Facile Ionization of the Nanochannels of Lamellar Membranes for Stable Ionic Liquid Immobilization and Efficient CO2 Separation

Two-dimensional (2D) lamellar membranes, with highly ordered nanochannels between the adjacent layers, have revealed potential application prospects in various fields. To separate gases with similar kinetic diameters, intercalation of a functional liquid, especially an ionic liquid (IL), into 2D lamellar membranes is proved to be an efficient method due to the capacity of imparting solubility-based separation and sealing undesired defects. Stable immobilization of a high content of liquid is challenging but extremely required to achieve and maintain high separation performance. Herein, we describe the intercalation of a typical IL, 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]), into the ionized nanochannels of sulfonated MXene lamellar membranes, where the sulfonate groups are anchored onto MXene nanosheets through a facile method based on metal-catechol chelating chemistry. Thanks to the intrinsic benefits of MXene as building blocks and the decorated sulfonate groups, the optimal membrane possesses adequate interlayer spacing (similar to 1.8 nm) and high IL uptake (similar to 47 wt %) and therefore presents a CO(2 )permeance of 519 GPU and a CO2/N2 selectivity of 210, outperforming the previously reported liquid-immobilized lamellar membranes. Moreover, the IL loss rate of the membrane within 7 days at elevated pressure (5 bar) is measured to be significantly decreased (from 43.2 to 9.0 wt %) after growing sulfonate groups on the nanochannel walls, demonstrating the excellent IL storage stability.