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
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.
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
The candidate An(III)/Ln(III) separation ligand hexa--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 (-dodecane) radical cation of (HONTA + R) = (7.61 0.82) 10 M s obtained by pulse radiolysis techniques. However, when this ligand is bound to either americium or europium ions, the observed -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 (s) HONTA triplet excited state. These HONTA species are important precursors to the suite of HONTA degradation products observed.
Toigawa, Tomohiro; Tsubata, Yasuhiro; Kai, Takeshi; Furuta, Takuya; Kumagai, Yuta; Matsumura, Tatsuro
Solvent Extraction and Ion Exchange, 39(1), p.74 - 89, 2021/00
Absorbed-dose estimation is essential for evaluation of the radiation feasibility of minor-actinide-separation processes. We propose a dose-evaluation method based on radiation permeability, with comparisons of heterogeneous structures seen in the solvent-extraction process, such as emulsions forming in the mixture of the organic and aqueous phases. A demonstration of radiation-energy-transfer simulation is performed with a focus on the minor-actinide-recovery process from high-level liquid waste with the aid of the Monte Carlo radiation-transport code PHITS. The simulation results indicate that the dose absorbed by the extraction solvent from alpha ray depends upon the emulsion structure, and that from beta and gamma ray depends upon the mixer-settler-apparatus size. Non-negligible contributions of well-permeable gamma rays were indicated in terms of the plant operation of the minor-actinide-separation process.
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.
Nakamura, Satoshi; Kimura, Takahiro; Ban, Yasutoshi; Tsubata, Yasuhiro; Matsumura, Tatsuro
JAEA-Technology 2020-009, 22 Pages, 2020/08
Partitioning and transmutation technology division is planning to measure fission rate ratios that contribute to validate nuclear data of minor actinides (MA). For this purpose, MA sources for fission chambers were prepared using electrodeposition method. The radioactivity of each MA source was quantified, and its uncertainty was evaluated. Seven types of MA sources with different radioactivity were prepared using four nuclides of Np, Am, Am, and Cm. A Cm source solution of which radioactivity was quantified by isotope dilution method was used to prepare working standard sources of Cm. The radioactivities were quantified as 1461 Bq, 2179 Bq, and 2938 Bq for Np sources, 1.428 MBq for Am source, 370.5 kBq and 89.57 kBq for Am sources, and 2.327 MBq for Cm source with, the uncertainty of 0.35% (1). This report summarizes the method for preparation and quantification of MA sources, and uncertainty evaluation.
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
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 -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 -dodecane system. These differences were attributed to the characteristics of the diluents. This study reveals high distribution ratios of Am ( ) and Cm ( ) for TDdPTDA, with the high separation factors (s) of Am from Lns enough for their separation.
Kino Zairyo, 40(1), p.60 - 71, 2020/01
no abstracts in English
Tsukahara, Takehiko*; Saga, Kaname*; Suzuki, Hideya*; Matsumura, Tatsuro
Kurin Tekunoroji, 29(12), p.4 - 7, 2019/12
no abstracts in English
Ban, Yasutoshi; Suzuki, Hideya*; Hotoku, Shinobu; Tsutsui, Nao; Tsubata, Yasuhiro; Matsumura, Tatsuro
Solvent Extraction and Ion Exchange, 37(7), p.489 - 499, 2019/11
A continuous counter-current experiment to separate minor actinides (MAs: Am and Cm) was performed with -hexaochyl nitrilotriacetamide (HONTA) as an extractant. Nitric acid of 0.08 M (mol/dm) 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 99% by optimizing separation conditions.
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 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, -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 Sb Sn Lns Fe. The extracted species was determined as Zr(HAA)(NO)(HNO). 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.
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
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 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.
Kaneko, Masashi; Suzuki, Hideya; Matsumura, Tatsuro
Inorganic Chemistry, 57(23), p.14513 - 14523, 2018/12
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)] and [M(ADAAM)(NO)(HO)]. 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)] and [M(ADAAM)(NO)(HO)], 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.
Fukaya, Yuji; Goto, Minoru; Ohashi, Hirofumi; Yan, X.; Nishihara, Tetsuo; Tsubata, Yasuhiro; Matsumura, Tatsuro
Journal of Nuclear Science and Technology, 55(11), p.1275 - 1290, 2018/11
To reduce environmental burden and thread of nuclear proliferation, multi-recycling fuel cycle with High Temperature Gas-cooled Reactor (HTGR) has been investigated. Those problems are solved by incinerating TRans Uranium (TRU) nuclides, which is composed of plutonium and Minor Actinoide (MA), and there is concept to realize TRU incineration by multi-recycling with Fast Breeder Reactor (FBR). In this study, multi-recycling is realized even with thermal reactor by feeding fissile uranium from outside of the fuel cycle instead of breeding fissile nuclide. In this fuel cycle, recovered uranium by reprocessing and natural uranium are enriched and mixed with recovered TRU by reprocessing and partitioning to fabricate fresh fuels. The fuel cycle was designed for a Gas Turbine High Temperature Reactor (GTHTR300), whose thermal power is 600 MW, including conceptual design of uranium enrichment facility. Reprocessing is assumed as existing Plutonium Uranium Redox EXtraction (PUREX) with four-group partitioning technology. As a result, it was found that the TRU nuclides excluding neptunium can be recycled by the proposed cycle. The duration of potential toxicity decaying to natural uranium level can be reduced to approximately 300 years, and the footprint of repository for High Level Waste (HLW) can be reduced by 99.7% compared with GTHTR300 using existing reprocessing and disposal technology. Suppress plutonium is not generated from this cycle. Moreover, incineration of TRU from Light Water Reactor (LWR) cycle can be performed in this cycle.
