Endo, Takashi*; Tachi, Yukio; Ishidera, Takamitsu; Terashima, Motoki
Nippon 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 5.77.2nm was investigated by the through-diffusion experiment in bentonite compacted to 0.8 Mg/m and saturated with 0.0050.5mol/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.
Cantarel, V.; Lambertin, D.*; Labed, V.*; Yamagishi, Isao
Journal of Nuclear Science and Technology, 58(1), p.62 - 71, 2021/01
The gas production of wasteforms is a major safety concern for encapsulating active nuclear wastes. For geopolymers and cements, the H 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 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.
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
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
The mercury target has large size as 18.104.22.168 m. 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 110 Pa m/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.
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
Takahashi, Hiroaki*; Tachi, Yukio
Applied Clay Science, 168, p.211 - 222, 2019/02
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.
Amemiya, Yutaro*; Nakada, Nobuo*; Morooka, Satoshi; Kosaka, Makoto*; Kato, Masaharu*
Tetsu To Hagane, 105(2), p.314 - 323, 2019/02
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.
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.
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.
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.
Tachi, Yukio; Ito, Tsuyoshi*; Akagi, Yosuke*; Sato, Hisao*; Martin, A. J.*
Water Resources Research, 54(11), p.9287 - 9305, 2018/11
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.
Yamamoto, Masahiro; Sato, Tomonori; Igarashi, Takahiro; Ueno, Fumiyoshi; Soma, Yasutaka
Proceedings of European Corrosion Congress 2017 (EUROCORR 2017) and 20th ICC & Process Safety Congress 2017 (USB Flash Drive), 6 Pages, 2018/09
The authors have studied the differences between outer surface and the crevice-like portion of SUS316L in high pressurized and high temperature water containing dissolved oxygen. We have already introduced that changes in the characteristics of corrosion products along the crevice directions and gap width. It is suggested that the environmental conditions are different with the features of crevice from these results. In this report, we introduce the changes in oxide films with crevice gaps and comparison with the numerical simulation data utilizing of FEM calculation.
Kawaguchi, Munemichi; Miyahara, Shinya; Uno, Masayoshi*
Journal of Nuclear Science and Technology, 55(8), p.874 - 884, 2018/08
As parts of severe accident studies in sodium-cooled fast reactor, experiments were performed to investigate the termination mechanism of sodium-concrete reaction (SCR). In the experiment, the reaction time was controlled to investigate the distribution change of sodium (Na) and the reaction products in the pool and around the reaction front. In the results, the Na around the reaction front decreased from the enough amount with the reaction time. The concentrations were 18-24 wt.% for Na, and 22-18 wt.% for Si after the termination. From the thermodynamics calculations, the stable materials around the reaction front comprised more than 90 wt.% solid products such as NaSiO, and no Na. Further, the distribution of Na and reaction products could be explained by a steady-state sedimentation-diffusion model. At the early stage of SCR, the reaction products were suspended as particles in the Na pool because of the high H-generation rate. As the concrete ablation proceeds, they start settling down due to the decreased H-generation rate, thereby allowing SCR termination. It was concluded that SCR termination was caused by the sediment of the reaction products and the lack of Na around the reaction front.
Shudo, Yasuyuki*; Izumi, Atsushi*; Hagita, Katsumi*; Yamada, Takeshi*; Shibata, Kaoru; Shibayama, Mitsuhiro*
Macromolecules, 51(16), p.6334 - 6343, 2018/08
Haga, Katsuhiro; Kogawa, Hiroyuki; Wakui, Takashi; Naoe, Takashi; Takada, Hiroshi
Journal of Nuclear Science and Technology, 55(2), p.160 - 168, 2018/02
The mercury target vessel used for the spallation neutron source in J-PARC has multi-walled structure made of stainless steel type 316L, which comprises a mercury vessel and a water shroud. In 2015, water leak incidents from the water shroud occurred while the mercury target was operated with a proton beam power of 500 kW. Several investigations were conducted to identify the cause of failure. The results of the visual inspections, mockup tests, and analytical evaluations suggested that the water leak was caused by the combination of two factors. One was the diffusion bonding failure due to the large thermal stress induced by welding of the bolt head, which fixes the mercury vessel and the water shroud, during the fabrication process. The other was the thermal fatigue failure of the seal weld due to the repetitive beam trip during the operating period. These target failures point to the importance of eliminating initial defects from welding lines and to secure the rigidity and reliability of welded structures. The next mercury target was fabricated with an improved design which adopted parts of monolithic structure machined by wire EDM to reduce welding lines, and intensified inspections to eliminate the initial defects. The operation with the improved target is planned to be started in October 2017.
