Catalysts comprising zeolite ZSM-5 impregnated with precious metals including Ag, Cu, Ni, Pd, Ir and Ru, have been tested for the methanol to hydrocarbons reaction in a continuous flow fixed bed reactor. Comparison with the activity of unmodified ZSM-5 showed that Ag, Cu and Ni enhanced the selectivity to C 6 -C 11 aromatic products by a factor of two or higher. Moreover, Ag/ ZSM-5 showed improved selectivity for the C 6 -C 7 fraction of aromatic products. Ni/ZSM-5 was found to be selective to naphthalene, while Cu/ZSM-5 was selective for C 9 -C 11 aromatic products. It was ascertained that all the impregnated metals were present as metal oxides in the starting materials. It is therefore proposed that the enhanced selectivity to aromatic products is due to the interaction of the acid sites of the zeolite with the basic sites of the metal oxide at the edge of the zeolite crystals, as well as the possible coordination of propene molecules formed during the reaction, that are likely to be the building blocks for the formation of aromatics.
The activation and use of oxygen for the oxidation and functionalization of organic substrates is among the most important reactions in a chemist's toolbox. Nevertheless, despite the vast literature on catalytic oxidation, the phenomenon of autoxidation, an ever-present background reaction that occurs in virtually every oxidation process, is often neglected. In contrast, autoxidation can affect the selectivity to a desired product, to those dictated by pure freeradical chain pathways, thus affecting the activity of any catalyst used to carry out a reaction.This critical review compares catalytic oxidation routes by transition metals versus autoxidation, particularly focusing on the industrial context, where highly selective and "green" processes are needed. Furthermore, the application of useful tests to discriminate between different oxygen activation routes, especially in the area of hydrocarbon oxidation, with the aim of an enhanced catalyst design, is described and discussed. In fact, one of the major targets of selective oxidation is the use of molecular oxygen as ultimate oxidant, combined with the development of catalysts capable to perform the catalytic cycle in a real energy and cost effective manner on a large scale. To achieve this goal, insights from metallo-proteins that could find application in some areas of industrial catalysis are presented, as well as considering the physicochemical principles that are at the fundament of oxidation and autoxidation processes.3
The aerobic oxidation of 1,2-propanediol in alkaline aqueous solvent over bimetallic AuPt/C catalysts has been studied and catalyst reusability has been assessed.
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