This study investigates the impact of integrating Pebax® Rnew® 30R51, a sustainable elastomer-type copolymer material, with zeolitic imidazolate frameworks (ZIFs) to develop advanced membranes for CO2/CH4 gas separation. The fabrication process of ZIF/Pebax® Rnew® 30R51 thin films was optimized to achieve uniform and defect-free thin film composite (TFC) membranes. Crucial membrane properties, including permeability, selectivity and separation efficiency, were analyzed with variations in ZIF type, loading levels, film thickness and operating conditions. Additionally, the resulting TFC and ZIF/Pebax® Rnew® 30R51 thin film nanocomposite (TFN) membranes were subjected to characterization via FTIR, XRD, TGA and SEM to evaluate their physicochemical properties. Nanoparticles of ZIF-8, NH2-ZIF-8 and ZIF-94 were individually added (at 5–15 wt% loadings) to the Pebax® Rnew® 30R51 matrix to develop the CO2 separation efficiency. The pristine TFC membrane showed a 66 GPU CO2 permeance and a 37.5 CO2/CH4 separation selectivity, primarily due to improved CO2 mass transport. Upon inclusion of ZIFs, the CO2 permeance with 5 wt% loadings of ZIF-8, NH2-ZIF-8 and ZIF-94 increased to 148, 99 and 125 GPU, respectively, despite this, the CO2/CH4 separation selectivity maintained at 29.4, 37.0 and 27.0, respectively.
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