For the separation of CH4 and CO2 from landfill gas, pure and binary adsorption behavior of these gases were studied up to 5 atmosphere pressure at 40, 70, and 100 degrees C for silicalite as the adsorbent. Pure and binary adsorption isotherms were determined experimentally and compared to predicted isotherms by several equilibrium models, as well as the other available data in the literature. Experimental binary isotherms at different concentrations were determined by using three concentration pulse methods (CPM). HT-CPM (Harlick-Tezel CPM) was observed to be the best one to describe the behavior of this binary system. Equilibrium phase diagrams and separation factors were obtained from the experimental binary isotherms. For this system, the integral thermodynamic consistency tests were also shown and discussed.