Abstract
The effect of the size of gold nanoparticles on their catalytic activity in aerobic oxidation of cyclohexene was established using supported gold nanoparticles that gradually undergo a change in size during the catalytic reaction. Two triphenylphosphine-stabilized clusters, Au9(PPh3)8(NO3)3 and Au101(PPh3)21Cl5, were synthesized and deposited on SiO2. The clusters did not retain their structure during the catalytic reaction; larger particles with mean diameters of ∼5–10 nm gradually formed. By combining kinetic experiments with the monitoring of catalyst transformations using transmission electron microscopy, diffuse-reflectance ultraviolet–visible spectroscopy, and X-ray photoelectron spectroscopy, we showed that catalytic activity appeared only after >2 nm Au0 particles had formed, while intact clusters and phosphine-free <2 nm particles were inactive in cyclohexene oxidation under the studied conditions.
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