Hamamoto, Takafumi*; Shibutani, Sanae*; Ishida, Keisuke*; Fujisaki, Kiyoshi*; Yamada, Motoyuki*; Tachi, Yukio
Proceedings of 6th East Asia Forum on Radwaste Management Conference (EAFORM 2017) (Internet), 6 Pages, 2017/12
NUMO has developed a generic safety case to demonstrate the feasibility and safety of geological disposal of HLW and TRU in Japan and to provide a basic structure for the safety case which will be applicable to any potential site. In this safety case, the safety assessment was carried out for the repositories tailored to site descriptive models developed for three representative rock groups (plutonic, Neogene sedimentary and Pre-Neogene sedimentary rocks). Radionuclide migration parameters in rocks, i.e. distribution coefficients (Kds) and effective diffusion coefficients (Des), were derived to allow safety analysis for a range of scenarios. In this generic stage, the values of these parameter were given as the statistical values derived from laboratory data for certain rock types. The data were extracted from the latest database, with interpretation based on radionuclide speciation derived from relevant groundwater thermodynamic modelings.
Arima, Tatsumi*; Idemitsu, Kazuya*; Inagaki, Yaohiro*; Kawamura, Katsuyuki*; Tachi, Yukio; Yotsuji, Kenji
Progress in Nuclear Energy, 92, p.286 - 297, 2016/09
Diffusion and adsorption behavior of uranyl (UO) species is important for the performance assessment of radioactive waste disposal. The diffusion behaviors of UO, K, CO and Cl and HO in the aqueous solutions were evaluated by molecular dynamics (MD) calculations. The diffusion coefficient (De) of UO is the smallest and is 26% less than the self-diffusion coefficient of HO. For the aqueous solution with high concentration of carbonate ions, uranyl carbonate complexes: UOCO and UO(CO) can be observed. For the clay (montmorillonite or illite)-aqueous solution systems, the adsorption and diffusion behaviors of UO and K were evaluated by MD calculations. The distribution coefficients (Kd) increase with the layer charge of clay, and Kd of UO might be smaller than that of K. Further, their two-dimensional diffusion coefficients were relatively small in the adsorption layer and were extremely small for illite with higher layer charge.
Yotsuji, Kenji; Tachi, Yukio; Okubo, Takahiro*
CMS Workshop Lectures, Vol.21, p.251 - 257, 2016/06
We have developed integrated sorption and diffusion model (ISD model) for assessment of diffusion parameters consistent with sorption processes in compacted bentonite. The ISD model gives consistent consideration to porewater chemistry, sorption and diffusion processes in compacted bentonite. The diffusion component based on the electric double layer theory and the homogeneous pore model in the ISD model accounts consistently for cation De overestimation and anion exclusion in narrow pores. The current ISD model can quantitatively account for diffusion of monovalent cations and anions, however, the model predictions disagree with diffusion data for multivalent cation and complex species. To improve the applicability of the model, it is necessary to consider the atomic level interactions between solute, solvent or clay mineral, and try that we apply the current ISD model to heterogeneous pore structure. In this study we try the application of the current ISD model to multiple pore structure. As results of numerical analysis of these models, the salinity dependence of effective diffusivity for the multi-pore model is comparatively smaller than that for the homogeneous pore model and the current diffusion model is improved.
Aihara, Jun; Ueta, Shohei; Nishihara, Tetsuo
JAEA-Technology 2015-040, 32 Pages, 2016/02
Original FORNAX-A is a calculation code for amount of fission product (FP) released from fuel rods of pin-in-type high temperature gas-cooled reactors (HTGRs). This report is for explanation what calculations become possible with minor changed FORNAX-A.
Tachi, Yukio; Suyama, Tadahiro; Yotsuji, Kenji; Ishii, Yasuo; Takahashi, Hiroaki*
CMS Workshop Lectures, Vol.21, p.241 - 250, 2016/00
Sorption and diffusion of radionuclides in argillaceous rocks are key processes in the safe geological disposal. The diffusion and sorption behavior of Ni(II), Am(III) and Se(IV) in mudstone from the Horonobe URL were investigated by experimental and modeling approaches. Effective diffusivities obtained by the through-diffusion experiments were in the sequence of Cs, Ni, HTO, I, Se(SeO), Am(Am(CO)) by comparison with the previous study. The distribution coefficient values were consistent with those obtained by batch sorption tests. These results were interpreted by the clay-based modeling approach coupling the thermodynamic sorption model assuming key contributions of clays (smectite and illite) and the diffusion model assuming the electrical double layer theory and the simplified pore model with size distribution. This clay-based model could provide reasonable account of observed trends and could be basically applicable for various radionuclides.