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Journal Articles

Thermodynamic interpretation of uranium(IV/VI) solubility in the presence of $$alpha$$-isosaccharinic acid

Kobayashi, Taishi*; Sasaki, Takayuki*; Kitamura, Akira

Journal of Chemical Thermodynamics, 138, p.151 - 158, 2019/11

The effect of $$alpha$$-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$$_{c}$$) range of 6$$sim$$13 and at total ISA concentration ([ISA]$$_{rm tot}$$) = 10$$^{-4}$$$$sim$$10$$^{-1.2}$$ mol/dm$$^{3}$$. The dependence of U(IV) solubility on pH$$_{c}$$ and [ISA]$$_{rm tot}$$ suggested the existence of U(OH)$$_{4}$$(ISA)$$_{2}$$$$^{2-}$$ as a dominant species within the investigated pH$$_{c}$$ range of 6$$sim$$12. For the U(VI)-ISA system, UO$$_{2}$$(OH)$$_{3}$$(ISA)$$_{2}$$$$^{2-}$$ was suggested as a dominant species at pH$$_{c}$$ 7$$sim$$13. 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.

Journal Articles

Development of phosphate modified CAC cementitious systems with reduced water content for the immobilization of radioactive wastes

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 (35$$^{circ}$$C, 60$$^{circ}$$C, 95$$^{circ}$$C, 110$$^{circ}$$C,180$$^{circ}$$C) 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 95$$^{circ}$$C.

Journal Articles

Apparent diffusion coefficients of Cs and I in hardened cement paste using mineral admixtures

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$$_{a}$$) of Cs and I in HCPs were obtained using electron probe microanalysis. For Cs, BFS and SF contributed to a reduction of D$$_{a}$$ for W/C=50% and 30%, respectively. For I, BFS reduced D$$_{a}$$ for W/C=50%, however a significant reduction in D$$_{a}$$ 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$$_{a}$$ in HCP.

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

Hydrogen gas measurements of phosphate cement irradiated during heat treatment

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

Journal Articles

Micro-PIXE analysis study of ferrite products synthesized from simulated radioactive liquid waste containing chemical hazardous elements

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

Journal Articles

Assessment of the potential for criticality in the far field of a used nuclear fuel repository

Atz, M.*; Salazar, A.*; Hirano, Fumio; Fratoni, M.*; Ahn, J.*

Annals of Nuclear Energy, 124, p.28 - 38, 2019/02

 Percentile:100(Nuclear Science & Technology)

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.

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

 Percentile:100(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

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

Conceptual uncertainties in modelling the interaction between engineered and natural barriers of nuclear waste repositories in crystalline rocks

Finsterle, S.*; Lanyon, B.*; ${AA}$kesson, M.*; Baxter, S.*; Bergstr$"o$m, M.*; Bockg${aa}$rd, N.*; Dershowitz, W.*; Dessirier, B.*; Frampton, A.*; Fransson, ${AA}$.*; 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 $"A$ps$"o$ 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.

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

Development of evaluation technique for long-term mechanical behavior of near-field

Takayama, Yusuke

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.

Journal Articles

New insights into the Cs adsorption on montmorillonite clay from $$^{133}$$Cs solid-state NMR and density functional theory calculations

Okubo, Takahiro*; Okamoto, Takuya*; Kawamura, Katsuyuki*; Gu$'e$gan, R.*; Deguchi, Kenzo*; Oki, Shinobu*; Shimizu, Tadashi*; Tachi, Yukio; Iwadate, Yasuhiko*

Journal of Physical Chemistry A, 122(48), p.9326 - 9337, 2018/12

 Percentile:100(Chemistry, Physical)

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.

Journal Articles

Electrochemical measurements in various environments; Corrosion monitoring of carbon steel in deep underground environment

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.

Journal Articles

Application of phosphate modified CAC for incorporation of simulated secondary aqueous wastes in Fukushima Daiichi NPP, 1; Characterization of solidified cementitious systems with reduced water content

Garcia-Lodeiro, I.*; Lebon, R.*; Machoney, D.*; Zhang, B.*; Irisawa, Keita; Taniguchi, Takumi; Namiki, Masahiro*; Osugi, Takeshi; Meguro, Yoshihiro; Kinoshita, Hajime*

Proceedings of 3rd International Symposium on Cement-based Materials for Nuclear Wastes (NUWCEM 2018) (USB Flash Drive), 4 Pages, 2018/11

Journal Articles

Thermodynamic data development; Solubility method and future research needs (PLENARY)

Rai, D.*; Yui, Mikazu; Kitamura, Akira

Progress in Nuclear Science and Technology (Internet), 5, p.19 - 26, 2018/11

The objectives of this presentation are (1) to describe the solubility method, (2) to list desirable criteria of the solubility method so that the reader can recognize which studies have been done in a way that yields quality information, (3) to present an example of how to use the evaluation criteria, and (4) to provide a few examples of future research needs where the solubility method is ideally suited and the other methods are unsuitable for these investigations.

Journal Articles

Sorption parameter setting approaches for radioactive waste disposal considering perturbation effects; Sorption reduction factors for organics

Tachi, Yukio; Ochs, M.*

Progress in Nuclear Science and Technology (Internet), 5, p.229 - 232, 2018/11

Various types of post-accident radioactive waste have been generated from cleanup and decommissioning activities at the Fukushima Daiichi Nuclear Power Plant. For the disposal of these wastes, perturbation effects resulting from co-existing substances (e.g., organic substances, boron, and salts) are needed to be considered. Such co-existing substances may influence on the radionuclide sorption parameters for the safety assessment of the disposal systems. The present study focuses on developing the methodology to quantify sorption parameters by considering such perturbation effects and illustrating example calculations regarding the sorption reduction factors (SRFs) due to the presence of organic ligands (ISA) for cement systems. Three approaches for the derivations of SRFs for cement-Am-ISA case were compared. These options should be applied as a stepwise manner according to the data availability for the perturbation effects resulting from the co-existing substances.

Journal Articles

Retention of uranium in cement systems; Effects of cement degradation and complexing ligands

Ochs, M.*; Vriens, B.*; Tachi, Yukio

Progress in Nuclear Science and Technology (Internet), 5, p.208 - 212, 2018/11

The clean-up activities related to the accident at the Fukushima Nuclear Power Plant give rise to several types of wastes containing cementitious materials, such as concrete. Further, the use of cement-based barriers may be considered, due to their favorable and stable chemical properties, including their ability to sorb or incorporate radionuclides. Wastes from Fukushima are expected to contain substances that can have perturbing effects on retention, especially organic complexing substances, boron, and chloride salts. The present study focuses on a methodology for quantifying the retention behaviour of UVI) and U(IV) in cement materials of different degradation and in the presence of organics, boron, and salts on the basis of available literature information. A stepwise approach is proposed and illustrated for Kd setting for U(VI) and U(IV).

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

 Percentile:100(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.

764 (Records 1-20 displayed on this page)