Nevertheless, there is still an important role for the U CCSD(T) parameter in yielding more accurate results for the full MOF system. Optimizing the geometry of a periodic MOF using a GGA such as PBE and then employing CCSD(T) calculations on a cluster SBU model of the MOF, a typical approach in MOF studies, can misrepresent the heat of adsorption. PBE tends to overbind the gas molecules, leading to an underestimation of the metal-molecule distances (Supporting Information Tables ). Especially for Co2(OH)2-BBTA and Co2Cl2-BBTA, the short metal-molecule distance of PBE-optimized structure causes the CCSD(T)-evaluated single-point energy to indicate a positive (repulsive) N2 adsorption energy. The potential energy curve for Co2(OH)2-BBTA interacting with N2 exemplifies the efficacy of the U CCSD(T) parameter in correcting the overbinding tendency of PBE. Indeed, the potential energy curve of the SBU calculated using PBE+U CCSD(T) aligns closely with that calculated using CCSD(T) (Supporting Information Figure ). Still, potential energy curves from both PBE and PBE+U calculations reveal that relying solely on the SBU can underestimate the adsorption strength compared to the MOF. Therefore, a full periodic MOF model combined with the U CCSD(T) correction can offer a more accurate representation of the gas adsorption, especially when the CCSD(T) results are unambiguous regarding the spin of MOF metal nodes.