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
Watanabe, So; Suzuki, Hideya; Goto, Ichiro*; Kofuji, Hirohide; Matsumura, Tatsuro
Nihon Ion Kokan Gakkai-Shi, 29(3), p.71 - 75, 2018/09
Fukaya, Yuji; Goto, Minoru; Ohashi, Hirofumi; Nishihara, Tetsuo; Tsubata, Yasuhiro; Matsumura, Tatsuro
Annals of Nuclear Energy, 116, p.224 - 234, 2018/06
Optimization of disposal method and scenario to reduce volume of High Level Waste (HLW) and the footprint in a geological repository for High Temperature Gas-cooled Reactor (HTGR) has been performed. It was found that HTGR has great advantages to reducing HLW volume and its footprint, which are high burn-up, high thermal efficiency and pin-in-block type fuel, compared with those of LWR and has potential to reduce those more in the previous study. In this study, the scenario is optimized, and the geological repository layout is designed with the horizontal emplacement based on the KBS-3H concept instead of the vertical emplacement based on KBS-3V concept employed in the previous study. As a result, for direct disposal, the repository footprint can be reduced by 20 % by employing the horizontal without change of the scenario. By extending 40 years for cooling time before disposal, the footprint can be reduced by 50 %. For disposal with reprocessing, the number of canister generation can be reduced by 20 % by extending cooling time of 1.5 years between the discharge and reprocessing. The footprint per electricity generation can be reduced by 80 % by extending 40 years before disposal. Moreover, by employing four-group partitioning technology without transmutation, the footprint can be reduced by 90 % with cooling time of 150 years.
Nakamura, Shoji; Kimura, Atsushi; Hales, B. P.; Iwamoto, Osamu; Tsubata, Yasuhiro; Matsumura, Tatsuro; Shibahara, Yuji*; Uehara, Akihiro*; Fujii, Toshiyuki*
JAEA-Conf 2017-001, p.15 - 22, 2018/01
Neutron nuclear data of long lived fission products (LLFPs) have been required as basic data for the technology of reduce environmental impact involved in high level radioactive wastes (HLW). The innovative large project called by "Impusing Paradigm Change through Disruptive Technologies Program: ImPACT" have been started from October, 2014. In the ImPACT project, some research groups of JAEA engaged in the Project No.2 (Nuclear Reaction Data Measurements), and have started measurements of neutron capture cross-section at J-PARC/MLF/ANNRI. In our research, we selected cesium-135 (Cs) nuclide (half life: 2.310 yr.) among LLFPs in the HLW, and decided to measure the neutron capture cross-sections of Cs. When measurement, the Cs sample might contained cecium-137 (Cs) as impurities because it's impossible to chemically separate each other. To measure the cross-sections of Cs, there should be also needed to know the cross-sections of Cs. In this work, sample maintenance also has been examined especially for selen-79 (Se) nuclide among LLFPs having difficulty in sample preparations. In this oral session, the outline of our research project will be presented together with a research motivation, situations of past reported data, total schedules, progress, future plans, and some of high light data for neutron capture cross-section measurements.
Suzuki, Hideya; Tsubata, Yasuhiro; Kurosawa, Tatsuya*; Sagawa, Hiroshi*; Matsumura, Tatsuro
Journal of Nuclear Science and Technology, 54(11), p.1163 - 1167, 2017/11
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.
Tsutsui, Nao; Ban, Yasutoshi; Sagawa, Hiroshi; Ishii, Sho; Matsumura, Tatsuro
Solvent Extraction and Ion Exchange, 35(6), p.439 - 449, 2017/08
Solvent extraction of uranium from a nitric acid medium was performed with ,-di(2-ethylhexyl)octanamide (DEHOA) by a single-stage batch method, and the distribution ratio equation of U(VI) was derived as = 1.1. Furthermore, the nitric acid distribution was also evaluated, and the distribution ratio equation = 0.12 was obtained. Batch experiments to evaluate the time dependence of U(VI) extraction and the U(VI) loading capacity of DEHOA were also performed. It was revealed that U(VI) extraction by DEHOA reached an equilibrium state within a few minutes, and the loading capacity was 0.71 mol/dm (M) when the concentrations of DEHOA and nitric acid were 1.5 and 3.0 M, respectively.
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.