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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

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:3 Percentile:75.76(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.

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:6 Percentile:39.88(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

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

Oral presentation

Current status of R&D of MA separation processes for P&T technology

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

no journal, , 

no abstracts in English

Oral presentation

Study of radiolysis of HONTA extractant for MA/Ln separation

Toigawa, Tomohiro; Suzuki, Hideya; Ban, Yasutoshi; Ishii, Sho; Matsumura, Tatsuro

no journal, , 

Degradation of extractants and generation of radiolytic products are considered as problem for feasibility of the minor actinides separation process. In this study, degradation amount of hexaoctyl-nitrilotriacetamide (HONTA), which is a candidate extaractant for MA/Ln separation, and its products yields were obtained by using $$gamma$$-rays emitted from Co-60. Our results showed the cleavage sites in HONTA radiolysis and suggest that the mechanism for HONTA radiolysis is differ depending on the absorbed dose.

Oral presentation

Radiolysis of HONTA extractant for MA/RE separation

Toigawa, Tomohiro; Suzuki, Hideya; Ban, Yasutoshi; Ishii, Sho*; Matsumura, Tatsuro

no journal, , 

R&D on partitioning process of the minor actinides (MA) from high level liquid waste (HLLW) were carried out for reduction of the strain on the radioactive wastes disposal. In this study, degradation amount of hexaoctyl-nitrilotriacetamide (HONTA), which is a candidate extaractant for MA/RE separation, and its products yields were obtained by using $$gamma$$-rays emitted from Co-60. Our results showed the cleavage sites in HONTA radiolysis and suggest that the mechanism for HONTA radiolysis is differ depending on the absorbed dose.

Oral presentation

Current status of R&D on reprocessing and minor actinide separation process with CHON ligands in JAEA

Matsumura, Tatsuro; Ban, Yasutoshi; Suzuki, Hideya; Tsubata, Yasuhiro; Hotoku, Shinobu; Tsutsui, Nao; Suzuki, Asuka; Toigawa, Tomohiro; Kurosawa, Tatsuya*; Shibata, Mitsunobu*; et al.

no journal, , 

PUREX process was established for industrial scale reprocessing plant. TRUEX and the 4 group separation were developed for partitioning of minor actinides from HLW, and demonstrated using genuine HLW. Although the extractants for the processes have excellent performance, the molecules contain phosphorus which could be cause for the secondary waste from the solvent extraction processes. To minimize the radioactive waste, we have conducted research and development of the new reprocessing and MA separation processes using innovative extractants in accord with CHON principle. The extractants for reprocessing process are monoamides as alternative extractants for TBP. For An(III)+RE recovery process, we developed TDdDGA. HONTA and ADAAM were developed for An(III)/RE separation process and Am/Cm separation process respectively. The separation performances of the flowsheets were evaluated by continuous extraction tests using simulated and genuine spent fuel and high level liquid waste.

Oral presentation

Influence of $$gamma$$-radiolysis of MA separation agent of HONTA on extraction performance

Toigawa, Tomohiro; Suzuki, Hideya; Ban, Yasutoshi; Ishii, Sho*; Matsumura, Tatsuro

no journal, , 

To evaluate the radiolytic stability of a novel tetradentate extractant of N, N, N', N', N", N"-hexaoctyl-nitrilotriacetamide (HONTA), batch extractions of lanthanide (Ln) elements were performed by using $$gamma$$-irradiated HONTA extraction solvents. The distribution ratios decreased exponentially with increasing the absorbed dose, and no difference between Ln could be observed. These indicate that the degradation products of HONTA did not act as Ln extractants, and the decay of Ln extraction were caused by degradation of HONTA.

