Characterizing Metal-Support Interaction of Atomically Dispersed Atoms and Clusters on Cu2O (111)
EMSL Project ID
51700
Abstract
Catalytic surfaces are prone to reconstruction depending on the adsorbates present, catalyst coverage, temperature, and other environmental factors. Through model studies, we can generate trends as to how different oxide configurations interact with precious metal single atoms, which would otherwise be more time consuming if conducted experimentally. Cu is a relatively affordable and abundant resource in which its oxide is potentially reducible. In our previous study, atomically dispersed Pt atoms on a particular CuxO film on Cu(111) has been found to be active for CO oxidation through the Mars van Krevelen (MvK) mechanism. However, not all single-site Pt catalysts on a thin oxide film on metallic Cu have shown the same activity for the same reaction. The research objective of this work is to correlate the energetic behavior of atomically dispersed atoms and clusters with their corresponding electronic properties. The central hypothesis is that atoms which interact more strongly with Cu2O(111), possessing higher diffusion barriers and cohesive energies, will have higher distortion of their local electronic properties, exhibiting distinct charge, energetic, and magnetic properties, from those with weaker interactions. To accomplish the research objective, we will use a combination of density functional theory (DFT) and ab initio molecular dynamics (AIMD) to investigate the electronic properties of Pt and Rh structures supported on Cu2O(111), when present as single atom dopants and as clusters. Our work will provide deep insight on atom rearrangement and diffusion on the Cu2O(111) surface through the characterization of their energy, charge, and magnetic moment distribution. This exploration will help save costs, time, and efforts in the design of catalytic materials by cutting down the experimental trial-and-error phase. Throughout these calculations, we will be validating our model with available experimental data provided by our collaborators at Tufts University to ensure the applicability of the developed theories. By understanding how different copper oxide surfaces interact with precious single atoms, we will gain insights for the local geometry suitable for increasing the oxide’s reducibility and stability. Such results will guide us as to how we can replace precious metals in traditional three-way catalytic converter catalysts with cheaper and more abundant materials.
Project Details
Start Date
2020-10-12
End Date
2021-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members