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Journal Articles

Pretransitional multiscale structure preceding third-phase formation in solvent extraction systems

Guerinoni, E.*; Ueda, Yuki; Motokawa, Ryuhei; Zemb, T.*; Pellet-Rostaing, S.*; Dourdain, S.*

Langmuir, 42(12), p.8313 - 8321, 2026/03

Journal Articles

Separation of Rh(III) and direct electrodeposition in phosphonium-based ionic liquids with electrochemical and spectroscopic analyses for extracted Rh(III) complex

Tokumitsu, Shun*; Matsumiya, Masahiko*; Sasaki, Yuji

Separation and Purification Technology, 382(Part 2), p.135631_1 - 135631_9, 2026/02

 Times Cited Count:0 Percentile:0.00

Journal Articles

Selective extraction and back-extraction of strontium using crown ether in 1-octanol/dodecane mixed solvents; Control of acid co-extraction and separation from multi-element systems

Saga, Kaname; Ban, Yasutoshi

Solvent Extraction and Ion Exchange, 18 Pages, 2026/00

 Times Cited Count:0 Percentile:0.00(Chemistry, Multidisciplinary)

JAEA Reports

Separation test of heat generating nuclides from high-level liquid waste

Hotoku, Shinobu; Ban, Yasutoshi; Konda, Miki; Kitatsuji, Yoshihiro

JAEA-Technology 2025-009, 33 Pages, 2025/11

JAEA-Technology-2025-009.pdf:1.9MB

High-level liquid waste (HLLW) produced from reprocessing of spent nuclear fuels contains heat generating nuclides such as Sr-90, Y-90, Cs-137, Ba-137m, and Am-241. Separation and recovery of these nuclides lead to reduce the volume and toxicity of high-level waste. Furthermore, the recovered nuclides and elements could be utilized as resources after purification. In this test, Sr separation by extraction chromatography using Sr resin and Pb resin, Cs separation by co-precipitation using ammonium phosphomolybdate (AMP), and Am separation by solvent extraction using alkyl diamideamine (ADAAM) were carried out, cold tests were performed for the separation of Cs and Sr in a nitric acid solution. Based on the results, hot tests were performed using dissolution solutions of spent fuel at the Nuclear Fuel Cycle Safety Engineering Research Facility (NUCEF), and each component contained in the separated solution was analyzed. In the Sr separation by extraction chromatography, most of Sr was separated from other elements using 8 mol/L nitric acid for absorption and 0.02 mol/L nitric acid for elution. In the separation of Cs, more than 99.9% of Cs was selectively co-precipitated by adding AMP to the HLLW, in which nitric acid concentration was adjusted to 3.1 mol/L. In solvent extraction of Am by ADAAM, 81.4% of Am-241 was recovered by a single stage batch experiment. Since Sr, Cs, and Am were properly separated and recovered from HLLW, the effectiveness of the present separation method was successfully demonstrated.

Journal Articles

A Simple process simulation method for radiation stability evaluation of minor actinides separation

Toigawa, Tomohiro; Tsubata, Yasuhiro; Kumagai, Yuta; Ban, Yasutoshi

Progress in Nuclear Science and Technology (Internet), 8, p.286 - 290, 2025/09

We propose a simple process simulation methodology that uses readily available information about radiation impact. A process simulation was conducted for a minor actinides (MA) separation process while considering the degradation of extraction ability by radiolysis. The simulation provided a processing limit of MA and enabled the evaluation of radiation stability.

Journal Articles

A Basic study for radioactive nuclides recovery from spent PUREX solvent using adsorbents

Arai, Tsuyoshi*; Nakamura, Fumiya*; Abe, Ryoji*; Ueno, Fuga*; Seko, Noriaki*; Arai, Yoichi; Watanabe, So

Progress in Nuclear Science and Technology (Internet), 7, p.147 - 153, 2025/03

no abstracts in English

Journal Articles

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, 61(7), p.883 - 893, 2024/07

 Times Cited Count:5 Percentile:63.07(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-$$n$$-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.

Journal Articles

Post-earthquake rapid resealing of bedrock flow-paths by concretion-forming resin

Yoshida, Hidekazu*; Yamamoto, Koshi*; Asahara, Yoshihiro*; Maruyama, Ippei*; Karukaya, Koichi*; Saito, Akane*; Matsui, Hiroya; Mochizuki, Akihito; Jo, Mayumi*; Katsuta, Nagayoshi*; et al.

