PNNL

Abstract

Nature is abundant with multi-functional catalysts such as redox enzymes that are highly active and energy efficient, which scientists wish to emulate when developing synthetic catalysts. One approach is to tune molecular catalysts through metal-organic ligands that are aimed to mimic the structures and functions of enzymes for highly efficient proton transport. However, there are grand challenges of molecular catalysts for real applications in energy field. Here we demonstrate a robust inorganic construct based on metal-metal oxide-carbon triple junction nanostructures (Pd-ZrO2-C) in which the electronic structure of the metal catalysts is tuned by the metal oxide for efficient adsorption and electron transfer, and the local acidic environment is enhanced for increased proton transport. Using electrocatalytic hydrogenation (ECH) of benzaldehyde as a model reaction, we show that both the intrinsic activity, i.e., turnover frequency (TOF) and mass activity of the metal catalyst toward the ECH of benzaldehyde are improved on the triple junction nanostructured catalysts. This study demonstrates the potential of rational design of multicomponent nanostructured catalysts to achieve enzyme like properties in synthetic catalysts.