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The strong metal-support interaction (SMSI) leads to substantial changes ofthe properties of an oxide-supported catalyst after annealing under reducingconditions. The common explanation is the formation of heavily reduced,ultrathin oxide films covering metal particles. This is typically encounteredfor reducible oxides such as TiO2 or Fe3O4. Zirconia (ZrO2), a typical catalystsupport, is difficult to reduce and therefore no obvious candidate for the SMSIeffect. In this work, we use inverse model systems with Rh(111), Pt(111), andRu(0001) as supports. Contrary to expectations, we show that SMSI isencountered for zirconia. Upon annealing in ultra-high vacuum, oxygen-deficientultrathin zirconia films ($\approx$ZrO$_{1.5}$) form on all three substrates.However, Zr remains in its preferred charge state of 4+, as electrons aretransferred to the underlying metal. At high temperatures, the stability of theultrathin zirconia films depends on whether alloying of Zr and the substratemetal occurs. The SMSI effect is reversible; the ultrathin suboxide films canbe removed by annealing in oxygen.

Substoichiometric ultrathin zirconia films cause strong metal-support interaction