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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
Times Cited Count：0 Percentile：0.00(Instruments & Instrumentation)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.
Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Suzuki, Hideya*
Journal of Nuclear Science and Technology, 61(7), p.883 - 893, 2024/07
Times Cited Count：3 Percentile：62.75(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-
-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.
Kinoshita, Ryoma; Sasaki, Yuji; Kaneko, Masashi; Matsumiya, Masahiko*; Shinoku, Kota*; Shiroishi, Hidenobu*
Hydrometallurgy, 222, p.106159_1 - 106159_12, 2023/10
Times Cited Count：2 Percentile：25.24(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
, 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.
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：3 Percentile：38.46(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
O complexes are formed in HCl media and show the slow exchange rate between Cl and HO. Using the UV spectrum, Rh-chloride solution having the peak of spectrum at 504 nm can be extracted effectively, where RhCl
(HO)
and RhCl
(H
O)
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.
Suzuki, Hideya*; Ban, Yasutoshi
Analytical Sciences, 39(8), p.1341 - 1348, 2023/08
Times Cited Count：4 Percentile：49.52(Chemistry, Analytical)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.
Kaneko, Masashi; Suzuki, Hideya; Matsumura, Tatsuro
Inorganic Chemistry, 57(23), p.14513 - 14523, 2018/12
Times Cited Count：24 Percentile：79.73(Chemistry, Inorganic & Nuclear)We elucidated the separation mechanism between Am(III) and Cm(III) ions by using two different types of diamide ligands, diglycolamide (DGA) and alkylated diamide amine (ADAAM), by means of the density functional theory technique and electron density analysis. The molecular geometries and formation reactions of the metal-ligand complexes were modeled by using [M(DGA)]
and [M(ADAAM)(NO)(HO)]. We successfully reproduced Cm(III) selectivity over Am(III) with DGA and Am(III) selectivity over Cm(III) with ADAAM. Furthermore, we analyzed the bonding properties between the metal ion and the diamide-type ligands by using model complexes, [M(DGA)] and [M(ADAAM)(NO)(HO)], and revealed the differences in terms of the bond dissociation energy and the metal 5f-orbital participation in the covalency between the Am(III) and the Cm(III) complexes. It was suggested that the differences were key factors to understand the Am(III)/Cm(III) selectivity.
Sasaki, Yuji; Morita, Keisuke; Ito, Keisuke; Suzuki, Shinichi; Shiwaku, Hideaki; Takahashi, Yuya*; Kaneko, Masaaki*; Omori, Takashi*; Asano, Kazuhito*
Proceedings of International Nuclear Fuel Cycle Conference (GLOBAL 2017) (USB Flash Drive), 4 Pages, 2017/09
no abstracts in English
Ogura, K.*; Asano, Masaharu; Yasuda, Nakahiro*; Yoshida, Masaru
Nuclear Instruments and Methods in Physics Research B, 185(1-4), p.222 - 227, 2001/12
Times Cited Count：33 Percentile：88.96(Instruments & Instrumentation)no abstracts in English
Osugi, Takeshi
no journal, ,
no abstracts in English
Suzuki, Hideya*; Ban, Yasutoshi; Tsubata, Yasuhiro; Hotoku, Shinobu; Toigawa, Tomohiro; Tsutsui, Nao; Shibata, Mitsunobu*; Kurosawa, Tatsuya*; Kawasaki, Tomohiro*; Matsumura, Tatsuro
no journal, ,
The Japan Atomic Energy Agency has been studying partitioning and transmutation (P&T) systems. In the P&T, the separation of minor actinides (MAs) from the chemically similar lanthanides is the key step. After MAs are separated from high-level waste, the mutual separation of Am and Cm (Am/Cm separation) can be conducted. Therefore, the removal of the pyrogenic Cm nuclide would reduce the difficulties associated with MA-fuel fabrication. However, Am/Cm separation is very challenging because the two elements have similar chemical and physical properties. Highly practical a new reagent, called ADAAM have been developed. The Am is subsequently selectively stripped from the light lanthanides. As a result, Am was separated with high efficiency.
Kato, Jun; Imaizumi, Ken*; Osugi, Takeshi; Sone, Tomoyuki; Kuroki, Ryoichiro; Kikuchi, Michio*; Yamamoto, Takeshi*; Otsuka, Taku*; Kaneda, Yoshihisa*; Osawa, Norihisa*
no journal, ,
Solidified cement and Alkali Activated Materials (AAM) containing simulated carbonated slurry was prepared, and the amount of Hydrogen gas generation on gamma-ray irradiation was determined. The obtained data was compared with the data of solidified material without any content of waste, and the effect for Hydrogen gas generation with the material containing simulated carbonated slurry was evaluated.
