Ca-decorated holey graphyne for reversible hydrogen storage: Insights from DFT analysis

Abstract

We theoretically examine the hydrogen storage capabilities of a newly synthesized carbon allotrope known as holey graphyne (HGY). HGY exhibits weak interaction with H2, making it unsuitable for storage, thus prompting surface modification. Ca binds to HGY with a binding energy of −2.03 eV and experiences a diffusion energy barrier of 1.49 eV. The supercell of HGY accommodates six Ca atoms, and each Ca atom binds five H2 with an average binding energy of −0.27 eV, resulting in an uptake capacity of 12.07 wt% and desorption temperature of 331K at 5 bar. AIMD simulation and positive phonon frequencies confirms thermal and dynamic stability of Ca-decorated HGY. RDG analysis reveals electrostatic interactions between Ca and HGY, and van der Waals interactions between H2 and Ca. Thus, Ca-decorated HGY shows exceptional uptake capacity, desirable adsorption energy and desorption temperature, making it a suitable material for on-board reversible hydrogen storage in light vehicles.