Hydrogen adsorption on pristine and modified graphene: DFT insights into defects, doping, and decoration

Graphene, defected graphene, and lithium-decorated nitrogen-doped graphene are investigated as potential hydrogen storage materials using first-principles density functional theory (DFT) calculations. To prevent metal-metal clustering and maintain stable configurations, Li atoms are strategically positioned within hexagonal carbon rings, enhancing the efficiency of hydrogen adsorption. The results indicate that Li-decoration enables graphene to adsorb three to five hydrogen molecules, achieving a gravimetric hydrogen storage capacity of up to 8.8 wt.%, surpassing the U.S. Department of Energy's recommended target. Among the systems studied, nitrogen doping combined with lithium decoration results in the highest adsorption energy of 0.26 eV per hydrogen molecule, attributed to enhanced charge redistribution. The adsorption energy range supports efficient and reversible hydrogen storage. These findings highlight the potential for defect engineering, doping, and decoration in the tailoring of graphene-based materials for hydrogen storage, which contributes to advances in sustainable energy technologies. • To prevent metal–metal clustering, Li is placed on hexagonal rings, ensuring stable H 2 adsorption • 2N-doped graphene with Li decoration exhibits the highest adsorption energy and H 2 storage capacity • Calculated adsorption energies confirm reversible H 2 storage under practical conditions • Li-decorated and N-doped graphene system showed a H 2 storage capacity of 8.8 wt%, according to DFT calculations • DFT calculations provide key insights into the electronic structure, charge distribution, and adsorption behavior