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An unusual Fe-H bonding rather than conventional OH bonding is identified atFe3O4 (001) surface. This abnormal behavior is associated with the oxygenvacancies which exist on the surface region but also penetrate deep into thebulk Fe3O4. In contrast, OH bonding becomes preferential as generally expectedon an ozone processed surface, which has appreciably less oxygen vacancies.Such bonding site selective behavior, depending on oxygen vacancyconcentrations, is further confirmed with DFT calculations. The resultsdemonstrate an opportunity for tuning the chemical properties of oxide surfacesor oxide clusters.

Unusual Fe-H bonding associated with oxygen vacancies at the (001) surface of Fe3O4