hjm+N387+E44 along with three large-pore best performing MOFs. In the same figure we also show CO2 and N2 adsorption isotherms for these materials and compare them with data for CALF-20 from Lin et al. . We observe trend similar to that of the first generation of materials: all materials adsorb very little nitrogen; large-pore materials tend to adsorb significant amount of CO2 (>15 mol/kg at 1 bar and 298 K). CO2 adsorption in hjm+N387+E44 is comparable to that of CALF-20, however N2 adsorption is much lower leading to a significant process improvement. In particular, due to its high adsorption selectivity, hjm+N387+E44 requires a significantly reduced time for adsorption step (~30 seconds) to meet purity constraints compared to CALF-20 (~250 seconds), resulting in enhanced productivity. In Figure of the SI we provide the geometric characterization and distributions of process design variables on the Pareto front for