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Journal Articles

Predictive modeling of a simple field matrix diffusion experiment addressing radionuclide transport in fractured rock. Is it so straightforward?

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

Nuclear Technology, 208(6), p.1059 - 1073, 2022/06

The SKB Task Force is an international forum on modelling 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 modelling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches and codes, participated in this exercise. An important conclusion from this exercise is that the modelling 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.

Journal Articles

Phase-field mobility for crystal growth rates in undercooled silicates, SiO$$_2$$ and GeO$$_2$$ liquids

Kawaguchi, Munemichi; Uno, Masayoshi*

Journal of Crystal Growth, 585, p.126590_1 - 126590_7, 2022/05

Phase-field mobility, $$L$$, and crystal growth rates in crystallization of 11 oxides or mixed oxides in undercooled silicates, SiO$$_2$$ and GeO$$_2$$ liquids were calculated with a simple phase-field model (PFM), and material dependence of the $$L$$ was discussed. Ratios between experimental crystal growth rates and the PFM simulation with $$L=1$$ were confirmed to be proportional to a power of $$frac{TDelta T}{eta}$$ on the solid/liquid interface process during the crystal growth in a log-log plot. We determined that parameters, $$A$$ and $$B$$, of the $$L=A(frac{k_{B}TDelta T}{6pi^{2}lambda^{3}eta T_{m} })^{B}$$ were $$A=6.7times 10^{-6}$$ to $$2.6$$m$$^4$$J$$^{-1}$$s$$^{-1}$$ and $$B=0.65$$ to $$1.3$$, which were unique for the materials. It was confirmed that our PFM simulation with the determined $$L$$ reproduced quantitively the experimental crystal growth rates. The $$A$$ has a proportional relationship with the diffusion coefficient of a cation molar mass average per unit an oxygen molar mass at $$T_{m}$$ in a log-log graph. The $$B$$ depends on the sum of the cation molar mass per the oxygen molar mass, $$frac{Sigma_{i}M_{i}}{M_{O}}$$, in a compound. In $$frac{Sigma_{i}M_{i}}{M_{O}}leq 25$$, the $$B$$ decreases with the cation molar mass increasing. The assumed cause is that the B represents the degree of the temperature dependence of the $$L$$. Since the cation molar mass is proportional to an inertial resistance of the cation transfer, the $$B$$ decreases with inverse of the cation molar mass. In crystallization of the silicates of heavy cation in $$frac{Sigma_{i}M_{i}}{M_{O}}geq 25$$, the $$B$$ saturates at approximately 0.67, which leads to $$T_{p}approx 0.9T_{m}$$.

Journal Articles

Recent studies on fuel properties and irradiation behaviors of Am/Np-bearing MOX

Hiroka, Shun; Yokoyama, Keisuke; Kato, Masato

Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Sustainable Clean Energy for the Future (FR22) (Internet), 8 Pages, 2022/04

Property studies on Am/Np-bearing MOX were carried out and how the properties influences on the irradiation behaviors was discussed. Both Am and Np inclusions increase the oxygen potential of MOX. Inter-diffusion coefficients obtained by using diffusion couple technique indicate that the inter-diffusion coefficient is larger in the order of U-Am, U-Pu and U-Np. Also, the inter-diffusion coefficients were evaluated to be larger at the O/M = 2 than those of O/M $$<$$ 2 by several orders. The increase of oxygen potential with Am/Np leads to higher vapor pressure of UO$$_{3}$$ and the acceleration of the pore migration along temperature gradient during irradiation. The redistributions of actinide elements were also considered with the relationship of the pore migration and diffusion in solid state. Thus, the obtained inter-diffusion coefficients directly influence on the redistribution rate. The obtained properties were modelled and can be installed in a fuel irradiation simulation code.

