Nanocomposite polymer blend membrane molecularly re-engineered with 2D metal-organic framework nanosheets for efficient membrane CO2 capture

Membrane gas separation technology is an energy-efficient alternative to the traditional industrial processes for CO2 capture towards the mitigation of global warming. To overcome the inherent performance trade-off behavior of polymeric membranes, many nanoarchitectures have been incorporated for developing high-performance mixed matrix membranes. Yet, a successful nanocomposite membrane design remains challenging, especially for CO2 capture, because of polymer-filler incompatibility and interfacial defects. Herein, 2D Cu-TCPP nanosheets were synthesized and incorporated into Pebax/Poly (ethylene glycol) methyl ether acrylate (PEGMEA) blends to design MMMs with exceptional CO2/N2 separation performance. This synergistic polymer blend after crosslinking, offers a highly accommodating and robust matrix environment for the homogenous distribution of nanosheets. Cu-TCPP particles were also produced as 3D nanoflowers to probe their morphological effect on gas transport. The finely dispersed 2D nanosheets expanded the free volume of the resultant nanocomposite membranes, leading to a significantly enhanced CO2 permeability of up to 1183 Barrer which was 93% higher than the neat polymers, while they also increased the transport pathway tortuosity that contributes to a very high CO2/N2 selectivity of 57.6 at a loading of merely 0.1 wt%. Not only do such separation performances surpassed the Robeson upper bound by a large margin and outcompeted many existing advanced MMM designs, but they also remained stable after long-term operations. By carefully elucidating the gas transport tuning effect of 2D metal-organic framework nanosheets in nanocomposite membranes, this work could help broaden their applicability for other environmentally important molecular separations.