I use and develop theoretical chemistry models and molecular simulation methods in order to study fluid adsorption in nanoporous cristalline materials, focussing on three main aspects. First, I have developped analytical statistical thermodynamics models describing the interplay between fluid adsorption and host solid structural transitions. These models help rationalize and predict the occurrence of adsorption and pressure-induced phase transitions in flexible metal-organic frameworks, in the multi-parameter space of gas pressure, gas mixture composition, temperature and mechanical stress. Secondly, I used molecular simulation methods to study the properties of these flexible MOFs, and their adsorption properties. I used a large gamuth of methods including quantum chemistry calculations, ab initio dynamics, and forcefield-based Monte Carlo simulations to that aim. I also developped non-Boltzmannian Monte Carlo methods specifically tailored for these issues of adsorption in systems of widely varying volume. Finally, I have performed some studies of hydrothermal and mechanical stability of both flexible and nonflexible MOFs.
