Hydrogen Storage of Mg Under an Ultralow Pressure of 1 Bar

Abstract

Magnesium hydride (MgH₂) has been regarded as an attractive candidate for solid-state hydrogen storage, yet its practical applications are limited by the requirement of elevated temperatures and sluggish hydrogen uptake and release kinetics. Herein, TiO₂ polyhedral frameworks with uniformly distributed V₂O₅ (denoted as V₂O₅/TiO₂) are constructed to improve hydrogen storage performance of Mg/MgH₂. During the reversible hydrogenation and dehydrogenation process, metallic V and Ti along with low-valent Ti- and V-based oxides are in situ formed. Among them, metallic V supported on TiO₂ exhibits the lowest hydrogen adsorption energy, enabling superior catalytic performance over TiO₂ and V₂O₅. As a result, the peak dehydrogenation temperature of MgH₂ decreases to 215°C, 105°C lower than that of pristine MgH₂, with a decrease of the apparent activation energy from 139.50 kJ·mol⁻¹ to 68.99 kJ·mol⁻¹. Moreover, electron migration from V toward TiO₂ leads to charge accumulation around Ti and O atoms, shifting the V 3d-band center toward the Fermi level and thereby improving the catalytic function of V's d-electrons, facilitating hydrogen dissociation without energy barriers. Therefore, the V₂O₅/TiO₂-catalyzed Mg absorbs 4.12 wt% H₂ under an ultralow pressure of 1 bar at 25°C. This provides a new strategy for developing advanced Ti and V-based catalysts for mild-condition hydrogen storage of MgH₂.

Keywords

catalyst / hydrogen storage material / magnesium / magnesium hydride / transition metal oxide

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