Abstract
Identification of structures of active sites of catalysts under realistic conditions is key forunderstanding the structure–reactivity relationship and mechanism of catalytic reactions.Various in situ techniques and novel theoretical concepts (e.g. ab initio atomisticthermodynamics) have been developed. As an example, oxidation of stepped Pt(110)and Pt(332) surfaces has been studied using density functional theory, scanningtunneling microscopy and high resolution x-ray photoemission spectroscopy. It wasfound that ridge Pt atoms are highly reactive and one-dimensional (1D) oxidestripes form along the Pt ridge. Within the 1D oxide stripes, the reactivity islow, and reaction occurs only at the defect sites and/or boundaries of 1DPtO2 stripes. Furthermore, for stepped Pt(332) surfaces, a site highly active in promoting carbonmonoxide (CO) oxidation was identified due to the formation of novel transition states atthe boundary of the 1D oxide and chemisorption domains. Since the ratio of the ridgeatoms increases with decrease of the particle sizes, the present study highlights theimportance of the 1D oxide components for the reactivity of supported nanosize catalysts.
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