Gas adsorption/desorption in silica aerogels: a theoretical study of scattering properties

TL;DR

This study uses a numerical lattice-gas model to analyze the structural correlations during gas adsorption and desorption in silica aerogels, explaining scattering experiment results and revealing extended fractal correlations during desorption.

Contribution

It provides a theoretical interpretation of scattering data in silica aerogels using a coarse-grained lattice-gas model and local mean-field analysis, highlighting differences between adsorption and desorption mechanisms.

Findings

Extended fractal correlations during desorption

Increased scattering intensity at small wave vectors

Correlations over distances larger than gel correlation length

Abstract

We present a numerical study of the structural correlations associated to gas adsorption/desorption in silica aerogels in order to provide a theoretical interpretation of scattering experiments. Following our earlier work, we use a coarse-grained lattice-gas description and determine the nonequilibrium behavior of the adsorbed gas within a local mean-field analysis. We focus on the differences between the adsorption and desorption mechanisms and their signature in the fluid-fluid and gel-fluid structure factors as a function of temperature. At low temperature, but still in the regime where the isotherms are continuous, we find that the adsorbed fluid density, during both filling and draining, is correlated over distances that may be much larger than the gel correlation length. In particular, extended fractal correlations may occur during desorption, indicating the existence of a ramified cluster of vapor filled cavities. This also induces an important increase of the scattering intensity at small wave vectors. The similarity and differences with the scattering of fluids in other porous solids such as Vycor are discussed.