Abstract
The temperature-dependent adsorption as well as the possible activation and dehydrogenation of methane mediated by small free palladium Pdx+ (x = 2–4) and palladium mono-oxide PdxO+ (x = 2–4) clusters have been studied in an ion trap experiment under multicollision conditions. The smallest clusters Pd2+ and Pd3+ are found to readily dehydrogenate methane, while Pd4+ is completely nonreactive within the whole investigated temperature range between 220 and 300 K. In the case of the oxides PdxO+, a critical number of at least three coadsorbed CD4 is required before methane dehydrogenation can be observed. Temperature-dependent kinetic studies of the reaction of Pd2+ and Pd2O+ with methane allow for the determination of catalytic reaction mechanisms that involve C–D bond cleavage and C–C bond formation processes. The catalytic activity of these two clusters is compared in terms of active species, cooperative effects, and activation barriers. Finally, the possible methane oxidation on PdxO+ is discussed.
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