Akagi, Hiroshi*; Kumada, Takayuki; Otobe, Tomohito*; Itakura, Ryuji*; Hasegawa, Hirokazu*; Oshima, Yasuhiro*
Chemistry Letters, 49(4), p.416 - 418, 2020/04
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.
Morita, Yasuji; Tsubata, Yasuhiro
JAEA-Data/Code 2019-015, 45 Pages, 2020/01
Decay heat from radioactive elements in high-level liquid waste (HLLW) and separated solutions in partitioning process was evaluated as a basic data for safety assessment of partitioning process. In the evaluation of HLLW from spent UO fuel burned-up to 45 GWd/t in light water reactor, decay heat value from fission products decreased as the cooling period become longer but heat from actinides, Am and Cm, was almost constant until 50-year cooling. Decay heat density in solutions of Am, Cm and rare earth elements and of Am and Cm without concentration for volume reduction does not exceed the heat density of HLLW, but the concentration should be required to minimize the scale of the partitioning process. Separated solution of Am and Cm must be concentrated to convert the two elements to a solid state to make fuel for transmutation, and the decay heat density of the concentrated solution of Am and Cm is 10 times higher compared with the Pu solution of same element concentration. Higher burn-up UO fuel and MOX fuel in light water reactor and minor-actinide-recycled MOX fuel in fast reactor were also considered and the evaluated decay heat was compared among the spent fuels.
Baron, P.*; Cornet, S. M.*; Collins, E. D.*; DeAngelis, G.*; Del Cul, G.*; Fedorov, Y.*; Glatz, J. P.*; Ignatiev, V.*; Inoue, Tadashi*; Khaperskaya, A.*; et al.
Progress in Nuclear Energy, 117, p.103091_1 - 103091_24, 2019/11
The results of an international review of separation processes for spent nuclear fuel (SNF) recycling in future closed fuel cycles with the evaluation of Technology Readiness Level are reported. This study was made by the Expert Group on Fuel Recycling Chemistry (EGFRC) organised by the Nuclear Energy Agency (NEA) of the Organisation for Economic Co-operation and Development (OECD). A unique feature of this study was that processes were classified according to a hierarchy of separations aimed at different elements within spent fuel (uranium; uranium-plutonium co-recovery; minor actinides; high heat generating radionuclides) and also the Head-end processes, used to prepare the SNF for chemical separation, were included. Separation processes covered both wet (hydrometallurgical) and dry (pyro-chemical) processes.
Sonoda, Tetsu*; Katayama, Ichiro*; Wada, Michiharu*; Iimura, Hideki; Sonnenschein, V.*; Iimura, Shun*; Takamine, Aiko*; Rosenbusch, M.*; Kojima, Takao*; Ahn, D. S.*; et al.
Progress of Theoretical and Experimental Physics (Internet), 2019(11), p.113D02_1 - 113D02_12, 2019/11
An in-flight separator, BigRIPS, at RIBF in RIKEN provides each experiment with specific nuclides separated from many nuclides produced by projectile fragmentation or in-flight fission. In this process, nuclides other than separated ones are discarded on the slits in BigRIPS, although they include many nuclides interested from the view point of nuclear structure. In order to extract these nuclides for parasitic experiments, we are developing a method using laser ion-source (PALIS). A test experiment with Se beam from RIBF has been performed by using a gas cell set in BigRIPS. Unstable nuclides around Se were stopped in the gas cell in accordance with a calculation using LISE code. The stopping efficiency has been estimated to be about 30%. As a next step, we will establish the technique for extracting reaction products from the gas cell.
Inagaki, Yoshiyuki; Sakaba, Nariaki
Shokubai, 61(2), p.92 - 96, 2019/04
The outline of the membrane IS process to produce hydrogen by thermochemical water splitting using solar heat at around 650C is described. The membrane technology has been applied to the three main reaction of the IS process to lower the reaction temperature and reduce the amount of circulation materials in the process. The key component technologies such as catalysts, membranes and corrosion resistant materials have been developed. The study was supported in part by the Council for Science, Technology and Innovation, Cross-ministerial Strategic Innovation Promotion Program, "Energy Carrier".
