Autor: |
Liu H; Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, 4 place Jussieu, 75005 Paris, France. ahmed.nait_abdi@sorbonne-universite.fr., Zhang L; Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, 4 place Jussieu, 75005 Paris, France. ahmed.nait_abdi@sorbonne-universite.fr., Lebègue S; Université de Lorraine, CNRS, Laboratoire de Physique et Chimie Théoriques, UMR 7019, 54000 Nancy, France., Bournel F; Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, 4 place Jussieu, 75005 Paris, France. ahmed.nait_abdi@sorbonne-universite.fr.; Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin, 91192 Gif sur Yvette, France., Gallet JJ; Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, 4 place Jussieu, 75005 Paris, France. ahmed.nait_abdi@sorbonne-universite.fr.; Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin, 91192 Gif sur Yvette, France., Naitabdi A; Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, 4 place Jussieu, 75005 Paris, France. ahmed.nait_abdi@sorbonne-universite.fr. |
Abstrakt: |
The study of the surface morphology and interface of metal-oxides is crucial for understanding the behavior of these model systems as nanocatalysts. Besides, understanding the interplay between morphology, stability, and reactivity is crucial for designing efficient catalysts. Here, we investigated the stability and dewetting of ZnO ultrathin films on Pt(111) under CO oxidation conditions. For films <1 monolayer (ML), CO-induced dewetting occurs at the metal-oxide interface or defects. The morphology, dependent on thickness, influences reactivity. (6 × 6) structures show greater CO binding and structural changes compared to (4 × 4) structures, which exhibit resilience due to Zn-OH formation. ZnO electronic properties, as revealed by Auger spectroscopy and scanning tunneling spectroscopy (STS) investigations, vary with thickness. Low-thickness films [<2 monolayers (ML)] exhibit metallic-like behavior, possibly due to Zn-Pt interaction, while thicker films show n-type semiconductor behavior with a bandgap opening ( E BG = 0.9 eV at 2 ML). DFT calculations of the local density of states (LDOS) as a function of ZnO thickness confirm the thickness-dependent electronic structure, with 0.3 ML films having a higher LDOS near the Fermi level than 1 ML films. These findings highlight the critical role of ZnO morphology in determining its stability and reactivity which opens up avenues for designing efficient and more stable ZnO-based nanocatalysts for a wide range of chemical reactions, including CO oxidation and CO 2 hydrogenation. |