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.
Keywords: CO2 separation; Maxwell–Stefan equation; chabazite; grand canonical Monte Carlo; molecular dynamics; zeolite membrane.