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 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 / 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 / HONTA - n-dodecane system are under 10 m/s.

Characteristics of TPDN/SiO-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

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

JAEA-Research-2016-024.pdf:6.73MB

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.

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

JAEA-Research-2015-021.pdf:2.3MB

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.

Measurement of neutron cross sections for yttrium and terbium at 287 MeV

Sekimoto, Shun*; Utsunomiya, Takashi*; Yashima, Hiroshi*; Ninomiya, Kazuhiko*; Omoto, Takashi*; Nakagaki, Reiko*; Shima, Tatsushi*; Takahashi, Naruto*; Shinohara, Atsushi*; Kinoshita, Norikazu*; et al.

Progress in Nuclear Science and Technology (Internet), 1, p.89 - 93, 2011/02

https://doi.org/10.15669/pnst.1.89

In this work, we tried to determine reaction cross sections for Y and Tb induced by neutrons at 300 MeV, which have never been reported. The irradiations were carried out using neutrons produced through Li(p, n) reaction at N0 beam line in the Research Center for Nuclear Physics (RCNP), Osaka University. To estimate quasi-monoenergetic neutron induced cross sections, the target stacks of Y and Tb were irradiated on the two angles of 0 degree and 30 degree for the axis of the primary proton beam. Neutron cross sections were estimated by subtracting the activities produced in the samples placed on 30 degree from those of 0 degree to correct the contribution of the low energy tail in the neutron spectrum.

Selective separation of Am(III) from Ln(III) with a novel synergistic extraction system, N,N,N',N'-tetrakis(2-methylpyridyl)ethylenediamine (TPEN) and carboxylic acid in 1-octanol

Mirvaliev, R.*; Watanabe, Masayuki; Matsumura, Tatsuro; Tachimori, Shoichi*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 41(11), p.1122 - 1124, 2004/11

https://doi.org/10.3327/jnst.41.1122

Transmutation is a technology aimed to reduce HLW from reprocessing process. Minor actinides in the HLW will be converted to short-lived nuclides. However, lanthanides in HLW adversely affects on the efficiency of the transmutation. It is well known that separating An(III) and Ln(III) is very difficult because of their similarity of chemical properties. Therefore, the separation is one of the essential subjects to establish the transmutation technology. Considerable efforts have been devoted to the development of new extractants for the separation. N,N,N',N'-tetrakis(2-methylpyridyl)ethylenediamine (TPEN) demonstrates 100-fold preference for Am(III) over Ln(III) between stability constants with the ions in the aqueous phase. We have reported that Am(III) was selectively extracted from the aqueous phase containing Ln(III) by TPEN in nitrobenzene system and synergistic system with TPEN and D2EHPA in octanol. This work presents our recent results that Am(III) is separated from Eu(III) by a synergistic extraction system with TPEN and decanoic acid diluted with 1-octanol.

Evidence for a narrow = +1 Baryon resonance in photoproduction from the neutron

Nakano, Takashi*; Ahn, D. S.*; Ahn, J. K.*; Akimune, Hidetoshi*; Asano, Yoshihiro; Chang, W. C.*; Date, S.*; Ejiri, Hiroyasu*; Fujimura, Hisako*; Fujiwara, Mamoru; et al.

Physical Review Letters, 91(1), p.012002_1 - 012002_4, 2003/07

https://doi.org/10.1103/PhysRevLett.91.012002

no abstracts in English

Shielding experiments at high energy accelerators of FERMI, 6; Measurement of reaction products

Matsumura, Hiroshi*; Kasugai, Yoshimi; Yashima, Hiroshi*; Iwase, Hiroshi*; Matsuda, Norihiro; Kinoshita, Norikazu*; Sanami, Toshiya*; Hagiwara, Masayuki*; Shigyo, Nobuhiro*; Arakawa, Hiroyuki*; et al.

no journal, , 

A gold activation detector was studied as a high energy neutron detector at high radiation field in a series of shielding experiment at Fermi National Accelerator Laboratory. We could measure spallation residual nuclei with wide threshold energy by using a combination method with radiological chemical separation and X-X- coincidence detection methods. It was shown the detector was effective for high energy neutron detector.

Evaluation of the flowsheet with TDdDGA by counter-current trials using mixer-settlers and centrifugal contactors

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

no journal, , 

The flowsheet with TDdDGA extractant for recovering MA(III) from PUREX raffinate was evaluated by counter-current trials with surrogate PUREX raffinate using mixer-settlers and centrifugal contactors. The extraction and back-extraction of Ln(III) which show the similar tendencies as MA(III) could be achieved successfully, especially their back-extraction proceeded more efficiently in centrifugal contactors, which might be due to superior phase separation performance of centrifugal contactors.

Computational study on the separation mechanism of Am from Eu by DGA and NTA extraction reagents

Kaneko, Masashi; Watanabe, Masayuki; Matsumura, Tatsuro

no journal, , 

In Japan Atomic Energy Agency, the extraction reagents for the inter- and intragroup separation of mainor-actinides from lanthanides have been developed in order to construct the partitioning and transmutation process. We aim to reveal the separation mechanism using various extraction materials at a molecular level and to design the novel extraction reagents. In this study, we apply density functional calculations to the separation behavior of Am(III) from Eu(III) by DGA and NTA ligands. All metal compounds were modeled by referring the literatures. As the result, DGA ligand selectively coordinates to Eu(III) than Am(III), on the other hand, NTA ligand preferably coordinates to Am(III) than Eu(III), being consistent with the experimental selectivity.