vacuum-swing adsorption (PSA/VSA) models at process scale that comply with the 95% CO 2 -purity and 90% CO 2 -recovery targets, respectively, issued by the the U.S. Department of Energy. Burns et al. integrated atomistic simulations with a VSA process simulator while Farmahini et al. studied the effect of mesoscale materials properties, such as size and porosity of the material constituents, on productivity and energy efficiency of the VSA process. These approaches, however, were based on the assumption that gas adsorption in MOFs does not depend on structure-dependent differences that occur at microscopic scales. Conceptually, this was reflected by assuming a constant mass transfer coefficient for all MOF candidates under investigation.