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Journal Articles

Hydrogen absorption and diffusion behaviors in cube-shaped palladium nanoparticles revealed by ambient-pressure X-ray photoelectron spectroscopy

Tang, J.*; Seo, O.*; Rivera Rocabado, D. S.*; Koitaya, Takanori*; Yamamoto, Susumu*; Namba, Yusuke*; Song, C.*; Kim, J.*; Yoshigoe, Akitaka; Koyama, Michihisa*; et al.

Applied Surface Science, 587, p.152797_1 - 152797_8, 2022/06

The hydrogen absorption and diffusion mechanisms on cube-shaped Pd nanoparticles (NPs) which are important hydrogen-storage materials were studied using X-ray photoelectron spectroscopy and DFT calculations. In the surface region, hydrogen absorption showed almost similar behavior regardless of the NPs size. It was found that the octahedral sites are more favorable than the tetrahedral sites for hydrogen occupation. We also clarified that the hydrogen atoms absorbing on the smaller-sized Pd NPs diffuse to the subsurface more actively because of the weakened Pd-H bond by the surface disordering, which plays an important role in hydrogen adsorption at a low H$$_{2}$$ pressure.

JAEA Reports

Analysis of the radioactivity concentrations in radioactive waste generated from JPDR Facility

Tobita, Minoru*; Haraga, Tomoko; Endo, Tsubasa*; Omori, Hiroyuki*; Mitsukai, Akina; Aono, Ryuji; Ueno, Takashi; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Data/Code 2021-013, 30 Pages, 2021/12

JAEA-Data-Code-2021-013.pdf:1.47MB

Radioactive wastes generated from nuclear research facilities in Japan Atomic Energy Agency are planning to be buried in the near surface disposal field. Therefore, it is required to establish the method to evaluate the radioactivity concentrations of radioactive wastes until the beginning of disposal. In order to contribute to this work, we collected and analyzed concrete samples generated from JPDR facility. In this report, we summarized the radioactivity concentrations of 21 radionuclides ($$^{3}$$H, $$^{14}$$C, $$^{36}$$Cl, $$^{41}$$Ca, $$^{60}$$Co, $$^{63}$$Ni, $$^{90}$$Sr, $$^{94}$$Nb, $$^{rm 108m}$$Ag, $$^{137}$$Cs, $$^{152}$$Eu, $$^{154}$$Eu, $$^{rm 166m}$$Ho, $$^{234}$$U, $$^{238}$$U, $$^{238}$$Pu, $$^{239}$$Pu, $$^{240}$$Pu, $$^{241}$$Am, $$^{243}$$Am, $$^{244}$$Cm) which were obtained from radiochemical analysis of the samples in fiscal year 2018-2019.

JAEA Reports

Update on the regional-scale 3D geological model in the Horonobe Underground Research Laboratory Project

Sakai, Toshihiro; Ishii, Eiichi

JAEA-Data/Code 2021-009, 13 Pages, 2021/08

JAEA-Data-Code-2021-009.pdf:1.9MB
JAEA-Data-Code-2021-009-appendix(CD-ROM).zip:42.79MB

Japan Atomic Energy Agency is performing the Horonobe Underground Research Laboratory Project, which includes a scientific study of the deep geological environment as a basis of research and development for the geological disposal of high level radioactive wastes, in order to establish comprehensive techniques for the investigation, analysis and assessment of the deep geological environment in the sedimentary rock. The numerical data of 3D geological model in regional-scale was compiled in 2019 as JAEA-Data/Code 2019-007, and then this report updates a part of the numerical data of 3D geological model around the underground facilities.

