The CNDO/2 method was used to study the interaction of CO₂ molecules with the cations situated in the S_II site of faujasite zeolites whiich have various Si/Al ratios. It was found that correlation between the electrostatic field strength of exchanged cations in the zeolites and interacting CO₂ molecules. The strengthe of interaction between them has the following order:Mg²⁺>Ca²⁺>Li⁺>Na⁺. When plotting the calculated C-O bond orders of CO₂ interac-ting with the cations and the asymmetriic stretching vibrational frequencies of corresponding CO₂, quite good correla-tion was obtained.