Journal
ACS CATALYSIS
Volume 3, Issue 12, Pages 2986-2991Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs400701j
Keywords
gold nanoparticles; gold clusters; oxidation; catalysis; size effect
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Funding
- University of Canterbury
- MacDiarmid Institute
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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, Au-9(PPh3)(8)(NO3)(3) and Au-101(PPh3)(2),Cl-5, were synthesized and deposited on SiO2. The clusters did not retain their structure during the catalytic reaction; larger particles with mean diameters of similar to 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 Au-0 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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