Towards green synthesis of organic carbonates: Utilization of CO2 as a chemical feedstock

Identifier:  TDX:2513

Handle: https://hdl.handle.net/20.500.11797/TDX2513

Authors:  Cuesta Aluja, Laia

Abstract:
This doctoral Thesis was focused on the use of carbon dioxide as both C1 building block for the synthesis of useful cyclic carbonates and polycarbonates and its uses as a plausible alternative solvent. We studied the catalytic potential of different metal-catalyzed systems, highlighting the high catalytic activity and selectivity; the use of mild conditions and environmentally friendly metal catalysts and also the elucidation of the possible reaction mechanism giving a plausible catalytic role of each component. It was described the high potential of a low-toxic and earth-abundant Al(III) and Fe(III) complexes bearing tetradentate N2O2-donor ligand whereas the high activity of Zn(II) and Fe(III) complexes bearing tridentate NN'O-donor ligands. An important and greener goal of this Thesis was the obtention of methyl oleate carbonate, derived from natural oils, with those metal earth abundant Al(III), Zn(II) and Fe(III) complexes. Moreover, iron complexes were found to be active both for olefin epoxidation and organic carbonate synthesis. A preliminary study of direct oxidative carboxylation of styrene towards styrene carbonate using scCO2 as both reactive and solvent with Fe(III) complex bearing NN'O-donor ligand was undertaken.