Scalable MOF-based mixed matrix membranes with enhanced permeation processes facilitate the scale application of membrane-based carbon capture technologies

• Scalable MOF used to prepare CO 2 separation membranes which has more potential for large-scale preparation assisting sustainable carbon capture. • MOF with only 5% doping significantly intensified the membrane. • MMMs achieved CO 2 permeability up to 8003 barrer with 25% improvement in CO 2 /N 2 selectivity. • DFT calculations combined with related permeation theory explain the mechanism of selective CO 2 transport. Mixed-matrix membranes (MMMs) leverage the processability of polymers and selectivity of Metal-Organic Frameworks (MOFs). However, they still suffer from poor interfacial compatibility and limited scalability in preparation. In certain polymers, MOFs can bridge the pores within the polymer membrane, enhancing the CO 2 adsorption and solubility properties, thus selectively boosting the CO 2 permeability. In this study, high-performance MMMs were prepared using scalable CALF-20 in combination with PIM-1. MMMs with a 5% doping level achieved CO 2 permeability up to 8003 barrer with 25% improvement in CO 2 /N 2 selectivity. This enhancement was attributed to well-designed MMMs, where MOFs matched the abundant non-interconnecting pores in the PIM-1 membrane. This study represents a significant advancement towards scaling up the preparation of high-performance MOF-based MMMs for carbon capture applications. Scalable prepared CALF-20 was applied to the preparation of MMMs and CO2 separation studies of MMMs. MOF uniformly distributed CALF-20@PIM-1 MMMs were prepared, and their separation performance (permeability and selectivity) was enhanced at the same time, which, together with the scalable CALF-20 and the expandable membrane preparation method, endowed the study with extraordinary scale-up and application potential.