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Jaramillo, David E; Jiang, Henry Z. H; Evans, Hayden A; Chakraborty, Romit; Furukawa, Hiroyasu; Brown, Craig M; Head-Gordon, Martin; Long, Jeffrey R
Journal of the American Chemical Society, 04/2021, Letnik: 143, Številka: 16Journal Article
The widespread implementation of H2 as a fuel is currently hindered by the high pressures or cryogenic temperatures required to achieve reasonable storage densities. In contrast, the realization of materials that strongly and reversibly adsorb hydrogen at ambient temperatures and moderate pressures could transform the transportation sector and expand adoption of fuel cells in other applications. To date, however, no adsorbent has been identified that exhibits a binding enthalpy within the optimal range of −15 to −25 kJ/mol for ambient-temperature hydrogen storage. Here, we report the hydrogen adsorption properties of the metal–organic framework (MOF) V2Cl2.8(btdd) (H2btdd, bis(1H-1,2,3-triazolo4,5-b,4′,5′-i)dibenzo1,4dioxin), which features exposed vanadium(II) sites capable of backbonding with weak π acids. Significantly, gas adsorption data reveal that this material binds H2 with an enthalpy of −21 kJ/mol. This binding energy enables usable hydrogen capacities that exceed that of compressed storage under the same operating conditions. The Kubas-type vanadium(II)–dihydrogen complexation is characterized by a combination of techniques. From powder neutron diffraction data, a V–D2(centroid) distance of 1.966(8) Å is obtained, the shortest yet reported for a MOF. Using in situ infrared spectroscopy, the H–H stretch was identified, and it displays a red shift of 242 cm–1. Electronic structure calculations show that a main contribution to bonding stems from the interaction between the vanadium d π and H2 σ* orbital. Ultimately, the pursuit of MOFs containing high densities of weakly π-basic metal sites may enable storage capacities under ambient conditions that far surpass those accessible with compressed gas storage.
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