An atomistic model of a disordered nanoporous solid: Interplay between Monte Carlo simulations and gas adsorption experiments

A combination of physisorption measurements and theoretical simulations was used to derive a plausible model for an amorphous nanoporous material, prepared by Friedel-Crafts alkylation of tetraphenylethene (TPM), leading to a crosslinked polymer of TPM connected by methylene bridges. The model was refined with a trial-and-error procedure, by comparing the experimental and simulated gas adsorption isotherms, which were analysed by QSDFT approach to obtain the details of the porous structure. The adsorption of both nitrogen at 77 K and CO2 at 273 K was considered, the latter to describe the narrowest pores with greater accuracy. The best model was selected in order to reproduce the pore size distribution of the real material over a wide range of pore diameters, from 5 to 80 Å. The model was then verified by simulating the adsorption of methane and carbon dioxide, obtaining a satisfactory agreement with the experimental uptakes. The resulting model can be fruitfully used to predict the adsorption isotherms of various gases, and the effect of chemical functionalizations or other post-synthesis treatments.