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Identifying the ripening modes of supported metal nanoparticles used in heterogeneous catalysis can provide important insights into the mechanisms that lead to sintering. We report the observation of a crossover from Smoluchowski to Ostwald ripening, under realistic reaction conditions, for monomodal populations of precisely defined gold particles in the nanometer size range, as a function of decreasing particle size. We study the effects of the CO oxidation reaction on the size distributions and atomic structures of mass-selected Au561±13, Au923±20 and Au2057±45 clusters supported on amorphous carbon films. Under the same conditions, Au561±13 and Au923±20 clusters are found to exhibit Ostwald ripening, whereas Au2057±45 ripens through cluster diffusion and coalescence only (Smoluchowski ripening). The Ostwald ripening is not activated by thermal annealing or heating in O2 alone.
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