Abstract: Alternative materials are needed to tackle the sustainability of membrane fabrication in light of the circular economy, so that membrane technology keeps playing a role as sustainable technology in CO2 separation processes. In this work, chitosan (CS)-based mixed matrix thin layers have been coated onto commercial polyethersulfone (PES) supports. The CS matrix was loaded by non-toxic 1-Ethyl-3-methylimidazolium acetate ionic liquid (IL) and/or laminar nanoporous AM-4 and UZAR-S3 silicates prepared without costly organic surfactants to improve CO2 permselectivity and mechanical robustness. The CO2/CH4 separation behavior of these membranes was evaluated experimentally at different feed gas composition (CO2/CH4 feed mixture from 20:80 to 70:30%), covering different separation applications associated with this separation. A cross-flow membrane cell model built using Aspen Custom Modeler was used to validate the process performance and relate the membrane properties with the target objectives of CO2 and CH4 recovery and purity in the permeate and retentate streams, respectively. The purely organic IL-CS and mixed matrix AM-4:IL-CS composite membranes showed the most promising results in terms of CO2 and CH4 purity and recovery. This is correlated with their higher hydrophilicity and CO2 adsorption and lower swelling degree, i.e., mechanical robustness, than UZAR-S3 loaded composite membranes. The purity and recovery of the 10 wt.% AM-4:IL-CS/PES composite membrane were close or even surpassed those of the hydrophobic commercial membrane used as reference. This work provides scope for membranes fabricated from renewable or biodegradable polymers and non-toxic fillers that show at least comparable CO2/CH4 separation as existing membranes, as well as the simultaneous feedback on membrane development by the simultaneous correlation of the process requirements with the membrane properties to achieve those process targets.

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