Neutron scattering studies of disordered carbon anode materials

Carbon-based anodes show many promising properties in lithium-ion rechargeable batteries. So-called 'disordered carbons' are characterized by a substantial amount of residual hydrogen, and exhibit large Li uptake capacities. We have employed a variety of neutron scattering techniques, coupled with computer simulations, to study the composition, local atomic structure, and vibrational dynamics of such materials. Radial distribution function analysis of neutron diffraction data, and incoherent inelastic scattering show that the structural motif is a planar graphene fragment, with edge carbons terminated by single hydrogen atoms, and random stacking between fragments. The vibrational spectra of the hydrogen-rich carbons are remarkably similar to the spectra of the polycyclic aromatic hydrocarbon coronene in the medium-frequency region. At low frequencies, only a boson peak is observed, characteristic for glassy and disordered materials, and this feature shifts upon doping. The results are consistent with two proposed mechanisms for Li capacity, one analogous to conventional intercalation but with Li on both sides of graphene fragments, the other involving bonding of Li to H-terminated edge carbons. (author)