Abstract

Three types of methoxy-like intermediates were generated at methane interaction with Cu-loaded ZSM-5 zeolite, containing copper in the form of either Cu2+ cations (Cu2+/H-ZSM-5) or [Cu3(µ-O)3]2+ oxo-clusters (CuO/H-ZSM-5). The methoxy species were tested for the reaction with benzene and carbon monoxide. 13C MAS NMR spectroscopy reveals that the methoxy species formed on CuO/H-ZSM-5 easily interact with benzene yielding toluene, whereas the methoxy species on Cu2+/H-ZSM-5 are less effective for benzene methylation. At the same time, the methoxy species on Cu2+/H-ZSM-5 can interact with CO forming surface acetate species, while strong adsorption of CO by [Cu3(µ-O)3]2+ oxo-clusters of CuO/H-ZSM-5 inhibits the reaction.

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