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Journal Articles

Density functional study on Am(III)/Eu(III) selectivity using crown ether type ligands

Fukasawa, Yuto*; Kaneko, Masashi; Nakashima, Satoru*

Journal of Radioanalytical and Nuclear Chemistry, 329(1), p.77 - 84, 2021/07

 Times Cited Count:0

Density functional theory calculations were applied to understand the selectivity between Am$$^{3+}$$ and Eu$$^{3+}$$ ions with the crown ethers type ligands. 18C6 is predicted to form the most stable complex with Eu$$^{3+}$$ and show the higher stability for Am$$^{3+}$$ over Eu$$^{3+}$$, being consistent with previously reported Am$$^{3+}$$/Eu$$^{3+}$$ selectivity. We modeled N- and S-donor complexes by using framework of 18C6 complex and analyzed the complexation Gibbs energies, indicating that 18C6 with N-donor atoms is suitable for both complexation and higher Am$$^{3+}$$ stability over Eu$$^{3+}$$ due to the stronger covalent interaction.

Journal Articles

Preventing nuclear fuel material adhesion on glove box components using nanoparticle coating

Segawa, Tomomi; Kawaguchi, Koichi; Ishii, Katsunori; Suzuki, Masahiro; Tachihara, Joji; Takato, Kiyoto; Okita, Takatoshi; Satone, Hiroshi*; Suzuki, Michitaka*

Mechanical Engineering Journal (Internet), 8(3), p.21-00022_1 - 21-00022_9, 2021/06

To reduce the hold-up of the nuclear fuel materials in the glove box and the external exposure dose, the technology of the MOX powder adhesion prevention by the nanoparticle coating to the acrylic panels of the glove box has been developed. The surface analysis by means of atomic force microscopy (AFM) showed that the acrylic test piece surface coated with nanoparticles had a higher root mean square roughness value than that non-coated with nanoparticles. Due to the formation of nano-sized tiny rugged surface, the nanoparticle coating reduced the minimum adhesion force between the UO$$_{2}$$ particles and the acrylic test piece surface with the smallest particle size of about 5 $$mu$$m where desorption was observed, by about one-tenth. Moreover, the nanoparticle coating reduced the amount of the MOX powder adhering to the acrylic test piece to about one-tenth. In this study, it was found that applying the nanoparticle coating to the acrylic panels of glove box can prevent the adhesion of nuclear fuel materials. This method is effective for reducing the hold-up of the nuclear fuel materials in the glove box, the external exposure dose and improving the visibility of the acrylic panels.

Journal Articles

250 kW LBE spallation target for ADS development in J-PARC

Sasa, Toshinobu; Saito, Shigeru; Obayashi, Hironari; Ariyoshi, Gen

JPS Conference Proceedings (Internet), 33, p.011051_1 - 011051_6, 2021/03

To realize Accelerator-driven system (ADS) for minor actinide transmutation, JAEA proposes to construct the Proton Irradiation Facility in J-PARC. The facility is planned to solve technical issues for safe application of Lead-bismuth Eutectic Alloy (LBE). The 250 kW LBE spallation target will be located in the facility to prepare material irradiation database by both proton and neutron irradiation in the temperature range for typical LBE-cooled ADS. Various studies for important technologies required to build the facilities are investigated such as oxygen concentration control, instruments development, remote handling techniques for target maintenance, and spallation target design. The large scale LBE loops for mock up the 250 kW LBE spallation target and material corrosion studies are also manufactured and applied to various experiments. The latest status of 250 kW LBE spallation target design works will be summarized.

Journal Articles

Chiral separation effect catalyzed by heavy impurities

Suenaga, Daiki*; Araki, Yasufumi; Suzuki, Kei; Yasui, Shigehiro*

Physical Review D, 103(5), p.054041_1 - 054041_17, 2021/03

 Times Cited Count:1 Percentile:0.01(Astronomy & Astrophysics)

We investigate the influence of the Kondo effect, namely, the nonperturbative effect induced by heavy impurities, on the chiral separation effect (CSE) in quark matter. We employ a simple effective model incorporating the Kondo condensate made of a light quark and a heavy quark, and compute the response function of the axial current to the magnetic field in the static and dynamical limits. As a result, we find that the Kondo effect catalyzes the CSE in both of the limits, and in particular the CSE in the dynamical limit can be enhanced by a factor of approximately 3. Our findings clearly show that the presence of heavy impurities in quark matter can play an important role in the transport phenomena of light quarks induced by a magnetic field.

