Structural, Mechanical, Electronic, and Optical Properties of Hydrogen-Storage Magnesium-Based Mg2XH9 (X = Cs, Rb)

Metal hydrides are emerging hydrogen-storage materials that have attracted much attention for their stability and practicality. The novel magnesium-based metal hydride Mg2CsH9 was investigated using the CALYPSO software (version 7.0). First-principles predictive methods were then employed to investigate the structural, mechanical, electronic, optical, and hydrogen-storage properties of Mg2CsH9 and its alkali metal substitution structure Mg2RbH9. The negative formation energy, compliance with the Born stability criterion, and absence of imaginary modes in the phonon spectrum collectively confirm the thermodynamic, mechanical, and dynamic stability of Mg2XH9 (X = Cs, Rb), fulfilling the basic criteria for practical hydrogen-storage applications. Mg2RbH9 is particularly outstanding in terms of its hydrogen-storage capacity, with a gravimetric capacity of 6.34 wt% and a volumetric capacity as high as 92.70 g H2/L, surpassing many conventional materials. The pronounced anisotropic characteristics of both compounds further enhance their practicality and adaptability to complex working conditions. An analysis of Poisson’s ratio revealed that the chemical bonding in both compounds is predominantly ionic. The details of the band structures and density of states indicate that Mg2CsH9 and Mg2RbH9 are semiconductors. Their optical properties confirm them as being high-refractive-index materials.