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Journal Articles

A Demonstration test to separate minor actinides in high-level liquid waste by ${it N,N,N',N',N'',N''}$-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 ${it N,N,N',N',N'',N''}$-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$$^{3}$$ in ${it n}$-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.

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, 11 Pages, 2023/11

https://doi.org/10.1080/00223131.2023.2283214
 Times Cited Count：0 Percentile：0.01(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

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
 Times Cited Count：2 Percentile：76.52(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 ($$SF$$$$_{rm Cm/Nd}$$ = 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.

Journal Articles

Extraction properties of trivalent rare earth ions from nitric acid using a triamide-amine extractant

Uchino, Seiko*; Narita, Hirokazu*; Kita, Keisuke*; Suzuki, Hideya*; Matsumura, Tatsuro; Naganawa, Hirochika*; Sakaguchi, Koichi*; Oto, Keisuke*

Solvent Extraction Research and Development, Japan, 30(1), p.39 - 46, 2023/00

https://doi.org/10.15261/serdj.30.39

The extraction of trivalent rare earth ions (RE$$^{3+}$$) from HNO$$_{3}$$ solution using a triamide amine, tris(N,N-di-2-ethylhexyl-ethylamide)amine (DEHTAA), was conducted, and the extraction mechanism was estimated from extraction behavior of HNO$$_{3}$$ and RE$$^{3+}$$ and the relationship between atomic number and extraction percentages (E%) for RE$$^{3+}$$. A DEHTAA molecule dominantly formed a DEHTAA HNO$$_{3}$$ at 1.0 M HNO$$_{3}$$ and a DEHTAA(HNO$$_{3}$$)$$_{2}$$ at 6.0 M HNO$$_{3}$$ in the acid-equilibrated organic phase. This would provide the unique dependence of E% for the light RE$$^{3+}$$ on the HNO$$_{3}$$ concentration, in which the E% value had a minimum and maximum at $$sim$$0.5 M and $$sim$$2 M HNO$$_{3}$$, respectively. The results of the slope analyses for the distribution ratios for RE$$^{3+}$$ suggested that the dominant RE$$^{3+}$$ complex was RE(NO$$_{3}$$)$$_{3}$$DEHTAA(DEHTAA HNO$$_{3}$$) at 1.0 M HNO$$_{3}$$. The E% for RE$$^{3+}$$ decreased from La$$^{3+}$$ to Lu$$^{3+}$$ at 1.0 M HNO$$_{3}$$; on the other hand, those increased from La$$^{3+}$$ to Nd$$^{3+}$$ at 0.25 M and from La$$^{3+}$$ to Sm$$^{3+}$$ and 6.0 M HNO$$_{3}$$.

JAEA Reports

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$$_{3}$$ 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$$_{3}$$ / 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$$_{3}$$ / HONTA - n-dodecane system are under 10$$^{-6}$$ m/s.

Journal Articles

Solvent extraction of technetium(VII) and rhenium(VII) using a hexaoctylnitrilotriacetamide extractant

Shimojo, Kojiro; Suzuki, Hideya; Yokoyama, Keiichi; Yaita, Tsuyoshi; Ikeda, Atsushi

Analytical Sciences, 36(12), p.1435 - 1437, 2020/12

https://doi.org/10.2116/analsci.20C014
 Times Cited Count：13 Percentile：64.65(Chemistry, Analytical)

Liquid-liquid extraction for the removal of pertechnetate ($$^{99}$$TcO$$_{4}$$$$^{-}$$) and perrhenate (ReO$$_{4}$$$$^{-}$$) is reported using tripodal extractant $$N,N,N',N',N'',N''$$-hexa-$$n$$-octylnitrilotriacetamide (HONTA) composed of three amide groups and a tertiary amine. The extraction behavior was compared with those using alkyldiamideamines (ADAAM(Oct) and ADAAM(EH)), and the commercial amine-type extractant, trioctylamine (TOA). HONTA quantitatively extracted $$^{99}$$TcO$$_{4}$$$$^{-}$$ and ReO$$_{4}$$$$^{-}$$ in the pH range from 1.0 to 2.5 by co-extraction of protons. Extraction performance of extractants was improved in the order of HONTA $$>$$ ADAAM(Oct) $$>$$ ADAAM(EH) $$>$$ TOA. $$^{99}$$TcO$$_{4}$$$$^{-}$$ and ReO$$_{4}$$$$^{-}$$ in the extracting phase were successfully stripped using neutral aqueous solutions as the receiving phase, and the extraction ability of HONTA was maintained after five repeated uses.

