Commercial bioethanol can be readily converted into ethylene by a dehydration process using solid acids, such as Brønsted acidic H-ZSM-5 zeolites, and thus, it is an ideal candidate to replace petroleum and coal for the sustainable production of ethylene. Now, strong Lewis acidic extra-framework three-coordinate Al3+ species were introduced into H-ZSM-5 zeolites to improve their catalytic activity. Remarkably, Al3+ species working with Brønsted acid sites can accelerate ethanol dehydration at a much lower reaction temperature and shorten the unsteady-state period within 1-2 h, compared to >9 h for those without Al3+ species, which can significantly enhance the ethanol dehydration efficiency and reduce the cost. The reaction mechanism, studied by solid-state NMR, shows that strong Lewis acidic EFAl-Al3+ species can collaborate with Brønsted acid sites and promote ethanol dehydration either directly or indirectly via an aromatics-based cycle to produce ethylene.
Keywords: MFI zeolite; acidity; aluminum; ethanol to olefin; solid-state NMR spectroscopy.
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