Pore matrices prepared at supercritical temperature by computer simulations: matrix characterization and studies of diffusion coefficients of adsorbed fluids

Abstract

We present series of molecular dynamics simulations to study the structure of different porous matrix configurations. The present simulations are an extension of recently reported data at a temperature below the critical. Here, we show how temperature modifies the structure and porosity of pore matrices during their preparation in comparison with the previous work. Moreover, in these studies at a higher temperature, we studied in more detail the structure of the porous matrix. Matrices were prepared by two different processes. The first method consisted of a single Lennard-Jones fluid simulated at a fixed density and at a supercritical temperature. Then, the matrix configuration was taken from the last configuration of the fluid. The second method was prepared from a binary mixture, where one of the components served as a template material. The final porous matrix configuration was obtained by removing template particles from the mixture. Matrices were prepared at two different densities and at different matrix particle interactions. The volume distribution, the cluster formation and the connectivity between the particles in the pore matrix were investigated. The importance of using template particles was clear since they produced larger voids and higher porosities. On the other hand, the temperature of preparation seems to modify the size of the voids and the porosity in the matrices. For instance, at this high temperature, the matrix porosity is higher when template particles are present in the system. These results point in the opposite direction compared to those found in a previous paper at a lower temperature. The diffusion of fluids immersed in the different matrices was also analysed by calculating the mean square displacements of their particles. It was observed that this quantity was higher when matrices were prepared with template particles. These results also point to different directions in contrast with pore matrices prepared at a lower temperature. Finally, the results show that temperature plays an important role in the pore matrix formation.