The design of an optimal catalyst for a given process is at the heart of what chemists do, but is in many times more an art than a science. The quest for molecular control of any, either existing or new, production process is one of the great challenges nowadays. The need for accurate rate constants is crucial to fulfil this task. Molecular modelling has become a ubiquitous tool in many fields of science and engineering, but still the calculation of reaction rates in nanoporous materials is hardly performed due to major methodological bottlenecks. The aim of this proposal is the accurate prediction of chemical kinetics of catalytic reactions taking place in nanoporous materials from first principles. Two types of industrially important nanoporous materials are considered: zeotype materials including the standard alumino-silicates but also related alumino-phosphates and the fairly new Metal-Organic Frameworks (MOFs). New physical models are proposed to determine: (i) accurate reaction barriers that account for long range host/guest interactions and (ii)the preexponential factor within a harmonic and anharmonic description, using cluster and periodic models and by means of static and dynamic approaches. The applications are carefully selected to benchmark the influence of each of the methodological issues on the final reaction rates. For the zeotype materials, reactions taking place during the Methanol-to-Olefin process (MTO) are chosen. A typical MTO catalyst is composed of an inorganic cage with essential organic compounds interacting as a supramolecular catalyst. For the hybrid materials, firstly accurate interaction energies between xylene based isomers and MOF framework, will be determined. The outcome serves as a step-stone for the study of oxidation reactions. This proposal creates perspectives for the design of tailor made catalyst from the molecular level.
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