Journal Articles

Dynamic accommodation of internal stress and selection of crystallographic orientation relationship in pearlite

Amemiya, Yutaro*; Nakada, Nobuo*; Morooka, Satoshi; Kosaka, Makoto*; Kato, Masaharu*

ISIJ International, 62(2), p.282 - 290, 2022/02

Journal Articles

Experimental analysis on dynamics of liquid molecules adjacent to particles in nanofluids

Hashimoto, Shunsuke*; Nakajima, Kenji; Kikuchi, Tatsuya*; Kamazawa, Kazuya*; Shibata, Kaoru; Yamada, Takeshi*

Journal of Molecular Liquids, 342, p.117580_1 - 117580_8, 2021/11

 Times Cited Count:0

Quasi-elastic neutron scattering (QENS) and pulsed-field-gradient nuclear magnetic resonance (PFGNMR) analyses of a nanofluid composed of silicon dioxide (SiO$$_{2}$$) nanoparticles and a base fluid of ethylene glycol aqueous solution were performed. The aim was to elucidate the mechanism increase in the thermal conductivity of the nanofluid above its theoretical value. The obtained experimental results indicate that SiO$$_{2}$$ particles may decrease the self-diffusion coefficient of the liquid molecules in the ethylene glycol aqueous solution because of their highly restricted motion around these nanoparticles. At a constant temperature, the thermal conductivity increases as the self-diffusion coefficient of the liquid molecules decreases in the SiO$$_{2}$$ nanofluids.

Journal Articles

A Scaling approach for retention properties of crystalline rock; Case study of the in-situ long-term sorption and diffusion experiment (LTDE-SD) at the $"A$sp$"o$ Hard Rock Laboratory in Sweden

Tachi, Yukio; Ito, Tsuyoshi*; Gylling, B.*

Water Resources Research, 57(11), 20 Pages, 2021/11

This paper focuses on the scaling approach for sorption and diffusion parameters from laboratory to in-situ conditions using the dataset of LTDE-SD experiment performed at the $"A$sp$"o$ HRL. The near-surface heterogeneities at both fracture surface and rock matrix could be evaluated by conceptual model with high porosity and diffusivity, and sorption capacity, and their gradual change at the near-surface zones. The modelling results for non-sorbing Cl-36 and weak-sorbing Na-22 could validate the model concept and the parameter estimation of porosity and diffusivity, by considering the disturbed zone of 5 mm thickness with gradual parameter changes. The De values of these cationic and anionic tracers showed typical cation excess and anion exclusion effects. The modelling results for high sorbing tracers (Cs-137, Ra-226, Ni-63 and Np-237) with different sorption mechanism could confirm the validity of the scaling approaches of Kd values as a function of particle size and their relation to the near-surface disturbances.

Journal Articles

Dynamics of water in a catalyst layer of a fuel cell by quasielastic neutron scattering

Ito, Kanae; Yamada, Takeshi*; Shinohara, Akihiro*; Takata, Shinichi; Kawakita, Yukinobu

Journal of Physical Chemistry C, 125(39), p.21645 - 21652, 2021/10

 Times Cited Count:0

Journal Articles

Evaluation report of Task 9B based on comparisons and analyses of modelling results for the $"A$sp$"o$ HRL LTDE-SD experiments

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Kek$"a$l$"a$inen, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Vete$v{s}$n$'i$k, A.*; Reimitz, D.*; et al.

SKB TR-20-17, 71 Pages, 2021/07

Task 9B of the SKB Task Force on Modelling of Groundwater Flow and Transport of Solutes in fractured rock focused on the modelling of experimental results from the LTDE-SD in situ tracer test performed at the $"A$sp$"o$ Hard Rock Laboratory in Sweden. Ten different modelling teams provided results for this exercise, using different concepts and codes. Three main types of modelling approaches were used: (1) analytical solutions to the transport-retention equations, (2) continuum-porous-medium numerical models, and (3) microstructure-based models accounting for small-scale heterogeneity (i.e. mineral grains and microfracture distributions). The modelling by the different teams allowed the comparison of many different model concepts, especially in terms of potential zonations of rock properties (porosity, diffusion, sorption), such as the presence of a disturbed zone at the rock and fracture surface, the potential effects of micro- and cm-scale fractures.