Journal Articles

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

Toigawa, Tomohiro; Murayama, Rin*; Kumagai, Yuta; Yamashita, Shinichi*; Suzuki, Hideya; Ban, Yasutoshi; Matsumura, Tatsuro

UTNL-R-0501, p.24 - 25, 2020/12

This report summarizes the results obtained in FY2019 at Electron Linac Facility of University of Tokyo. The radiolysis process of a diglycolamide extractant, which is expected to be used in the separation process of minor actinides (MA), in dodecane and octanol solutions was investigated by pulse radiolysis. As a result, it was suggested that by adding alcohol, the decomposition process of the diglycolamide extractant was different from the decomposition processes in the single solvent of dodecane considered that the decomposition occurred via a radical cation species of the extractant.

Journal Articles

Effects of diluents on the separation of minor actinides from lanthanides with tetradodecyl-1,10-phenanthroline-2,9-diamide from nitric acid medium

Tsutsui, Nao; Ban, Yasutoshi; Suzuki, Hideya*; Nakase, Masahiko*; Ito, Sayumi*; Inaba, Yusuke*; Matsumura, Tatsuro; Takeshita, Kenji*

Analytical Sciences, 36(2), p.241 - 246, 2020/02

https://doi.org/10.2116/analsci.19P275
 Times Cited Count：21 Percentile：79.8(Chemistry, Analytical)

To investigate the effective separation of actinides (Ans) from lanthanides (Lns), single-stage batch extraction experiments were performed with a novel extractant, tetradodecyl-1,10-phenanthroline-2,9-diamide (TDdPTDA) with various diluents such as 3-nitrobenzotrifluoride (F-3), nitrobenzene, and ${it n}$-dodecane for Am, Cm, and Lns. The extraction kinetics with TDdPTDA was rapid enough to perform the actual extraction flow sheet. The slopes of the distribution ratio versus TDdPTDA concentration and the distribution ratio versus nitric acid concentration were similar for F-3 and nitrobenzene systems but different from ${it n}$-dodecane system. These differences were attributed to the characteristics of the diluents. This study reveals high distribution ratios of Am (${it D}$ $$_{Am}$$) and Cm (${it D}$ $$_{Cm}$$) for TDdPTDA, with the high separation factors (${it SF}$s) of Am from Lns enough for their separation.

Journal Articles

No secondary waste recycle technology for rare metals using the hydrophilic extraction with phase transfer phenomena

Tsukahara, Takehiko*; Saga, Kaname*; Suzuki, Hideya*; Matsumura, Tatsuro

Kurin Tekunoroji, 29(12), p.4 - 7, 2019/12

no abstracts in English

Journal Articles

Minor actinides separation by ${it N,N,N',N',N'',N''}$-hexaoctyl nitrilotriacetamide (HONTA) using mixer-settler extractors in a hot cell

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

Solvent Extraction and Ion Exchange, 37(7), p.489 - 499, 2019/11

https://doi.org/10.1080/07366299.2019.1693486
 Times Cited Count：15 Percentile：52.81(Chemistry, Multidisciplinary)

A continuous counter-current experiment to separate minor actinides (MAs: Am and Cm) was performed with ${it N,N,N',N',N'',N''}$-hexaochyl nitrilotriacetamide (HONTA) as an extractant. Nitric acid of 0.08 M (mol/dm$$^{3}$$) containing MAs and rare earths (REs) recovered from high-level waste was used as the Feed, and the experiment was conducted for 14 h. The ratios of Am and Cm recovered into the MA fraction measured 94.9% and 78.9%, respectively. HONTA hardly extracted Y, La, and Eu in the Feed (99.9% for Y, 99.9% for La, and 96.7% for Eu), most of which were distributed to the RE fraction. A portion of Nd was extracted by HONTA, and consequently the ratio of Nd in the RE fraction was 83.5%. The concentrations of MAs and some REs in each stage were calculated using a simulation code, and the results are consistent with the experimental values. This code indicates that the ratios of MAs in the MA fraction and REs in the RE fraction could be $$geq$$99% by optimizing separation conditions.

