“…Covalent organic frameworks (COFs) are an emerging class of porous crystalline polymers connected by organic building units through covalent bonds into highly ordered and periodic network structures. − These materials have gained tremendous attention because of their potential applications in diverse fields such as gas adsorption for separation and storage, catalysis, energy storage, optoelectronics, and many more. − Given by the versatile architectures, tunable functionalities, and well-organized pore system as well as good thermal and chemical stability, the COFs, especially the Schiff base-related 2D COF family, hold great potential for energy-efficient membrane-based molecular/ion separations in the chemical industry. − For this purpose, the development of COF membranes has attracted extensive interest in the last five years and is booming right now. − A variety of self-supporting or supported high-quality COF membranes were developed with a fascinating performance in liquid-phase separation processes such as desalination, , dye wastewater purification, − and organic solvent nanofiltration. − However, progress on COF-based membranes in selective gas separation is lagging, mainly due to the intrinsic nanometer-sized pores of the COF family (typically 0.6–10 nm) which are much larger than the kinetic diameter of ordinary gas molecules (0.25–0.5 nm). − Based on the topology diagrams and pore-wall surface engineering, − it is difficult to design the COFs with an aperture size in the gas molecular-selective region. Approaches including staggered stacking, − oriented growth, and hybridization with other microporous nanomaterials , have been explored to reduce the effective pore size of COF membranes toward the ultramicroporous range, mainly aiming at improving the molecular sieving mechanism.…”