Catalytic Hydrocarboxylation of Olefins with CO2 and H2 – a DFT Computational Analysis

摘要: One of the major challenges for utilization carbon dioxide as a chemical feedstock is to devise thermodynamically feasible transformations valuable chemicals through efficient catalytic processes. In this paper, we examine feasibility experimentally not yet realized direct hydrocarboxylation alkenes, using computational methods. A conceivable cycle was devised addition H2 and CO2 ethene, which affords propionic acid. The corresponding energy profiles were calculated with state-of-the-art DFT methods three rhodium pincer complexes potential catalyst. Several junctions within productive identified, leading competing hydrogenation reactions ethene or CO2. profound analysis reaction network by means energetic span model allowed us identify parameters that facilitate carboxylation favor it over reaction. comparison relevant activation energies revealed two investigated slightly favour but one complex preferentially stays cycle.