Estimation of CO₂ Separation Performances through CHA-Type Zeolite Membranes Using Molecular Simulation

Chabazite (CHA)-type zeolite membranes are a potential material for CO₂ separations because of their small pore aperture, large pore volume, and low aluminum content. In this study, the permeation and separation properties were evaluated using a molecular simulation technique with a focus on improving the CO₂ separation performance. The adsorption isotherms of CO₂ and CH₄ on CHA-type zeolite with Si/Al = 18.2 were predicted by grand canonical Monte Carlo, and the diffusivities in zeolite micropores were simulated by molecular dynamics. The CO₂ separation performance of the CHA-type zeolite membrane was estimated by a Maxwell-Stefan equation, accounting for mass transfer through the support tube. The results indicated that the permeances of CO₂ and CH₄ were influenced mainly by the porosity of the support, with the CO₂ permeance reduced due to preferential adsorption with increasing pressure drop. In contrast, it was important for estimation of the CH₄ permeance to predict the amounts of adsorbed CH₄. Using molecular simulation and the Maxwell-Stefan equation is shown to be a useful technique for estimating the permeation properties of zeolite membranes, although some problems such as predicting accurate adsorption terms remain.