화학공학소재연구정보센터
Journal of Molecular Catalysis A-Chemical, Vol.411, 349-363, 2016
The effects of gold nanoparticles obtained from the thermolysis of n-hexanethiolate-stabilized gold nanoparticles on isobutane oxidation over metal oxide catalysts
The complete oxidation of isobutane has been studied using the oxidation catalysts beta-MnO2, alpha-Fe2O3, Co3O4 and NiO, prior to and following addition of 5 wt% Au nanoparticles. The activity order is Co3O4 > beta-MnO2 > alpha-Fe2O3, with the position of NiO dependent on the Ni3+ content which changes with temperature. Preformed n-hexanethiolate-stabilized gold nanoparticles, following adsorption and thermolysis in air, introduce a small amount of sulfur as adsorbed sulfate. The sulfate appears to block the reoxidation step in the Mars-van Krevelen mechanism. This can have a significant effect on catalytic activity, as observed for beta-MnO2. TEM/STEM studies indicate that gold nanoparticles of 2-4 nm in diameter form, which depends on the identity of the metal oxide and its specific surface area. Gold nanoparticle size effects have been studied on NiO, and show that the apparent activation energy and temperature of initial reaction depend on nanoparticle size. Comparisons of the multicomponent Au/MOx/gamma-Al2O3 (M:Al = 1:10) catalysts, where M = Mn, Fe, Co, Ni, have also been studied, and all are more active catalysts than Au/-gamma-Al2O3, but less active than the unsupported catalysts. Gold 4f(7/2) XPS studies on Au/MOx and Au/MOx/gamma-Al2O3 have shown that the only common species present is Au(0), suggesting that higher oxidation states of Au are not important in oxidation catalysis. (C) 2015 Elsevier B.V. All rights reserved.