Abstract
Experimental screening of Metal Organic Frameworks (MOFs) for separation applications can be costly and time-consuming. Computational methods can provide many benefits in this process, as expensive compounds and a wide range of operating conditions can be tested while crucial mechanistic insights are gained. TAMOF-1, a recently developed MOF, stands out for its exceptional stability, robustness and cost-effective synthesis. Its good CO(2) uptake capacity makes it a promising agent for flue gas separation applications. In this work, we combine experiments with simulations at the atomistic and numerical level to investigate the adsorption and separation of CO(2) and N(2). Using Monte Carlo simulations, we accurately reproduce experimental adsorption isotherms and elucidate the adsorption mechanisms. TAMOF-1 effectively separates CO(2) from N(2) because of preferential binding sites near Cu(2+) atoms. To assess separation performance in equilibrium at different conditions along the entire isotherm pressure range, adsorbed mole fractions, selectivities, and the trade-off between selectivity and uptake (TSN) are calculated. The dynamic separation performance is assessed by breakthrough experiments and numerical simulations, demonstrating efficient dynamic separation of CO(2) and N(2), with CO(2) being retained in the column.