The highest oxidation state observed in graphene-supported sub-nanometer iron oxide clusters

Size-selected iron oxide nanoclusters are outstanding candidates for technological-oriented applications due to their high efficiency-to-cost ratio. However, despite many theoretical studies, experimental works on their oxidation mechanism are still limited to gas-phase clusters. Herein we investiga...

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Published in:Communications chemistry 2023-04, Vol.6 (1), p.61-61, Article 61
Main Authors: Perco, Deborah, Loi, Federico, Bignardi, Luca, Sbuelz, Luca, Lacovig, Paolo, Tosi, Ezequiel, Lizzit, Silvano, Kartouzian, Aras, Heiz, Ueli, Baraldi, Alessandro
Format: Article
Language:English
Subjects:
639/638/542/971
639/925/357/354
639/925/930/12
Binding energy
Chemistry
Chemistry and Materials Science
Chemistry/Food Science
Clusters
Electron density
Graphene
High resolution
Iron oxides
Nanoclusters
Oxidation
Photoelectron spectroscopy
Photoelectrons
Spectrum analysis
Valence
Vapor phases
X ray photoelectron spectroscopy
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Summary:Size-selected iron oxide nanoclusters are outstanding candidates for technological-oriented applications due to their high efficiency-to-cost ratio. However, despite many theoretical studies, experimental works on their oxidation mechanism are still limited to gas-phase clusters. Herein we investigate the oxidation of graphene-supported size-selected Fe n clusters by means of high-resolution X-ray Photoelectron Spectroscopy. We show a dependency of the core electron Fe 2p 3/2 binding energy of metallic and oxidized clusters on the cluster size. Binding energies are also linked to chemical reactivity through the asymmetry parameter which is related to electron density of states at the Fermi energy. Upon oxidation, iron atoms in clusters reach the oxidation state Fe(II) and the absence of other oxidation states indicates a Fe-to-O ratio close to 1:1, in agreement with previous theoretical calculations and gas-phase experiments. Such knowledge can provide a basis for a better understanding of the behavior of iron oxide nanoclusters as supported catalysts. Iron oxide nanoclusters are of interest for a broad range of applications, but limited experimental information on their oxidation mechanism is available outside of the gas phase. Here, the oxidation of graphene-supported size-selected Fe n clusters is studied using high-resolution X-ray Photoelectron Spectroscopy.
ISSN:2399-3669
2399-3669
DOI:10.1038/s42004-023-00865-x