The present proposal plans the rational design of a new generation of bio-inspired catalysts with improved reactivity, efficiency and selectivity through their accurate kinetic and thermodynamic study and tuning.
Recently, it has been elucidated that some organocatalytic reactions follow a Curtin-Hammett principle where the bond-forming step is not normally the rate-determining step, and after the bond-forming step catalytic downstream intermediates appear in fast equilibria compared to the overall rate of the catalytic process. This project will exploit the difference in energy of these downstream intermediates through an iterative approach as a key feature to catalyst design. To do so, an unprecedented multibinding pre-catalysts inspired in the enzymatic allosteric regulation will be used. First, to evaluate their behaviour, a complete study of the equilibria involved in both the allosteric and the active sites using different NMR techniques will be performed. Subsequently, we will carry out a set of mechanistic studies by using differential methods to reaction monitoring on a continuous way together with the Reaction Progress Kinetic Analysis (RPKA) protocol. The quantitative information acquired in these studies will allow to perform key structural modifications of the pre-catalysts to improve their performance. Then, the process will start again in an iterative way with the improved prototypes until reaching the optimal catalysts. The new generated catalysts will be highly selective and efficient through accurate molecular recognition. Moreover, it is expected to be synthetically useful in really low amounts (1-5 mol%).
Consequently, the present bio-inspired and iterative approach for catalyst design will contribute to perform reactions in a more environmentally friendly and economically sustainable way. In addition, the new kinetic and thermodynamic information released during these studies will provide more insights about catalyst behaviour.
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