Hydrogen Adsorption on Type-5 Penta-MgN₈ Sheet, Nanotube, and 3D Porous Structure

Motivated by the recent report on penta-MgN 8 sheet [ Mater. Today Phys. 2023, 38, 101259] that is the first realization of type-5 pentagonal 2D tessellation with exposed regularly distributed Mg ions, we carried out density functional theory studies on the interactions of H 2 molecules with 1D penta-nanotube, 2D penta-sheet, and 3D porous structures based on penta-MgN 8 . We found that when the penta-MgN 8 sheet is assembled to a 3D porous structure or curved to a nanotube, the bandgap increases from 1.18 to 1.35 and 1.88 eV, and the resulting derivatives are stable dynamically. When H 2 molecules are introduced, the nanotube behaves best in adsorption, where each Mg ion can adsorb three H 2 molecules: two on the outer surface and one on the inner surface. The curved geometry of the nanotube makes the Mg ion on the outer surface more exposed as compared with the situations of the 2D sheet and 3D porous structure, resulting in stronger adsorptions to H 2 . The gravimetric capacity (volumetric capacity) is 4.25 wt % (63 g/L) and 4.25 wt % (65 g/L) for the studied penta-sheet and penta-nanotube, and the corresponding desorption temperature is 115 and 162 K at 1 atm pressure, respectively, while for the 3D porous structure, the adsorption performance is poor due to the limited space and the less curvature, leading to strong steric hindrance and less exposed configuration for Mg ions. Moreover, the effects of temperature and pressure on adsorption are also discussed.