Yin, HaoYan, Yu-WeiFang, WeiBrune, Harald2024-03-182024-03-182024-03-182024-02-2010.1021/acsnano.3c11400https://infoscience.epfl.ch/handle/20.500.14299/206566WOS:001173730000001The spatially resolved identification of active sites on the heterogeneous catalyst surface is an essential step toward directly visualizing a catalytic reaction with atomic scale. To date, ferrous centers on platinum group metals have shown promising potential for low-temperature CO catalytic oxidation, but the temporal and spatial distribution of active sites during the reaction and how molecular-scale structures develop at the interface are not fully understood. Here, we studied the catalytic CO oxidation and the effect of co-adsorbed hydrogen on the FeO2-x /Ir(111) surface. Combining scanning tunneling microscopy (STM), isotope-labeled pulse reaction measurements, and DFT calculations, we identified both FeO2/Ir and FeO2/FeO sites as active sites with different reactivity. The trilayer O-Fe-O structure with its Moire pattern can be fully recovered after O-2 exposure, where molecular O-2 dissociates at the FeO/Ir interface. Additionally, as a competitor, dissociated hydrogen migrates onto the oxide film with the formation of surface hydroxyl and water clusters down to 150 K.Physical SciencesTechnologyIron OxidesCo OxidationSurface ScienceHydrogen SpilloverModel CatalystProbing Catalytic Sites and Adsorbate Spillover on Ultrathin FeO2-x Film on Ir(111) during CO Oxidationtext::journal::journal article::research article