Year: 2014
Type: dissertation
Abstract: In this study, the feasibility of the insertion of CO[subscript 2] in an aliphatic ether function was demonstrated for the first time. This finding results from a thermodynamic and kinetic study on dimethyl carbonate (DMC) decarboxylation into dimethyl ether (DME) and CO[subscript 2] at the surface of a zinc(II) exchanged faujasite catalyst. The typical reversible profile of carbonates synthesis chemistry was observed, higher temperature being favorable to CO[subscript 2] release and lower temperature being favorable to CO[subscript 2] insertion. A structural resolution of the rate determining transition structure between DMC and DME was then achieved by correlating molecular modelling calculations to the thermodynamic measurements on DMC decarboxylation. The calculation method developed during the mechanistical analysis was further applied to theoretical catalyst activity screening, which allowed determining structural catalytic sites parameters that favor DME carboxylation over DMC decarboxylation.
Author: Jean-François Lacroix
Language: French
Subfield: Process Chemistry and Technology
Field: Chemical Engineering
Domain: Physical Sciences
SDG: Climate action
Open Access status: green
Funders: Enerkem, Alberta Innovates
OpenAlex ID: W2600666696