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Journal Articles

A Large-scale particle-based simulation of heat and mass transfer behavior in EAGLE ID1 in-pile test

Zhang, T.*; Yao, Y.*; Morita, Koji*; Liu, X.*; Liu, W.*; Imaizumi, Yuya; Kamiyama, Kenji

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 9 Pages, 2023/05

Journal Articles

Long-term density-dependent groundwater flow analysis and its effect on nuclide migration for safety assessment of high-level radioactive waste disposal with consideration of interaction between fractures and matrix of rock formation in coastal crystalline groundwater systems

Park, Y.-J.*; Sawada, Atsushi; Ozutsumi, Takenori*; Tanaka, Tatsuya*; Hashimoto, Shuji*; Morita, Yutaka*

Proceedings of 3rd International Conference on Discrete Fracture Network Engineering (DFNE 2022) (Internet), 8 Pages, 2022/00

Safety analysis for underground disposal facilities for high-level radioactive waste requires thorough understanding of long-term groundwater flow and nuclide migration processes in geologic media. In the coastal subsurface systems, groundwater flow is defined by the complex interactions between freshwater of meteoric origin and denser saline water from the sea. In addition, sea levels are expected to fluctuate significantly due to a transgression and regression of the sea over the millions of years for safety analysis. This study presents long-term evolution of groundwater environment such as salinity concentration and flow velocity with focus of the interaction between fractures and matrix blocks in regional and near-field scale analysis framework for groundwater flow and nuclide migration for underground disposal facilities in hypothetical fractured crystalline coastal systems.

Journal Articles

Production of $$^{266}$$Bh in the $$^{248}$$Cm($$^{23}$$Na,5$$n$$)$$^{266}$$Bh reaction and its decay properties

Haba, Hiromitsu*; Fan, F.*; Kaji, Daiya*; Kasamatsu, Yoshitaka*; Kikunaga, Hidetoshi*; Komori, Yukiko*; Kondo, Narumi*; Kudo, Hisaaki*; Morimoto, Koji*; Morita, Kosuke*; et al.

Physical Review C, 102(2), p.024625_1 - 024625_12, 2020/08

 Times Cited Count:7 Percentile:52.49(Physics, Nuclear)

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:115 Percentile:94.22(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

First direct mass measurements of nuclides around $$Z$$ = 100 with a multireflection time-of-flight mass spectrograph

Ito, Yuta*; Schury, P.*; Wada, Michiharu*; Arai, Fumiya*; Haba, Hiromitsu*; Hirayama, Yoshikazu*; Ishizawa, Satoshi*; Kaji, Daiya*; Kimura, Sota*; Koura, Hiroyuki; et al.

Physical Review Letters, 120(15), p.152501_1 - 152501_6, 2018/04

 Times Cited Count:66 Percentile:92.14(Physics, Multidisciplinary)

Masses of $$^{246}$$Es, $$^{251}$$Fm and the transfermium nuclei $$^{249-252}$$Md, and $$^{254}$$No, produced by hot- and cold-fusion reactions, in the vicinity of the deformed $$N=152$$ neutron shell closure, have been directly measured using a multi-reflection time-of-flight mass spectrograph. The masses of $$^{246}$$Es and $$^{249,250,252}$$Md were measured for the first time. Using the masses of $$^{249,250}$$Md as anchor points for $$alpha$$ decay chains, the masses of heavier nuclei, up to $$^{261}$$Bh and $$^{266}$$Mt, were determined. These new masses were compared with theoretical global mass models and demonstrated to be in good agreement with macroscopic-microscopic models in this region. The empirical shell gap parameter $$delta_{2n}$$ derived from three isotopic masses was updated with the new masses and corroborate the existence of the deformed $$N=152$$ neutron shell closure for Md and Lr.

Journal Articles

Observation of doubly-charged ions of francium isotopes extracted from a gas cell

Schury, P.*; Wada, Michiharu*; Ito, Yuta*; Kaji, Daiya*; Haba, Hiromitsu*; Hirayama, Yoshikazu*; Kimura, Sota*; Koura, Hiroyuki; MacCormick, M.*; Miyatake, Hiroari*; et al.

