Storing molecular hydrogen in porous media is one of the promising avenues for mobile hydrogen storage. In order to achieve technologically relevant levels of gravimetric density, the density of adsorbed H-2 must be increased beyond levels attained for typical high surface area carbons. Here, we demonstrate a strong correlation between exposed and coordinatively unsaturated metal centers and enhanced hydrogen surface density in many framework structures. We show that the MOF-74 framework structure with open Zn2+ sites displays the highest surface density for physisorbed hydrogen in framework structures. Isotherm and neutron scattering methods are used to elucidate the strength of the guest-host interactions and atomic-scale bonding of hydrogen in this material. As a metric with which to compare adsorption density with other materials, we define a surface packing density and model the strength of the H-2-surface interaction required to decrease the H-2-H-2 distance and to estimate the largest possible surface packing density based on surface physisorption methods.
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