Communications Engineering (Internet), 3, p.67_1 - 67_10, 2024/05

A capability to permanently seal fluid flow-paths through bedrock, like boreholes or underground tunnels, is needed to ensure the long-term safety and effectiveness of many underground activities e.g. CO$$_{2}$$ storage, hydrocarbon field abandonment, and nuclear waste disposal. Commonly used cementitious seals may not be sufficiently durable due to chemical and physical degradation. Learning from natural calcite (CaCO$$_{3}$$) concretion formation, a more durable sealing method was developed using a "concretion-forming solvent". The method was tested by sealing flow-paths next to a tunnel in an underground research laboratory at 350 meters depth. The flow-paths initially sealed rapidly, then resealed after disturbance by earthquakes (M5.4). The treated rock recovered its very low natural permeability, demonstrating permanent sealing that is robust.

Journal Articles

Organization of malonamides from the interface to the organic bulk phase

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Yamada, Norifumi*; Yamada, Masako*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.

Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05

 Times Cited Count:4 Percentile:54.90(Chemistry, Physical)

Journal Articles

Rapid and long-lasting bedrock flow-path sealing by a "concretion-forming resin"; Results from ${it in-situ}$ evaluation tests in an Underground Research Laboratory, Horonobe, Japan

Yoshida, Hidekazu*; Yamamoto, Koshi*; Asahara, Yoshihiro*; Maruyama, Ippei*; Karukaya, Koichi*; Saito, Akane*; Matsui, Hiroya; Mochizuki, Akihito; Katsuta, Nagayoshi*; Metcalfe, R.*

Powering the Energy Transition through Subsurface Collaboration; Proceedings of the 1st Energy Geoscience Conference (Energy Geoscience Conference Series, 1), 20 Pages, 2024/00

A capability to permanently seal fluid flow-paths in bedrock, such as natural faults/fractures, and damaged zones around boreholes/excavations, is needed to ensure the long-term safety and effectiveness of many underground activities. Cementitious materials are commonly used as seals, however these materials unavoidably undergo physical and chemical degradation, therefore potentially decreasing seal durability. In order to solve these problems, a more durable sealing method using concretion-forming resin has been developed by learning from natural calcite (CaCO$$_{3}$$) concretion formation. The sealing capability of resin was tested by ${it in-situ}$ experiments on bedrock flow-paths in an underground research laboratory (URL), Hokkaido, Japan. The results showed a decrease the permeability rapidly down to 1/1,000 of the initial permeability due to calcite precipitation over a period of one year. During the experiment inland earthquakes occurred with foci below the URL (depths 2-7 km and maximum magnitude 5.4). Due to the earthquakes the hydraulic conductivities of the flow-paths sealed initially by concretion-forming resin increased. However, these flow-paths subsequently resealed rapidly, and within a few months recovered the same hydraulic conductivities as before the earthquakes. This new technique for rapidly producing long-lasting seals against fluid flow through rocks will be applicable to many kinds of underground activities.

Journal Articles

Extraction of Rh(III) from hydrochloric acid by protonated NTAamide(C6) and analogous compounds and understanding of extraction equilibria by using UV spectroscopy and DFT calculations

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:21.47(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$$_{2}$$O complexes are formed in HCl media and show the slow exchange rate between Cl and H$$_{2}$$O. Using the UV spectrum, Rh-chloride solution having the peak of spectrum at 504 nm can be extracted effectively, where RhCl$$_{4}$$(H$$_{2}$$O)$$^-$$ and RhCl$$_5$$(H$$_2$$O)$$^2$$$$^-$$ 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.

