Extra-framework charge and impurities effect, Grand Canonical Monte Carlo and volumetric measurements of CO2/CH4/N2 uptake on NaX molecular sieve

In this work, Monte Carlo simulation of CO2, N-2, and CH4 adsorption on zeolite 13X is carried out in grand canonical ensemble. FAU framework was used to reproduce the structure of zeolite 13X. Universal force field was used to calculate the interactions between adsorbates and 13X. Metropolis method was used for calculating adsorption isotherm. Volumetric measurements were carried out to confirm the simulation results. The simulation results using Universal force field showed good agreement with experimental results. Highest CO2 uptake for this zeolite was found as 5.67 mol/kg from GCMC. Isosteric heat of adsorption was investigated to find the heat released during adsorption of each gas. The simulation result of isosteric heat of adsorption for CO2, N-2, and CH4 was utmost 17.00, 4.37, and 6.14 kcal/mole, respectively. Radial distribution graphs were used to find affinity of constituents of zeolite for CO2. Henry's constant evaluation was also performed at low pressure to find the selectivity of the structure. Henry's constant of CO2 in an equimolar mixture of N-2 and CH4 was calculated 3.49 and 1.49 mol/kg.kPa, respectively. Finally, simulation results were fitted to Toth and dual-site Langmuir isotherms to find the best fit that belongs to dual-site Langmuir.