Untwisting Strategy of MOF Nanosheets in Ultrathin Film Membrane for High Molecular Separation Performance.

Oriented 2D metal-organic framework (MOF) membranes hold considerable promise for industrial separation processes. Nevertheless, the lattice misalignment caused by the twisted stacking of 2D nanosheets reduces the in-plane pore size and exerts a significant impact on the membrane separation performance. Precisely regulating the stacking pattern of oriented 2D MOF membranes remains a significant challenge. Here, a scalable scrape-coating technique supplemented by a vapor untwisting strategy is proposed to directly construct non-twisted and ultrathin Zr-BTB membranes (Zr-BTB-M) on polyvinylidene fluoride (PVDF) substrates. The Zr-BTB nanosheets are induced to undergo lattice reorganization during the coating process, resulting in highly overlapped lattices and the largest in-plane pore channels. The exceptional butyl acetate selective adsorption capacity of non-twisted Zr-BTB, combined with its provision of highly ordered vertical penetrating pathways, significantly enhances molecular transport. After facile polydimethylsiloxane (PDMS) coating, the pervaporation separation index of the PDMS/Zr-BTB-M/PVDF membrane is found to be 9.74 times higher than that of conventional PDMS/PVDF membranes, paving the way for innovative, high-efficiency, energy-saving membrane separation technologies.