Mixed Matrix Membranes (MMMs) have shown advantages in overcoming trade-off effects, but there is still an urgent need to enhance CO2 separation performance in the design of multifunctional fillers. To overcome the trade-off effects in MMMs, a rational design of fillers with selective recognition for CO2 molecules is an effective strategy. A microporous nanosheet Qc-5-Cu was synthesized and incorporated into a Pebax MH 1657 (Pebax) to prepare MMMs for efficiently separating CO2 from CH4. The H atoms of the aromatic rings on the surface of pores in Qc-5-Cu constructed positive electrostatic environments, which significantly improves the CO2/CH4 separation performance of MMMs. On one hand, the constructed positive electrostatic environments in the MMMs attracted the negatively charged O atoms of CO2 molecules through electrostatic attraction, which effectively accelerated CO2 transport. On the other hand, the positive electrostatic environments established a selective barrier for preventing CH4 transport, achieving high CO2/CH4 selectivity in MMMs. Compared to pure Pebax membrane, the Pebax/Qc-5-Cu-0.5 MMM exhibited a remarkable enhancement of 99.52 % in CO2 permeability (934.24 Barrer) and a significant increase of 37.64 % in CO2/CH4 selectivity (25.01). The constructed positive electrostatic environments of nanosheets in MMMs offers a potential prospect for efficient CO2/CH4 separation.
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