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

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--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.

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.

Design of accelerator-driven system consistent to partitioning technology

Sugawara, Takanori; Ban, Yasutoshi; Katano, Ryota; Tateno, Haruka; Nishihara, Kenji

Proceedings of International Conference on the Management of Spent Fuel from Nuclear Power Reactors 2019 (Internet), 9 Pages, 2019/06

The JAEA has proposed the double-strata strategy which will introduce a dedicated minor actinide (MA) transmutation cycle using an accelerator-driven system (ADS). In the previous study, the ideal fuel condition was supposed in the neutronics design of the ADS. For example, impurities such as rare earth (RE) nuclides which would accompany with MA, were not assumed. However, these nuclides would accompany with the ADS fuel and the capture reaction of these nuclides deteriorates the neutron economy of the ADS core. This study investigates a new fuel composition based on the SELECT (Solvent Extraction from Liquid-waste using Extractants of CHON-type for Transmutation) process proposed by JAEA. By performing the neutronics calculation of the ADS with the new fuel composition, a feasibility of the new fuel composition will be investigated.

Extraction of trivalent rare earths and minor actinides from nitric acid with -tetradodecyldiglycolamide (TDdDGA) by using mixer-settler extractors in a hot cell

Ban, Yasutoshi; Suzuki, Hideya; Hotoku, Shinobu; Kawasaki, Tomohiro*; Sagawa, Hiroshi*; Tsutsui, Nao; Matsumura, Tatsuro

Solvent Extraction and Ion Exchange, 37(1), p.27 - 37, 2019/00

https://doi.org/10.1080/07366299.2019.1586347

A continuous counter-current experiment using TDdDGA was performed using mixer-settler extractors installed in a hot cell. Nitric acid containing minor actinides (MAs: Am and Cm), rare earths (REs: Y, La, Nd, and Eu), and other fission products (Sr, Cs, Zr, Mo, Ru, Rh, and Pd) was fed to the extractor. TDdDGA effectively extracted MAs and REs from the feed, while other fission products were barely extracted. The extracted MAs and REs were back-extracted by bringing them in contact with 0.02 mol/dm nitric acid, and they were collected as the MA-RE fraction. The proportions of MA and RE in the MA-RE fraction were 98% and 86%, respectively. These results demonstrated the applicability of TDdDGA as an extractant for MAs and REs.

Uranium and plutonium extraction by -dialkylamides using multistage mixer-settler extractors

Ban, Yasutoshi; Hotoku, Shinobu; Tsutsui, Nao; Suzuki, Asuka; Tsubata, Yasuhiro; Matsumura, Tatsuro

Procedia Chemistry, 21, p.156 - 161, 2016/12

https://doi.org/10.1016/j.proche.2016.10.022

A continuous counter-current experiment was carried out to demonstrate the validity of a process using -dialkylamides for recovering U and Pu. This process consisted of two cycles, and the 1st cycle and the 2nd cycle employed -di(2-ethylhexyl)-2,2-dimethylpropanamide and -di(2-ethylhexyl)butanamide as extractants, respectively. The feed solution for the 1st cycle was 5.1 mol/dm (M) nitric acid containing 0.92 M U, 1.6 mM Pu, and 0.6 mM Np. The raffinate collected in the 1st cycle was used as the feed for the 2nd cycle. The ratios of U recovered in the U fraction and U-Pu fraction were 99.1% and 0.8%, respectively. The ratio of Pu recovered in the U-Pu fraction was 99.7%. The concentration ratio of U with respect to Pu in the U-Pu fraction was 9, and this indicated that Pu was not isolated. The decontamination factor of U with respect to Pu in the U fraction was obtained as 4.510. These results supported the validity of the proposed process.