InthispaperweusedMOF-5andCu3(BTC)2toseparateCO2/CH4andCH4/N2mixturesunderdynamicconditions.Bothmaterialsweresynthesizedandpelletized,thusallowingforameaningfulcharacterizationinviewofprocessscale-up.ThematerialswerecharacterizedbyX-raydiffraction(XRD)andscanningelectronmicroscopy(SEM).Byperformingbreakthroughexperiments,wefoundthatCu3(BTC)2separatedCO2/CH4slightlybetterthanMOF-5.BecausethecrystalstructureofCu3(BTC)2includesunsaturatedaccessiblemetalsitesformedviadehydration,itpredominantlyinteractedwithCO2moleculesandmoreeasilycapturedthem.Conversely,MOF-5withasuitableporesizeseparatedCH4/N2moreefficientlyinourbreakthroughtest.