(765h) Creating Metal-Oxide Interfaces in Metal Organic Framework for Efficient Methanol Synthesis from CO2
AIChE Annual Meeting
2019
2019 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Novel Active Phases in Catalyst Design II: Noble Metals
Friday, November 15, 2019 - 2:36pm to 2:54pm
Figure 1. (A) Schematic view of the approach for
creating interfaces between metal nanoparticles in 3-D frameworks. (B) The Cu
k-edge XAFS and the fitted spectrum suggesting Cu nanoclusters locate in the
pores of MOF with ~30% Cu-O-Zr interfacial sites. (C) The activity in selective
hydrogenation of CO2 to methanol suggesting Cu/UiO66 has superior
performance.
Interfaces
between metals and metal oxides 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-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.