The separation and capture of CO₂ have become an urgent and important agenda because of the CO₂-induced global warming and the requirement of industrial products. Membrane-based technologies have proven to be a promising alternative for CO₂ separations. To make the gas-separation membrane process more competitive, productive membrane with high gas permeability and high selectivity is crucial. Herein, we developed new cellulose triacetate (CTA) and cellulose diacetate (CDA) blended membranes for CO₂ separations. The CTA and CDA blends were chosen because they have similar chemical structures, good separation performance, and its economical and green nature. The best position in Robeson’s upper bound curve at 5 bar was obtained with the membrane containing 80 wt.% CTA and 20 wt.% CDA, which shows the CO₂ permeability of 17.32 barrer and CO₂/CH₄ selectivity of 18.55. The membrane exhibits 98% enhancement in CO₂/CH₄ selectivity compared to neat membrane with only a slight reduction in CO₂ permeability. The optimal membrane displays a plasticization pressure of 10.48 bar. The newly developed blended membranes show great potential for CO₂ separations in the natural gas industry.

Currently, cellulose acetate (CA) membranes dominate membrane-based CO₂ separation for natural gas purification due to their economical and green nature. However, their lower CO₂ permeability and ease of plasticization are the drawbacks. To overcome these weaknesses, we have developed high-performance mixed matrix membranes (MMMs) consisting of cellulose triacetate (CTA), cellulose diacetate (CDA), and amine functionalized zeolitic imidazolate frameworks (NH₂-ZIF-8) for CO₂ separation. The NH₂-ZIF-8 was chosen as a filler because (1) its pore size is between the kinetic diameters of CO₂ and CH₄ and (2) the NH₂ groups attached on the surface of NH₂-ZIF-8 have good affinity with CO₂ molecules. The incorporation of NH₂-ZIF-8 in the CTA/CDA blend matrix improved both the gas separation performance and plasticization resistance. The optimized membrane containing 15 wt.% of NH₂-ZIF-8 had a CO₂ permeability of 11.33 Barrer at 35 °C under the trans-membrane pressure of 5 bar. This is 2-fold higher than the pristine membrane, while showing a superior CO₂/CH₄ selectivity of 33. In addition, the former had 106% higher CO₂ plasticization resistance of up to about 21 bar and an impressive mixed gas CO₂/CH₄ selectivity of about 40. Therefore, the newly fabricated MMMs based on the CTA/CDA blend may have great potential for CO₂ separation in the natural gas industry.

Cu-BTC (HKUST-1) metal–organic framework (MOF) is widely recognized for its carbon capture capability due to its unsaturated copper sites, high surface area, and well-defined porous structure. This study developed mixed matrix membranes (MMMs) using cellulose triacetate (CTA), incorporating bimetallic Ni-Cu-BTC MOFs for CO₂/CH₄ separation, and benchmarked them against membranes fabricated with monometallic Cu-BTC. CTA was selected for its biodegradability, membrane-forming properties, and cost-effectiveness. The optimized membrane with 10 wt.% Ni-Cu-BTC achieved a CO₂ permeability of 22.9 Barrer at 25 °C and 5 bar—more than twice that of pristine CTA—with a CO₂/CH₄ selectivity of 33.8. This improvement stems from a 51.66% increase in fractional free volume, a 49.30% rise in the solubility coefficient, and a 51.94% boost in the diffusivity coefficient. Dual-sorption model analysis further confirmed enhanced solubility and adsorption mechanisms. These findings establish CTA/Ni-Cu-BTC membranes as promising candidates for high-performance CO₂ separation in natural gas purification and related industrial processes.