Highly air-stable magnesium hydrides encapsulated by nitrogen-doped graphene nanospheres with favorable hydrogen storage kinetics

Severe surface oxidation and sluggish kinetic rates of Mg hydrides (MGHs) are the main bottlenecks for their industrial applications. Herein, we present a strategy to simultaneously tackle these problems. The nano-size MGHs were encapsulated in nitrogen-doped graphene nanospheres (NGNSs) via a facile wet-chemical method. This configuration not only prevented the MGHs from oxidation when exposed to air even after a long duration, but also stimulated faster kinetic rates of hydrogen absorption and desorption owing to the nano-size effect of MGHs and the unique electronic structure of NGNSs. As a result, MGHs of ca. 20 nm were coated by a few layered NGNSs to form MGH@NGNSs nanocomposite. A high hydrogen absorption capacity of 6.5 wt% was achieved at 200 degrees C within 0.4 h, with a releasing hydrogen capacity of 5.5 wt% at 300 degrees C within 0.5 h, indicating that this composite has obtained remarkably hydrogen storage performance. Density Functional Theory (DFT) based calculations suggested that the hydrogen adsorption/desorption kinetics were significantly fast at the interface of Mg surface and NGNSs with pyridinic configuration. This strategy paves a way for the development of high-performance Mg-based hydrogen storage materials for industrial applications.