Adsorption-enhanced carbon membranes derived from copolyimide for ultrafast subangstrom discriminating CO<sub>2</sub> separation.

Wang, Kaifang; Zhu, Zhongtai; Liu, Yuqi; Zheng, Weiran; Yuan, Ziyi; Lin, Zhihong; Semiat, Raphael; Shao, Lu et al. · Sci Adv · 2025

basic_science · Level V

Where this comes from

Abstract

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°C exhibit exceptional CO<sub>2</sub> separation performance, with CO<sub>2</sub> permeabilities up to 15,700 barrer and CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CH<sub>4</sub> 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 CO<sub>2</sub> and larger gases. This work demonstrates a facile, tunable strategy to engineer carbon membranes with outstanding CO<sub>2</sub> separation capabilities, offering previously unexplored opportunities for energy-efficient gas separation processes in industrial applications.