Lithium Functionalization in a Three-Dimensional Graphene Monolith for Enhanced Adsorption–Desorption Hydrogen Storage
Majid EL Kassaoui, Mohammed Loulidi, A. Benyoussef, A. El Kenz, O. Mounkachi
Abstract
Three-dimensional (3D) carbon allotropes have been extensively researched for their potential new applications in batteries, gas separation, and electronic devices. Therefore, this current study investigates the suitability of 3D porous HZGM-42 for efficient hydrogen storage due to its enlarged pore size, mechanical rigidity, and the stability of decorating lithium (Li) atoms on the channels by a polarization mechanism, using state-of-the-art theoretical simulations. Our findings demonstrate that 3D HZGM-42 is an ideal material with high thermal and thermodynamic stability, high Li-binding strength (−2.92 eV), hydrogenation adsorption in the appropriate range (−0.233 eV/H 2 ), theoretical H 2 storage capacity (6.08 wt %), and very-low activation barriers (0.018–0.026 eV) for H 2 migration. Furthermore, the exploration of the effect of equilibrium pressure on the van’t Hoff desorption temperature of the HZGM-42 system shows that, at 100 Atm, the dehydrogenation temperature reaches standard conditions (243 K) with a desorption time of 67 ns. The effectiveness of hydrogen adsorption–desorption cycles of fully hydrogenated Li@HZGM-42 at near room temperature was also investigated using ab initio molecular dynamics calculations. We believe that this study expands the scope of valuable insights into experimental explorations of 3D carbon networks for high-performance hydrogen storage.