"All Polyimide" Mixed Matrix Membranes for High Performance Gas Separation

To improve the interfacial compatibility of mixed matrix membranes (MMMs) for gas separation, microporous polyimide particle (AP) was designed, synthesized, and introduced into intrinsic microporous polyimide matrix (6FDA-Durene) to form "all polyimide" MMMs. The AP fillers showed the feature of thermal stability, similar density with polyimide matrix, high porosity, high fractional free volume, large microporous dimension, and interpenetrating network architecture. As expected, the excellent interfacial compatibility between 6FDA-Durene and AP without obvious agglomeration even at a high AP loading of 10 wt.% was observed. As a result, the CO₂ permeability coefficient of MMM with AP loading as low as 5 wt.% reaches up to 1291.13 Barrer, which is 2.58 times that of the pristine 6FDA-Durene membrane without the significant sacrificing of ideal selectivity of CO₂/CH₄. The improvement of permeability properties is much better than that of the previously reported MMMs, where high filler content is required to achieve a high permeability increase but usually leads to significant agglomeration or phase separation of fillers. It is believed that the excellent interfacial compatibility between the PI fillers and the PI matrix induce the effective utilization of porosity and free volume of AP fillers during gas transport. Thus, a higher diffusion coefficient of MMMs has been observed than that of the pristine PI membrane. Furthermore, the rigid polyimide fillers also result in the excellent anti-plasticization ability for CO₂. The MMMs with a 10 wt.% AP loading shows a CO₂ plasticization pressure of 300 psi.