Abstract

Controlled charge transfer between a support and small metal particles provides unique opportunities to tune the activity of supported metal catalysts, as first proposed by Schwab [G. M. Schwab et al., Angew. Chem. 1959, 71, 101–104]. By controlling the thickness of polycrystalline anatase TiO2 films, the TiO2 carrier concentration can be manipulated by an order of magnitude. When 1 nm Pt particles are deposited on these TiO2 films, the variation in the charge transfer between the TiO2 support and the Pt particles is found to dramatically increase the ethylene hydrogenation activity. The sensitivity of ethylene hydrogenation to charge transfer was anticipated from the large effect of the Pt charge on the ethylene and ethylidyne adsorption energy, e.g., compared to CO and H. Our results demonstrate that the controllable Schwab effect provides a powerful tool to tune catalytic activity. An even larger effect can be expected for supported sub-nanometer clusters, and for the selectivity of hydrogenation reactions.

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