The intrinsic porosity in the periodic structures of metal-organic frameworks (MOFs) endows them with a great potential for membrane separation. However, facile fabrication of crystalline MOF membranes has been challenging and limited to few materials for economic and environmental considerations. Herein, a continuous Zr-MOF thin film with a thickness of ≈180 nm has been fabricated via in situ recrystallization of MOF nanoparticles on the porous support under formic acid vapor. Owing to the inherent microporosity and the well-established hydrophilicity during membrane fabrication, the MOF thin films exhibit excellent pervaporation performance with separation factors of 2630, 501 and fluxes of 1.45, 1.41 kg m −2 h −1 ) for n-butanol dehydration and methanol/methyl tert-butyl ether (MeOH/MTBE) separation, respectively. The structural stability of the film has been further confirmed by its steady performance in the 10-day pervaporation test. This in situ recrystallization method induced by a trace amount of acid vapor with no extra ingredients opens a new avenue for the facile membrane fabrication of various MOF materials to feasibly realize their versatile potential as membrane materials.

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