Graphdiyne (GDY) is a recently discovered two-dimensional carbon allotrope that holds significant promise for applications in hydrogen adsorption and storage technology. This study investigates the impact of nitrogen doping and sodium decoration on the hydrogen adsorption capacity of GDY nanosheets while examining their influence on electronic and structural properties. Various deliberate impurities are introduced to create modified-GDY structures.

Nitrogen doping triggers a transition from a semiconductor to a semi-metallic state, driven by differences in electronegativity and adjustments in bond lengths. Cohesive energy (Ecoh) is found to be -7.231 eV for the most stable N-doped GDY. In contrast, sodium decoration enhances conduction by modifying charge distribution. The other most stable structures are Na-decorated GDY with Eads of -3.804 eV and N, Na-decorated GDY with -3.347 eV. Modified-GDY structures exhibit higher hydrogen adsorption energies compared to pristine GDY, with N-doped GDY displaying the highest energy levels (Eads = -0.455eV ). Maximum hydrogen adsorption capacities are assessed for each structure, and a notable improvement is observed in Na-decorated GDY (19 H2), significantly enhancing the storage capacity to 13.8 wt%, which shows a 10.21 wt% increase in H2 adsorption compared to pure GDY (3.59 wt%).

These findings underscore the potential of modified-GDY for hydrogen storage applications, highlighting the effectiveness of structural carbon modification in enhancing hydrogen adsorption capacity.