Nuclear Instruments and Methods in Physics Research B, 407, p.160 - 165, 2017/06

 Times Cited Count:16 Percentile:77.98(Instruments & Instrumentation)

Various isotopes of Ac, Ra, Fr, and Rn were produced by fusion-evaporation reactions using a $$^{48}$$Ca beam. The energetic ions were stopped in and extracted from a helium gas cell. The extracted ions were identified using a multi-reflection time-of-fight mass spectrograph. In all cases, it was observed that the predominant charge state for the extracted ions, including the alkali Fr, was 2+.

Journal Articles

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; D$"u$llmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.

EPJ Web of Conferences, 131, p.07005_1 - 07005_7, 2016/12

 Times Cited Count:3 Percentile:70.66(Chemistry, Inorganic & Nuclear)

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO)$$_{6}$$. Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO)$$_{6}$$, W(CO)$$_{6}$$, and Sg(CO)$$_{6}$$.

Journal Articles

Decomposition studies of group 6 hexacarbonyl complexes, 1; Production and decomposition of Mo(CO)$$_6$$ and W(CO)$$_6$$

Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; et al.

Radiochimica Acta, 104(3), p.141 - 151, 2016/03

 Times Cited Count:36 Percentile:94.39(Chemistry, Inorganic & Nuclear)

Conditions of the production and decomposition of hexacarbonyl complexes of short-lived Mo and W isotopes were investigated to study thermal stability of the heaviest group 6 hexacarbonyl complex Sg(CO)$$_6$$. A tubular flow reactor was tested to decompose the hexacarbonyl complexes and to extract the first bond dissociation energies. A silver was found to be the most appropriate reaction surface to study the decomposition of the group 6 hexacarbonyl. It was found that the surface temperature at which the decomposition occurred was correlated to the first bond dissociation energy of Mo(CO)$$_6$$ and W(CO)$$_6$$, indicating that the first bond dissociation energy of Sg(CO)$$_6$$ could be determined with this technique.

Journal Articles

EBR-II passive safety demonstration tests benchmark analyses; Phase 2

Briggs, L.*; Monti, S.*; Hu, W.*; Sui, D.*; Su, G. H.*; Maas, L.*; Vezzoni, B.*; Partha Sarathy, U.*; Del Nevo, A.*; Petruzzi, A.*; et al.

Proceedings of 16th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-16) (USB Flash Drive), p.3030 - 3043, 2015/08

The International Atomic Energy Agency Coordinated Research Project, "Benchmark Analyses of an EBR-II Shutdown Heat Removal Test" is in the third year of its four-year term. Nineteen participants representing eleven countries have simulated two of the most severe transients performed during the Shutdown Heat Removal Tests program conducted at Argonne's Experimental Breeder Reactor II. Benchmark specifications were created for these two transients, enabling project participants to develop computer models of the core and primary heat transport system, and simulate both transients. In phase 1 of the project, blind simulations were performed and then evaluated against recorded data. During phase 2, participants have refined their models to address areas where the phase 1 simulations did not predict as well as desired the experimental data. This paper describes the progress that has been made to date in phase 2 in improving on the earlier simulations and presents the direction of planned work for the remainder of the project.

Journal Articles

In situ synthesis of volatile carbonyl complexes with short-lived nuclides

Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03

 Times Cited Count:15 Percentile:72.86(Chemistry, Analytical)

Rapid In situ synthesis of metal carbonyl complexes has been demonstrated using short-lived isotopes produced in nuclear fission and fusion reactions. The short-lived isotopes with high recoil energy directly react with carbon-monoxides and form carbonyl complexes. Only highly volatile complexes were fast transported in a gas stream to counting and chemistry devices. Short-lived Mo, Tc, Ru, Rh, W, Re, Os, and Ir were found to form volatile carbonyl complexes, while no volataile complex of Hf and Ta were detected. This technique has been applied to a chemical investigation of the superheavy element Sg (atomic number 106), and will be applicable to various fields of nuclear science with short-lived transition metal isotopes.