Oral presentation

Influence of $$gamma$$-radiolysis of a minor actinide extractnt on lanthanides extraction

Toigawa, Tomohiro; Suzuki, Hideya; Ishii, Sho*; Tsutsui, Nao; Ban, Yasutoshi; Matsumura, Tatsuro

no journal, , 

To evaluate the radiolytic stability of an extractant agents for minor actinides such as N, N, N', N', N", N"-hexaoctyl-nitrilotriacetamide (HONTA), batch extractions of lanthanide (Ln) elements were performed by using $$gamma$$-irradiated extraction solvents. The distribution ratios decreased exponentially with increasing the absorbed dose, and no initial decrease could be observed.

Oral presentation

Research and development of the "SELECT process" for actinide separation, 2; Investigation of new extractants for MA/RE separation

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

no journal, , 

The Japan Atomic Energy Agency is engaged in research and development of the "SELECT process" which is a separation technology for recovering actinides from spent fuel. A highly practical reagent, called HONTA, was developed. In the present study, HONTA was tested for the mutual separation of MA and RE.

Oral presentation

Study on radiolytic degradation of extractants for minor actinide separation

Toigawa, Tomohiro; Kumagai, Yuta; Yamashita, Shinichi*; Suzuki, Hideya; Matsumura, Tatsuro

no journal, , 

The radiolytic degradation of amidic extractants excepted to be used in the minor actinide sepation were observed by using the pulse radiolysis system in The University of Tokyo. It was found that a intermediate specie for degradation was generated not only by direct ionization of the extractant but also derived from the diluent ionization.

Oral presentation

Study on mass transfer kinetics in solvent extraction systems for minor actinides recovery

Sano, Yuichi; Kawanobe, Kazunori*; Sakamoto, Atsushi; Kofuji, Hirohide; Takeuchi, Masayuki; Suzuki, Hideya; Matsumura, Tatsuro

no journal, , 

Japan Atomic Energy Agency (JAEA) has developed several new extractants which are significantly effective in trivalent minor actinides (MA(III)) recovery from high acidic media such as high level liquid waste (HLLW). In order to design an efficient MA(III) recovery process using these new extractants, it is important to obtain their kinetic data as well as equilibrium ones in the solvent extraction system. In this study, mass transfer coefficients of trivalent lanthanides (Ln(III)), which are surrogates of MA(III), between HNO$$_{3}$$ solution and tetra dodecyl diglycol amide (TDdDGA) or hexa octyl nitrilo triacetic amide (HONTA) / n-dodecane solvent were evaluated by the single drop technique and Nitsch cell tests. The mass transfer coefficients of Ln(III) back-extraction in HNO$$_{3}$$ / TDdDGA system were relatively smaller than those in the extraction step, but they could be improved by the addition of 2-ethyl-1-hexanol into the TDdDGA / n-dodecane solvent. The mass transfer of Ln(III) between HNO$$_{3}$$ solution and HONTA/n-dodecane solvent was considerably slower than that between HNO$$_{3}$$ solution and TDdDGA / n-dodecane solvent. Based on the mass transfer coefficients obtained in these evaluations, process conditions for MA(III) recovery using mixer-settlers and centrifugal contactors were discussed.

Oral presentation

Investigation of new extractants for MA/RE separation

Suzuki, Hideya; Tsubata, Yasuhiro; Matsumura, Tatsuro

no journal, , 

The Japan Atomic Energy Agency has been studying partitioning and transmutation systems. In this partitioning process, new extractants with highly practical and high extraction ability for minor actinoids was developed. New extractants, called NTAamide, were tested for mutual separation of trivalent minor actinoids and trivalent rare earth elements. Among the four NTAamides, hexaoctylnitrilotriacetamide (HONTA) provided the largest distribution ratio of trivalent americium, and was chosen. A continuous liquid-liquid extraction test was conducted using a multistage countercurrent mixer-settler extractor with HONTA. In this test, separation of MA(III) and RE(III) was achieved with very high yield.