Journal Articles

Effect of oxygen-donor charge on adjacent nitrogen-donor interactions in Eu$$^{3+}$$ complexes of mixed N,O-donor ligands demonstrated on a 10-fold [Eu(TPAMEN)]$$^{3+}$$ chelate complex

Schnaars, K.; Kaneko, Masashi; Fujisawa, Kiyoshi*

Inorganic Chemistry, 60(4), p.2477 - 2491, 2021/02

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

To reduce high-level radiotoxic waste generated by nuclear power plants, highly selective separation agents for minor actinides are mandatory. The mixed N,O-donor ligand ${it N,N,N',N'}$-tetrakis[(6-carboxypyridin-2-yl)methyl]ethylenediamine (H$$_{4}$$TPAEN) has shown good performance as a masking agent in Am$$^{3+}$$/Eu$$^{3+}$$ separation studies. In this work, we examine whether a decrease in O-donor basicity can promote the M$$^{3+}$$-N$$_{am}$$ interactions. Therefore, we replace the deprotonated "charged" carboxylic acid groups of TPAEN$$^{4-}$$ by neutral amide groups and introduce ${it N,N,N',N'}$-tetrakis[(6-${it N",N"}$-diethylcarbamoylpyridin-2-yl)methyl]ethylenediamine (TPAMEN) as a new ligand. TPAMEN was crystallized with Eu(OTf)$$_{3}$$ and Eu(NO$$_{3}$$)$$_{3}$$ 6H$$_{2}$$O to form positively charged 1:1 [Eu(TPAMEN)]$$^{3+}$$ complexes in the solid state. Alterations in the M-O/N bond distances are compared to [Eu(TPAEN)]$$^{-}$$ and investigated by DFT calculations to expose the differences in charge/energy density distributions at europium(III) and the donor functionalities of the TPAEN$$^{4-}$$ and TPAMEN. On the basis of estimations of the bond orders, atomic charges spin populations, and density of states in the Eu and potential Am and Cm complexes, the specific contributions of the donor-metal interaction are analyzed. The prediction of complex formation energy differences for the [M(TPAEN)]$$^{-}$$ and [M(TPAMEN)]$$^{3+}$$ (M$$^{3+}$$ = Eu$$^{3+}$$, Am$$^{3+}$$) complexes provide an outlook on the potential performance of TPAMEN in Am$$^{3+}$$/Eu$$^{3+}$$ separation.

Journal Articles

Optimization of light water reactor high level waste disposal scenario in the situation of delayed reprocessing with existing and demonstrated technology

Fukaya, Yuji

Annals of Nuclear Energy, 144, p.107503_1 - 107503_7, 2020/09

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

Disposal scenario of High Level Waste (HLW) of Light Water Reactor (LWR) have been optimized to reduce waste volume and repository footprint in geological disposal. The optimization was performed with existing and demonstrated technology in the situation where the reprocessing will be delayed. In general, the scenario with Partitioning and Transmutation (P&T) is optimized to minimize waste package number generated in the situation where the spent fuel will be reprocessed immediately with the minimum cooling time. With considering the delay of reprocessing, it is found that the more simplified and effective optimization with the high-waste-loading glass and cold crucible induction melter technologies and without partitioning. The optimized case can achieve significant reduction of number of waste package generation and the repository footprint to half of those of non-P&T case with 100 years cooling.

Journal Articles

Research on activation assessment of a reactor structural materials for decommissioning, 2

Seki, Misaki; Ishikawa, Koji*; Sano, Tadafumi*; Nagata, Hiroshi; Otsuka, Kaoru; Omori, Takazumi; Hanakawa, Hiroki; Ide, Hiroshi; Tsuchiya, Kunihiko; Fujihara, Yasuyuki*; et al.

KURNS Progress Report 2019, P. 279, 2020/08

no abstracts in English

Journal Articles

First online operation of TRIGA-TRAP

Grund, J.*; Asai, Masato; Blaum, K.*; Block, M.*; Chenmarev, S.*; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Lohse, S.*; Nagame, Yuichiro*; Nagy, Sz.*; et al.