JAEA Reports

Mesh effect around burnable poison rod of cell model for HTTR fuel block

Fujimoto, Nozomu*; Fukuda, Kodai*; Honda, Yuki*; Tochio, Daisuke; Ho, H. Q.; Nagasumi, Satoru; Ishii, Toshiaki; Hamamoto, Shimpei; Nakano, Yumi*; Ishitsuka, Etsuo

JAEA-Technology 2021-008, 23 Pages, 2021/06


The effect of mesh division around the burnable poison rod on the burnup calculation of the HTTR core was investigated using the SRAC code system. As a result, the mesh division inside the burnable poison rod does not have a large effect on the burnup calculation, and the effective multiplication factor is closer to the measured value than the conventional calculation by dividing the graphite region around the burnable poison rod into a mesh. It became clear that the mesh division of the graphite region around the burnable poison rod is important for more appropriately evaluating the burnup behavior of the HTTR core..

Journal Articles

Development of evaluation method for diffusion and filtration behavior of colloid in compacted bentonites using dendrimers

Endo, Takashi*; Tachi, Yukio; Ishidera, Takamitsu; Terashima, Motoki

Nihon Genshiryoku Gakkai Wabun Rombunshi, 20(1), p.9 - 22, 2021/03

Evaluation method of colloid diffusion and filtration in compacted bentonites was developed using dendrimers. Diffusion and filtration behavior of PAMAM dendrimers with the size of 5.7$$sim$$7.2nm was investigated by the through-diffusion experiment in bentonite compacted to 0.8 Mg/m$$^{3}$$ and saturated with 0.005$$sim$$0.5mol/L NaCl. Effective diffusivities (De) and filtration ratios (Rf) of dendrimers were determined from the breakthrough curves and the depth profiles in compacted bentonite, respectively. The De values of negatively charged dendrimer increased when porewater salinity increased and dendrimer size decreased as influenced by anion exclusion effect in negatively charged clay surfaces. The Rf values increased when porewater salinity decreased and dendrimer size increased, demonstrating significant fractions of dendrimer were filtered by narrow pores in complex pore networks. These trends consistent with the previous studies emphasize the validity of the evaluation method using dendrimer.

Journal Articles

Online measurement of the atmosphere around geopolymers under gamma irradiation

Cantarel, V.; Lambertin, D.*; Labed, V.*; Yamagishi, Isao

Journal of Nuclear Science and Technology, 58(1), p.62 - 71, 2021/01

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

The gas production of wasteforms is a major safety concern for encapsulating active nuclear wastes. For geopolymers and cements, the H$$_{2}$$ produced by radiolytic processes is a key factor because of the large amount of water present in their porous structure. Herein, the gas composition evolution around geopolymers was monitored on line under $$^{60}$$Co gamma irradiation. Transient evolution of the hydrogen production yield was measured for samples with different formulations. The rate of its evolution and the final values are consistent with the presence of a chemical reaction of the pseudo-first order consuming hydrogen in the samples. The results show this phenomenon can significantly reduce the hydrogen source term of geopolymer wasteform provided their diffusion constant remains low. Lower hydrogen production rates and faster kinetics were observed with geopolymers formulations in which pore water pH was higher. Besides hydrogen production, a steady oxygen consumption was observed for all geopolymers samples. The oxygen consumption rates are proportional to the diffusion constants estimated in the modelization of hydrogen recombination by a pseudo first order reaction.

Journal Articles

Extraction mechanism of lanthanide ions into silica-based microparticles studied by single microparticle manipulation and microspectroscopy

Otaka, Toshiki*; Sato, Tatsumi*; Ono, Shimpei; Nagoshi, Kohei; Abe, Ryoji*; Arai, Tsuyoshi*; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Nakatani, Kiyoharu*

Analytical Sciences, 35(10), p.1129 - 1133, 2019/10

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

Journal Articles

Optimum temperature for HIP bonding invar alloy and stainless steel

Wakui, Takashi; Ishii, Hideaki*; Naoe, Takashi; Kogawa, Hiroyuki; Haga, Katsuhiro; Wakai, Eiichi; Takada, Hiroshi; Futakawa, Masatoshi

Materials Transactions, 60(6), p.1026 - 1033, 2019/06

 Times Cited Count:1 Percentile:13.55(Materials Science, Multidisciplinary)

