Interfaces between metals and support have high activity for activation and conversion of CO2, whereas they are just accessible on the perimeter of the metal nanoparticles on traditional supported catalysts. We present here a strategy for the synthesis of well-defined metal-support (e.g., metal oxide) interfaces by incorporating metal nanoparticles into the pores of metal-organic frameworks (UiO-66 and ZIF-8) (Figure 1A). Pd or Cu nanoparticles bind to the hydroxyl groups of the secondary building units (SBUs), i.e., Zr6 oxide or ZnN4 clusters (UiO-66 and ZIF-8, respectively). As a result, the proportion of metal atoms located at the interfaces with the SBUs is maximized (Cu in UiO-66, Figure 1B). Our novel systems are highly active for the selective conversion of CO2 to methanol even compared to commercial catalysts and highly dispersed metal clusters deposited in zeolites. For instance, Cu/UiO-66 is more active than the Cu on bulk ZrO2 and commercial Cu/ZnO/Al2O3 catalyst (Figure 1C). Our work highlights the advantages of combining the architecture and chemical features of MOF with small metal entities for CO2 and H2 activation.

Creating metal-support interfaces in metal-organic frameworks for efficient methanol synthesis from CO2

2019 Fall National Meeting

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