Nuclear Instruments and Methods in Physics Research A, 972, p.164013_1 - 164013_8, 2020/08

 Times Cited Count:2 Percentile:66.08(Instruments & Instrumentation)

We report on the successful coupling of the Penning-trap mass spectrometry setup TRIGA-TRAP to the research reactor TRIGA Mainz. This offers the possibility to perform direct high-precision mass measurements of short-lived nuclei produced in neutron-induced fission of a $$^{235}$$U target located near the reactor core. An aerosol-based gas-jet system is used for efficient transport of short-lived neutron-rich nuclei from the target chamber to a surface ion source. In conjunction with new ion optics and extended beam monitoring capabilities, the experimental setup has been fully commissioned. The design of the surface ion source, efficiency studies and first results are presented.

Journal Articles

Bromine-isotope selective ionization using field-free alignment of IBr isotopologues with a switched nanosecond laser pulse

Akagi, Hiroshi*; Kumada, Takayuki; Otobe, Tomohito*; Itakura, Ryuji*; Hasegawa, Hirokazu*; Oshima, Yasuhiro*

Chemistry Letters, 49(4), p.416 - 418, 2020/04

 Times Cited Count:0 Percentile:0(Chemistry, Multidisciplinary)

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:3 Percentile:45.02(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

Study of quasielastic barrier distributions as a step towards the synthesis of superheavy elements with hot fusion reactions

Tanaka, Taiki*; Morita, Kosuke*; Morimoto, Koji*; Kaji, Daiya*; Haba, Hiromitsu*; Boll, R. A.*; Brewer, N. T.*; Van Cleve, S.*; Dean, D. J.*; Ishizawa, Satoshi*; et al.

Physical Review Letters, 124(5), p.052502_1 - 052502_6, 2020/02

 Times Cited Count:4 Percentile:74.08(Physics, Multidisciplinary)

JAEA Reports

Evaluation of decay heat value from high-level liquid waste; Data for safety assessment of partitioning process

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$$_{2}$$ 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$$_{2}$$ 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.

Journal Articles

Development of select process for minor actinides partitioning from high level waste

Matsumura, Tatsuro

Kino Zairyo, 40(1), p.60 - 71, 2020/01

no abstracts in English

Journal Articles

A Review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments

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

 Times Cited Count:17 Percentile:89.16(Nuclear Science & Technology)

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.

Journal Articles

Conceptual study on parasitic low-energy RI beam production with in-flight separator BigRIPS and the first stopping examination for high-energy RI beams in the parasitic gas cell

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


 Times Cited Count:0 Percentile:0.01(Physics, Multidisciplinary)

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 $$^{78}$$Se beam from RIBF has been performed by using a gas cell set in BigRIPS. Unstable nuclides around $$^{67}$$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.

Journal Articles

Contribution of membrane technology to hydrogen society; Development of membrane IS process

Inagaki, Yoshiyuki; Sakaba, Nariaki; Tanaka, Nobuyuki; Nomura, Mikihiro*; Sawada, Shinichi*; Yamaki, Tetsuya*

Nihon Kaisui Gakkai-Shi, 73(4), p.194 - 202, 2019/08

The thermochemical IS process is a promising hydrogen production method which can produce hydrogen in a large amount and stably with high efficiency by thermal splitting of water. Research and development on chemical reaction technology with membranes was conducted for the purpose of improving the efficiency of IS process and application of solar heat. The basic technology of ceramic membranes applied to decomposition reactions of hydrogen iodine and sulfuric acid was developed, and it is expected that the conversion rate on decomposition in each reaction can be remarkably improved. The basic technology of a cation exchange membrane applied to Bunsen reaction was developed with radiation-induced grafting technique, it is expected that the amount of iodine can be reduced to about one-fifth compared to the conventional method. These achievements are important technologies for practical use of the IS process.

Journal Articles

Development of hydrogen production technology by thermal water splitting with solar heat

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 650$$^{circ}$$C 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".

JAEA Reports

Comparison of potential radiotoxicity of actinide elements; Data for consideration of optimum recovery of actinide elements

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$$_{2}$$ 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.

Journal Articles

A Quasiclassical trajectory calculation to compute the reaction cross section and thermal rate constant for the cesium exchange reaction $$^{133}$$CsI + $$^{135}$$Cs $$rightarrow$$ $$^{133}$$Cs + I$$^{135}$$Cs

Kobayashi, Takanori*; Matsuoka, Leo*; Yokoyama, Keiichi

Computational and Theoretical Chemistry, 1150, p.40 - 48, 2019/02

 Times Cited Count:0 Percentile:0(Chemistry, Physical)

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 $$times$$ 10$$^{-10}$$ cm$$^{3}$$molecule$$^{-1}$$s$$^{-1}$$, 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.

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:12 Percentile:68.99(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.

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