Oral presentation

Development on SELECT process for reprocessing and minor actinide separation in JAEA

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

no journal, , 

To minimize the radioactive waste from nuclear fuel cycle, we have conducted research and development of the new reprocessing and MA separation process, SELECT process (Solvent Extraction from Liquid-waste using Extractants of CHON-type for Transmutation), using innovative extractants. The extractants for each solvent extraction processes were developed in JAEA. The extractants for reprocessing process are monoamides as alternative extractants for TBP. For MA+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 MA/RE separation process and Am/Cm separation process respectively. All of the extractants consist of C, H, O, and N elements, and can be decomposed to gases by incineration. The demonstration tests using genuine spent fuel and high level liquid waste of the SELECT process have been conducted. Uranium solution and U+Pu mixed solution were separated from spent fuel, and MA, americium and curium, were recovered and separated from HLW effectively. The details of the extraction tests for each separation processes will be presented in correspond presentations in this conference.

Oral presentation

Study on mass transfer kinetics in solvent extraction systems for minor actinides recovery

Sano, Yuichi; Sakamoto, Atsushi; Takeuchi, Masayuki; Suzuki, Hideya*; Matsumura, Tatsuro; Kawanobe, Kazunori*; Asano, Shusaku*; Maki, Taisuke*; Mae, Kazuhiro*

no journal, , 

The mass transfer coefficients during the extraction and back-extraction of lanthanide elements in the solvent extraction process using new extractants (TDdDGA, HONTA) developed for minor actinides (MA) recovery were evaluated. In the TDdDGA system, it was confirmed that the mass transfer coefficients during back extraction were improved by the addition of alcohol to the solvent, etc., and in the HONTA system, the mass transfer coefficients were relatively small.

Oral presentation

Development of new extraction methods for minor actinide separation

Suzuki, Hideya*; Ban, Yasutoshi; Tsubata, Yasuhiro; Tsutsui, Nao; Toigawa, Tomohiro; Kurosawa, Tatsuya*; Shibata, Mitsunobu*; Kawasaki, Tomohiro*; Matsumura, Tatsuro

no journal, , 

The Japan Atomic Energy Agency (JAEA) has been studying partitioning technology. Recently, JAEA proposed a new liquid-liquid extraction technology called SELECT process to separate minor actinide (MA) from high-level liquid waste for transmutation. In this process, new extractants (HONTA, ADAAM) with highly practical and high extraction ability for MA was developed. A mixed solvent of HONTA and ADAAM was tested for mutual separation of MA and rare earth elements (RE). In this test, separation of MA and RE was achieved with very high yield. Furthermore, Americium (Am) and Curium (Cm) were separated efficiently with high separation factor values.

Oral presentation

Structural analysis on Eu-HONTA complex formed in adsorbent

Watanabe, So; Okada, Makoto*; Matsuura, Haruaki*; Kada, Wataru*; Koka, Masashi*; Yamagata, Ryohei*; Yamada, Naoto*; Sato, Takahiro*; Ishii, Yasuyuki*

no journal, , 

no abstracts in English

Oral presentation

Investigation of a new extraction method for americium separation from high-level liquid waste

Suzuki, Hideya*; Ban, Yasutoshi; Tsubata, Yasuhiro; Hotoku, Shinobu; Morita, Keisuke; Toigawa, Tomohiro; Tsutsui, Nao; Kurosawa, Tatsuya*; Shibata, Mitsunobu*; Kawasaki, Tomohiro*; et al.

no journal, , 

The Japan Atomic Energy Agency has been studying partitioning and transmutation (P&T) systems. In the P&T, the separation of minor actinide (MA) from the chemically similar lanthanides is the key step. After MAs are separated from high-level liquid waste (HLLW), 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 new reagents, called HONTA and ADAAM have been developed. Solvent extraction tests were performed using a mixture of HONTA and ADAAM. As a result, the separation of Am from the simulated HLLW was achieved with high yield.

Oral presentation

Development of MA separation system using the extraction chromatography method

Kida, Fukuka*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki

no journal, , 

Focusing on the extraction chromatography method using DGA-based and NTA-based extractants for MA recovery process that can be applied to MOX fuel reprocessing, we developed an adsorbent and investigated the separation conditions by column tests.

23 (Records 1-20 displayed on this page)