▎ 摘　　要

One of the most technically challenging barriers to the widespread commercialization of hydrogen-fueled devices and vehicles remains hydrogen storage. More environmentally friendly and effective nonmetal catalysts are required to improve hydrogen sorption. In this paper, through a combination of experiment and theory, we evaluate and explore the catalytic effects of layered graphene nanofibers toward hydrogen release of light metal hydrides such as sodium alanate. Graphene nanofibers, especially the helical kind, are found to considerably improve hydrogen release from NaAlH4, which is of significance for the further enhancement of this practical material for environmentally friendly and effective hydrogen storage applications. Using density functional theory, we find that carbon sheet edges, regardless of whether they are of zigzag or armchair type, can weaken Al-H bonds in sodium alanate, which is believed to be due to a combination of NaAlH4 destabilization and dissociation product stabilization. The helical form of graphene nanofibers, with larger surface area and curved configuration, appears to benefit the functionalization of carbon sheet edges. We believe that our combined experimental and theoretical study will stimulate more explorations of other microporous or mesoporous nanomaterials with an abundance of exposed carbon edges in the application of practical complex light metal hydride systems.