The stronger interaction of TCS with protonated zeolites can be attributed to the formation of hydrogen bonds between the framework proton and the Oh atom of TCS, which, unlike the weak Hh•••OZeo hydrogen bonds found in all-silica zeolites, are too stable to be broken at room temperature. However, calculations including the co-adsorption of water showed that the stronger interaction would not necessarily translate into higher removal efficiencies: The HZeo•••Oh hydrogen bond is not strong enough to remain stable in the presence of a cluster of water molecules, and framework deprotonation with concurrent formation of a hydronium ion in the pores is energetically favored. Thus, it appears unlikely that a bonding of TCS to framework protons could be realized in real systems, where these more hydrophilic areas of the structure will be occupied by clusters of H2O molecules. In such a material, TCS could still be adsorbed in the more hydrophobic areas of the pore system, meaning that the presence of some framework Al atoms and charge-balancing protons will not necessarily have a completely detrimental effect on the removal efficiency. However, it can be inferred that the removal efficiency will deteriorate with decreasing Si/Al ratio, as indeed observed experimentally. Putting together the findings outlined above, it appears that the hydrophobicity should be maximized in order to develop adsorbents with maximal TCS removal efficiency. Since smaller pores afford stronger dispersion interactions with the pore walls, the pores of an "ideal" adsorbent should, of course, be large enough to accommodate TCS and allow its diffusion, but not much larger. However, there appears to be little scope to optimize specific features of the pore shape. Although the present work looked exclusively at high-silica zeolites, it seems likely that these general criteria could also be applied to adsorbents from other classes. Furthermore, similar relationships should be valid for organic molecules of similar hydrophobicity and flexibility. In contrast, the shape and size of the pores have a much larger impact on the affinity towards more rigid molecules like CBZ. This difference highlights that guest molecule flexibility should be taken into account when searching for suitable adsorbents.