Molybdenum sulfide cluster catalysts in hydrogenation and dehydrogenation reactionsa combined theoretical and experimental study
- Gutiérrez Blanco, María
- Rosa María Llusar Barelles Directeur/trice
- Vicent Sixte Safont Villareal Co-directeur/trice
Université de défendre: Universitat Jaume I
Fecha de defensa: 25 janvier 2024
- Karl Kirchner President
- Marta Feliz Rodriguez Secrétaire
- Cristina Santamaría Angulo Rapporteur
Type: Thèses
Résumé
This doctoral thesis addresses the synthesis, structural characterization and applications as homogeneous catalysts of molybdenum sulfide clusters decorated with ligands containing amino groups. In particular, hydrogenation and dehydrogenation processes catalyzed by these compounds have been investigated. The synthesis of a series of new imidazolyl amino Mo3S4 clusters is presented, and their catalytic activity is assessed in the stereoselective semihydrogenation of internal alkynes to obtain the (Z)-alkene. Besides, the potential of these and other closely related Mo3S4 clusters for the catalytic hydrogen production from formic acid is shown. The best results are found for aminophosphine-based Mo3S4 clusters. Both transformations have been tackled using an integrative approach that combines experimental methodologies with theoretical calculations. Such approach has allowed us to postulate hydrogenation and dehydrogenation reaction mechanisms based on solid evidence.