Collaborative Research: Experimental and theoretical study on the structure and catalytic activity of metal cluster/metal oxide interfaces

Project: Research project

Project Details



van Duin

The most successful metal/metal oxide catalysts currently available involve highly-dispersed, low-concentration metal atoms embedded in a metal oxide surface. Palladium metal supported on cerium oxide, is an important example of a highly active catalyst, with applications as an automotive three-way catalyst, in catalytic combustion, and as a solid oxide fuel cell anode material. The activity of these metal/metal oxide catalysts can be uniquely controlled by the support surface structure. Furthermore, these low-concentration metal catalysts have demonstrated significant resistance against sintering, a common multi-component catalyst degradation mechanism, thus indicating superior resistance to heating/cooling cycles and changes in redox enviroment. However, the structure of the active site is challenging to define at the atomistic scale. For the metal-ceria (M/CeO2) catalytic system, dynamic restructuring occurs under reaction conditions and both the ceria and metal structure alter reactivity.

So how then to explain the catalytic and performance behaviors of Pd on ceria? Three Investigators, A.C. van Duin and M. J. Janik of Pennsylvania State University and M. M. Batzill of the University of South Florida, hypothesize that mixed surface oxides of Ce1-xPdxO2-d may provide unique active sites with high activity and stability under certain reaction conditions. To confirm this and in order to fully develop the potential of Pd/CeOx and similar metal/metal oxide catalysts, they believe a detailed, atomistic-scale knowledge of the catalytic conversion mechanisms and the surface dynamics related to substrate-surface interactions is required for the Pd/ceria system. In a collaborative study, the PIs propose to utilize atomistic simulation with Reactive Force-Field (ReaxFF) and Density Functional Theory (DFT) approaches together with experimental surface science studies to investigate the dynamic structure and reactivity of Pd/CeO2 systems. The combined surface science and ReaxFF/DFT approach will provide detailed determination of the structure, stability, and activity of Ce1-xPdxO2-n mixed oxide surfaces. This will help answer questions about this catalyst system.

From the broader perspective, the combination of experimental and computational approaches applied to this complex catalytic system will advance the fundamental understanding of the effect of reducible oxide supports on catalyst stability and activity, as well as provide guidance towards the preparation of highly active M/CeO2 catalysts. Further, the development of an integrated, two-component simulation environment, which is validated against experiment is the outcome of this project. This collaboration between simulation and experiment will provide a roadmap for future catalytic research; the computational tools developed here are generally applicable, thus providing straightforward extension to other catalytic materials.

The research program also closely integrates education and outreach activities. Specifically, at PSU, courses for engineers on atomistic-scale simulation methods will be introduced, which will be complemented by lectures and tutorials on experimental techniques.

Effective start/end date9/1/108/31/14


  • National Science Foundation: $259,026.00


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