Journal Articles

Zr separation from high-level liquid waste with a novel hydroxyacetoamide type extractant

Morita, Keisuke; Suzuki, Hideya; Matsumura, Tatsuro; Takahashi, Yuya*; Omori, Takashi*; Kaneko, Masaaki*; Asano, Kazuhito*

Proceedings of International Nuclear Fuel Cycle Conference / Light Water Reactor Fuel Performance Conference (Global/Top Fuel 2019) (USB Flash Drive), p.464 - 468, 2019/09

High level liquid waste (HLLW) contains several radionuclides with half-lives longer than 10$$^{6}$$ year. For reduce environmental burden of waste disposal, minor actinoids and long-lived fission products will to be partitioned and transmuted. JAEA and Toshiba developed process for recovering Se, Zr, Pd and Cs from HLLW. Solvent extraction for Zr with novel extractant, ${it N,N}$-didodecyl-2-hydroxyacetoamide (HAA) was detailed. The HAA system showed high selectivity for Zr, as indicated by the extraction order of Zr $$>$$ Mo $$>$$ Pd $$>$$ Ag $$approx$$ Sb $$>$$ Sn $$>$$ Lns $$>$$ Fe. The extracted species was determined as Zr(HAA)$$_{3}$$(NO$$_{3}$$)$$_{4}$$(HNO$$_{3}$$)$$_{x}$$. A continuous countercurrent extraction with HAA was applied to a simulated, concentrated HLLW after Pd, Se, and Cs removal, where the quantitative extraction of Zr and Mo was effectively demonstrated.

Journal Articles

Mechanism of palladium(II) adsorption from nitric acid solutions by a styrene-divinylbenzene copolymer functionalized with $$N,N,N$$-trimethylglycine

Suzuki, Tomoya*; Narita, Hirokazu*; Ogata, Takeshi*; Suzuki, Hideya; Matsumura, Tatsuro; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi

Solvent Extraction Research and Development, Japan, 26(1), p.11 - 19, 2019/06

https://doi.org/10.15261/serdj.26.11
 Times Cited Count：3 Percentile：14.02(Chemistry, Multidisciplinary)

The ability of AMP03, a styrene-divinylbenzene copolymer functionalized with $$N,N,N$$-trimethylglycine moieties, to adsorb Pd(II) from HNO$$_{3}$$ solutions was investigated to elucidate the affinity of $$N,N,N$$-trimethylglycine for Pd(II). In the present study, we investigated the mechanism of Pd(II) adsorption by AMP03 by means of adsorption experiments, Fourier Transform Infrared (FT-IR) spectroscopy, and Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy.

Journal Articles

Direct temperature-swing extraction of rare-earth elements from acidic solution using the hydrophobic interactions of poly($$N$$-isopropylacrylamide) with diglycolamide-typed ligands

Saga, Kaname*; Suzuki, Hideya; Matsumura, Tatsuro; Tsukahara, Takehiko*

Analytical Sciences, 35(4), p.461 - 464, 2019/04

https://doi.org/10.2116/analsci.18N023
 Times Cited Count：3 Percentile：7.76(Chemistry, Analytical)

The phase transition-based gelification phenomenon of poly-$$N$$-isopropylacrylamide (PNIPAAm) in aqueous solutions has a great potential in developing new waste-free extraction processes of metal ions. By using hydrophobic diglycolamide-typed ligands in gelification extraction, a one-step complete extraction of all the RE ions from a nitric acid solution was successfully realized.

