partial charges were either computed via the DDEC 12 protocol or the extended charge equilibration (EQeq) method 13 for the experimental and in silico structures, respectively. Geometric properties are obtained using Zeo ++ , 14 including the crystal density and void fraction. Even though the crystal structures are assumed to be rigid, the probe radii used to compute the void fraction and adsorption properties for CH 4 molecules are scaled by 80% to account for some amount of flexibility in MOFs. In our molecular simulations, the crystal structures are assumed to be rigid, and the UFF force field 11 is used to describe the framework atoms. The TraPPE 16 force field is used to describe the CH 4 -CH 4 interactions. The guest-framework interactions are defined using the Lorentz-Berthelot 17 combining rules. The pure component adsorption isotherms at 298.15 K for CH 4 are computed using the procedure developed by Moubarak et al. . The Automated Interactive Infrastructure and Database for Computational Science, AiiDA 19 workflow named IsothermAccurateWorkChain, which is part of the aiida-lsmo plugin, 20 is used to run all the calculations.