Computational chemistry has reached such a degree of maturity that studies that just 5 years ago were a milestone are now routine. New chemical reactions that seem simple usually hide complex mechanisms, multiple reaction paths, and subtle effects that challenge theoretical models. Molecular metal oxides in aqueous solution involve condensation and self-assembling reactions, as well as multiple balances that dynamically determine the final result. The project that we present here aims at tackling reactivity and catalysis problems for a wide range of systems with varying levels of complexity. To this end, we plan to use DFT methods together with classic molecular
dynamics simulations, and combine them in multiscale atomistic models. On the other hand, we intend to (i) develop workflows that ease tedious tasks and complex calculation protocols, (ii) develop predictive methods based on machine-learning techniques.
The reaction of carbon dioxide with epoxides to obtain carbonates or polycarbonates, which has been extensively studied by our group, will be addressed to obtain kinetic models that allow direct comparison with experiments. We plan to be able to perform simulations with explicit solvent at high pressures in order to achieve models that are as realistic as possible. Borylation reactions, with multiple additives and sensitive reaction conditions are difficult because ion pairs and multiple balances are involved. In some cases we do not rule out the possibility that radical species come also into play. Especially in the new decarboxylative borylation reaction.
There are still key questions to answer in polyoxometalate chemistry, such as the formation of pentagonal patterns that make up the building-blocks of Keplerates and other species. Recent findings about this pentagonal piece in other metals like titanium suggest that the formation of these clusters must have a common origin. We intend to apply all the available techniques to tackle this matter. Finally, new X-ray scattering experiments allow detecting molecular cluster structures in disolution. Nowadays, vanadates, niobates, and tantalates disolutions are being studied as precursors of molecular clusters in the obtention of materials. The present project will determine the
structures of these new polyoxometalates and will contribute to the understanding of their properties in disolution.