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.
| Identifer | oai:union.ndltd.org:CCSD/oai:tel.archives-ouvertes.fr:tel-00808487 |
| Date | 04 April 2013 |
| Creators | Coudert, François-Xavier |
| Publisher | Université Pierre et Marie Curie - Paris VI |
| Source Sets | CCSD theses-EN-ligne, France |
| Language | French |
| Detected Language | English |
| Type | habilitation ࠤiriger des recherches |
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