Modelling of Catalytic Systems Towards Green Fuels

With the current growth of the global population and the unsustainable increase of the energy demand and CO₂ emissions, we need to  move forward to more environmentally friendly socialeconomic models to mitigate the effects of climate change. In this scenario, the development of technologies related to renewable energies and the valorisation of CO₂ are called to play a crucial role, which are the two central ideas of this thesis. In order make these two processes affordable, I have employed density functional theory simulations and established tight synergies with experimental testing and characterization to contribute in the search and design of novel catalytic materials towards green fuels. I have assessed the electrocatalytic properties of Earth-abundant based MOF-74 for oxygen evolution reaction, which is the bottleneck of green H₂ production via water splitting. Defective structures have been identified as the active sites of these materials. In reference to CO₂ valorisation, I have explored synthesis-structure-performance relationships of three metal-promoted metal oxides systems: ZnZrO_x, metal-promoted In₂O₃, and the ternary Pd-In₂O₃/ZrO₂. These systems have shown high stability and catalytic activity for the CO₂hydrogenation with green H₂ to methanol, which is a vital commodity with a great potential as fuel. The proper combination of oxidic and metallic phases has been revealed as key for maximizing the catalytic properties of these systems and achieving high methanol productivity. Overall, the features that dictate the electrocatalytic activity of MOF-74 materials for oxygen evolution reaction and the thermocatalytic properties of metal-promoted metal oxides for CO₂ hydrogenation have been identified in this thesis. This paves the way  to the rational design of novel catalytic materials for energy applications.

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