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Mixed‐matrix membranes (MMMs) of Matrimid® and polyaniline/clay (PC) are investigated for CO2/CH4 separation and CO2‐induced plasticization. PC particles are synthesized through in‐situ polymerization of aniline in the presence of organophilic clay and then incorporated into Matrimid by solution casting method. Chemical structure and morphology of PC powder and fabricated membranes are analyzed by Fourier transform infrared (FTIR), X‐ray diffraction (XRD), differential scanning calorimetry/thermogravimetric analysis (DSC/TGA) and scanning electron microscopy (SEM). The XRD spectra of PC particles show the exfoliation of silicate layers throughout the polyaniline (PAni) matrix, and SEM images indicate flower‐petal morphology for PC particles. The permeability values of CO2 and CH4 increase 30–35% by incorporation of 10 wt% PC without any significant drop in selectivity. PC particles with flower‐petal morphology plays an important role in increasing the gas permeability values of both gases while Matrimid is the only phase that controls CO2/CH4 selectivity. The plasticization pressure was increased to 30 bar by incorporation of 10 wt% PC in the Matrimid matrix. CO2 permeability and pplast improved 35% and 200%, respectively, resulting in 300% enhancement in the capacity of MMM in the purification of natural gas with a selectivity of about 40. Copyright © 2016 John Wiley & Sons, Ltd.

To minimize the cost and energy consumption of liquid separations, there is a widespread research interest in developing newly emerging materials, such as supramolecular materials. Supramolecular materials with non-covalent interactions and dynamic bonds show robust and reversible physiochemical properties and have advantages for liquid separations due to their easy synthesis by simply mixing appropriate counterparts, fascinating reversibility of the ensembles, and diverse functionalities. Molecular recognition-driven self-assembly plays a key role in the fabrication of supramolecular aggregates and networks through cross-linking and block copolymerization. Block copolymers prohibit the degradation or depolymerization of supramolecular structures under various physicochemical and biological conditions. Water-based supramolecular membranes that are sustainable in harsh conditions and effective in contaminants’ removal have attained much interest. Polyelectrolytes are the other suitable precursors for the preparation of supramolecular materials. Self-healing and stimuli-responsiveness are also discussed as the novel features of these materials with diverse applications as membranes and adsorbents. Finally, the main challenges and perspectives in the fabrication of supramolecular membranes are represented.