Given that the unique chemical environments of MOFs are primarily attributed to the presence of metals, the role of metals was investigated. Supplementary Figure illustrates the distribution of point charges across various metals, revealing that metals with higher point charges tend to exhibit greater discrepancies between UFF+DDEC and DAC-SIM results in Supplementary Figure ). Metals with elevated point charges can function as hard Lewis acids and polarize neighboring atoms nearby metals (typically oxygen or nitrogen atoms within MOFs). This polarization effect decreases the polarizability of adjacent atoms relative to similar atoms in different environments, while the metal's polarizability remains largely unchanged. However, since UFF utilizes fixed parameters, it is unable to accurately account for this variation in polarizability. Although point charges such as DDEC are generally applied to enhance interaction modeling by providing additional electrostatic potential, they are only partially effective in specific cases and often exacerbate discrepancies. Therefore, the overestimation of Qst in UFF+DDEC calculations is particularly pronounced for H2O molecule, which can induce stronger electrostatic potential compared to CO2 molecule.