radioactivity was quantified by isotope dilution method was used to prepare working standard sources of Cm. The radioactivities were quantified as 1461 Bq, 2179 Bq, and 2938 Bq for Np sources, 1.428 MBq for Am source, 370.5 kBq and 89.57 kBq for Am sources, and 2.327 MBq for Cm source with, the uncertainty of 0.35% (1). This report summarizes the method for preparation and quantification of MA sources, and uncertainty evaluation.

Preliminary study on separation of Dy and Nd by multi-step extraction using TDdDGA

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

Solvent Extraction Research and Development, Japan, 27(1), p.63 - 67, 2020/00

https://doi.org/10.15261/serdj.27.63

Mutual separation technique of Dy and Nd in Nd magnet is studied. Dy is more valuable than Nd, then Dy might be isolated and reused. Lanthanide elements can be extracted thoroughly by diglycolamide (DGA) extractants, we use this reagent for the recovery and isolation of Dy. Tetradodecyl-DGA (TDdDGA) has relatively high separation factors(SF) between Dy and Nd (SF=17-18) in HNO extraction system, counter-current extraction using TDdDGA was applied for their mutual separation. From the present study, using the condition, four extraction stages, organic phase: 0.1M TDdDGA in n-dodecane, aqueous phase: 0.3M HNO, 92% Dy can be recovered with 0.7% co-extraction of Nd.