Sugiura, Yuki; Tomura, Tsutomu*; Ishidera, Takamitsu; Doi, Reisuke; Francisco, P. C. M.; Shiwaku, Hideaki; Kobayashi, Toru; Matsumura, Daiju; Takahashi, Yoshio*; Tachi, Yukio
Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05
Terashima, Motoki; Endo, Takashi*; Miyakawa, Kazuya
Journal of Nuclear Science and Technology, 57(4), p.380 - 387, 2020/04
Tachi, Yukio; Suyama, Tadahiro*; Mihara, Morihiro
JAEA-Data/Code 2019-021, 101 Pages, 2020/03
Sorption of radionuclides in cement and bentonite as engineered barrier materials, and rocks as natural barrier is the one of key processes in the performance assessment of geological disposal of TRU and highlevel waste. The magnitude of sorption, expressed normally by a distribution coefficient (K), needs to be measured and determined taking into account the properties of barrier materials and geochemical conditions and associated uncertainty in the performance assessment. The basic concept for TRU waste disposal contains cementitious materials as an engineered barrier materials, in addition to bentonite and rock. It is therefore needed to consider the effects of the cement degradation and co-existing substances such as nitrates on radionuclide sorption. This report focused on data acquisition of distribution coefficient (K) by batch sorption experiments for the systems coupling barrier material-chemical condition-radionuclides that are needed to consider for the performance assessment of geological disposal of TRU waste. The barrier materials considered are ordinary Portland cement (OPC), degraded OPC and tuff rock. The chemical conditions are distilled water and synthetic seawater equilibrated with OPC and those containing nitrates and ammonium salts, etc. The radionuclides considered are organic carbon, inorganic carbon, Cl, I, Cs, Ni, Se, Sr, Sn, Nb, Am and Th. Although K values have been partly reported previously as RAMDA (Radionucldie Migration Datasets) for the performance assessment in the TRU-2 report, these results and addition K data are reported with the details of experimental methods and conditions.
Sato, Junya; Shiota, Kenji*; Takaoka, Masaki*
Journal of Hazardous Materials, 385, p.121109_1 - 121109_9, 2020/03
Lead is a hazardous heavy metal that can be stabilized by incorporation into the matrix of aluminosilicate bearing phases as they solidify. The actual mechanism by which lead is stabilized, however, continues to be unclear because the individual mechanisms of Pb incorporation into crystalline and amorphous aluminosilicate phases have not yet been studied separately. A detailed investigation of the incorporation of Pb into the amorphous phase of aluminosilicate solids was therefore performed. Amorphous aluminosilicate solids were synthesized with 0.7, 1.5, and 3.7 wt% of Pb from aluminosilicate gel produced from chemical reagents. Based on Raman spectroscopy, the Si-O stretching vibration bond shifted to lower wavenumbers with increasing Pb concentration. This shift suggested that covalent bonding between Pb and O in the matrix of the aluminosilicate solids increased. In addition, sequential extraction revealed that most of the Pb (75-90%) in the aluminosilicate solids was in a poorly soluble form (i.e. reducible, oxidizable, and residual fractions). These findings indicate that most of Pb is bonded covalently to the amorphous phase in aluminosilicate solids.
Francisco, P. C. M.; Mitsui, Seiichiro; Ishidera, Takamitsu; Tachi, Yukio; Doi, Reisuke; Shiwaku, Hideaki
Geochimica et Cosmochimica Acta, 270, p.1 - 20, 2020/02
Geological Disposal Research and Development Department
JAEA-Evaluation 2019-010, 69 Pages, 2020/01
Japan Atomic Energy Agency (JAEA) consulted the advisory committee, "Evaluation Committee on Research and Development (R&D) Activities for Geological Disposal of High-Level Radioactive Waste", for an interim review of R&D activities on high-level radioactive waste disposal in accordance with "General Guideline for the Evaluation of Government Research and Development (R&D) Activities" by the Cabinet Office, Government of Japan, "Guideline for Evaluation of R&D in Ministry of Education, Culture, Sports, Science and Technology" and JAEA's "Regulation on Conduct for Evaluation of R&D Activities". In response to JAEA's request, the Committee reviewed mainly the progress of the R&D project on geological disposal, the relevance of the project outcome during the period of FY2015-2018. This report summarizes the results of the assessment by the Committee with the Committee report attached.
Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira
Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11
The effect of -isosaccharinic acid (ISA) on the solubility and redox of tetravalent and hexavalent uranium (U(IV), U(VI)) was investigated in the hydrogen ion concentration (pH) range of 613 and at total ISA concentration ([ISA]) = 1010 mol/dm. The dependence of U(IV) solubility on pH and [ISA] suggested the existence of U(OH)(ISA) as a dominant species within the investigated pH range of 612. For the U(VI)-ISA system, UO(OH)(ISA) was suggested as a dominant species at pH 713. The formation constants of the U(IV)-ISA and U(VI)-ISA complexes were determined by least-squares fitting of the solubility data. The solubility of U(IV) and U(VI) in the presence of ISA and its effect on the redox behavior were thermodynamically interpreted based on the obtained constants.
