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Structure and Reactivity of Al-O(H)-Al Moieties in Siloxide Frameworks: Solution and Gas-Phase Model Studies. | LitMetric
Even though aluminas and aluminosilicates have found widespread application, a consistent molecular understanding of their surface heterogeneity and the behavior of defects resulting from hydroxylation/dehydroxylation remains unclear. Here, we study the well-defined molecular model compound, [Al (μ -OH) (THF) (PhSi(OSiPh O) ) ], 1, to gain insight into the acid-base reactivity of cyclic trinuclear Al (μ -OH) moieties at the atomic level. We find that, like zeolites, they are sufficiently acidic to catalyze the isomerization of olefins. DFT and gas phase vibrational spectroscopy on solvent-free and deprotonated 1 show that the six-membered ring structure of its Al (μ -OH) core is unstable with respect to deprotonation of one of its hydroxy groups and rearranges into two edge-sharing four-membered rings. This renders Al -O(H)-Al units strong acid sites, and all results together suggest that their acidity is similar to that of zeolitic Si -O(H)-Al groups.
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