JAEA Reports

Study on the radioactivity evaluation method of biological shielding concrete of JPDR for near surface disposal

Kochiyama, Mami; Okada, Shota; Sakai, Akihiro

JAEA-Technology 2021-010, 61 Pages, 2021/07

JAEA-Technology-2021-010.pdf:3.56MB
JAEA-Technology-2021-010(errata).pdf:0.75MB

It is necessary to evaluate the radioactivity inventory in wastes in order to dispose of radioactive wastes generated from dismantling nuclear reactor in the shallow ground. In this report, we examined radioactivity evaluation method for near surface disposal about biological shield concrete near the core generated from the dismantling of JPDR. We calculated radioactive concentration of the target biological concrete using the DORT code and the ORIGEN-S code, and we estimated radioactivity concentration Di (Bq/t). For DORT calculation, the cross-section library created from the MATXSLIB-J40 file from JENDL-4.0 was used, and for ORIGEN-S, the attached library of SCALE6.0 was used. As a result of comparing the calculation results of the radioactivity concentration with the past measured values in the radial direction and the vertical direction, we found that the trends were generally the same. We calculated radioactive concentration of the target biological concrete Di (Bq/t), and we compared with the estimated Ci (Bq/t) equivalent to the dose criteria of trench disposal calculated for 140 nuclides. As a result we inferred that the except for about 2% of target waste could be disposed of in the trench disposal facility. We also preselected important nuclides for trench disposal based on the ratios (Di/Ci) for each nuclide, H-3, C-14, Cl-36, Ca-41, Co-60, Sr-90, Eu-152 and Cs-137 were selected as important nuclides.

JAEA Reports

Analysis of the radioactivity concentrations in low-level radioactive waste generated from JRR-3 and JPDR facilities

Tsuchida, Daiki; Haraga, Tomoko; Tobita, Minoru*; Omori, Hiroyuki*; Omori, Takeshi*; Murakami, Hideaki*; Mitsukai, Akina; Aono, Ryuji; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Data/Code 2020-022, 34 Pages, 2021/03

JAEA-Data-Code-2020-022.pdf:1.74MB

Radioactive wastes generated from nuclear research facilities in Japan Atomic Energy Agency are planning to be buried in the near surface disposal field. Therefore, it is required to establish the method to evaluate the radioactivity concentrations of radioactive wastes until the beginning of disposal. In order to contribute to this work, we collected and analyzed concrete samples generated from JRR-3 and JPDR. In this report, we summarized the radioactivity concentrations of 22 radionuclides($$^{3}$$H, $$^{14}$$C, $$^{36}$$Cl, $$^{41}$$Ca, $$^{60}$$Co, $$^{63}$$Ni, $$^{90}$$Sr, $$^{94}$$Nb, $$^{rm 108m}$$Ag, $$^{133}$$Ba, $$^{137}$$Cs, $$^{152}$$Eu, $$^{154}$$Eu, $$^{rm 166m}$$Ho, $$^{234}$$U, $$^{238}$$U, $$^{238}$$Pu, $$^{239+240}$$Pu, $$^{241}$$Am, $$^{243}$$Am, $$^{244}$$Cm) which were obtained from radiochemical analysis of the samples.

JAEA Reports

JAEA-TDB-RN in 2020; Update of JAEA's thermodynamic database for solubility and speciation of radionuclides for performance assessment of geological disposal of high-level and TRU wastes

Kitamura, Akira

JAEA-Data/Code 2020-020, 164 Pages, 2021/03

JAEA-Data-Code-2020-020.pdf:3.11MB
JAEA-Data-Code-2020-020-appendix(DVD-ROM).zip:0.56MB

