Scandium decorated C$_{24}$ fullerene as high capacity reversible hydrogen storage material: Insights from density functional theory simulations

Abstract

Using first-principles density functional theory simulations, we have observed that the scandium decorated C$_{24}$ fullerene can adsorb up to six hydrogen molecules with an average adsorption energy of -0.35 eV per H$_2$ and average desorption temperature of 451 K. The gravimetric wt % of hydrogen for the scandium decorated C$_{24}$ fullerene system is 13.02%, which is sufficiently higher than the Department of Energy, United States demand. Electronic structure, orbital interactions, and charge transfer mechanisms are explained using the density of states, spatial charge density difference plots, and Bader charge analysis. A total amount of 1.44e charge transfer from the 3d and 4s orbitals of scandium to the 2p carbon orbitals of C$_{24}$ fullerene. Hydrogen molecules are attached to scandium decorated C$_{24}$ fullerene by Kubas type of interactions. Diffusion energy barrier calculations predict that the existence of a sufficient energy barrier will prevent metal-metal clustering. Ab-initio molecular dynamics (A.I.M.D.) simulations confirm the solidity of the structure at the highest desorption temperature. Therefore, we believe that the scandium decorated C$_{24}$ fullerene system is a thermodynamically stable, promising reversible high-capacity hydrogen storage device.