Journal Articles

Synthesis and detection of a Seaborgium carbonyl complex

Even, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Haba, Hiromitsu*; Asai, Masato; Sato, Tetsuya; Brand, H.*; Di Nitto, A.*; Eichler, R.*; Fan, F. L.*; et al.

Science, 345(6203), p.1491 - 1493, 2014/09

 Times Cited Count:70 Percentile:83.33(Multidisciplinary Sciences)

A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and $$alpha$$-detection apparatus COMPACT. Nuclear reaction products of short-lived $$^{265}$$Sg preseparated with a gas-filled recoil ion separator GARIS at RIKEN were directly injected into a gas cell filled with He/CO mixture gas, and chemical reaction products of volatile carbonyl complexes were trasported to COMPACT. The Sg carbonyl complex detected with COMPACT was found to be very volatile with adsorption enthalpy of $$-$$50 kJ/mol, from which we have concluded that this complex should be a Sg hexacarbonyl Sg(CO)$$_{6}$$. This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.

Journal Articles

Separation and recovery of Cm from Cm-Pu mixed oxide samples containing Am impurity

Hayashi, Hirokazu; Hagiya, Hiromichi; Kim, S.-Y.*; Morita, Yasuji; Akabori, Mitsuo; Minato, Kazuo

Journal of Radioanalytical and Nuclear Chemistry, 296(3), p.1275 - 1286, 2013/06

 Times Cited Count:4 Percentile:29.90(Chemistry, Analytical)

$$^{244}$$Cm was separated and recovered as an oxalate from $$^{244}$$Cm-$$^{240}$$Pu mixed oxide which had been $$^{244}$$Cm oxide sample prepared 40 years ago. Plutonium ions were removed from the solution prepared by dissolution of $$^{244}$$Cm-$$^{240}$$Pu mixed oxide in nitric acid, by using an anion exchange resin column. Curium oxalate, a precursor compound of curium oxide, was prepared from the purified curium solution and supplied for the syntheses and measurements of the thermochemical properties of curium compounds.

Journal Articles

Development of advanced reprocessing system based on precipitation method using pyrrolidone derivatives as precipitants; Overall evaluation of system

Ikeda, Yasuhisa*; Kawasaki, Takeshi*; Harada, Masayuki*; Nogami, Masanobu*; Kawata, Yoshihisa*; Kim, S.-Y.*; Morita, Yasuji; Chikazawa, Takahiro*; Someya, Hiroshi*; Kikuchi, Toshiaki*

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 5 Pages, 2011/12

An advanced reprocessing system for spent FBR fuels based on two precipitation processes using pyrrolidone derivatives as precipitants has been developed. Experimental results of precipitation behavior of U, Pu and other elements, the heat- and radiation-resistance of precipitants, the thermal decomposition properties of precipitates showed that N-n-butyl-2-pyrrolidone and N-neopentyl-2-pyrrolidone are the appropriate precipitants for the first and second precipitation steps, respectively. From the engineering investigation, We confirmed that the precipitation and the filtration can be done efficiently using the engineering scale equipment and that the fuel pellets are directly prepared by the calcination of the precipitates. On the basis of these results, we evaluated that the proposed system is expected to be one of candidates of the future reprocessing systems for spent FBR fuels.

Journal Articles

Molecular and crystal structures of plutonyl(VI) nitrate complexes with N-alkylated 2-pyrrolidone derivatives; Cocrystallization potentiality of U$$^{VI}$$ and Pu$$^{VI}$$

Kim, S.-Y.; Takao, Koichiro*; Haga, Yoshinori; Yamamoto, Etsuji; Kawata, Yoshihisa; Morita, Yasuji; Nishimura, Kenji*; Ikeda, Yasuhisa*

Crystal Growth & Design, 10(5), p.2033 - 2036, 2010/04

 Times Cited Count:15 Percentile:76.67(Chemistry, Multidisciplinary)

