Effects of Supersaturated Silicic Acid Concentration on Deposition Rate Around Geological Disposal System

Author(s):  
Tsuyoshi Sasagawa ◽  
Taiji Chida ◽  
Yuichi Niibori

Cementitious materials for the construction of a geological repository of radioactive waste alter the pH of groundwater to a highly alkaline condition (pH ≈ 13). While this alkaline groundwater dissolves silicate minerals, the soluble silicic acid polymerizes or deposits on the surface of rock with the decrease in pH by mixing with the surrounding groundwater (pH = 8). In particular, the deposition of silicic acid leads to a clogging effect in flow-paths, which retards the migration of radionuclides. This study estimated the clogging of silicic acid in flow-paths with the one-dimensional advection–dispersion model considering the deposition rate constants evaluated in our previous study. As some of the most important parameters, these estimations focused on the initial supersaturated concentration of silicic acid and the density of deposited minerals. As a result, the aperture of flow-paths (initial width: 0.1 mm, flow-rate: 5 m/y, initial supersaturated concentration of silicic acid: 0.01, 0.1 and 1.0 mM) was almost clogged within about 200 y by the deposition of silicic acid. The period for the clogging became shorter under the conditions of higher initial supersaturated concentration and lower density of deposited minerals. In other words, the use of cementitious materials for constructing the repository might produce a retardation effect of radionuclide migration by the deposition/clogging processes of the supersaturated silicic acid.

Author(s):  
Tsuyoshi Sasagawa ◽  
Taiji Chida ◽  
Yuichi Niibori

For the disposal system of high-level radioactive waste in Japan, Na-type bentonite is used as one of backfilling and buffer materials for preventing the migration of groundwater and radionuclide. However, the alteration to Ca-type bentonite will cause the degradation of the barrier performance. On the other hand, silicate minerals around the repository dissolve under the high alkaline condition of groundwater (about pH 13) altered by alkaline components leaching from cementitious materials used for the construction of the repository. Such high-concentration silicic acid becomes supersaturated with the decrease in pH by mixing with natural downstream groundwater (pH 8) because of the change in the solubility of silicic acid. So far, the authors have examined the deposition rates of supersaturated silicic acid on Ca-type bentonite under the condition of room temperature, showing the clogging effect of flow-paths with the deposition. However, the dynamic behaviors of silicic acid are much sensitive to temperature change. Therefore, the present study focuses on the effect of temperature on the deposition rate of silicic acid on Ca-type bentonite. As a result, in the range up to 323 K, the deposition of supersaturated silicic acid on Ca-type bentonite was promoted with the increase in temperature. This suggests that the deposition of silicic acid will clog the flow-paths in Ca-type bentonite in this temperature range.


2014 ◽  
Vol 1665 ◽  
pp. 55-60
Author(s):  
Taiji Chida ◽  
Yuichi Niibori ◽  
Hayata Shinmura ◽  
Hitoshi Mimura

ABSTRACTAround the radioactive waste repository, the pH of the groundwater greatly changes from 8 to 13 and the groundwater contains a relatively large quantity of calcium (Ca) and sodium (Na) ions due to cementitious materials used for the construction of the geological disposal system. Under such conditions, the deposition behavior of silicic acid is one of the key factors for the migration assessment of radionuclides. The deposition and precipitation of silicic acid with the change of pH and coexisting ions may contribute to the clogging in flow paths, which is expected as the retardation effect of radionuclides. Thus, this study focused on the deposition behavior of silicic acid under the condition of relatively high Ca or Na concentration.In the experiments, Na2SiO3 solution (250 ml, 14 mM, pH>10, 298 K) was prepared in a polyethylene vessel containing amorphous silica powder (0.5 g) as the solid phase. Then, a buffer solution (to adjust to 8 in pH), HNO3, and Ca(NO3)2 as Ca ions or NaCl as Na ions were sequentially added. Such a silicic acid solution becomes supersaturated, gradually forming colloidal silicic-acid and/or the deposit on the solid surface. In this study, the both concentrations of soluble and colloidal silicic-acid were monitored over a 40-day period. As a result, the deposition rate of silicic acid decreased with up to 5 mM in Ca ions. Besides, Na ions with up to 0.1 M slightly increased the deposition rate. Under the conditions of [Na+]>0.1 M or [Ca2+]>5 mM, the supersaturated silicic acid immediately deposited. These suggest that Na or Ca ions strongly affect the deposition behavior of supersaturated silicic-acid, depending on the surface alteration of solid phase, the change of zeta potential and the decrease of water-activity due to the addition of electrolytes (coexisting ions).


