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Title: Atomic level fluxional behavior and activity of CeO2-supported Pt catalysts for CO oxidation

Reducible oxides are widely used catalyst supports that can increase oxidation reaction rates by transferring lattice oxygen at the metal-support interface. There are many outstanding questions regarding the atomic-scale dynamic meta-stability (i.e., fluxional behavior) of the interface during catalysis. Here, we employ aberration-correctedoperandoelectron microscopy to visualize the structural dynamics occurring at and near Pt/CeO2interfaces during CO oxidation. We show that the catalytic turnover frequency correlates with fluxional behavior that (a) destabilizes the supported Pt particle, (b) marks an enhanced rate of oxygen vacancy creation and annihilation, and (c) leads to increased strain and reduction in the CeO2support surface. Overall, the results implicate the interfacial Pt-O-Ce bonds anchoring the Pt to the support as being involved also in the catalytically-driven oxygen transfer process, and they suggest that oxygen reduction takes place on the highly reduced CeO2surface before migrating to the interfacial perimeter for reaction with CO.

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Nature Communications
Nature Publishing Group
Sponsoring Org:
National Science Foundation
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