The mercury target has large size as 1.3$$times$$1.3$$times$$2.5 m$$^{3}$$. In view of reducing the amount of wastes, we studied the structure so that the fore part could be separated. The flange is required to have high seal performance less than 1$$times$$10$$^{-6}$$ Pa m$$^{3}$$/s. Invar with low thermal expansion is a candidate. Due to its low stiffness, however, the flange may deform when it is fastened by bolts. Practically invar is reinforced with stainless steel where all interface between them has to be bonded completely with the HIP bonding. In this study, we made specimens at four temperatures and conducted tensile tests. The specimen bonded at 973 K had little diffusion layer, and so fractured at the interface. The tensile strength reduced with increasing the temperature, and the reduced amount was about 10% at 1473 K. The analyzed residual stresses near the interface increased by 50% at maximum. Then, we concluded that the optimum temperature was 1173 K.

Journal Articles

A Systematic radionuclide migration parameter setting approach for potential siting environments in Japan

Hamamoto, Takafumi*; Ishida, Keisuke*; Shibutani, Sanae*; Fujisaki, Kiyoshi*; Tachi, Yukio; Ishiguro, Katsuhiko*; McKinley, I. G.*

Proceedings of 2019 International High-Level Radioactive Waste Management Conference (IHLRWM 2019) (USB Flash Drive), p.77 - 82, 2019/04

Journal Articles

3D-microstructure analysis of compacted Na- and Cs-montmorillonites with nanofocus X-ray computed tomography and correlation with macroscopic transport properties

Takahashi, Hiroaki*; Tachi, Yukio

Applied Clay Science, 168, p.211 - 222, 2019/02

 Times Cited Count:8 Percentile:70.54(Chemistry, Physical)

Microstructural and mass transport properties of compacted Na- and Cs-montmorillonites with different swelling properties were investigated by combining 3D microstructure analysis using nanofocus X-ray CT and diffusion measurement of HDO. The X-ray CT observations indicated that macropores in the dry state of compacted Na-montmorillonite are filled with gel phases, and the grain sizes of clay particles shifted toward smaller values through the saturation and swelling processes. By contrast, no gel phase and no decrease in the grain and pore volumes were observed for saturated Cs-montmorillonite. The geometrical factors of the macropores including tortuosity and geometric constrictivity of saturated Cs-montmorillonite determined by the X-ray CT was consistent with the corresponding values derived in the HDO diffusion test. In the case of Na-montmorillonite, the larger differences between the geometric factors evaluated by the X-ray CT and the diffusion tests can be explained by the electrostatic constrictivity factor and the additional geometrical factors in gel phase and interlayer that are smaller than the detection limit of the X-ray CT.

Journal Articles

Dynamic accommodation of internal stress and selection of crystallographic orientation relationship in pearlite

Amemiya, Yutaro*; Nakada, Nobuo*; Morooka, Satoshi; Kosaka, Makoto*; Kato, Masaharu*

Tetsu To Hagane, 105(2), p.314 - 323, 2019/02

 Times Cited Count:3 Percentile:37.05(Metallurgy & Metallurgical Engineering)

For deeper understanding of a dynamic accommodation mechanism of internal stress in pearlite originated from the lattice misfit between ferrite and cementite phases, the lattice parameter ratios of cementite were locally analyzed in detail by using the electron backscatter diffraction (EBSD) technique. The EBSD analysis has revealed that lattice parameter ratios of cementite lamellae obviously differ from those of spheroidized cementite particles, which demonstrates that pearlite has a certain amount of internal stress as long as it maintains lamellar structure. The internal stress in pearlite gradually decreased during isothermal holding at 923 K after pearlitic transformation due to interfacial atomic diffusion of iron atoms. However, comparing with theoretical values under Pitsch-Petch orientation relationship, it was understood that large amount of internal stress had been already accommodated upon pearlitic transformation by introduction of misfit dislocations and structural ledges on ferrite/cementite lamellar interfaces. That is, the internal stress of pearlite is dynamically reduced by two different processes; built-in accommodation upon pearlitic transformation and additional time-dependent relaxation after pearlitic transformation. On the other hand, EBSD analysis and neutron diffraction technique gave remarkably different lattice parameters of cementite. From this result, it is concluded that various crystallographic orientation relationships between ferrite and cementite coexist in pearlite. Furthermore, elastic strain energy analysis suggests that the invariant-line criterion on ferrite/cementite interface plays an important role for the selection of orientation relationships in pearlite.

