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Cu-exchanged aluminosilicate zeolites have been intensively studied for the selective oxidation of methane to methanol via a chemical looping manner, while the nature of active Cu-oxo species for these catalysts is still under debate. This study inquired into the effects of Al distribution on methane oxidation over Cu-exchanged aluminosilicate zeolites, which provided an effective way to discern the activity difference between mononuclear and polynuclear Cu-oxo species. Specifically, conventional Na+/Co2+ ion-exchange methods were applied to quantify isolated Al and Al pair (i.e., Al−OH−(Si−O)1–3−Al−OH) sites for three mordenite (MOR) zeolites, and a correlation was established between the reactivity of the resultant Cu-MOR catalysts and the portions of the accessible framework Al sites. These results indicated that the Cu-oxo clusters derived from the Al pair sites were more reactive than the CuOH species grafted at the isolated Al sites, which is consistent with in situ ultraviolet-visible spectroscopic characterization and density functional theory calculations. Further theoretical analysis of the first C–H bond cleavage in methane on these Cu-oxo species unveiled that stabilization of the formed methyl group was the predominant factor in determining the reactivity of methane oxidation.

Critical Role of Al Pair Sites in Methane Oxidation to Methanol on Cu-Exchanged Mordenite Zeolites