Using CO2 as building block to make chemicals and energy carriers is increasingly becoming indispensable for the sustainable use of renewable energies and for curbing global warming. Diverting CO2 into liquid methanol is a facile and safe approach for the chemical storage of green hydrogen.1 For this reaction, ZnO supported metal nanoparticles (Cu, Au and Pd) are by far amongst the most active catalysts, especially Au/ZnO catalysts, which show higher activity and selectivity toward methanol compared to other metals. Additionally, being more oxidation-resistant, Au is an ideal choice for fundamental understanding of ZnO-based catalysts in general. In this contribution, we will discuss structure-reactivity correlations in CO2 reduction on Au/ZnO catalysts in studies ranging from industrial to idealized / model reaction conditions, relying on a rational synthetic control of Au/ZnO catalysts,2 and applying a multimodal analytical approach including micro-kinetics, in-situ / operando spectroscopies (e.g., lab-based NAP-XPS studies) and high resolution scanning transmission electron microscopy.3 These results shall be supplemented by findings on the activation and spillover of hydrogen on Au/ZnO obtained from temperature-programmed reduction (TPR) in H2 and D2 streams, and will be compared to earlier results from surface oxygen titration using temporal analysis of products (TAP) reactor.4 These studies demonstrate together a direct correlation between the formation/replenishment of O-vacancies, Au charging, hydrogen adsorption capacity, and the methanol formation activity from CO2/H2, while on the other hand CO formation rates either correlated inversely to changes in these parameters or were independent of changes therein.

Surface science approach to understand structure-reactivity correlations in methanol synthesis from CO2 on supported ZnO catalysts

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