Journal Articles

Separation and recovery of raremetals using the hydrophiric extraction with phase transfer phenomena

Tsukahara, Takehiko*; Suzuki, Hideya*; Matsumura, Tatsuro; Saga, Kaname*

Bunri Gijutsu, 49(4), p.221 - 225, 2019/04

https://cir.nii.ac.jp/crid/1520290884182105728

no abstracts in English

Journal Articles

Extraction of trivalent rare earths and minor actinides from nitric acid with ${it N,N,N',N'}$-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
 Times Cited Count：21 Percentile：65.06(Chemistry, Multidisciplinary)

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$$^{3}$$ 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.

Journal Articles

Theoretical elucidation of Am(III)/Cm(III) separation mechanism with diamide-type ligands using relativistic density functional theory calculation

Kaneko, Masashi; Suzuki, Hideya; Matsumura, Tatsuro

Inorganic Chemistry, 57(23), p.14513 - 14523, 2018/12

https://doi.org/10.1021/acs.inorgchem.8b01624
 Times Cited Count：20 Percentile：78.15(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)$$_{3}$$]$$^{3+}$$ and [M(ADAAM)(NO$$_{3}$$)$$_{3}$$(H$$_{2}$$O)]. 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)$$_{3}$$]$$^{3+}$$ and [M(ADAAM)(NO$$_{3}$$)$$_{3}$$(H$$_{2}$$O)], 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.

Journal Articles

Characteristics of TPDN/SiO$$_{2}$$-P adsorbent for MA(III) recovery

Kofuji, Hirohide; Watanabe, So; Takeuchi, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.61 - 65, 2018/11

https://doi.org/10.15669/pnst.5.61

Journal Articles

Continuous liquid-liquid extraction of uranium from uranium-containing wastewater using an organic phase-refining-type emulsion flow extractor

Nagano, Tetsushi; Naganawa, Hirochika; Suzuki, Hideya; Toshimitsu, Masaaki*; Mitamura, Hisayoshi*; Yanase, Nobuyuki*; Grambow, B.

Analytical Sciences, 34(9), p.1099 - 1102, 2018/09

https://doi.org/10.2116/analsci.18N002
 Times Cited Count：12 Percentile：45.99(Chemistry, Analytical)

A previously reported emulsion flow (EF) extraction system does not include a device for refining used solvent. Therefore, the processing of large quantities of wastewater by using the EF extractor alone could lead to the accumulation of wastewater components into the solvent and diminished extraction performance. In the present study, we have developed a solvent-washing-type EF system, which is equipped with a unit for washing used solvent to prevent accumulation, and successfully applied it for treating uranium-containing wastewater.

Journal Articles

Selective Sc recovery from rare earths in nitric acid medium by extraction chromatography

Watanabe, So; Suzuki, Hideya; Goto, Ichiro*; Kofuji, Hirohide; Matsumura, Tatsuro

Nihon Ion Kokan Gakkai-Shi, 29(3), p.71 - 75, 2018/09

https://doi.org/10.5182/jaie.29.71

Journal Articles

Continuous extraction and separation of Am(III) and Cm(III) using a highly practical diamide amine extractant

Suzuki, Hideya; Tsubata, Yasuhiro; Kurosawa, Tatsuya*; Sagawa, Hiroshi*; Matsumura, Tatsuro

Journal of Nuclear Science and Technology, 54(11), p.1163 - 1167, 2017/11

https://doi.org/10.1080/00223131.2017.1299050
 Times Cited Count：26 Percentile：93.3(Nuclear Science & Technology)

A highly practical diamide-type extractant, which is an alkyl diamide amine with 2-ethylhexyl alkyl chains (ADAAM(EH)), was investigated for mutual separation of Am(III) and Cm(III). ADAAM(EH) is a multidentate ligand with one soft N-donor atom and two hard O-donor atoms in its central frame. This tridentate arrangement of donor atoms provides selective binding to Am(III) compared to that with Cm(III) in highly acidic media, resulting in separation factors of up to 5.5. A continuous liquid-liquid extraction and stripping test was conducted using a multistage countercurrent mixer-settler extractor with ADAAM(EH) in n-dodecane. In this test, separation of Am(III) and Cm(III) was achieved with very high yield.

121 (Records 1-20 displayed on this page)