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Impact of pore connectivity on the design of long-lived zeolite catalysts.

Angewandte Chemie (International ed. in English) (2014-11-08)
Maria Milina, Sharon Mitchell, David Cooke, Paolo Crivelli, Javier Pérez-Ramírez
RÉSUMÉ

Without techniques sensitive to complex pore architectures, synthetic efforts to enhance molecular transport in zeolite and other porous materials through hierarchical structuring lack descriptors for their rational design. The power of positron annihilation lifetime spectroscopy (PALS) to characterize the pore connectivity in hierarchical MFI zeolites is demonstrated, establishing a direct link with the enhanced catalyst lifetime in the conversion of methanol to valuable hydrocarbons. The unique ability to capture subtleties of the hierarchical structure originates from the dynamic nature of the ortho-positronium response to the pore network. The findings reveal the strong dependence on the way in which the hierarchical zeolites are manufactured, having direct implications for the practical realization of these advanced catalysts.

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