Theoretical study of cross-coupling reactions: homogeneous and heterogeneous catalysis

Abstract

In-depth study of catalytic reactions that occur in homogeneous and / or heterogeneous medium still represents a challenge for computational chemistry, mainly when the model becomes even more closer to the real systems. Design and rethink of new catalysts, in order to produce C-C and C-N bonds, attracts considerable interest of the scientific community nowadays. Palladium-based catalysts occupy a leading position in enabling highly selective C-C and C-N bonds forming reactions in both homogeneous and heterogeneous medium. Calculations based on the Density Function Theory (DFT) will be used to study mainly two cross-coupling reactions involving palladium-based catalysts: i) Heck-Matsuda reactions and ii) Buchwald-Hartwig reactions in the presence of P, N-ligands ("Dalphos"). Both reactions are examples of processes that occur in homogeneous media. After a detailed study of catalytic cycles in homogeneous medium we will address the possibility of such ligands playing a similar role as auxiliary groups in the surface of a heterogeneous catalyst. (AU)