Creation of Al-Enriched Mesoporous ZSM-5 Nanoboxes with High Catalytic Activity: Converting Tetrahedral Extra-Framework Al into Framework Sites by Post Treatment

制备具有高催化活性的富铝介孔ZSM-5纳米盒:通过后处理将四面体骨架外铝转化为骨架位点

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Abstract

ZSM-5 zeolite nanoboxes with accessible meso-micro-pore architecture and strong acid sites are important in relevant heterogeneous catalysis suffering from mass transfer limitations and weak acidities. Rational design of parent zeolites with concentrated and non-protective coordination of Al species can facilitate post-synthetic treatment to produce mesoporous ZSM-5 nanoboxes. In this work, a simple and effective method was developed to convert parent MFI zeolites with tetrahedral extra-framework Al into Al-enriched mesoporous ZSM-5 nanoboxes with low silicon-to-aluminium ratios of ≈16. The parent MFI zeolite was prepared by rapid ageing of the zeolite sol gel synthesis mixture. The accessibility to the meso-micro-porous intra-crystalline network was probed systematically by comparative pulsed field gradient nuclear magnetic resonance diffusion measurements, which, together with the strong acidity of nanoboxes, provided superb catalytic activity and longevity in hydrocarbon cracking for propylene production.

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