Here, we report that a cationic bimetallic site consisting of one Pd and three Zn atoms (PdZn) supported on ZnO (PdZn/ZnO) exhibits an extraordinarily high catalytic activity for the generation of H through methanol partial oxidation (MPO) that is 2-3 orders of magnitude higher than that of a metallic Pd-Zn site on Pd-Zn nanoalloy (Pd-Zn/ZnO). Computational studies uncovered that the positively charged Pd atom of the subnanometer PdZn bimetallic site largely decreases the activation barrier for dehydrogenation of methanol as compared to a metallic Pd atom of Pd-Zn alloy, thus switching the rate-determining step of MPO from methanol dehydrogenation over a Pd-Zn alloy with high barrier to the O dissociation step on a cationic PdZn site with a low barrier, which is supported by our kinetics studies. The significantly higher catalytic activity and selectivity for H production over a cationic bimetallic site suggest a new approach to design bimetallic catalysts.
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