Abstract The adsorption of single Pd atoms on the various CeO2 surfaces, including (111), (110), and (100), has been studied based on the first-principles calculations. It is found that, according to the calculated adsorption energy, interaction strength between Pd and the three CeO2 surfaces follows the order of (100)>(110)>(111). Interestingly, the effect of the electron localization on the surface Ce ions due to the Pd adsorption on its adsorption stability is more significant for the (110) surface than that for the (111) and (100) surfaces. We also find that the formal oxidation states of Pd0, Pdδ+ (δ<1) and Pd1+ may appear on the CeO2 (111) surface, and Pdδ+ (δ<1) and Pd1+ could coexist on the CeO2 (100) surfaces. However, under suitable conditions the CeO2 (110) surface may be covered with Pd2+ ions. Present theoretical results clearly suggest that the interaction between Pd and CeO2 nanocrystals significantly depends on the crystal planes of CeO2. It is expected that our study will give useful insights into the effect of CeO2 crystal plane on the physicochemical and catalytic properties of CeO2 supported Pd catalyst. Highlights The interaction between the single Pd atoms and different CeO2 surfaces is investigated using the first-principles calculations. The interaction strength between Pd and the three CeO2 surfaces follows the order of (100)>(110)>(111). The stability of the adsorbed Pd atoms with respect to the reduction of the surface Ce is crystal-plane dependent. • The formal oxidation state of the adsorbed Pd atoms is also shows a crystal-plane dependence.
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