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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

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

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

 Times Cited Count:1 Percentile:33.83(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

 Times Cited Count:0 Percentile:100(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

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

 Times Cited Count:7 Percentile:25.96(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

 Times Cited Count:4 Percentile:50.9(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

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

 Times Cited Count:6 Percentile:45.81(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

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

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

 Times Cited Count:11 Percentile:9.09(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.

JAEA Reports

Countercurrent extraction/stripping experiments using TDdDGA solvent extractant in a centrifugal contactor system,2; Evaluation on the improved flowsheet for MA recovery

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

JAEA-Research 2016-024, 40 Pages, 2017/02


The Japan Atomic Energy Agency has been developing some flowsheets with TDdDGA (N,N,N,Ntetradodecyldiglycolamide) extractant to recover MA (minor actinide) from raffinate. In this study, countercurrent experiments with the improved flowsheet, e.g. the addition of alcohol into the solvent for preventing the precipitation, were performed using miniature centrifugal contactors in order to compare the extraction/stripping behavior of each element with the mixer-settler type. As a result, no entrainments were observed and sufficient phase separation was achieved by centrifugal contactors without any abnormal fluid behavior, such as overflow. The extraction and stripping of Ln(III) which show the similar tendencies as MA could be achieved successfully, especially their stripping proceeded more efficiently in centrifugal contactors. This might be due to the increase in stripping rates by improving the flowsheet and to superior phase separation performance of centrifugal contactors.

Journal Articles

High-performance alkyl diamide amine and water-soluble diamide ligand for separating of Am(III) from Cm(III)

Suzuki, Hideya; Tsubata, Yasuhiro; Matsumura, Tatsuro

Analytical Sciences, 33(2), p.239 - 242, 2017/02

 Times Cited Count:7 Percentile:51.56(Chemistry, Analytical)

Alkyl diamide amine (ADAAM), a new high-performance reagent with a simple structure, was examined for the mutual separation of Am(III) and Cu(III). The combination of ADAAM and Tetraethyldiglycolamide (TEDGA) as a masking agent shows selectivity for Am(III) over Cm(III) in highly acidic media with separation factors up to 41.

Journal Articles

Highly practical and simple ligand for separation of Am(III) and Eu(III) from highly acidic media

Suzuki, Hideya; Tsubata, Yasuhiro; Kurosawa, Tatsuya; Shibata, Mitsunobu; Kawasaki, Tomohiro; Urabe, Shunichi*; Matsumura, Tatsuro

Analytical Sciences, 32(4), p.477 - 479, 2016/04

 Times Cited Count:14 Percentile:32.5(Chemistry, Analytical)

An impeccable, high-performance new reagent called alkyl diamide amine (ADAAM) was examined from the viewpoint of mutual separation of Am(III) and Eu(III). ADAAM has three donor atoms, one soft N-donor atom and two hard O-donor atoms, in the central frame. The combination of soft and hard atoms affords a tridentate donor set of atoms that ensures remarkable extractability and selectivity of Am(III) and Eu(III) in highly acidic media.

JAEA Reports

Countercurrent extraction/stripping experiments using TDdDGA solvent extractant in a centrifugal contactors system

Kibe, Satoshi; Fujisaku, Kazuhiko*; Ambai, Hiromu; Sakamoto, Atsushi; Sano, Yuichi; Takeuchi, Masayuki; Suzuki, Hideya; Tsubata, Yasuhiro; Matsumura, Tatsuro

JAEA-Research 2015-021, 40 Pages, 2016/02


The flowsheet with TDdDGA extractant has been being developed for recovering MA from PUREX raffinate. In the previous study, the yields of MA and other elements in countercurrent extraction/stripping experiments using mixer-settlers were not enough for the target and it would be due to the insufficient phase (aqueous/organic) separation. In this study, we carried out countercurrent experiments with surrogate PUREX raffinate using centrifugal contactors which had superior phase separation ability, and evaluated the extraction/stripping behavior of each element. During the operation, abnormal fluid behavior, such as overflow and entrainment, was not observed, and sufficient phase separation was achieved by centrifugal contactors. Extraction behavior of lanthanides was similar to that in mixer-settlers, but their stripping efficiencies decreased. This would be due to shorter residence time in mixing zone.

