Surface phonons of lithium ion battery active materials

Abstract

Surfaces of active materials are understood to play an important role in the performance and lifetime of lithium-ion batteries, but they remain poorly characterized and therefore cannot yet be systematically designed. Here, we combine inelastic neutron scattering and ab initio simulations to demonstrate that the structure of the surface of active materials differs from the interior of the particle. We use LiFePO₄ (LFP) as a model system, and we find that carbon coating influences the Li–O bonding on the (010) LFP surface relative to the bulk. Our results highlight how coatings can be used to systematically engineer the vibrations of atoms at the surface of battery active materials, and thereby impact lithium ion transport, charge transfer, and surface reactivity.