To understand the nature of the binding interactions between H2 and the M I centers in MOF clusters we employed Energy Decomposition Analysis based on Absolutely Localized Molecular Orbitals (ALMO-EDA). The ALMO-EDA was performed at the ωB97M-V/Def2-SVP level of theory as implemented in the Q-Chem 6.1 code. In the ALMO-EDA procedure the MOF cluster and the adsorbed hydrogen are divided into two fragments. The first portion of ALMO-EDA, is computed as the energy difference between isolated fragments at their equilibrium geometry and isolated fragments at their geometry in the complex. This portion is called the preparation energy or ΔPrep and can be interpreted as the energy necessary to distort the unbound MOF cluster and free hydrogen into their bound configurations. Subsequent single point calculations were performed on the bound complex using the frozen orbitals of isolated fragments yielding the frozen density matrix and energy (ΔFrz). The polarization energy (ΔPol) was characterized using fragment electric-field response functions (FERFs), enabling a fragment orbital to adapt to the local electric fields of its counterpart (and its electron density) in a way that is exact for dipolar and quadrupolar responses. Lastly, the charge transfer term (ΔCT) was computed from the energy difference between the fully relaxed and polarized electron density.