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We combine low-temperature scanning tunneling microscopy and measurements of the catalytic activity to establish a structure-reactivity correlation for the CO oxidation on Pt nanoclusters on rutile TiO2(110)-(1 x 1). Annealing of the clusters to 1100 K leads to their encapsulation by a reduced titania layer. We present a method how this catalytically passive strong metal-support interaction state can be transformed into a very active one. We believe that our method is of general interest well beyond the presented system.

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