Nondissociative Adsorption ofH2Molecules in Light-Element-Doped Fullerenes

Abstract

First-principles density functional and quantum Monte Carlo calculations of light-element doped fullerenes reveal significantly enhanced molecular ${\mathrm{H}}_2$ binding for substitutional B and Be. A nonclassical three-center binding mechanism between the dopant and ${\mathrm{H}}_2$ is identified, which is maximized when the empty $p_z$ orbital of the dopant is highly localized. The calculated binding energies of $0.2–0.6\mathrm{eV}/{\mathrm{H}}_2$ is suited for reversible hydrogen storage at near standard conditions. The calculated ${\mathrm{H}}_2$ sorption process is barrierless, which could also significantly simplify the kinetics for the storage.