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Hierarchical Fe-MFI were synthesized by post-treatment with TPAOH and applied as catalysts in liquid phase dehydration of 1-phenylethanol. The catalysts were characterized by XRD, TEM and N2 physisorption et al. After treatment, more ferric ions occupied zeolite framework sites, leading to increase in Brønsted acid sites content. Moreover, secondary pores with pore size range in 8–100 nm were introduced into inside zeolite. The secondary pores improved the accessibility of active centers and diffusion properties of reactants. The conversion of 1-phenylethanol reached 90% with 99% styrene selectivity in 1.5 h at 80 °C, while the reaction time of hierarchical Fe-MFI is only a half of microporous Fe-MFI zeolite. Moreover, the hierarchical Fe-MFI could be reused for at least five times. [ABSTRACT FROM AUTHOR]