Homogenous catalysis by molybdenum sulfide clusters and the study of their sulfur-centered mechanisms

Abstract

The present doctoral thesis is included within the homogenous catalysis field. A comprehensive study has been conducted on the catalytic activity of molybdenum sulfide cluster compounds coordinated with nitrogen-donor ligands. First, the synthesis of a novel compound containing the ethylenediamine ligand was optimized and characterized using classical spectrometric and spectroscopic techniques. Additionally, the crystalline structure of this complex was determined through single-crystal analysis using electron diffraction techniques. The catalytic activity of molybdenum clusters with the Mo3S4 unit was investigated in C–C coupling reactions for the production of esters, sulfoxide hydrogenation to obtain sulfides, and the methanolysis of hydrosilanes for the synthesis of methoxysilanes and hydrogen. Kinetic studies and control experiments demonstrated that these transformations occur via sulfur atoms, enabling an in-depth investigation of the reaction mechanisms. Finally, using DFT techniques, the reaction mechanisms for sulfoxide hydrogenation and methanolysis were elucidated based on experimental evidence obtained.