Garcia-Lodeiro, I.*; Irisawa, Keita; Meguro, Yoshihiro; Kinoshita, Hajime*
Proceedings of 15th International Congress on the Chemistry of Cement (ICCC 2019) (Internet), 10 Pages, 2019/09
The immobilization of low or intermediate-level radioactive wastes in cements is a common practise. Grout, a mixture of Portland cement and supplemental cementitious materials, is commonly used to encapsulate the wastes. However, the conventional cementing process based on portland cement has the risk of hydrogen gas generation, due to the radiolysis of the water intrinsically present in the cement matrix both in the pore solution and the hydrated products. The addition of phosphates to calcium aluminate cement (CAC) is interesting because this system sets and hardens via the acid-based reaction, between the acid phosphate solution and the basic CAC cement. Due to this different mechanism of reaction, it would be possible to generate a solid cementitious product with a reduced water content, which can be beneficial to minimize the risk of hydrogen gas generation associated with the radiolysis of water by radioactive wastes. The present study investigates the effect of water reduction on a phosphate modified CAC systems at different temperatures (35C, 60C, 95C, 110C,180C) in the initial 7 days of curing. Experimental results indicate that these phosphate-based cements do not form the conventional CAC crystalline hydration products in the condition tested, but provide a structural integrity despite a significant amount of water loss. The results also suggest the formation of hydroxyapatite in samples cured at 95C.
Mihara, Morihiro; Harasawa, Shuichi*; Torii, Kazuyuki*
Genshiryoku Bakkuendo Kenkyu (CD-ROM), 26(1), p.15 - 23, 2019/06
Hardened cement pastes (HCPs) of water/cement ratio (W/C) 50% and 30% using fly ash (FA), blast furnace slag (BFS) and silica fume (SF) for 28 days were prepared. Apparent diffusion coefficients (D) of Cs and I in HCPs were obtained using electron probe microanalysis. For Cs, BFS and SF contributed to a reduction of D for W/C=50% and 30%, respectively. For I, BFS reduced D for W/C=50%, however a significant reduction in D for W/C=30% was not observed. Using SF enhanced sorption of Cs on HCP, and using BFS slightly improved sorption of Cs on HCP. It was also confirmed that the pore structures of HCP using SF and BFS were connected by fine pores. It was therefore considered that using SF and BFS contributes to the reduction of D in HCP.
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
Irisawa, Keita; Kudo, Isamu*; Taniguchi, Takumi; Namiki, Masahiro*; Osugi, Takeshi; Nakazawa, Osamu
QST-M-16; QST Takasaki Annual Report 2017, P. 63, 2019/03
no abstracts in English
Abe, Tomohisa; Shimazaki, Takejiro; Osugi, Takeshi; Nakazawa, Osamu; Yamada, Naoto*; Yuri, Yosuke*; Sato, Takahiro*
QST-M-16; QST Takasaki Annual Report 2017, P. 140, 2019/03
no abstracts in English
Atz, M.*; Salazar, A.*; Hirano, Fumio; Fratoni, M.*; Ahn, J.*
Annals of Nuclear Energy, 124, p.28 - 38, 2019/02
The likelihood for criticality in the far field of a repository was evaluated for direct disposal of commercial light water reactor used nuclear fuel. Two models were used in combination for this evaluation: (1) a neutronics model to estimate the minimum critical masses of spherical, water-saturated depositions of fuel material; (2) a transport model to simulate the dissolution of fuel material from multiple canisters and the subsequent transport of the solutes through host rock to a single accumulation location. The results suggest that accumulation of a critical mass is possible under conservative conditions but that these conditions are unlikely to occur, especially in the vicinity of a carefully-arranged repository.
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.
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.
Finsterle, S.*; Lanyon, B.*; kesson, M.*; Baxter, S.*; Bergstrm, M.*; Bockgrd, N.*; Dershowitz, W.*; Dessirier, B.*; Frampton, A.*; Fransson, .*; et al.
Geological Society, London, Special Publications, No.482, p.261 - 283, 2019/00
Nuclear waste disposal in geological formations relies on a multi-barrier concept that includes engineered components which in many cases includes a bentonite buffer surrounding waste packages and the host rock. An SKB's (Swedish Nuclear Fuel and Waste Management Co.) Modelling Task Force project facilitated to improve the overall understanding of rock - bentonite interactions, as 11 teams used different conceptualisations and modelling tools to analyse the in-situ experiment at the ps Hard Rock Laboratory. The exercise helped identify conceptual uncertainties that led to different assessments of the relative importance of the engineered and natural barrier subsystems and of aspects that need to be better understood to arrive at reliable predictions of bentonite wetting.
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.
Genshiryoku Bakkuendo Kenkyu (CD-ROM), 25(2), p.103 - 106, 2018/12
At the 34th Back-end Summer Seminar, I introduce the evaluation technique for long-term mechanical behavior of near field. This report summarizes the presentation at the seminar.
Okubo, Takahiro*; Okamoto, Takuya*; Kawamura, Katsuyuki*; Gugan, R.*; Deguchi, Kenzo*; Oki, Shinobu*; Shimizu, Tadashi*; Tachi, Yukio; Iwadate, Yasuhiko*
Journal of Physical Chemistry A, 122(48), p.9326 - 9337, 2018/12
The structures of Cs adsorption on montmorillonite were investigated by the nuclear magnetic resonance (NMR) spectroscopy. The NMR spectra of Cs adsorbed on montmorillonite samples were measured under different Cs contents and relative humidity levels. NMR parameters were evaluated by the first principle calculations in order to identify the relationship between adsorbed Cs structures and NMR parameters. The comparisons between experimental and theoretical NMR spectra revealed that Cs is preferentially adsorbed at sites near Al for low Cs substituted montmorillonites, and that non-hydrated Cs present in partially Cs substituted samples, even after being hydrated under high relative humidity.
Taniguchi, Naoki; Nakayama, Masashi
Zairyo To Kankyo, 67(12), p.487 - 494, 2018/12
This article describes the current status of corrosion monitoring methods and examples of the measurement under deep underground environments for carbon steel overpacks for high-level radioactive waste disposal. Based on the studies on corrosion monitoring using AC Impedance technique, some of the typical measurement systems such as the electrodes arrangement are introduced. In-situ corrosion monitoring in engineering scale test is also being attempted using a deep underground research facility, and the measurement method and results are presented in this article.