From this figure, it is clear that the employed approach generates materials with progressively better characteristics (high CO2 update and low N2 uptake). This is particularly evident when comparing the shift of the Pareto front for clouds formed by cycles 1-2 with the initial set of materials (the cloud of back symbols). However, there is almost no change between the clouds corresponding to cycle 2 (red symbols) and 3 (blue symbols), indicating that we must have reached the limits of performance that can be attained using this particular design strategy. To further identify optimal MOFs based on their process-level performance, we use data from all three cycles, and we filter the structures with a CO2/N2 selectivity greater than 80 for use in process modeling and optimization. We identify 650 MOFs that meet this criterion. To somewhat save the computational load, we select 300 random structures from this pool of materials and investigate them in process simulations. Out of this group, 247 meet purity and recovery constraints.