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Adsorption as an air purification method is widely employed to remove volatile organic compounds with low concentration using zeolites. In this study, ZSM-5 and LSX zeolites modified by alkali metal cations (Li+, Na+ and K+) were used as adsorbents for the abatement of toluene. The adsorption behaviors of toluene onto adsorbents with different pore sizes and cation contents were evaluated systematically based on the experiments of adsorption equilibrium, kinetic diffusion and desorption. Besides, Langmuir and Freundlich model, constant-pattern wave propagation model and Kissinger method were applied to fit with the above experimental data. The adsorption amount followed the sequence of Li-LSX > Na-LSX > K-LSX > Li-ZSM-5 > Na-ZSM-5 > K-ZSM-5 obtained from equilibrium isotherms. LSX zeolites showed twice adsorption capacity on unit volume compared to ZSM-5. The mechanisms of steric hindrances and electrostatic interactions controlling the diffusion rate under high and low concentrations were proposed, respectively. At relatively low loadings of toluene, the diffusion resistances were primarily affected by electrostatic interaction due to preferential adsorption of toluene on cationic sites. While at relatively high loadings, the diffusion resistance was mainly restricted by steric effect because of saturated cationic sites. The strength of adsorbate-adsorbent interactions was assessed by temperature programmed desorption experiments. It showed that both adsorption sites and microporous walls contributed to the desorption energy. [ABSTRACT FROM AUTHOR]