Part of JAEA's Thermodynamic Database (JAEA-TDB) for solubility and speciation of radionuclides (JAEA-TDB-RN) for performance assessment of geological disposal of high-level radioactive and TRU wastes has been updated with subsuming the database for geochemical calculations (JAEA-TDB-GC). This report has focused to update JAEA-TDB-RN after selecting change in standard Gibbs free energy of formation ($$Delta_{rm f}$$$$G^{circ}_{rm m}$$), change in standard enthalpy change of formation ($$Delta$$$$H$$$$^{circ}$$$$_{rm m}$$), standard molar entropy ($$S^{circ}$$$$_{rm m}$$) and, heat capacity ($$C^{circ}_{rm p}$$), change in standard Gibbs free energy of reaction ($$Delta_{rm r}G^{circ}$$$$_{rm m}$$), change in standard enthalpy change of reaction ($$Delta$$$$_{rm r}$$$$H$$$$^{circ}$$$$_{rm m}$$) and standard entropy change of reaction ($$Delta_{rm r}S^{circ}_{rm m}$$) as well as logarithm of equilibrium constant (log$$_{10}$$$$K^{circ}$$) at standard state. The extent of selection of these thermodynamic data enables to evaluate solubility and speciation of radionuclides at temperatures other than 298.15 K. Furthermore, the latest thermodynamic data for iron which have been critically reviewed, selected and compiled by the Nuclear Energy Agency within Organisation for Economic Co-operation and Development (OECD/NEA) have been accepted. Most of previously selected log$$_{10}$$$$K^{circ}$$ have been refined to confirm internal consistency with JAEA-TDB-GC. Text files of the updated JAEA-TDB have been provided for geochemical calculation programs of PHREEQC and Geochemist's Workbench.

Journal Articles

Corrosion cracking of JPDR the first Japanese light water reactor

Tsukada, Takashi; Soma, Yasutaka

Hozengaku, 19(4), p.37 - 44, 2021/01

Corrosion Cracking phenomena in JPDR (Japan Power Demonstration Reactor) the first Japanese Light Water Reactor is reviewed. This review describes two major cracking failure. The first was found during inspection in 1966 as the cracking failure on weld-overlay cladding at the inner wall of the top head. A series of analysis showed that some of the cracks reached the base metal across the weld boundaries and further penetrated into the vessel wall. Significant depletion of ferrite content was detected in manually welded part considered to assisted the cracking. These inspection result in improvement of the welding procedure and no similar failures have been reported in Japanese reactor. This mode of failure gave rise to a new research field studying the corrosion fatigue behavior of low alloy steel because of importance to assess pressure boundary of the reactor. The experiment of JPDR also contributed to the establishment of international cooperation for studying EAC (environmentally assisted cracking). The second failure was found in 1972 near the welded part between stainless piping and safe end. The extensive research concluded that this failure was caused by Stress Corrosion Cracking.

Journal Articles

Determination of atomistic deformation of tricalcium silicate paste with high-volume fly ash

Jee, H.*; Im, S.*; Kanematsu, Manabu*; Suzuki, Hiroshi; Morooka, Satoshi; Koyama, Taku*; Machida, Akihiko*; Bae, S.*

Journal of the American Ceramic Society, 103(12), p.7188 - 7201, 2020/12

 Times Cited Count:2 Percentile:40.39(Materials Science, Ceramics)

JAEA Reports

Analysis of the radioactivity concentrations in low-level radioactive waste generated from JPDR and JRR-4

Aono, Ryuji; Mitsukai, Akina; Haraga, Tomoko; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Data/Code 2020-006, 70 Pages, 2020/08

JAEA-Data-Code-2020-006.pdf:2.59MB

Radioactive wastes which generated from research and testing reactors in Japan Atomic Energy Agency are planning to be buried at the near surface disposal field. Therefore, it is required to establish the method to evaluate the radioactivity concentrations of radioactive wastes by the time it starts disposal. In order to contribute to this work, we collected and analyzed the samples generated from JPDR and JRR-4. In this report, we summarized the radioactivity concentrations of 19 radionuclides ($$^{3}$$H, $$^{14}$$C, $$^{36}$$Cl, $$^{60}$$Co, $$^{63}$$Ni, $$^{90}$$Sr, $$^{94}$$Nb, $$^{99}$$Tc, $$^{rm 108m}$$Ag, $$^{129}$$I, $$^{137}$$Cs, $$^{152}$$Eu, $$^{154}$$Eu, $$^{234}$$U, $$^{238}$$U, $$^{238}$$Pu, $$^{239+240}$$Pu, $$^{241}$$Am, $$^{244}$$Cm) which were obtained from radiochemical analysis of those samples.

