Selective side-chain oxidation of alkyl aromatic compounds catalyzed by cerium modified silver catalysts
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Author list: Beier MJ, Schimmoeller B, Hansen TW, Andersen JET, Pratsinis SE, Grunwaldt JD
Publisher: Elsevier
Place: AMSTERDAM
Publication year: 2010
Journal: Journal of Molecular Catalysis A: Chemical (1381-1169)
Journal acronym: J MOL CATAL A-CHEM
Volume number: 331
Issue number: 1-2
Start page: 40
End page: 49
Number of pages: 10
ISSN: 1381-1169
eISSN: 1873-314X
Languages: English-Great Britain (EN-GB)
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Abstract
Silver supported on silica effectively catalyzes the aerobic side-chain oxidation of alkyl aromatic compounds under solvent-free conditions. Toluene, p-xylene, ethylbenzene and cumene were investigated as model substrates. Typically, the reaction was performed at ambient pressure; only for toluene an elevated pressure was required. Carboxylic acids, such as benzoic acid or p-toluic acid, additionally increased the reaction rate while CeO2 could act both as a promoter and an inhibitor depending on the substrate and the reaction conditions. Silver catalysts were prepared both by standard impregnation and Flame spray pyrolysis. Addition of a Ce precursor to the FSP catalyst resulted in significantly smaller silver particles. Ce-doped FSP catalysts in general exhibited a superior catalytic performance with TONs up to 2000 except for cumene oxidation that appeared to proceed mainly by homogeneous catalysis. In addition, Flame-made catalysts were more stable against silver leaching compared to the impregnated catalysts. The structure of the silver catalysts was studied in detail both by X-ray absorption spectroscopy and transmission electron microscopy suggesting metallic silver to be required for catalytic activity. Catalytic studies point to a radical mechanism which differs depending on the type of substrate. (C) 2010 Elsevier B.V. All rights reserved.
Keywords
Flame spray pyrolysis, Homogeneous vs. heterogeneous catalysis, p-Xylene, Selective aerobic oxidation, Silver catalysis
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