In Fig. and, we can observe that similar conclusions can be drawn for CO 2 : the Henry coefficient is mispredicted by cDFT for strong MOF-CO 2 interactions and small maximal pore sizes. cDFT underestimates the Henry coefficient for stronger MOF-CO 2 interactions, whereas the Coulombic interactions are included for CO 2 . A possible explanation is that the stronger the Coulombic interactions, the more likely the sampling algorithm for the Coulombic interactions (described in the Supplementary Materials S1B) is to miss the optimal orientation, leading to interactions that are less strong than they should be. Concerning the effect of the small pores, a similar explanation could be given here as for N 2