Morita, Yasuji; Nishihara, Kenji; Tsubata, Yasuhiro
JAEA-Data/Code 2018-017, 32 Pages, 2019/02
Potential radiotoxicity defined as a summation of intake dose was estimated for each actinide element to suppose target of recovery ratio of minor actinide (MA). Importance of each element from the viewpoint of the radiotoxicity was evaluated from the evolution of the radiotoxicity and ratio to the total radiotoxicity. In all the 4 types of spent fuels examined, Am is the most important element. For instance, the potential radiotoxicity of Am accounts for 93% of the total radiotoxicity of actinide elements in HLW produced by reprocessing of spent fuel from pressurized water reactor (PWR). Residual Pu after the recovery of 99.5% in reprocessing still gives contribution that cannot be ignored in radiotoxicity. When the burn-up of the UO fuel in PWR increased, the potential radiotoxicity of actinide elements increased almost in proportion to the burn-up, but in case of MOX fuel in PWR and minor-actinide-recycled MOX fuel in fast reactor, the radiotoxicity of actinide elements increased further. Much consideration is required for the recovery of actinide elements in HLW from different types of fuel.
Kobayashi, Takanori*; Matsuoka, Leo*; Yokoyama, Keiichi
Computational and Theoretical Chemistry, 1150, p.40 - 48, 2019/02
One of important research targets in the development of cesium isotope separation system is design of recovery process of cesium atom. Relevant to this research target, the reaction cross section and reaction rate constant of a cesium exchange reaction through collision of the cesium iodide molecules with cesium atoms are calculated by a quasi-classical trajectory calculation based on a potential energy surface obtained by quantum chemistry calculations. Consequently, the rate constant is calculated to be 3.6 10 cmmolecules, as large as collision rate in the present condition. In addition, slightly positive temperature dependence is observed in the rate constant. This behavior is explained with the long-range attractive force and effect of subsequent dissociation process.
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.
Genshiryoku Bakkuendo Kenkyu (CD-ROM), 25(2), p.131 - 134, 2018/12
Impact of reduction of source term on design and safety assessment of disposal concept for high level radioactive waste is considered. Reduction of source term in partitioning and transmutation technology is shown with impact on disposal concept. Moreover, cost and technological readiness is outlined.
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.
Sasaki, Yuji; Morita, Keisuke
Progress in Nuclear Science and Technology (Internet), 5, p.27 - 32, 2018/12
no abstracts in English
Kimura, Taiki*; Kaneko, Masashi; Watanabe, Masayuki; Miyashita, Sunao*; Nakashima, Satoru*
Dalton Transactions (Internet), 47(42), p.14924 - 14931, 2018/11
We demonstrated density functional calculations of Eu(III) and Am(III) complexes with pnictogen-donor (X) ligands, CH)X-CH-CH-X(CH) (X = N, P, As and Sb). We investigated the optimized structures of the cmoplexes and the Gibbs energy differences in the complex formation reactions. Those results indicated that the N- and P-donor ligands have Am(III) ion selectivity over Eu(III) ion, especially, the P-donor ligand showed the highest selectivity. The tendency of the Am(III)/Eu(III) selectivity by the pnictogen-dono ligands was found to be comparable to that of soft acid classification in hard and soft acids and bases rule. Mulliken's spin population analysis indicated that the bonding property between the metal ion and the pnictogen atoms correlated with the Am(III)/Eu(III) selectivity. In particular, the participation of f-orbital electrons of the metal ion in the covalency was indicated to have an important role for the selectivity.
Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Beerwerth, R.*; Kaneya, Yusuke*; Makii, Hiroyuki; Mitsukai, Akina*; Nagame, Yuichiro; Osa, Akihiko; Toyoshima, Atsushi; et al.
Journal of the American Chemical Society, 140(44), p.14609 - 14613, 2018/11
The first ionization potential (IP) yields information on valence electronic structure of an atom. IP values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.
