Hydrogen storage in Mg/MgH2 materials is still an active research topic. In this work, a mixture of Mg-15wt.% VCl3 was produced by cryogenic ball milling and tested for hydrogen storage. Short milling time (1 h), liquid N2 cooling, and the use of VCl3 as an additive produced micro-flaked particles approximately 2.5–5.0 µm thick. The Mg-15wt.% VCl3 mixture demonstrated hydrogen uptake even at near room-temperature (50 °C). Mg-15wt.% VCl3 achieved ~5 wt.% hydrogen in 1 min at 300 °C/26 bar. The fast hydriding kinetics is attributed to a reduction of the activation energy of the hydriding reaction (Ea hydriding = 63.8 ± 5.6 kJ/mol). The dehydriding reaction occurred at high temperatures (300–350 °C) and 0.8–1 bar hydrogen pressure. The activation energy of the dehydriding reaction is 123.11 ± 0.6 kJ/mol. Cryomilling and VCl3 drastically improved the hydriding/dehydriding of Mg/MgH2.
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