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.

Journal Articles

Molecular dynamics simulations of physical properties of water and cations in montmorillonite interlayer; Application to diffusion model

Yotsuji, Kenji*; Tachi, Yukio; Kawamura, Katsuyuki*; Arima, Tatsumi*; Sakuma, Hiroshi*

Nendo Kagaku, 58(1), p.8 - 25, 2019/00

Molecular dynamics (MD) simulations were conducted to investigate physical properties of water and cations in montmorillonite interlayer nanopores. The swelling behaviors and hydration states were firstly evaluated as functions of interlayer cations and layer charge. The diffusion coefficients of water and cations in interlayer nanopores were decreased in comparison with those in bulk water and came closer to those in bulk water when basal spacing increased. The viscosity coefficients of interlayer water estimated indicated a significant effect of viscoelectricity at 1- and 2-layer hydration states and higher layer charge of montmorillonite. These trends from MD calculations were confirmed to be consistent with existing measured data and previous MD simulation. In addition, model and parameter related to viscoelectric effect used in the diffusion model was refined based on comparative discussion between MD simulations and measurements. The series of MD calculations could provide atomic level understanding for the developments and improvements of the diffusion model for compacted montmorillonite.

Journal Articles

Diffusion and sorption behavior of HTO, Cs, I and U in mortar

Akagi, Yosuke*; Kato, Hiroyasu*; Tachi, Yukio; Sakamoto, Hiroyuki*

Progress in Nuclear Science and Technology (Internet), 5, p.233 - 236, 2018/11

A large amount of radioactive contaminated concrete will be generated from the decommissioning in the Fukushima Dai-ichi Nuclear Power Plant (NPP). For developing the plans of decommissioning and waste management including decontamination and disposal, it is important to estimate radionuclides inventory and concentration distribution in the concrete materials. In this study, effective diffusivities (De) and distribution coefficients (Kd) of HTO, Cs, I and U in OPC mortar were measured by through-diffusion and batch sorption experiments. De values derived were in the sequence of HTO, I, Cs, U, implying that cation exclusion effects may be important mechanisms in OPC mortar. Kd values derived by batch tests were higher by more than one order of magnitude than the diffusion-derived Kd values, indicating that crushing of samples had a strong influence on sorption. Diffusion and sorption mechanisms in OPC mortar were evaluated to predict the penetration behavior of these radionuclides.

Journal Articles

Effects of fine-scale surface alterations on tracer retention in a fractured crystalline rock from the Grimsel Test Site

Tachi, Yukio; Ito, Tsuyoshi*; Akagi, Yosuke*; Sato, Hisao*; Martin, A. J.*

Water Resources Research, 54(11), p.9287 - 9305, 2018/11

 Times Cited Count:4 Percentile:37.78(Environmental Sciences)

Effects of fine-scale surface alterations on radionuclide migration in fractured crystalline rocks were investigated by a comprehensive approach coupling a series of laboratory tests, microscopic observations and modelling, using a single fractured granodiorite sample from the Grimsel Test Site, Switzerland. Laboratory tests including through-diffusion, batch sorption and flow-through tests using five tracers indicated that tracer retention was consistently in the sequence of HDO, Se, Cs, Ni, Eu, and as well as showing the existence of a diffusion-resistance layer near the fracture surface, cation excess and anion exclusion effects for diffusion. Microscale heterogeneities in structural properties around the fracture were clarified quantitatively by coupling X-ray CT and EPMA. A three layer model including weathered vermiculite, foliated mica and undisturbed matrix layers, and their properties such as porosity, sorption and diffusion parameters, could provide a reasonable interpretation for breakthrough curves and concentration distributions near fracture surface of all tracers, measured in flow-through tests.

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