Adsorption-enhanced carbon membranes derived from copolyimide for ultrafast subangstrom discriminating CO2 separation

KF Wang and ZT Zhu and YQ Liu and WR Zheng and ZY Yuan and ZH Lin and R Semiat and L Shao and XZ He, SCIENCE ADVANCES, 11, eadv8650 (2025).

DOI: 10.1126/sciadv.adv8650

Carbon membranes are emerging as a versatile platform for the selective separation of gas mixtures with similar molecular sizes. Here, a high- performance carbon membrane is developed from an asymmetric, rigid copolyimide precursor via a precisely controlled carbonization process. Membranes carbonized at 800 degrees C exhibit exceptional CO2 separation performance, with CO2 permeabilities up to 15,700 barrer and CO2/N2 and CO2/CH4 selectivities of 63 and 52, respectively-surpassing the 2019 upper bounds. Molecular dynamic simulations, in conjunction with in situ thermogravimetric analysis-mass spectroscopy and thermogravimetric analysis-Fourier transform infrared spectroscopy, reveal the evolution of a bimodal carbon matrix with micropores (7 to 20 angstroms) and ultramicropores (4 to 7 angstroms). Gas transport is dominated by synergistic adsorption-selective and molecular sieving mechanisms, enabling subangstrom discrimination between CO2 and larger gases. This work demonstrates a facile, tunable strategy to engineer carbon membranes with outstanding CO2 separation capabilities, offering previously unexplored opportunities for energy-efficient gas separation processes in industrial applications.

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