Journal Articles

$$f$$-electron states of NpPd$$_5$$Al$$_2$$ and the isostructural family; Heavy fermion superconductivity accompanied by valence crossover

Metoki, Naoto

Kotai Butsuri, 55(7), p.285 - 296, 2020/07

Electron states are the main theme of "solid-state physics", which is essential for microscopic understanding of multipoles and superconductivity, etc. Rare earths (4$$f$$) and actinides (5$$f$$) provide variety of interesting states realized with competing interactions between the increasing number of $$f$$ electrons. Since crystal field splitting of many-body $$f$$ electron system is smaller than the bandwidth, (1) high resolution experiments are needed, (2) essentially no clear spectrum with well defined peaks is expected in itinerant Ce and U compounds, and (3) Np and Pu is strictly regulated. Therefore, systematic research on magnetic excitations by neutron scattering experiments of localized compounds and rare earth iso-structural reference is useful. We describe the $$f$$ electron states of heavy electron compounds NpPd$$ _5$$Al$$_2$$ and actinide and rare earth based iso-structural family.

Journal Articles

Evaluation of oxidation efficiency of hydrophobic palladium catalyst for $$^{3}$$H monitoring in radioactive gaseous waste

Furutani, Misa; Kometani, Tatsunari; Nakagawa, Masahiro; Ueno, Yumi; Sato, Junya; Iwai, Yasunori*

Hoken Butsuri (Internet), 55(2), p.97 - 101, 2020/06

Herein, an oxidation catalyst was introduced after heating it to 600$$^{circ}$$C to oxidize tritium gas (HT) existing in exhaust into tritiated water vapor (HTO). This study aims to establish a safer $$^{3}$$H monitoring system by lowering the heating temperature required for the catalyst. In these experiments, which were conducted in the Nuclear Science Research Institute, Japan Atomic Energy Agency, cupric oxide, hydrophobic palladium/silicon dioxide (Pd/SiO$$_{2}$$), and platinum/aluminum oxide (Pt/Al$$_{2}$$O$$_{3}$$) catalysts were ventilated using standard hydrogen gas. After comparing the oxidation efficiency of each catalyst at different temperatures, we found that the hydrophobic Pd/SiO$$_{2}$$ and Pt/Al$$_{2}$$O$$_{3}$$ catalysts could oxidize HT into HTO at 25$$^{circ}$$C.

Journal Articles

Analysis of atomistic structural deformation characteristics of calcium silicate hydrate in 53-year-old tricalcium silicate paste using atomic pair distribution function

Bae, S.*; Jee, H.*; Suh, H.*; Kanematsu, Manabu*; Shiro, Ayumi*; Machida, Akihiko*; Watanuki, Tetsu*; Shobu, Takahisa; Morooka, Satoshi; Geng, G.*; et al.

Construction and Building Materials, 237, p.117714_1 - 117714_10, 2020/03

 Times Cited Count:4 Percentile:69.91(Construction & Building Technology)

Journal Articles

Separation of palladium by solvent extraction with methylamino-bis-$$N,N$$-dioctylacetamide and direct electrodeposition from loaded organic phase

Matsumiya, Masahiko*; Song, Y.*; Tsuchida, Yusuke*; Sasaki, Yuji

Separation and Purification Technology, 234, p.115841_1 - 115841_8, 2020/03

The development of solvent extraction and direct electrodeposition processes is an important task to reduce the volume of secondary wastes. In this study, the extraction of Pd(II) from hydrochloric/chloride media using methylimino-bis-$$N,N$$-dioctylacetamide (MIDOA) in three diluents (acetophenone; AP, 1,2-dichloroethane; DCE, or 1-octanol; OC) and the electrochemical behavior of the extracted Pd(II) complex in the MIDOA/AP bath was investigated. Pd(II) was found to be reduced to Pd(0) metal via a two-electron transfer between -2.38 V and -3.40 V. The potentiostatic electrodeposition of the extracted Pd(II) complex enabled us to recover the blackish electrodeposits, which were identified as Pd metal.

