Manadé, MontserratViñes Solana, FrancescGil, AdriàIllas i Riera, Francesc2020-06-162020-06-162018-02-071463-9076https://hdl.handle.net/2445/165806The attachment of H-2 to the full set of transition metal (TM) adatoms supported on graphene is studied by using density functional theory. Methodology validation calculations on the interactions of H-2 with benzene and graphene show that any of the vdW corrections under study, the Grimme D2, D3, D3 with Becke-Jonson damping (D3BJ), and Tkatchenko-Scheffler methods, applied on the PBE functional, are similarly accurate in describing such subtle interactions, with an accuracy of almost 2 kJ mol(-1) compared to experiments. The PBE-D3 results show that H-2 physisorbs on especially stable d(5) or d(10) TMs. In other 5d metals, and the rightmost 3d and 4d ones, H-2 dissociates, and only for Y, Mn, Fe, and Zr the H-2 binds strongly enough for its storage in the so-called Kubas mode, where the H-2 bond is sensibly elongated. Other metals (Co, Ni, Ru, Rh and Pd) feature also an elongated Kubas mode, interesting as well for H-2 storage. Sc and Ti display a Kubas modes especially suited, given their lightness, for meeting the gravimetric requirements. The H-2 interactions with TM adatoms imply a TM -> H-2 charge transfer, although the magnetic moment of the system tends to remain intact, except for the early 5d TMs, where the unpaired electron transfer seems to be associated with the H-2 bond breakage.12 p.application/pdfeng(c) Manadé, Montserrat et al., 2018Absorció de gasosTeoria del funcional de densitatAbsorption of gasesDensity functionalsinfo:eu-repo/semantics/article6781842020-06-16info:eu-repo/semantics/openAccess