Abstract
Supported Pt/CeO2 catalysts have been widely used in carbon monoxide (CO) oxidation; however, the high oxygen vacancy formation energy (Evac) in the process leads to the poor performance of these catalysts. Herein, we explored different element (Pr, Cu, or N) doped CeO2 supports using Ce-based metal-organic frameworks (MOFs) as precursors via calcination treatment. The obtained CeO2 supports were used to load Pt nanoparticles. These catalysts were systematically characterized by various techniques, and they showed superior catalytic activity for CO oxidation compared to undoped catalysts which could be attributed to the formation of Ce3+, and high amounts of Oads/(Oads + Olat) and Ptδ+/Pttotal. Moreover, density functional theory calculations with on-site Coulomb interaction correction (DFT+U) were performed to provide atomic-scale insights into the reaction process by the Mars-van Krevelen (M-vK) mechanism, which revealed that the element-doped catalysts could simultaneously reduce the adsorption energies of CO and lower reaction energy barriers in the *OOCO associative pathway.
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