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Nouveaux carbones mésostructurés comme supports de nanoparticules d’or pour des oxydations sélectives aérobies

Abstract : Highly dispersed gold nanoparticles in ordered mesoporous carbons CMK-3 have been obtained by an original method which consists in replicating mesoporous SBA-15 silicas containing gold nanoparticles. The gold particle size is smaller when the silica surface is functionalized with a thiol (mercaptopropyl graft, MPTMS) (dAu ~ 2 nm) than with an ammonium (TPTAC) (dAu ~ 6 nm). The gold particle size in replicas can be controlled by both the calcination temperature of the silica template and the pyrolysis temperature of the carbon source. Although the carbon replicas are much better dispersed in non polar solvents than the corresponding silica templates, they are less active in the aerobic oxidations of cyclohexene and trans-stilbene in the liquid phase. The best performances in the oxidation of these two molecules have been obtained on replicas pyrolysed at 750°C and containing gold particles with an average size of about 2 nm. The very small particles are unexpectedly less active probably because they are completely coated by carbon, and thus inaccessible. The catalytic performances of our replicas have been compared with those of a Au/CMK-3 catalyst prepared by colloidal deposition onto a preformed mesoporous carbon replica. The results show that our catalysts are much less active than that prepared by colloidal deposition because the majority of particles in our replicas are covered by carbon. The inaccessibility of particles to gases has been confirmed by hydrogen chemisorption on a Pt/CMK-3 catalyst prepared by an identical method.
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Submitted on : Wednesday, June 12, 2013 - 2:22:19 PM
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  • HAL Id : tel-00833320, version 1


Fatmé Kerdi. Nouveaux carbones mésostructurés comme supports de nanoparticules d’or pour des oxydations sélectives aérobies. Autre. Université Claude Bernard - Lyon I, 2011. Français. ⟨NNT : 2011LYO10170⟩. ⟨tel-00833320⟩



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