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By means of scanning tunneling microscopy (STM) measurements, we studied in situ he oxidation and reduction of FeO bilayer islands on Au(111) by oxygen (O 2 ) and hydrogen (H 2 ), respectively. The FeO islands respond very dynamically toward O 2 , with the coordinatively unsaturated ferrous (CUF) sites at the island edges being essential for O 2 dissociation and O atom incorporation. An STM movie obtained during oxidation reveals how further O 2 molecules can dissociate after the consumption of all initially existing CUF sites through the formation of new CUF sites. In contrast, we found that H 2 molecules only dissociate when vibrationally excited through the ion gauge and only at the basal plane of FeO islands, implying that the CUF sites are not relevant for H 2 dissociation. Our STM results reveal how excess O atoms are incorporated and released in O 2 and H 2 and thus shed light onto the stability of inverse catalysts during a catalyzed reaction.

Atomic-Scale View of the Oxidation and Reduction of Supported Ultrathin FeO Islands