We investigate a total of 24 MOFs that are derived from the combination of six 3d metals (Cr, Mn, Fe, Co, Ni, Cu) and four MOF structures: M-DOBDC (DOBDC = 2,5-dioxido-1,4benzenedicarboxylate), M-DSBDC (DSBDC = 2,5-disulfhydryl-1,4-benzenedicarboxylate), M2(OH)2-BBTA (BBTA = 1H,5H-benzo(1,2-d:4,5-d')bistriazole), and M2Cl2-BBTA (Supporting Information Figure ). We selected these MOFs based on the availability of corresponding experimental data for benchmarking. These MOFs possess a hexagonal array of onedimensional channels that facilitate the diffusion of gas molecules within the pores. Their undercoordinated metal sites serve as adsorption sites that can be tailored by switching the metal to selectively capture specific types of molecules. These features make these MOFs particularly promising for gas storage, capture, and separation, where selectivity is a critical factor in device performance. The SBUs of these MOFs were identified by modifying the extraction scheme implemented in MOFSimplify. Each metal atoms and all non-metal atoms up to two bonds away from it were first added to the SBU. Distinct from our previous approach, in the case where any non-metal atom is a member of a ring, all atoms within the ring are included as part of the SBU. Since the MOFs in our data set have metal clusters that are infinitely extended in one dimension, they were truncated to a repeat of three metal atoms, and the adsorbate was aligned with the central metal atom (Figure ). To avoid dangling bonds or strongly negative charges, truncated bonds were capped with hydrogen. All metals were assumed to have oxidation states of +2 with metals in high-spin states and ferromagnetically coupled. The triplet spin of O2 was assumed to be parallel with the spin of the metal atoms unless specified otherwise. The charge of the SBU was determined by summing the charge of the metal and the ligands. The full list of charge and magnetization state of MOF and SBU are provided in Supporting Information Table . The U parameter is only applied to the 3d orbitals of metal atoms. The binding energy (Eb) of a gas molecule to an SBU is calculated using PBE+U as follows: