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In Olkiluoto Finland colloidal silica called silica sol (EKA Chemicals) will be used as a non-cementitious grout for the sealing of fractures of the hydraulic apertures of 0.05 mm or less. The use of colloidal material has to be considered in the long-term safety assessment of a spent nuclear fuel repository. The potential relevance of colloid-mediated radionuclide transport is highly dependent on their stability in different geochemical environments. Objective of this work was to study the effect of ionic strength on stability of silica colloids released from silica gel. Silica gel samples were stored in contact with NaCl and CaCl2 electrolyte solutions and in deionized water. Colloid release and stability were followed for two years by taking the samples after one month and then twice in a year. The release and stability of colloids were followed by measuring particle size, colloidal silica concentrations and zeta potential. The particle size distributions were determined applying the dynamic light scattering (DLS) method and zeta potential based on dynamic electrophoretic mobility.
In dilute NaCl (10-7–10-2 M) and CaCl2 (3 10-7– 3 10-3 M) solutions, a mean colloid diameter was less than 100 nm and high negative zeta potential values suggests the existence of stable silica colloids. After two years, the mean particle diameter was increased but it was still less than 500 nm and absolute value of zeta potential was decreased. In 0.1–1 M NaCl and 0.03–3 M CaCl2 solutions, wide particle size distribution and zeta potential values around zero suggested particle aggregation and instable colloids. In deionized water, particle size remained rather stable and zeta potential remained high negative suggests stable silica colloids. The threshold value of ionic strength was 0.03–0.1 M when salinity had an effect on the stability of colloids. In Olkiluoto, the ionic strength of saline groundwater is order of magnitude higher than the range of effect value obtained in this study. Under the prevailing conditions in Olkiluoto, silica colloids are instable, but the possible influence of glacial melt waters has to be considered.
Non-cementitious grouts have been tested in Olkiluoto for the sealing of fractures with the small hydraulic apertures. A promising non-cementitious inorganic grout material for sealing the fractures with the apertures less than 0.05 mm is commercial colloidal silica called silica sol. The potential relevance of colloid-mediated radionuclide transport is highly dependent on their stability in different geochemical environments. The objective of this work was to follow stability of silica sol colloids in low salinity Allard and saline OLSO reference groundwater (pH 7–11) and in deionized milliQ water. Stability of silica sol colloids was followed by measuring particle size distribution, zeta potential, colloidal and reactive silica concentrations. The particle size distributions were determined applying the dynamic light scattering (DLS) method and zeta potential based on dynamic electrophoretic mobility. The colloidal silica concentration was calculated from DLS measurements applying a calibration using a standard series of silica sol. Dissolved reactive silica concentration was determined using the molybdate blue (MoO4) method.
These results confirmed that the stability of silica colloids dependent significantly on groundwater salinity. In deionized water, particle size distribution and zeta potential was rather stable except the most diluted solution. In low salinity Allard, particle size distribution was rather constant and the mean particle diameter remained less than 100 nm. High negative zeta potential values indicated the existence of stable silica colloids. In saline OLSO, particle size distribution was wide from a nanometer scale to thousands of nanometers. The disappearance of large particles, decrease in colloidal particle concentration and zeta potential near zero suggest flocculation or coagulation. Under prevailing saline groundwater conditions in Olkiluoto silica colloids released from silica sol are expected to be instable but the possible influence of low salinity glacial melt water has to be considered.
Non-cementitious grouts have been tested in Olkiluoto for the sealing of fractures with the small hydraulic aperture. A promising non-cementitious inorganic grout material for sealing the fractures of the apertures less than 0.05 mm is commercial colloidal silica called silica sol. The use of colloidal material has to be considered in the long-term safety assessment of a spent nuclear fuel repository. Objective of this work was to determine colloid release from the silica sol gel and stability of silica colloids in different groundwater conditions. To use silica sol as a grout, the injected colloids have to aggregate and form a gel within a predictable time by using a saline solution as an accelerator. Silica sol gel samples were stored in contact with medium salinity and low salinity groundwater simulates. Release of silica colloids and colloid stability was followed by analyzing the colloid concentration, particle size distribution, concentration of reactive silicon, solution pH and zeta potential after one month, half a year and one year. Malvern Zetasizer Nano ZS equipment was used to determine colloidal particle size distributions applying the dynamic light scattering method and zeta potential based on dynamic electrophoretic mobility. The colloidal particle concentration was estimated from Zetasizer measurements applying a standard series. Dissolved reactive silica concentration was determined using the molybdate blue method and total silica concentrations were determined using ICP–MS.
The release and stability of silica colloids were found to be dependent significantly on groundwater salinity. Zeta potential values near zero and the increase in particle size at first and then the disappearance of large particles indicated particle flocculation or coagulation and instable colloidal dispersion in a saline groundwater simulate. In low salinity ground water simulate high negative zeta potential values, small particle size and constant size distribution indicate the existence of stable silica colloids. The concentrations of the released colloids were slightly higher than determined in natural granitic ground waters. Under prevailing saline groundwater conditions in Olkiluoto no significant release of colloids from silica sol is expected but the possible influence of low salinity glacial melt waters has to be considered.
Concentration profiles in rock matrix around water-carrying fissures were measured at Palmottu U deposit. The profiles were interpreted by the classical matrix diffusion concept. Site-specific sorption studies were performed for U using standard batch experiments and surface complexation modelling; the response of sorption isotherms was also tested. Sitespecific matrix properties as well as initial and boundary conditions were used in simulations. Our results indicate that matrix diffusion alone cannot explain the observed enrichment of U and its daughters in the rock matrix.
Radionuclides transported by ground water flowing through fractures may be delayed by interactions with the fracture surfaces. The migration of radionuclides in fractures was studied under well defined laboratory conditions using tonal-ite drill core columns with a fracture running parallel to the core axis. The hydrodynamic characterization of the columns was performed using tritiated water, pertechnetate and chloride ions as non-sorbing tracers. Strontium and neptunium were used to study the retardation of radionuclides on the fracture surfaces.
The experimental set-up is described, and break-through curves of non-sorbing tracers, strontium and neptunium are presented. The results were interpreted using models for dispersion and diffusion into the rock matrix. From the shape of the break-through curves it was concluded that for non-sorbing tracers there was very little or no diffusion at all into the rock matrix. Retardation of strontium in a column with intact tonalite surfaces indicated a Ka factor identical with that earlier determined by batch experiments. The break-through curve of neptunium indicated a non-sorbing fraction.
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