Among the SBUs analyzed, Ag I M II 4Cl3(bta)6 (M II =Zn, Mn) and Ni I Cd II 4Cl3(bta)6 outperform the Cu I Cd II 4Cl3(bta)6 cluster that is related to the node in the recently synthesized Cu I Cd-MFU-4l. In particular, Ag I Zn II 4Cl3(bta)6 demonstrates the most efficient performance, achieving 62% usable capacity, closely approaching the theoretical maximum of 63% for the given pressure range from 5 to 100 bar. This analysis suggests that our combinatorial optimization has computationally identified candidate MFU-4type frameworks that can very closely approach the maximum possible usable hydrogen storage capacity of the peripheral open metal site that binds a single hydrogen molecule. We will discuss the Ag I M II 4Cl3(bta)6 SBUs below in more detail. To elucidate the origin of the weakening of hydrogen binding for Ag I clusters compared to the corresponding Cu I structures, we utilized the ALMO-EDA analysis to dissect the components of this noncovalent interaction. Given the similar enthalpy increase observed across structures with Zn II , Mn II , or Cd II as central atoms, our analysis concentrated on the Ag I Zn II 4Cl3(bta)6 and Cu I Zn II 4Cl3(bta)6 clusters. The ALMO-EDA results, as shown in Table , indicate that the most pronounced difference between the Cu and Ag ions lies in the polarization (ΔPol) term. This suggests that the larger ionic radius of Ag (115 pm) compared to Cu (77 pm) leads to less effective polarization of the H2 molecule. To further understand the variation in the ΔPol component, we can apply a classical dipole approximation. Given that induced dipoledipole interactions diminish with the sixth power of the distance (1/r 6 ) and knowing the distances between the metal ion and the H2 molecule in the coordinated complex, we can estimate that ΔPol for the Agcontaining structure should be about (1.7 Å / 1.9 Å) 6 = 0.51 times that of its Cu counterpart. Remarkably, the ALMO-EDA provides a ratio of ΔPol(Ag)/ΔPol(Cu) of 0.53, aligning closely with the classical estimation. We note that the preparation energy (ΔPrep) for the Ag framework should be lower than that for Cu, due to the reduced structural distortions when coordinating the H2 molecule. Additionally, the Cu cluster exhibits somewhat more repulsive ΔFrz due to stronger Pauli repulsions that are associated with its stronger overall binding. Collectively, these three factors -the change in polarization energy, the lower preparation energy, and stronger Pauli repulsion -result in an overall reduction in the total interaction energy by ~10 kJ/mol for the Ag I M II 4Cl3(bta)6 clusters. Identifying measurable characteristics that correlate with the strength of interaction between the peripheral metal site and hydrogen is essential for the future characterization of the Ag I M II -MFU-4l frameworks. In general, a longer H-H distance typically indicates a stronger metal-hydrogen interaction. In turn, H-H bond elongation can be quantitatively assessed via IR spectroscopy shifts.