Abstract
Femtosecond two-pulse correlation spectroscopy, temperature program desorption spectroscopy, and density functional theory calculations are used to elucidate the mechanisms and the ultrafast dynamics of carbon monoxide (CO) oxidation reaction on palladium nanoparticle (Pd NP) surfaces. Two different time scales for the CO oxidation reaction on Pd NPs are observed: a fast channel (time constant ∼7 ps) is found for the oxidation reaction when strongly bound CO is involved, and a slow channel (time constant ∼15 ps) is found for the oxidation reaction when weakly bound CO is involved. Temperature-programmed desorption spectroscopy confirms that the fast and the slow channels are associated with CO oxidations mostly on (111) facets and at edges of the Pd NPs, respectively. This is the first report on heterogeneous gas-phase ultrafast dynamics study of CO oxidation reaction on transition metal (which is an active catalyst in catalytic converter) NP surfaces.
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