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Immobilization of phosphonium ionic liquid (IL) onto activated carbon (AC) was synthesized via grafting and impregnated methods, and the modified materials were analyzed via Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction, thermal gravity analysis, scanning electron microscope, pore structure and CO2/N2 adsorption selectivity. The effect of the gas flow rate (100–500 mL/min) and adsorption pressure (0.2–0.6 MPa) on the dynamic adsorption behavior of mixture gas containing 15 vol.% CO2 and 85 vol.% N2 was explained using a breakthrough method. By analyzing the breakthrough curves, the adsorption capacity was determined. The results show that surface functionalization of activated carbon with phosphonium ionic liquid is conducive to improving CO2/N2 selectivity, especially ionic liquid-impregnated film. The different adsorption behaviors of impregnated and grafted adsorbents are observed under various conditions. The grafted AC had better CO2 adsorption and mass transfer due to a lower blockage of pores by ionic liquid.