CO2 valorization as a low, or even negative-cost feedstock, has gained a lot of attention recently. The use of CO2 as C-containing feedstock can be a means for the abatement of CO2 as an environmental pollutant during the search for, and scale up of, fossil fuel alternatives. In the likely case that even “negative carbon emissions” will become imperative to facilitate the minimization of the environmental impact of greenhouse gases, the scientific exploration of appropriate concepts is needed. The hydrogenation of CO2 is a reaction with the potential to be applied in this concept through chemical storage of electricity in e.g. methane. In this way, via a closed-cycle process CO2 can be captured and utilized as chemical energy. Continuous efforts in the field of materials science have allowed scientists to generate smaller and smaller (supported) metal nanoparticles, creating new opportunities to understand catalytic properties that depend on the metal particle size and shape. Structure-sensitivity is the phenomenon where not all surface atoms in a supported metal catalyst have the same activity. Using a unique set of well-defined SiO2-supported Ni nanoclusters (in the range 1-7 nm) and advanced characterization methods (i.e., FT-IR, and quick X-ray absorption spectroscopy), we prove how structure-sensitivity influences the mechanism of catalytic CO2 reduction to form methane, the nature of which has been long debated. These findings bring fundamental new understanding of CO2 hydrogenation over Ni and allow us to control both activity and selectivity towards the formation of different chemicals (Power-to-Chemicals concept). Furthermore, we gain also insight into the formation of these chemicals via theoretical calculations and rationalize the effect of support oxide and promotor elements. This Power-to-Chemicals concept can be regarded as a means for CO2 emission abatement through its valorization as a low, or even negative cost feedstock, on a low-cost transition metal catalyst.

Catalytic hydrogenation of carbon dioxide: Structure sensitivity and mechanistic insights to steer activity and selectivity

2019 Spring National Meeting

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