Journal Articles

Pseudo-triplet 5$$f$$ electron state in the heavy fermion superconductor NpPd$$_5$$Al$$_2$$

Metoki, Naoto; Aoki, Dai*; Griveau, J.-C.*; Otsuki, Junya*

Journal of the Physical Society of Japan, 89(2), p.024707_1 - 024707_6, 2020/02

 Times Cited Count:2 Percentile:51.78(Physics, Multidisciplinary)

The pseudo triplet ground state in the heavy-fermion superconductor NpPd$$_5$$Al$$_2$$ was concluded. The magnetic susceptibility $$chi$$ can be reproduced by the singlet ground state $$Gamma_{t1}$$ with the main component of $$|0rangle$$ and the first excited doublet $$Gamma_{t5}$$ dominated by $$|pm1rangle$$ at $$Delta E=49$$,K. The magnetization curve can be explained from the effective local hamiltonian for pseudo spin $$J$$=1 with $$DJ_z^2$$($$D=Delta E$$) equivalent to the quadrupole operator $$O_{20}$$. The specific heat can be described with the Kondo model normalized to give the entropy R$$ln3$$, corresponding to the pseudo triplet state. The derived Kondo temperature $$T_{rm K}=55$$,K comparable to the level splitting $$Delta E=49$$,K indicates the contribution of the excited doublet $$Gamma_{t5}$$ to the possible multi-channel Kondo effect.

Journal Articles

$$f$$-electron states of heavy-fermion superconductor NpPd$$_5$$Al$$_2$$ and rare-earth- and actinide-based isostructural compounds

Metoki, Naoto

Journal of the Physical Society of Japan, 89(2), p.025001_1 - 025001_2, 2020/02

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

Good correspondence of the $$LS$$ and $$j$$-$$j$$ coupling scheme can be realized in the $$f$$-electron states of the heavy-fermion superconductor NpPd$$_5$$Al$$_2$$ and the isostructural family. The rare-earth and actinide elements are under a common strong uniaxial point charge potential with tetragonal point symmetry $$D_{4h}$$. The systematic development of the $$f$$-electron states can be understood in the $$LS$$ coupling scheme of $$^nf$$ configuration (the number of $$f$$ electrons $$nleq6$$). We can find the corresponding states in $$j$$-$$j$$ coupling scheme with three $$f$$-orbitals $$Gamma_7^{rm; i}, Gamma_7^{rm; ii}$$, and $$Gamma_6$$ determined from CePd$$_5$$Al$$_2$$ with $$^1f$$ configuration.

JAEA Reports

The Regional-scale 3D geological model in the Horonobe Underground Research Laboratory Project

Sakai, Toshihiro; Matsuoka, Toshiyuki

JAEA-Data/Code 2019-007, 29 Pages, 2019/09

JAEA-Data-Code-2019-007.pdf:53.07MB
JAEA-Data-Code-2019-007-appendix(CD-ROM).zip:340.04MB

Japan Atomic Energy Agency is performing the Horonobe Underground Research Laboratory Project, which includes a scientific study of the deep geological environment as a basis of research and development for the geological disposal of high level radioactive wastes, in order to establish comprehensive techniques for the investigation, analysis and assessment of the deep geological environment in the sedimentary rock. This report summarize numerical data of 3D geological model in regional-scale constructed by Maptek$$^{rm TM}$$ Vulcan$$^{rm TM}$$.

