Size-exclusivity predicAon -Lastly, size-exclusivity is quanVfied by the overlap of the porous host KDE and the solvent KDE; as a representaVve example, KDEs of two solvents (chloroform and 15-crown-5) and CC3 are compared, and the calculated overlaps are presented (Figure ). We observe a large KDE overlap for chloroform/CC3, which indicates that the cage window and chloroform molecule are likely to take on conformaVons that are similar in size, and a small KDE overlap for 15-crown-5/CC3, which indicates that the 15-crown-5 solvent molecule takes on conformaVons that are larger than the cage window. This is expected considering chloroform is experimentally known to not be size-excluded, while 15-crown-5 is known to be size-excluded (Figure ). The KDE overlap is used as a metric that assesses the probability that a cage window and solvent molecule will be similar sizes. Using the KDE overlap, we can classify cage/solvent pairs as porous (KDE overlap < 0.25), not porous (KDE overlap > 0.35), or potenVally porous (0.25 < KDE overlap < 0.35). These designaVons are determined by the KDE kernel. Indeed, the KDE overlap cutoffs used to label candidate solvents (KDE overlap = 0.30) may be linked to the Gaussian kernel that was used to derive the KDE -within a standard Gaussian normal distribuVon, 34% of the area is one standard deviaVon away from the distribuVon mean. It should be noted that for the edge cases where the solvent molecule is sufficiently small and the pore carrier window distribuVon is sufficiently large enough to yield KDE overlap < 0.25, we further check the predicVons by verifying that the mean of the pore carrier window distribuVon is smaller than the mean of the solvent size distribuVon. If this is not the case, the pore carrier/solvent pair is flagged for manual inspecVon. We validated our size-exclusivity predicVon algorithm using a subset of the solvents from the curated database of solubility measurements above, focusing on those where it was experimentally known if the solvent was size-excluded from the caviVes of the scrambled 3 3 :13 -R POC mixture or not (Figure ). We correctly predict the size-exclusivity of all the solvents in the validaVon set. The size-exclusivity algorithm suggested that four of the solvent molecules might be size-excluded; including 2'-hydroxyacetophenone, hexachloropropene, 1,1,2,2,3,3-hexachloropropane, and perchloroethylene. We can examine the KDE overlaps for each of the systems in relaVon to the experimental gas uptake results. Experimentally, 2'hydroxyacetophenone (KDE overlap = 0.260) and hexachloropropene (KDE overlap = 0.264) are sizeexcluded. Whereas 1,1,2,2,3,3-hexachloropropane (KDE overlap = 0.292) and perchloroethylene (KDE overlap = 0.349) are not size-excluded. This result further reinforces the use of the KDE overlap as a sizeexclusivity predicVon metric; the lower the KDE overlap, the more likely the pore carrier/solvent are sizeexcluded, and vice versa. The size-exclusivity of the candidate solvents idenVfied by the computaVonal solubility screening protocol were then predicted (Figure ). From the calculated KDE overlaps, we see that diphenyl ether, 2-phenyl-1-propanol, 2-methylphenol, and 2-ethylphenol should be size-excluded, and 2-methyl-1-phenyl-2propanol and 1-phenylethanol are potenVally size-excluded. While four of the six solvents were predicted to be size-excluded, all combinaVons were taken forward as a means of validaVng the size-exclusivity predicVon algorithm.