Plutonyl(VI) nitrate complexes with N-cyclohexyl-2-pyrrolidone (NCP) and N-neopentyl-2-pyrrolidone (NNpP) were prepared, and their molecular and crystal structures were determined by single crystal X-ray analysis. The obtained compounds have the similar composition, PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NRP)$$_{2}$$ (NRP = NCP, NNpP), which are analogous to the corresponding U(VI) complexes. Both PuO$$_{2}$$(NO$$_{3}$$)$$_{2}$$(NRP)$$_{2}$$ complexes show typical structural properties of actinyl(VI) nitrates, i.e., hexagonal-bipyramidal geometry consisting of two NRP molecules and two NO$$_{3}$$$$^{-}$$ ions located in trans positions in the equatorial plane of PuO$$_{2}$$$$^{2+}$$ moiety. These findings provide one of criteria in selection of suitable NRP as a precipitation agent for the spent nuclear fuel reprocessing based on the precipitation method.

Journal Articles

Development of advanced reprocessing system based on precipitation method using pyrrolidone derivatives as precipitants; Precipitation behavior of U(VI), Pu(IV), and Pu(VI) by pyrrolidone derivatives with low hydrophobicity

Morita, Yasuji; Takao, Koichiro*; Kim, S.-Y.; Kawata, Yoshihisa; Harada, Masayuki*; Nogami, Masanobu*; Nishimura, Kenji*; Ikeda, Yasuhisa*

Journal of Nuclear Science and Technology, 46(12), p.1129 - 1136, 2009/12

 Times Cited Count:19 Percentile:74.32(Nuclear Science & Technology)

A reprocessing system for spent FBR fuels consisting of two precipitation processes has been proposed. In this system, first only U(IV) species are precipitated using pyrrolidone derivative with low hydrophobicity and donicity, and secondly residual U(VI) and Pu(IV, VI) are precipitated simultaneously using pyrrolidone derivative with high precipitation ability. In this study, we have examined precipitation behavior of U(VI), Pu(IV), and Pu(VI) species in nitric acid solutions by using $$N$$-$$n$$-propyl-2-pyrrolidone (NProP), $$N$$-butyl-2-pyrrolidone (NBP), $$N$$-$$iso$$-butyl-2-pyrrolidone (NiBP), or $$N$$-cyclohexyl-2-pyrrolidone (NCP) to select the precipitants for the first precipitation process. As a result, NBP were found to be the most promising precipitant for the first precipitation process.

Journal Articles

Development of advanced reprocessing system using highly selective and controllable precipitants; Precipitation behavior of plutonium from U-Pu solution

Morita, Yasuji; Kim, S.-Y.; Kawata, Yoshihisa; Ikeda, Yasuhisa*; Kikuchi, Toshiaki*

Proceedings of International Conference on Advanced Nuclear Fuel Cycle; Sustainable Options & Industrial Perspectives (Global 2009) (CD-ROM), p.1081 - 1085, 2009/09

We have been developing an advanced reprocessing system for spent FBR fuels based on precipitation method using pyrrolidone derivatives, which consists of two precipitation steps; the first selective U precipitation step and the second U-Pu co-precipitation step. In the present study, precipitation behavior of Pu with pyrrolidone derivatives with high precipitation ability of N-(1,2-dimethyl)propyl-2-pyrrolidone (NDMProP), N-neopenthyl-2-pyrrolidone (NNpP) and N-cyclohexyl-2-pyrrolidone (NCP) has been examined with solutions of U-Pu mixture in order to evaluate their applicability to the second step. Since NNpP showed the highest precipitation ability for Pu(IV) and the best physical property as precipitate, NNpP would be the most appropriate precipitant for the U-Pu co-precipitation process. Precipitation of Np(IV, V, VI) with NNpP was also examined and it was found that Np(VI) could be quantitatively co-precipitated with U(VI) and Pu(IV).

