Density Functional Theory Study of Light Metal (Li/Na/Ca) Functionalized Borophosphene for Reversible Hydrogen Storage

Abstract: Borophosphene is investigated for hydrogen storage by density functional theory calculations through Li, Na and Ca decoration. Decoration enhances the binding energy from -0.047 eV/H2 to -0.20 -- -0.42 eV/H2. PDOS and Bader charge analysis elucidate the role of adatom decoration in charge transfer and better binding. Up to 10, 12 and 20 H2 molecules can be adsorbed over a single Li, Na and Ca adatom, respectively, in a supercell of 32 atoms. Desorption temperature is calculated from the binding energies. A complete discharge of the stored molecules from decorated borophosphene can be realized in temperature range of 125 to 531 K. Further, decoration at multiple sites of the substrate is performed to evaluate the theoretical gravimetric density. With Li, Na, and Ca overloading, gravimetric densities of 6.22%, 5.34%, and 6.08% are obtained. NEB results show that inter-site energy barriers of the adatoms are larger than their thermal energy by an order.