Structural and rheological evolution of silicananoparticle gels

Abstract

The gelation dynamics of a sol of colloidal silica of approximately 7 nm radius particles is studied using a combination of light scattering and rheometry. By changing the ionic strength (by addition of a salt solution resulting in different ultimate molarities) of the mixture, a stable sol can be destabilized, leading to aggregation and later gelation. The gel time t_gel can be varied from hours to weeks, indicating a reaction-limited aggregation process. Static light scattering is used to extract the fractal dimension D_f of the aggregates, which is found to be approximately 2. The evolution of cluster size is probed by dynamic light scattering, and follows an exponential growth. Rheometry is used to assess the gelation time and further development of the network strength after gelation. The elastic modulus (G′) is found to scale as G′ ∼ ϕ^3.3, where ϕ is the silica particle volume fraction. It was observed that the gel time (after salt solution addition) depends on both the particle volume fraction and salt concentration, showing a divergence at low volume fraction or low salt concentration. For a single solid fraction, data for the cluster hydrodynamic radius, normalized by the single particle radius, from experiments with a wide range of gel times can be collapsed onto a master curve when the time after the salt addition, t, is scaled as t/t_gel; a similar collapse of viscosity and the linear viscoelastic data after gelation can be obtained using the same scaling of time. Salt concentration affects the gel time but not the strength of the gel network, thus allowing very accurate prediction of network formation times and mechanical properties.