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The effect of in situ formed silica gel on the permeability of a porous material was investigated experimentally. Gelling solutions of tetra-methyl-ortho-silicate (TMOS) and methanol in water were imbibed into dry sandstone plates and cured for several days. The permeability of the untreated sandstone is on the order of 1 μm2, whereas the intrinsic permeability of the silica alcogel is 5–6 orders of magnitude lower. The method of beam bending was employed to measure concurrently the permeability D and Young’s modulus Ep of cylindrical gel rods, prepared from the TMOS-based sol-gel solutions. Second, the permeabilities and moduli of the treated sandstones were measured. For both types of samples the gel structure was varied by varying the concentration of the TMOS in a solution and the pH of the water used. The parameters D and Ep follow from a detailed analysis of the measured relaxation of the load that is applied to the sample under constant deflection. In case of the gels, the relaxation was interpreted using common expressions for hydrodynamic relaxation and viscoelastic (VE) relaxation. It was found that the permeability of the gels decreases with increasing silica content and that acid-catalyzed gels exhibit a significantly lower permeability than base-catalyzed gels. The modulus Ep increases with increasing silica content and aging time. The relaxation data of the sandstone—treated with gel—exhibited a more complex behavior. The normalized load curves showed hydrodynamic relaxation as well as strong and fast VE relaxation. The relaxation data for the rock samples treated with the lowest concentration gel was fitted successfully with the predictions. For higher concentrations the fit was less accurate, but the permeability estimates were within an order of magnitude. The overall permeability of the treated rock is higher than the intrinsic permeability of the gels; this indicates that the gel does not completely fill the pore space. Nevertheless, the permeability is reduced by a factor 104 with respect to untreated sandstone, and therefore the gel adequately blocks the pores. [ABSTRACT FROM AUTHOR]

The coupled mass transfer and chemical reactions of a gel-forming compound in a two-phase system were studied in detail. Tetra-methyl-ortho-silicate (TMOS) is often used as a precursor in sol-gel chemistry to produce silica gels in aqueous systems. TMOS can also be mixed with many hydrocarbons without chemical reaction, which allows for various applications in multiphase systems. In this study, TMOS was mixed with n-hexadecane and placed together with water in small cylinders. Upon contact of the mixture with the water, TMOS transfers completely to the aqueous phase where it forms a gel through a heterogeneous reaction. Nuclear magnetic resonance imaging and relaxation time measurements were employed to monitor the mass transfer of TMOS from the oleic to the aqueous phase. The longitudinal relaxation time (T1) was calibrated and used to determine the concentration of TMOS in n-hexadecane during the transfer. The mass transfer rate was obtained at various temperatures (25–45 °C) and for several initial concentrations of TMOS. In the aqueous phase a sharp decrease in the transversal relaxation time (T2) is observed which is attributed to the gel reaction, in particular the formation of methanol in the initial stage. The minimum in T2 indicates the gelation point, and was found to be strongly dependent on temperature and concentration. [ABSTRACT FROM AUTHOR]

The coupled mass transfer and chemical reactions of a gel-forming compound in a two-phase system were recently analyzed in detail [Castelijns et al. J. Appl. Phys. 2006, 100, 024916]. In this successive work, the gel-forming chemical tetramethylorthosilicate (TMOS) was dissolved in a mineral oil and placed together with heavy water (D2O) in small cylinders. The transfer of TMOS from the oleic phase to the aqueous phase was monitored through nuclear magnetic resonance (NMR) relaxation time measurements of hydrogen in the oleic phase. The rate of gelation was measured through NMR relaxation time measurements of deuterium in the aqueous phase. The temperature, the initial concentration of TMOS, and the type of buffer in the aqueous phase were varied in the experiments. The mass transfer is driven by the rate of hydrolysis, which increases with temperature. The hydrolysis rate is the lowest at a neutral pH and is the highest at a low pH. In the aqueous phase, a sharp decrease in the transverse relaxation time (T2) of 2H is observed, which is attributed to the gel reaction. The plateau in T2 indicates the gel transition point. The gel rates increase with increasing temperature and increasing concentration, and are the highest at a neutral pH.