Okubo, Nariaki; Okuno, Yasuki; Kitamura, Akane; Taguchi, Tomitsugu*
Nuclear Instruments and Methods in Physics Research B, 435, p.198 - 202, 2018/11
Accelerator driven system (ADS) adopts the lead-bismuth eutectic (LBE) as both coolant and spallation target. The oxygen concentration control is one of the most important technical developments. Estimation of durability under gamma-ray irradiation for the oxygen sensor is necessary for the integrity evaluation of ADS components. The Zirconia added by Yttria (YSZ) is the main element in oxygen sensor. Effect of gamma-ray irradiation on the mechanical property and structural change for three types of YSZ with 3, 6, 8 mol% Yttria was evaluated by using 4 points bend test, XRD, SEM and Raman spectroscope. The gamma-ray irradiations were conducted at 1 and 2 kGy/h, which corresponded to the LBE activity after 1 year ADS operation. In the cases of 8Y and 6Y, degradation of strength was not measured and the fracture surface did not change the morphology. In the case of 3Y, however, the strength did not change but phase transformation from tetragonal to monoclinic crystal structure was observed in XRD results, depending on the irradiation dose. This implies that the gamma-ray irradiation causes the phase transformation in 3Y-YSZ.
Yamamoto, Masahiko; Taguchi, Shigeo; Horigome, Kazushi; Kuno, Takehiko
Proceeding IAEA Symposium on International Safeguards; Building Future Safeguards Capabilities (Internet), 8 Pages, 2018/11
In this study, the single-column extraction chromatographic separation has been developed for analysis of U and Pu in highly active liquid waste by isotope dilution mass spectrometry (IDMS). The commercially available TEVA resin is selected as an extraction chromatography resin. The U is chromatographically separated from fission products (FP) elements by nitric acid while Pu(IV) is adsorbed on the resin. After that, Pu is eluted by reducing to Pu(III). The method has been successfully achieved the separation with yielding the enough recovery and sufficient decontamination factors for subsequent IDMS analysis. The column dose rate after the FP removal is decreased to the background. The analytical results obtained by the developed method are in a good agreement with those of the conventional method. It provides simple and rapid separation and expected that the method can be applied to join IAEA/Japan on-site analytical laboratory.
Sekiguchi, Tetsuhiro; Yokoyama, Keiichi; Uozumi, Yuki*; Yano, Masahiro; Asaoka, Hidehito; Suzuki, Shinichi; Yaita, Tsuyoshi
Progress in Nuclear Science and Technology (Internet), 5, p.161 - 164, 2018/11
For nuclear transmutation of cesium-135 (Cs), which is long-lived fission product, we are developing selective absorbent which takes only Cs atom in, but does not CsI. In this study, absorbing property of Cs atom onto the surface of fullerene (C) film has been investigated using synchrotron-based angle-dependent X-ray photoelectron spectroscopy (XPS). The results were compared with those of CsI. It was found that Cs penetrates into C deep bulk. In contrast, CsI deposits on shallow surface. Furthermore, XPS spectra were measured as a function of Ar-sputtering time in order to know Cs concentration profiles in deep region. Results showed that Cs penetrates into deep region of several hundreds .
Miyamoto, Yutaka; Yasuda, Kenichiro
Journal of Nuclear and Radiochemical Sciences (Internet), 18, p.13 - 15, 2018/07
A sequential separation technique using an anion-exchange column developed in the previous works have the potential to completely separate picograms of Am from the lanthanides using mixtures of acetic acid, hydrochloric acid, and nitric acid as the eluents, without any functional ligands or special columns. This experimental result implies that ultra-trace actinides, including Am, Pu, U, and Th in environmental samples can be sequentially separated by combination of these mixed-media eluents and an anion exchange column.
Taguchi, Shigeo; Yamamoto, Masahiko; Furuse, Takahiro*; Masaki, Yuji*; Kuno, Takehiko
JAEA-Technology 2018-005, 14 Pages, 2018/06
The method to remove Pu, Am and Np from plutonium nitrate solution recovered from spent nuclear fuel prior to ICP-OES measurement has been developed for the determination of 18 impurity metal elements (Fe, Cr, Ni, Mn, Al, Cd, V, Cu, Si, Zn, Mo, Sn, Ca, Mg, Na, Ag, Pb, B). In this method, two TRU resin packed columns were used for separation. In the first column, Pu and Am were mainly removed by adsorption. The recovered solution from the fist column was added to the second column after reduction of Np, and Am(III) and Np(IV) were removed by adsorption. The Pu nitrate solution (22g/L) of 2mL were treated by proposed method. The alpha emission nuclide was decreased to 5.8 Bq/mL in a solution diluted to 100mL. As a result of ICP-OES measurement, the recoveries of impurity metals separated by proposed method were almost 100%. This separation scheme can apply to the metal impurity elemental analysis in Pu nitrate solution recovered from spent nuclear fuel.
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.