The heat of adsorption was obtained by adding 5/2RT to the calculated adsorption energy to account for the translational and rotational degree of freedom of the gas molecule, where R is the gas constant and T is the temperature. The median temperature of the range used in the relevant experiment was employed (Supporting Information Table ). The temperature variation during the experiment only influences the heat of adsorption by at most 3 kJ/mol. We neglect the zero-point vibrational (i.e., phonon) energy contribution to the adsorption energy, which is less than 5 kJ/mol and should not significantly impact the comparison with experimental data. The energy difference between the ferromagnetic and antiferromagnetic phase of the bare MOF's metal centers is also not expected to have a substantial effect on the results. For example, the difference is 4 kJ/mol for Co2(OH)2-BBTA 60 and 10 kJ/mol for Fe-DOBDC.