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The adsorption of binary gas mixtures of CO₂–N₂, CO₂–CH₄ and CH₄–N₂ were studied by using H-ZSM-5 as the adsorbent with a SiO₂/Al₂O₃ ratio of 280. Pure isotherms for N₂ and CH₄ at 40°C and CH₄–N₂ binary isotherms at 40°C and 1.0 atm total pressure have been determined using concentration pulse chromatography. For CO₂–N₂ and CO₂–CH₄ pure and binary systems, previously published data were used. The applicability of the binary adsorption prediction models, Extended Langmuir (EL), ideal adsorbed solution theory (IAST), and the Flory–Huggins form of the vacancy solution theory (FH-VST) have been studied. The CH₄–N₂ binary isotherms exhibit behavior similar to the pure component isotherms, with CH₄ as the dominant adsorbate. The CH₄ binary isotherm did not change from the pure component isotherm. The N₂ binary isotherm decreased relative to the pure component N₂ isotherm …