Charge transfer through interfaces in metal-ion intercalation systems

Lithium-ion batteries have become the dominant power sources for portable electronics, and are regarded as the primary battery technology for electric vehicles. Despite the tremendous success in the practical application of lithium-ion batteries, the fundamentals of their operation are still being actively studied. Charge transfer through complex multicomponent and dynamic interfaces still remains the most obscure process, as no kinetic or molecular-level model is capable of adequately describing the sequence of elementary events during metal-ion intercalation into a solid host. In this chapter, we summarize the current knowledge of charge transfer through interfaces in lithium-ion batteries, which is available both from experimental studies of intercalation kinetics and from molecular modeling of various interfaces in these systems. Despite the controversies in interpretation, the current state of understanding of charge transfer in lithium-ion batteries allows us to hope for a self-consistent description of ion intercalation, which will be built in the near future, relying largely on the latest advances in ab initio modeling of complex systems.