Journal Articles

Separation of Am and Cm from HLLW by extraction chromatography using novel R-BTP extraction resins

Wei, Y.*; Hoshi, Harutaka; Morita, Yasuji; Bruggeman, A.*; Goethals, P.*

Proceedings of International Conference on Advanced Nuclear Fuel Cycle; Sustainable Options & Industrial Perspectives (Global 2009) (CD-ROM), p.1086 - 1093, 2009/09

To separate the long-lived minor actinides (MA = Am, Cm) from high level liquid waste (HLLW), we have been studying an advanced process by extraction chromatography which uses minimal organic solvent and compact equipment. Generally, the process consists of two separation columns packed with CMPO extraction resin for elemental group separation and R-BTP extraction resin for the isolation of MA from lanthanides (Ln), respectively. R-BTP is a family of nitrogen-donor ligand which has been verified to have stronger adsorption affinity for trivalent MA over Ln(III). As an extractant or adsorbent, it is generally considered that R-BTP compounds shall be used in a weakly acid medium, since the compounds show less stability in acidic medium due to the protonation of nitrogen atoms. However, we have found that the adsorption selectivity for Am(III) and Cm(III) and chemical stability of R-BTP adsorbents strongly depend on the length and structure of the alkyl group.

Journal Articles

Study on valence of Pu, Np and Tc in nitric acid after electrolytic reduction

Hoshi, Harutaka*; Wei, Y.-Z.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Journal of Alloys and Compounds, 444-445, p.663 - 667, 2007/10

 Times Cited Count:4 Percentile:31.99(Chemistry, Physical)

no abstracts in English

Journal Articles

Development of an advanced reprocessing system based on use of pyrrolidone derivatives as novel precipitants with high selectivity and control ability; Precipitation behavior of plutonium

Morita, Yasuji; Kim, S.-Y.; Ikeda, Yasuhisa*; Nogami, Masanobu*; Nishimura, Kenji*

Proceedings of International Conference on Advanced Nuclear Fuel Cycles and Systems (Global 2007) (CD-ROM), p.1508 - 1512, 2007/09

We have been developing an advanced reprocessing system for spent FBR fuels based on precipitation method using pyrrolidone derivatives. In previous investigation, N-cyclohexyl-2-pyrrolidone (NCP) is used as a precipitant and a process consisting of selective U precipitation step and U-Pu co-precipitation step was developed. In order to make the process more effective and more economical, we are now studying precipitation of U and Pu with other pyrrolidone derivatives. In the present study, precipitation behavior of Pu was examined using N-butyl-2-pyrrolidone (NBP) and N-propyl-2-pyrrolidone (NProP), which have lower hydrophobicity than NCP. The experiments with Pu(IV) or Pu(VI) solutiona and U(VI)-Pu(IV) solutions showed that Pu is less precipitated with NBP or NProP than with NCP. From these results, it is expected that NBP and NProP can be used as precipitants for the selective U precipitation step and make the step more selective and effective.

Journal Articles

Experiments on synthesis of the heaviest element at RIKEN

Morita, Kosuke*; Morimoto, Koji*; Kaji, Daiya*; Akiyama, Takahiro*; Goto, Shinichi*; Haba, Hiromitsu*; Ideguchi, Eiji*; Kanungo, R.*; Katori, Kenji*; Kikunaga, Hidetoshi*; et al.

AIP Conference Proceedings 891, p.3 - 9, 2007/03

A series of experiments studying the productions and their decays of the heaviest elements have been performed by using a gas-filled recoil separator GARIS at RIKEN. Results on the isotope of the 112th element, $$^{277}$$112, and on that of the 113th element, $$^{278}$$113, are reviewed. Two decay chains which are assigned to be ones originating from the isotope $$^{277}$$112 were observed in the $$^{208}$$Pb($$^{70}$$Zn, n) reaction. The results provide a confirmation of the production and decay of the isotope $$^{277}$$112 reported by a research group at GSI, Germany, produced via the same reaction by using a velocity filter. Two decay chains, both consisted of four consecutive alpha decays followed by a spontaneous fission, were observed also in the reaction $$^{209}$$Bi($$^{70}$$Zn, n). Those are assigned to be the convincing candidate events of the isotope of the 113th element, $$^{278}$$113, and its daughter nuclei. $$^{274}$$Rg, $$^{270}$$Mt, $$^{266}$$Bh, and $$^{262}$$Db.

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