Rational design of adsorbent materials by molecular simulation and experimental techniques

Resumen

Adsorbent materials are suitable for diverse industrial operations. The optimal use of these materials comes from both an accurate characterization of them, and the knowledge of their structural and energetic properties. This characterization requires: a) an experimental measurement of its adsorption capacity and b) an interpretation of this result by an appropriate theory. The intention of this thesis was to bring a little piece of new information to this research field by means of experimental and mechanical statistical tools. The two major interest are: to study and improve the structural characterization of novel materials, and to develop versatile and transferable statistical mechanical tools and methodologies to investigate the optimal performance of a given adsorption system. Throughout this work we have developed versatile modeling tools based on the Grand Canonical Monte Carlo method, to describe the adsorption behavior on different adsorbents and adsorbates. These methods were supported by the experimental information of theses systems, such as adsorption/desorption isotherms, structural and crystallographic data, and fluid phase equilibria. We have developed a protocol for the analysis of the Pore Size Distribution of adsorbent materials. The applicability of the developed protocol was tested over different silica based materials such as MCM-41, SBA-15, PHTS and CPG. The proposed molecular models for both materials and fluids had been refined with the information obtained from the molecular simulations and experiments, and in this way we tested some methods/theories available for interpreting different experimental results (such BJH and BET). The developed molecular simulation tools and the synergetic (modeling-experimental) methodology achieved, endorse a fully predictive molecular simulation framework for the gas adsorption on different porous materials. The prediction of the behavior of separation process involving the use of adsorbent microporous mate