All DFT calculations of MOFs and DFT+U calculations of SBUs were performed using Quantum-ESPRESSO version 7.0 62 with projector-augmented wave pseudopotentials and an 80 Ry kinetic energy cutoff. An empirical dispersion correction of Grimme's DFT-D3 with Becke-Johnson damping was applied. Geometry optimization and DFT+U calculations of MOFs were performed with the PBE functional 66 on a 3x2x2 k-point mesh for M2(OH)2-BBTA and M2Cl2-BBTA, and a 4x2x2 k-point mesh for M-DOBDC and M-DSBDC. HSE06 calculations 56 of MOFs were performed only at the G point due to the high computational cost of these calculations. DFT+U calculations of SBUs for Hubbard U parameter fitting were performed by adding 20 Å of vacuum in all directions and applying the Martyna-Tuckerman correction for an isolated molecule.