Executive Summary : | Plastics, with their strong resistance to degradation and durable nature, pose significant health, economic, and environmental risks. To address this, a new project aims to convert plastics into fuel using an olefin-intermediate heterogeneous catalytic approach. This involves activating poorly reactive aliphatic substrates through dehydrogenation and fragmenting them by highly-active olefin catalysts. The project will focus on the initiation step, activating aliphatic substrate through dehydrogenation, with a focus on quantum mechanical investigations of dehydrogenation of small alkanes to produce olefins over metal and supported metal oxides. The current commercial process for producing light olefins is on-purpose catalytic dehydrogenation, which is highly endothermic and thermodynamically limited. Oxidative dehydrogenation over metal oxides is a cost-saving alternative but suffers from poor yield and overoxidation of alkanes and product olefins to CO₂. The project aims to formulate advanced catalysts with improved selectivity and eliminate overoxidation. Active catalyst sites will be scrutinized, including different metal surfaces, supported metal oxide nanoparticles, and well-dispersed isolated metal oxide species. The project will also explore the synergistic effect of conventional dehydrogenation catalysts with active olefin metathesis catalysts on the dehydrogenation of small alkanes. The Potential Energy Surface of the overall reaction network will be drawn to identify the lowest energy barrier pathway. A microkinetic reaction model will be developed and solved to extract kinetic reaction data. The mechanistic knowledge of dehydrogenation of small alkanes into alkenes obtained from these extensive computational investigations will guide the experimentalists in initiating advanced plastics to fuel conversion. |