Modular Customization and Regulation of Metal–Organic Frameworks for Efficient Membrane Separations

Abstract Metal–organic frameworks (MOFs) are considered ideal membrane candidates for energy‐efficient separations. However, the MOF membrane amount to date is only a drop in the bucket compared to the material collections. The fabrication of an arbitrary MOF membrane exhibiting inherent separation capacity of the material remains a long‐standing challenge. Herein, we report a MOF modular customization strategy by employing four MOFs with diverse structures and physicochemical properties and achieving innovative defect‐free membranes for efficient separation validation. Each membrane fully displays the separation potential according to the MOF pore/channel microenvironment, and consequently, an intriguing H 2 /CO 2 separation performance sequence is achieved (separation factor of 1656–5.4, H 2 permeance of 964–2745 gas permeation unit). Taking advantage of this strategy, separation performance can be manipulated by a non‐destructive modification separately towards the MOF module. This work establishes a universal full‐chain demonstration for membrane fabrication‐separation validation‐microstructure modification and opens an avenue for exclusive customization of membranes for important separations.