Mixed Matrix Membranes for Efficient CO₂ Separation Using an Engineered UiO-66 MOF in a Pebax Polymer

Mixed matrix membranes (MMMs) have attracted significant attention for overcoming the limitations of traditional polymeric membranes for gas separation through the improvement of both permeability and selectivity. However, the development of defect-free MMMs remains challenging due to the poor compatibility of the metal-organic framework (MOF) with the polymer matrix. Thus, we report a surface-modification strategy for a MOF through grafting of a polymer with intrinsic microporosity onto the surface of UiO-66-NH₂. This method allows us to engineer the MOF-polymer interface in the MMMs using Pebax as a support. The insertion of a PIM structure onto the surface of UiO-66-NH₂ provides additional molecular transport channels and enhances the CO₂ transport by increasing the compatibility between the polymer and fillers for efficient gas separation. As a result, MMM with 1 wt% loading of PIM-grafted-MOF (PIM-g-MOF) exhibited very promising separation performance, with CO₂ permeability of 247 Barrer and CO₂/N₂ selectivity of 56.1, which lies on the 2008 Robeson upper bound. Moreover, this MMM has excellent anti-aging properties for up to 240 days and improved mechanical properties (yield stress of 16.08 MPa, Young's modulus of 1.61 GPa, and 596.5% elongation at break).