2020 ◽  
Vol 75 (8) ◽  
pp. 713-725 ◽  
Author(s):  
Guenbo Hwang

AbstractInitial-boundary value problems for the one-dimensional linear advection–dispersion equation with decay (LAD) are studied by utilizing a unified method, known as the Fokas method. The method takes advantage of the spectral analysis of both parts of Lax pair and the global algebraic relation coupling all initial and boundary values. We present the explicit analytical solution of the LAD equation posed on the half line and a finite interval with general initial and boundary conditions. In addition, for the case of periodic boundary conditions, we show that the solution of the LAD equation is asymptotically t-periodic for large t if the Dirichlet boundary datum is periodic in t. Furthermore, it can be shown that if the Dirichlet boundary value is asymptotically periodic for large t, then so is the unknown Neumann boundary value, which is uniquely characterized in terms of the given asymptotically periodic Dirichlet boundary datum. The analytical predictions for large t are compared with numerical results showing the excellent agreement.


2018 ◽  
Vol 761 ◽  
pp. 152-158 ◽  
Author(s):  
Philip van den Heede ◽  
Bjorn van Belleghem ◽  
Maria Adelaide Araújo ◽  
João Feiteira ◽  
Nele de Belie

The service life of steel reinforced concrete in aggressive marine environments could be increased substantially by embedding a self-healing mechanism that ensures autonomous healing of cracks upon their occurrence. Previous proof-of-concept experiments have shown that the incorporation of encapsulated polymer-based healing agents (HAs) counts as a very appropriate way to achieve this goal. Over the years, several polymer-precursor-capsule systems have been developed in that perspective at our laboratory. Cementitious materials containing either commercial or in-house developed encapsulated HAs have been subjected to preliminary feasibility tests (water absorption, permeability tests, etc.). However, these experiments did not yet allow for a fast and straightforward assessment of the self-healing efficiency (SHE) in relation to the expected durability and service life performance of the material. This approach would have many advantages when having to select the most suitable polymer-precursor-capsule system for a particular concrete application. In this paper, a modified chloride migration test based on the one prescribed in NT Build 492 has been proposed to support the development of self-healing concrete for marine environments. Four polymer-based HAs have been screened that way, i.e. an in-house developed high-viscosity polyurethane (PU) precursor, a commercial low-viscosity PU precursor, the same commercial PU precursor with addition of accelerator and benzoyl peroxide (BPO), and an in-house developed 2-component acrylate-endcapped precursor + cross-linker. For now, a highly repeatable SHE value of 100% could only be obtained for the second option.


Author(s):  
Morimasa Naito ◽  
Hirokazu Kishi ◽  
Naomi Fukuoka ◽  
Tsutomu Yamada ◽  
Hideaki Ishida

As an alternative grouting material for the geological repository of long-lived radioactive waste, the “Superfine Spherical silica Grout” (SFSG) material is developed using a fine spherical silica and a fine calcium hydroxide. The developed SFSG material takes an advantage of its smaller particle size distribution (max. ∼1 micron or less) than those of the cementitious materials, and also provides a low alkaline environment so as to reduce unfavorable effects on the long-term performance of geological disposal system. The SFSG is a mixture of the “super fine silica powder”, the superfine calcium hydroxide and additives such as superplasticizer. Presently, the mixture being investigated for grouting materials is focused on water/binder ratio (W/B) of 1.2. Some preliminary laboratory experiments were carried out to characterize its fundamental properties from the viewpoint of practical use for geological disposal, which is required to be equivalent with the conventional cementitious materials in terms of penetrability, strength, pH performance and workability. From a series of experiments, it was concluded that SFSG is expected to become an alternative grouting material for a geological repository.


