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


Myrzakhmetov B. Shomenov T. Sultanov F. Wang Y. Mentbayeva A.
9 May 2025Elsevier Ltd

International Journal of Hydrogen Energy
2025#126413 - 428 pp.

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 Energys 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.

Adsorption energy , Defective graphene , Density functional theory , Gravimetric hydrogen capacity , Hydrogen storage , Lithium-decorated graphene , Nitrogen-doped graphene

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Center for Energy and Advanced Materials Science, National Laboratory Astana, Nazarbayev University, 53 Kabanbay Batyr Avenue, Astana, 010000, Kazakhstan
Department of Chemical and Materials Engineering, School of Engineering and Digital Sciences, Nazarbayev University, 53 Kabanbay Batyr Avenue, Astana, 010000, Kazakhstan

Center for Energy and Advanced Materials Science
Department of Chemical and Materials Engineering

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