Computer-generated mesoporous materials and associated structural characterization

Abstract

This study aims to computationally generate and fully characterize realistic three-dimensional mesoporous materials. Notably, a new algorithm reproducing gas adsorption porosimetry was developed to calculate the specific surface area and pore size distribution of computer-generated structures. The diffusion-limited cluster-cluster aggregation (DLCCA) method was used to generate point-contact or surface-contact mesoporous structures made of monodisperse or polydisperse spherical particles. The generated structures were characterized in terms of particle overlapping distance, porosity, specific surface area, interfacial area concentration, pore size distribution, and average pore diameter. The different structures generated featured particle radius ranging from 2.5 to 40 nm, porosity between 35 and 95%, specific surface area varying from 35 to 550 m2/g, and average pore diameter between 3.5 and 125 nm. The specific surface area and pore size distribution of computer-generated mesoporous materials were in good agreement with experimental data reported for silica aerogels. Finally, widening the particle size distribution and increasing the particle overlapping were shown to strongly decrease the specific surface area and increase the average pore size of the mesoporous structures. The developed computational tools and methods can accelerate the discovery and optimization of mesoporous materials for a wide range of applications.