Water ◽  
2019 ◽  
Vol 11 (10) ◽  
pp. 2145
Author(s):  
Sokáč ◽  
Velísková ◽  
Gualtieri

Analytical solutions of the one-dimensional (1D) advection–dispersion equations, describing the substance transport in streams, are often used because of their simplicity and computational speed. Practical computations, however, clearly show the limits and the inaccuracies of this approach. These are especially visible in cases where the streams deform concentration distribution of the transported substance due to hydraulic and morphological conditions, e.g., by transient storage zones (dead zones), vegetation, and irregularities in the stream hydromorphology. In this paper, a new approach to the simulation of 1D substance transport is presented, adapted, and tested on tracer experiments available in the published research, and carried out in three small streams in Slovakia with dead zones. Evaluation of the proposed methods, based on different probability distributions, confirmed that they approximate the measured concentrations significantly better than those based upon the commonly used Gaussian distribution. Finally, an example of the application of the proposed methods to an iterative (inverse) task is presented.


Author(s):  
Nikolai Fahrmeier ◽  
Nadine Goeppert ◽  
Nico Goldscheider

AbstractSingle-borehole dilution tests (SBDTs) are a method for characterizing groundwater monitoring wells and boreholes, and are based on the injection of a tracer into the saturated zone and the observation of concentration over depth and time. SBDTs are applicable in all aquifer types, but especially interesting in heterogeneous karst or fractured aquifers. Uniform injections aim at a homogeneous tracer concentration throughout the entire saturated length and provide information about inflow and outflow horizons. Also, in the absence of vertical flow, horizontal filtration velocities can be calculated. The most common method for uniform injections uses a hosepipe to inject the tracer. This report introduces a simplified method that uses a permeable injection bag (PIB) to achieve a close-to-uniform tracer distribution within the saturated zone. To evaluate the new method and to identify advantages and disadvantages, several tests have been carried out, in the laboratory and in multiple groundwater monitoring wells in the field. Reproducibility of the PIB method was assessed through repeated tests, on the basis of the temporal development of salt amount and calculated apparent filtration velocities. Apparent filtration velocities were calculated using linear regression as well as by inverting the one-dimensional (1D) advection-dispersion equation using CXTFIT. The results show that uniform-injection SBDTs with the PIB method produce valuable and reproducible outcomes and contribute to the understanding of groundwater monitoring wells and the respective aquifer. Also, compared to the hosepipe method, the new injection method requires less equipment and less effort, and is especially useful for deep boreholes.


2006 ◽  
Vol 932 ◽  
Author(s):  
Yuichi Niibori ◽  
Yasunori Kasuga ◽  
Hiroaki Yoshikawa ◽  
Kouichi Tanaka ◽  
Osamu Tochiyama ◽  
...  

ABSTRACTIn the geological disposal of radioactive wastes, cement used for the repository construction alters the condition of groundwater to highly alkaline of pH about 13. Such alkaline groundwater around the repository would alter the surfaces of the rocks in the flow paths to the amorphous phase. Once the surface is altered, it takes a geological period (so much long time) to restore the surface to its former condition. This study examined the sorption behavior of europium (Eu-152 (tracer), Eu-151 (5×10-5 M, carrier) onto some silica minerals with polymeric silicic acid. Polymeric silicic acid also affects the alteration of the solid surface.The results showed that the kinds of silica minerals strongly affect the sorption behavior in the range of 5<pH<8. The main difference was due to the degree of crystallization of the solid phase, the specific surface area and the concentration of polymeric silicic acid. Since the amorphous silica or polymeric silicic acid takes a loose structure, the isoelectric point is high compared to the crystal ones such as opal-CT and cristobalite, which in turn decreases the sorption. The crystalline silica with polymeric silicic acid remarkably decreased the sorption of europium. This suggested that the surface of solid phase was altered by polymeric silicic acid.


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