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Galvanin, Federico; Sankar, Meenakshisundaram; Cattaneo, Stefano; Bethell, Donald; Dua, Vivek; Hutchings, Graham J.; Gavriilidis, Asterios
Chemical engineering journal (Lausanne, Switzerland : 1996), 06/2018, Volume: 342Journal Article
Display omitted •Simplified kinetic models were developed for benzyl alcohol oxidation.•Model discrimination was applied to find the most appropriate kinetic model.•At low temperature, toluene formation is dominated by disproportionation.•At high temperature, toluene formation is dominated by hydrogenolysis. Bimetallic Au-Pd nanoparticles supported on TiO2 show excellent catalytic activity and selectivity to benzaldehyde in the solvent-free transformation of benzyl alcohol to benzaldehyde, where toluene is the main observed by-product, together with smaller amounts of benzoic acid, benzyl benzoate and dibenzyl ether. However, despite the industrial relevance of this reaction and importance of tuning the selectivity to the desired benzaldehyde, only a few attempts have been made in the literature on modeling the reaction kinetics for a quantitative description of this reaction system. A kinetic model for the oxidation of benzyl alcohol over Au-Pd is proposed in this paper. The model assumes that hydrogenolysis, disproportionation and dehydrogenation reactions may occur in parallel, and it has been found satisfactory after a model discrimination procedure was applied to a number of simplified candidate models developed from microkinetic studies. Despite its relative simplicity, the proposed model is capable of representing the reactant conversion and distribution of products observed in experiments carried out at different temperature, pressure and catalyst mass in a stirred batch reactor. Major findings include the quantitative evaluation of the impact of hydrogenolysis and disproportionation pathways on benzaldehyde production. At low temperature the disproportionation reaction is the dominant route to toluene formation, while hydrogenolysis dominates at high temperature.
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