Overall, the inclusion of molecular diffusion has led to the exclusion of up to 20% of MOF candidates from the initial rank-order. This is because either the structures did not achieve the 95% CO 2 purity threshold or because of their performance loss in terms of productivity and energy cost. In the rank-order obtained by using structure-dependent diffusivity and mass transfer coefficients, 27 MOFs have achieved volumetric productivity larger than 1.5 kg/(day.L) and specific energy consumption lower than 1 MJ/kg. For comparison, reference CO 2 solid sorbents such as Zeolite 13X and the MOF materials UTSA-16 and Mg-MOF-74, have reported productivity and energy consumption of 1-3 kg/(day.L) and 0.5-1 MJ/kg, respectively, in vacuum-swing adsorption. More recently, CALF-20 has achieved industrial-scale production with a productivity of 0.53 kg/(day.L) and an energy cost of 0.72 MJ/kg, respectively, in pressure-vacuum-swing adsorption. In Table , we provide our TOP-20 performance list that exemplifies the effect of microscopic diffusivity on rank-order that increases with crystallite diameter. For R µ = 1, 10 and 100 µm, respectively, a total of 3, 7, and 10 MOFs have dropped off the initial ranking. In case of the best-performing, TOP-1 material BOHGOU, the inclusion of molecular diffusivity in the process simulation has decreased volumetric productivity, from 1.84 to 1.33 kg/(day.L), and increased the energy cost, from 1.07 to 1.50 MJ/kg of CO 2 . We note that in the case of R µ = 100 µm, BOHGOU drops out of the TOP-20 while the TOP-2 material for all other crystallite sizes, VASFON, moves to the TOP-1 position. This highlights the importance of MOF crystallite size on CO 2 capture performance.