Journal Articles

Continuous liquid-liquid extraction of nickel from simulated electroless nickel plating liquid wastes by using a counter current emulsion flow extractor

Nagano, Tetsushi; Mitamura, Hisayoshi; Yamashita, Yuji; Yanase, Nobuyuki; Suzuki, Hideya; Naganawa, Hirochika

Solvent Extraction Research and Development, Japan, 21(1), p.111 - 117, 2014/00

Simulated electroless nickel plating liquid wastes have been processed by using an emulsion flow extractor of a counter current type with a special focus on influences of dilution of the liquid wastes on the extraction performance. The emulsion flow extractor provides an efficient liquid-liquid extraction by sending solutions without additional stirring or shaking. A solvent used in the present study was Shellsol D70 solution containing LIX84-I as an extractant for nickel and PC88A as an accelerating agent. As a result, it was found that increasing degree of dilution with water resulted in improvement of nickel extractabilities obtained from the emulsion flow experiments with a maximum value of 96% as well as those obtained from batch experiments. Droplet sizes at the lower and the upper sides of emulsion phases, estimated by using high-speed microscope, were 214 $$pm$$ 36 $$mu$$m and 415 $$pm$$ 110 $$mu$$m, respectively.

Journal Articles

Isotope dilution inductively coupled plasma mass spectrometry for determination of $$^{126}$$Sn content in spent nuclear fuel sample

Asai, Shiho; Toshimitsu, Masaaki; Hanzawa, Yukiko; Suzuki, Hideya; Shinohara, Nobuo; Inagawa, Jun; Okumura, Keisuke; Hotoku, Shinobu; Kimura, Takaumi; Suzuki, Kensuke*; et al.

Journal of Nuclear Science and Technology, 50(6), p.556 - 562, 2013/06

 Times Cited Count:7 Percentile:41.73(Nuclear Science & Technology)

The $$^{126}$$Sn content in a spent nuclear fuel solution was determined by ICP-MS for its inventory estimation in high-level radioactive waste. An irradiated UO$$_{2}$$ fuel was used as a sample to evaluate the reliability of the methodology. Prior to the measurement, Sn was separated from $$^{126}$$Te, which causes major isobaric interference in the determination of $$^{126}$$Sn content, along with highly radioactive coexisting elements using an anion-exchange column. The absence of counts attributed to Te in the Sn-containing effluent indicates that Te was completely removed. After washing, Sn retained on the column was readily eluted with 1 M HNO$$_{3}$$. The isotope ratios of Sn were successfully determined and showed good agreement with those obtained through ORIGEN2 calculations. The results reported in this paper are the first experimental values of $$^{126}$$Sn content in the spent nuclear fuel solution originating in spent nuclear fuel irradiated at a nuclear power plant in Japan.

Journal Articles

Simple cation-exchange separation for ICP-MS measurement of $$^{79}$$Se in spent nuclear fuel sample

Asai, Shiho; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Okumura, Keisuke; Shinohara, Nobuo; Kimura, Takaumi; Inagawa, Jun; Suzuki, Kensuke*; Kaneko, Satoru*

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 5 Pages, 2011/12

Journal Articles

Analyses of assay data of LWR spent nuclear fuels with a continuous-energy Monte Carlo code MVP and JENDL-4.0 for inventory estimation of $$^{79}$$Se, $$^{99}$$Tc, $$^{126}$$Sn and $$^{135}$$Cs

Okumura, Keisuke; Asai, Shiho; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Inagawa, Jun; Okamoto, Tsutomu; Shinohara, Nobuo; Kaneko, Satoru*; Suzuki, Kensuke*

Progress in Nuclear Science and Technology (Internet), 2, p.369 - 374, 2011/10

For accurate inventory estimation of long-lived fission products in LWR spent fuels, a new burn-up chain model and decay data based on the latest nuclear data such as JENDL-4.0 was developed. MVP-BURN with the latest nuclear data was applied to several post irradiation examinations including inventory measurements of $$^{79}$$Se, $$^{99}$$Tc, $$^{126}$$Sn and $$^{135}$$Cs. One of them is a new measurement by JAEA. From the PIE analyses, it is found that the new PIE data obtained by JAEA is consistent with the other PIE data by different laboratory with different techniques. It is also confirmed that the present calculation results show good agreements with experimental ones within about 10% for productions of $$^{79}$$Se and $$^{135}$$Cs. In contrast, amounts of $$^{99}$$Tc and $$^{126}$$Sn are overestimated by about 50%. These discrepancies are likely due to the effect of insoluble residue produced during sample dissolution and/or errors of fission yields in the analyses.

Journal Articles

Validation of correlations between Nd isotopes and difficult-to-measure nuclides predicted with burn-up calculation code by post irradiation examination

Asai, Shiho; Okumura, Keisuke; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Inagawa, Jun; Kimura, Takaumi; Kaneko, Satoru*; Suzuki, Kensuke*

Proceedings of 14th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2011) (CD-ROM), p.1437 - 1442, 2011/09

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