Dynamic adsorption of CO2 by CHA zeolites – Size matters

Abstract

The performance of K-CHA nanozeolite composed of discrete nanoparticles prepared by an organic template-free direct synthesis is compared to that of conventional micron-sized K-CHA with an order of magnitude difference in particle size and identical chemical composition (Si/Al ratio and cations) for the separation of dilute CO2 from N2. Breakthrough curve analysis of the zeolites meshed to identical sizes demonstrates the superior performance of nanozeolites for gas separation due to the significantly faster diffusion of CO2 molecules through the bed composed of meshed nanozeolite particles evidenced by the enhanced mass transfer, more rapid establishment of equilibrium, and faster desorption of CO2. Modelling of the CO2 breakthrough curves indicates enhanced mass transfer properties of the CHA nanozeolite due to the higher linear driving force parameter values. Variation of the modelling parameters and back-calculation of the diffusion coefficients indicates that axial diffusion contributes significantly to the mass transfer behaviour, yet also reveals significantly lower micropore diffusion resistance for the nano-sized K-CHA. These results demonstrate for rapid kinetically controlled sorption-based separations, that by reducing the size of the discrete crystallites of the meshed adsorbent particle by an order of magnitude, significant improvements in the utilization of the bed can be achieved due to the shortening of the mass-transfer zone, improving the separation performance.