Abstract: Membrane technology is acknowledged as one of the most efficient for biogas upgrading, separating simultaneously CH4 and CO2 in the retentate and permeate streams, respectively. The sustainability would still be improved by using renewable and environmentally friendly materials for membrane fabrication. Specifically, this study is focused on laboratory-scale mixed gas separation tests of composite membranes prepared from chitosan (CS), a hydrophilic, biodegradable and biocompatible polymer from abundant natural resources, with good adhesive and film forming properties and high affinity for CO2 due to the primary amine and hydroxyl groups functionalities in CS. To improve mechanical resistance and CO2/CH4 separation, CS was hybridized by a 5 wt% loading of non-toxic ionic [emim][acetate] liquid (IL), and variable loadings of compatible inorganic fillers, such as 3D zeolite 4A and NaETS-10, and layered AM-4 titanosilicate. The CS-based mixed matrix layer was coated on porous polyether sulfone (PES) support. The CO2 permeance and CO2/CH4 separation were measured at different feed concentrations to evaluate the membranes performance in the treatment of different streams. This separation behavior was explained by the wet thickness, water uptake, morphology and ionic resistance of the composite membrane. As such, the 5 wt% Zeolite 4A and NaETS-10-filled ILCS/PES membranes provided a good dispersion in the ILCS matrix and the mixed matrix layer a good adhesion with the porous PES support, leading to high CO2 permeances and separation factors up to 30, whereas the more hydrophilic lamellar AM-4 titanosilicate-filled ILCS layer showed cluster agglomeration in the matrix and a faster detachment of the coated layer from the PES substrate. With increasing filler loading, an increase of the permeance of both CO2 and CH4 gas components was, although selectivity decreased upon increasing AM-4 filler loading. The CO2/CH4 mixed gas separation performance was validated by a custom-built model for a wide range of feed composition, to cover such processes as natural gas sweetening, biogas upgrading and enhanced oil recovery with acceptable relative error below 10% (absolute value), except for the AM-4 titanosilicate-filled ILCS membranes, showing morphological fabrication defects.

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