Abstract
The catalytic low-temperature oxidation of CO to CO2 with molecular oxygen is of particular industrial and ecological interest. Gas-phase reaction kinetics measurements in conjunction with first-principles calculations provide comprehensive insight into the mechanisms and energetics of the low-temperature CO combustion reaction catalyzed by small free palladium clusters Pdx+ (x = 2–7). Similar to the cases of extended palladium single crystals and supported nanoparticles, the catalytic activity of the free palladium clusters was found to be largely determined by the fast adsorption and dissociation of molecular oxygen and the binding strength of carbon monoxide. In particular, Pd4+, Pd5+, and Pd6+ were found to catalyze the oxidation of CO at room temperature, with Pd6+ being most active. Detailed mechanistic investigations of the CO oxidation reaction catalyzed by Pd6+ reveal a Langmuir–Hinshelwood reaction mechanism, similar to that found earlier for CO oxidation on palladium single crystals, with compa...
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