Effect of bimodal surface modification of graphyne on enhanced H2 storage: Density functional theory study

Studies on hydrogen storage materials are proceeding worldwide to enhance adsorptive capacity with a proper adsorption energy between physisorption and chemisorption. Graphyne is the carbon allotropes having sp- and sp2-hybridized carbon atoms. It has not been synthesized yet, but have taken the center stage for decades owing to its promising electronic properties and applicability. Therefore, we performed geometry optimization using density functional theory calculation to determine the adsorptive behaviors of graphyne with decoration and doping approaches for improving hydrogen storage. Graphyne decorated with alkali metal cations showed highly adsorptive properties owing to the enhanced basicity by cations, whereas doped graphyne showed a lower adsorption energy within the desirable hydrogen storage range (−0.20 eV to −0.70 eV). Therefore, we applied bimodal surface modification using doped/co-doped graphyne in the presence of alkali decoration. We found that both decoration and doping approaches compensated each other, yielding an energy suitable for hydrogen storage (min: −0.24 eV, max: −0.32 eV), which elucidates the promising properties of a hydrogen storage material.