Facile Morphology and Porosity Regulation of Zeolite ZSM-5 Mesocrystals with Synergistically Enhanced Catalytic Activity and Shape Selectivity

Abstract

The morphology and mesoporosity of zeolite are two vital properties to determine its performance in diverse applications involving adsorption and catalysis; while it remains a big challenge for the synthesis and regulation of zeolites with exceptional morphology/porosity only through inorganic-ions-based modification. Herein, by simply optimizing the alkali metal type (K+ or Na+), as well as alkali/water ratio and crystallization temperature, the zeolite ZSM-5 mesocrystals with diverse mesostructures are simply and controllably prepared via fine-tuning the crystallization mechanism in an organotemplate-free, ions-mediated seed-assisted system. Moreover, the impacts of these key parameters on the evolution of seed crystals, the development and assembly behavior of alumi-nosilicate species and the solution-phase process during zeolite crystallization are investigated by means of directional etching in NH4 F or NaOH solutions. Except for the morphology/mesoporosity modulation, their physical and chemical properties, such as particle size, microporosity, Si/Al ratio and acidity, can be well maintained at a similar level. As such, the p/o-xylene adsorption and catalytic performance of o-xylene isomerization are used to exhaustively evaluate the synergistically enhanced catalytic activity and shape selectivity of the obtained products. This work demonstrates the possibil-ity of effectively constructing novel zeolite mesostructures by simply altering parameters on simple ions-controlled crystallization and provides good models to inspect the impacts of mesoporosity or morphology on their catalytic performances.