Journal Articles

Local structure of functional solids

Shamoto, Shinichi

Journal of the Physical Society of Japan, 88(8), p.081008_1 - 081008_11, 2019/08

AA2019-0006.pdf:1.06MB

 Times Cited Count:1 Percentile:20.66(Physics, Multidisciplinary)

JAEA Reports

Update of JAEA-TDB; Update of thermodynamic data for zirconium and those for isosaccahrinate, tentative selection of thermodynamic data for ternary M$$^{2+}$$-UO$$_{2}$$$$^{2+}$$-CO$$_{3}$$$$^{2-}$$ system and integration with JAEA's thermodynamic database for geochemical calculations

Kitamura, Akira

JAEA-Data/Code 2018-018, 103 Pages, 2019/03

JAEA-Data-Code-2018-018.pdf:5.66MB
JAEA-Data-Code-2018-018-appendix1(DVD-ROM).zip:0.14MB
JAEA-Data-Code-2018-018-appendix2(DVD-ROM).zip:0.15MB
JAEA-Data-Code-2018-018-appendix3(DVD-ROM).zip:0.19MB

The latest available thermodynamic data were critically reviewed and the selected values were included into the JAEA-TDB for performance assessment of geological disposal of high-level radioactive and TRU wastes. This critical review specifically addressed thermodynamic data for (1) a zirconium-hydroxide system through comparison of thermodynamic data selected by the Nuclear Energy Agency within the Organisation for Economic Co-operation and Development (OECD/NEA), (2) complexation of metal ions with isosaccharinic acid based on the latest review papers. Furthermore, the author performed (3) tentative selection of thermodynamic data on ternary complexes among alkaline-earth metal, uranyl and carbonate ions, and (4) integration with the latest version of JAEA's thermodynamic database for geochemical calculations. The internal consistency of the selected data was checked by the author. Text files of the updated and integrated thermodynamic database have been prepared for geochemical calculation programs of PHREEQC and Geochemist's Workbench.

Journal Articles

Determination of $$^{107}$$Pd in Pd purified by selective precipitation from spent nuclear fuel by laser ablation ICP-MS

Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro

Analytical and Bioanalytical Chemistry, 411(5), p.973 - 983, 2019/02

 Times Cited Count:5 Percentile:57.47(Biochemical Research Methods)

Determination of radiopalladium $$^{107}$$Pd is required for ensuring the radiation safety of Pd extracted from spent nuclear fuel for recycling or disposal. We employed laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to simplify an analytical procedure of $$^{107}$$Pd. Pd was separated through selective Pd precipitation reaction from spent nuclear fuel. Laser ablation allows direct measurement of the Pd precipitates, skipping the dissolution and dilution procedure. In this study, $$^{102}$$Pd in natural Pd standard solution was used as an internal standard, taking advantage of its absence in spent nuclear fuel. The Pd precipitate was uniformly embedded on the surface of the centrifugal filter, forming a microscopically thin flat surface of Pd. The resulting homogeneous Pd layer is suitable for obtaining a stable signal ratio of $$^{107}$$Pd/$$^{102}$$Pd. The amount of $$^{107}$$Pd obtained by LA-ICP-MS corresponds to the values obtained by conventional solution nebulization measurement.

Journal Articles

Evaluation and modelling report of Task 9A based on comparisons and analyses of predictive modelling results for the REPRO WPDE experiments; Task 9 of SKB Task Force GWFTS - Increasing the realism in solute transport modelling based on the field experiments REPRO and LTDE-SD

Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Trinchero, P.*; Iraola, A.*; Ebrahimi, H.*; Molinero, J.*; et al.

SKB R-17-10, 153 Pages, 2019/01

The SKB Task Force is an international forum on modeling of groundwater flow and solute transport in fractured rock. The WPDE experiments are matrix diffusion experiments in gneiss performed at the ONKALO underground facility in Finland. Synthetic groundwater containing several conservative and sorbing tracers was injected along a borehole interval. The objective of Task 9A was the predictive modeling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches, participated in this exercise. An important conclusion from this exercise is that the modeling results were very sensitive to the magnitude of dispersion in the borehole opening, which is related to the flow of water. Focusing on the tails of the breakthrough curves, which are more directly related to matrix diffusion and sorption, the results from the different teams were more comparable. The modeling results have also been finally compared to the measured breakthroughs.

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