Journal Articles

Evaluation of the remaining spent extraction solvent in vermiculite after leaching tests via PIXE analysis

Arai, Yoichi; Watanabe, So; Hasegawa, Kenta; Okamura, Nobuo; Watanabe, Masayuki; Takeda, Keisuke*; Fukumoto, Hiroki*; Ago, Tomohiro*; Hagura, Naoto*; Tsukahara, Takehiko*

Nuclear Instruments and Methods in Physics Research B, 542, p.206 - 213, 2023/09

 Times Cited Count:1 Percentile:17.23(Instruments & Instrumentation)

Journal Articles

Extraction of Se(iv) and Se(vi) from aqueous HCl solution by using a diamide-containing tertiary amine

Narita, Hirokazu*; Maeda, Motoki*; Tokoro, Chiharu*; Suzuki, Tomoya*; Tanaka, Mikiya*; Shiwaku, Hideaki; Yaita, Tsuyoshi

RSC Advances (Internet), 13(25), p.17001 - 17007, 2023/06

 Times Cited Count:3 Percentile:19.64(Chemistry, Multidisciplinary)

no abstracts in English

Journal Articles

Combining a lipophilic phenanthroline carboxamide and a hydrophilic diglycolamide to increase the separation factors of adjacent light lanthanides

Simonnet, M.; Sasaki, Yuji; Yaita, Tsuyoshi

Solvent Extraction and Ion Exchange, 41(7), p.857 - 867, 2023/00

 Times Cited Count:5 Percentile:33.52(Chemistry, Multidisciplinary)

Journal Articles

Cs extraction from chloride media by calixarene crown-ethers

Simonnet, M.; Sittel, T.*; We${ss}$ling, P.*; Geist, A.*

Energies (Internet), 15(20), p.7724_1 - 7724_10, 2022/10

 Times Cited Count:8 Percentile:29.61(Energy & Fuels)

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:9 Percentile:39.79(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

Study on phenanthroline carboxamide for lanthanide separation; Influence of amide substituents

Simonnet, M.; Kobayashi, Toru; Shimojo, Kojiro; Yokoyama, Keiichi; Yaita, Tsuyoshi

Inorganic Chemistry, 60(17), p.13409 - 13418, 2021/09

 Times Cited Count:30 Percentile:91.31(Chemistry, Inorganic & Nuclear)

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:4 Percentile:22.15(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

Synthesis of graft polymerization-type porous silica adsorbent with IDA group and evaluation of adsorption performance using micro-PIXE analysis

Arai, Yoichi; Watanabe, So; Ono, Shimpei; Nakamura, Masahiro; Shibata, Atsuhiro; Nakamura, Fumiya*; Arai, Tsuyoshi*; Seko, Noriaki*; Hoshina, Hiroyuki*; Fukumoto, Hiroki*; et al.

QST-M-29; QST Takasaki Annual Report 2019, P. 54, 2021/03

Journal Articles

Radiation-induced effects on the extraction properties of hexa-$$n$$-octylnitrilo-triacetamide (HONTA) complexes of americium and europium

Toigawa, Tomohiro; Peterman, D. R.*; Meeker, D. S.*; Grimes, T. S.*; Zalupski, P. R.*; Mezyk, S. P.*; Cook, A. R.*; Yamashita, Shinichi*; Kumagai, Yuta; Matsumura, Tatsuro; et al.

Physical Chemistry Chemical Physics, 23(2), p.1343 - 1351, 2021/01

 Times Cited Count:25 Percentile:82.92(Chemistry, Physical)

The candidate An(III)/Ln(III) separation ligand hexa-$$n$$-octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions using a solvent test loop in conjunction with cobalt-60 gamma irradiation. We demonstrate that HONTA undergoes exponential decay with increasing gamma dose to produce a range of degradation products which have been identified and quantified by HPLC-ESI-MS/MS techniques. The combination of HONTA destruction and degradation product ingrowth, particularly dioctylamine, negatively impacts the extraction and back-extraction of both americium and europium ions. The loss of HONTA was attributed to its reaction with the solvent (${it n}$-dodecane) radical cation of ${it k}$(HONTA + R$$^{.+}$$) = (7.61 $$pm$$ 0.82) $$times$$ 10$$^{9}$$ M$$^{-1}$$ s$$^{-1}$$ obtained by pulse radiolysis techniques. However, when this ligand is bound to either americium or europium ions, the observed ${it n}$-dodecane radical cation kinetics increase by over an order of magnitude. This large reactivity increase to additional reaction pathways occurring upon metal-ion binding. Lastly nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived ($$<$$100 ns) HONTA radical cation as well as a longer-lived ($$mu$$s) HONTA triplet excited state. These HONTA species are important precursors to the suite of HONTA degradation products observed.

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