Abstract
In this paper, a new hydrogen storage composite based on magnesium hydride and metal-organic framework MIL-101(Cr) (an acronym for Material Institute Lavoisier) has been mechanically synthesized and investigated. The hydrogen sorption and desorption behavior in the composite was investigated for the temperature and pressure ranges of (593−653) K and (0−3) MPa, respectively. According to the pressure-composition-temperature isotherms of hydrogen sorption/desorption, the MgH2–5 wt%MIL-101(Cr) composite starts to absorb hydrogen at a lower pressure at 593 K. In addition, the hydrogen release peak for composite shifts to lower temperatures by about 140 K compared to the pure milled MgH2 during temperature programmed desorption at a heating rate of 6 K/min. The activation energy of hydrogen desorption from the composite is 120 ± 2 kJ/mol, which is 36% lower than the activation energy of hydrogen desorption from magnesium hydride (189 ± 2 kJ/mol). The enthalpy of hydrogen absorption was found to be 73 kJ/mol H2 and 60 kJ/mol H2 for milled MgH2 and MgH2–5 wt%MIL-101(Cr) composites, respectively. It is showed that the MIL-101(Cr) MOF structures decompose during ball milling and the chromium oxide nanoparticles form a core-shell structure with MgH2 particles. Thus, composite has better sorption and desorption properties than pure magnesium/magnesium hydride due to the nanoconfinement of MgH2. The chromium oxide nanoparticles act as active sites on the surface of the magnesium particles and facilitate the dissociative chemisorption or recombinative desorption of hydrogen. The main regularities of the phase transition in the magnesium-hydrogen system for the composite and magnesium hydride during dehydrogenation have been studied for temperatures in the range of 298–750 K. The in situ analysis of the phase transitions during the dehydrogenation of MgH2 and MgH2–5 wt%MIL-101(Cr) composite indicates a pronounced catalytic effect of the addition of MIL-101(Cr) to the Mg/MgH2. Based on the experimental results and ab initio calculations, a mechanism for the sorption and desorption of hydrogen by the composite has been proposed.
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