A first-principles study of the tuning effect of a Fe2O3 cluster on the dehydrogenation properties of a LiBH4 (001) surface

Abstract

First-principles calculations were performed to investigate the effects of a Fe₂O₃ cluster on the structural, electronic and dehydrogenation properties of a LiBH₄ (001) surface. O atoms interact with Li atoms to form Li–O bonds, corresponding to an experimentally found ternary Li–Fe oxide. The DOS results show that the coupling effect of the spin-unrestricted Fe d orbitals, especially the spin-up state of Fe d orbitals, plays a crucial role in the hybridizations of H s, B p, and Fe d orbitals. The Fe₂O₃ cluster will serve as the nucleation site of surface activation at the surface of LiBH₄ to improve the dehydrogenation kinetics of LiBH₄. The doping of the Fe₂O₃ cluster is advantageous to facilitate the release of a H₂ molecule from not only the surface layer but also the inner layer of the LiBH₄ (001) surface.