Taniguchi, Takumi; Namiki, Masahiro*; Osugi, Takeshi; Sone, Tomoyuki; Kuroki, Ryoichiro; Kikuchi, Michio*; Yamamoto, Takeshi*; Otsuka, Taku*; Kaneda, Yoshihisa*; Osawa, Norihisa*; et al.
no journal, ,
no abstracts in English
Kakuda, Ayaka; Osone, Osamu*; Hiraki, Yoshihisa; Osugi, Takeshi; Sone, Tomoyuki; Kuroki, Ryoichiro; Kudo, Isamu*; Elakneswaran, Y.*; Sato, Tsutomu*
no journal, ,
no abstracts in English
Hiraki, Yoshihisa; Kakuda, Ayaka; Saito, Toshimitsu*; Sone, Tomoyuki; Elakneswaran, Y.*; Sato, Tsutomu*; Osugi, Takeshi; Kuroki, Ryoichiro
no journal, ,
no abstracts in English
Sasaki, Yuji; Kaneko, Masashi; Ban, Yasutoshi; Suzuki, Hideya*
no journal, ,
Am and Cm as minor actinides, have the similar chemical behavior, thus both metals are, in general, hard to separate. On the other hand, separation of Am with long-lived radionuclide to transmute from Cm to emit neutrons by spontaneous fission has been requesting. Although the mutual separation by solvent extraction is a tough work, ADAAM (Alkyl DiAmide AMine) developed in JAEA show high separation factor of Am/Cm of around 6 at HNO-n-dodecane system. We focus on basic research on solvent extraction using ADAAM and investigate the physical properties, i.e., polarity and viscosity, and separation factors of Am/Cm variated in combination with water-soluble masking agent of An, and will show the information at the meeting.
Suzuki, Hideya*; Shimojo, Kojiro; Nakamura, Satoshi; Emori, Tatsuya; Kurosawa, Tatsuya*; Shibata, Mitsunobu*; Kawasaki, Tomohiro*; Ban, Yasutoshi
no journal, ,
The Japan Atomic Energy Agency (JAEA) has been studying partitioning and transmutation (P&T) systems. In P&T, JAEA proposed a novel hydrometallurgical process called "SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process" for nuclear fuel reprocessing and minor actinides (MA) separation. In this study, a new MA separation method was investigated to further improve the efficiency of the SELECT process. Batch tests were conducted in a mixed solvent system using the acidic amide-type extractants nitrilotriacetic acid diacetamide with branched side chains (B-TONAADA) and alkyl diamidoamine (ADAAM). As a result, we found an efficient method for separating only americium (Am) from an aqueous nitric acid solution containing MA and rare earth elements by adjusting nitric acid concentration.
Kobayashi, Yutaro*; Osawa, Norihisa*; Haga, Kazuko*; Kaneda, Yoshihisa*; Chaerun, R. I.; Sato, Tsutomu*; Taniguchi, Takumi; Kuroki, Ryoichiro; Okada, Takashi; Yoshida, Yukihiko; et al.
no journal, ,
no abstracts in English
Kaneko, Masashi; Watanabe, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro
no journal, ,
Nitrilotriacetamide (NTAamide) is considered to be a candidate for the separation reagent of minor-actinides (MA) from lanthanides (Ln) for an application to partitioning and transmutation. We have elucisdated the separation mechanism of Am from Eu with NTAamide by means of density functional theory (DFT). The present study applied the DFT method to Ln pattern of distribution ratio with NTAamide by solvent extraction. The extracted complex by NTAamide was modeled as [Ln(NTAamide)] (Ln = La, Ce, Nd, Sm, Eu, Gd) by referring the analogous crystal structure. Calculated geometry was indicated to belong to a pseudo-S
point group with the Ln-N(amine) axis as C rotational axes. Gibbs energy difference indicated that NTAamide ligands more stably coordinate to light or middle Ln ions than La ion. This tendency was comparable to the experimental result of distribution ratio for Ln ions reported previously.
Kaneko, Masashi; Watanabe, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro
no journal, ,
Japan Atomic Energy Agency has developed separation reagents between Am and Cm ions, which are minor actinides, to achieve partitioning and transmutation strategy. We aim to elucidate the Am/Cm separation mechanism by various reagents at a molecular level to design a novel extraction reagent. This study focused on the Am/Cm separation with diglycolamide (DGA) and alkyl-diacetoamidamine (ADAAM) reagents by using density functional theory. We modeled the complex formation reactions by referring to reported single crystal structures and solvent extraction experiments. As the result, we succeeded in reproducing the Am/Cm separation behaviors with DGA and ADAAM reagents. Moreover, the electronic state analyses of the extracted complexes indicated that a difference in chemical bonding property of 5f-electrons between Am and Cm differentiates the Am/Cm selectivity.
Matsumura, Tatsuro; Ban, Yasutoshi; Suzuki, Hideya; Tsubata, Yasuhiro; Hotoku, Shinobu; Tsutsui, Nao; Suzuki, Asuka; Toigawa, Tomohiro; Kurosawa, Tatsuya*; Shibata, Mitsunobu*; et al.
no journal, ,
To continue the utilization of the nuclear fission energy, the management of the high-level radioactive waste is one of the most important issues to be solved. Partitioning and Transmutation technology is expected to be effective to mitigate the burden of the HLW disposal by reducing the radiological toxicity and heat generation. JAEA has been conducting R&D on the MA separation process to remove of MA from HLW and supply the recovered MA to the transmutation system such as ADS. The MA separation process contains three steps. For An(III)+RE recovery process, we developed TDdDGA which has very high performance to recover of MA from high level waste. HONTA and ADAAM were developed for An(III)/RE separation process and Am/Cm separation process respectively. All extractants satisfy CHON principle to minimization of the secondary waste from the process. The separation performances of the flowsheets were evaluated by continuous extraction tests using simulated and genuine high level liquid waste.
