1 Department of Chemistry, Technical University of Denmark2 Centre for Catalysis and Sustainable Chemistry, Department of Chemistry, Technical University of Denmark3 Center for Electron Nanoscopy, Technical University of Denmark4 Max-Planck-Institut
With the ongoing developments in biomass conversion, the oxidation of bioethanol to acetaldehyde may become a favorable and green alternative to the preparation from ethylene. Here, a simple and effective method to encapsulate gold nanoparticles in zeolite silicalite-1 is reported and their high activity and selectivity for the catalytic gas-phase oxidation of ethanol are demonstrated. The zeolites are modified by a recrystallization process, which creates intraparticle voids and mesopores that facilitate the formation of small and disperse nanoparticles upon simple impregnation. The individual zeolite crystals comprise a broad range of mesopores and contain up to several hundred gold nanoparticles with a diameter of 2-3nm that are distributed inside the zeolites rather than on the outer surface. The encapsulated nanoparticles have good stability and result in 50% conversion of ethanol with 98% selectivity toward acetaldehyde at 200 degrees C, which (under the given reaction conditions) corresponds to 606molacetaldehyde/molAuhour-1.
Angewandte Chemie-international Edition, 2014, Vol 53, Issue 46, p. 12513-12516