Abstract
Structural properties of a series of mordenite and ZSM-5 zeolites with different framework Al distribution modified with oxygenated extraframework Ga, Zn, Al, Cu and Fe complexes were investigated by means of periodic density functional theory calculations. It is demonstrated that mononuclear oxygenated and hydroxylated cationic metal complexes in high-silica zeolites tend to self-organize into binuclear complexes. In the cases of Ga- and Fe-modified zeolites, it is shown that the catalytic activity of the most stable binuclear extraframework cations is much higher than that of the hypothetical very reactive mononuclear counterparts. This is due to a weaker binding of reaction intermediates and easier regeneration of the initial active complexes in the course of the catalytic reaction. The formation of multiple-charged binuclear oxygenated metal species in zeolites is a general phenomenon. It does not require a specific distribution of the equivalent number of negative framework charges that compensate for the positive charge of the cationic complexes. The location and the stability of cationic complexes in zeolite micropores are mainly determined by the coordination properties of the metal centres.
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