All zeolite models were optimized using the GULP code and potential parameters developed by Sanders, Leslie, and Catlow (SLC). The majority of the SLC-optimized zeolite models were already used in a previous study, where information on the experimental structure data taken as starting points for the GULP calculations is provided. The newly optimized frameworks are listed in the following, including labels of type materials and references to experimental structure data: MTT (ZSM-23 ), TUN (TNU-9 ), EUO (EU-1 ), MEI (ZSM-18 ), IWR (ITQ-24 ), and MSE (MCM-68 ), as well as CHA. The optimized cell parameters are provided in Table of the Supplementary Information, together with the size of the supercells used in Henry constant and adsorption isotherm simulations. CIF files of the SLC-optimized zeolite models are also provided as Supplementary Information. The structures of ETH and all CEs were optimized using parameters of the PCFF force field, and the N2 molecule was optimized using COMPASS parameters (although this force field is proprietary, parameters for certain small molecules are freely available ). The Lennard-Jones (LJ) parameters and partial charges from these force fields were also used to represent these molecules in the adsorption simulations. For the framework, two different sets of LJ parameters and charges were compared, namely, (1) the original PCFF parameters and